Formulations, methods of making and uses thereof

Abstract

The present invention relates generally to antimicrobial formulations and methods of formulating the same. Specifically, the present invention relates to antibacterial and antiviral formulations comprising cashew extract, iron particles and / or oxidized iron particles, and a carbohydrate. The weight ratio of cashew extract to iron particles and / or oxidized iron particles is from about 100:1 to about 1:200; the weight ratio of carbohydrate to cashew extract and iron particles and / or oxidized iron particles is from about 8:1 to about 1:300; and the cashew extract is at least partially incorporated into the iron particles and / or oxidized iron particles.

Description

Technical Field

[0001] In general, this invention relates to antimicrobial preparations and methods of their formulation. Specifically, this invention relates to antibacterial and antiviral preparations made from natural products and their uses. Background Technology

[0002] The development of microbial infections and antimicrobial resistance has recently garnered attention, becoming one of the more critical issues facing public health sectors. Microbial contamination refers to the unintentional or accidental introduction of microorganisms such as bacteria, yeasts, molds, fungi, viruses, prions, protozoa, or their toxins and byproducts. The increasing number of hospital-acquired infections (HAIs) is also a growing concern.

[0003] Diseases caused by highly pathogenic viruses that can be transmitted between humans and animals are increasingly attracting the attention of health authorities. Recent prominent examples include outbreaks of diseases caused by SARS and MERS coronaviruses (SARS-CoV, MERS-CoV), avian influenza virus (AIV), and Ebola virus (EBOV). With increasing globalization, the threat posed by these highly pathogenic viruses continues to expand.

[0004] Highly pathogenic viruses (HP viruses) can cause fatal systemic diseases in humans if left untreated.

[0005] For a concrete example, recently, coronavirus disease (COVID-19) has become an infectious disease caused by a novel virus. This disease causes respiratory illness (similar to the flu), with symptoms including cough, fever, and in severe cases, difficulty breathing.

[0006] Besides the fact that all these viruses can cause fatal diseases in humans and there are currently no effective treatments or vaccines, another important thing they have in common is that they are all zoonotic viruses, meaning they were originally transmitted from animals to humans.

[0007] Another common characteristic they share is a relatively high human mortality rate. In some cases, such as avian influenza, they have the potential to become pandemics, causing mass deaths and posing significant challenges to frontline healthcare workers who may be infected.

[0008] These types of diseases (such as coronavirus disease) are primarily spread through contact with an infected person who is coughing or sneezing. The virus can also spread when a person touches a surface or object contaminated with the virus and then touches their eyes, nose, or mouth. Therefore, it is necessary to disinfect or clean surfaces or objects, especially in public places.

[0009] With increasing focus on cleanliness across industries, the demand for antimicrobial products is also rising. These products can be used to protect surfaces from microbial invasion and are applicable to medical devices and packaging. The demand for antimicrobial additives is also rapidly expanding due to population growth and urbanization.

[0010] As a result, the global antimicrobial coatings market reached $7.1 billion in 2019 and is projected to grow at a CAGR of 12.8% from 2020 to 2027.

[0011] Currently available antimicrobial products rely on titanium, zinc, and silver compounds to produce their antimicrobial effects. While these elements are effective, they are expensive, toxic, and susceptible to heavy metal contamination. Furthermore, their antimicrobial efficacy is relatively low due to their dependence on light exposure.

[0012] There are also concerns about the potential toxicity of these products to humans and animals. Furthermore, if irritating chemicals are used in the synthesis process, toxic precursors (such as heavy metals) may always remain in the final product, necessitating extensive cleaning. This increases production costs.

[0013] In Singapore, food waste is one of the largest waste streams, with a staggering 744 million kilograms generated in 2019. This puts immense pressure on Singapore's land-scarce waste management facilities and limited landfill capacity. Furthermore, food waste increases the overall carbon footprint by wasting resources used to grow and import food. It is imperative to address this emerging issue of food waste to ensure the sustainable development of our environment and ecosystems.

[0014] We need to overcome or improve at least one of the above problems. Summary of the Invention

[0015] This invention is based on the understanding that certain natural products possess antimicrobial properties and can exert synergistic (or at least additive) effects when used in combination in formulations. In particular, the inventors have discovered that cashew nut extract possesses antimicrobial efficacy. For example, this extract exhibits antibacterial properties against Gram-negative bacteria *Escherichia coli* and Gram-positive bacteria *Staphylococcus aureus*. The natural product extract can be used in green solvents and demonstrates penetrating effects when tested on surfaces and textiles. Studies have also found that this extract possesses antiviral properties. Furthermore, synergistic (or at least additive) antimicrobial effects can be observed when used in combination with other ingredients such as iron particles and / or iron oxide particles. For example, cashew nut extract can be used as a precursor for the synthesis of iron particles and / or iron oxide particles. Additionally, when cashew nut extract is used in combination with carbohydrates, further synergistic (or at least additive) antimicrobial effects can be obtained by improving the residence time of free radicals. Because these formulations are synthesized / manufactured from biological or natural materials, they are safe for humans and animals. This green biosynthesis method is low-cost, waste-free, non-toxic, and environmentally friendly. This invention can be used as an antimicrobial coating, disinfectant, hand sanitizer and / or soap.

[0016] This invention provides a formulation comprising:

[0017] a) Cashew nut extract;

[0018] b) Iron particles and / or iron oxide particles; and

[0019] c) Carbohydrates;

[0020] The cashew nut extract is present in a weight ratio of approximately 100:1 to approximately 1:200 to iron particles and / or iron oxide particles; and

[0021] The weight ratio of carbohydrates (c) to cashew extract and iron particles and / or iron oxide particles (a and b) is approximately 8:1 to approximately 1:300; and

[0022] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles.

[0023] Advantageously, when formulated in this ratio, carbohydrates improve the residence time of free radicals generated by cashew nut extract and iron particles and / or iron oxide particles on the application surface. Furthermore, carbohydrates also enhance the adhesion of cashew nut extract and iron particles and / or iron oxide particles to the application surface. Therefore, a synergistic (or at least additive) effect of antimicrobial activity can be observed.

[0024] In some embodiments, the weight ratio of carbohydrates (c) to cashew extract and iron particles and / or iron oxide particles (a and b) is from about 8:1 to about 1:1.

[0025] In some embodiments, the carbohydrate content relative to the formulation is from about 1 wt% to about 15 wt%.

[0026] In some implementations, the carbohydrate is selected from chitosan.

[0027] In some embodiments, the cashew extract and iron particles and / or iron oxide particles (a and b) are present in a weight ratio of about 0.5 wt% to about 8 wt% relative to the formulation.

[0028] In some implementations, the pH of the formulation is approximately 4 to 5.

[0029] In some embodiments, the formulation further includes excipients selected from colorants, humectants, fragrances, stabilizers, penetrants, adhesion promoters, film-forming agents, transdyants, surfactants, solvents, antioxidants, or combinations thereof.

[0030] In some embodiments, the formulation further comprises a colorant selected from β-carotene, astaxanthin, or a combination thereof.

[0031] Advantageously, the colorant provides users with a visual cue indicating that an antimicrobial coating has been applied to the surface. This not only enhances user confidence but also provides an indication of when the coating needs to be reapplied.

[0032] In some embodiments, the colorant is present in a weight ratio of about 0.01 wt% to about 10 wt% of the formulation.

[0033] In some embodiments, the formulation further comprises a humectant selected from glycerin, urea, pyrrolidine carboxylic acid, aloe vera, or combinations thereof.

[0034] In some embodiments, the humectant is present at a weight ratio of about 2% to about 60% relative to the formulation.

[0035] In some embodiments, the formulation also includes a fragrance, wherein the fragrance includes essential oils.

[0036] In some embodiments, the flavoring is present in a weight ratio of about 0.01 wt% to about 40 wt% of the formulation.

[0037] In some embodiments, the formulation further comprises a penetrant selected from polyethyleneimine (PEI), lactic acid, or combinations thereof.

[0038] Advantageously, the permeabilizer makes the microbial cell membrane more susceptible to the influence of cashew extract and iron particles and / or iron oxide particles, thereby improving the antimicrobial effect.

[0039] In some embodiments, the weight ratio of the penetrant to the formulation is from about 0.01 wt% to about 25 wt%.

[0040] In some embodiments, the formulation further comprises a surfactant selected from cocoamphoacetate, taurine, isosulfate, olefin sulfonate, sulfosuccinate, sodium lauryliminodipropionate, disodium lauroamphodiacetate, and polysorbate.

[0041] In some implementations, the surfactant is decyl glucoside.

[0042] In some embodiments, the surfactant is present in a weight ratio of about 0.5% to about 80% of the formulation.

[0043] In some embodiments, the formulation further comprises a film-forming agent selected from (3-glycidoxypropyl)trimethoxysilane and / or gelatin.

[0044] In some embodiments, the film-forming agent is present in a weight ratio of about 10 wt% to about 25 wt% of the formulation.

[0045] In some embodiments, the formulation further comprises a solvent selected from water, ethyl acetate, or combinations thereof.

[0046] In some embodiments, the formulation also includes powdered cellulose.

[0047] In some embodiments, the weight ratio of cellulose to the formulation is from about 1 wt% to about 20 wt%.

[0048] In some implementations, powdered cellulose is extracted from fruit peel and / or bacterial-yeast symbiotic culture (SCOBY).

[0049] In some implementations, the formulation also contains maltodextrin.

[0050] In some embodiments, the cashew extract comprises a phenolic compound selected from tannins, catechins, epicatechins, epigallocatechins, p-coumarins, gallic acid, or combinations thereof.

[0051] In some embodiments, iron particles and / or iron oxide particles are at least partially passivated by phenolic compounds from cashew extract.

[0052] In some embodiments, cashew extract also contains proteins, amino acids, sugars, carbohydrates, or combinations thereof.

[0053] In some embodiments, iron particles and / or iron oxide particles are at least partially passivated by proteins, amino acids, sugars, carbohydrates, or combinations thereof.

[0054] In some embodiments, the iron particles and / or iron oxide particles are core-shell particles, with the core being a pure iron core or an iron alloy core, and the shell being an iron oxide shell.

[0055] In some embodiments, cashew extract is at least partially incorporated into the shells of iron particles and / or iron oxide particles.

[0056] In some implementations, the preparation reduces the log number of E. coli by at least about 2 after 5 minutes.

[0057] In some implementations, the formulation reduces the log number of E. coli by at least about 2 after 1 minute.

[0058] In some implementations, the preparation reduces the logarithm of Staphylococcus aureus by at least about 2 after 5 minutes.

[0059] In some embodiments, the preparation reduces the logarithm of Staphylococcus aureus by at least about 2 after 1 minute.

[0060] In some implementations, the formulation can be used as an antimicrobial coating, disinfectant, hand sanitizer, and / or soap.

[0061] In some embodiments, the formulation is applied to at least one surface of a fabric and used as a wet wipe.

[0062] In some implementations, the fabric is a nonwoven fabric.

[0063] In some implementations, the fabric is made from cellulose extracted from fruit peels and / or bacterial-yeast symbiotic cultures (SCOBY).

[0064] In some implementations, cellulose is extracted from durian peel.

[0065] The present invention also provides a method for disinfecting non-biological surfaces, including using the formulations of the present invention.

[0066] The present invention also provides a method for applying an antimicrobial coating to a non-biological surface, including using the formulations of the present invention.

[0067] The present invention also provides a method for disinfecting biological surfaces, including using the formulations of the present invention.

[0068] The present invention also provides a method for providing antimicrobial properties to textiles, including using the formulations of the present invention.

[0069] This invention also provides a method for preparing a formulation, comprising:

[0070] a) Mix cashew extract, iron granules and / or iron oxide granules with carbohydrates;

[0071] The cashew nut extract is present in a weight ratio of approximately 100:1 to approximately 1:200 to iron particles and / or iron oxide particles; and

[0072] The weight ratio of carbohydrates to cashew extract and iron particles and / or iron oxide particles is approximately 30:1 to approximately 1:300; and

[0073] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles.

[0074] In some embodiments, the method further includes a step following step (a) to adjust the pH of the natural ingredient formulation to approximately 4 to approximately 5.

[0075] In some embodiments, the method further includes a step of adding excipients after step (a), the excipients being selected from colorants, humectants, fragrances, stabilizers, penetrants, adhesion promoters, film-forming agents, transdyeing agents, surfactants, solvents, antioxidants, or combinations thereof.

[0076] In some embodiments, the method further includes a step following step (a) of diluting the formulation in an aqueous medium.

[0077] In some embodiments, the method further includes a step prior to step (a), namely, reacting cashew extract with an iron precursor to form cashew extract and iron particles and / or iron oxide particles. Attached Figure Description

[0078] Embodiments of the present invention will now be described with reference to the accompanying drawings and through non-limiting examples:

[0079] Figure 1 This is an illustrative schematic diagram of a cashew nut extract composition;

[0080] Figure 2 This is an illustrative schematic diagram of a cashew nut extract composition;

[0081] Figure 3 The degradation of Coomasie Brilliant Blue R dye after exposure to cashew nut extract composition is shown.

[0082] Figure 4 The degradation of Coomasie Brilliant Blue R dye after exposure to cashew nut extract composition is shown.

[0083] Figure 5 The results of OH radical measurements after exposure to the cashew extract composition are shown.

[0084] Figure 6 The results of O2 radical measurements are shown after 2 hours of exposure to the cashew extract composition.

[0085] Figure 7A-D shows a scanning electron microscope (SEM) image of iron particles and / or iron oxide particles incorporating cashew extract. Detailed Implementation

[0086] The inventors believe that formulations possessing antimicrobial (antibacterial and / or antiviral) properties are advantageous. Such formulations can be applied or used on object surfaces as disinfectants or applied or used on textiles. To this end, the inventors have found that extracts from natural products are particularly advantageous. In particular, the inventors have discovered that cashew nut extract has antimicrobial efficacy. When formulated according to the formulation disclosed in this application, the antimicrobial efficacy is synergistically improved. Food waste problems can also be reduced by utilizing and recycling food waste and transforming it into higher-value products.

[0087] Not wanting to be bound by theory, we believe cashew extract has the ability to kill viruses and bacteria through contact. When the extract is applied to a substrate, the compounds in the extract can kill viruses and bacteria on the substrate surface. It is hypothesized that the extract can capture microorganisms by mimicking the sites where they typically attach to human cells, and then eliminate them by disrupting the surface (viruses) and cell walls (bacteria). Studies have found that the extract can kill pathogens that cause influenza A, avian influenza, SARS, measles, pneumonia, the common cold, tuberculosis, herpes, MRSA, and gastroenteritis.

[0088] The antibacterial mechanism is believed to involve the binding of proteins on the bacterial cell membrane to phenolic compounds in the extract, thereby disrupting the structure and function of the bacterial cell. Further complexation with essential metal ions can also inhibit fibrin formation. In addition, cashew extract also possesses antiviral activity. It is thought that compounds in cashew extract can target different stages of viral replication. This includes the extracellular virus itself, the process of viral attachment to cells, the process of viral penetration into cells, viral replication within host cells, and the assembly of new viral particles, transport proteins, polysaccharides, and viral enzymes. In almost all of these stages, the complex permanently binds to proteins on the envelope or superenveloping membrane. These proteins may be specific viral enzymes required for viral replication or newly synthesized viral proteins involved in the generation of new viral particles.

[0089] Therefore, the inventors discovered that the antimicrobial efficacy of cashew nut extract is enhanced when coupled with iron particles and / or iron oxide particles. It is believed that the addition of iron particles and / or iron oxide particles provides a multi-layered defense mechanism against bacteria and viruses. Iron particles and / or iron oxide particles are active ingredients that generate reactive oxygen species (ROS). These active ingredients continuously generate ROS, diffusing free radicals, thereby killing various bacteria and viruses over a prolonged period.

[0090] Even more advantageously, natural polymers (such as carbohydrates) can kill microorganisms immediately upon contact. Furthermore, they help the active ingredients bind to the surface, forming a positively charged "electric fence," thus achieving long-term integrity and durability. For this reason, when used in combination with carbohydrates in specific proportions, it has been found that carbohydrates can prolong the residence time of free radicals generated by cashew extract and iron microparticles and / or iron oxide microparticles on the applied surface. This combination of sustained diffusion and acute contact mechanisms ensures highly effective antibacterial and antiviral properties.

[0091] For example, a dual defense system against bacteria and viruses can be provided by spraying the formulation onto a surface. After drying, a thin coating forms on the treated surface. As the first line of defense, free radicals steadily diffuse (approximately 1 mm) into the surrounding area, killing bacteria and viruses that do not approach the surface. This diffusion of free radicals can last for up to 3 months, providing long-lasting efficacy. As the second line of defense, any bacteria or virus that breaches the first line of defense and comes into direct contact with the surface will have their cell membranes physically torn apart, instantly killing the microorganism. The combined killing effect of sustained diffusion and acute contact ensures effective antibacterial and antiviral properties.

[0092] Therefore, the present invention provides a formulation comprising:

[0093] a) Cashew nut extract;

[0094] b) Iron particles and / or iron oxide particles; and

[0095] c) Carbohydrates;

[0096] The cashew nut extract is present in a weight ratio of approximately 100:1 to approximately 1:200 to iron particles and / or iron oxide particles; and

[0097] The weight ratio of carbohydrates (c) to cashew fruit extract and iron particles and / or iron oxide particles (a and b) is approximately 8:1 to approximately 1:300.

[0098] In some embodiments, the formulation includes:

[0099] a) Cashew nut extract;

[0100] b) Iron particles and / or iron oxide particles; and

[0101] c) Carbohydrates;

[0102] The cashew nut extract is present in a weight ratio of approximately 100:1 to approximately 1:200 to iron particles and / or iron oxide particles; and

[0103] The weight ratio of carbohydrates (c) to cashew fruit extract and iron particles and / or iron oxide particles (a and b) is approximately 30:1 to approximately 1:300.

[0104] In some embodiments, the formulation includes:

[0105] a) Cashew nut extract;

[0106] b) Iron particles and / or iron oxide particles; and

[0107] c) Carbohydrates;

[0108] The cashew nut extract is present in a weight ratio of approximately 100:1 to approximately 1:200 to iron particles and / or iron oxide particles; and

[0109] The weight ratio of carbohydrates (c) to cashew fruit extract and iron particles and / or iron oxide particles (a and b) is approximately 8:1 to approximately 1:300; and

[0110] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles.

[0111] In some embodiments, the formulation includes:

[0112] a) Cashew nut extract;

[0113] b) Iron particles and / or iron oxide particles; and

[0114] c) Carbohydrates;

[0115] The cashew nut extract is present in a weight ratio of approximately 100:1 to approximately 1:200 to iron particles and / or iron oxide particles; and

[0116] The weight ratio of carbohydrates (c) to cashew fruit extract and iron particles and / or iron oxide particles (a and b) is approximately 30:1 to approximately 1:300; and

[0117] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles.

[0118] In some embodiments, the formulation includes:

[0119] a) Cashew nut extract;

[0120] b) Iron particles and / or iron oxide particles; and

[0121] c) Carbohydrates;

[0122] The cashew nut extract is present in a weight ratio of approximately 100:1 to approximately 1:100 with iron particles and / or iron oxide particles; and

[0123] The weight ratio of carbohydrates (c) to cashew fruit extract and iron particles and / or iron oxide particles (a and b) is approximately 15:1 to approximately 15:14; and

[0124] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles.

[0125] In some embodiments, the formulation includes:

[0126] a) Cashew nut extract;

[0127] b) Iron particles and / or iron oxide particles; and

[0128] c) Carbohydrates;

[0129] The cashew nut extract is present in a weight ratio of approximately 100:1 to approximately 1:100 with iron particles and / or iron oxide particles; and

[0130] The weight ratio of carbohydrates (c) to cashew fruit extract and iron particles and / or iron oxide particles (a and b) is approximately 8:1 to approximately 1:1; and

[0131] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles.

[0132] Advantageously, this formulation does not rely on irritating chemicals that could damage the surface or the user's hands. Therefore, we use natural products whenever possible to achieve the antimicrobial effect.

[0133] Cashew extract

[0134] Cashews (Anacardium occidentale) are a widely consumed nut worldwide. The outer shell of this nut is reddish-brown and called the cashew husk. Because of its bitter taste, the cashew husk is usually removed and discarded during processing. Utilizing these waste materials to synthesize antimicrobial components has advantages because it is low-cost and environmentally friendly.

[0135] Cashew extract contains various polyphenols, including tannins. Tannins are water-soluble, reddish-brown molecules. It is generally believed that tannins, along with common phenolic compounds, can bind to bacteria, disrupt the integrity of bacterial cell membranes, and interfere with various intracellular functions, thus exerting an antimicrobial effect.

[0136] One hypothesis is that phenolic compounds alter cell wall rigidity due to hydrogen binding to enzymes or different interactions with the cell membrane, leading to loss of integrity and thus changes in various intracellular functions. This can cause irreversible damage to the cytoplasmic membrane and coagulation of cellular contents, and even inhibition of intracellular enzymes. For example, condensed phenylacetone-tannic acid can damage the cell membrane and even inactivate metabolism by binding to enzymes, while phenolic acids have been shown to disrupt membrane integrity by causing leakage of important intracellular components. Flavonoids can bind to soluble proteins and bacterial cell walls outside the cell, thereby promoting complex formation. Flavonoids may also affect protein and RNA synthesis by inhibiting energy metabolism and DNA synthesis. In Gram-positive bacteria, intracellular pH has been reported to change, and the energy (ATP) production system has been disrupted.

[0137] In some embodiments, the cashew extract comprises polyphenols or phenolic compounds, such as tannins, catechins, epicatechin, epigallocatechin, p-coumarin, gallic acid, or combinations thereof. These polyphenols possess strong antioxidant and free radical scavenging activities. The phenolic compounds can be in any desired percentage or proportion. The phenolic compounds used in this invention refer to compounds containing at least one aromatic ring and bearing a hydroxyl group (-OH).

[0138] In some embodiments, cashew extract comprises proteins, amino acids, sugars, carbohydrates, or combinations thereof.

[0139] In this application, the terms "polypeptide," "peptide," and "protein" are used interchangeably to refer to any polymer of amino acid residues (dipeptides or more peptides) linked by peptide bonds or modified peptide bonds, as well as their variants and synthetic analogs. Therefore, these terms apply to amino acid polymers in which one or more amino acid residues are synthetic non-naturally occurring amino acids (such as chemical analogs of the corresponding naturally occurring amino acids), as well as naturally occurring amino acid polymers. The polypeptides of this invention include, but are not limited to, naturally purified products, chemically synthesized products, and products produced from prokaryotic or eukaryotic hosts (e.g., including bacterial, yeast, higher plant, insect, and mammalian cells) through recombinant technology. The polypeptides of this invention may contain non-peptide components, such as carbohydrate groups. Carbohydrates and other non-peptide substituents may be added to the polypeptide by the cell producing the polypeptide and vary depending on the cell type. For recombinantly produced polypeptides, the nature and extent of modification depend largely on the post-translational modification capacity of the specific host cell and the modification signals present in the relevant polypeptide amino acid sequence. For example, glycosylation patterns vary between different types of host cells. Polypeptides are defined herein by their amino acid backbone structure; substituents such as carbohydrate groups are generally not described but may be present. Furthermore, the polypeptides of the present invention may also include initially modified methionine residues, in some cases as a result of host-mediated processes. Proteins may exist in monomeric or multimeric forms, such as dimers (homodimers or heterodimers) or trimers.

[0140] In this specification, the term "amino acid" is defined as having at least one primary, secondary, tertiary, or quaternary amino group and at least one acid group, wherein the acid group can be a carboxylic acid, sulfonic acid, or phosphonic acid, or a mixture thereof. The amino group can be "α", "β", "γ", ... to "Ω" relative to the acid group. The skeleton of an amino acid can be substituted by one or more groups selected from halogens, hydroxyl groups, guanidino groups, and heterocyclic groups. Therefore, the scope of the term "amino acid" also includes glycine, alanine, valine, leucine, isoleucine, methionine, proline, phenylalanine, tryptophan, serine, threonine, cysteine, tyrosine, asparagine, glutamine, insulin aspart, glutamine, lysine, arginine, histidine, taurine, betaine, N-methylalanine, etc. The (L) and (D) forms of these amino acids are also included within the scope of protection of this invention.

[0141] In some embodiments, the cashew extract includes:

[0142] a) Phenolic compounds selected from tannic acid, catechin, epicatechin, epigallocatechin, p-coumarin, gallic acid, or combinations thereof; and

[0143] b) Proteins, amino acids, sugars, carbohydrates, or combinations thereof.

[0144] In some embodiments, the weight ratio of the phenolic compound to the protein is from about 1:100 to about 100:1. In other embodiments, the weight ratio is from about 1:90 to about 100:1, from about 1:80 to about 100:1, from about 1:70 to about 100:1, from about 1:60 to about 100:1, from about 1:50 to about 100:1, from about 1:40 to about 100:1, from about 1:20 to about 100:1, from about 1:10 to about 100:1, from about 1:1 to about 100:1, from about 10:1 to about 100:1, from about 20:1 to about 100:1, from about 30:1 to about 100:1, from about 40:1 to about 100:1, from about 50:1 to about 100:1, from about 60:1 to about 100:1, or from about 70:1 to about 100:1.

[0145] In some embodiments, the weight ratio of the phenolic compound to the sugar is from about 1:100 to about 100:1. In other embodiments, the weight ratio is from about 1:90 to about 100:1, from about 1:80 to about 100:1, from about 1:70 to about 100:1, from about 1:60 to about 100:1, from about 1:50 to about 100:1, from about 1:40 to about 100:1, from about 1:20 to about 100:1, from about 1:10 to about 100:1, from about 1:1 to about 100:1, from about 10:1 to about 100:1, from about 20:1 to about 100:1, from about 30:1 to about 100:1, from about 40:1 to about 100:1, from about 50:1 to about 100:1, from about 60:1 to about 100:1, or from about 70:1 to about 100:1.

[0146] Cashew extract combined with iron and / or iron oxide particles

[0147] The inventors have discovered that combining cashew nut extract with iron particles and / or iron oxide particles can further enhance its antimicrobial effect. For example, the retention time of the extract on the surface can be further improved. The compounds in the extract of the contrast agent are also easily degraded, thus the antimicrobial effect declines rapidly. The study further found that when the contrast agent is coated on a porous film, the compounds in the contrast agent extract can only remain at the interface and cannot penetrate. Therefore, the antimicrobial effect is not durable.

[0148] The development of microbial infections and antimicrobial resistance has recently garnered attention, becoming one of the most critical issues facing public health and safety. Creating clean, antimicrobial surfaces with long-term stability and activity has immense application value, impacting almost every aspect of our daily lives, such as medical devices, hospital surfaces, textiles, packaging, appliances, marine antifouling, filters, and public surfaces. Inorganic antimicrobial materials, especially semiconductor antimicrobial materials, are less susceptible to chemical contamination and exhibit long-term stability. Some metals or metal oxides, such as silver, zinc oxide, and titanium oxide particles, have been used as antimicrobial components or antimicrobial surface coatings in various products. However, these materials also have limitations, such as heavy metal contamination / toxicity (for silver-based materials). As for ZnO and TiO2 materials, their antimicrobial efficiency is low due to their reliance on light irradiation, limiting their applications. Furthermore, the uncertainty of nanotoxicity is another issue with nanomaterials.

[0149] Therefore, the inventors have discovered that by adding iron particles and / or iron oxide particles, the antimicrobial efficacy can be further synergistically (or at least additively) enhanced. Advantageously, the inventors have found that iron-based antimicrobial materials are non-toxic but exhibit high activity against microorganisms, are very stable, and possess long-term activity. For example, iron-iron oxide compositions can be synthesized under non-organic solvent conditions by modifying iron powder (micrometer size) with carbohydrates, amino acids, food additives, or nutrients. For example, synthesis can be carried out using a fluidized bed reactor or an ultrasonic generator.

[0150] Iron powder has redox activity, reacting slowly with oxygen and moisture to form iron oxide and release hydrogen. Iron powder itself does not produce reactive oxygen species (ROS) and does not kill bacteria. Some iron cations may be released from the iron powder, but their concentration is very low and will not harm cells.

[0151] Iron particles can have a protective nanostructured shell covering the iron core. For example, the protective shell could be an iron oxide shell. This core-shell structure forms a unique interface between the iron core and the iron composite shell, thereby altering the potential of the iron core and changing the pathway of the redox reaction. Therefore, we believe that this self-corrosion process may also occur in Fe / Fe... e O3, Fe / Fe eOn O3 particles and / or combinations thereof. Electrons generated by iron corrosion can be transferred in an energy-efficient manner to the conduction band (CB) of iron oxide. Electrons in the CB can reduce oxygen and generate ROS. Iron particles can generate various ROS, including superoxide, singlet oxygen, and hydroxyl radicals. In other words, electrons are donated from iron to iron oxide (CB) and reduced to oxygen molecules in an energy-efficient manner, generating free radicals. The entire system is independent of external stimuli, the ROS generation process is controllable, and it has long-term stability. The ROS then kills bacteria and viruses upon contact. Although the ROS killing mechanism of this material is similar to that of photocatalytic materials such as ZnO and TiO2, iron / iron oxide particles are autocatalytic materials that do not rely on light irradiation to generate ROS. Iron particles sacrifice their iron nuclei to generate ROS. New materials designed based on this concept can play a key role as a non-toxic and safe antimicrobial technology, replacing organic disinfectants, preservatives, and antibiotics in multiple fields, particularly in controlling the spread of infectious diseases and antimicrobial resistance (AMR).

[0152] In this application, "particle" refers to micron-sized particles and / or nanon-sized particles. Micron-sized particles are particles with a size between 1 and 1000 μm. Nanoparticles are particles with a size between 1 nanometer and 1000 nanometers. Particles can be of any shape or form, such as spherical, rod-shaped, or asymmetrical.

[0153] In some embodiments, the iron particles and / or iron oxide particles are provided in powder form with a particle size of about 10 nanometers to 500 micrometers. The iron particles and / or iron oxide particles can be micrometer-sized particles. In other embodiments, the particle size is about 1 micrometer to about 450 micrometers, about 1 micrometer to about 400 micrometers, about 1 micrometer to about 350 micrometers, about 1 micrometer to about 300 micrometers, about 1 micrometer to about 250 micrometers, about 1 micrometer to about 200 micrometers, about 1 micrometer to about 150 micrometers, about 1 micrometer to about 100 micrometers, about 1 micrometer to about 90 micrometers, about 1 micrometer to about 80 micrometers, about 1 micrometer to about 70 micrometers, about 1 micrometer to about 60 micrometers, about 1 micrometer to about 50 micrometers, about 1 micrometer to about 50 micrometers, about 1 micrometer to about 40 micrometers, or about 10 micrometers to about 40 micrometers. The iron particles and / or iron oxide particles can be nanoscale particles. In other embodiments, the particle size is about 10 nm to about 900 nm, about 10 nm to about 800 nm, about 10 nm to about 700 nm, about 10 nm to about 600 nm, about 10 nm to about 500 nm, about 10 nm to about 400 nm, about 10 nm to about 300 nm, about 10 nm to about 200 nm, about 10 nm to about 100 nm, about 10 nm to about 80 nm, about 10 nm to about 60 nm, or about 10 nm to about 40 nm.

[0154] In some embodiments, iron particles are used. In other embodiments, iron oxide particles are used. In this application, the distribution of iron or iron oxide throughout the particles is uniform. In some embodiments, the iron particles and / or iron oxide particles are core-shell particles. For example, the core may be a pure iron core or an iron alloy core. The shell may be an iron oxide shell. In some embodiments, the iron particles and / or iron oxide particles are a single iron-iron oxide particle. In some embodiments, the iron-iron oxide composition comprises iron, iron(II) oxide, and iron(III) oxide. In some embodiments, the weight ratio of iron relative to the iron oxide-iron composition exceeds 90%. In other embodiments, the iron content relative to the iron oxide-iron composition exceeds 91% w / w, 92% w / w, 93% w / w, 94% w / w, 95% w / w, 96% w / w, or 97% w / w. In other embodiments, the proportion of iron relative to the iron-iron oxide composition is greater than 15% w / w, greater than 20% w / w, greater than 25% w / w, greater than 30% w / w, greater than 35% w / w, greater than 40% w / w, greater than 45% w / w, greater than 50% w / w, greater than 55% w / w, greater than 60% w / w, greater than 65% w / w, greater than 70% w / w, or greater than 75% w / w. In other embodiments, the proportion of iron oxide (II) and iron oxide (III) relative to the iron oxide-iron composition is less than 10% w / w. In other embodiments, the proportion of iron oxide (II) and iron oxide (III) relative to the iron oxide-iron composition is less than 9% w / w, less than 8% w / w, less than 7% w / w, less than 6% w / w, less than 5% w / w, less than 4% w / w, or less than 3% w / w. In other embodiments, the weight ratio of iron oxide (II) and iron oxide (III) relative to the iron oxide-iron composition is less than 45% w / w, less than 40% w / w, less than 35% w / w, less than 30% w / w, less than 25% w / w, less than 20% w / w, less than 15% w / w, less than 10% w / w%, or less than 5% w / w. For example, the relative weight ratio can be determined using energy-dispersive X-ray spectroscopy (EDX).

[0155] In some embodiments, the iron is elemental iron. In other embodiments, the iron(II) oxide is FeO. In other embodiments, the iron(II) oxide is Fe2O3. In other embodiments, the iron(II) oxide and iron(III) oxide are Fe3O4. In this respect, the iron-iron oxide composition can be a mixture of Fe, FeO, Fe2O3 and Fe3O4.

[0156] In some embodiments, the iron particles and / or iron oxide particles comprise elemental iron, FeO, Fe2O3, Fe3O4, or combinations thereof.

[0157] In some embodiments, the cashew extract is physically mixed with iron particles and / or iron oxide particles. In this regard, the components of the cashew extract can be at least partially incorporated into the iron particles and / or iron oxide particles by forming a shell enveloping them. Alternatively, the cashew extract can at least partially passivate the surface of the iron particles and / or iron oxide particles to form cashew iron particles. For example, the particles may have an iron core, which can be encased in a cashew extract shell. In some embodiments, the shell comprises phenolic compounds, amino acids, carbohydrates, or mixtures thereof. In some embodiments, the shell comprises amino acids. In some embodiments, the shell comprises carbohydrates. In some embodiments, the shell comprises phenolic compounds.

[0158] Advantageously, we found that the physical binding of cashew nut extract with iron particles and / or iron oxide particles can synergistically (or at least additively) enhance antimicrobial efficacy. Not wanting to be bound by theory, we believe that when compounds in the cashew nut extract passivate iron / iron oxide particles to form cashew iron particles, the aggregation and / or clumping of iron / iron oxide particles is reduced. Furthermore, with improved particle stability, we also found that when the particles are applied to surfaces, they can remain on the surface without rapid degradation. This contrasts sharply with cashew nut extract alone (which tends to degrade rapidly) or iron / iron oxide particles alone (which do not remain on the surface). Therefore, the residence time of the formulation on the surface is improved, and the antimicrobial efficacy is correspondingly enhanced.

[0159] In addition, when at least some phenolic compounds are adsorbed on the surface of iron / iron oxide particles, the particles are slightly protected from degradation, thus ensuring a longer-lasting antimicrobial effect.

[0160] In some embodiments, iron particles and / or iron oxide particles are at least partially passivated by cashew nut extract to form cashew iron particles. In some embodiments, iron oxide particles are at least partially passivated by phenolic compounds in the cashew nut extract. For this purpose, the cashew nut extract can be physically adsorbed onto the surface of the iron oxide particles through similar interactions. This improves the stability of the composition, thereby extending its shelf life.

[0161] In some embodiments, the iron oxide particles are at least partially passivated by sugars and / or carbohydrates in the cashew extract. In other embodiments, the iron particles and / or iron oxide particles also include carbohydrates. In some embodiments, the carbohydrate content relative to the iron-iron oxide composition is from about 2% w / w to about 6% w / w. In other embodiments, the carbohydrate content relative to the iron-iron oxide composition is from about 2% w / w to about 5% w / w, or from about 3% w / w to about 5% w / w. In other embodiments, the carbohydrate content relative to the iron-iron oxide composition is from about 20% w / w to about 60% w / w, from about 20% w / w to about 55% w / w, from about 20% w / w to about 50% w / w, from about 20% w / w to about 45% w / w, from about 20% w / w to about 40% w / w, from about 20% w / w to about 35% w / w, or from about 20% w / w to about 30% w / w. For example, the relative weight ratio can be determined using energy-dispersive X-ray spectroscopy (EDX).

[0162] Carbohydrates can be selected from monosaccharides, disaccharides, oligosaccharides, and polysaccharides. Examples of carbohydrates include, but are not limited to, glucose, galactose, fructose, xylose, sucrose, lactose, maltose, trihalomethanes, sorbitol, mannitol, maltodextrin, raffinose, stachyose, fructooligosaccharides, amylose, amylopectin, modified starch, glycogen, dextran, chitosan, glucosamine, alginate, ulmoides polysaccharide, gum arabic, gellan gum, cellulose, hemicellulose, ethylcellulose, methylcellulose, pectin, hydrocolloids, and combinations thereof.

[0163] In some embodiments, the iron oxide particles are at least partially passivated by amino acids from the cashew extract. In other embodiments, the iron particles and / or iron oxide particles further comprise amino acids. In some embodiments, the amino acids are present in a ratio of about 2% w / w to about 6% w / w relative to the iron-iron oxide composition. In other embodiments, the amino acids are present in a ratio of about 2% w / w to about 5% w / w, or about 3% w / w to about 5% w / w relative to the iron-iron oxide composition.

[0164] In some embodiments, the iron oxide particles are at least partially passivated by carboxylic acid groups or hydroxyl groups. In some embodiments, the carboxylic acid is selected from fatty acids, aromatic carboxylic acids, dicarboxylic acids, tricarboxylic acids, keto acids, α-hydroxy acids, divinyl ether fatty acids, phosphoric acid, polyphosphoric acid, tungstic acid, vanadate, molybdate, heteropolyacids, or combinations thereof. In some embodiments, the carboxylic acid is selected from benzoic acid, phosphoric acid, sulfuric acid, or combinations thereof.

[0165] In some embodiments, the volume or weight ratio of cashew extract to iron particles and / or iron oxide particles is from about 100:1 to about 1:200. In other embodiments, the ratio is approximately 100:1 to approximately 1:180, approximately 100:1 to approximately 1:160, approximately 100:1 to approximately 1:140, approximately 100:1 to approximately 1:120, approximately 100:1 to approximately 1:100, approximately 90:1 to approximately 1:90, 80:1 to approximately 1:80, 70:1 to approximately 1:70, 60:1 to approximately 1:60, 50:1 to approximately 1:50, 40:1 to approximately 1:40, 30:1 to approximately 1:30, 20:1 to approximately 1:20, 10:1 to approximately 1:10, or approximately 10:9, approximately 10:8, approximately 10:7, approximately 10:6, approximately 10:5, approximately 10:4, approximately 10:3, or approximately 10:2. In other embodiments, the weight ratio is about 90:1 to about 1:200, about 80:1 to about 1:200, about 70:1 to about 1:200, about 60:1 to about 1:200, about 50:1 to about 1:200, about 40:1 to about 1:200, about 30:1 to about 1:200, about 20:1 to about 1:200, about 10:1 to about 1:200, about 1:1 to about 1:200, about 90:1 to about 1:100, about 90:1 to about 1:90, about 80:1 to about 1:90, about 80:1 to about 1:80, about 70:1 to about 1:80, about 70: 1 to approximately 1:70, approximately 60:1 to approximately 1:70, approximately 60:1 to approximately 1:60, approximately 50:1 to approximately 1:60, approximately 50:1 to approximately 1:50, approximately 40:1 to approximately 1:50, approximately 40:1 to approximately 1:40, approximately 30:1 to approximately 1:40, approximately 30:1 to approximately 1:30, approximately 20:1 to approximately 1:30, approximately 20:1 to approximately 1:20, approximately 10:1 to approximately 1:20, approximately 10:1 to approximately 1:10, approximately 10:1 to approximately 1:8, approximately 10:1 to approximately 1:6, approximately 10:1 to approximately 1:4, approximately 10:1 to approximately 1:2, or approximately 10:1 to approximately 1:1.

[0166] Alternatively, iron particles and / or iron oxide particles can be chemically synthesized in situ in the presence of an iron precursor and cashew nut extract. In some embodiments, iron particles and / or iron oxide particles are formed in situ by mixing an iron precursor with cashew nut extract. As illustrated by examples, the iron particle precursor can be elemental iron powder, iron (III) salt, or a combination thereof.

[0167] In some embodiments, the anion of the iron(III) salt is selected from nitrates, chlorides, bromides, fluorides, iodides, sulfates, oxalates, perchlorates, phosphates, tetrafluoroborates, or combinations thereof. The iron(III) salt may be in its hydrated form.

[0168] Cashew extract can be incorporated into iron and / or iron oxide particles by forming them in situ. For example, cashew extract can be incorporated into the core or shell of iron and / or iron oxide particles. This improves the stability of the iron and / or iron oxide particles, preventing aggregation and clumping.

[0169] For example, cashew nut extract can react with iron powder (an iron precursor) to form iron particles and / or iron oxide particles. Advantageously, by reacting cashew nut extract with iron powder, an activated shell of iron oxide and cashew nut extract can be formed on a core of elemental iron or an iron alloy. The thickness of the iron oxide shell can be controlled by the reaction conditions and the ratio of cashew nut extract to iron powder. The formation of the cashew iron oxide shell provides stronger antimicrobial efficacy due to its longer retention time and larger contact surface area. Furthermore, studies have found that a core of elemental iron or an iron alloy is beneficial because it can regenerate the outer iron oxide shell when it is "used up."

[0170] In some embodiments, cashew extract is first reacted with iron powder (iron precursor), and then with an iron (III) salt (iron precursor) to form iron particles and / or iron oxide particles. This yields iron particles and / or iron oxide particles with a core comprising elemental iron and cashew extract, and a shell formed from an iron (III) salt. Alternatively, the iron particles and / or iron oxide particles may have an elemental iron core and a biphase (layered) shell comprising cashew extract and iron (III).

[0171] In other embodiments, cashew extract is first reacted with an iron (III) salt (iron precursor) and then with iron powder (iron precursor) to form iron particles and / or iron oxide particles. These iron particles and / or iron oxide particles may have an elemental iron core and a single-phase shell comprising a mixture of cashew extract and iron (III).

[0172] In some embodiments, cashew extract is reacted simultaneously with iron (III) salt (iron precursor) and iron powder (iron precursor) to form iron particles and / or iron oxide particles. This yields iron particles and / or iron oxide particles with a core comprising elemental iron and cashew extract, and a shell comprising cashew extract and iron (III). Advantageously, this allows for the formation of an activated shell of iron oxide and cashew extract on an activated elemental iron or iron alloy core. The thickness of the iron oxide shell can be controlled by the reaction conditions and the ratio of cashew extract to iron precursor. The formation of the cashew iron oxide shell results in stronger antimicrobial efficacy due to longer retention time and a larger contact surface area. Furthermore, studies have found that having a core of elemental iron or iron alloy is beneficial because it allows for the regeneration of the outer iron oxide shell when it is "used up."

[0173] Therefore, in some embodiments, the iron particles and / or iron oxide particles comprise iron, Fe3O4, and phenolic compounds, amino acids, carbohydrates, or mixtures thereof. In some embodiments, the proportion of iron to the iron-iron oxide composition exceeds 95% w / w, the proportion of Fe3O4 to the iron-iron oxide composition is less than 2% w / w, and the proportion of phenolic compounds, amino acids, carbohydrates, or mixtures thereof to the iron-iron oxide composition is from about 3% w / w to about 5% w / w.

[0174] In some embodiments, the iron particles and / or iron oxide particles comprise iron, Fe3O4, and carbohydrates. In some embodiments, the proportion of iron to the iron-iron oxide composition exceeds 95% w / w, the proportion of Fe3O4 to the iron-iron oxide composition is less than 2% w / w, and the proportion of carbohydrates to the iron-iron oxide composition is from about 3% w / w to about 5% w / w.

[0175] In some embodiments, the iron particles and / or iron oxide particles comprise iron, Fe3O4, and amino acids. In some embodiments, the proportion of iron relative to the iron-iron oxide composition is greater than 95% w / w, the proportion of Fe3O4 relative to the iron-iron oxide composition is less than 2% w / w, and the proportion of amino acids relative to the iron-iron oxide composition is from about 3% w / w to about 5% w / w. In some embodiments, the amino acids are selected from glycine, alanine, valine, leucine, isoleucine, methionine, proline, phenylalanine, tryptophan, serine, threonine, cysteine, tyrosine, asparagine, aspartic acid, glutamine, glutamic acid, lysine, arginine, histidine, taurine, betaine, N-methylalanine, or combinations thereof.

[0176] In other embodiments, the iron particles and / or iron oxide particles further comprise amino acids, carbohydrates, or mixtures thereof. In some embodiments, the proportion of amino acids, carbohydrates, or mixtures thereof relative to the iron-iron oxide composition is from about 2% w / w to about 6% w / w. In other embodiments, the proportion of amino acids, carbohydrates, or mixtures thereof relative to the iron-iron oxide composition is from about 2% w / w to about 5% w / w, or from about 3% w / w to about 5% w / w. For example, a mixture of methylcellulose and corn gluten can be used.

[0177] In some embodiments, the iron particles and / or iron oxide particles are core-shell particles, wherein the core contains iron and the shell contains amino acids. In other embodiments, the iron particles and / or iron oxide particles are multiple core-shell particles, wherein the core contains iron, the shell contains amino acids, and the interface between the core and the shell contains iron oxide. In some embodiments, the iron oxide is Fe3O4.

[0178] In some embodiments, the iron particles and / or iron oxide particles are core-shell particles, wherein the core contains iron and the shell contains iron and amino acids. In other embodiments, the iron particles and / or iron oxide particles are core-shell particles, wherein the core contains iron, the shell contains iron and amino acids, and the interface between the core and shell contains iron oxide. In some embodiments, the iron oxide is Fe3O4.

[0179] Advantageously, when iron particles are encapsulated in a shell, the iron core can be protected by the shell material containing amino acids and / or carbohydrates. This can further delay the formation of iron oxide, thereby delaying the generation of ROS until it is used in a face mask. This can prevent or reduce excessive oxidation of iron particles, thereby extending the shelf life of the face mask and / or allowing ROS to persist for a longer period. Furthermore, the amino acid and / or carbohydrate encapsulation material can alter the potential of the iron core, changing the redox reaction pathway. For example, the generated iron oxide can form an interface layer between the shell and the iron core. This allows for control over the generation and release of ROS. Thus, the shell on the iron particles can control the rate of iron oxidation, thereby continuously releasing ROS, sufficient to achieve antibacterial and / or antiviral effects. This improves its versatility and allows for more frequent washing. Another advantage is that, due to the use of natural compounds such as biopolymers to encapsulate the iron particles, the biodegradable properties of the biopolymers extend the shell decomposition time. For example, the shell may only decompose over time after multiple washes. This provides additional antimicrobial and / or antiviral durability, as the previously inaccessible internal iron core is now more readily accessible.

[0180] In some embodiments, the shell thickness is from about 5 nanometers to about 1 micrometer, or from about 50 nanometers to about 400 nanometers. In other embodiments, the thickness is from about 50 nanometers to 350 nanometers, from about 50 nanometers to about 300 nanometers, from about 100 nanometers to about 300 nanometers, from about 150 nanometers to about 300 nanometers, or from about 200 nanometers to about 300 nanometers.

[0181] The shell may also contain iron. In this regard, in some embodiments, the shell contains iron and amino acids, carbohydrates, or mixtures thereof. Advantageously, because the iron is closer to the particle surface, the iron present in the shell can "initiate" the process of oxidizing iron to iron oxide. In this sense, upon first use of the mask, ROS is suddenly released, thus providing protection to the user before sufficient moisture is provided to the iron core.

[0182] In some embodiments, the volume or weight ratio of cashew extract to iron precursor is from about 100:1 to about 1:100. In other embodiments, the ratio is from about 90:1 to about 1:90, 80:1 to about 1:80, 70:1 to about 1:70, 60:1 to about 1:60, about 50:1 to about 1:50, about 40:1 to about 1:40, about 30:1 to about 1:30, about 20:1 to about 1:20, about 10:1 to about 1:10, or about 10:9, about 10:8, about 10:7, about 10:6, about 10:5, about 10:4, about 10:3, or about 10:2. In other embodiments, the ratio is approximately 1:1 to approximately 1:100, approximately 1:10 to approximately 1:100, approximately 1:20 to approximately 1:100, approximately 1:30 to approximately 1:100, approximately 1:40 to approximately 1:100, approximately 1:50 to approximately 1:100, approximately 1:60 to approximately 1:100, approximately 1:70 to approximately 1:100, approximately 1:80 to approximately 1:100, or approximately 1:90 to approximately 1:100. In other embodiments, the ratio is approximately 100:1 to approximately 1:1, approximately 100:1 to approximately 10:1, approximately 100:1 to approximately 20:1, approximately 100:1 to approximately 30:1, approximately 100:1 to approximately 40:1, approximately 100:1 to approximately 50:1, approximately 100:1 to approximately 60:1, approximately 100:1 to approximately 70:1, approximately 100:1 to approximately 80:1, or approximately 100:1 to approximately 90:1.

[0183] In some embodiments, the weight ratio of cashew extract to the iron content in the iron precursor is from about 100:1 to about 1:100. In other embodiments, the ratio is from about 90:1 to about 1:90, 80:1 to about 1:80, 70:1 to about 1:70, 60:1 to about 1:60, about 50:1 to about 1:50, about 40:1 to about 1:40, about 30:1 to about 1:30, about 20:1 to about 1:20, about 10:1 to about 1:10, or about 10:9, about 10:8, about 10:7, about 10:6, about 10:5, about 10:4, about 10:3, or about 10:2. In other embodiments, the ratio is approximately 1:1 to approximately 1:100, approximately 1:10 to approximately 1:100, approximately 1:20 to approximately 1:100, approximately 1:30 to approximately 1:100, approximately 1:40 to approximately 1:100, approximately 1:50 to approximately 1:100, approximately 1:60 to approximately 1:100, approximately 1:70 to approximately 1:100, approximately 1:80 to approximately 1:100, or approximately 1:90 to approximately 1:100. In other embodiments, the ratio is approximately 100:1 to approximately 1:1, approximately 100:1 to approximately 10:1, approximately 100:1 to approximately 20:1, approximately 100:1 to approximately 30:1, approximately 100:1 to approximately 40:1, approximately 100:1 to approximately 50:1, approximately 100:1 to approximately 60:1, approximately 100:1 to approximately 70:1, approximately 100:1 to approximately 80:1, or approximately 100:1 to approximately 90:1.

[0184] In some implementations, the average particle size of the iron powder is about 10 nanometers to about 100 micrometers.

[0185] In some embodiments, the iron particles and / or iron oxide particles are iron oxide nanoparticles. Iron oxide nanoparticles can be synthesized via a plant-mediated green chemistry approach, i.e., using plant extracts as reducing agents and metal precursors under appropriate conditions. This process comprises three steps: (1) an activation phase, in which metal ions are reduced by phenolic compounds in the plant extract, subsequently nucleating the reduced metal atoms; (2) a growth phase, in which small NPs attach to form larger NPs (Ostwald ripening); and (3) a termination phase, during which the NPs develop their own shape. The phenolic compounds can also act as stabilizers, coating the surface of the nanoparticles.

[0186] Iron oxide nanoparticles can be supplied to cashew nut extract for physical mixing. Alternatively, in other embodiments, the iron oxide nanoparticles are chemically synthesized in situ in the presence of an iron precursor and cashew nut extract. The iron precursor may be an iron (III) salt.

[0187] Advantageously, activated iron oxide and cashew extract nanoparticles can be formed by reacting cashew extract with an iron precursor. In this method, the entire nanoparticle is activated. The size of the iron oxide nanoparticles can be controlled by the reaction conditions and the ratio of cashew extract to iron oxide precursor. Due to the increased surface area and surface energy, these nanoparticles exhibit higher activity, which is beneficial for achieving dissolution equilibrium.

[0188] In some embodiments, the iron oxide nanoparticles comprise elemental iron. In other embodiments, the iron oxide nanoparticles comprise an iron-cashew extract complex. In still other embodiments, the iron oxide nanoparticles comprise an iron-phenolic compound complex. For this purpose, the nanoparticles consist of a network or matrix of iron atoms and phenolic compounds (or at least carbon atoms).

[0189] Cashew nut extract can stabilize iron oxide nanoparticles. In some embodiments, the iron oxide nanoparticles are at least partially passivated by phenolic compounds. Therefore, unreacted cashew nut extract can be physically adsorbed onto the surface of the iron oxide nanoparticles through similar interactions. This improves the stability of the composition, thereby extending shelf life.

[0190] In some embodiments, the average particle size of the iron oxide nanoparticles is from about 1 nanometer to about 1000 nanometers. In other embodiments, the average particle size is from about 10 nanometers to about 50 nanometers.

[0191] Another example is that iron oxide nanoparticles can react with iron powder to form iron oxide particles.

[0192] In both physical mixing and chemical reaction methods of cashew extract compositions with iron particles and / or iron oxide particles, these methods may further include a step of adding an alkali. An alkali such as NaOH, KOH, or NH4OH may be added to the iron particles and / or iron oxide particles. For example, adding an alkali can promote the formation of iron oxide on the iron particles through an oxidation process.

[0193] Alkali can also be added to the iron oxide particle precursor. Since Fe(OH)2 and Fe(OH)3 can be formed under conditions >8 via the hydroxylation of ferrous and ferric ions, they can promote the formation of iron oxide particles.

[0194] An alkali can also be added to the cashew extract composition. For example, the oxidation of phenolic compounds can be controlled by the amount of NaOH added in the reaction. This promotes the formation of iron oxide particles and the adsorption of phenolic compounds, thereby passivating the surface. Furthermore, controlling the ionization of phenolic compounds in the cashew extract composition by controlling the pH value can also alter the antimicrobial efficacy.

[0195] For example, reaction reagents can be added in sequence:

[0196]

[0197] In some embodiments, the cashew extract is present in a weight ratio of about 0.5 wt% to about 8 wt% of the iron particles and / or iron oxide particles (a and b) relative to the formulation. In some embodiments, the weight ratio is about 1 wt% to about 8 wt%, about 1 wt% to about 7 wt%, about 1 wt% to about 6 wt%, about 1 wt% to about 5 wt%, or about 1 wt% to about 4 wt%.

[0198] A combination of cashew extract, iron granules and / or iron oxide granules with carbohydrates

[0199] Natural ingredient preparations contain carbohydrates.

[0200] The carbohydrates used in this application are biological macromolecules composed of carbon (C), hydrogen (H), and oxygen (O) atoms. Typically, the ratio of hydrogen to oxygen atoms is 2:1 (e.g., in water), therefore, their empirical formula is C. m (H2O) n (Where, m can be different from n). However, not all carbohydrates meet this precise stoichiometric definition (e.g., uric acid, deoxyglucose such as fucose). The term is synonymous with carbohydrates, which include sugars, starches, and cellulose. Carbohydrates are divided into four chemical groups: monosaccharides, disaccharides, oligosaccharides, and polysaccharides. Monosaccharides and disaccharides are the smallest (lowest molecular weight) carbohydrates and are often simply called sugars. Examples of carbohydrates or sugars include monosaccharides such as glucose, galactose, fructose, and xylose; disaccharides such as sucrose, lactose, maltose, and trihalomethanes; polyols such as sorbitol and mannitol; oligosaccharides such as maltodextrin, raffinose, stachyose, and fructooligosaccharides; and polysaccharides such as starches (amylose, amylopectin, and modified starches) and non-starch polysaccharides (glycogen, cellulose, hemicellulose, pectin, and hydrocolloids).

[0201] The weight ratio of carbohydrates (c) to cashew fruit extract and iron particles and / or iron oxide particles (a and b) is about 8:1 to about 1:300. In other embodiments, the weight ratio is about 8:1 to about 1:250, about 8:1 to about 1:200, about 8:1 to about 1:150, about 8:1 to about 1:100, about 8:1 to about 1:50, about 8:1 to about 1:10, about 8:1 to about 1:5, about 8:1 to about 1:1, about 6:1 to about 1:1, or about 5:1 to about 1:1. In other embodiments, the weight ratio is about 5:1, about 4:1, about 3:1, about 2:1, or about 1:1. In other embodiments, the weight ratio is approximately 30:1 to approximately 1:300, approximately 30:1 to approximately 1:280, approximately 30:1 to approximately 1:260, approximately 30:1 to approximately 1:240, approximately 30:1 to approximately 1:220, approximately 30:1 to approximately 1, approximately 30:1 to approximately 1:200, approximately 30:1 to approximately 1:180, approximately 30:1 to approximately 1:160, approximately 30:1 to approximately 1:140, approximately 30:1 to approximately 1:120, approximately 30:1 to approximately 1:100, approximately 30:1 to approximately 1:90, approximately 30:1 to approximately 1:80, approximately 3 0:1 to about 1:70, about 30:1 to about 1:60, about 30:1 to about 1:50, about 30:1 to about 1:40, about 30:1 to about 1:30, about 30:1 to about 1:25, about 30:1 to about 1:20, about 25:1 to about 1:30, about 20:1 to about 1:30, about 20:1 to about 1:20, about 15:1 to about 15:12, about 15:1 to about 15:10, about 15:1 to about 15:8, about 15:1 to about 15:6, about 15:1 to about 15:4, or about 15:1 to about 15:2.

[0202] Advantageously, when formulated in this ratio, carbohydrates can improve the residence time of free radicals generated by cashew nut extract and iron particles and / or iron oxide particles on the application surface. Furthermore, carbohydrates can also enhance the adhesion of cashew nut extract and iron particles and / or iron oxide particles to the application surface. This helps to further improve the antimicrobial effect of cashew nut extract and iron particles and / or iron oxide particles.

[0203] In some embodiments, the carbohydrate content relative to the formulation is from about 1 wt% to about 15 wt%. In other embodiments, the weight ratio is from about 2 wt% to about 15 wt%, from about 3 wt% to about 15 wt%, from about 4 wt% to about 15 wt%, from about 5 wt% to about 15 wt%, from about 5 wt% to about 14 wt%, from about 5 wt% to about 13 wt%, from about 5 wt% to about 12 wt%, from about 5 wt% to about 11 wt%, or from about 5 wt% to about 10 wt%.

[0204] In some embodiments, the carbohydrate is selected from chitosan, maltodextrin, raffinose, stachyose, fructooligosaccharides; polysaccharides such as starch (amylose, amylopectin, modified starch); and non-starch polysaccharides (glycogen, cellulose, hemicellulose, pectin, hydrocolloids). In other embodiments, the carbohydrate is chitosan.

[0205] Chitosan is a linear polysaccharide composed of randomly distributed β-(1→4)-linked D-glucosamine (deacetylated units) and N-acetyl-D-glucosamine (acetylated units). It can be produced by treating the chitinous shells of shrimp and other crustaceans with an alkaline substance such as sodium hydroxide.

[0206] In some embodiments, the molecular weight of chitosan is from about 2 kDa to about 500 kDa. In other embodiments, the molecular weight of chitosan is from about 2 kDa to about 400 kDa, from about 2 kDa to about 350 kDa, from about 2 kDa to about 300 kDa, from about 2 kDa to about 250 kDa, from about 2 kDa to about 200 kDa, from about 2 kDa to about 150 kDa, from about 2 kDa to about 100 kDa, from about 2 kDa to about 80 kDa, or from about 2 kDa to about 50 kDa. In other embodiments, the molecular weight of chitosan is about 10 kDa to about 300 kDa, about 10 kDa to about 250 kDa, about 10 kDa to about 240 kDa, about 10 kDa to about 230 kDa, about 10 kDa to about 220 kDa, about 10 kDa to about 210 kDa, about 10 kDa to about 200 kDa, about 20 kDa to about 200 kDa, about 30 kDa to about 200 kDa, about 40 kDa to about 200 kDa, and about... 50kDa to about 200kDa, about 50kDa to about 190kDa, about 60kDa to about 190kDa, about 70kDa to about 190kDa, about 80kDa to about 190kDa, about 90kDa to about 190kDa, about 100kDa to about 190kDa, about 100kDa to about 180kDa, about 100kDa to about 170kDa, about 100kDa to about 160kDa, about 100kDa to about 150kDa, or about 100kDa to about 140kDa.

[0207] In some embodiments, the viscosity of chitosan is from about 100 cP to about 1500 cP. In other embodiments, the viscosity of chitosan is from about 100 cP to about 1400 cP, from about 100 cP to about 1300 cP, from about 100 cP to about 1200 cP, from about 100 cP to about 1100 cP, from about 100 cP to about 1000 cP, from about 200 cP to about 1000 cP, from about 200 cP to about 900 cP, from about 300 cP to about 900 cP, from about 400 cP to about 900 cP, from about 400 cP to about 800 cP, from about 400 cP to about 700 cP, or from about 400 cP to about 600 cP.

[0208] Other auxiliary materials

[0209] In some implementations, the natural ingredient formulation also includes excipients.

[0210] "Excipients" are inactive substances that serve as carriers or media for active substances, including any and all solvents, dispersion media, inert diluents or other liquid carriers, dispersants or suspending agents, granulators, surfactants, disintegrants, isotonic agents, thickeners or emulsifiers, preservatives, binders, lubricants, buffers, oils, etc. Various excipients for formulating compositions and their known preparation techniques are disclosed in Garrettington: The Science and Practice of Pharmacy, 21st ed. (2006), Lippincott Williams & Wilkins. Any conventional excipient, unless it is incompatible with a substance or its derivatives, producing any adverse biological effects or otherwise interacting with any other component of the pharmaceutical composition in a harmful manner, should be within the scope of this invention.

[0211] Depending on the formulator's judgment, excipients such as colorants, coating agents, antioxidants or preservatives, and fragrances may also appear in the composition. Examples of excipients include colloidal silica, hydroxypropyl methylcellulose, vitamin A, vitamin E, vitamin C, retinyl palmitate, selenium, sodium metabisulfite, propyl gallate, cysteine, methionine, citric acid, sodium citrate, methylparaben, propylparaben, benzalkonium chloride hydrochloride, and lanolin.

[0212] This approach facilitates the transportation and storage of the composition. The shelf life of the composition can also be further extended.

[0213] In some embodiments, the excipients are selected from colorants, humectants, fragrances, stabilizers, penetrants, adhesion promoters, film-forming agents, transdyants, surfactants, solvents, antioxidants, or combinations thereof.

[0214] In some embodiments, the natural ingredient formulation further comprises a colorant selected from the terpene family. In other embodiments, the colorant is selected from β-carotene, astaxanthin, or combinations thereof. In other embodiments, the colorant is a component extracted from a natural source. The colorant may be carbon black, carmine, caramel, chlorophyll Cu complex, guaiac blue, henna, guanine, spirulina, chlorophyll (green algae), blue pea, or combinations thereof.

[0215] Beta-carotene is an organic, bright orange-red pigment found abundantly in fungi, plants, and fruits. It is a type of carotenoid, belonging to the terpenoid class of compounds, and is synthesized biochemically from eight isoprene units, thus having 40 carbon atoms. A distinctive feature of beta-carotene is the presence of beta-rings at both ends of its molecule.

[0216] Astaxanthin (3,3'-dihydroxy-β,β-carotene-4,4'-dione) is a common nutritional organic red pigment. The empirical formula for ATX is (C... 40 H 52 O4, produced by microorganisms such as fungi and algae, and also found in marine animals (such as salmon and crustaceans), gives them their distinctive red color. It is a ketone carotenoid. It belongs to the terpenoid class of compounds and consists of a five-carbon precursor, isopentenyl diphosphate, and dimethylallyl diphosphate. Astaxanthin is classified as a flavonoid, a type of carotenoid compound containing oxygen, hydroxyl groups, or ketones, such as zeaxanthin and canthaxanthin.

[0217] Advantageously, the colorant provides the user with a visual cue indicating that an antimicrobial coating has been applied to the surface. Because the active ingredients in the formulation can also degrade the dye, the colorant's strength decreases as the antimicrobial effect diminishes. This not only enhances user confidence but also provides an indication for recoating.

[0218] Even more advantageously, β-carotene and astaxanthin possess potent biological activities. For example, β-carotene exhibits significant antibacterial activity against P. syringae, P. carotovorum, and B. subtilis. For instance, ATX can significantly inhibit the growth of both Gram-positive and Gram-negative pathogens.

[0219] In some embodiments, the colorant is present in a weight ratio of about 0.01 wt% to about 10 wt% of the formulation. In other embodiments, the weight ratio is about 0.01 wt% to about 9 wt%, about 0.01 wt% to about 8 wt%, about 0.01 wt% to about 7 wt%, about 0.01 wt% to about 6 wt%, about 0.05 wt% to about 10 wt%, about 0.1 wt% to about 10 wt%, about 0.1 wt% to about 9 wt%, about 0.1 wt% to about 8 wt%, about 0.1 wt% to about 7 wt%, about 0.1 wt% to about 6 wt%, or about 0.1 wt% to about 5 wt%.

[0220] In some implementations, the natural ingredient formulation also includes a humectant. A humectant is a moisture-absorbing substance used to retain moisture. It is commonly used in moisturizers or emollients to protect, hydrate, and lubricate the skin. These functions are typically achieved by the sebum produced by healthy skin.

[0221] In some embodiments, the moisturizer is selected from glycerin, urea, pyrrolidine carboxylic acid, aloe vera, or combinations thereof. In other embodiments, the moisturizer is glycerin.

[0222] In some embodiments, the weight ratio of the humectant to the carbohydrate is from about 50:15 to about 150:15. In other embodiments, the weight ratio is from about 60:15 to about 150:15, from about 70:15 to about 150:15, from about 80:15 to about 150:15, from about 90:15 to about 150:15, from about 100:15 to about 150:15, from about 60:15 to about 100:15, from about 60:15 to about 90:15, from about 70:15 to about 90:15, or from about 70:15 to about 80:15.

[0223] In some embodiments, the humectant is present in a weight ratio of about 2 wt% to about 60 wt% relative to the formulation. In other embodiments, the weight ratio is about 2 wt% to about 55 wt%, about 2 wt% to about 50 wt%, about 2 wt% to about 45 wt%, about 2 wt% to about 40 wt%, about 2 wt% to about 35 wt%, about 2 wt% to about 30 wt%, about 2 wt% to about 25 wt%, about 2 wt% to about 20 wt%, about 2 wt% to about 18 wt%, about 2 wt% to about 16 wt%, about 2 wt% to about 14 wt%, about 2 wt% to about 12 wt%, about 2 wt% to about 10 wt%, about 2 wt% to about 9 wt%, about 2 wt% to about 8 wt%, about 2 wt% to about 7 wt%, about 2 wt% to about 6 wt%, or about 2 wt% to about 5 wt%.

[0224] In some embodiments, the natural ingredient preparation also includes a fragrance. The fragrance or perfume can be an aromatic essential oil or a mixture of aromatic compounds. The fragrance can be provided in the form of an essential oil or a mixture thereof. For example, the essential oil can be selected from lavender, peach, agar oil or agarwood, chili oil, angelica root oil, star anise oil, licorice, asafoetida root oil, balsam, basil oil, oyster oil, bergamot oil, black pepper oil, geranium oil, birch oil, camphor oil, hemp flower essential oil, calamus oil or calamus essential oil, coriander seed oil, cardamom seed oil, carrot seed oil, cedarwood oil (or cedarwood oil), chamomile oil, sweet flag oil, cinnamon oil, cistanche oil, citronella oil, lemongrass oil, sage oil, etc. Coconut oil, clove oil, coffee oil, coriander oil, mignonette oil (bible leaf oil), mignonette root oil, cranberry seed oil, kubebu oil, fennel seed oil / black seed oil, cypress oil, cedarwood oil, curry leaf oil, davana oil, dill oil, eucalyptus oil, fennel seed oil, fenugreek oil, fir oil, frankincense oil, galangal oil, glauca oil, garlic oil, geranium oil, ginger oil, St. John's wort oil, grapefruit oil, senna leaf oil, thyme oil, pecan oil, horseradish oil, hyssop, and adapalene. The following essential oils are grown in Holland: Salvia miltiorrhiza, jasmine oil, juniper berry oil, laurel oil, lavender oil, croton oil, lemon oil, lemongrass, lime, seaweed oil, linalool, citrus, marjoram, lemon balm oil, peppermint oil, moringa oil, alpine peppermint, wormwood oil, mustard oil, myrrh oil, myrtle, neem oil, neroli (bitter orange), nutmeg oil, orange oil, oregano oil, iris oil, parsley oil, patchouli oil, perilla oil, and palm oil. Peppermint oil, mandarin orange, pine oil, red cedarwood, Roman chamomile, rose oil, rosehip oil, rosemary oil, rosewood oil, sage oil, star anise oil, sandalwood oil, sassafras oil, peppermint oil, schisandra oil, peppermint oil, spike flower oil, spruce oil, mandarin orange, tarragon oil, tea tree oil, thyme oil, tsugae, turmeric, valerian, gentian, vetiver oil (cous oil), western red cedarwood, holly, yarrow oil, ylang-ylang, grapefruit oil, grapefruit seed oil, citrus peel oil, or combinations thereof.

[0225] In some embodiments, the fragrance is provided in an encapsulated form. In this case, the fragrance may be encapsulated in a tiny particle within a micron-sized shell made of a rigid or flexible polymer film. When the formulation is applied to a surface, this shell ruptures, releasing the fragrance. Alternatively, the shell may have a porous structure for controlled fragrance release. Examples of polymers used to form the shell include (but are not limited to) ethyl cellulose, polyvinyl alcohol, gelatin, sodium alginate, or combinations thereof. The advantage of this is that the formulation exhibits both durable antimicrobial activity and good olfactory reception.

[0226] In some embodiments, the weight ratio of flavoring to carbohydrates is from about 1:15 to about 60:15. In other embodiments, the weight ratio is from about 1:15 to about 55:15, from about 1:15 to about 50:15, from about 1:15 to about 45:15, from about 1:15 to about 40:15, from about 1:15 to about 35:15, from about 1:15 to about 30:15, from about 1:15 to about 25:15, from about 1:15 to about 20:15, from about 1:15 to about 18:15, from about 1:15 to about 16:15, from about 1:15 to about 14:15, from about 1:15 to about 12:15, from about 1:15 to about 10:15, from about 1:15 to about 8:15, from about 1:15 to about 6:15, from about 1:15 to about 4:15, or from about 1:15 to about 2:15.

[0227] In some embodiments, the flavoring is present in a weight ratio of about 0.01 wt% to about 40 wt% relative to the formulation. In other embodiments, the weight ratio is about 0.01 wt% to about 35 wt%, about 0.01 wt% to about 30 wt%, about 0.01 wt% to about 25 wt%, about 0.01 wt% to about 20 wt%, about 0.01 wt% to about 15 wt%, about 0.01 wt% to about 10 wt%, about 0.01 wt% to about 5 wt%, about 0.01 wt% to about 4 wt%, about 0.01 wt% to about 3 wt%, about 0.01 wt% to about 2 wt%, about 0.01 wt% to about 1 wt%, about 0.01 wt% to about 0.5 wt%, or about 0.01 wt% to about 0.1 wt%.

[0228] In some embodiments, the natural ingredient formulation also includes a penetrant. The role of the penetrant is to make the formulation permeable to microorganisms or more permeable. Penetrants may be selected from polyethyleneimine (PEI) and lactic acid.

[0229] Polyethyleneimine (PEI) is a polymer whose repeating unit consists of an amino group and two carbon aliphatic CH2CH2 spacer groups. Linear PEI contains all secondary amines, while branched polyethyleneimine contains primary, secondary, and tertiary amines. Fully branched dendritic polyethyleneimine can also be used, and this is also included within the scope of this invention. Copolymers and block copolymers containing PEI are also included within the scope of this invention. For example, poly(ethylene glycol)-block-polyethyleneimine can be used.

[0230] In some implementations, the molecular weight of PEI is from about 1,000 Da to 50,000 Da. The molecular weight can be measured by methods such as gel permeation chromatography (GPC). In other embodiments, the molecular weight is about 1,000 Da to about 50,000 Da, about 1,000 Da to about 45,000 Da, about 1,000 Da to about 40,000 Da, about 1,000 Da to about 35,000 Da, about 1,000 Da to about 30,000 Da, about 1,000 Da to about 25,000 Da, about 1,000 Da to about 20,000 Da, about 1,000 Da to about 15,000 Da, about 1,000 Da to about 10,000 Da, about 2,000 Da to about 10,000 Da, about 3,000 Da to about 10,000 Da, about 4,000 Da to about 10,000 Da, about 5,000 Da to about 10,000 Da, about 6,000 Da to about 10,000 Da, about 7,000 Da to about 10,000 Da, or about 8,000 Da to about 10,000 Da.

[0231] In some embodiments, the weight ratio of the penetrant to carbohydrates is from about 0.1:15 to about 40:15. In other embodiments, the weight ratio is from about 0.1:15 to about 35:15, from about 0.1:15 to about 30:15, from about 0.1:15 to about 25:15, from about 0.1:15 to about 20:15, from about 0.1:15 to about 15:15, from about 0.1:15 to about 10:15, from about 0.1:15 to about 5:15, from about 0.1:15 to about 4:15, from about 0.1:15 to about 3:15, from about 0.1:15 to about 2:15, or from about 0.5:15 to about 2:15.

[0232] In some embodiments, the weight ratio of the penetrant to the formulation is from about 0.01 wt% to about 25 wt%. In other embodiments, the weight ratio is from about 0.01 wt% to about 20 wt%, from about 0.01 wt% to about 15 wt%, from about 0.01 wt% to about 10 wt%, from about 0.01 wt% to about 8 wt%, from about 0.01 wt% to about 5 wt%, from about 0.01 wt% to about 4 wt%, from about 0.01 wt% to about 3 wt%, from about 0.01 wt% to about 2 wt%, from about 0.01 wt% to about 1 wt%, from about 0.01 wt% to about 0.5 wt%, or from about 0.01 wt% to about 0.1 wt%.

[0233] In some embodiments, the natural ingredient formulation also includes a surfactant. A surfactant is a molecule that spontaneously binds together to form vesicles. A surfactant is a compound that reduces the surface tension (or interfacial tension) between two liquids, between a gas and a liquid, or between a liquid and a solid. Surfactants can be used as detergents, wetting agents, emulsifiers, foaming agents, or dispersants, and generally have a hydrophilic head and a hydrophobic tail. Surfactants can be anionic, cationic, amphoteric, or nonionic. Surfactants can be selected from cocoamphoacetate, sodium lauryl sulfate, ammonium lauryl sulfate, sodium lauryl sulfate, taurine, isosulfate, olefin sulfonate, sulfosuccinate, hexadecyl ammonium chloride, stearyl ammonium chloride, sodium lauryliminodipropionate, disodium lauroylamphoacetate, hexadecyl or stearyl alcohol, polysorbate, etc. For example, disodium cocoamphoacetate (DSCADA) is a synthetic amphoteric surfactant. In some embodiments, the surfactant is decyl glucoside.

[0234] In some embodiments, the weight ratio of surfactant to carbohydrate is from about 5:15 to about 750:15. In other embodiments, the weight ratio is from about 5:15 to about 700:15, from about 5:15 to about 650:15, from about 5:15 to about 600:15, from about 5:15 to about 550:15, from about 5:15 to about 500:15, from about 5:15 to about 450:15, from about 5:15 to about 400:15, from about 5:15 to about 350:15, from about 5:15 to about 300:15, from about 5:15 to about 250:15, from about 5:15 to about 200:15, and from about 5:15... About 150:15, about 5:15 to about 250:15:15, about 5:15 to about 200:15, about 5:15 to about 150:15, about 5:15 to about 100:15, about 5:15 to about 50:15, about 5:15 to about 20:15, about 5:15 to about 18:15, about 5:15 to about 16:15, about 5:15 to about 14:15, about 5:15 to about 12:15, about 7:15 to about 12:15, or about 8:15 to about 12:15.

[0235] In some embodiments, the surfactant is present in a weight ratio of about 0.5 wt% to about 80 wt% of the formulation. In other embodiments, the weight ratio is about 0.5 wt% to about 70 wt%, about 0.5 wt% to about 60 wt%, about 0.5 wt% to about 50 wt%, about 0.5 wt% to about 40 wt%, about 0.5 wt% to about 30 wt%, about 0.5 wt% to about 20 wt%, about 0.5 wt% to about 10 wt%, about 0.5 wt% to about 5 wt%, about 0.5 wt% to about 2 wt%, about 0.5 wt% to about 1.5 wt%, about 0.5 wt% to about 1 wt%, about 0.5 wt% to about 0.9 wt%, or about 0.5 wt% to about 0.8 wt%.

[0236] In some embodiments, the natural ingredient formulation also includes a film-forming agent. A film-forming agent is a substance that, when applied to a surface, leaves a cohesive, continuous coating on the surface. Film-forming agents can be highly hydrophilic, thus providing a smooth feel. Examples of film-forming agents include polyvinylpyrrolidone (PVP), acrylates, acrylamide, and copolymers. In some embodiments, the formulation also includes a film-forming agent selected from (3-glycidoxypropyl)trimethoxysilane and / or gelatin.

[0237] In some embodiments, the film-forming agent is present in a weight ratio of about 0.01 wt% to about 10 wt% of the formulation. In other embodiments, the weight ratio is about 0.01 wt% to about 9 wt%, about 0.01 wt% to about 8 wt%, about 0.01 wt% to about 7 wt%, about 0.01 wt% to about 6 wt%, about 0.01 wt% to about 5 wt%, about 0.01 wt% to about 4 wt%, about 0.01 wt% to about 3 wt%, about 0.05 wt% to about 3 wt%, about 0.1 wt% to about 3 wt%, about 0.1 wt% to about 2 wt%, about 0.1 wt% to about 1 wt%, or about 0.5 wt% to about 1 wt%. For example, the amount of (3-glycidoxypropyl)trimethoxysilane and / or gelatin added may be about 0.5 wt% to about 1 wt%.

[0238] In some embodiments, the film-forming agent is present in a weight ratio of about 10 wt% to about 25 wt% of the formulation. In other embodiments, the weight ratio is about 12 wt% to about 25 wt%, about 14 wt% to about 25 wt%, about 16 wt% to about 25 wt%, about 18 wt% to about 25 wt%, or about 18 wt% to about 20 wt%.

[0239] Advantageously, the addition of a film-forming agent enhances the antimicrobial effect. The film-forming agent also improves the coating effect on metal surfaces. Thus, the formulation can be used as a long-term coating for up to 6 months.

[0240] In some embodiments, the natural ingredient formulation also includes a solvent. The solvent may be an aqueous medium. For example, the solvent may be water and / or ethyl acetate.

[0241] As used in this application, the terms "aqueous solution" or "aqueous medium" refer to an aqueous solvent or solvent system that is primarily composed of water. Such solvents can be polar or nonpolar, and / or protonated or aprotic. A solvent system refers to a combination of solvents that ultimately form a single phase. Both "solvent" and "solvent system" include, but are not limited to, pentane, cyclopentane, hexane, cyclohexane, benzene, toluene, dioxane, chloroform, diethyl ether, dichloromethane, tetrahydrofuran, ethyl acetate, acetone, dimethylformamide, acetonitrile, dimethyl sulfoxide, nitromethane, propylene carbonate, formic acid, butanol, isopropanol, propanol, ethanol, methanol, acetic acid, ethylene glycol, diethylene glycol, or water. Aqueous solvents or solvent systems may also include dissolved ions, salts, and molecules such as amino acids, proteins, sugars, and phospholipids. These salts can be, but are not limited to, sodium chloride, potassium chloride, ammonium acetate, magnesium acetate, magnesium chloride, magnesium sulfate, potassium acetate, potassium chloride, sodium acetate, sodium citrate, zinc chloride, sodium HEPES, calcium chloride, ferric nitrate, sodium bicarbonate, potassium dihydrogen phosphate, and sodium phosphate. Therefore, biological fluids, physiological solutions, and culture media also fall within this definition. In most embodiments, the aqueous solution is water. In some embodiments, the aqueous solution is deionized water. In some embodiments, the aqueous solution is Millipore water.

[0242] In some embodiments, the weight ratio of solvent to carbohydrate is from about 100:15 to about 3000:15. In other embodiments, the weight ratio is from about 100:15 to about 2500:15, from about 100:15 to about 2000:15, from about 100:15 to about 1500:15, from about 200:15 to about 1500:15, from about 300:15 to about 1500:15, from about 400:15 to about 1500:15, from about 500:15 to about 1500:15, from about 600:15 to about 1500:15, from about 700:15 to about 1500:15, or from about 700:15 to about 1200:15.

[0243] In some implementations, the natural ingredient formulation also includes antioxidants. For example, antioxidants may be oxalic acid, phytic acid, tannic acid, ascorbic acid, glutathione, lipoic acid, uric acid, carotene, panthenol, and α-tocopherol. Another example of an antioxidant is butylated hydroxytoluene.

[0244] Advantageously, we found that adding antioxidants helps to "preserve" or at least slow down the generation of iron particle free radicals. This extends the shelf life of the formulation without reducing its antimicrobial efficacy.

[0245] In some embodiments, the antioxidant is present in a weight ratio of about 0.01 wt% to about 5 wt% of the formulation. In other embodiments, the weight ratio is about 0.01 wt% to about 4 wt%, about 0.01 wt% to about 3 wt%, about 0.01 wt% to about 2 wt%, about 0.01 wt% to about 1 wt%, about 0.01 wt% to about 0.5 wt%, or about 0.01 wt% to about 0.1 wt%.

[0246] In some embodiments, the formulation also comprises cellulose. The cellulose may be in powder form with a particle size between 1 micrometer and 100 micrometers. Cellulose can be extracted from fruit peels and / or symbiotic cultures of bacteria and yeast (SCOBY). SCOBY is an ingredient used in the fermentation and production of kelp tea. In some embodiments, the cellulose is extracted from durian peel.

[0247] Adding powdered cellulose produces a sustainable filler powder that is easy to transport. Using cellulose derived from food waste reduces the energy required for transportation, thus reducing the carbon footprint. Using recyclable bottles and powder filler kits can reduce the number of plastic bottles by more than one million per year, enabling a shift towards fillable cleaning agents. Users can then simply add water to the filler powder to reconstitute the formulation into a liquid for use.

[0248] Furthermore, we found that the antimicrobial activity of cellulose extracted from durian peel and / or SCOBY was reduced by 0.3 log compared to cellulose from other sources. The addition of cellulose extracted from durian peel and / or SCOBY can synergistically (or at least additively) enhance the antimicrobial activity of the formulation.

[0249] In some embodiments, the weight ratio of cellulose to the formulation is from about 1 wt% to about 20 wt%. In other embodiments, the weight ratio is from about 1 wt% to about 15 wt%, from about 2 wt% to about 15 wt%, from about 4 wt% to about 15 wt%, from about 6 wt% to about 15 wt%, from about 8 wt% to about 15 wt%, from about 10 wt% to about 15 wt%, or from about 12 wt% to about 15 wt%.

[0250] The formulation may further contain maltodextrin. Maltodextrin can improve the flowability of filled powders.

[0251] In some embodiments, the weight ratio of maltodextrin to the formulation is from about 1 wt% to about 20 wt%. In other embodiments, the weight ratio is from about 1 wt% to about 15 wt%, from about 2 wt% to about 15 wt%, from about 4 wt% to about 15 wt%, from about 6 wt% to about 15 wt%, from about 8 wt% to about 15 wt%, from about 10 wt% to about 15 wt%, or from about 12 wt% to about 15 wt%.

[0252] Natural ingredient preparations

[0253] In some implementations, the pH of the natural ingredient formulation is approximately 4 to approximately 5. The pH can be adjusted by controlling the amount of acetic acid or any other pH buffer added. We have found that free radicals are more stable when the pH is within this range.

[0254] In some embodiments, the natural ingredient formulation reduces the log number of E. coli by about 2 after 5 minutes. In other embodiments, the natural ingredient formulation reduces its log number by at least about 3, about 4, or about 5.

[0255] In some embodiments, the natural ingredient formulation reduces the log number of E. coli by about 2 after 1 minute. In other embodiments, the natural ingredient formulation reduces its log number by at least about 3, about 4, or about 5.

[0256] In some embodiments, the natural ingredient formulation exhibits a logarithmic reduction of at least about 2 in its antibacterial rate against Staphylococcus aureus after 5 minutes. In other embodiments, the natural ingredient formulation exhibits a logarithmic reduction of at least about 3, about 4, or about 5.

[0257] In some embodiments, the natural ingredient formulation exhibits a logarithmic reduction of at least about 2 in its antibacterial rate against Staphylococcus aureus after 1 minute. In other embodiments, the natural ingredient formulation exhibits a logarithmic reduction of at least about 3, about 4, or about 5.

[0258] In some embodiments, the antiviral activity of the formulation is at least about 90%. In other embodiments, its antiviral activity is at least about 91%, about 92%, about 93%, about 94%, about 95%, about 96%, about 97%, about 98%, or about 99%. The formulation may have antiviral activity against viruses such as HCoV-229E virus, mouse hepatitis virus, and / or H3N2 virus.

[0259] This invention provides a method for using the formulation in the field of antimicrobial applications. The formulation disclosed in this application can be in any suitable form. For example, the formulation can be formulated as a gel, liquid, or sprayable form.

[0260] In some implementations, the natural ingredient formulation can be used as an antimicrobial coating, disinfectant, hand sanitizer, and / or soap. The formulation can also be used in detergents, aerosols, general cleaners, pest control solutions, and dishwashing liquids.

[0261] For example, to make it suitable for use as a spray, a viscosity reducer can be added to give the final product a viscosity of approximately 80,000 cPs to approximately 900,000 cPs. Because the iron particles are in the nanometer and / or micrometer range, they are able to disperse and suspend in the air for an appropriate period of time. When sprayed onto a surface, the non-polymerized iron particles are also uniformly dispersed on the surface.

[0262] This formulation can be used for air purification because it can break down harmful particulate matter, volatile organic compounds, and polyaromatics when they come into contact with treated surfaces. It can also be used to form coatings for air filters and filtration systems as an additional layer of protection.

[0263] This formulation can also be used in combination with resins or polymers (such as varnishes) to form an antimicrobial coating. It can also be used in combination with resins or polymers (such as varnishes) to form a non-fouling coating.

[0264] This formulation can also be used for wastewater treatment or management. For example, the composition can be added to wastewater to kill microorganisms and / or reduce aromatic pigments and impurities.

[0265] This formulation can also be used for water purification. In some embodiments, the formulation can reduce the dye coloring rate by at least 60%. In some embodiments, the formulation can reduce the Brilliant Blue R colorant by at least 60%.

[0266] In some embodiments, the formulation is applied at least to the surface of the fabric, serving as a wet wipe. The fabric is immersed in the formulation solution, thereby uniformly applying the formulation to the fabric. The fabric can be impregnated with the formulation.

[0267] In some embodiments, the weight ratio of the formulation to the fabric is from about 2:1 to about 10:1. In other embodiments, the weight ratio is from about 2:1 to about 9:1, from about 2:1 to about 8:1, from about 2:1 to about 7:1, from about 2:1 to about 6:1, or from about 2:1 to about 5:1.

[0268] In some embodiments, the fabric is a porous fabric. In other embodiments, the fabric is a nonwoven fabric. A nonwoven fabric is a fabric-like material made of short fibers and long fibers (continuous long fibers) bonded together by chemical, mechanical, thermal, or solvent treatment. Examples of nonwoven fabrics include polyester or polypropylene.

[0269] In some embodiments, the fabric contains cellulose extracted from fruit peel and / or a symbiotic culture of bacteria and yeast (SCOBY). SCOBY is an ingredient used in the fermentation and production of kelp tea. In some embodiments, the cellulose is extracted from durian peel. In some embodiments, the fabric also includes bamboo fiber.

[0270] Durian season generates a significant amount of durian peel waste. In the first half of 2018 alone, Singaporeans consumed 6 million durians, equivalent to approximately 12 million durians consumed annually. Durian peels comprise 60% of the entire durian fruit. These peels are discarded and incinerated as waste, potentially causing environmental problems if not properly handled. Approximately 14,000 tons of durian shells are incinerated each year. Studies show that durian peels contain 31-35% cellulose. This means that about one-third (30%) of the durian peel can be converted into cellulose. Another type of cellulose-rich food waste is scoby, a byproduct of kelp tea production. Scoby contains approximately 90% cellulose.

[0271] As described above, cellulose extracted from durian peel and / or SCOBY exhibits antimicrobial activity with a logarithmic reduction of approximately 0.3. Therefore, the present invention also provides a fabric comprising cellulose extracted from fruit peel and / or bacterial-yeast symbiotic culture (SCOBY).

[0272] This invention also provides a method for extracting cellulose from pericarps and / or scoby fruit. For example, the method may include freeze-drying, grinding and / or milling, cellulose extraction, and drying steps. Cellulose extraction can be achieved by dispersing the ground sample in a solution and then centrifuging to separate the cellulose. Alternatively, a bioreactor may be used.

[0273] The present invention also provides a method for disinfecting surfaces, including using the natural ingredient preparation of the present invention. For example, the natural ingredient preparation can be sprayed onto the surface.

[0274] In this application, "disinfection" refers to the act of cleaning something to kill microorganisms such as bacteria and / or viruses.

[0275] The present invention also provides a method for applying an antimicrobial coating to a surface, comprising using the natural ingredient formulation of the present invention. The antimicrobial coating can be used as a long-term coating, for example, for more than one month. For example, the natural ingredient formulation can be sprayed or brushed onto the surface.

[0276] In some implementations, when used as a surface disinfectant or coating, the natural ingredient formulation comprises:

[0277] a) Cashew nut extract;

[0278] b) Iron particles and / or iron oxide particles;

[0279] c) Carbohydrates; and

[0280] d) Penetrant;

[0281] The weight ratio of cashew extract to iron particles and / or iron oxide particles is approximately 100:1 to approximately 1:100.

[0282] The weight ratio of carbohydrates (c) to cashew extract and iron particles and / or iron oxide particles (a and b) is from about 15:1 to about 15:14.

[0283] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles; and

[0284] The weight ratio of the penetrant to the formulation is from 0.01 wt% to about 5 wt%.

[0285] In some implementations, when used as a surface disinfectant or coating, the natural ingredient formulation comprises:

[0286] a) Cashew nut extract;

[0287] b) Iron particles and / or iron oxide particles;

[0288] c) Carbohydrates; and

[0289] d) Penetrant;

[0290] The weight ratio of cashew extract to iron particles and / or iron oxide particles is approximately 100:1 to approximately 1:100.

[0291] The weight ratio of carbohydrates (c) to cashew extract and iron particles and / or iron oxide particles (a and b) is approximately 8:1 to approximately 1:1.

[0292] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles; and

[0293] The permeation enhancer is present in a weight ratio of 0.01 wt% to approximately 25 wt% relative to the formulation.

[0294] In some implementations, when used as a surface disinfectant or coating, the natural ingredient formulation comprises:

[0295] a) Cashew nut extract;

[0296] b) Iron particles and / or iron oxide particles;

[0297] c) Carbohydrates; and

[0298] d) Penetrant;

[0299] The weight ratio of cashew extract to iron particles and / or iron oxide particles is approximately 100:1 to approximately 1:200.

[0300] The weight ratio of carbohydrates (c) to cashew extract and iron particles and / or iron oxide particles (a and b) is approximately 8:1 to approximately 1:300.

[0301] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles; and

[0302] The permeation enhancer is present in a weight ratio of 0.01 wt% to approximately 25 wt% relative to the formulation.

[0303] In some implementations, when used as a surface disinfectant or coating, the natural ingredient formulation comprises:

[0304] a) Cashew nut extract;

[0305] b) Iron particles and / or iron oxide particles;

[0306] c) Chitosan; and

[0307] d)PEI;

[0308] The weight ratio of cashew extract to iron particles and / or iron oxide particles is approximately 100:1 to approximately 1:200.

[0309] The weight ratio of chitosan to cashew extract and iron particles and / or iron oxide particles is approximately 8:1 to approximately 1:300.

[0310] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles; and

[0311] The weight ratio of PEI to the formulation is from about 0.01 wt% to about 25 wt%.

[0312] In some implementations, when used as a surface disinfectant or coating, the natural ingredient formulation comprises:

[0313] a) Cashew nut extract;

[0314] b) Iron particles and / or iron oxide particles;

[0315] c) Carbohydrates;

[0316] d) Penetrants; and

[0317] e) Film-forming agents;

[0318] The weight ratio of cashew extract to iron particles and / or iron oxide particles is approximately 100:1 to approximately 1:200.

[0319] The weight ratio of carbohydrates to cashew extract and iron particles and / or iron oxide particles is approximately 8:1 to approximately 1:300.

[0320] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles;

[0321] The penetrant, by weight, is approximately 0.01 wt% to approximately 25 wt% of the formulation; and

[0322] The film-forming agent is present in a weight ratio of approximately 10 wt% to approximately 25 wt% relative to the formulation.

[0323] In some implementations, when used as a surface disinfectant or coating, the natural ingredient formulation comprises:

[0324] a) Cashew nut extract;

[0325] b) Iron particles and / or iron oxide particles;

[0326] c) Chitosan;

[0327] d) PEI; and

[0328] e) Gelatin;

[0329] The weight ratio of cashew extract to iron particles and / or iron oxide particles is approximately 100:1 to approximately 1:200.

[0330] The weight ratio of chitosan to cashew extract and iron particles and / or iron oxide particles is approximately 30:1 to approximately 1:300.

[0331] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles;

[0332] The weight ratio of PEI to the formulation is from approximately 0.01 wt% to approximately 5 wt%; and

[0333] The weight ratio of gelatin to the formulation is from about 0.01 wt% to about 10 wt%.

[0334] In some implementations, when used as a surface disinfectant or coating, the natural ingredient formulation comprises:

[0335] a) Cashew nut extract;

[0336] b) Iron particles and / or iron oxide particles;

[0337] c) Chitosan;

[0338] d)PEI;

[0339] e) Gelatin; and

[0340] f) 3-Glycidoxypropyltrimethoxysilane;

[0341] The weight ratio of cashew extract to iron particles and / or iron oxide particles is approximately 100:1 to approximately 1:200.

[0342] The weight ratio of chitosan to cashew extract and iron particles and / or iron oxide particles is approximately 30:1 to approximately 1:300.

[0343] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles;

[0344] The weight ratio of PEI to the formulation is from approximately 0.01 wt% to approximately 5 wt%; and

[0345] The combination of gelatin and 3-glycidoxypropyltrimethoxysilane is present in a weight ratio of about 0.01 wt% to about 10 wt% relative to the formulation.

[0346] In some implementations, when used as a surface disinfectant or coating, the natural ingredient formulation comprises:

[0347] a) Cashew nut extract;

[0348] b) Iron particles and / or iron oxide particles;

[0349] c) Chitosan;

[0350] d) PEI; and

[0351] e) 3-Glycidoxypropyltrimethoxysilane;

[0352] The weight ratio of cashew extract to iron particles and / or iron oxide particles is approximately 100:1 to approximately 1:200.

[0353] The weight ratio of chitosan to cashew extract and iron particles and / or iron oxide particles is approximately 8:1 to approximately 1:300.

[0354] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles;

[0355] The weight ratio of PEI to the formulation is from approximately 0.01 wt% to approximately 25 wt%; and

[0356] The weight ratio of 3-glycidoxypropyltrimethoxysilane to the formulation is from about 10 wt% to about 25 wt%.

[0357] The present invention also provides a method for disinfecting a user's hands, including using the natural ingredient preparation of the present invention. For example, the natural ingredient preparation may be in the form of a hand sanitizer or an ethanol / water spray.

[0358] In some implementations, when used as a hand sanitizer, the natural ingredient formulation contains:

[0359] a) Cashew nut extract;

[0360] b) Iron particles and / or iron oxide particles;

[0361] c) Carbohydrates; and

[0362] d) Moisturizer;

[0363] The weight ratio of cashew extract to iron particles and / or iron oxide particles is approximately 100:1 to approximately 1:200.

[0364] The weight ratio of carbohydrates to cashew extract and iron particles and / or iron oxide particles is approximately 30:1 to approximately 1:300.

[0365] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles; and

[0366] The humectant is present in a weight ratio of about 2 wt% to about 60 wt% relative to the formulation.

[0367] In some implementations, when used as a hand sanitizer, the natural ingredient formulation contains:

[0368] a) Cashew nut extract;

[0369] b) Iron particles and / or iron oxide particles;

[0370] c) Carbohydrates; and

[0371] d) Moisturizer;

[0372] The weight ratio of cashew extract to iron particles and / or iron oxide particles is approximately 100:1 to approximately 1:100.

[0373] The weight ratio of carbohydrates to cashew extract and iron particles and / or iron oxide particles is approximately 15:1 to approximately 15:14.

[0374] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles; and

[0375] The humectant is present in a weight ratio of about 2 wt% to about 60 wt% relative to the formulation.

[0376] In some implementations, when used as a hand sanitizer, the natural ingredient formulation contains:

[0377] a) Cashew nut extract;

[0378] b) Iron particles and / or iron oxide particles;

[0379] c) Chitosan; and

[0380] d) Glycerin;

[0381] The weight ratio of cashew extract to iron particles and / or iron oxide particles is approximately 100:1 to approximately 1:200.

[0382] The weight ratio of chitosan to cashew extract and iron particles and / or iron oxide particles is approximately 30:1 to approximately 1:300.

[0383] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles; and

[0384] The weight ratio of glycerol to the formulation is from about 2 wt% to about 60 wt%.

[0385] In some implementations, when used as a hand sanitizer, the natural ingredient formulation contains:

[0386] a) Cashew nut extract;

[0387] b) Iron particles and / or iron oxide particles;

[0388] c) Carbohydrates;

[0389] d) Moisturizers; and

[0390] e) Perfume;

[0391] The weight ratio of cashew extract to iron particles and / or iron oxide particles is approximately 100:1 to approximately 1:200.

[0392] The weight ratio of carbohydrates to cashew extract and iron particles and / or iron oxide particles is approximately 30:1 to approximately 1:300.

[0393] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles; and

[0394] The humectant is present in a weight ratio of about 2 wt% to about 60 wt% relative to the formulation.

[0395] In some implementations, when used as a hand sanitizer, the natural ingredient formulation contains:

[0396] a) Cashew nut extract;

[0397] b) Iron particles and / or iron oxide particles;

[0398] c) Chitosan;

[0399] d) Glycerin; and

[0400] e) Perfume;

[0401] The weight ratio of cashew extract to iron particles and / or iron oxide particles is approximately 100:1 to approximately 1:200.

[0402] The weight ratio of chitosan to cashew extract and iron particles and / or iron oxide particles is approximately 30:1 to approximately 1:300.

[0403] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles; and

[0404] The weight ratio of glycerol to the formulation is from about 2 wt% to about 60 wt%.

[0405] In some implementations, when used as a hand sanitizer, the natural ingredient formulation contains:

[0406] a) Cashew nut extract;

[0407] b) Iron particles and / or iron oxide particles;

[0408] c) Chitosan;

[0409] d) Glycerin;

[0410] e) Perfume; and

[0411] f) Surfactants;

[0412] The weight ratio of cashew extract to iron particles and / or iron oxide particles is approximately 100:1 to approximately 1:200.

[0413] The weight ratio of chitosan to cashew extract and iron particles and / or iron oxide particles is approximately 30:1 to approximately 1:300.

[0414] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles;

[0415] The glycerol content in the formulation is approximately 2% to approximately 60% by weight; and

[0416] The surfactant is present in a weight ratio of approximately 0.5 wt% to approximately 20 wt% relative to the formulation.

[0417] The present invention also provides a method for imparting antimicrobial properties to textiles, comprising using the natural ingredient formulation of the present invention. For example, the natural ingredient formulation can be used as soap to wash textiles, during which the natural ingredient formulation is transferred to the textiles, thereby imparting antimicrobial properties.

[0418] In some embodiments, the natural ingredient formulation comprises:

[0419] a) Cashew nut extract;

[0420] b) Iron particles and / or iron oxide particles;

[0421] c) Carbohydrates; and

[0422] d) Surfactants;

[0423] The weight ratio of cashew extract to iron particles and / or iron oxide particles is approximately 100:1 to approximately 1:200.

[0424] The weight ratio of carbohydrates to cashew extract and iron particles and / or iron oxide particles is approximately 30:1 to approximately 1:300.

[0425] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles; and

[0426] The surfactant is present in a weight ratio of approximately 0.5 wt% to approximately 80 wt% relative to the formulation.

[0427] In some embodiments, the natural ingredient formulation comprises:

[0428] a) Cashew nut extract;

[0429] b) Iron particles and / or iron oxide particles;

[0430] c) Carbohydrates; and

[0431] d) Surfactants;

[0432] The weight ratio of cashew extract to iron particles and / or iron oxide particles is approximately 100:1 to approximately 1:100.

[0433] The weight ratio of carbohydrates to cashew extract and iron particles and / or iron oxide particles is approximately 15:1 to approximately 15:14.

[0434] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles; and

[0435] The surfactant is present in a weight ratio of approximately 0.5 wt% to approximately 80 wt% relative to the formulation.

[0436] In some embodiments, the natural ingredient formulation comprises:

[0437] a) Cashew nut extract;

[0438] b) Iron particles and / or iron oxide particles;

[0439] c) Chitosan; and

[0440] d) Cocoamphoacetate;

[0441] The weight ratio of cashew extract to iron particles and / or iron oxide particles is approximately 100:1 to approximately 1:200.

[0442] The weight ratio of chitosan to cashew extract and iron particles and / or iron oxide particles is approximately 30:1 to approximately 1:300.

[0443] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles; and

[0444] The weight ratio of cocoamphoacetate to the formulation is from about 0.5 wt% to about 2 wt%.

[0445] The present invention also provides a method for cleaning non-biological surfaces, comprising contacting an agent with the non-biological surface.

[0446] In this application, "cleaning" refers to the act of making an object clean by means of removing dirt, marks, or stains.

[0447] As shown in this application, the formulation can also degrade colored compounds. Through this degradation, the color of the compound disappears due to the destruction of its aromaticity / conjugated system.

[0448] In some implementations, ROS can be generated in the dark. In other implementations, ROS can be generated without ultraviolet radiation. In still other implementations, the generated ROS is selected from ˙O2. − H2O2, ˙OH 1 O2, α-O, or combinations thereof.

[0449] In some implementations, when FeCl3 is used in the synthesis, Cl - The presence of anions also contributes to the generation of ROS. ROS can be Cl˙ and / or Cl2. - Another advantage of this approach is that it enhances the antimicrobial effect, particularly extending it to areas some distance from the coated surface. In this sense, an antimicrobial effect can be achieved without microorganisms coming into contact with the surface.

[0450] In some embodiments, ROS can be dispersed at a certain distance from the application area or surface. In other embodiments, this distance is from about 0.1 mm to about 10 cm. In still other embodiments, this distance is about 1 cm, 2 cm, 5 cm, 7 cm, or 10 cm.

[0451] Formulation of natural ingredient preparations

[0452] This invention also provides a method for preparing a natural ingredient preparation, comprising:

[0453] a) Mix cashew extract, iron granules and / or iron oxide granules with carbohydrates;

[0454] The cashew nut extract is present in a weight ratio of approximately 100:1 to approximately 1:200 to iron particles and / or iron oxide particles; and

[0455] The weight ratio of carbohydrates to cashew extract and iron particles and / or iron oxide particles is approximately 30:1 to approximately 1:300; and

[0456] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles.

[0457] In some embodiments, a method for preparing a natural ingredient formulation includes:

[0458] a) Mix cashew extract, iron granules and / or iron oxide granules with carbohydrates;

[0459] The cashew nut extract is present in a weight ratio of approximately 100:1 to approximately 1:100 with iron particles and / or iron oxide particles; and

[0460] The weight ratio of carbohydrates to cashew extract and iron particles and / or iron oxide particles is approximately 15:1 to approximately 15:14; and

[0461] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles.

[0462] In some embodiments, the method further includes a step after step (a) of adjusting the pH of the natural ingredient formulation to approximately 4 to approximately 5. The pH can be adjusted using acetic acid or any other pH buffer. Examples include, but are not limited to, citric acid, KH₂PO₄, N-cyclohexyl-2-aminoethanesulfonic acid (CHES), and borates.

[0463] In some embodiments, the method further includes a step of adding an excipient after step (a), the excipient being selected from colorants, humectants, fragrances, stabilizers, penetrants, adhesion promoters, transdyants, surfactants, solvents, antioxidants, or combinations thereof.

[0464] In some embodiments, the method further includes a step following step (a) of diluting the formulation in an aqueous medium.

[0465] In some embodiments, the method further includes a step of filtering the formulation after step (a).

[0466] As described above, cashew extract can be physically mixed with iron particles and / or iron oxide particles to form cashew extract passivated iron particles and / or iron oxide particles.

[0467] Therefore, in some embodiments, the mixing of cashew extract with iron particles and / or iron oxide particles is intended to passivate the iron oxide particles at least partially by the cashew extract.

[0468] Therefore, in some embodiments, a method for preparing a natural ingredient formulation includes:

[0469] i) Mix cashew extract with iron granules and / or iron oxide granules; and

[0470] a) Mix the mixture from (i) with carbohydrates;

[0471] The cashew nut extract is present in a weight ratio of approximately 100:1 to approximately 1:200 to iron particles and / or iron oxide particles; and

[0472] The weight ratio of carbohydrates to cashew extract and iron particles and / or iron oxide particles is approximately 30:1 to approximately 1:300.

[0473] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles.

[0474] Alternatively, iron particles and / or iron oxide particles can also be formed from iron precursors. For example, cashew extract and iron precursors can first undergo a chemical reaction to form iron particles and / or iron oxide particles incorporating cashew extract. Carbohydrates are then then mixed in.

[0475] Therefore, in some embodiments, the method further includes a step prior to step (a), namely, reacting cashew extract with an iron precursor to form cashew extract and iron particles and / or iron oxide particles.

[0476] Therefore, in some embodiments, a method for preparing a natural ingredient formulation includes:

[0477] i) React cashew extract with iron precursor to form cashew extract and iron particles and / or iron oxide particles.

[0478] a) Mix the cashew extract and iron particles and / or iron oxide particles obtained in step (i) with carbohydrates;

[0479] The cashew nut extract is present in a weight ratio of approximately 100:1 to approximately 1:200 to iron particles and / or iron oxide particles; and

[0480] The weight ratio of carbohydrates to cashew extract and iron particles and / or iron oxide particles is approximately 30:1 to approximately 1:300.

[0481] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles.

[0482] In other embodiments, a method for preparing a natural ingredient formulation includes:

[0483] i) React cashew extract with iron precursor to form cashew extract and iron particles and / or iron oxide particles.

[0484] a) Mix the cashew extract and iron particles and / or iron oxide particles obtained in step (i) with carbohydrates;

[0485] The weight ratio of cashew extract to iron oxide nanoparticles is approximately 100:1 to approximately 1:200; and

[0486] The weight ratio of carbohydrates to cashew extract and iron oxide nanoparticles is approximately 30:1 to approximately 1:300.

[0487] Cashew extract is at least partially incorporated into iron particles and / or iron oxide particles.

[0488] In some embodiments, the mixing in step (i) or step (a) is carried out for at least about 1 hour. In other embodiments, the mixing is carried out for at least about 2 hours, 4 hours, 6 hours, 12 hours, or 24 hours.

[0489] In some embodiments, the mixing in step (a) is carried out at room temperature. In other embodiments, the mixing is carried out at about 15°C to about 30°C or about 20°C to about 30°C.

[0490] Example

[0491] Cashew extract

[0492] - Appearance: Brown liquid

[0493] - Physicochemical properties: High free radical scavenging activity (antioxidant activity)

[0494] -Composition: A mixture of compounds including catechins, epicatechins, and tannins.

[0495] - Thermal stability up to 200℃

[0496] - Its solubility in water is 2850 g / L.

[0497] Example 1: Synthesis of iron-polyphenol composite nanoparticles (core is iron-cashew, shell is Fe(NO3)3·9H2O, core...) (Covered by a shell) (Complex A)

[0498] Cashew nut extract and 2 grams of iron powder were mixed and bubbled under nitrogen for 1 hour. During this process, the iron and cashew nut extract combine to form an iron-cashew compound. Separately, a 0.1 M Fe(NO3)3·9H2O solution was prepared and bubbled under nitrogen for 1 hour. The iron-cashew solution and the 0.5 M Fe(NO3)3·9H2O solution were then mixed at a 1:1 volume ratio. The reaction was continued under nitrogen protection for 24 hours, and the product was stored at 4°C. This resulted in the formation of iron-cashew nut core nanoparticles coated with a Fe(NO3)3·9H2O shell. Figure 1 )

[0499] Alternatively, mix 2 g of iron with 5 mL of cashew nut extract and incubate with stirring at room temperature for 1 hour. Then add 5 mL of 0.1 M FeCl3 and incubate the mixture with stirring at room temperature for 1 hour. Centrifuge the entire mixture at 5000 rpm and collect the black precipitate. Wash with water first, then with ethanol.

[0500] In the embodiments disclosed in this application, different types of iron salts, such as FeCl3, FeSO4, Fe2(SO4)3, Fe(NO3)3, and Fe(NO3)2, were tested.

[0501] Example 2: Synthesis of iron-polyphenol composite nanoparticles (core is iron, shell is cashew-Fe(NO3)3·9H2O, core...) (Covered by a shell) (Complex B)

[0502] 2 grams of iron powder in water were bubbled with nitrogen for 1 hour. Separately, 5 ml of cashew extract and 5 ml of 0.1 MFe(NO3)3·9H2O were mixed separately and bubbled with nitrogen for 1 hour to form a cashew-Fe(NO3)3·9H2O linker compound. Subsequently, the iron solution and the cashew-Fe(NO3)3·9H2O solution were mixed at a 1:1 volume ratio. The reaction was continued under nitrogen protection for 24 hours, and the product was stored at 4°C. This produced iron-core nanoparticles coated with a cashew-Fe(NO3)3·9H2O shell. Figure 2 )

[0503] Example 3: Synthesis of cashew nut extract-activated iron powder (complex C)

[0504] Fresh iron powder (4 g) was mixed with cashew nut extract (4 ml) and stirred at 80°C for 24 hours. After cooling to room temperature, the solid residue complex C was collected.

[0505] Example 4: Synthesis of cashew extract iron nanoparticles (complex D)

[0506] 16.23 g of the iron-cashew nanoparticles were added to 1 L of Milli-Q water to prepare a 0.1 M FeCl3 solution. Subsequently, the 0.1 M FeCl3 solution was added to the cashew extract at a 1:1 ratio. The formation of iron-cashew nanoparticles was characterized by the appearance of a black iron precipitate, which was collected by centrifugation at 7000 rpm. The iron-cashew nanoparticle powder was then frozen at -20°C and subsequently dried at -45°C under 10 Pa pressure for 24 hours using a freeze dryer.

[0507] Alternatively, a 0.1M FeCl3 solution can be incubated with cashew nut extract at a 1:1 ratio at room temperature for 1 hour. The entire mixture is then centrifuged at 5000 rpm, and the black precipitate is collected. The precipitate is washed first with water, then with ethanol.

[0508] Example 5: Synthesis of cashew nut extract iron nanoparticles (complex E)

[0509] 0.1M FeCl3 and cashew nut extract were mixed in a 1:1 ratio and incubated at room temperature for 1 hour. Then, 1M NaOH was added until the pH reached 11. The entire mixture was centrifuged at 5000 rpm, and the black precipitate was collected. The precipitate was washed first with water and then with ethanol.

[0510] Example 6: Iron-FeCl3 as the core, cashew nut as the shell (complex F)

[0511] Mix 2g of Fe with 5ml-20ml of 0.1M-0.5M FeCl3 and incubate with stirring at room temperature for 1 hour. Then add 5ml-20ml of cashew nut extract and incubate the mixture with stirring at room temperature for 1 hour. Centrifuge the entire mixture at 5000rpm and collect the precipitate. Wash with water first, then with ethanol.

[0512] Energy dispersive X-ray spectroscopy (EDX) analysis of iron particles and / or iron oxide particles

[0513] The EDX results shown below were obtained based on Example 6, using different amounts of iron precursors and cashew extract.

[0514]

[0515]

[0516]

[0517]

[0518]

[0519] Scanning electron microscopy (SEM) analysis

[0520] The SEM results of Example 6 are as follows: Figure 7A -D is shown.

[0521] X-ray photoelectron spectroscopy (XPS)

[0522] Analytical Electron Spectroscopy (ESCA) is a surface analysis technique that analyzes the elemental composition and chemical bond states of a sample surface. XPS analysis of iron-iron oxide complexes showed three peaks, indicating the presence of Fe 2p and Fe... 2+ and Fe 3+ Therefore, it is a mixed iron oxide system. 2+ It can react with oxygen to form FeO, with a binding energy of approximately 708.4 eV. 3+ It can react with oxygen to form FeOOH (binding energy 710 eV) or Fe2O3 (binding energy 709.8 eV). This indicates that cashew extract reacts with iron particles and / or iron oxide particles to form an iron-iron oxide complex. It has an iron core and a shell structure containing a mixture of iron oxides. The continuous electron conduction band generated on the shell by the iron oxides is the reason for the continuous generation of reactive oxygen species (ROS) (such as O2, H2O2, etc.), which is also the mechanism behind its antibacterial and antiviral properties.

[0523] Formulation 1A (Hand sanitizer / disinfectant)

[0524] Weigh chitosan and cashew iron granules in a beaker at a ratio of 15:1 to 15:14. Add 40-80 mL of glycerin. Add essential oil as needed. Add acetic acid to adjust the pH of the solution to 4-5, stirring constantly. Make up the volume with water.

[0525] Formulation 1B (Hand sanitizer / disinfectant)

[0526] Weigh chitosan and cashew iron granules in a beaker at a ratio of 8:1 to 1:1. Add 20 mL to 80 mL of glycerin. Add essential oil as needed. Add decyl glucoside (approximately 5 mL to 20 mL) to improve the solubility of the essential oil in the preparation.

[0527] Formulation 2A (Disinfectant)

[0528] Weigh chitosan and cashew iron granules in a ratio of 15:1 to 15:14 into a beaker. Weigh 0.5g-10g of PEI and add it to the beaker. While stirring continuously, add acetic acid to adjust the pH of the solution to 4-5. Make up the volume with water.

[0529] Formulation 2B (Disinfectant)

[0530] Weigh chitosan and cashew iron granules in a beaker at a ratio of 8:1 to 1:1. Weigh 0.5g-10g of PEI and add it to the beaker. Add essential oil as needed. Add decyl glucoside (approximately 5mL to 20mL) to improve the solubility of the essential oil in the preparation. While stirring continuously, add acetic acid to adjust the pH of the solution to 4-5.

[0531] Formulation 3 (Disinfectant and Long-Lasting Coating)

[0532] Weigh chitosan and cashew iron granules in a beaker at a ratio of 15:1 to 15:14. Weigh 0.5g-10g of PEI and add it to the beaker. Add 10mL-100mL of ethyl acetate. While stirring continuously, add acetic acid to adjust the pH of the solution to 4-5. Make up the volume with water.

[0533] Formulation 4A (Long-lasting coating)

[0534] Weigh chitosan and cashew iron granules in a beaker at a ratio of 15:1 to 15:14. Weigh 0.5g-10g of PEI and add it to the beaker. Then add 0.1%-1% gelatin and 0.1%-10% 3-glycidoxypropyltrimethoxysilane. While stirring continuously, add acetic acid to adjust the pH of the solution to 4-5. Make up the volume with water.

[0535] Formulation 5A (Soap for textiles)

[0536] Weigh chitosan and cashew iron granules into a beaker at a ratio of 30:1 to 1:300. Weigh 1-20g of cocoamphoacetate and add it to the beaker. While stirring continuously, add acetic acid to adjust the pH of the solution to 4-5. Make up the volume with water.

[0537] Formulation 5B (Soap for textiles)

[0538] Weigh chitosan and cashew iron granules in a beaker at a ratio of 8:1 to 1:1. Add 20-80 mL of glycerin. Add essential oil as needed. Add decyl glucoside (approximately 50 mL to approximately 400 mL) to improve the solubility of the essential oil in the preparation.

[0539] Antimicrobial effect of iron cashew nanoparticles against Staphylococcus aureus

[0540]

[0541] Antimicrobial effect of the formulation on bacterial cells

[0542] Formulation 1A: Hand sanitizer / disinfectant

[0543]

[0544] Formulation 2A: Disinfectant (short-term; ASTM E2315)

[0545]

[0546] Formulation 2A: Disinfectant (short-term; ASTM E2180)

[0547]

[0548] Quantitative suspension test for evaluating the bacterial activity of disinfectants

[0549]

[0550] This disinfectant meets the bactericidal efficacy requirements of EN 1276.

[0551] Formulation 3: Disinfectant (Interim)

[0552]

[0553] Formulation 3: Long-term coating

[0554]

[0555] Formulation 4A: Long-lasting coating (ASTM E2315)

[0556]

[0557] Formulation 4A: Long-lasting coating (ASTM E2180)

[0558]

[0559] Formulations 3 and 4B: Long-term coating (ASTM E2180)

[0560]

[0561]

[0562]

[0563]

[0564] Long-term coating (JIS Z 2801)

[0565] The test was conducted under typical laboratory conditions, including inoculating treated surfaces with a known concentration of Staphylococcus aureus and then assessing the reduction in bacterial count. To evaluate the lifetime of antimicrobial performance, the test was repeated every 30 days over a 180-day period.

[0566] The results showed that the inoculation was reduced by approximately 99.99% over a period of 180 days.

[0567] To simulate the natural wear and tear that occurs under everyday household chores, the glass slides used for antimicrobial testing were cleaned and disinfected daily with a multi-purpose cleaner and then dried.

[0568] Despite simulating routine cleaning and wiping procedures during the 6-month testing period, it can still be concluded that an average efficiency reduction of 99.99% was achieved.

[0569] ATP test for coating durability - wood flooring

[0570] Observe the results immediately after spraying on the wooden floor / Day 0

[0571] After spraying on the wood floor and allowing it to dry completely for approximately 8 hours, ATP readings were taken (using Kikkoman-LuciPacPens and Lumitester PD30). Lower ATP readings are better, as they indicate higher antibacterial activity of the solution.

[0572]

[0573] ATP test for coating durability - marble flooring

[0574] Results observed after spraying and wiping the marble floor with a damp cloth daily for 7 days.

[0575]

[0576] ATP test after spraying plastic - always wiped only once

[0577]

[0578] ATP test for long-term coating durability (Formulation 4A)

[0579]

[0580] Long-term coating durability ATP test (single application)

[0581]

[0582] Coomasie Brilliant Blue R dye degradation

[0583] 0.1 g of cashew seed coat nanoparticles were added to brilliant blue dye and incubated at room temperature for 15 minutes. The absorbance was then measured at 550 nm using a UV spectrophotometer. A blank control was used. Results are as follows: Figure 3 and Figure 4 As shown.

[0584] Absorbance at 550nm after 15 minutes (in any unit):

[0585] Blank space = 3.243

[0586] Comparative example (iron / iron oxide only) = 2.905

[0587] Example 1 using Fe(NO3)3 = 0.882

[0588] Example 4 using FeCl3 = 2.59

[0589] Example 6 using FeSO4 = 2.926

[0590] Example 6 using FeCl3 = 2.87

[0591] Example 1 using FeSO4 = 2.81

[0592] The results showed that, compared with the blank and control, the cashew extract composition (when containing iron / iron oxide particles) was able to degrade the dye.

[0593] Detection results for HCoV-229E virus

[0594] Test method: ISO 18184:2019 Determination of antiviral properties of textiles (cashew iron granules)

[0595]

[0596] Cashew iron granules have been shown to have antiviral properties.

[0597] Test method: EN 14476:2013+A2:2019 (Antiviral activity of the formulation against human coronavirus 229E)

[0598] The antiviral activity of the preparation was tested using human coronavirus 229e (P1 ATCC VR-740; host MRC5 ATCC CCL-171). Using a pipette, transfer 1 ml of 0.3 g / L bovine albumin to an appropriately sized container and mix well. Add 1 ml of the viral detection suspension to the container, carefully avoiding the upper part of the sidewalls. While mixing, add 8 ml of the preparation (20 g / L). Mix, immediately start a stopwatch, and place the container in a water bath maintained at the selected test temperature. The activity of the product should be determined within a 10-minute contact time. At the end of the 10-minute contact time, immediately mix, and using a pipette, transfer 0.5 ml of the detection mixture to 4.5 ml of ice-cold maintenance medium, then place in an ice bath. Prepare a series of 10-fold dilutions of this mixture (detection mixture + maintenance medium) over 30 minutes. Replace the pipette tip after each dilution to avoid viral carryover. After incubation, calculate the viral titer and determine the reduction in viral infectivity based on the difference in the logarithm of the viral titer. Infectivity is determined by the plaque assay.

[0599] Blank samples (without added formulation) showed no log reduction in viral activity. Samples containing the formulation, under clean conditions, showed a log reduction of at least 4 in human coronavirus 229e within 10 minutes.

[0600] Test method: ISO 21702:2019 Determination of antiviral activity of plastics and other nonporous surfaces (Formulation 2A)

[0601]

[0602]

[0603]

[0604] We also found that this formulation is effective against the H3N2 virus. This formulation does not inhibit the antiviral activity of cashew iron granules.

[0605] Disinfection of hard, non-porous surfaces contaminated with mouse hepatitis virus

[0606] Virus treatment using dry coated slides—preparing coated slides (treated) and uncoated slides (blank). Add 50 μl of mouse hepatitis virus (MHV) to the slides and allow them to dry completely (time: 50 min), then incubate at room temperature for 60 min. The treated and blank slides were then rehydrated with 2% DMEM medium, and the supernatant was collected for virus plaque assay. The experimental protocol followed the surface method of “US EPA copper method and prEN16777 / ASTM 2197”.

[0607] This experiment used the viral plaque assay with H2.35 cells. H2.35 cells were seeded into 24-well plates. MHV-treated supernatant was serially diluted 10-fold to 10⁶, and 100 μL of the diluted supernatant was added to the H2.35 cells. The plates were incubated for 1 hour to allow for virus binding, with shaking intervals of 15 minutes. The plates were then washed twice with 1X PBS, and 1.2% Avicel was added to each well. The plates were incubated for 3 days. Finally, the 1.2% Avicel was removed, and crystal violet was added to stain the countable plaques. Plaques were then counted using plaque-forming units per milliliter.

[0608] The average total viral titers of blank and processed slides after 60 minutes are shown below.

[0609]

[0610] Total log suppression: 2.11 PFU / ml

[0611] Relative reduction: 126.31

[0612] Relative reduction percentage: 99.21%

[0613] Maintenance of antiviral properties on treated surfaces after use

[0614] The plastic samples were treated with the formulation. An untreated plastic sample was used as a blank. Both the treated and untreated plastic samples were rubbed 300 times under an application load of 1 kg according to ASTM D4828. No visible scratches / defects were observed after wiping.

[0615] After wiping, the antiviral activity of the plastic samples was tested using human coronavirus 229e (P1 ATCC VR-740; host MRC5 ATCC CCL-171). Untreated plastic samples showed no log reduction in viral activity. Treated plastic samples showed a log reduction of at least 2.2 in human coronavirus 229e. The tests were performed according to ISO 21702:2019 (Test method for antiviral activity of plastics and other nonporous surfaces).

[0616] For comparison, cashew iron granules were individually and uniformly dispersed on plastic and rubbed 300 times under an application load of 1 kg according to ASTM D4828. No visible scratches / defects were observed after wiping. When the antiviral activity of the plastic samples was tested using human coronavirus 229e, the samples did not show a logarithmic reduction in viral activity.

[0617] Maintaining the antiviral properties of post-treated fabrics

[0618] The virus-killing performance of treated and untreated fabrics upon challenge with human coronavirus strain OC43 (Beta-coronavirus, ZeptoMetrix Corp. #0810024CF) was tested. Treatment and untreated fabric samples, after 1 minute, 5 minutes, 15 minutes, and 60 minutes of exposure to the virus, were evaluated. The tests were based on ISO 18184:2019(E).

[0619] Before washing, the infectivity of coronavirus OC43 was reduced by an average of 2.4 log10 (99.6%) after 60 minutes of exposure to the treated fabric, which can be classified as having good antiviral effect (≥2.0 log10).

[0620] After 15 hand washes, the infectivity of the treated fabric against coronavirus OC43 decreased by an average of 3.0 log10 (99.9%) after 60 minutes of exposure, which can be classified as having good antiviral effect (≥2.0 log10).

[0621] Untreated fabrics did not show any antiviral effect.

[0622] For comparison, cashew iron particles were individually and uniformly dispersed on fabrics, and the fabrics were evaluated after 1 minute, 5 minutes, 15 minutes, and 60 minutes of exposure to the virus, both before washing and after 15 hand washes. The test was based on ISO 18184:2019(E).

[0623] Before washing, fabrics treated with cashew iron granules alone showed an average reduction of 2.4 log10 (99.6%) in infectivity of coronavirus OC43 after 60 minutes of exposure, which can be classified as having good antiviral effect (≥2.0 log10).

[0624] After 15 hand washes, fabrics treated with cashew iron granules alone showed an average reduction of approximately 2 log10 (99.0%) in infectivity of coronavirus OC43 after 60 minutes of exposure, which can be classified as having good antiviral effects (≥2.0 log10).

[0625] Application of formulations in woven fabrics

[0626] Fabric samples were treated with a formulation. Untreated samples were used as blanks. Treated and untreated samples were rubbed 15,000 and 30,000 times respectively, according to ISO 12947 Part 2-2016 (Martindale abrasion tester). No visible scratches / defects were observed after wiping.

[0627] Formulation used as a long-term coating

[0628] The formulation was applied to various surfaces, including plastics, metals, and painted surfaces. The formulation passed tests for intercalation corrosion (ASTM D1193), total immersion corrosion (ASTM F 483), low-embrittlement cadmium board (ASTM F 1111), hydrogen embrittlement (ASTM F 519), flash point (ASTM D 56), effects on plastics (ASTM F 484), effects on painted surfaces (ASTM F 502), and effects on unpainted surfaces (ASTM F 485). During accelerated storage stability tests at both high and low temperatures, the samples showed no signs of stratification, separation, solidification, or crystallization.

[0629] Antibacterial activity of cellulose extracted from durian peel

[0630] Using ASTM E 2315 standard, with 10 8 A 1 mL suspension of 0.6 g of wet durian cellulose powder was incubated for 10 minutes, followed by serial dilution and counting on Mueller-Hinton agar. The 0.6 g wet weight durian cellulose showed a 0.3-log reduction in Staphylococcus aureus after 10 minutes.

[0631]

[0632] Spray drying of formulations using maltodextrin and durian cellulose as wall materials

[0633] The formulation was mixed with 1-15% maltodextrin and 1-15% durian cellulose using a mini spray dryer (Buchi B-290, Switzerland). The inlet temperature was 120-170°C, and the outlet temperature was 95-105°C. The formulation containing durian cellulose imparted an additional 0.1-1 log reduction in antimicrobial activity to the resulting spray-dried powder.

[0634] Analysis of ·OH levels produced by cashew nut particles in water using a hydroxyphenyl fluorescein (HPF) probe.

[0635] Example 1 using Fe(NO3)3 and Example 4 using FeCl3 were used as samples.

[0636] Add 0.01 g of sample to a 1.5 mL centrifuge tube. Add 1 mL of 10 μM HPF test solution to each sample. Mix the solution thoroughly by vortexing and store in the dark at room temperature. At a certain time point, centrifuge the solution (16800 rpm × 5 min) and transfer 100 μL of the solution to a black 96-well microplate for fluorescence detection. Collect the fluorescence at 490 / 515 nm using a microplate reader.

[0637] FeNO3-cashew (Example 1) releases ·OH radicals as ROS after 2 hours in the dark. FeCl3-cashew (Usage Method 1) does not release ·OH radicals. Figure 5 ).

[0638] The level of ·O2 free radicals generated by cashew nuts was determined using nitroblue tetrazolium (NBT).

[0639] Example 1 using Fe(NO3)3 and Example 4 using FeCl3 were used as samples.

[0640] Add 0.2g of iron-rich cashew granules to 10mL of 1000 mg·L⁻¹ −1 NBT was placed in water and stored in the dark. At a certain time point, the absorption spectrum of NBT was measured using a UV-Vis-NIR spectrophotometer. The absorption peak of NBT continued to decrease after 2 hours, indicating that FeCl3-cashew continuously generates ·O2 free radicals and reacts with NBT. Figure 6 ).

[0641] Comparative examples were prepared in a similar manner. The absorbance values ​​of NBT did not change over a 2-hour time interval.

[0642] It should be understood that many further modifications and arrangements of the various aspects of the described embodiments are possible. Therefore, the described aspects are intended to ensure that all such changes, modifications, and variations fall within the spirit and scope of the appended claims.

[0643] In this specification and the following claims, unless the context otherwise requires, the word “comprising” and its variations “including” and “containing” shall be understood to include the said integer or step or group of integers or steps, without excluding any other integer or step or group of integers or steps.

[0644] In this specification and the following claims, unless the context otherwise requires, the phrase "consistently of..." and its variation "consistently made of..." should be understood as meaning that the stated element is an essential element of the invention. This phrase allows for the presence of other unlisted elements that do not substantially affect the features of the invention, but excludes other unlisted elements that would affect the fundamental and novel features of the defined method.

[0645] References to any existing publications (or information obtained from them) or to any known matters in this specification shall not be construed as an admission or endorsement or recommendation of any kind that the existing publications (or information obtained from them) or known matters constitute part of the general knowledge in the field covered by this specification.

Claims

1. A formulation comprising: a) Cashew nut extract; b) Iron particles and / or iron oxide particles; as well as c) Chitosan; The cashew nut extract, in weight ratio to iron particles and / or iron oxide particles, is 10:1 to 1:10; and The weight ratio of chitosan (c) to cashew nut extract and iron particles and / or iron oxide particles (a and b) is 8:1 to 1:10; and Cashew extract includes a mixture of compounds of catechin, epicatechin, and tannic acid, and cashew extract is at least partially incorporated into the shells of iron particles and / or iron oxide particles. Iron particles and / or iron oxide particles are at least partially passivated by phenolic compounds from cashew extract; Iron particles and / or iron oxide particles are complexes consisting of an iron core and an outer layer of iron oxide adsorbed with phenolic compounds.

2. The formulation according to claim 1, wherein, The weight ratio of chitosan (c) to cashew extract and iron particles and / or iron oxide particles (a and b) is 8:1 to 1:

1.

3. The formulation according to claim 1 or 2, wherein, The weight ratio of chitosan to the formulation is 1 wt% to 15 wt%.

4. The formulation according to claim 3, wherein, Cashew extract and iron particles and / or iron oxide particles (a and b) are present in a weight ratio of 0.5 wt% to 8 wt% relative to the formulation.

5. The formulation according to claim 4, wherein, The pH value of the formulation is 4 to 5.

6. The formulation according to claim 5, wherein, The formulation also includes excipients selected from colorants, humectants, fragrances, stabilizers, penetrants, adhesion promoters, film-forming agents, transdyeing agents, surfactants, solvents, antioxidants, or combinations thereof.

7. The formulation according to claim 6, wherein, The formulation also contains a colorant selected from β-carotene, astaxanthin, or a combination thereof.

8. The formulation according to claim 7, wherein, The colorant is present in a weight ratio of 0.01 wt% to 10 wt% relative to the formulation.

9. The formulation according to claim 8, wherein, The formulation also contains a humectant selected from glycerin, urea, pyrrolidine carboxylic acid, aloe vera, or a combination thereof.

10. The formulation according to claim 9, wherein, The humectant is present in a weight ratio of 2% to 60% relative to the formulation.

11. The formulation according to claim 10, wherein, The formulation also includes a perfume containing essential oils.

12. The formulation according to claim 11, wherein, The perfume is present in a weight ratio of 0.01 wt% to 40 wt% relative to the formulation.

13. The formulation according to claim 12, wherein, The formulation also contains a penetrant selected from polyethyleneimine (PEI), lactic acid, or a combination thereof.

14. The formulation according to claim 13, wherein, The weight ratio of the penetrant to the formulation is from 0.01 wt% to 25 wt%.

15. The formulation according to claim 14, wherein, The formulation also contains a surfactant selected from cocoamphoacetate, taurine, isosulfate, olefin sulfonate, sulfosuccinate, sodium lauryliminodipropionate, disodium lauroamphodiacetate, and polysorbate.

16. The formulation according to claim 14, wherein, The formulation also contains a surfactant, namely decyl glucoside.

17. The formulation according to claim 16, wherein, The surfactant accounts for 0.5% to 80% of the weight of the formulation.

18. The formulation according to claim 17, wherein, The formulation also includes a film-forming agent selected from (3-glycidoxypropyl)trimethoxysilane and / or gelatin.

19. The formulation according to claim 18, wherein, The film-forming agent is present in a weight ratio of 10 wt% to 25 wt% relative to the formulation.

20. The formulation according to claim 19, wherein, The formulation also includes a solvent selected from water, ethyl acetate, or a combination thereof.

21. The formulation according to claim 20, wherein, The formulation also contains powdered cellulose.

22. The formulation according to claim 21, wherein, The powdered cellulose is present in a weight ratio of 1 wt% to 20 wt% relative to the formulation.

23. The formulation according to claim 22, wherein, Powdered cellulose is extracted from fruit peel and / or symbiotic culture of microorganism PISG-CN2300882 and yeast (SCOBY).

24. The formulation according to claim 23, wherein, The formulation also contains maltodextrin.

25. The formulation according to claim 24, wherein, Cashew extract also contains proteins, amino acids, sugars, or combinations thereof.

26. The formulation according to claim 25, wherein, Iron particles and / or iron oxide particles are at least partially passivated by proteins, amino acids, sugars or combinations thereof.

27. The formulation according to claim 26, wherein, The formulation reduced the log number of E. coli by at least 2 after 5 minutes.

28. The formulation according to claim 27, wherein, The formulation reduced the log number of E. coli by at least 2 after 1 minute.

29. The formulation according to claim 28, wherein, This preparation reduced the number of Staphylococcus aureus by at least 2 after 5 minutes.

30. The formulation according to claim 29, wherein, This preparation reduced the number of Staphylococcus aureus by at least 2 after 1 minute.

31. The formulation according to claim 30, wherein, The antiviral activity of this preparation is at least 90%.

32. The formulation according to claim 31, wherein, This formulation is used as an antimicrobial coating, disinfectant, hand sanitizer, and / or soap.

33. The formulation according to claim 32, wherein, The formulation is applied to at least one surface of fabric PISG-CN2300883 and used as a wet wipe.

34. The formulation according to claim 33, wherein, The fabric is a non-woven fabric.

35. The formulation according to claim 33 or 34, wherein, The fabric is made from cellulose extracted from fruit peels and / or symbiotic cultures of bacteria and yeast (SCOBY).

36. The formulation according to claim 35, wherein, The peel is durian peel.

37. A method for disinfecting non-biological surfaces, comprising using the preparation of any one of claims 1-36.

38. A method of applying an antimicrobial coating to a non-biological surface, comprising using the formulation of any one of claims 1-36.

39. A method of providing antimicrobial function to textiles, comprising using the formulation of any one of claims 1-36.

40. A method for preparing a formulation according to any one of claims 1-36, comprising: a) Mix cashew extract, iron particles and / or iron oxide particles with chitosan.

41. The method of claim 40, further comprising a step after step (a) of adjusting the pH of the formulation to 4 to 5.

42. The method according to claim 40 or 41, further comprising the step of adding an excipient after step (a), the excipient being selected from colorants, humectants, fragrances, stabilizers, penetrants, adhesion promoters, film-forming agents, transdyeing agents, surfactants, solvents, antioxidants, or combinations thereof.

43. The method of claim 42, further comprising a step after step (a) of diluting the formulation in an aqueous medium.

44. The method of claim 43, further comprising a step prior to step (a), namely, reacting cashew extract with an iron precursor to form cashew extract and iron particles and / or iron oxide particles.

Images