Sustained release formulations, methods for preparation and uses thereof

Abstract

The present disclosure relates to a method of preparing a sustained release formulation, the method comprises, mixing of a carrier composition with a volatile organic substance to form a blend; the carrier composition comprises: (i) a hydrophobic organic carrier; and (ii) a quaternary amine, as well as to methods of preparing the sustained release formulation. Also forming part of the present disclosure is a sustained release formulation comprising a blend of: (i) a hydrophobic organic carrier; (ii) a quaternary amine and (iii) a volatile organic substance; wherein the sustained release formulation is essentially water free; and wherein the quaternary amine is of a source different from the source of the hydrophobic organic carrier, as well as to the uses of the sustained release formulation for controlling a target organism. Finally, there is a disclosed carrier composition comprising a blend of: (i) a hydrophobic organic carrier; and (ii) a quaternary amine.

Description

[0001] SUSTAINED RELEASE FORMULATIONS, METHODS FOR PREPARATION AND USES THEREOF

[0002] TECHNOLOGICAL FIELD

[0003] The present disclosure relates to formulations that allow controlled release of volatile compounds.

[0004] BACKGROUND ART

[0005] References considered to be relevant as background to the presently disclosed subject matter are listed below:

[0006] US Patent Application Publication No. 20150147288

[0007] - US Patent No. 10,624,337

[0008] - US Patent No. US8, 137,715

[0009] Song C et al. "Self -assembled thymol-betaine co-crystals with controlled release and hygroscopic properties as green preservatives for aflatoxin prevention" Food Chemistry 456 (2024a) 140037

[0010] Song C J et al. "Small to supra: Self-assembling cocrystals for controlled release of active volatiles - An emerging strategy for food preservation" Trends in Food Science & Technology 152 (2024b) 104664

[0011] Abranches, D. O. et al., "Understanding the Formation of Deep Eutectic Solvents: Betaine as a Universal Hydrogen Bond Acceptor," ChemSusChem, 2020, DOI: 10.1002 / cssc.202001331.

[0012] US patent application publication no. 2009 / 0263511

[0013] US patent application publication no. 2017 / 0332629 Acknowledgement of the above references herein is not to be inferred as meaning that these are in any way relevant to the patentability of the presently disclosed subject matter.BACKGROUND

[0014] US Patent Application Publication No. 20150147288 describes environmentally friendly pesticide compounds, formulations, methods of preparation and application and utilities thereof.

[0015] US Patent No. 10,624,337 describes particles with a controllable release of at least one pheromone, wherein a) the particle has a core which is surrounded by one or more layers, and b) the core and at least one layer surrounding the core comprises at least one pheromone to be released, wherein the core and / or at least one layer surrounding the core comprises a substrate for binding or for absorbing the at least one pheromone to be released, wherein the substrate is capable of dispensing the absorbed pheromone in a delayed manner, and the substrate comprises zeolite.

[0016] US Patent No. US8,137,715 describes the use of dill oil or a mixture of two or more components thereof as a potentiator for a pesticide, such as an insecticide and in particular a pyrethroid is described, together with compositions containing dill oil, and their use in agriculture and in veterinary applications.

[0017] Song et al. (2024a, 2024b) describe the use of self-assembling co-crystal systems based on betaine and volatile organic compounds, such as thymol, for controlling the release of active volatiles, in the context of food preservation and green preservative technologies.

[0018] Abranches et al. (2020) investigate the molecular interactions governing the formation of betaine-based deep eutectic solvents, focusing on hydrogen-bonding mechanisms between betaine and organic compounds.

[0019] US20090263511 and US20170332629 describe pesticidal compositions in which dill oil or components thereof are used as potentiators for insecticides, particularly pyrethrin-based formulations, including emulsifiable concentrates and oil-in-water emulsions for agricultural and public health applications.GENERAL DESCRIPTION

[0020] The present disclosure provides, in accordance with a first of its aspects, a method of preparing a sustained release formulation, the method comprises mixing a carrier composition with a volatile organic substance; wherein the carrier composition comprises:

[0021] (i) a hydrophobic organic carrier; and

[0022] (ii) a quaternary amine of a general formula (I),

[0023]

[0024] wherein

[0025] Ri, R2 and R3 represent, independently, a C1-C3 alkyl chain;

[0026] X represents Ci-Ce alkylene or Ci-Ce alkenylene chain; and

[0027] Y represents an end moiety selected from the group consisting of carboxylic acid, ester, hydroxyl and quaternary ammonium moiety; and wherein the mixing provides a blend of the hydrophobic organic carrier and the quaternary amine.

[0028] An alternative method of preparing a sustained release formulation, in accordance with the presently disclosed first aspect, comprises mixing (i) a hydrophobic organic carrier (ii) a quaternary amine having a general formula (I):

[0029]

[0030] wherein

[0031] Ri, R2 and R3 represents, independently C1-C3 alkyl chain;

[0032] X represents Ci-Ce alkylene or alkenylene chain; andY represents an end moiety selected from the group consisting of carboxylic acid, ester, hydroxyl, quaternary ammonium moiety;

[0033] and (iii) a volatile organic substance, the quaternary amine

[0034] wherein the mixing forms a blend; and

[0035] wherein the hydrophobic organic carrier, the quaternary amine and volatile organic substance, are as defined

[0036] The present disclosure also provides, in accordance with a second of its aspects, a sustained release formulation comprising a blend of: (i) a hydrophobic organic carrier; (ii) a quaternary amine having a general formula (I):

[0037]

[0038] wherein

[0039] Ri, R2 and R3 represents, independently C1-C3 alkyl;

[0040] X represents Ci-Ce alkylene or alkenylene chain; and

[0041] Y represents an end moiety selected from the group consisting of carboxyl, ester, hydroxyl, quaternary ammonium moiety, and

[0042] and (iii) a volatile organic substance ;

[0043] wherein the sustained release formulation is essentially water free; and

[0044] wherein the quaternary amine is of a source different from the source of the hydrophobic organic carrier.

[0045] It is to understood that when referring to different sources, it means the quaternary amine is not inherently present in the hydrophobic organic carrier and is introduced as a distinct component.

[0046] The present disclosure further provides, in accordance with a third aspect, a method of controlling a target organism, the method comprises exposing a targetorganism or a habitat of a target organism to a sustained release formulation comprising (i) a hydrophobic organic carrier; (ii) a quaternary amine of general formula (I):

[0047]

[0048] wherein

[0049] Ri, R2 and R3 represents, independently C1-C3 alkyl;

[0050] X represents Ci-Ce alkylene or alkenylene chain; and

[0051] Y represents an end moiety selected from the group consisting of carboxyl, ester, hydroxyl, quaternary ammonium moiety, and

[0052] (iii) a volatile organic substance;

[0053] wherein the sustained release formulation is essentially water free.

[0054] In accordance with yet a fourth aspect of the presently disclosed subject matter, there is provided the use of a sustained release formulation for controlling a target organism, the sustained release formulation comprising (i) a hydrophobic organic carrier, (ii) a quaternary amine having the general formula (I) as defined herein; and (iii) a volatile organic substance.

[0055] In accordance with a fifth aspect, the present disclosure provides a carrier formulation, the carrier formulation comprising a blend of: (i) a hydrophobic organic carrier; and (ii) a quaternary amine of general formula (I)

[0056]

[0057] wherein

[0058] Ri, R2 and R3 represent, independently, a C1-C3 alkyl;

[0059] X represents a Ci-Ce alkylene or alkenylene chain; andY represents an end moiety selected from the group consisting of carboxylic acid, ester, hydroxyl, and quaternary ammonium moiety.

[0060] Finally, in accordance with a sixth aspect, the present disclosure provides a carrier composition comprising the carrier composition comprising a blend of: (i) a hydrophobic organic carrier; and (ii) a quaternary amine of general formula (I)

[0061]

[0062] wherein Ri, R2 and R3 represent, independently, a C1-C3 alkyl; X represents a Ci-Ce alkylene or alkenylene chain; and Y represents an end moiety selected from the group consisting of carboxylic acid, ester, hydroxyl, and quaternary ammonium moiety.

[0063] BRIEF DESCRIPTION OF THE DRAWINGS

[0064] In order to better understand the subject matter that is disclosed herein and to exemplify how it may be carried out in practice, embodiments will now be described, by way of non-limiting example only, with reference to the accompanying drawings, in which:

[0065] Figure 1 is a graph showing release rates of thymol over time at a temperature of 50°C in various formulations: as a free thymol, in a formulation without amino acids ("Formulated, no amino acid"), and in formulations with different amino acids, including glycine betaine ("Glycine-Betaine”), beta-alanine ("Beta-Alanine”), Valine ("Valine"), Glutamine ("Glutamine"), Arginine ("Arginine"), Histidine ("Histidine"), and Tryptophan ("Tryptophan").

[0066] Figure 2 is a graph showing release rates of thymol over time at a temperature of 50 °C in different forms: as a free molecule ("Free Thymol"), in a formulation without amino acids ("Formulated, no amino acid"), and in formulations containing various glycine types, including glycine ("Glycine"), glycine betaine ("Glycine-Betaine"), and glycine-betaine-calcium stearate ("Glycine-Betaine-Ca-stearate").Figure 3 is a graph showing release rates of thymol over time at a temperature of 50 °C in various forms: as a free molecule ("Free Thymol"), in a formulation without amino acids ("Formulated, No amino acid"), and in formulations with different quaternary ammonium salts, such as glycine betaine ("Glycine-Betaine") and cetyltrimethylammonium chloride ("cetyltrimethylammonium chloride").

[0067] Figure 4 is a graph showing evaporation rates over time at a temperature of 50°C of clove oil ("Free Clove oil"), tea tree oil ("Free Tea Tree oil"), and mint oil ("Free Mint oil") in their natural (free) state, and when incorporated into formulations containing glycine-betaine ("Formulated Clove oil", "Formulated Tea Tree oil" and "Formulated Mint oil").

[0068] Figure 5 is a graph showing the remaining amount of the pheromone methyl eugenol (ME) in different formulations after a period of 203 days, the formulation including a commercial formulation ("Commercial") and from exemplified formulations containing 10%w / w ("Formulation A" or "Formulation B") or 20%w / w ("Formulation C") of ME as defined by Gas Chromatography Mass Spectrometry (GC / MS) analysis; dark grey bars indicate the amount of ME in the formulation on day 1 and light grey bars indicate the amount of ME in the formulation on day 203.

[0069] Figure 6 is a graph showing the decrease in the amount of thymol from the tested formulation over 80 days as defined by GC / MC analysis.

[0070] DETAILED DESCRIPTION

[0071] The present disclosure is based on the development of environmentally friendly formulation that provides sustained release of beneficial volatile, water-immiscible, organic substances.

[0072] Specifically, it was unexpectedly found that when combining a volatile organic substance in a formulation comprising a hydrophobic organic carrier and at least one quaternary amine, such as glycine betaine, that is essentially homogenously blended within (and embedded within) the hydrophobic organic carrier, the release profile of the volatile substance is statistically significantly slower (in terms of days, or even weeksslower) than its release from the same formulation absent of the quaternary amino acid and / or absent of the hydrophobic carrier.

[0073] A unique feature of the presently disclosed subject matter is that the hydrophobic organic carrier together with the quaternary amine are used as a platform, carrier composition, and later combined with a volatile organic substance of interest to form the sustained release formulation for the particular volatile organic substance, before actual use.

[0074] Thus, in accordance with a first of its aspects, the present disclosure provides method of preparing a sustained release formulation, the method comprising mixing a carrier composition with a volatile organic substance; the carrier composition comprises (i) a hydrophobic organic carrier; and (ii) a quaternary amine wherein the mixing provides a blend of the hydrophobic organic carrier and the quaternary amine.

[0075] The quaternary amine, according to the present disclosure, has the general formula (I):

[0076] R2- N i: - X - Y

[0077] R3 (I)

[0078] in which

[0079] Ri, R2 and R3 represent, independently, a C1-C3 alkyl chain;

[0080] X represents Ci-Ce alkylene or Ci-Ce alkenylene chain; and

[0081] Y represents an end moiety selected from the group consisting of carboxylic acid, ester, hydroxyl and quaternary ammonium moiety.

[0082] An alternative method forming part of the first aspect of the present disclosure is one that provides a same sustained release formulation, however, by any order of addition of the components. Thus, the alternative method of the first aspect of the present disclosure, comprises mixing (i) a hydrophobic organic carrier, (ii) a quaternary amine of the general formula (I) as defined herein, and (iii) a volatile organic substance, wherein the mixing forms a blend.ln accordance with a second aspect of the presently disclosed subject matter, there is provided a sustained release formulation comprising a blend of a hydrophobic organic carrier, (ii) a quaternary amine having the general formula (I) as defined herein, and (iii) a volatile organic substance.

[0083] An essential feature of the disclosed sustained release formulation is that it is in a non-emulsion form, and this is due to the absence of sufficient water to form an emulsion, thus being considered essentially water free, as further detailed and defined herein.

[0084] An additional feature of the disclosed sustained release formulation is that the quaternary amine and the hydrophobic organic carrier are from different sources, i.e. it is not a natural hydrophobic material that inherently comprises the quaternary amine as defined herein.

[0085] In accordance with yet a further aspect, there is provided the carrier composition per se, namely, a composition comprising a blend of: (i) a hydrophobic organic carrier; and (ii) a quaternary amine of general formula (I)

[0086] R2- N 11 - X - Y

[0087] R3 (I),

[0088] wherein Ri, R2 and R3 represent, independently, a C1-C3 alkyl; X represents a Ci-Ce alkylene or alkenylene chain; and Y represents an end moiety selected from the group consisting of carboxylic acid, ester, hydroxyl, and quaternary ammonium moiety. This carrier composition can be used for later blending with the volatile organic substance, to obtain the presently disclosed sustained release formulation.

[0089] As used herein, it is to be understood that, unless the context clearly indicates otherwise, terms used with respect to the disclosed methods, sustained release formulations, and carrier compositions are intended to have the same meaning and scope when applied mutatis mutandis to each other.

[0090] In some examples of the presently disclosed subject matter, the sustained release formulation described herein is obtained or obtainable by the disclosed methods(according to the first aspect of the present disclosure). It is to be understood, in the context of the present disclosure that, unless otherwise explicitly stated, the term "sustained release formulation" relates to the formulation as defined herein, irrespective of the method of its preparation.

[0091] Further, in the context of the presently disclosed subject matter, the term "sustained release formulation" which can be used, at times, interchangeably with the term "slow release formulation" refer to a formulation where, while the volatile organic substance is releasable or released from the formulation upon its exposure, no more than 11% of the volatile organic substance is release within the first 14 days as determinable by Gas Chromatography mass spectra (GC-MS). The release is determinable with test conditions comprising a 50 gram sample (measured at room temperature), evenly placed in an uncapped cylinder container with a diameter of 65mm and height of 20-40mm, in 50°C unsealed incubator.

[0092] In some examples of the presently disclosed subject matter, the release is of no more than 20% at 28 consecutive days, as determined by the aforesaid sample size and test conditions.

[0093] In some examples of the presently disclosed subject matter, the release is of no more than 30% at 49 consecutive days, as determined by the aforesaid sample size and test conditions.

[0094] In some examples of the presently disclosed subject matter, the release is of no more than 42% at 98 consecutive days, as determined by the aforesaid sample size and test conditions.

[0095] In some examples of the presently disclosed subject matter, the release is of no more than 52% at 140 consecutive days, as determined by the aforesaid sample size and test conditions.

[0096] In some examples of the presently disclosed subject matter, the formulation has a sustained release formulation rate is one exhibiting an essentially linear release rate under essentially constant environmental conditions (e.g. temperature, humidity, UV exposure, surface area of exposure, ratio between surface area and volume offormulation, etc.). As used herein, the term "essentially linear release rate" refers to a release profile of the volatile organic substance in which the cumulative amount of the active ingredient released over a specified time period approximates a straight-line function. In some embodiments, the release rate does not deviate by more than about 10% from a best-fit linear slope for at least about 80% of the total release duration. Minor deviations outside these parameters are within the scope of this definition, provided the overall release pattern remains substantially linear when evaluated according to standard analytical methods.

[0097] As noted above, a unique feature of the presently disclosed sustained release formulation is that it is essentially water free or if water is detected, the amount of the water is less than the amount capable of forming an emulsion when the volatile organic substance is mixed with a hydrophobic organic carrier as defined herein.

[0098] In the context of the presently disclosed subject matter, the term "essentially water free" is to be understood to mean that there is no detectable amount of water or if detected, the amount is insufficient to form an oil in water emulsion. In other words, it is to be understood that the presently disclosed sustained release formulation is not an emulsion.

[0099] The presence of water in the formulation can be determined using any analytical method known in the art, including, without being limited thereto, Karl Fischer (KF) titration, which provides precise and quantitative measurement of water content; loss on drying (LOD) or thermogravimetric analysis (TGA), which determines water content based on weight loss upon heating; near-infrared spectroscopy (NIR), which enables rapid, non-destructive water content analysis in formulations by measuring water absorption in the near-infrared spectrum; and gas chromatography (GC) with thermal conductivity or mass spectrometry detection, which allows for the detection of trace water in volatile formulations. Other suitable analytical techniques may also be used, depending on the formulation type and the required sensitivity.

[0100] For the avoidance of doubt, the term "essentially water free" as used herein encompasses any one or more of the following alternative definitions: (i) no intentionally added water; (ii) no detectable free water as determined by an analyticalmethod having a detection limit of 0.5 wt% or less; (iii) a total water content below 5 wt%, at times below 3 wt%, at times below 1 wt%; and / or (iv) a water content insufficient to form a stable oil-in-water or water-in-oil emulsion under ambient conditions. These definitions are to be understood as alternative and cumulative characterizations of a substantially non-aqueous system.

[0101] In some examples of the presently disclosed subject matter, when referring to an amount of water that is less than the amount capable of forming an emulsion when mixed with a hydrophobic carrier it refers to an amount of less than 5% (w / w) out of a total weight of the formulation. At times, the amount is less than 4% (w / w) out of a total weight of the formulation; at times, less than 3% (w / w) out of a total weight of the formulation; at times, less than 2% (w / w) out of a total weight of the formulation; at times, less than 1% (w / w) out of a total weight of the formulation; at times, even less than 0.5% (w / w) out of a total weight of the formulation.

[0102] In some examples of the presently disclosed methods and the presently disclosed formulation comprise the hydrophobic organic carrier is of natural source.

[0103] As used herein, the term "source," when referring to the origin of a component, denotes the biological or natural origin from which the component is derived, including plant, animal, microbial, or mineral origin, and does not refer to supplier, manufacturer, or commercial origin.

[0104] In some embodiments, the phrase "of a source different from the source of the hydrophobic organic carrier" means that the quaternary amine is not inherently present within, and is not naturally co-extracted from, the same biological material from which the hydrophobic organic carrier is obtained.

[0105] Further, as used herein, the term "hydrophobic organic carrier of natural source” is to be understood to mean an organic, carbon-containing substance obtained from naturally occurring sources, including but not limited to waxes, lipids, fatty acids, fatty alcohols, triglycerides, phospholipids, sterols, and polymers of plant, animal, or microbial origin.In some examples of the presently disclosed subject matter, the hydrophobic organic carrier comprises lipids and / or polymers.

[0106] It is to be understood, in the context of the present disclosure, that the term "hydrophobic organic carrier" also includes synthetic or semi-synthetic substances that are chemically identical to, or materially indistinguishable on a molecular basis from, their naturally occurring counterparts, as well as chemical derivatives thereof that retain the functional characteristics of a hydrophobic organic carrier suitable for embedding, retaining, and releasing volatile substances, including derivatives obtained by chemical modification that does not materially alter the hydrophobic carrier function.

[0107] For the avoidance of doubt, hydrophobic organic carriers exclude inorganic materials such as mineral-based substances.

[0108] In some examples of the presently disclosed subject matter, the hydrophobic organic carrier comprises any one or a combination of wax(es), fatty acid(s) and triglyceride(s).

[0109] In some examples of the presently disclosed subject matter, the hydrophobic organic carrier comprises at least one wax.

[0110] When referring to wax, in the context of the presently disclosed subject matter it is to be understood to have its commonly acceptable meaning, i.e. esters formed from a long-chain fatty acid (typically 14-36 carbons) and a long-chain alcohol (typically 16-30 carbons).

[0111] In some examples of the presently disclosed subject matter, the at least one wax comprises or is naturally occurring wax, i.e. a wax that is found in nature.

[0112] When referring to naturally occurring wax it is to be understood to encompass any one or combination of plant-derived waxes, animal-derived waxes and mineral-derived waxes.

[0113] In some examples of the presently disclosed subject matter, the hydrophobic organic carrier comprises plant-derived wax(es).A non-limiting list of plant-derived waxes includes Carnauba wax, Candelilla wax, Rice Bran wax, Soy wax, Jojoba wax, Sunflower wax, Ouricury wax, Sugarcane wax, Bayberry wax (Myrtle wax), Esparto Grass wax, Flax wax, Corn wax, Peanut wax, Kapok wax, Cocoa Butter wax, Mango wax, Shea wax, Grape wax, Olive wax and Castor wax.

[0114] In some examples of the present disclosed subject matter, the hydrophobic organic carrier comprises at least carnauba wax.

[0115] In some examples of the presently disclosed subject matter, the hydrophobic organic carrier comprises animal derived wax(es).

[0116] A non-limiting list of animal-derived waxes includes beeswax, lanolin and shellac wax, Spermaceti wax and Chinese insect wax.

[0117] In some examples of the presently disclosed subject matter, the hydrophobic organic carrier comprises beeswax.

[0118] A non-limiting list of other waxes that are hydrocarbon organic carriers, includes montan wax, ozokerite wax, ceresin wax, paraffin wax, microcrystalline wax, and petrolatum.

[0119] In some examples of the presently disclosed subject matter, the at least one wax comprises or is a synthetic wax.

[0120] A non-limiting list of synthetic waxes includes polyethylene waxes, fischer-tropsch waxes, silicone waxes, polypropylene waxes and polyalphaolefin (PAO) waxes.

[0121] In some examples of the presently disclosed subject matter, the at least one wax comprises or is a semi-synthetic wax.

[0122] As used herein, the term "semi-synthetic wax" refers to a wax that comprises at least one chemically modified natural wax or a blend of natural and synthetic components. In some examples, semi-synthetic wax is derived from natural plant-based, animal-based, or petroleum-based waxes that have been subjected to any one or combination of hydrogenation, esterification, polymer modification, oxidation, or blending with synthetic waxes or polymers. All semi-synthetic waxes, in accordance with the present disclosure, retain the functionality of embedding volatile substances.A non-limiting list of semi-synthetic waxes includes hydrogenated beeswax, hydrogenated Jojoba wax, hydrogenated castor wax, polymer modified carnauba wax, modified montan wax, chemically hydrogenated rice bran wax, hydrogenated soy wax, modified sunflower wax, esterified natural wax, modified petroleum-derived microcrystalline wax, oxidized polyethylene wax, polyglycerol esters of fatty acids derived from plant sources, and the like.

[0123] It is to be appreciated that the wax component of the hydrophobic organic carrier, if present, can be a combination of waxes.

[0124] In some examples of the presently disclosed subject matter, wax component of the hydrophobic organic carrier comprises or consists of naturally occurring wax(es).

[0125] In some examples of the presently disclosed subject matter, the hydrophobic organic carrier comprises triglyceride(s).

[0126] In the context of the presently disclosed subject matter, triglycerides within the hydrophobic organic carrier are naturally occurring triglycerides. In this context, it is to be understood that naturally occurring triglycerides are typically encompassed within natural oils, as most natural oils are primarily composed of triglycerides (the natural oils may also contain minor amounts of free fatty acids and other components such as phospholipids, sterols, and antioxidants).

[0127] Thus, in the context of the presently disclosed subject matter, natural triglycerides and natural oils can be used interchangeably, when referring to their use as part of the hydrophobic organic carrier.

[0128] A non-limiting list of natural oils that can be used in the context of the hydrophobic organic carrier of the presently disclosed formulation includes avocado oil, coconut oil, corn oil, canola oil, neem oil, linseed oil, soybean oil, olive oil, sunflower oil, safflower oil and palm oil, cranberry seed oil, hemp oil, rosehip oil, moringa oil, mustard oil, perilla oil, tobacco oil, coffee oil, henna oil, carrot seed oil.

[0129] The hydrophobic organic carrier may include also non-natural triglycerides (which are not sourced from the natural oil), these including, for example, non-naturaltriglycerides such as petrochemical-derived synthetic triglycerides and CO2-based synthetic triglycerides.

[0130] In some examples of the presently disclosed subject matter, the hydrophobic organic carrier comprises a combination of at least one wax and at least one natural oil, preferably plant-derived oil.

[0131] In some examples of the presently disclosed subject matter, that hydrophobic organic carrier comprises a combination of a naturally occurring wax and a naturally occurring oil.

[0132] In some examples of the presently disclosed subject matter, that hydrophobic organic carrier comprises a combination of at least carnauba wax, coconut oil and neem oil.

[0133] In some examples of the presently disclosed subject matter, that hydrophobic organic carrier comprises a combination of at least beeswax and avocado oil.

[0134] In some examples of the presently disclosed subject matter, that hydrophobic organic carrier comprises a combination of at least rice wax and any modified form thereof that essentially retains the hydrophobic character of the rice wax, shea butter and sesame seed oil.

[0135] In some examples of the presently disclosed subject matter, the hydrophobic organic carrier comprises polymers, such as environmentally friendly polymers.

[0136] The amount of the hydrophobic organic carrier to be used in the presently disclosed methods and / or as part of the presently disclosed sustained release formulation is at least 10% (w / w) out of a total weight of the formulation.

[0137] In some examples of the presently disclosed subject matter, the amount of the hydrophobic organic carrier to be used in the presently disclosed methods and / or as part of the presently disclosed formulations and / or carrier compositions is at least 20% (w / w) out of a total weight of the sustained release formulation.

[0138] In some examples of the presently disclosed subject matter, the amount of the hydrophobic organic carrier to be used in the presently disclosed methods and / or aspart of the presently disclosed sustained release formulation is at least 30% (w / w) out of a total weight of the formulation.

[0139] In some examples of the presently disclosed subject matter, the amount of the hydrophobic organic carrier to be used in the presently disclosed methods and / or as part of the presently disclosed sustained release formulation is up to 95% (w / w) out of a total weight of the formulation.

[0140] In some examples of the presently disclosed subject matter, the amount of the hydrophobic organic carrier to be used in the presently disclosed methods and / or as part of the presently disclosed sustained release formulation to be used in the presently disclosed methods and / or as part of is up to 90% (w / w) out of a total weight of the sustained release formulation.

[0141] In some examples of the presently disclosed subject matter, the amount of the hydrophobic organic carrier to be used in the presently disclosed methods and / or as part of the presently disclosed sustained release formulation is up to 85% (w / w) out of a total weight of the sustained release formulation.

[0142] In some examples of the presently disclosed subject matter, the amount of the hydrophobic organic carrier to be used in the presently disclosed methods and / or as part of the presently disclosed sustained release formulation is up to 80% (w / w) out of a total weight of the sustained release formulation.

[0143] In some examples of the presently disclosed subject matter, the amount of the hydrophobic organic carrier to be used in the presently disclosed methods and / or as part of the presently disclosed sustained release formulation is between about 10% (w / w) and about 95% out of a total weight of the formulation.

[0144] In some examples of the presently disclosed subject matter, the amount of the hydrophobic organic carrier to be used in the presently disclosed methods and / or as part of the presently disclosed sustained release formulation is between about 10% (w / w) and about 90% out of a total weight of the formulation.

[0145] In some examples of the presently disclosed subject matter, the amount of the hydrophobic organic carrier to be used in the presently disclosed methods and / or aspart of the presently disclosed sustained release formulation is between about 10% (w / w) and about 80% out of a total weight of the formulation.

[0146] In some examples of the presently disclosed subject matter, the amount of the hydrophobic organic carrier to be used in the presently disclosed methods and / or as part of the presently disclosed sustained release formulation is between about 10% (w / w) and about 70% out of a total weight of the formulation.

[0147] In some examples of the presently disclosed subject matter, the amount of the hydrophobic carrier to be used in the presently disclosed methods and / or as part of the presently disclosed sustained release formulation is between about 10% (w / w) and about 65% out of a total weight of the formulation.

[0148] In some examples of the presently disclosed subject matter, the amount of the hydrophobic organic carrier to be used in the presently disclosed methods and / or as part of the presently disclosed sustained release formulation is between about 10% (w / w) and about 55% out of a total weight of the formulation.

[0149] In some examples of the presently disclosed subject matter, the amount of the hydrophobic organic carrier to be used in the presently disclosed methods and / or as part of the presently disclosed sustained release formulation is between about 10% (w / w) and about 65% out of a total weight of the formulation.

[0150] As noted above, the presently disclosed methods, sustained release formulation and carrier composition comprise at least one quaternary amine.

[0151] When referring to a quaternary amine it is to be understood primarily to refer to compound having the general formula (I):

[0152]

[0153] where

[0154] Ri, R2 and R3 represent, independently, a C1-C3 alkyl chain;

[0155] X represents Ci-Ce alkylene or Ci-Ce alkenylene chain; andY represents an end moiety selected from the group consisting of carboxylic acid, ester, hydroxyl and quaternary ammonium moiety;

[0156] as well as to any salt form of the compound of formula (I).

[0157] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the Ri, R2 and R3 represent the same alkyl chain.

[0158] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition the Ri, R2 and R3 are a methyl.

[0159] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, X represents Ci-Ce alkylene.

[0160] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, X represents C1-C5 alkylene.

[0161] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, X represents C1-C4 alkylene.

[0162] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, X represents C1-C3 alkylene.

[0163] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition X represents C1-C2 alkylene.

[0164] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition Y represents a carboxyl group.

[0165] In some preferred examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the quaternary amine comprises or is glycine betaine (a zwitterionic molecule derived from glycine, with a quaternary ammonium group and a carboxylate group). Glycine betaine has the chemical structure:

[0166]

[0167] ln some preferred examples of the presently disclosed methods, sustained release formulation, and carrier composition, the quaternary amine is a betaine compound.

[0168] In some more specific examples, the quaternary amine is a zwitterionic betaine compound.

[0169] In some examples of the presently disclosed subject matter, the quaternary amine is a zwitterionic quaternary amino acid.

[0170] As used herein, the term "zwitterionic quaternary amino acid” refers to a smallmolecule compound comprising (i) a quaternary ammonium moiety bearing a permanent positive charge and (ii) a carboxylate moiety bearing a negative charge within the same molecular structure, wherein the net charge of the molecule is neutral under ambient conditions.

[0171] In some examples, the zwitterionic quaternary amino acid comprises a C1-C3 alkylene linker between the quaternary ammonium group and the carboxylate group.

[0172] In some examples, the zwitterionic quaternary amino acid is selected from glycine betaine and structural analogues thereof retaining both zwitterionic character and molecular mobility within a hydrophobic matrix.

[0173] In some further preferred examples, the betaine compound is a small-molecule betaine having a molecular weight of less than 1,000 g / mol, at times less than 700 g / mol, at times less than 500 g / mol, at times less than 400 g / mol, at times less than 300 g / mol.

[0174] In some examples, the present disclosure provides a non-aqueous hydrophobic matrix containing a small-molecule quaternary amino acid (preferably betaine-type) that modulates volatility of hydrophobic volatiles via interaction and controlled diffusion.

[0175] In some particularly preferred examples, the betaine compound is selected from the group consisting of glycine betaine (trimethylglycine), alanine betaine, proline betaine, hydroxyproline betaine, carnitine, acetylcarnitine, betaine aldehyde, betaine esters, betaine salts, and fatty acid salts of betaines, including glycine betaine-calcium stearate, and any combination thereof.In some embodiments, the quaternary amine consists essentially of glycine betaine.

[0176] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, Ri, R2 and R3 represent the same alkyl chain; X represents C1-C2 alkylene and Y represents an end moiety selected from the group consisting of carboxyl, methylester and hydroxyl.

[0177] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, Y represents a methylester.

[0178] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, when Y represents a methylester, the quaternary amine is acetylcholine chloride, having the chemical structure:

[0179]

[0180] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, Y represents a hydroxyl.

[0181] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, when Y represents a hydroxyl, the quaternary amine is choline HCI, having the chemical structure:

[0182]

[0183] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, Y represents a quaternary ammonium moiety of formula (II):

[0184]

[0185] where R'i, R'2 and R'3 represent, independently a C1-C3 alkyl chain.

[0186] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, when Y represents a quaternary ammonium moiety of general formula (II), R'i, R'2 and R'3 are identical, respectively, to Ri, R2 and R3, and preferably, are also identical to each other, i.e. represent the same alkyl group.

[0187] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, when Y represents a quaternary ammonium moiety of general formula (II), the quaternary amine is a hexamethonium salt, with the chemical structure:

[0188] " " "

[0189]

[0190] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the quaternary amine is a zwitterionic form of the compound of general formula (I).

[0191] The quaternary amine to be used in accordance with the presently disclosed subject matter can be in free form or complexed, e.g. in a form of a salt, with another chemical entity. As such, unless stated to be in a particular form, the term quaternary amine covers both the free form, complexed or salt form of the structure of general formula (I).

[0192] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the quaternary amine is a small molecular weight compound.

[0193] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the quaternary amine is a small molecularweight having a molecular weight below 500g / mole, at times, below 400g / mole; or even below 300g / mole.

[0194] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the, the quaternary amine has a molecular weight of up to 300g / mole.

[0195] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the quaternary amine comprises a betaine and has a molecular weight below 300g / mole.

[0196] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the quaternary amine is complexed with a hydrocarbon containing molecules.

[0197] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the, the quaternary amine is complexed with a fatty acid.

[0198] In some preferred examples of the presently disclosed methods, sustained release formulation and carrier composition, the quaternary amine comprises a betaine compound.

[0199] In the context of the presently disclosed methods, sustained release formulation and carrier composition, the term "betaine" is to be understood to refer to any zwitterionic compound characterized by the presence of a quaternary ammonium cation and a carboxylate anion being linked by an alkylene (e.g. methylene) group, within the same molecular structure.

[0200] It is to be understood that in the context of the presently disclosed methods, sustained release formulation and carrier composition, and unless specifically stated otherwise, term betaine denotes both simple betaines such as trimethylglycine (glycine betaine) as well as more complexed betaine, such as structural variants and analogs encompassing a quaternary amino acid structure. This may include, for example, fatty acid salts of betaines, such as glycine betaine fatty acid salt, or specifically glycine betaine Ca stearate.A non-limiting list of quaternary amino acid having a betaine structure includes glycine betaine, alanine-betaine, proline betaine, arginine betaine, homocysteine betaine, cysteine betaine, glutamine betaine, lysine betaine, aspartic acid betaine, serine betaine, carnitine, glycine betaine aldehyde, betaine ester, betaine hydrochloride, sulfobetaine, acetylcarnitine, hydroxyproline betaine, choline betaine, beta-Alanine betaine, GABA betaine, aspartate betaine, ornithine betaine and any combination of same.

[0201] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the quaternary amine comprises or is glycine betaine.

[0202] The amount of quaternary amine within the sustained release formulations may vary, and the desired amount will dictate the amount used in the presently disclosed methods, as well as in the presently disclosed carrier composition.

[0203] Without being bound thereto, it is assumed that the quaternary amine is complexed or forms a co-crystal with the volatile organic substance once mixed therewith. As such, the amount of quaternary amine may also dictate that amount of volatile organic substance that can be held by the presently disclosed carrier composition. In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the weight ratio between the quaternary amine and the volatile organic substance is at least 1:1, at times, between 1:1 and 1:3, preferably about 1:2.

[0204] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the weight amount of the quaternary amine to be used in the disclosed methods or to be introduced into the sustained release formulations and / or carrier composition, is between about 5% and about 40% out of a total weight of the eventual sustained release formulation.

[0205] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the weight amount of the quaternary amine to be used in the disclosed methods or to be introduced into the sustained releaseformulations and / or carrier composition, is between about 5% and about 35% out of a total weight of the eventual sustained release formulation; at times, between about 5% and about 30% out of a total weight of the eventual sustained release formulation between about 5% and about 25% out of a total weight of the eventual sustained release formulation; between about 5% and about 20% out of a total weight of the eventual sustained release formulation.

[0206] As noted above, the presently disclosed sustained release formulation also comprises one or more volatile organic substances. Such volatile organic substances are organic compounds that under ambient conditions (e.g. temperature, humidity), exhibit a vapor pressure sufficient to result in evaporation or sublimation into the surrounding atmosphere. These substances are carbon-containing compounds characterized by a tendency to partition into the vapor phase at or near room temperature, for example, due to a relatively low boiling point or elevated vapor pressure under standard conditions.

[0207] In the context of the presently disclosed methods, formulations and / or carrier composition, the volatile organic substances are preferably environmentally friendly and / or agriculturally acceptable volatile organic substances, as would be known to those versed in the art at the time of performing the presently disclosed subject matter.

[0208] The volatile organic substances are preferably water-immiscible. As used herein, the term "water-immiscible" refers to volatile organic substances having a solubility in water of less than about 1 g / L at 25 °C; in some examples less than about 0.9 g / L, less than about 0.5 g / L, or less than about 0.1 g / L at 25 °C, and which do not form a single homogeneous phase with water under ambient conditions.

[0209] Further, in the context of the presently disclosed methods, formulations and / or carrier composition, the volatile organic substances include any organic compound that is capable of being incorporated into, by dissolution or dispersion, without observable phase separation under ambient conditions for at least 10 hours, or even after 24 hours, or even after 48 hours, or even after a week.In some examples of the presently disclosed methods, formulations and / or carrier composition, the volatile organic substance is selected from hydrophobic volatile compounds having (i) a boiling point below 300°C at atmospheric pressure and / or (ii) a vapor pressure of at least 0.001 mmHg at 25°C.

[0210] In some embodiments, the volatile organic substance consists essentially of an essential oil or a component thereof having a molecular weight below 350 g / mol.

[0211] In some examples of the presently disclosed subject matter, the one or more volatile organic substances include volatile compounds selected based on their chemical classification, including terpenes, terpenoids, volatile lipids, volatile fatty acids, volatile esters, volatile alcohols, volatile ketones, and volatile aldehydes and any functional derivative and / or combination thereof.

[0212] In some additional or alternative examples of the presently disclosed subject matter, the one or more volatile compounds are selected based on their biological or functional activity, including essential oils, allelochemicals, pheromones, allomones, and kairomones, as well as any volatile derivatives and / or combinations thereof. For simplicity, in the present disclosure the one or more volatile organic substances are collectively referred to as volatile organic substances, irrespective of their chemical classification or functional categorization, and include terpenes, terpenoids, essential oils, allelochemicals, pheromones, volatile lipids, volatile fatty acids, volatile esters, volatile alcohols, volatile ketones, volatile aldehydes, and any volatile derivatives and / or combinations thereof.

[0213] In some examples of the presently disclosed methods, formulations and / or carrier composition, the volatile organic substance comprises a monoterpene, sesquiterpene, monoterpenoid, or phenylpropanoid compound.

[0214] In some embodiments, the volatile organic substance comprises a compound selected from thymol, carvacrol, menthol, eugenol, methyl eugenol, linalool, citronellal, limonene, geraniol, verbenone, farnesene, and any combination thereof.- 1 - In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the volatile organic substance comprises at least one essential oil.

[0215] The term "essential oils” is intended to encompass mixtures that generally comprise terpenes and terpenoids, and therefore the listing of terpenes and terpenoids separately is not intended to be limiting. Similarly, while volatile fatty acids, volatile esters, volatile alcohols, volatile ketones, and volatile aldehydes may be derivable from or be components of volatile lipids, each is listed separately to facilitate the identification of compounds having distinct functional properties.

[0216] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the volatile organic substance comprises at least one terpene, terpenoid, essential oil and / or pheromone.

[0217] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the volatile organic substance comprises at least one terpene.

[0218] A non-limiting list of terpenes forming part of the volatile organic substances, in accordance with the presently disclosed methods, sustained release formulation and / or carrier composition, includes farnesene, caryophyllene, humulene, germacrene D, beta-elemene, squalene, lanosterol, beta-carotene, lycopene, neurosporene, a-Pinene, a-Terpinene, P-Caryophyllene, P-Myrcene, P-Pinene, camphene, delta-Selinene, y-Terpinene, limonene, p-Cymene, terpinene, terpinolene, and trans-Carane. The disclosed methods, sustained release formulation and / or carrier composition can use one or a combination of the above listed terpenes.

[0219] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the volatile organic substance comprises at least one terpenoid.

[0220] A non-limiting list of terpenoids forming part of the volatile organic substances, in accordance with the presently disclosed methods, sustained release formulation and / or carrier composition, includes thymol, menthol, camphor, geraniol, linalool,carvone, citronellol, eucalyptol (1,8-cineole), menthone, sabinene hydrate, farnesol, bisabolol, caryophyllene oxide, nerolidol, patchuol, artemisinin, costunolide, taxol, retinol, gibberellin, phytol, forskolin, geranylgeraniol, pimaric acid, steviol, abietic acid, isopimaric acid, ginsenosides, ursolic acid, betulinic acid, lupeol, saponins, Asiatic acid, corosolic acid, zeaxanthin, astaxanthin, violaxanthin, cryptoxanthin, canthaxanthin, fucoxanthin, chlorophyll, vitamin K1;vitamin E, tanshinone, dihydroartemisinin, and valerenic acid, borneol, bornyl acetate, carvacrol, citronellal, citronellil formate, citral, gedunin, geranial, geranyl acetate, isomenthol, margolone, margolonone, neral, nimbidin, nimbin, nimbolide, pulegone, salannin, somargolonone, terpinen-4-ol, terpineol, tetrahydrocannabinol (THC), cannabidiol (CBD), cannabinol (CBN), and verbenone.

[0221] The presently disclosed methods, sustained release formulation and / or carrier composition can use one or a combination of the above listed terpenoids.

[0222] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the at least one volatile organic substance comprises or consists of thymol.

[0223] In the context of the presently disclosed methods, sustained release formulation and / or carrier composition, the term "essential oil" should also or alternatively be understood in accordance with its commonly accepted meaning, namely a volatile, aromatic composition obtained from plant materials, for example by steam distillation or other suitable extraction methods, and typically comprising terpenes, terpenoids, and related volatile organic constituents.

[0224] Thus, when considering plant material as a source of the essential oil, a non-limiting list of essential oils, in accordance with the presently disclosed methods, sustained release formulation and / or carrier composition, includes mint oil, clove oil, tea tree oil, lavender oil, peppermint oil, eucalyptus oil, lemon oil, orange oil, bergamot oil, grapefruit oil, rose oil, geranium oil, jasmine oil, ylang-ylang oil, cedarwood oil, sandalwood oil, patchouli oil, vetiver oil, frankincense oil, myrrh oil, cinnamon oil, ginger oil, black pepper oil, cardamom oil, nutmeg oil, basil oil, rosemary oil, thyme oil, sage oil, spearmint oil, Wintergreen oil, lemongrass oil, chamomile oil, neroli oil, lime oil,mandarin oil, clary sage oil, marjoram oil, cypress oil, helichrysum oil, palo santo oil, garlic oil, agar oil, agarwood (oud) oil, allspice oil, aloeswood oil, ajwain oil, ambrette seed absolute oil, amyris oil, angelica root oil, anise oil, mugwort oil, anthopogon oil, asafoetida oil, attar oil, balsam fir oil, balsam of Peru oil, bay leaf oil, birch oil, blue tansy oil, bois de rose oil, budda wood oil, buchu oil, cade oil, cajeput oil, calamansi oil, calamus oil, camphor oil, cananga oil, cannabis oil (steam-distilled), caraway seed oil, cassia oil, catnip oil, cilantro oil, champaca oil, cistus oil, citron oil, citronella oil, coriander oil, cornmint oil, costmary oil, costus oil, cubeb oil, cumin seed oil, curry leaf oil, cypriol oil, davana oil, dill oil, Douglas-fir oil, elecampane oil, elemi oil, ericifolia oil, fennel oil, fir oil, fragonia oil, galangal oil, galbanum oil, goldenrod oil, grapefruit oil, hemlock spruce oil, hinoki oil, hops oil, horseradish oil, hyssop oil, ishpingo oil, immortelle oil, jatamansi oil, java pepper oil, juniper berry oil, kaffir lime oil, kanuka oil, kunzea oil, labdanum oil, laurel leaf oil, lavandin oil, ledum oil, litsea cubeba oil, magnolia oil, may chang oil, manuka oil, melissa oil, mountain savory oil, muhuhu oil, myrtle oil, nard oil, niaouli oil, ocotea oil, olibanum oil, opoponax oil, oud oil, oregano oil, orris oil, palmarosa oil, parsley oil, pennyroyal oil, petitgrain oil, pimento oil, pine oil, plai oil, ravensara oil, ravintsara oil, red cedar oil, rock rose oil, Roman chamomile oil, rosalina oil, rosewood oil, saro oil, sassafras oil, savory oil, schisandra oil, spikenard oil, spruce oil, star anise oil, tagetes oil, tarragon oil, tsuga oil, tulsi oil, turmeric oil, valerian oil, verbena oil, western red cedar oil, xanthoxylum oil, yarrow oil, yuzu oil, sweet orange oil, tangerine oil and any combination of same.

[0225] In some more specific examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the at least one essential oil is selected from the group consisting of mint oil, clove oil, tea tree oil, lavender oil, peppermint oil, eucalyptus oil, lemon oil, orange oil, bergamot oil, grapefruit oil, rose oil, geranium oil, jasmine oil, ylang-ylang oil, cedarwood oil, sandalwood oil, patchouli oil, vetiver oil, frankincense oil, myrrh oil, cinnamon oil, ginger oil, black pepper oil, cardamom oil, nutmeg oil, basil oil, rosemary oil, thyme oil, sage oil, spearmint oil, Wintergreen oil, lemongrass oil, chamomile oil, neroli oil, lime oil, mandarin oil, clary sage oil, marjoramoil, cypress oil, helichrysum oil, palo santo oil, sweet orange oil, tangerine oil and any combination of same.

[0226] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the at least one essential oil comprises or consists of at least one of mint oil, clove oil and tea tree oil.

[0227] For example, mint oil can be used to effectively repel mice, rats and / or bats, as known in the art.

[0228] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the volatile organic substance comprises at least one pheromone.

[0229] In the context of the presently disclosed methods, sustained release formulation and / or carrier composition, the term "pheromone" means a chemical substance produced and secreted by an organism that elicits a specific behavioral or physiological response in another member of the same species. The pheromone may be naturally produced or synthetically derived and may function as a sex attractant, aggregation agent, alarm signal, trail marker, queen regulator, brood modulator, oviposition deterrent, host marker, defensive signal, or as a semiochemical of other types. In one non-limiting aspect, the volatile pheromones of the present disclosure include, without limitation, the following:

[0230] Sex Pheromones, such as (Z)-7-dodecen-l-yl acetate, (E)-ll-tetradecen-1-yl acetate, (Z)-ll-tetradecen-l-yl acetate, (Z)-9-tetradecen-l-yl acetate, (E)-10-dodecen-l-ol, (Z)-lO-dodecenal, (Z)-9-hexadecenal, (Z)-ll-hexadecenal, (E,E)-8,10-dodecadien-l-ol, (Z,E)-9,ll-tetradecadien-l-ol acetate, (E,Z)-3,13-octadecadien-l-yl acetate, (E,E)-10,12-hexadecadienal, (E)-6-hexadecenal, bombykol, bombykal, (Z,Z)-11,13-pentadecadienal, (Z)-6-cis-octadecen-l-yl acetate, methyl (E)-2-dodecenoate, and 2,6-dimethyl-4-heptanol;

[0231] Aggregation Pheromones such as frontalin, ipsdienol, ipsenol, verbenone, exo-brevicomin, sulcatone (6-methyl-5-hepten-2-one), (S)-2-methylbutan-l-ol, (R)-(+)-limonene, 4-methyl-5-nonanol, 3-methyl-2-butanol, 2-methyl-3-buten-2-ol,methyl-4-hexenoate, (E)-2-hexen-l-ol, 1-methylcyclohexanol, (E)-2-methyl-6-methyleneoct-7-en-2-ol, 3-hydroxy-2-butanone, and (Z)-8-heptadecen-2-one;

[0232] Alarm Pheromones such as isopentyl acetate, (E)-p-farnesene, 2-heptanone, citral (a mixture of geranial and neral), geraniol, l-octen-3-ol, hexanal, nonanal, formic acid, undecane, pentadecane, (Z)-3-hexenal, octadecanal, (E)-2-decenal, methyl palmitate, dodecanal, tridecane, and tetradecane;

[0233] Trail Pheromones such as farnesol, (Z)-9-hexadecenal, methyl anthranilate, (E)-2-butyl-2-octenal, undecanoic acid, (Z)-ll-eicosen-l-ol, methyl salicylate, sulcatol (6-methyl-5-hepten-2-ol), (E,E)-2,4-decadienal, geranyl acetate, n-tridecane, decanoic acid, (Z)-9-tricosene, methyl heptanoate, (E)-3-dodecen-l-ol, and hexanoic acid;

[0234] Queen Pheromones such as 9-hydroxy-2-decenoic acid (9-HDA), 10-hydroxy-2-decenoic acid, homovanillyl alcohol, 2-methyl-3-buten-2-ol, geranylgeranyl acetate, methyl dodecanoate, tetradecanal, 3-hydroxybutyric acid, 4-hydroxyphenylacetic acid, and heptadecane;

[0235] Brood Pheromones such as methyl palmitate, methyl linoleate, ethyl oleate, methyl linolenate, methyl stearate, methyl myristate, (E)-p-ocimene, a-pinene, geranyl formate, and decyl acetate;

[0236] Oviposition Deterrent Pheromones such as p-cresol, 2,6-dichlorophenol, methyl eugenol, limonene, carvone, l-octen-3-ol, (Z)-3-hexen-l-ol acetate, eugenol, anethole, and citronellal;

[0237] Host-Marking Pheromones such as (E)-p-caryophyllene, cis-verbenol, geranyl acetate, (E)-2-butenyl acetate, linalool oxide, p-anisyl alcohol, y-terpinene, terpinen-4-ol, a-terpineol, and methyl chavicol;

[0238] Defensive Pheromones such as formic acid, hexanoic acid, butyric acid, caproic acid, undecane, (E)-2-decenal, skatole, dodecane, octanoic acid, and benzyl isothiocyanate;In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the volatile organic substance comprises at least one volatile allelochemical.

[0239] As used herein, the term "allelochemical" refers to a biologically active chemical compound produced by a plant, microorganism, or other organism that mediates an interaction with an organism of a different species.

[0240] In the context of the presently disclosed subject matter, the term "volatile allelochemical" refers to an allelochemical that is capable of vaporization under ambient or application conditions and that exerts its biological effect, at least in part, via the gas phase. Volatile allelochemicals may be released from an emitting organism or composition into the surrounding environment and may influence the growth, behavior, physiology, or survival of a receiving organism.

[0241] Without being limited thereto, the volatile allelochemicals may include:- Kairomones (Semi-chemicals for Host Attraction) such as (E)-2-hexenal, (Z)-3-hexen-l-ol, phenylacetaldehyde, benzyl alcohol, eugenol, methyl eugenol, eugenol acetate, methyl jasmonate, indole, l-octen-3-ol, ethyl isovalerate, isoamyl acetate, and hexyl acetate;

[0242] Allomones such as camphor, citronellal, menthol, cineole, thymol, a-terpineol, piperitone, -ionone, D-limonene; and

[0243] Synomones such as (Z)-ll-hexadecenyl acetate, methyl jasmonate, salicylic acid, (E,E)-a-farnesene, cis-jasmone, linalool, benzyl benzoate, germacrene-D, P-caryophyllene, and heptadecanone.

[0244] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the at least one volatile organic compound comprises or is a pheromone selected from the group consisting of farnesene, indole, bombykal, bombykol and verbenone, citral, dodecanal, farnesol, formic acid, frontaline, geraniol, geranyl acetate, hexanoic acid, ipsenol, ipsdienol, isopentyl acetate, limonene, methyl anthranilate, methyl eugenol, methyl jasmonate, methyl palmitate, sulcatone, (E)-2-Hexenal, (E)-2-Decenal, (E)-ll-Tetradecen-l-yl acetate, (E)- -Caryophyllene, (E)- -Farnesene, (E,E)-8,10-Dodecadien-l-ol, (E,E)-a-Farnesene, (E)-6-Hexadecenal, (E)-8-Heptadecen-2-one, (E,Z)-3,13-Octadecadien-l-yl acetate, (Z)-lO-Dodecenal, (Z)-ll-Tetradecen-l-yl acetate, (Z)-3-Hexenal, (Z)-3-Hexen-l-ol acetate, (Z)-6-Cis-octadecen-l-yl acetate, (Z)-7-Dodecen-l-yl acetate, (Z)-9-Tetradecen-l-yl acetate, (Z,E)-9,11-Tetradecadien-l-ol acetate, (Z,Z)-ll,13-Pentadecadienal, l-Octen-3-ol, 2,6-Dimethyl-4-heptanol, 3-Hydroxy-2-butanone, 9-Hydroxy-2-decenoic acid (9-HDA).

[0245] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the at least one volatile organic substance comprises or consists of methyl eugenol.

[0246] The type and amount of volatile organic substances may vary, depending on the target organism, the type and / or weight amount of quaternary amine in the carrier composition, the hydrophobic carrier material, and other considerations. Yet, for slow release of the volatiles, for a period of time that exceeds at least 7 days, preferably 10 days, in an open environment, the amount of volatile organic substances, , is within a range of between about 5wt% and about 40wt% out of a total weight of said sustained release formulation, at times, in a range between about 10wt% and about 40wt%; at times, in a range between about 15wt% and about 40wt%; at times, in a range between about 20wt% and about 40wt%; at times, in a range between about 25wt% and about 30wt%; at times, in a range between about 35wt% and about 40wt%.

[0247] In some examples of the presently disclosed subject matter, the presently disclosed sustained release formulation also comprises a tackifying agent. Or when such tackifying agent is included, it can be added to the carrier composition, during its preparation or after its preparation, or to the mixing of the carrier composition with the volatile organic substance, or to the prepared final blend of the carrier composition with the volatile organic substance.

[0248] In some preferred examples, the tackifying agent is part of the carrier composition.

[0249] In the context of the presently disclosed methods, sustained release formulation and / or carrier composition, the term "tackifying agent” refers to a substance typicallyincorporated into a formulation to impart adhesive or sticky properties, thereby enhancing the formulation's structural integrity. The tackifying agent may be natural, synthetic, or chemically modified form of a naturally occurring substance.

[0250] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the tackifying agent is an agent selected from the group consisting of resins, rosin derivatives, polyterpenes, and hydrocarbon-based compounds.

[0251] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the tackifying agent comprises resins and / or rosins.

[0252] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the tackifying agent comprises or is a resin selected from the group consisting of dammar resin, gum resin, hydrocarbon resin, mastic resin, phenolic resin and any combination thereof.

[0253] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the tackifying agent comprises a rosin selected from rosin esters.

[0254] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the rosin ester is selected from the group consisting of triethylene glycol ester of gum rosin, glycerol ester of gum rosin, wood rosin, tall oil rosin, ester rosin, glycerol ester rosin, pentaerythritol ester rosin, modified rosin, hydrogenated rosin, polymerized rosin, maleic rosin and any combination thereof.

[0255] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the rosin ester comprises triethylene glycol ester of gum rosin and / or glycerol ester of gum rosin.

[0256] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the tackifying agent comprises a rosin selected from the group consisting of wood rosin, tall oil rosin, modified rosin, hydrogenated rosin, polymerized rosin, maleic rosin and any combination thereof.In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the tackifying agent, if present, is used in an amount that would constitute up to about 40wt%, out of the total weight of the final sustained release formulation. For the purposes of the present disclosure, a tackifying agent amount of 0% (i.e., null percent) shall be understood to mean that the formulation is devoid of a detectable amount of tackifying agent.

[0257] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the carrier composition and / or the sustained release formulation also comprise a thickening agent. The thickening agent can form part of the carrier composition, before combining with the organic volatile substances, or it can be added during or after the combining of the organic volatile substances with the carrier composition. In the context of the presently disclosed methods, sustained release formulation and / or carrier composition, the term "thickening agent" is to be understood to denote a substance that, when present in the sustained release formulation, increases viscosity, structural integrity, mechanical stability, resistance to flow and / or consistency thereby modifying the rheological properties of the formulation relative to the same formulation in the absence of the thickening agent.

[0258] The thickening agent may function by physical entanglement, network formation, particle interaction, or other mechanisms.

[0259] The thickening agent may be natural, synthetic, semi-synthetic or chemically modified materials.

[0260] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, that thickening agent is a naturally occurring material.

[0261] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the thickening agent is or comprises mineralbased (mineral-derived) thickening agents.

[0262] Mineral based thickening agents to be used in the context of the presently disclosed methods, sustained release formulation and / or carrier composition can be anymineral selected from the group consisting of silica-containing minerals, such as fumed silica, Quartz (crystalline silica), amorphous silica; aluminosilicate minerals, such as zeolite and magnesium aluminum silicate; clay (phyllosilicates), such as Kaolinite (Kaolin), Bentonite (Montmorillonite-rich), Attapulgite (Palygorskite), Sepiolite, Halloysite.

[0263] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the thickening agent is or comprises fumed silica.

[0264] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the thickening agent is or comprises inorganic salts. A non-limiting list of inorganic salts that can be used as a thickening agent includes carbonates, such as Calcium Carbonate and Dolomite; sulfates such as Gypsum (calcium sulfate); metallic soaps, such as aluminum stearate.

[0265] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the thickening agent is or comprises organic and polymeric thickening agents, some of which are also classified as Superabsorbent Polymers (SAPs).

[0266] A non-limiting list of organic and polymeric thickening agents includes polysaccharides, such as starch, agar and alginate, cellulose, plant-derived gum (e.g. xanthan gum); proteins such as gelatin and casein; and synthetic polymers, such as carbomers and polyacrylates.

[0267] The amount of thickening may depend on the desired viscosity of the eventual sustained release formulation. In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the thickening agent is present in an amount of up to 5wt% of a total weight of the formulation; at times, up to 4wt%; at times, up to 3wt%.

[0268] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the thickening agent is present in an amount ofbetween about 0.001wt% and about 5wt% of the total weight of said sustained release formulation.

[0269] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the thickening agent is present in an amount between about 0.05wt% and about 4wt% of the total weight of the sustained release formulation; at times, between about 0.1wt% and about 3wt%.

[0270] The presently disclosed formulation can also comprise, at times, a filler material (or in brief, filler), essentially homogeneously blended (i.e. essentially uniformly blended) with the blend comprising at least hydrophobic organic carrier, the volatile organic compound and the quaternary amine mixture. The filler can be added to the carrier composition before mixing with the volatile organic substances, or during or after the mixing with the volatile organic substance.

[0271] In the context of the presently disclosed methods, sustained release formulation and / or carrier composition, the term filler should be understood to refer to substances that can function as an absorbent and / or increase volume, and / or provide the formulation with bulkiness and / or improve mechanical properties, and / or enhance structural integrity and / or improve chemical or physical stability, and / or adjust viscosity.

[0272] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the filler can be natural, synthetic, or chemically modified materials.

[0273] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the filler is in particulate form.

[0274] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the filler comprises any particulate substance selected from organic based fillers, bone derived fillers, mineral-based fillers, clay fillers, aluminosilicates, polymeric particles and any combination of same.

[0275] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the filler particles comprise organic basedfillers, such as polysaccharide derived from plant or animal source. These include, without being limited thereto, lignocellulose, cellulose, hemicellulose, lignin.

[0276] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the filler particles comprise bone derived fillers.

[0277] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the filler particles comprise mineral-based fillers, such as silica (e.g. fumed silica), zeolite, Talcum, Calcium Carbonate and Aluminum Stearate.

[0278] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the filler particles comprise clay fillers, such as bentonite and kaolin.

[0279] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the filler particles comprise aluminosilicates, such as natural aluminosilicates, e.g. Magnesium Aluminum Silicate.

[0280] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the filler particles comprise polymeric particles, e.g. super absorbent polymers.

[0281] In the context of the presently disclosed subject matter, the term super absorbent polymers (SAPs) refer to polymers that selectively absorb and retain significant quantities of oil-based liquids while exhibiting minimal absorption of water. The term super absorbent polymer as used herein encompasses any polymer system, regardless of its specific chemical composition or structural configuration, that meets the criteria of high oil absorption capacity and controlled release performance in oildominant environments.

[0282] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the filler comprises a plant-derived polysaccharide, modified polysaccharide-based SAPs, superabsorbent polyacrylates, oleophilic crosslinked polymers, nanoporous and hybrid SAPs.In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the filler comprises or is a lignocellulose.

[0283] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the filler comprises or is wood-derived filler, such as wood saw and / or wood dust.

[0284] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the filler particles have a size (longest dimension) ranging from 1 nm and 1 mm, at times, between about 10 nm and about 1 mm, as can be determined by conventional analytical methods, e.g. microscope.

[0285] In some examples of the presently disclosed subject matter, the filler particles have a longest dimension of between about 10 nm and about 500 pm; at times between about 1pm and about 200 pm; with at least 90% of the particles being below 500 pm, as determined by laser diffraction.

[0286] The amount of the filler particles may vary depending on the desired effect on the final formulation, and can be determined by those skilled in the art. In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the amount of the filler is at least 5wt%.

[0287] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the amount of the filler is at least 10wt%, at times, between 5 wt% and 40 wt%; at times, between 5 wt% and 20 wt%; at times, between 10 wt% and 30 wt%; at times, between 15 wt% and 25 wt%; and at times, between 20 wt% and 40 wt%, based on the total weight of the formulation or carrier composition.

[0288] In some examples of the presently disclosed methods, the volatile organic substances is first absorbed onto the filler, and only then the filler holding the volatile organic substance is mixed into the carrier composition.

[0289] Certain substances described in the present disclosure may serve both as a thickening agent and as a filler, depending on their concentration / amount and function within the presently disclosed formulation. When a substance can serve both roles, itscontribution as a thickening agent is determined within the 5% limit. In other words, a substance that falls under the definition of filler and thickening agent, and is present in an amount of 5wt% or less of the final formulation, is considered in the context of the present disclosure a thickening agent, and vice versa, a substance present in an amount above 5wt% of the final formulation would be considered a filler.

[0290] The presently disclosed formulation may include other components such as formulation additives including, without being limited thereto anti-oxidants, UV absorbents and / or vitamins, etc., as acceptable in the art in which the formulation is intended to be used. These can be added to the carrier composition and / or to the final sustained release formulation.

[0291] It is an essential feature of the presently disclosed methods, sustained release formulation and / or carrier composition, that the components of the sustained release formulation, namely, the hydrophobic organic carrier material, the quaternary amine and the volatile organic substance, and if present, the tackifying agent, the thickening agent, and / or the filler are formed into a homogenous blend. In other words, it is to be understood that at least the hydrophobic organic carrier material, the quaternary amine and the volatile organic substance are not in core-shell formation, where the core or the shell is other than the disclosed formulation, or a two or more phase formation. It should however be noted that the formulation can be in a multilayer formulation, all layers comprising the presently disclosed sustained release formulation, however, optionally with different compositions of the possible components.

[0292] In some examples, the sustained release formulation is a single-phase continuous hydrophobic matrix in which the quaternary amine and the volatile organic substance are molecularly dispersed or finely distributed.

[0293] In some examples, the formulation is not in the form of microcapsules, core-shell particles, inclusion complexes, emulsions, liposomes, zeolite-loaded particles, or encapsulated droplets.

[0294] In some embodiments, the sustained release formulation consists essentially of a homogeneous non-encapsulated matrix.In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the carrier composition is in a form of a paste.

[0295] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the carrier composition is in a form of nonaqueous gel form.

[0296] In some examples of the presently disclosed methods, sustained release formulation and / or carrier composition, the carrier composition is in liquid form.

[0297] It has been unexpectedly found that the presently disclosed formulation, including the quaternary amine within the hydrophobic organic carrier, exhibits an evaporation rate of the volatile organic substance that is between about 5 and about 100 times slower compared to the evaporation rate of the same volatile organic substance when in its free, unformulated form.

[0298] Even more surprisingly, it has been unexpectedly found that the presently disclosed formulation, including the quaternary amine within the hydrophobic organic carrier, exhibits an evaporation rate of the volatile organic substance that is between about 2 and about 50 times, or even between 3 and about 50 times, or even between 5 and 50 times, slower compared to the evaporation rate of the same volatile organic substance when combined only with the quaternary amine.

[0299] Further, it has been unexpectedly found that the presently disclosed formulation, including glycine betaine as the quaternary amine, formulated with an essential oil as the organic volatile substance, both within hydrophobic organic carrier, exhibited an evaporation rate of the formulated essential oil that is between about 5 and about 10 times slower compared to the evaporation rate of the same essential oil when in its free, unformulated form or in the absence of the hydrophobic organic carrier and / or in the presence of non-hydrophobic carrier.

[0300] Further, specifically, it has been unexpectedly found that the presently disclosed formulation, including glycine betaine as the quaternary amine, formulated with a terpenoid as the organic volatile substance, both within the hydrophobic organic carrier, exhibited an evaporation rate of the formulated terpenoid that is between about 10 andabout 100 times slower compared to the evaporation rate of the same terpenoid when in its free, unformulated form.

[0301] In some examples of the presently disclosed subject matter, the presently disclosed formulation comprises the components ranges as specified in Table 1:

[0302] Table 1 - Formulation component ranges

[0303]

[0304] In some examples of the presently disclosed subject matter, the presently disclosed formulation comprises combinations of components as described in Table 2:

[0305] Table 2 -Sustained-Release Formulations

[0306]

[0307]

[0308] Turning now to the presently disclosed methods for producing the sustained release formulation, it is to be appreciated that the mixing of the components, irrespective of the order of their mixing, is under conditions that involve no externally added (i.e. no intentionally added) water. As such, the conditions are such that no emulsion is formed, and specifically, no oil in water emulsion is or can be formed.

[0309] The presently disclosed methods thus provide essentially water free formulation, as defined hereinabove. Yet, in the context of the presently disclosed methods, according to the presently disclosed first aspect, it is to be understood that while there is no intentional addition of water or exposure to external humidity, some amount of water can be present, e.g. due to unintentional absorption, water inherently present in one or more of the components etc. notwithstanding the reasons of having water, it is to be understood that the water content, if present, is not more than 5%, as detailed hereinabove with respect to the term "essentially water free” in the context of the presently disclosed subject matter .

[0310] In some examples of the presently disclosed methods, the mixing provides an essentially homogenous mixture.

[0311] In some examples of the presently disclosed second aspect, the method comprises a priori mixing of the quaternary amine and the organic volatile substance with a filler, to form an intermediate mixture (which could be referred to as the "functional" or "active" intermediate mixture) and mixing the intermediate mixture into the hydrophobic organic carrier composition to form the final formulation.

[0312] In some examples of the presently disclosed methods, the a priori mixing of the quaternary amine and the organic volatile substance with the filler is such that the volatile organic substance is absorbed onto the filler prior to mixing with the quaternary amine.

[0313] The mixing conditions in the absence of the volatile organic substance may include, for example, elevated temperatures, so as to facilitate the homogenousblending of the components of the mixture. A person versed in the art would appreciate which temperatures to use in order to facilitate homogeneity of the carrier mixture, and to which temperature to bring the carrier composition before introducing the organic volatile substance, and which would still allow effective and efficient mixing of the intermediate mixture into the carrier mixture.

[0314] In some examples of the presently disclosed methods, introducing the organic volatile substance into the carrier composition is only after all other components are mixed together to thereby form a "base" carrier composition. The base carrier composition can be considered as the inert formulation, as it has no functionality other than to carry the volatile organic solvent, once the latter is added. In the context of the presently disclosed subject matter, when referring to a base carrier composition it is to be understood to refer to the formulation comprising at least the hydrophobic carrier and the quaternary amine, and at times, preferably also the thickening agent and / or filler and / or tackifying agent but not the organic volatile substance.

[0315] In some examples of the presently disclosed methods, the term "carrier composition" comprises all components of the sustained release formulation albeit the organic volatile substance and at times, without the filler. Such carrier composition would allow the introduction of desired organic volatile substance(s) at a later stage, e.g. before actual use.

[0316] As noted above, the formation of the carrier composition is typically under conditions that allow the essentially homogenous mixing of the components. The conditions may include, for example, elevated temperatures. Such elevated temperatures may be between about 50°C-180°C, preferably between about 60°-140°C and the introduction of the organic volatile substance would be at a temperature below its boiling temperature or flash point. In the context of the presently disclosed methods, when referring to homogenous mixing or mixture it is to be understood to refer to a mixture or blend where all components are essentially uniformly distributed throughout, as can be evident by conventional analytical methods.

[0317] In cases where a carrier composition is a priori formed (i.e. without the volatile organic substance), the carrier composition can be packed and stored until needed.Further, when a carrier composition is a priori formed, it is to be appreciated that the later mixing of the organic volatile substance into the carrier composition would be under conditions that avoid undesired evaporation of the volatile organic substance, e.g. the temperature is lower than the boiling temperature of volatile substance or below the flash point of the volatile substance.

[0318] In some examples of the presently disclosed methods the carrier composition is a priori prepared, and is later mixed with an organic volatile substance. The carrier composition, a priori prepared, comprises, a priori mixed combination of at least the hydrophobic organic carrier and the quaternary amine.

[0319] In some examples of the presently disclosed methods, the a priori prepared carrier composition comprises also the tackifying agent and / or the filler and / or the thickening agent, prior to mixing with the volatiles.

[0320] In some examples of the presently disclosed methods, the a priori prepared carrier composition comprises, in addition to the hydrophobic organic carrier and quaternary amine, the tackifying agent and the thickening agent.

[0321] Irrespective of the order of mixing of the components, the resulting mixture (be it the sustained release formulation and / or the carrier composition) are preferably an essentially homogenous (i.e. uniform) mixture of the components.

[0322] The presently disclosed methods enable the production of sustained release formulations in various physical forms, such as gels, solids, liquids, and pastes. Typically, the physical form is determined by the type and amount of components excluding the organic volatile substance— and those skilled in the art would readily recognize the amounts of each component required to achieve the desired form.

[0323] It is to be appreciated that any sustained release formulation obtained or obtainable by the presently disclosed methods, also form part of the present disclosure.

[0324] The presently disclosed subject matter also relates, in accordance with yet another aspect, to a method of controlling a target organism, the method comprises exposing a target organism or a habitat of a target organism to a sustained releaseformulation comprising (i) a hydrophobic organic carrier, (ii) a quaternary amine of general formula (I) as defined herein; and (iii) a volatile organic substance.

[0325] Unless the context clearly indicates otherwise, it is to be understood that all terms, definitions, characteristics, embodiments, and descriptions provided herein with respect to the described methods, carrier compositions, and sustained release formulations apply mutatis mutandis to each other and to the presently disclosed method of controlling a target organism.

[0326] In the context of the presently disclosed subject matter, the term "target organism control” or "controlling a target organism" should be understood to mean any pre-desired manipulation on a target organism and / or on a habitat of a target organism.

[0327] In some examples of the presently disclosed subject matter, the term "target organism control" or "controlling a target organism" refers to any modification or management of the organisms' population or behaviors, to reduce, redirect, or prevent their impact, including but not limited to preventing or limiting infestation, repelling, deterring, incapacitating, sterilizing, killing, and attracting organism as well as interfering with organism reproduction, disrupting the organism's life cycles or otherwise altering the organism's activity by the sustained release formulation, according to the first or second aspects of the present disclosure.

[0328] Further, in the context of the presently disclosed method of controlling aspect, the term "target organism" refers to an organism or group of organisms that require manipulation, in the context of the present disclosure.

[0329] In the context of the presently disclosed subject matter, the term "habitat of target organism" is to be understood to refer to the environment or living area— whether natural or artificial— in which the targeted organism resides, reproduces, or seeks refuge, including soil, water, plant surfaces, human-made structures, or any other locale that supports the organism's life cycle.

[0330] In some examples of the presently disclosed subject matter, the target organism is a pest or other biological entity that negatively impact agriculture, public health, stored goods, or living environments.A non-limiting list of target organisms may be considered to have a negative impact, including insects, nematodes, mites, ticks, fungi, molds, bacteria, herbs, mollusks, arthropods, deer, birds, bats, and rodent.

[0331] In some examples of the presently disclosed subject matter, the target organism is an arthropod.

[0332] In some examples, the arthropod is any one of an insect and myriapod.

[0333] In some examples, the target organism comprises insects.

[0334] Without being limited thereto, the insect can be an insect selected from the group consisting of one or more moth, butterfly, beetle, true bug, aphid, cicada, planthopper, fly and mosquito, grasshoppers and locust, thrip, whiteflies and scale insect, Mealybugs, Leafhoppers, Caterpillars, weevil, ants, termites, Cockroaches, lice, Fleas, Bed bugs, Ticks, Fruit flies, Stink bugs, Earwigs, Japanese beetles, Potato beetles, Carpet beetles, Silverfish, Leaf miners, Greenfly, Blackfly, Diamondback moths, Cutworms, Sawflies, Red palm weevil, Cocoa pod borer, Corn earworm, Seed corn maggot, Cabbage worms, Red imported fire ants, Vine weevils, Spotted lanternfly, Root weevils, Aphididae, Mealybug wilt virus vectors, White grub beetles, Root aphids, Pine weevil, Leatherjackets and Springtails.

[0335] In some examples of the presently disclosed subject matter, the insect comprises at least ants.

[0336] In some examples of the presently disclosed subject matter, the insect comprises at least fruit flies.

[0337] In some examples of the presently disclosed subject matter, the target organism is nematode.

[0338] Without being limited thereto, the nematode can be a nematode selected from the group consisting of root-knot nematode and / or cyst nematode, Root-knot nematodes (Meloidogyne spp.), Cyst nematodes (Globodera spp.), Lesion nematodes (Pratylenchus spp.), Dagger nematodes (Xiphinema spp.), Pin nematodes (Bitylenchus spp.), Spiral nematodes (Helicotylenchus spp.), Stubby root nematodes (Trichodorus spp.), Lance nematodes (Hoplolaimus spp.), Needle nematodes (Longidorus spp.), Crimpnematodes (Criconemoides spp.), Leaf nematodes (Aphelenchoides spp.), Burrowing nematodes (Radopholus spp.), Root-lesion nematodes (Pratylenchus penetrans), Reniform nematodes (Rotylenchulus reniformis), Pine wilt nematode (Bursaphelenchus xylophilus), Soybean cyst nematode (Heterodera glycines), Tomato root-knot nematode (Meloidogyne incognita), Sugar beet cyst nematode (Heterodera schachtii), Coconut nematode (Bursaphelenchus cocophilus), Potato cyst nematode (Globodera rostochiensis), Wheat cyst nematode (Heterodera avenae), Root-knot nematode (Meloidogyne javanica), Mating disruption nematode (Meloidogyne hapla), Tobacco root-knot nematode (Meloidogyne hapla), Citrus nematode (Tylenchulus semipenetrans), Vine nematode (Xiphinema index), Meadow nematode (Pratylenchus punctatus), Cereal cyst nematode (Heterodera filipjevi), and Vegetable cyst nematode (Heterodera rostochiensis).

[0339] In some examples of the presently disclosed subject matter, the target organism comprises mites and / or ticks.

[0340] Without being limited thereto, the mites and / or ticks can be selected from the group consisting of Two-spotted spider mite, Red spider mite, Broad mite, Cyclamen mite, Strawberry mite, Apple rust mite, European red mite, Southern red mite, Two spotted spider mite, Pear psylla, Orchid mite, Spruce spider mite, Clover mite, Tetranychus urticae, Pacific mite, Russet mite, Bulb mite, Stinging mite, Walnut mite, Pink mite, Fern mite, Spider mite, Dust mite, Strawberry leaf mite, Tomato russet mite, Pea mite, Citrus red mite, Mulberry mite, Cotton leaf mite, Varroa mite (Varroa destructor), Broad mite (Polyphagotarsonemus latus), Strawberry russet mite (Aculops lycopersici), Root-feeding mite (Tyrophagus putrescentiae), Clover rust mite (Acariicus bursarius), Gall mite (Eriophyes spp.), Boxwood mite (Eriophyes buxi), Pine mite (Dendrocnemus spp.), Grain mite (Acarus siro), Brown wheat mite (Petrobia latens), Pea leafhopper mite (Tetranychus kanzawai), Sweet potato mite (Aculops sweetpotatoi), Raspberry bud mite (Aculops rhododendri). spider mite and gall mite.

[0341] In some examples of the presently disclosed subject matter, mites and / or ticks comprise at least varroa mites (varroa destructor).In some examples of the presently disclosed subject matter, mites and / or ticks comprise at least spider mites.

[0342] In some examples of the presently disclosed subject matter, the target organism is a mollusk.

[0343] Without being limited thereto, the mollusk is selected from the group consisting of Common garden snail (Cornu aspersum), Brown-lipped snail (Cepaea nemoralis), Giant African land snail (Achatina achatina), Apple snail (Pomacea canaliculata), Silver slug (Arion subfuscus), Black slug (Arion ater), European brown garden snail (Cornu aspersum), Marsh snail (Cochliopa texana), Golden apple snail (Pomacea canaliculata), Pinecone snail (Leptoxis carinata), Ramshorn snail (Planorbella duryi), Water pond snail (Lymnaea stagnalis), Bladder snail (Physa acuta), Chinese mystery snail (Cipangopaludina chinensis), Zebra nerite snail (Neritina natalensis), Mediterranean land snail (Eobania vermiculata), Giant land snail (Achatina fulica), Black cupped snail (Albinaria coerulea), Slender slug (Deroceras laeve), Greenhouse slug (Arion vulgaris), Field slug (Deroceras reticulatum), Pond snail (Lymnaea stagnalis), Ivory snail (Pomacea bridgesii), New Zealand mud snail (Potamopyrgus antipodarum), Shagreen snail (Eobania vermiculata), Freshwater mollusks (Corbicula fluminea), Marshland mollusk (Peringia ulvae), Gulf Coast mud snail (Tritia obsoleta), Black mud snail (llyanassa obsoleta), European slug (Arion lusitanicus). In some examples, the mollusk is a slug or snail.

[0344] In some examples of the presently disclosed subject matter, the target organism is a rodent. Without being limited thereto, the rodent can be selected from the group consisting of mice, rat vole or lemming, Groundhogs, gopher, hystrix (porcupine).

[0345] In some examples of the presently disclosed subject matter, the target organism comprises or is a microorganism. The microorganism can be any one or combination of fungi or bacterium.

[0346] In some examples of the presently disclosed subject matter, the target organism comprises herbs.In some examples of the presently disclosed subject matter, the target organism is a mammal, preferably non-human mammal includes rodents, bats, deer, badgers cats and dogs.

[0347] The method of pest control disclosed herein involves at least a step of exposing the presently disclosed sustained release formulation to the target organism and / or habitat of a target organism.

[0348] The manner of exposing the presently disclosed sustained release formulation depends, inter alia, on the physical state of the formulation, e.g. gel form, liquid form, solid form, paste form, etc.

[0349] The exposure of the sustained release formulation can be by any means known in the art, including, for example, spreading, smearing, spraying, substrate coating, placing the formulation in the surrounding of the target organism. As shown in the nonlimiting examples forming part of the present disclosure, the sustained release formulation exemplified herein exhibited sustained release at elevated temperatures (about 50°C) as well as by the mere placement of the sustained release formulation in an outside environment (temperature of about 10-40°C).

[0350] Finally, there is provided, in accordance with yet another aspect, a use of the presently disclosed sustained release formulation for controlling repelling pests.

[0351] Unless expressly indicated otherwise, all definitions and non-limiting examples provided in connection with the sustained release formulation and / or carrier composition —including definitions of groups of components, amounts of components, and examples thereof— shall also apply to the presently disclosed methods as well as to the presently disclosed use and shall be deemed an integral part thereof.

[0352] All definitions provided herein override any dictionary definitions, definitions in documents incorporated by reference, or ordinary meanings, unless otherwise specified.

[0353] The term "about" may cover a deviation of up to 1%, 5%, 10%, 15%, or 20% above or below the specified value, encompassing both integer and non-integer values. In some embodiments, "about" refers to ±10%.Unless clearly indicated otherwise, the indefinite articles "a" and "an" mean "at least one." Likewise, the singular forms "a", "an" and “the" include plural forms unless the context clearly dictates otherwise.

[0354] "And / or" means "either or both" of the elements it joins (i.e., they may appear together or separately). Where multiple elements are listed with "and / or" it should be read as "one or more" of those elements, potentially together with other elements not explicitly listed.

[0355] In this specification and the claims, "or" has the same inclusive meaning as "and / or" above. Unless terms such as "only one of', "exactly one of' or the transitional phrase "consisting of' are used, "or" covers one or more of the listed items, possibly alongside additional unlisted items.

[0356] The phrase "at least one” when referring to a list of elements, means selecting at least one element from the list without requiring each and every element in that list. It does not exclude the presence of additional elements beyond those identified.

[0357] Unless otherwise indicated, methods described with multiple steps do not require those steps to be performed in the specific order recited.

[0358] Transitional phrases like "comprising" "including" "carrying" "having" "containing" "involving" "holding" and "composed of' are open-ended, meaning "including but not limited to”. The phrase "consisting of' mean including and limited to while the phrase "consisting essentially of allows the inclusion of additional ingredients, steps, or parts that do not materially alter the basic and novel characteristics of the claimed composition, method, or structure.

[0359] Where ranges are presented, they are for convenience and do not limit the invention's scope. Each range is understood to disclose all sub-ranges and individual values within it, including fractional and integral values. For example, a range of 1 to 6 includes sub-ranges like 1 to 3, 2 to 6, and 3 to 6, as well as individual points 1, 2, 3, 4, 5, and 6. Phrases such as "ranging between" or "ranging from ... to ..." similarly include the endpoints and all values in between.As used herein, "method" refers to any manner, means, technique, or procedure for accomplishing a given task, including those known or readily developed by practitioners.

[0360] As used herein, the term "essentially" is to be understood to mean that the referenced parameter, composition, structure, or property may vary to a degree that does not materially affect the intended function or technical effect of the subject matter, such that minor deviations are permitted, for example deviations of no more than about ±10%, and in some examples no more than about ±5%, relative to the stated value or condition, provided that the relevant functional performance remains substantially unchanged.

[0361] Features described separately may be combined into a single embodiment, and those described in one embodiment may be used separately or in any suitable combination in other embodiments. Unless an embodiment cannot operate without a particular feature, that feature is not to be considered indispensable.

[0362] The following examples support various embodiments and aspects of the present invention as described above and as claimed below. Although these examples illustrate preferred embodiments, the scope of the invention is defined only by the appended claims and their equivalents. Practitioners in the art may make modifications without departing from the spirit or scope of the disclosed subject matter.

[0363] LIST OF PARAGRAPHS

[0364] The following paragraphs are provided to further illustrate the subject matter of the present disclosure. Each paragraph may be implemented independently or in any technically feasible combination with one or more features, steps, parameters, ranges, or alternatives described in other embodiments or in the claims. Unless the context clearly indicates otherwise, any embodiment, feature, or optional characteristic described herein with respect to one aspect of the disclosure is equally applicable, mutatis mutandis, to any other aspect, including any method, composition, formulation, use, or system as claimed.1. A method of preparing a sustained release formulation, the method comprises, mixing of a carrier composition with a volatile organic substance to form a blend;

[0365] the carrier composition comprises:

[0366] (i) a hydrophobic organic carrier; and

[0367] (ii) a quaternary amine of a general formula (I):

[0368] i:

[0369] R2- N - X - Y

[0370] R3 (I)

[0371] wherein

[0372] Ri, R2 and R3 represent, independently, a C1-C3 alkyl chain;

[0373] X represents Ci-Ce alkylene or Ci-Ce alkenylene chain; and Y represents an end moiety selected from the group consisting of carboxylic acid, ester, hydroxyl and quaternary ammonium moiety. 2. The method according to paragraph 1, wherein the hydrophobic carrier is essentially water free and the mixing of the carrier composition with the volatile organic substance is without formation of an emulsion.

[0374] 3. The method according to any one or combination of the above paragraphs wherein the mixing of the hydrophobic carrier with the volatile organic substance is without externally added water.

[0375] 4. The method according to any one or combination of the above paragraphs wherein the mixing of the hydrophobic carrier with the volatile organic substance is under conditions that provide an essentially uniform mixture.

[0376] 5. The method according to anyone or combination of the above paragraphs, wherein the hydrophobic carrier comprises lipids and / or polymers.6. The method according to anyone or combination of the above paragraphs, wherein the hydrophobic carrier comprises at least wax and at least one plant-derived oil.

[0377] 7. The method according to anyone or combination of the above paragraphs, wherein the hydrophobic organic carrier is of natural sources.

[0378] 8. The method according to anyone or combination of the above paragraphs, wherein Ri, R2 and R3 represent the same alkyl chain.

[0379] 9. The method according to anyone or combination of the above paragraphs, wherein Ri, R2 and R3 are each a methyl.

[0380] 10. The method according to anyone or combination of the above paragraphs, wherein X represents Ci-Ce alkylene.

[0381] 11. The method according to anyone or combination of the above paragraphs, wherein X represents C1-C2 alkylene.

[0382] 12. The method according to anyone or combination of the above paragraphs, wherein Y represents a carboxyl group.

[0383] 13. The method according to anyone or combination of the above paragraphs, wherein the quaternary amine comprises or is glycine betaine.

[0384] 14. The method according to any one or combination of paragraphs 1 to 11, wherein Y represents methylester.

[0385] 15. The method according to any one or combination of paragraphs 1 to 11, wherein Y represents a hydroxyl.

[0386] 16. The method according to any one or combination of paragraphs 1 to 11, wherein Ri, R2, and R3 are same alkyl chain; X represents C1-C2 alkylene and Y represents an end moiety selected from the group consisting of carboxyl, methylester and hydroxyl.

[0387] 17. The method according to any one or combination of paragraphs 1 to 11, wherein Y represents a quaternary ammonium moiety of formula (II)

[0388]

[0389] wherein R'I, R , and R'3 represent, independently a C1-C3 alkyl chain.

[0390] 18. The method according to paragraph 17, wherein R'I, R , and R'3 are identical, respectively to Ri, R2, and R3.

[0391] 19. The method according to any one or combination of the above paragraphs, wherein the quaternary amine is in an amount of between about 5wt% and about 40wt% out of the total weight of the sustained release formulation.

[0392] 20. The method according to any one or combination of the above paragraphs, wherein the hydrophobic carrier is in an amount of between about 10wt% and about 95wt% out of the total weight of the sustained release formulation.

[0393] 21. The method according to any one or combination of the above paragraphs, wherein the volatile organic substance is selected from the chemical group consisting of terpenes, terpenoids, volatile lipids, volatile fatty acids, volatile esters, volatile alcohols, volatile ketones, and volatile aldehydes and any functional derivatives and / or combination thereof, and / or from the biological or functional group consisting of essential oils, allelochemicals, pheromones, allomones, and kairomones, as well as any volatile derivatives and / or combinations thereof.

[0394] 22. The method according to any one or a combination of the above paragraphs, wherein the volatile organic substance is selected from the collective group consisting of terpenes, terpenoids, essential oils, pheromones and any combination of same.

[0395] 23. The method according to any one or combination of the above paragraphs, wherein the volatile organic substance is in an amount of between about 5wt% and about 40wt% out of the total weight of the sustained release formulation.24. The method according to anyone or combination of the above paragraphs, further comprising adding to the carrier composition and / or to the blend at least one of (i) thickening agent, (ii) tackifying agent, (iii) filler.

[0396] 25. The method according to paragraph 24, wherein the thickening agent is selected from the group consisting of mineral based thickening agents, inorganic salt based thickening agents, organic and polymeric thickening agents and any combination of same.

[0397] 26. The method according to any one or a combination of paragraphs 24 or 25, wherein the thickening agent comprises a mineral-based thickening agent.

[0398] 27. The method according to any one or combination of paragraphs 24 to 26, wherein the thickening agent comprises fumed silica.

[0399] 28. The method according to anyone or combination of the above paragraphs, when combined with paragraph 24, wherein the tackifying agent is selected from the group consisting of resins and rosins.

[0400] 29. The method according to anyone or combination of the above paragraphs, when combined with paragraph 24, wherein the filler comprises lignocellulose particles.

[0401] 30. The method according to any one or combination of the above paragraphs when combined with paragraph 24, wherein the filler is in an amount of up to about 10wt%.

[0402] 31. The method according to anyone or combination of the above paragraphs, when combined with paragraph 24, further comprising absorbing the volatile organic substance onto the filler, prior to mixing the volatile organic substance with the carrier composition.

[0403] 32. The method according to anyone or combination of the above paragraphs, wherein the mixing with the volatile organic substance is at a temperature below the boiling temperature or below the flash point temperature of the volatile organic substance.33. A method of preparing a sustained release formulation, the method comprises mixing, to form a blend, of

[0404] (i) a hydrophobic organic carrier;

[0405] (ii) a quaternary amine of a general formula (I),

[0406]

[0407] wherein

[0408] Ri, R2 and R3 represents, independently C1-C3 alkyl chain;

[0409] X represents Ci-Ce alkylene or alkenylene chain; and

[0410] Y represents an end moiety selected from the group consisting of carboxylic acid, ester, hydroxyl, quaternary ammonium moiety; and

[0411] (iii) a volatile organic substance;

[0412] the hydrophobic organic carrier, the quaternary amine and volatile organic substance, are as defined in any one of paragraphs 1 to 23.

[0413] 34. The method according to paragraph 33, comprising combining the quaternary amine with the volatile organic substance to form an intermediate mixture and mixing the intermediate mixture with the hydrophobic carrier thereby forming the blend.

[0414] 35. The method according to any one or combination of paragraphs 33 or 34, wherein the mixing further comprises including in the blend at least one of (i) a thickening agent, (ii) a tackifying agent and (iii) a filler, the thickening agent, the tackifying agent and the filler being defined in any one of the relevant paragraphs above.

[0415] 36. A sustained release formulation comprising a blend of:

[0416] (i) a hydrophobic organic carrier;

[0417] (ii) a quaternary amine of a general formula (I)

[0418]

[0419] wherein

[0420] Ri, R2 and R3 represents, independently C1-C3 alkyl;

[0421] X represents Ci-Ce alkylene or alkenylene chain; and

[0422] Y represents an end moiety selected from the group consisting of carboxyl, ester, hydroxyl, quaternary ammonium moiety, and

[0423] (iii) a volatile organic substance;

[0424] wherein the sustained release formulation is essentially water free; and

[0425] wherein the quaternary amine is of a source different from the source of the hydrophobic organic carrier, i.e. the quaternary amine is not inherently present in the hydrophobic organic carrier and is introduced as a distinct component.

[0426] 37. The sustained release formulation according to paragraph 36, obtained or obtainable by the method according to any one or combination of the above paragraphs relating to the method.

[0427] 38. The sustained release formulation according to any one or combination of paragraphs 36 or 37, comprising an amount of water of less than 5wt%.

[0428] 39. The sustained release formulation according to any one or any combination of the above paragraphs relating to sustained release formulation, wherein the quaternary amine and the volatile organic substance are essentially homogenously dissolved or dispersed within the hydrophobic organic carrier.

[0429] 40. The sustained release formulation according to any one or any combination of the above paragraphs relating to sustained release formulation, wherein the hydrophobic carrier comprises lipids and / or polymers.

[0430] 41. The sustained release formulation according to any one or any combination of the above paragraphs relating to sustained release formulation, whereinthe hydrophobic organic carrier comprises at least one wax and at least one plant-derived oil.

[0431] 42. The sustained release formulation according to any one or any combination of the above paragraphs relating to sustained release formulation, wherein the hydrophobic organic carrier is from natural sources.

[0432] 43. The sustained release formulation according to any one or any combination of the above paragraphs relating to sustained release formulation, wherein Ri, R2 and R3 represent the same alkyl chain.

[0433] 44. The sustained release formulation according to any one or any combination of the above paragraphs relating to sustained release formulation, wherein Ri, R2 and R3 are each methyl.

[0434] 45. The sustained release formulation according to any one or any combination of the above paragraphs relating to sustained release formulation, wherein X represents Ci-Ce alkylene.

[0435] 46. The sustained release formulation according to any one or any combination of the above paragraphs relating to sustained release formulation, wherein X represents C1-C2 alkylene.

[0436] 47. The sustained release formulation according to any one or any combination of the above paragraphs relating to sustained release formulation, wherein Y represents a carboxyl group.

[0437] 48. The sustained release formulation according to any one or combination of paragraphs 36 to 46, wherein Y represents a methylester.

[0438] 49. The sustained release formulation according to any one or combination of paragraphs 36 to 46, wherein Y represents a hydroxyl.

[0439] 50. The sustained release formulation according to any one or combination of paragraphs 36 to 46, wherein Y represents a quaternary ammonium moiety.

[0440] 51. The sustained release formulation according to any one or combination of paragraphs 36 to 46, wherein Ri, R2 and R3 represent the same alkyl chain; X representsCi-C2alkylene and Y represents an end moiety selected from the group consisting of carboxyl, methylester and hydroxyl.

[0441] 52. The sustained release formulation according to any one or combination of paragraphs 36 to 47 or 51, wherein the quaternary amine comprises or is glycine betaine.

[0442] 53. The sustained release formulation according to any one or combination of paragraphs 36 to 46 or 50, wherein Ri, R2 and R3 represent the same alkyl chain; X represents Ci-Ce alkylene and Y represents a quaternary amine of formula (II)

[0443]

[0444] wherein R'i, R'2 and R'3 represent, independently, a C1-C3 alkyl chain.

[0445] 54. The sustained release formulation according to any one or combination of the above paragraphs related to sustained release formulation, wherein the quaternary amine is in an amount of between about 5wt% and about 40wt% out of the total weight of the sustained release formulation.

[0446] 55. The sustained release formulation according to any one or combination of the above paragraphs relating to sustained release formulation, wherein the volatile organic substance is selected from the chemical group consisting of terpenes, terpenoids, volatile lipids, volatile fatty acids, volatile esters, volatile alcohols, volatile ketones, and volatile aldehydes and any functional derivatives and / or combination thereof, and / or from the biological or functional group consisting of essential oils, allelochemicals, pheromones, allomones, and kairomones, as well as any volatile derivatives and / or combinations thereof.

[0447] 56. The sustained release formulation according to any one or combination of the above paragraphs relating to sustained release formulation, wherein the volatile organic substance is selected from the collective group consisting of terpenes, terpenoids, essential oils pheromones and any combination of same.57. The sustained release formulation according to any one or combination of the above paragraphs relating to sustained release formulation, wherein the volatile organic substance is in an amount of between about 5wt% and about 40wt% out of the total weight of the sustained release formulation.

[0448] 58. The sustained release formulation according to any one or combination of the above paragraphs relating to sustained release formulation, wherein the hydrophobic organic carrier is in an amount of between about 10wt% and about 95wt% out of the total weight of the sustained release formulation.

[0449] 59. The sustained release formulation according to any one or combination of the above paragraphs related to sustained release formulation, wherein the blend further comprises at least one of (i) thickening agent; (ii) tackifying agent; (iii) filler. 60. The sustained release formulation according to paragraph 59, wherein the thickening agent is selected from the group consisting of mineral-based thickening agents, inorganic salt based thickening agents, organic thickening agents, polymeric thickening agents and any combination of same.

[0450] 61. The sustained release formulation according to any one or a combination of paragraphs 59 or 60, wherein the thickening agent is a mineral based thickening agent.

[0451] 62. The sustained release formulation according to any one or combination of paragraphs 59 to 61, wherein the thickening agent comprises fumed silica.

[0452] 63. The sustained release formulation according to any one or a combination of paragraphs 59 to 62, wherein the thickening agent is in an amount of up to 5wt%.

[0453] 64. The sustained release formulation according to any one or combination of the above paragraphs related to sustained release formulation, when combined with paragraph 59, wherein the tackifying agent is resins and / or rosins.

[0454] 65. The sustained release formulation according to any one or combination of the above paragraphs related to sustained release formulation, when combined with paragraph 59, wherein the tackifying agent is in an amount of between about 0wt% and about 40wt%.66. The sustained release formulation according to any one or combination of the above paragraphs related to sustained release formulation, when combined with paragraph 59, wherein the filler comprises lignocellulose particles.

[0455] 67. The sustained release formulation according to any one or combination of the above paragraphs related to sustained release formulation, when combined with paragraph 59, wherein the filler is in an amount of up to about 10wt%.

[0456] 68. A method of controlling a target organism, the method comprises exposing a target organism or a habitat of a target organism to a sustained release formulation comprising a blend of:

[0457] (i) a hydrophobic organic carrier;

[0458] (ii) a quaternary amine of a general formula (I)

[0459] it

[0460] R2- N - X - Y

[0461] R3 (I),

[0462] wherein

[0463] Ri, R2 and R3 represents, independently C1-C3 alkyl;

[0464] X represents Ci-Ce alkylene or alkenylene chain; and

[0465] Y represents an end moiety selected from the group consisting of carboxyl, ester, hydroxyl, quaternary ammonium moiety,

[0466] and

[0467] (iii) a volatile organic substance;

[0468] wherein the sustained release formulation is essentially free of water.

[0469] 69. The method according to paragraph 68, wherein the sustained release formulation is as defined in any one or a combination of the above paragraphs relating to the sustained release formulation or is obtained or obtainable by the method as defined in any one or a combination of paragraphs relating to the method of preparing sustained release formulation.70. The method according to any one or combination of paragraphs 68 or 69, wherein the sustained release formulation comprises an amount of water of less than 5wt%.

[0470] 71. The method according to any one or combination of the above paragraphs relating to method of controlling a target organism, wherein the quaternary amine and the volatile organic substance are essentially homogenously dissolved or dispersed within the hydrophobic organic carrier.

[0471] 72. The method according to any one or combination of the above paragraphs relating to method of controlling a target organism, wherein the hydrophobic organic carrier comprises lipids and / or polymers.

[0472] 73. The method according to any one or combination of the above paragraphs relating to method of controlling a target organism, wherein the hydrophobic organic carrier is from natural source.

[0473] 74. The method according to any one or combination of the above paragraphs relating to method of controlling a target organism, wherein the hydrophobic carrier comprises at least one wax and at least one plant-derived oil.

[0474] 75. The method according to any one or combination of the above paragraphs relating to method of controlling a target organism, wherein Ri, R2 and R3 represent the same alkyl chain.

[0475] 76. The method according to any one or combination of the above paragraphs relating to method of controlling a target organism, wherein Ri, R2 and R3 are each a methyl.

[0476] 77. The method according to any one or combination of the above paragraphs relating to method of controlling a target organism, wherein X represents Ci-Ce alkylene.

[0477] 78. The method according to any one or combination of the above paragraphs relating to method of controlling a target organism, wherein X represents C1-C2 alkylene.79. The method according to any one or combination of the above paragraphs relating to method of controlling a target organism, wherein Y represents a carboxyl group.

[0478] 80. The method according to any one or combination of the above paragraphs relating to method of controlling a target organism, wherein the quaternary amine comprises or is glycine betaine.

[0479] 81. The method according to any one or combination of paragraphs 68 to 78, wherein Y represents a hydroxyl.

[0480] 82. The method according to any one or combination of paragraphs 68 to 78, wherein Y represents a quaternary ammonium moiety.

[0481] 83. The method according to any one or combination of the above paragraphs relating to method of controlling a target organism, wherein Ri, R2 and R3 represent the same alkyl chain; X represents C1-C2 alkylene and Y represents an end moiety selected from the group consisting of carboxyl, methylester and hydroxyl.

[0482] 84. The method according to any one or combination of paragraphs 68 to 78 or 82, wherein Ri, R2 and R3 represent the same alkyl chain; X represents Ci-Ce alkylene and Y represents a quaternary amine of formula (II)

[0483]

[0484] where R'i, R'2 and R'3 represent, independently, a C1-C3 alkyl chain.

[0485] 85. The method according to any one or combination of the above paragraphs relating to method of controlling a target organism, wherein the quaternary amine is in an amount of between about 5wt% and about 40wt%.

[0486] 86. The method according to any one or combination of the above paragraphs relating to method of controlling a target organism, wherein the volatile organic substance is selected from the chemical group consisting of terpenes, terpenoids, volatile lipids, volatile fatty acids, volatile esters, volatile alcohols, volatile ketones, andvolatile aldehydes and any functional derivatives and / or combination thereof, and / or from the biological or functional group consisting of essential oils, allelochemicals, pheromones, allomones, and kairomones, as well as any volatile derivatives and / or combinations thereof.

[0487] 87. The method according to any one or combination of the above paragraphs relating to method of controlling a target organism, wherein the volatile organic substance is in an amount of between about 5wt% and about 40wt%.

[0488] 88. The method according to any one or combination of the above paragraphs relating to method of controlling a target organism, wherein the hydrophobic organic carrier is in an amount of between about 10wt% and about 95wt%.

[0489] 89. The method according to any one or combination of the above paragraphs relating to method of controlling a target organism, wherein the sustained release formulation further comprises at least one of (i) thickening agent, (ii) tackifying agent, (iii) filler.

[0490] 90. The method according to paragraph 89, wherein the thickening agent is selected from the group consisting of mineral-based thickening agents, inorganic salt based thickening agents, organic thickening agents, polymeric thickening agents and any combination of same.

[0491] 91. The method according to any one or combination of paragraphs 89 or 90, wherein the thickening agent is a mineral based thickening agent.

[0492] 92. The method according to any one or combination of paragraphs 89 to 91, wherein the thickening agent is or comprises fumed silica.

[0493] 93. The method according to any one or combination of paragraphs 89 to 92, wherein the thickening agent is in an amount of up to 5wt%.

[0494] 94. The method according to any one or combination of the above paragraphs relating to method of controlling a target organism, when combined with paragraph 89, wherein the tackifying agent is or comprises resins and / or rosins.95. The method according to any one or combination of the above paragraphs relating to method of controlling a target organism, when combined with paragraph 89, wherein the tackifying agent is in an amount of between about Owt% and about 40wt%.

[0495] 96. The method according to any one or combination of the above paragraphs relating to method of controlling a target organism, when combined with paragraph 89, wherein the filler is or comprises lignocellulose particles.

[0496] 97. The according to any one or combination of the above paragraphs relating to method of controlling a target organism, wherein a single application of the sustained release formulation, in an open field, provides release of the volatile organic substance for period of at least 7 days.

[0497] 98. Use of a sustained release formulation for controlling a target organism, wherein the sustained release formulation comprises (i) a hydrophobic carrier including any one or combination of waxes, fatty acids and triglycerides, (ii) a quaternary amino acid and (iii) a volatile organic substance.

[0498] 99. The use according to paragraph 98, wherein the hydrophobic carrier, the quaternary amine and volatile organic substance, are as defined in any one or combination of the above paragraphs relating the method of preparing sustained release formulation.

[0499] 100. The use according to any one or combination of paragraphs 98 or 99, wherein the sustained release formulation further comprises any one of a thickening agent, a tackifying agent, a filler; wherein the thickening agent, the tackifying agent, and the filler are as defined in any one or combination of the above paragraphs relating the method of preparing sustained release formulation

[0500] 101. A carrier composition comprising a blend of: (i) a hydrophobic organic carrier ; and (ii) a quaternary amine of general formula (I)

[0501]

[0502] wherein Ri, R2 and R3 represent, independently, a C1-C3 alkyl; X represents a Ci-Ce alkylene or alkenylene chain; and Y represents an end moiety selected from the group consisting of carboxylic acid, ester, hydroxyl, and quaternary ammonium moiety.

[0503] 102. The carrier composition according to paragraph 101, wherein the hydrophobic organic carrier comprises at least one wax and at least one plant-derived oil.

[0504] 103. The carrier composition according to any one or combination of paragraphs 101 or 102, wherein the hydrophobic organic carrier is in an amount of from about 10wt% to about 95wt% out of the carrier composition.

[0505] 104. The carrier composition according to any one or combination of the above paragraphs relating to carrier composition, wherein the quaternary amine is in an amount of from about 5wt% to about 20wt% out of the carrier composition.

[0506] 105. The carrier composition according to any one or combination of the above paragraphs relating to carrier composition, wherein Ri, R2 and R3 represent the same alkyl chain.

[0507] 106. The carrier composition according to any one or combination of the above paragraphs relating to carrier composition, wherein Ri, R2 and R3 are each a methyl. 107. The carrier composition according to any one or combination of the above paragraphs relating to carrier composition, wherein X represents a Ci-Ce alkylene chain.

[0508] 108. The carrier composition according to any one or combination of the above paragraphs relating to carrier composition, wherein X represents a C1-C2 alkylene chain.

[0509] 109. The carrier composition according to any one or combination of the above paragraphs relating to carrier composition, wherein Y represents a carboxyl group. 110. The carrier composition according to any one or combination of the above paragraphs relating to carrier composition, wherein the quaternary amine comprises glycine betaine.

[0510] 111. The carrier composition according to any one or combination of paragraphs 101 to 108, wherein Y represents a methyl ester.112. The carrier composition according to any one or combination of paragraphs 101 to 108, wherein Y represents a hydroxyl group.

[0511] 113. The carrier composition according to any one or combination of the above paragraphs relating to carrier composition, wherein Ri, R2 and R3 represent the same alkyl chain; X represents C1-C2 alkylene and Y represents an end moiety selected from the group consisting of carboxyl, methylester and hydroxyl.

[0512] 114. The carrier composition according to any one or combination of paragraphs 101 to 108, wherein Y represents a quaternary ammonium moiety.

[0513] 115. The carrier composition according to paragraph 114, wherein Ri, R2 and R3 are a same alkyl chain; X represents Ci-Ce alkylene and Y represents a quaternary amine of formula (II)

[0514]

[0515] where R'i, R'2 and R'3 represent, independently, a C1-C3 alkyl chain.

[0516] 116. The carrier composition according to any one or combination of the above paragraphs relating to carrier composition, further comprising within the blend at least one of (i) thickening agent, (ii) tackifying agent, (iii) filler.

[0517] 117. The carrier composition according to paragraph 116, wherein the thickening agent is selected from the group consisting of mineral-based thickening agents, inorganic salt based thickening agents, and organic thickening agents, polymeric thickening agents and any combination of same.

[0518] 118. The carrier composition according to any one or combination of paragraphs 116 or 117, wherein the thickening agent is a mineral based thickening agent.

[0519] 119. The carrier composition according to any one or combination of paragraphs 116 to 118, wherein the thickening agent is or comprises fumed silica.120. The carrier composition according to any one or combination of paragraphs 116 to 119, wherein the thickening agent is present in an amount of up to about 5wt%.

[0520] 121. The carrier composition according to any one or combination of the above paragraphs relating to carrier composition, when combined with paragraph 116, wherein the tackifying agent is or comprises resins and / or rosins.

[0521] 122. The carrier composition according to any one or combination of the above paragraphs relating to carrier composition, when combined with paragraph 116, wherein the tackifying agent is present in an amount of from about 0wt% to about 40wt%.

[0522] 123. The carrier composition according to any one or combination of the above paragraphs relating to carrier composition, when combined with paragraph 116, wherein the filler comprises lignocellulose particles.

[0523] 124. The carrier composition according to any one or combination of the above paragraphs relating to carrier composition, when combined with paragraph 116, wherein the filler is present in an amount of up to about 10wt%.

[0524] 125. The carrier composition according to any one or combination of the above paragraphs relating to carrier composition, wherein the quaternary amine is of a natural source different from the natural source of the hydrophobic carrier.

[0525] DESCRIPTION OF SOME NON-LIMITING EXAMPLES

[0526] Sustained release formulation

[0527]

[0528] :ine betaine

[0529]

[0530] Two methods are available to prepare the presently disclosed sustained release formulation.

[0531] The two exemplary methods make use of components and amounts, as listed in Table 3. Table 3 also includes two reference samples, a first reference including allcomponents albeit glycine betaine (the tertiary amino acid) and a second reference being free thymol.

[0532] No water was added to the formulation.

[0533] Table 3: Components of formulation

[0534]

[0535]

[0536] Pre-mixing formulation refers to the method when the volatile active ingredient is added during the preparation process of the carrier composition. The resulting formulation is already "pre-mixed" with the active ingredient.

[0537] In the method for preparing the "pre-mixed" formulation, components 1 to 4 of Table 3 (carnauba wax, triethylene glycol ester of gum rosin, glycerol ester of gum rosin and coconut oil) were weighted into container A ("Part A") and placed on a hot plate set to a temperature range of about 100-130°C, while stirring at low speed, until a homogeneous liquid mixture is formed.

[0538] Once the homogeneity of Part A was reached, medium stirring was applied while slowly reducing the temperature to a range of 70-80°C (lower than the boiling temperature of thymol being around 232°C).

[0539] In an open container B ("Part B"), components 5 and 7 from Table 3 (thymol, glycine betaine and softwood natural fibers) were thoroughly mixed for 2 minutes until all lumps disappeared.

[0540] After that component 6 of Table 3 (glycine betaine) was mixed into container B to form a formulation precursor, followed by the addition of component 8 of Table 3 (neem oil) and mixing well.

[0541] When the mixture of Part A reached the desired temperature range (70-80°C), the mixture of Part B was slowly added into container A, while continuously stirring, until a paste-like mixture is formed.

[0542] Finally, component 9 of Table 3 (fumed silica) was slowly added in portions to the paste-like mixture while stirring at medium speed.

[0543]

[0544] The "post-mixing" formulation provides a carrier composition (referred to as a base formulation) into which the active ingredient can be added at a later stage, e.g. upon need.The base formulation (post mixing) is prepared using the same steps as described in Method A above, but without adding the - thymol into the homogenous mixture of Part A and Part B. Additionally, since the volatile active ingredient, thymol, is not added to the mixture, there is no need to cool down Part A before combining it with Part B.

[0545] Specifically, components 1-4 are mixed together in container A at a temperature of 100-130 °C until a homogeneous liquid-like mixture is formed. In a container B, softwood natural fibers and glycine betaine are mixed together. Then, neem oil is added and mixed with softwood natural fibers and glycine betaine. Then Part B is combined with the homogeneous liquid-like mixture of Part A to form a paste-like mixture. Then fumed silica is added in portions to provide a ready for use base formulation.

[0546] The resulting ready for use base formulation can be packed until use. Upon need of use, thymol can be mixed into the base formulation, under conditions that avoid evaporation of the thymol, e.g. the temperature is lower than the boiling temperature of thymol.

[0547]

[0548] The ready to use mixing involves mixing all components in one pot, apart from the filler and volatile compound. The resulting carrier mixture can be stored until need to combine with the volatile compound. Upon need, the volatile compound is adsorbed onto the filler material and combined into the carrier mixture. If necessary, the carrier mixture is softened to allow essentially homogenous mixing of the filler and volatile compound into the carrier. Softening can be by at any temperature below the boiling temperature or below the flash point temperature of the volatile organic substance. Impact of glycine betaine on release rate of thymol

[0549] The purpose of this experiment is to exhibit the importance of using quaternary amine, over non-quaternary amino acids.

[0550] Different pre-mixed formulations having thymol as the volatile organic substance were prepared by method A as described in Example 1 using glycine betaine or amino acids instead of glycine betaine, as detailed in Table 4 below.To test the release rate of thymol, the different pre-mixed formulations were placed in an oven set at 50°C.

[0551] The amount of each component in a formulation is shown in Table 4. Initial weight was recorded, and the samples were weighed daily for the first week and weekly following the first week. The differences in the weights of formulations seem to be due to the evaporation of selected active ingredient. It noted that glycine betaine per se absorbs water in an amount that is not more than 60% of its weight and as such, if water is absorbed, it would result in an increase in weight in the below formulation, of not more than 5%, or even not more than 3% (data not shown).

[0552] Table 4: Components of the pre-mixed formulations

[0553]

[0554]

[0555] Figure 1 shows comparisons of release rates of thymol over time, at a temperature or 50°C, in various forms: as a free molecule, in a formulation without glycine betaine or an amino acid, and in formulations with different primary amino acids, such as glycine betaine, beta-alanine, valine, glutamine, arginine, histidine, or with the secondary amino acid tryptophan.

[0556] As can be seen from Figure 1, free thymol fully evaporated after about 60 days in its free form. The formulation, albeit without the amino acid, slowed the thymol release rate by about 5 times. Presence of an amino acid other than the quaternary amino acid glycine betaine, namely glutamine, histidine, beta alanine, tryptophan, valine and arginine showed the same release profile as with the formulation absent of an amino acid, and an inferior effect in comparison to glycine betaine. Without being bound by theory, it appears that the negative release values of thymol during the first 125 days can be attributed to minor absorption of water molecules by glycine betaine.

[0557] The formulation containing glycine betaine slowed down the release rate by "'100, demonstrating the slowest release rate and thus supporting the disclosed invention, that the slow-release rate of thymol is as a result of incorporating glycine betaine, the quaternary amino acid into the carrier formulation.

[0558] Impact of glycine types on release rates of thymol

[0559] The purpose of this experiment is to show the effect of the type of quaternary ammonium used in the formulation.

[0560] Four separate pre-mixed formulations were prepared according to method A, with thymol as an active ingredient. Three pre-mixed formulations contained glycine, glycine betaine (GB), glycine betaine-calcium stearate (GB-Ca-stearate), the fourth beinga pre-mixed formulation albeit without an amino acid. The details of the formulations are provided in Table 5.

[0561] Table 5: Formulations with alternatives glycine

[0562]

[0563] Figure 2 shows comparisons of release rates of thymol over time at a temperature of 50°C in different forms: as a free molecule, in a formulation without an amino acid, and in formulations containing glycine, glycine betaine, or glycine-betaine-calcium stearate.As can be seen from Figure 2, during the first 70 days the formulated without quaternary amine released 36% of the thymol and 53% after 140 days. The composition with glycine (with no quaternary amine) has released 26% in the first 70 days and 40% after 140 days. The compositions with glycine betaine and glycine betaine with Ca-stearate performed the best showing the contribution of the quaternary amine to the release rate.

[0564] The release rates of thymol from the formulation containing no amino acid or from formulation containing glycine were significantly faster than the formulation with glycine betaine or glycine-betaine-Ca-stearate. Further, the data presented in Table 5 and Figure 2 support the results of Figure 1, showing that glycine per se (non-quaternary amino acid), has no significant effect on the release rate compared to the formulation without an amino acid.

[0565]

[0566] ammonium on release rates of

[0567]

[0568] The purpose of this experiment is to show the significance of the presence of a quaternary amino acid in the formulation.

[0569] Two separate pre-mixed formulations were prepared according to Method A with thymol as an active ingredient. The formulations contained glycine betaine or cetyltrimethylammonium chloride, as detailed in Table 6.

[0570] The purpose of this experiment was to understand the effect of the presence of an amino acid moiety in quaternary ammonium form on the release rate of thymol. The release rate of thymol was also compared to its free form and to a formulation that does not contain any amino acid.Table 6: Formulations containing quaternary ammonium

[0571]

[0572] The cetyltrimethylammonium chloride inherently included water which resulted in a small amount of water in the final formulation, which was insufficient to form an emulsion.

[0573] Figure 3 shows comparisons of release rates of thymol over time at a temperature of 50°C in its various forms: as a free molecule, in a formulation withoutamino acids, in a formulation with cetyltrimethylammonium chloride or with glycine betaine.

[0574] As can be seen from Figure 3, the formulation containing the quaternary ammonium cetyltrimethylammonium chloride (i.e. without the amino acid) did not slow the thymol release rate and has almost the same release profile as the free thymol. The slowest release rate of thymol was obtained for formulation containing glycine-betaine.

[0575] These results indicate that the inhibition of the release rate of thymol is not only associated with quaternary ammonium but with the presence of an amino acid in the quaternary ammonium molecule, in this case glycine betaine form.

[0576] Evaporation of different volatile oil

[0577] The purpose of this experiment is to show the effect of the formulation on the release rate of different volatile oils (different active ingredients).

[0578] Three separate pre-mixed formulations were prepared according to Method A, with different essential oils as active ingredients. All formulations contained glycine betaine as the quaternary amino acid. The different formulations are provided in Table 7.

[0579] Table 7: Components in the formulations containing various essential oils.

[0580]

[0581]

[0582] Figure 4 shows comparisons of evaporation rates of clove oil, tea tree oil, or mint oil in their natural, free form and when incorporated into the carrier formulation containing glycine-betaine.

[0583] As can be seen from Figure 4, the formulations containing glycine betaine resulted in a significantly lower evaporation rate for each of the essential oils as compared to their evaporation in their free state.

[0584] On day 28, each of the oil's evaporation rate was between 5 times (clove oil) to 7 times (mint oil) slower than their evaporation in a free state.

[0585] Even after day 200, less than about 60% of the essential oil has been evaporated, while clove oil showed about 50% evaporation.

[0586] From the data presented in Figure 4 it is clearly evident that the carrier formulation containing the quaternary amino acid, glycine betaine was also effective insignificantly slowing the release rate of other essential oils, and thus can be used as a platform for the controlled, slow release of essential oils.

[0587] Evaporation rates of methyl eugenol from different formulations

[0588] The purpose of this experiment was to assess the effect of 1 gram of each tested formulation on the release rate of the pheromone methyl eugenol (ME) as compared to 1 gram of a commercial formulation.

[0589] Specifically, the tested formulations included:

[0590] Commercial Formulation - One (1) gram of a commercial formulation manufactured by Pherobank BV of Bactrocera Zonata (Dacus) pheromone (Methyl Eugenol) impregnated in a solid plug of cellulose acetate and waxes dispenser, including 28.2% w / w ME (determined by GC / MS, while declared by manufacture to be 33%) Formulation A- One (1) gram of a hydrophobic carrier as defined in Table 8, in gel form, and holding 10% ME out of total weigh of formulation.

[0591] Formulation B- Two (2) grams of a hydrophobic carrier as defined in Table 8, in gel form, and holding 10% ME out of total weight of formulation (i.e. same concentration as product B, yet twice the amount).

[0592] Formulation C- One (1) gram of a hydrophobic carrier as defined in Table 8, in gel form, and holding 20% ME out of total weight of formulation.

[0593] Table 8 - Formulations with Methyl Eugenol

[0594]

[0595]

[0596] The different tested products were placed across the orchard and exposed to the same environmental conditions. Four repetitions were performed for each type of formulation.

[0597] After 203 days the formulations were collected and analyzed by GC / MS to determine the percentages of ME left in each formulation. To this end, about 30 mg was taken from the center of each tested product and extracted with 10 ml hexane. The extracted samples were then filtered through 0.22 pm filter and injected into the GC / MS.

[0598] As can be seen from Figure 5, during the 203-days test period, the commercial product exhibited the greatest reduction in ME, decreasing from 28.2% to 5.16%, whichcorresponds to an approximate loss of 82%. At the same time, tested formulations A to C lost only around half of their original concentration. Formulation A started at 10% and reached 5.4%. Formulation B had double the amount with the same ME%, starting with 10% and ending with 4.76%. Formulation C had double the percentage of ME and the same total amount as Formulation A, with 20% at the beginning and 9.99% at the end.

[0599] Additionally, the standard deviation for formulations A-C was considerably lower than that of the commercial product, suggesting that the evaporation rates for formulations A-C were consistent with one another and remained stable throughout the experimental period.

[0600] These results confirm that formulations A-C exhibited slow release of ME s with a superior advantage over commercial formulations.

[0601] ion

[0602]

[0603] The purpose of this experiment was to show the pattern of evaporation rate of thymol from the formulation of Table 3.

[0604] 24 samples of ~7g of formulated material containing thymol were transferred into 20 ml head-space GC / MS glass vials. Initial weights of all samples were recorded, and samples were placed open (no lid) in a 50°C oven. At each time point, two samples were removed from the oven, weighed, cap screwed, and placed at -20°C for storage.

[0605] After 84 days the formulations were analyzed by GC / MS to determine the percentages of thymol left in each formulation. To this end, about 30 mg was taken from the center of each tested product and extracted with 10 ml hexane. The extracted samples were then filtered through 0.22 pm filter and injected into the GC / MS.

[0606] The results showed the initial percentage after the first week is around 17% and constantly lowering over time until reaching 12% after 84 days. Although the initial formulation had 20% thymol during the preparation but 16-18% thymol during the first week might indicate that some thymol evaporated during the processing.

[0607] As can be seen from Figure 6, the results clearly show that the formulation holds the thymol and lets it evaporate slowly with a linear behavior into the surroundings.Example 2: sustained release formulation with other quaternary amines Preparation

[0608] The purpose of this experiment is to show the significance of the presence of a quaternary amine in the formulation.

[0609] Seven separate pre-mixed formulations were prepared according to Method A with thymol as an active ingredient as detailed in Table 9.

[0610] The purpose of this experiment was to understand the effect of the presence of a quaternary amine moiety form on the release rate of thymol. The release rate of thymol was also compared to its free form and to a formulation that does not contain any quaternary amine.

[0611] Table 9 - sustained release formulation with other quaternary amines

[0612]

[0613]

[0614] The samples were placed in uncapped containers within an unsealed incubator at 50 °C and weighed weekly.

[0615] Characterization

[0616] The results of this example showed a linear trend in evaporation over a 20-week period. The free thymol was completely evaporated (100% evaporated) after around 50 days. The control group without any quaternary amine has lost approximately 50% of the initial thymol amount. During the 20-week period, the glycine betaine, glycine betaine Ca-stearate, acetylcholine chloride, and choline HCI formulations showed the lowest evaporation. Hexamethonium bromide has evaporated around 20% at the same time. At the same time, glycine betaine HCI has evaporated approximately 40% of the initial thymol.

[0617] As the results clearly show, the molecular weight of the quaternary amine, its functional groups, and their polarity, mobility, and other properties affect the release rate.

[0618] Example 3: Impact of carrier composition

[0619] In order to test the necessity of the hydrophobic carrier, it is possible to test the effect of the hydrophobic organic carrier compared to a formulation without it. Theformulation with the hydrophobic carrier will be prepared with glycine betaine and with thymol as the volatile organic compound. The formulation without the hydrophobic carrier will consist solely of glycine betaine and thymol (same ratio). The glycine betaine and thymol will be ground together and melted in a solvent solution (e.g. dichloromethane and methanol). The solution will then be heated to evaporate the solvents, leaving only glycine betaine and thymol in a co-crystalline structure. Then, both formulations with an identical amount of thymol will be placed uncapped in an incubator at 50 °C and weighed weekly.

[0620] In this case, the results of the formulation without the hydrophobic carrier will be similar to those reported in the literature, and that 50% of the thymol will evaporate in approximately two weeks. While at the same time, less than 10% of the thymol will evaporate from the formulation with the hydrophobic carrier, as determined by GC-MS.

Claims

CLAIMS:

1. A method of preparing a sustained release formulation, the method comprises, mixing of a carrier composition with a volatile organic substance to form a blend; the carrier composition comprises:(i) a hydrophobic organic carrier; and(ii) a quaternary amine of a general formula (I):I’- R2- N - X - YR3 (I)whereinRi, R2 and R3 represent, independently, a C1-C3 alkyl chain;X represents Ci-Ce alkylene or Ci-Ce alkenylene chain; and Y represents an end moiety selected from the group consisting of carboxylic acid, ester, hydroxyl and quaternary ammonium moiety.

2. The method of claim 1, wherein the hydrophobic carrier is essentially water free and the mixing of the carrier composition with the volatile organic substance is without formation of an emulsion.

3. The method of claim 1 or 2, wherein the hydrophobic carrier comprises lipids and / or polymers.

4. The method of any one of claims 1 to 3, wherein the hydrophobic carrier comprises at least wax and at least one plant-derived oil.

5. The method of any one of claims 1 to 4, wherein the hydrophobic organic carrier is of natural sources.

6. The method of any one of claims 1 to 5, wherein Ri, R2 and R3 represent the same alkyl chain.

7. The method of any one of claims 1 to 6, wherein Ri, R2 and R3 are each a methyl.

8. The method of any one of claims 1 to 7 , wherein Y represents a carboxyl group.

9. The method of any one of claims 1 to 8, wherein the quaternary amine comprises or is glycine betaine.

10. The method of any one of claims 1 to 9, wherein Y represents a hydroxyl.

11. The method of any one of claims 1 to 10, wherein the quaternary amine is in an amount of between about 5wt% and about 40wt% out of the total weight of the sustained release formulation.

12. The method of any one of claims 1 to 11, wherein the volatile organic substance is selected from the group consisting of terpenes, terpenoids, essential oils, pheromones, allelomones, volatile lipids, volatile fatty acids, volatile esters, volatile alcohols, volatile ketones, and volatile aldehydes, any functional volatile derivatives and / or combination thereof.

13. The method of any one of claims 1 to 12, wherein the hydrophobic carrier is in an amount of between about 10wt% and about 95wt% out of the total weight of the sustained release formulation.

14. The method of any one of claims 1 to 13, wherein the volatile organic substance is in an amount of between about 5wt% and about 40wt% out of the total weight of the sustained release formulation.

15. The method of any one of claims 1 to 14, further comprising adding to the carrier composition and / or to the blend at least one of (i) thickening agent, (ii) tackifying agent, (iii) filler.

16. The method of claim 15, wherein the thickening agent comprises a mineralbased thickening agent.

17. The method of claim 16, wherein the thickening agent comprises fumed silica.

18. The method of any one of claims 1 to 17, when dependent on claim 15, wherein the tackifying agent is selected from the group consisting of resins and rosins.

19. The method of any one of claims 1 to 18, when dependent on claim 15, wherein the filler comprises lignocellulose particles.

20. The method of any one of claims 1 to 19, when dependent on claim 15, further comprising absorbing the volatile organic substance onto the filler, prior to mixing the volatile organic substance with the carrier composition.

21. The method of any one of claims 1 to 20, wherein the mixing with the volatile organic substance is at a temperature below the boiling temperature or below the flash point temperature of the volatile organic substance.

22. A method of preparing a sustained release formulation, the method comprises mixing, to form a blend, of(i) a hydrophobic organic carrier;(ii) a quaternary amine of a general formula (I),whereinRi, R2 and R3 represents, independently C1-C3 alkyl chain;X represents Ci-Ce alkylene or alkenylene chain; andY represents an end moiety selected from the group consisting of carboxylic acid, ester, hydroxyl, quaternary ammonium moiety; and (iii) a volatile organic substance;the hydrophobic organic carrier, the quaternary amine and volatile organic substance, are as defined in any one of claims 1 to 14.

23. The method of claim 22, wherein the mixing further comprises including in the blend at least one of (i) a thickening agent, (ii) a tackifying agent and (iii) a filler, the thickening agent, the tackifying agent and the filler being as defined in any one of claims 17 to 19.

24. A sustained release formulation comprising a blend of:(i) a hydrophobic organic carrier;(ii) a quaternary amine of a general formula (I)itR2- N - X - YR3 (I),whereinRi, R2 and R3 represents, independently C1-C3 alkyl;X represents Ci-Ce alkylene or alkenylene chain; andY represents an end moiety selected from the group consisting of carboxyl, ester, hydroxyl, quaternary ammonium moiety, and(iii) a volatile organic substance;wherein the sustained release formulation is essentially water free; andwherein the quaternary amine is of a source different from the source of the hydrophobic organic carrier.

25. The sustained release formulation of claim 24, obtained or obtainable by the method of any one of claims 1 to 23.

26. The sustained release formulation of claim 24 or 25, wherein the quaternary amine and the volatile organic substance are essentially homogenously dissolved or dispersed within the hydrophobic organic carrier.

27. The sustained release formulation of any one of claims 24 to 26, wherein the hydrophobic carrier comprises lipids and / or polymers.

28. The sustained release formulation of any one of claims 24 to 27, wherein the hydrophobic organic carrier comprises at least one wax and at least one plant-derived oil.

29. The sustained release formulation of any one of claims 24 to 28, wherein the hydrophobic organic carrier is from natural sources.

30. The sustained release formulation of any one of claims 24 to 29, wherein Ri, R2 and R3 represent the same alkyl chain.

31. The sustained release formulation of any one of claims 24 to 30, wherein Ri, R2 and R3 are each a methyl.

32. The sustained release formulation of any one of claims 24 to 31, wherein Y represents a carboxyl group.

33. The sustained release formulation of any one of claims 24 to 32, wherein Y represents a hydroxyl.

34. The sustained release formulation of any one of claims 24 to 33, wherein the quaternary amine comprises or is glycine betaine.

35. The sustained release formulation of any one of claims 24 to 34, wherein the quaternary amine is in an amount of between about 5wt% and about 40wt% out of the total weight of the sustained release formulation.

36. The sustained release formulation of any one of claims 24 to 35, wherein the volatile organic substance is selected from the group consisting of terpenes, terpenoids, essential oils, pheromones, allomones, kairomones, volatile lipids, volatile fatty acids, volatile esters, volatile alcohols, volatile ketones, and volatile aldehydes any functional volatile derivatives and / or combinations thereof.

37. The sustained release formulation of any one of claims 24 to 36, wherein the volatile organic substance is in an amount of between about 5wt% and about 40wt% out of the total weight of the sustained release formulation.

38. The sustained release formulation of any one of claims 24 to 37, wherein the hydrophobic organic carrier is in an amount of between about 10wt% and about 95wt% out of the total weight of the sustained release formulation.

39. The sustained release formulation of any one of claims 24 to 38, wherein the blend further comprises at least one of (i) thickening agent; (ii) tackifying agent; (iii) filler.

40. The sustained release formulation of claim 39, wherein the thickening agent is a mineral based thickening agent.

41. The sustained release formulation of claim 40, wherein the thickening agent comprises fumed silica.

42. The sustained release formulation of any one of claims 24 to 41, when dependent on claim 39, wherein the tackifying agent is resins and / or rosins.

43. The sustained release formulation of any one of claims 24 to 42, when dependent on claim 39, wherein the filler comprises lignocellulose particles.

44. A method of controlling a target organism, the method comprises exposing a target organism or a habitat of a target organism to a sustained release formulation comprising a blend of:(i) a hydrophobic organic carrier ;(ii) a quaternary amine of a general formula (I)itR2- N - X - YR3 (I),whereinRi, R2 and R3 represents, independently C1-C3 alkyl;X represents Ci-Ce alkylene or alkenylene chain; andY represents an end moiety selected from the group consisting of carboxyl, ester, hydroxyl, quaternary ammonium moiety, and(iii) a volatile organic substance;wherein the sustained release formulation is essentially free of water.

45. The method of claim 44, wherein the sustained release formulation is as defined in any one of claims 24 to 43 or is obtained or obtainable by the method of any one of claims 1 to 23.

46. The method of claim 44 or 45, wherein the quaternary amine and the volatile organic substance are essentially homogenously dissolved or dispersed within the hydrophobic organic carrier.

47. The method of any one of claims 44 to 46, wherein the hydrophobic organic carrier comprises lipids and / or polymers.

48. The method of any one of claims 44 to 47, wherein the hydrophobic organic carrier is from natural source.

49. The method of any one of claims 44 to 48, wherein the hydrophobic carrier comprises at least one wax and at least one plant-derived oil.

50. The method of any one of claims 44 to 49, wherein Ri, R2 and R3 represent the same alkyl chain.

51. The method of any one of claims 44 to 50, wherein Ri, R2 and R3 are each a methyl.

52. The method of any one of claims 44 to 51, wherein Y represents a carboxyl group.

53. The method of any one of claims 44 to 52, wherein the quaternary amine comprises or is glycine betaine.

54. The method of any one of claims 44 to 53, wherein Y represents a hydroxyl.

55. The method of any one of claims 44 to 54, wherein the quaternary amine is in an amount of between about 5wt% and about 40wt%.

56. The method of any one of claims 44 to 55, wherein the volatile organic substance is selected from the group consisting of terpenes, terpenoids, essential oils, pheromones, allomones, kairomones, volatile lipids, volatile fatty acids, volatile esters, volatile alcohols, volatile ketones, volatile aldehydes any functional volatile derivatives and / or combination thereof.

57. The method of any one of claims 44 to 56, wherein the volatile organic substance is in an amount of between about 5wt% and about 40wt%.

58. The method of any one of claims 44 to 57, wherein the hydrophobic organic carrier is in an amount of between about 10wt% and about 95wt%.

59. The method of any one of claims 44 to 58, wherein the sustained release formulation further comprises at least one of (i) thickening agent, (ii) tackifying agent, (iii) filler.

60. The method of claim 59, wherein the thickening agent is a mineral based thickening agent.

61. The method of claim 60, wherein the thickening agent is or comprises fumed silica.

62. The method of any one of claims 44 to 61, when dependent on claim 59, wherein the tackifying agent is or comprises resins and / or rosins.

63. The method of any one of claims 44 to 62, when dependent on claim 59, wherein the filler is or comprises lignocellulose particles.

64. The method of any one of claims 44 to 63 wherein a single application of the sustained release formulation, in an open field, provides release of the volatile organic substance for period of at least 7 days.

65. A carrier composition comprising a blend of: (i) a hydrophobic organic carrier ; and (ii) a quaternary amine of general formula (I)wherein Ri, R2 and R3 represent, independently, a C1-C3 alkyl; X represents a Ci-Ce alkylene or alkenylene chain; and Y represents an end moiety selected from the group consisting of carboxylic acid, ester, hydroxyl, and quaternary ammonium moiety.

66. The carrier composition of claim 65, wherein the hydrophobic organic carrier comprises at least one wax and at least one plant-derived oil.

67. The carrier composition of claim 65 or 66, wherein the hydrophobic organic carrier is in an amount of from about 10wt% to about 95wt% out of the carrier composition.

68. The carrier composition of any one of claims 65 to 66, wherein the quaternary amine is in an amount of from about 5wt% to about 20wt% out of the carrier composition.

69. The carrier composition of any one of claims 65 to 68, wherein Ri, R2 and R3 represent the same alkyl chain.

70. The carrier composition of any one of claims 65 to 69, wherein Ri, R2 and R3 are each a methyl.

71. The carrier composition of any one of claims 65 to 70, wherein Y represents a carboxyl group.

72. The carrier composition of any one of claims 65 to 71, wherein the quaternary amine comprises glycine betaine.

73. The carrier composition of any one of claims 65 to 72, wherein Y represents a hydroxyl group.

74. The carrier formulation of any one of claims 65 to 73, further comprising within the blend at least one of (i) thickening agent, (ii) tackifying agent, (iii) filler.

75. The carrier formulation of claim 74, wherein the thickening agent is a mineral based thickening agent.

76. The carrier composition of claim 74 or 75, wherein the thickening agent is or comprises fumed silica.

77. The carrier composition of any one of claims 65 to 76, when dependent on claim 74, wherein the tackifying agent is or comprises resins and / or rosins.

78. The carrier composition of any one of claims 65 to 77, when dependent on claim 74, wherein the filler comprises lignocellulose particles.

79. The carrier composition of any one of claims 65 to 78, wherein the quaternary amine is of a natural source different from the natural source of the hydrophobic carrier.

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