Luggage article or luggage accessory

Abstract

The present invention relates to a mechanochemically carbonized magnesium silicate having a BET surface area in the range of 20 to 100 m2 / g, preferably 30 to 80 m2 / g, more preferably 40 to 70 m2 / g, most preferably 45 to 65 m2 / g and / or an amorphous content of at least 30 wt%, preferably at least 40 wt%, more preferably at least 50 wt%, even more preferably at least 60 wt%, as determined by XRD; a CO2 content of at least 3% by weight. The invention also relates to a method for the production thereof and to the use thereof, for example as a filler in polymers. Compositions comprising a mechanochemically carbonized magnesium silicate and a polymer, such as a polyolefin, provide the benefit as a CO2 negative emission material with excellent functional properties, useful for various purposes, for example as a component of apparel or apparel, or as a component of a backpack, such as a button.

Description

Technical Field

[0001] The present invention relates to a mechanochemical carbide magnesium silicate, a method for its preparation and its use as a filler in a polymer, a composition comprising the mechanochemical carbide magnesium silicate and a polymer and a method for its preparation. Background Art

[0002] Synthetic polymers are well-known and important materials used in a wide variety of industries for various purposes. For example, polymers are used as packaging materials, in building and construction, as textiles, etc. Polymers are usually used in the form of compositions comprising the actual polymer material (e.g. polyethylene) and additives such as fillers, plasticizers, UV stabilizers, antioxidants, fibers, etc. Fillers can be particulate materials such as minerals added to polymers to reduce costs and / or improve mechanical properties.

[0003] An example of a widely used polymer filler is magnesium silicate. A comprehensive overview of fillers in polymer materials can be found in Rothon, Roger, ed., Fillers for polymer applications. Vol. 489, Berlin, Germany: Springer, 2017.

[0004] Polymers have come under heavy criticism for their environmental impact. While research into bio-based and recycled polymers is advancing rapidly, the majority of virgin polymer manufacturing is still based on raw material streams from the oil and gas industry, which is associated with large and significant CO2 emissions.

[0005] The present inventors have determined that it is desirable to develop cost-effective filler additives that can result in CO2 emission reduction results without deleteriously affecting the properties of the polymer.

[0006] WO2019012474A1 discloses certain mechanochemically delaminated nanoparticles.

[0007] It is an object of the present invention to provide improved fillers for polymers.

[0008] Another object of the present invention is to provide improved fillers for polymers that are inexpensive to manufacture.

[0009] Another object of the present invention is to provide improved fillers for polymers made using carbon capture and sequestration technology.

[0010] Another object of the present invention is to provide improved fillers for polymers which improve the properties of the resulting polymer composition, such as tensile modulus. Summary of the invention

[0011] In a first aspect, the present invention provides a mechanochemical carbide magnesium silicate having

[0012] · Between 20 and 100m 2 / g and / or an amorphous content of at least 30% by weight as determined by XRD; and

[0013] A CO2 content of at least 3 wt.-%, preferably at least 6 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by thermogravimetric analysis (TGA) using a temperature trace, wherein the temperature is increased from temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min.

[0014] As will be shown in the accompanying examples, it was found that when such mechanochemical carbide magnesium silicate is used as a filler in various polymers (particularly polyolefins), excellent mechanical properties can be obtained while achieving a large amount of CO2 storage in the polymer composition material. The mechanochemical carbide magnesium silicate of the present invention advantageously provides a CO2 negative emission filler, and it has a neutral color, so that polymer compositions containing CO2 negative emission fillers of various colors can be provided.

[0015] The inventors have found that the mechanochemical carbonization of the present invention achieves an increase in the overall amorphous content of the magnesium silicate precursor. Without wishing to be bound by any theory, it is believed that the mechanochemical process of the present invention can lead to an increase in the amorphous content when analyzed by XRD, wherein at least some of the crystalline domains that may be present in the feedstock are maintained by an internal framework in the form of microcrystallinity that adheres to a more extensive disordered structure. Thus, the disordered microstructure promotes higher reactivity.

[0016] The manufacture of the mechanochemical carbide magnesium silicate filler relies on an inexpensive CO2 capture technology platform, providing a filler that can be manufactured in an economically viable manner and combines both CO2 emission reductions achieved through reduced polymer consumption and CO2 emission reductions achieved through carbon capture technology.

[0017] In another aspect, the present invention provides a method for producing the mechanochemical magnesium carbide silicate of the present invention, comprising the following steps:

[0018] a) providing a solid raw material comprising magnesium silicate;

[0019] b) providing a gas comprising CO2;

[0020] c) introducing the solid raw material and the gas into a mechanical stirring unit; and

[0021] d) subjecting the solid raw material to a mechanical stirring operation in the presence of the gas at a pressure of at least 1 atm in the mechanical stirring unit to obtain mechanochemical magnesium carbide silicate.

[0022] In another aspect, the present invention provides a mechanochemical magnesium carbide silicate obtainable by the method for making a mechanochemical magnesium carbide silicate as described herein.

[0023] In another aspect, the present invention provides a method for co-manufacturing a mixture of mechanochemical magnesium carbide silicate and mechanochemical graphite oxide, comprising the steps of:

[0024] a) providing a solid raw material comprising magnesium silicate and graphite;

[0025] b) providing a gas comprising CO2;

[0026] c) introducing the solid raw material and the gas into a mechanical stirring unit; and

[0027] d) subjecting the solid raw material to a mechanical stirring operation in the mechanical stirring unit in the presence of the gas at a pressure of at least 1 atm to obtain a mixture of mechanochemical magnesium carbide silicate and mechanochemical graphite oxide.

[0028] In another aspect, the present invention provides a mixture of mechanochemically carbided magnesium silicate and mechanochemically graphite oxide obtainable by a process for co-manufacturing a mixture of mechanochemically carbided magnesium silicate and mechanochemically graphite oxide as described herein.

[0029] In another aspect, the present invention provides a composition comprising the mechanochemical carbide magnesium silicate as described herein and a polymer. Preferably, the composition further comprises mechanochemical graphite oxide.

[0030] In another aspect, the present invention provides a method for preparing a composition as described herein, comprising the steps of:

[0031] (i) providing a mechanochemical magnesium carbide silicate as described herein;

[0032] (ii) providing a polymer as described herein;

[0033] (iii) optionally providing mechanochemical graphite oxidation as described herein; and

[0034] (iv) combining the mechanochemical carbide magnesium silicate of step (i) with the polymer of step (ii) and optionally the mechanochemical graphite oxide of step (iii).

[0035] In another aspect, the present invention provides the use of a mechanochemical carbide magnesium silicate as described herein:

[0036] Used as filler in polymers;

[0037] Increase the crystallization temperature of the polymer;

[0038] Increase the tensile modulus of the polymer;

[0039] Increase the yield stress of the polymer; and / or

[0040] Increase the impact strength of polymers.

[0041] In another aspect, the present invention provides a method of:

[0042] Increase the crystallization temperature of the polymer

[0043] Increase the tensile modulus of the polymer;

[0044] Increase the yield stress of the polymer; and / or

[0045] Increase the impact strength of polymers,

[0046] The method comprises adding a mechanochemical magnesium carbide silicate as described herein to the polymer.

[0047] Another aspect of the present invention provides a luggage item or luggage accessory comprising a hardware component, wherein the hardware component contains a hardware composition comprising a mechanochemical magnesium carbide silicate as described herein and / or a mechanochemical graphite oxide as described herein, and optionally an optional polymer. DETAILED DESCRIPTION

[0048] According to the present invention, the BET surface area as mentioned herein is determined by mass spectrometry using 0.5 to 1 g of sample at a temperature of 77 K. The BET surface area as mentioned herein is determined using nitrogen. A preferred analytical method for determining the BET surface area comprises heating the sample to 400° C. for a desorption cycle prior to the surface area analysis. A suitable and therefore preferred analytical apparatus for determining the BET surface area is a Micromeritics Gemini 2375 preferably equipped with a Micromeritics FlowPrep 060 flow gas degassing unit.

[0049] The amorphous content determined by X-ray diffraction (XRD) as referred to herein is preferably determined using a corundum standard. A suitable and therefore preferred XRD analysis setup is by using a PANalytical Aeris X-ray diffractometer with Rietveld refinement (eg using HighScore Plus XRD analysis software).

[0050] As used herein, TGA refers to thermogravimetric analysis (a technique known to those skilled in the art). A preferred TGA setup for determining the CO2 content of feedstock and mechanochemical carboxylation materials in the context of the present invention is a Setaram TAG 16 TGA / DSC dual chamber balance using 0.1 to 2 mg sample. According to the present invention, TGA is performed under an inert atmosphere such as nitrogen or argon.

[0051] According to the present invention, particle size distribution characteristics such as D10, D50, D90 and D(4:3) are measured by using a laser light scattering particle size analyzer using Fraunhofer light scattering theory, such as Fritsch Analysette 22 Nanotec or another instrument of equal or better sensitivity and reporting data using a volume equivalent sphere model. As known to the skilled artisan, D50 is the mass median diameter, i.e., the diameter at which 50% of the mass of the sample is composed of smaller particles. Similarly, D10 and D90 represent the diameter at which 10 or 90% of the mass of the sample is composed of smaller particles. As known to the skilled artisan, the D(4:3) is the volume median diameter.

[0052] As used herein, "magnesium silicate" very preferably refers to a salt having the chemical formula Mg3Si4O 10 Hydrated magnesium silicate of (OH)2, also known as "talc".

[0053] As used herein, "mechanically carbided magnesium silicate" refers to a magnesium silicate which has been subjected to a CO sequestration or carbonization process, in particular the process described herein, resulting in a partial conversion of the magnesium silicate into a carbonate with minerals. The expression "mechanically carbided magnesium silicate" includes a mechanochemically carbided magnesium silicate which has been surface-modified, in particular by treatment with an agent such as an organosilane, a polyol (e.g. a diol), a stearate or any other compatibilizer (e.g. a compatibilizer as described elsewhere herein). The surface modification may have been performed before or after the mechanochemical carbonization.

[0054] The expression “comprise” and variations thereof (such as “comprises” and “comprising”) as used herein should be interpreted in an open, inclusive sense, meaning that the described embodiments include the recited features but not excluding the presence of other features as long as they do not render the described embodiments inoperative.

[0055] The expressions "one embodiment," "a particular embodiment," "an embodiment," and the like, as used herein, should be interpreted as indicating that a particular feature, structure, or characteristic described in connection with the embodiment is included in at least one embodiment. Thus, the appearances of such expressions in different places throughout this specification are not necessarily all referring to the same embodiment. Furthermore, in one or more embodiments, the particular features, structures, or characteristics may be combined in any suitable manner. For example, certain features of the invention described herein in the context of separate embodiments are also expressly contemplated in combination in a single embodiment.

[0056] Unless the context clearly indicates otherwise, the singular forms "a", "an", and "the" as used herein should be construed to include plural referents. It should also be noted that unless the context clearly indicates otherwise, the term "or" is generally used in its broadest sense, i.e., meaning "and / or".

[0057] As used herein, the expression "particulate solid" is not particularly limited to the nature of the particulate solid and relates to any solid material consisting of distinct particles or pieces, such as dust, fibers, fines, chips, chunks, flakes, granules, pellets, prills, pastilles, powders, etc. Preferably, the particulate solid is a powder.

[0058] As used herein, the expression "gas containing CO2" is not particularly limited and is intended to mean any gas containing CO2. In particular, the gas may contain other reactive components such as O2, NH3, H2S, SO2, NO x Etc., and this is generally true of industrial waste gas streams. For the purposes of this invention, it is assumed that the ideal gas law causes any volume % mentioned herein in the context of a gas to be equal to the mole % .

[0059] As used herein, the expression "tensile modulus" refers to Young's modulus measured according to ASTM 638 (2014).

[0060] As used herein, the expression "yield stress" refers to the pressure exhibited at yield as measured according to ASTM 638 (2014).

[0061] As used herein, the expression “impact strength” refers to the impact strength measured according to the Charpy impact test of ASTM D6110 (2018).

[0062] Mechanochemical magnesium carbide silicate

[0063] In a first aspect, the present invention provides a mechanochemical carbide magnesium silicate having

[0064] · Between 20 and 100m 2 / g, preferably 30 to 80m 2 / g, more preferably 40 to 70m 2 / g, more preferably 45 to 65m 2 / g, and / or an amorphous content of at least 30 wt.-%, preferably at least 40 wt.-%, more preferably at least 50 wt.-%, more preferably at least 60 wt.-% as determined by XRD; and

[0065] · A CO2 content of at least 3 wt.-%, preferably at least 6 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min.

[0066] Untreated magnesium silicate (which has not been mechanochemically carbonized according to the process described elsewhere herein) shows only a slight mass loss above 200°C as measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min. For untreated magnesium silicate (i.e., native magnesium silicate, also known as regular magnesium silicate), the mass loss is less than 2 wt%. Thus, when measured as described herein, the CO2 content of the mechanochemically carbonized magnesium silicate of the present invention provides a good approximation of the amount of CO2 that has been sequestered by the mechanochemical carbonization of the magnesium silicate, the CO2 content being high enough to contribute negligibly to the mass loss that may be present when measuring native magnesium silicate.

[0067] In a preferred embodiment of the present invention, there is provided a mechanochemical carbide magnesium silicate of the present invention, wherein A is greater than 1 wt %, preferably greater than 2 wt %, more preferably greater than 3.5 wt %,

[0068] Where A = CO2 (treated) - CO2 (original),

[0069] wherein CO2 (treated) is determined on the mechanochemical magnesium carbide silicate of the invention as the mass loss above 200°C measured by TGA using a temperature trace wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min,

[0070] Wherein CO2(original) was determined on magnesium silicate before mechanochemical carbonization as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature was increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min.

[0071] In an embodiment of the present invention, the particle size distribution of the mechanochemical carbide magnesium silicate has one, two or all of the following characteristics, preferably all:

[0072] D10 in the range of 0.01 to 5 μm, preferably 0.1 to 3 μm, most preferably 0.5 to 1.5 μm;

[0073] D50 in the range of 0.1 to 50 μm, preferably 1 to 25 μm, most preferably 2 to 10 μm;

[0074] • D90 in the range of 5 to 150 μm, preferably 10 to 100 μm, most preferably 15 to 40 μm.

[0075] In a very preferred embodiment of the present invention, the mechanochemical carbide magnesium silicate has a carbon content of 20 to 100 m 2 / g, preferably 30 to 80m 2 / g, more preferably 40 to 70m 2 / g, most preferably 45 to 65m 2 / g and an amorphous content of at least 30 wt %, preferably at least 40 wt %, more preferably at least 50 wt % and most preferably at least 60 wt % as determined by XRD. For example, in some embodiments, the mechanochemical carbide magnesium silicate has a BET surface area of ​​20 to 100 m 2 / g, preferably 30 to 80m 2 / g, more preferably 40 to 70m 2 / g, most preferably 45 to 65m 2 / g BET surface area and an amorphous content of at least 50% by weight, more preferably at least 60 to %, as determined by XRD. For example, in some embodiments, the mechanochemical carbide magnesium silicate has 40 to 70 m 2 / g, preferably 45 to 65m 2 / g and an amorphous content determined by XRD of at least 50% by weight, more preferably at least 60% by weight.

[0076] In a preferred embodiment of the present invention, the mechanochemical carbide magnesium silicate has a CO2 content in the range of 3 to 40 wt%, preferably 5 to 35 wt%, more preferably 7 to 30 wt%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min. The CO2 content is typically less than 25 wt%. In a specific embodiment, the CO2 content as described herein is in the range of 7 to 22 wt%.

[0077] Therefore, in a preferred embodiment of the present invention, the mechanochemical carbide magnesium silicate has

[0078] · Between 20 and 100m 2 / g, preferably 30 to 80m 2 / g, more preferably 40 to 70m 2 / g, most preferably 45 to 65m 2 BET surface area in the range of 1000 Å / g; and

[0079] a CO2 content in the range of 3 to 40 wt.-%, preferably 5 to 35 wt.-%, more preferably 7 to 30 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min, and

[0080] a D50 in the range of 0.1 to 50 μm, preferably 1 to 25 μm, most preferably 2 to 10 μm, and

[0081] - An amorphous content of at least 30 wt.-%, preferably at least 40 wt.-%, more preferably at least 50 wt.-%, even more preferably at least 60 wt.-%, as determined by XRD.

[0082] The other particle size distribution characteristics D10, D90 and D(4:3) are preferably as described herein before.

[0083] In a more preferred embodiment of the present invention, the mechanochemical carbide magnesium silicate has

[0084] · Between 40 and 70 m 2 / g, most preferably 45 to 65m 2 BET surface area in the range of 1000 Å / g; and

[0085] a CO2 content in the range of 7 to 30 wt. %, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min, and

[0086] - An amorphous content of at least 50% by weight, even more preferably at least 60% by weight, as determined by XRD.

[0087] In some embodiments, the mechanochemical magnesium carbide silicate is not surface modified.

[0088] The mechanochemical carbide magnesium silicates described herein have various uses and applications that provide the benefit of storing large amounts of CO2. In particularly preferred embodiments, the mechanochemical carbide magnesium silicates described herein are suitable for use in a hardware composition employed in a hardware component for manufacturing a luggage item or luggage accessory, wherein the hardware component is as defined herein and the luggage item or luggage accessory is as defined herein. Also disclosed herein is a luggage item or luggage accessory comprising a hardware component, wherein the hardware component contains a hardware composition comprising a mechanochemical carbide magnesium silicate, wherein the mechanochemical carbide magnesium silicate is as described herein. The hardware composition may, for example, contain at least 1% by weight (based on the total weight of the composition) of the mechanochemical carbide magnesium silicate, preferably at least 5% by weight of the mechanochemical carbide magnesium silicate.

[0089] Method for producing mechanochemical magnesium carbide silicate

[0090] In another aspect, the present invention provides a method for producing a mechanochemical magnesium carbide silicate as described herein, comprising the following steps;

[0091] a) providing a solid raw material comprising magnesium silicate;

[0092] b) providing a gas comprising CO2;

[0093] c) introducing the solid raw material and the gas into a mechanical stirring unit; and

[0094] d) subjecting the solid raw material to a mechanical stirring operation in the presence of the gas at a pressure of at least 1 atm in the mechanical stirring unit to obtain mechanochemical magnesium carbide silicate.

[0095] Those skilled in the art can adjust the relevant process parameters according to the guidance provided in the present invention to obtain mechanochemical magnesium carbide silicate having the properties listed herein.

[0096] The solid starting material provided in step (a) is typically a particulate material.

[0097] In an embodiment of the present invention, the solid raw material has a moisture content of less than 3 wt%, preferably less than 2 wt%, more preferably less than 1 wt% and / or a D50 in the range of 0.1 to 500 μm, preferably in the range of 0.2 to 50 μm, more preferably in the range of 0.5 to 15 μm.

[0098] In an embodiment, the method for making the mechanochemical carbide magnesium silicate of the present invention comprises spraying the solid magnesium silicate raw material with an aqueous composition such as water and / or humidifying the gas containing CO2 contacting the solid raw material. Humidification of the gas stream is within the routine capabilities of the skilled artisan and can be performed by any means, such as bubbling or sparging the gas through an aqueous composition (e.g., water), membrane-driven water humidification of the gas, mixing the gas stream with water vapor, etc.

[0099] Very preferably, the solid raw material comprises at least 80%, preferably at least 90%, more preferably at least 95% hydrated magnesium silicate as determined by X-ray diffraction. The solid raw material will typically be a magnesium silicate obtained from a natural deposit, so that it contains other minerals close to the hydrated magnesium silicate, typically such as magnesite, dolomite and / or chlorite. Thus, the solid raw material optionally comprises at least 0.1% of minerals that are not hydrated magnesium silicate as determined by X-ray diffraction. Typically, the solid raw material will comprise less than 20%, preferably less than 10%, more preferably less than 5% of minerals that are not hydrated magnesium silicate as determined by X-ray diffraction. Such minerals that are not hydrated magnesium silicate present in conjunction with magnesium silicate obtained from a natural deposit are, for example, magnesite, dolomite and / or chlorite. Therefore, in some embodiments of the present invention, the solid raw material optionally contains at least 0.1% of minerals selected from magnesite, dolomite and / or chlorite as determined by X-ray diffraction, preferably, the solid raw material contains 0.1 to 20%, preferably 0.1 to 10%, more preferably 0.1 to 5% of minerals selected from magnesite, dolomite and / or chlorite as determined by X-ray diffraction.

[0100] The gas provided in step (b) may be any gas stream containing CO2, such as normal air, a waste gas stream with a low CO2 concentration, or a concentrated CO2 stream. In an embodiment, the gas stream containing CO2 is normal air. In a very preferred embodiment, the gas stream containing CO2 is a combustion flue gas, in particular a flue gas from the combustion of fossil fuels, the combustion of wood particles, the combustion of biomass or the combustion of municipal waste. The fossil fuel combustion may be coal, petroleum, petroleum coke, natural gas, shale oil, asphalt, tar sand oil, or heavy oil combustion or any combination thereof. The combustion flue gas may optionally be treated to reduce the water content, SO2 content and / or NO x content.

[0101] Typical CO2 concentrations of such combustion flue gases are in the range of 1 to 15 vol%, such as 1 to 10 vol% or 2 to 10 vol%, so that preferably, the gas provided in step (b) has a CO2 concentration in the range of 1 to 15 vol%, such as 2 to 10 vol%.

[0102] In an embodiment of the present invention, the gas provided in step (b) contains less than 80% by volume of CO2, preferably less than 50% by volume of CO2. In such embodiments, the CO2 concentration in the gas can be extremely low, such as less than 1% by volume, or less than 0.1% by volume. The CO2 concentration in the gas provided in step (b) is preferably at least 0.1% by volume, more preferably at least 0.5% by volume. Typically and preferably, the low-enriched gas stream is a combustion flue gas having a CO2 concentration in the range of 1 to 15% by volume, such as 1 to 10% by volume or 2 to 10% by volume, or 2 to 5% by volume. In an alternative embodiment of the present invention, the gas provided in step (b) contains at least 80% by volume of CO2, preferably at least 95% by volume of CO2.

[0103] In some embodiments of the present invention, the gas provided in step (b) contains less than 1000 ppm (v / v) of H2O, preferably less than 100 ppm (v / v) of H2O. In a more preferred embodiment of the present invention, the gas provided in step (b) contains more than 1000 ppm (v / v) of H2O, preferably more than 10000 ppm (v / v) of H2O.

[0104] In some embodiments of the present invention, the gas provided in step (b) comprises at least 80% by volume of CO2, preferably at least 95% by volume of CO2 and less than 1000 ppm (v / v) of H2O, preferably less than 100 ppm (v / v) of H2O. In a more preferred embodiment of the present invention, the gas provided in step (b) comprises at least 80% by volume of CO2, preferably at least 95% by volume of CO2 and greater than 1000 ppm (v / v) of H2O, preferably greater than 10000 ppm (v / v) of H2O.

[0105] In some embodiments of the present invention, the gas provided in step (b) comprises 1 to 15% by volume of CO2 and less than 1000 ppm (v / v) of H2O, preferably less than 100 ppm (v / v) of H2O. In a more preferred embodiment of the present invention, the gas provided in step (b) comprises 1 to 15% by volume of CO2, and greater than 1000 ppm (v / v) of H2O, preferably greater than 10000 ppm (v / v) of H2O.

[0106] In any embodiment of the present invention, the gas provided in step (b) is generally not in a supercritical state, as this is not necessary for the mild mechanochemical carbonization process of the present invention. Therefore, in any embodiment of the present invention, it is very preferred that the gas is not in a supercritical state in any step of the process.

[0107] In an embodiment of the present invention, step (d) is carried out at a pressure of at least 3 atm, preferably at least 6 atm. In an embodiment of the present invention, step (d) is carried out at a temperature of less than 150°C, preferably less than 100°C, preferably less than 90°C, more preferably less than 80°C, most preferably less than 75°C. In a very preferred embodiment of the present invention, step (d) is carried out at a temperature in the range of 45 to 85°C, preferably 55 to 70°C. In a preferred embodiment of the present invention, active heating is not applied and any increase in temperature is attributed to friction due to mechanical stirring or to exothermic reactions occurring during mechanochemical carbonization. The temperature is preferably determined according to the solid material in the reactor (i.e., the mechanical stirring unit) during the treatment.

[0108] The low temperature requirement of the process means that fossil fuels are not required, and in case the friction caused by mechanical stirring is not sufficient to reach the desired temperature (e.g. greater than 45°C), it is practical to use electric heating elements (or low calorific value green fuel sources) to provide heat. In this way, fossil fuels can be avoided throughout the entire production chain.

[0109] In an embodiment of the present invention, step (d) is performed for at least 1 hour, preferably at least 4 hours, more preferably at least 8 hours.

[0110] As with any chemical process, suitable reaction times are highly dependent on the degree of carbonization desired, the surface area desired, and the pressure, temperature, and mechanochemical agitation applied and can be readily determined by periodically sampling the material and monitoring the progress of the reaction, for example by BET analysis, particle size analysis, amorphous content, and / or CO2 content determination as described herein.

[0111] In addition, the inventors have found that the mechanochemical carbonization method described herein can be advantageously carried out without using an additional oxidant such as an acid. Therefore, the mechanochemical carbonization method described herein is preferably carried out without using a strong acid, preferably without using any other oxidant other than the gas provided in step (b).

[0112] In a preferred embodiment of the present invention, the mechanical stirring operation of step (d) includes grinding, milling, mixing, stirring (slow speed stirring or high speed stirring), shearing (high torque shearing), shaking, blending, fluidized bed or ultrasonic treatment, preferably grinding, grinding, mixing, stirring (slow speed stirring or high speed stirring), shearing (high torque shearing) or ultrasonic treatment. The inventors have found that if the mechanochemical stirring operation of step (d) is carried out in the presence of inert grinding or grinding media (referred to herein as inert media) (preferably inert balls or beads), the mechanochemical carbonization process is convenient to carry out. A preferred inert medium is stainless steel. In such a very preferred embodiment, the mechanical stirring operation can be simply rotating a mechanical stirring unit containing solid raw materials, inert grinding or grinding media and gas. This can be easily carried out in a rotating drum.

[0113] In a preferred embodiment of the present invention, step (d) is carried out in the presence of a catalyst, preferably a transition metal oxide catalyst, more preferably a transition metal dioxide catalyst, most preferably a transition metal dioxide catalyst selected from the group consisting of iron oxide, cobalt oxide, ruthenium oxide, titanium oxide, nickel oxide and a combination thereof.

[0114] Thus, as will be understood from the above, in a highly preferred embodiment of the present invention, step (d) comprises a mechanical agitation operation in the presence of an inert grinding medium and a transition metal oxide catalyst, preferably milling, grinding, mixing, stirring (slow speed stirring or high speed stirring), shearing (high torque shearing), shaking, blending, fluidized bed or ultrasonic treatment. The inventors have found that it is advantageous to use an inert medium as described above with a view to the efficiency of mechanochemical carbonization (e.g., reaction time, CO2 absorption and particle size reduction), wherein the inert medium is coated with the transition metal oxide catalyst. As described elsewhere herein, the mechanical agitation operation may be simply rotating a mechanical agitation unit containing a solid feedstock, an inert milling or grinding medium, a transition metal oxide catalyst and a gas. This can be conveniently performed in a rotating drum.

[0115] As will be apparent from the process descriptions provided herein, step d) of various processes according to the present invention is a gas-solid reaction. A small amount of solvent (such as water) may be added for wetting purposes as described previously herein. In embodiments, no solvent (such as water) is added.

[0116] In another aspect, the present invention provides a mechanochemical magnesium carbide silicate obtainable by a method for making a mechanochemical magnesium carbide silicate as described herein. The mechanochemical magnesium carbide silicate is preferably obtainable by a method for making a mechanochemical magnesium carbide silicate as described herein, wherein the process is performed such that the mechanochemical magnesium carbide silicate has

[0117] · Between 20 and 100m 2 / g, preferably 30 to 80m 2 / g, more preferably 40 to 70m 2 / g, most preferably 45 to 65m 2 BET surface area in the range of 1000 Å / g; and

[0118] a CO2 content in the range of 3 to 40 wt.-%, preferably 5 to 35 wt.-%, more preferably 7 to 30 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min, and

[0119] a D50 in the range of 0.1 to 50 μm, preferably 1 to 25 μm, most preferably 2 to 10 μm, and

[0120] - An amorphous content of at least 30 wt.-%, preferably at least 40 wt.-%, more preferably at least 50 wt.-%, even more preferably at least 60 wt.-%, as determined by XRD.

[0121] Without wishing to be bound by any theory, the inventors believe that the increase in amorphous content achieved by the dry mechanochemical carbonization process of the present invention is associated with the observed beneficial properties such as yield stress and impact strength. Therefore, in an embodiment of the present invention, a mechanochemically carburized magnesium silicate obtainable by concomitant carbonization and increase in the amorphous content of a magnesium silicate precursor is provided, wherein the absolute difference between the amorphous content (expressed as % by total weight) of the mechanochemically carburized magnesium silicate and the amorphous content (expressed as % by total weight) of the magnesium silicate precursor is at least 20 percentage points, preferably at least 25 percentage points, more preferably at least 30 percentage points, more preferably at least 35 percentage points. The amorphous content is determined by XRD.

[0122] In another aspect, the present invention provides a mechanochemical magnesium carbide silicate obtainable by a method for making a mechanochemical magnesium carbide silicate as described herein. The mechanochemical magnesium carbide silicate is preferably obtainable by a method for making a mechanochemical magnesium carbide silicate as described herein, wherein the process is performed such that the mechanochemical magnesium carbide silicate has

[0123] · Between 20 and 100m 2 / g, preferably 30 to 80m 2 / g, more preferably 40 to 70m 2 / g, most preferably 45 to 65m 2 / g range and,

[0124] a CO2 content in the range of 3 to 40 wt.-%, preferably 5 to 35 wt.-%, more preferably 7 to 30 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min, and,

[0125] - An amorphous content of at least 30 wt.-%, preferably at least 40 wt.-%, more preferably at least 50 wt.-%, even more preferably at least 60 wt.-%, as determined by XRD.

[0126] Compositions comprising mechanochemical carbide magnesium silicate and polymers

[0127] The mechanochemical carbide magnesium silicates described herein have various unique properties due to the evolution of chemical identity represented by a high degree of carbonization in the context of various aspects of the present invention. It has been surprisingly found that such materials can be used, for example, as fillers in polymers without adversely affecting material properties. In fact, it has been found that the mechanochemical carbide magnesium silicates of the present invention constitute excellent fillers for various polymers, especially polyolefins, which combine unique mechanical properties with cost-effective CO2 capture technology.

[0128] Thus, in another aspect, the present invention provides a composition comprising a mechanochemical carbide magnesium silicate as described herein and a polymer. The polymer is a synthetic polymer. The term "polymer" as used herein includes copolymers, such as block copolymers.

[0129] In an embodiment, the polymer is selected from a thermoplastic polymer and a thermosetting polymer. In a preferred embodiment, the polymer is selected from the group consisting of: epoxy resin, phenol-formaldehyde resin, polyalkylene terephthalate (preferably polyethylene terephthalate), polyalkylene adipate terephthalate (preferably polybutylene adipate terephthalate), polyisosorbide terephthalate (preferably polyisosorbide terephthalate), polyalkylene aromatic polyamide (preferably polyethylene aromatic polyamide), polyacrylonitrile, poly Acetal, polyimide, aromatic polyester, polyisoprene (preferably cis-1,4-polyisoprene), polyethylene, polypropylene, polyurethane, polyisocyanurate, polyamide, polyether, polyester, polyhydroxyalkanoate, polylactic acid, polylactic acid-co-glycolic acid, polyvinylidene fluoride, polyvinyl acetate, polyvinyl chloride, polystyrene, polytetrafluoroethylene, acrylonitrile-butadiene-styrene, nitrile rubber, styrene-butadiene, ethylene vinyl acetate, copolymers thereof and combinations thereof. Notably, the copolymer is a homogeneous or heterogeneous PE-PP copolymer. The polymer is preferably selected from polyacetal, polyethylene terephthalate, polypropylene, polyethylene and polybutylene adipate terephthalate, copolymers thereof and combinations thereof. Very preferred are polyolefins, such as polypropylene, polyethylene, copolymers thereof and combinations thereof, in particular polypropylene. Polyethylene includes HDPE, LDPE, LLDPE, etc.

[0130] Polymers have been heavily criticized for their environmental impact. Many virgin polymers are produced based on raw material streams from the oil and gas industry. One way to use polymers to reduce negative environmental impacts is to avoid using virgin polymers and / or use polymer waste materials. Therefore, in an embodiment of the present invention, the polymer is not a virgin polymer. Therefore, for example, the polymer may be a recycled polymer, wherein the polymer is as defined herein. The polymer can be recycled using any known recycling technology. Preferred recycled polymers include recycled polyacetals, recycled polyethylene terephthalate, recycled polypropylene, recycled polyethylene and recycled polybutylene adipate terephthalate, copolymers thereof and combinations thereof. Highly preferred recycled polymers are recycled polyolefins, such as recycled polypropylene, recycled polyethylene, copolymers thereof and combinations thereof, particularly polypropylene. Recycled polyethylene includes recycled HDPE, recycled LDPE, recycled LLDPE, etc.

[0131] In an embodiment of the present invention, the composition comprises at least 0.1 wt% (based on the total weight of the composition) of mechanochemical carbide magnesium silicate, preferably at least 1 wt% of mechanochemical carbide magnesium silicate, more preferably at least 5 wt% of mechanochemical carbide magnesium silicate and / or at least 50 wt% (based on the total weight of the composition) of polymer, preferably at least 55 wt% of polymer, more preferably at least 60 wt% of polymer, for example, at least 65 wt% of polymer or at least 70 wt% of polymer. Typically, the composition will comprise at least 5 wt% of mechanochemical carbide magnesium silicate and at least 50 wt% (based on the total weight of the composition) of polymer, preferably at least 55 wt% of polymer, more preferably at least 60 wt% of polymer.

[0132] In an embodiment of the present invention, the composition comprises less than 40 wt% (based on the total weight of the composition) of mechanochemical carbide magnesium silicate, preferably less than 30 wt% of mechanochemical carbide magnesium silicate, more preferably less than 20 wt% of mechanochemical carbide magnesium silicate.

[0133] In a preferred embodiment of the present invention, the composition comprises 0.1 to 40% by weight (based on the total weight of the composition) of mechanochemical carbide magnesium silicate, preferably 1 to 30% by weight of mechanochemical carbide magnesium silicate, more preferably 5 to 30% by weight of mechanochemical carbide magnesium silicate, and at least 50% by weight (based on the total weight of the composition) of polymer, preferably at least 55% by weight of polymer, more preferably at least 60% by weight of polymer. In a particularly preferred embodiment, the composition comprises at least 10% by weight (based on the total weight of the composition), preferably at least 12% by weight, more preferably at least 15% by weight of mechanochemical carbide magnesium silicate. For example, the composition comprises 10 to 40% by weight (based on the total weight of the composition) of mechanochemical carbide magnesium silicate, preferably 12 to 30% by weight of mechanochemical carbide magnesium silicate, more preferably 15 to 30% by weight of mechanochemical carbide magnesium silicate, and at least 50% by weight (based on the total weight of the composition) of polymer, preferably at least 55% by weight of polymer, more preferably at least 60% by weight of polymer.

[0134] In a particular embodiment of the invention, the composition comprises at least 3% by weight (based on the total weight of the composition) of mechanochemical carbide magnesium silicate, preferably at least 4% by weight of mechanochemical carbide magnesium silicate. In such embodiments, the polymer is preferably a polyolefin, such as polypropylene or polyethylene. As described elsewhere herein, the composition preferably comprises at least 50% by weight (based on the total weight of the composition) of polymer, preferably at least 55% by weight of polymer, more preferably at least 60% by weight of polymer. In these embodiments, the amount of polymer may be at least 80% by weight (based on the total weight of the composition). As shown in the accompanying examples, it has been surprisingly found that when the mechanochemical carbide magnesium silicate is employed at these levels, a significant increase in crystallization temperature is exhibited.

[0135] In a particular embodiment of the invention, the composition comprises at least 13% by weight (based on the total weight of the composition) of mechanochemical carbide magnesium silicate, preferably at least 14% by weight of mechanochemical carbide magnesium silicate. In such embodiments, the polymer is preferably a polyolefin, such as polypropylene or polyethylene. As described elsewhere herein, the composition preferably comprises at least 50% by weight (based on the total weight of the composition) of polymer, preferably at least 55% by weight of polymer, more preferably at least 60% by weight of polymer. In these embodiments, the amount of polymer may be at least 80% by weight (based on the total weight of the composition). As shown in the accompanying examples, it was surprisingly found that when mechanochemical carbide magnesium silicate is used in these contents, a significant increase in tensile modulus is exhibited.

[0136] In a particular embodiment of the present invention, the composition comprises 3 to 13 wt % (based on the total weight of the composition) of mechanochemical carbide magnesium silicate, preferably 4 to 12 wt % of mechanochemical carbide magnesium silicate. In such embodiments, the polymer is preferably a polyolefin, such as polypropylene or polyethylene. As described elsewhere herein, the composition preferably comprises at least 50 wt % (based on the total weight of the composition) of polymer, preferably at least 55 wt % of polymer, more preferably at least 60 wt % of polymer. In these embodiments, the amount of polymer may be at least 80 wt % (based on the total weight of the composition). As shown in the accompanying examples, it has been surprisingly found that when the mechanochemical carbide magnesium silicate is used in these contents, an increase in tensile modulus, yield stress and impact strength is exhibited, while avoiding the unexpected reduction in impact strength at higher loads of mechanochemical carbide magnesium silicate.

[0137] In some embodiments of the present invention, the composition described herein is provided in the form of a masterbatch concentrate, the masterbatch concentrate comprising a mechanochemical carbide magnesium silicate as described herein and a polymer as described herein, wherein the composition comprises at least 40 wt % (based on the total weight of the composition), preferably at least 50 wt % of the mechanochemical carbide magnesium silicate.

[0138] The compositions of the present invention will typically contain other additives such as fillers, light stabilizers, heat stabilizers, compatibilizers, antioxidants, rheology modifiers (such as plasticizers), impact modifiers, flame retardants, lubricants and / or antistatic agents.

[0139] In a particular embodiment of the present invention, the composition of the present invention further comprises a compatibilizer. Examples of suitable compatibilizers include, but are not limited to, ethylene-glycidyl methacrylate, diazirine, grafted polyethylene derivatives (particularly maleic anhydride grafted polyethylene, maleic anhydride grafted polypropylene, or maleic anhydride grafted HDPE), organometallics containing titanium or zirconium, organosilanes (particularly organosilanes containing polar functional groups (such as amino functional groups) or trialkylvinylsilanes (such as triethoxyvinylsilane)), polyester waxes, paraffin waxes, and functionalized waxes (particularly functionalized paraffin waxes, such as oxidized paraffin waxes). The inventors have found that, although such compatibilizers are not strictly required, they can facilitate the incorporation of mechanochemical carbide magnesium silicate into the polymer during processing.

[0140] In a particular embodiment of the present invention, the composition of the present invention further comprises a filler selected from rubber (preferably selected from styrene-butadiene rubber, polyisoprene, chloroprene, nitrile rubber, polyisobutylene, polybutadiene and combinations thereof, preferably styrene-butadiene rubber). An example of a suitable and preferred rubber filler is recycled tire rubber, in particular styrene-butadiene rubber from recycled tires. In a preferred embodiment of the present invention, the composition comprises a filler selected from rubber (preferably recycled tire rubber as described herein) in an amount of at least 0.1% by weight (based on the total weight of the composition), preferably at least 1% by weight. Typically, the filler selected from rubber is present in an amount of 0.1 to 10% by weight (based on the total weight of the composition), preferably 1 to 8% by weight, and more preferably 4 to 6% by weight.

[0141] The compositions described herein have various uses and application areas, wherein they can provide benefits as CO2 negative emission materials with excellent functional properties. In particularly preferred embodiments, the compositions described herein are suitable for use in hardware compositions employed in the manufacture of hardware components for luggage articles or luggage accessories, wherein the hardware components are as defined herein and the luggage articles or luggage accessories are as defined herein. Also disclosed herein are luggage articles or luggage accessories comprising hardware components, wherein the hardware components contain a hardware composition comprising mechanochemical carbide magnesium silicate and a polymer. The hardware components preferably comprise a hardware composition comprising mechanochemical carbide magnesium silicate and a polymer as described herein and a filler selected from rubber as described herein, preferably recycled tire rubber.

[0142] The composition comprising mechanochemical carbide magnesium silicate and a polymer further comprises mechanochemical graphite oxide

[0143] The inventors have furthermore found that the mechanochemical carbide magnesium silicate of the present invention can advantageously be combined with mechanochemical graphite oxide for use as a filler in polymers. This has the particular advantage of not requiring the addition of other colorants (such as carbon black) to achieve a dark color while maximizing CO2 storage in the polymer composition. Furthermore, without wishing to be bound by any theory, the inventors believe that when mechanochemical carbide magnesium silicate and mechanochemical graphite oxide are used in combination, a synergistic effect occurs, thereby improving specific material properties (such as tensile modulus, impact strength, yield stress or crystallization temperature) or overall mechanical properties compared to the same amount of mechanochemical carbide magnesium silicate or mechanochemical graphite oxide alone.

[0144] Therefore, in a particularly preferred embodiment of the present invention, there is provided a composition comprising mechanochemical carbide magnesium silicate and a polymer as described above, and further comprising mechanochemical graphite oxide.

[0145] In an embodiment of the present invention, a composition is provided, which comprises a mechanochemical carbide magnesium silicate and a polymer as described above, and further comprises at least 0.1 wt% (based on the total weight of the composition) of mechanochemical graphite oxide, preferably at least 1 wt% of mechanochemical graphite oxide, more preferably at least 5 wt% of mechanochemical graphite oxide and / or at least 50 wt% (based on the total weight of the composition) of polymer, preferably at least 55 wt% of polymer, more preferably at least 60 wt% of polymer. Typically, the composition will comprise at least 5 wt% of mechanochemical graphite oxide and at least 50 wt% (based on the total weight of the composition) of polymer, preferably at least 55 wt% of polymer, more preferably at least 60 wt% of polymer.

[0146] In an embodiment, a composition is provided, comprising a mechanochemical carbide magnesium silicate and a polymer as described above, and further comprising mechanochemical graphite oxide, wherein the composition comprises less than 40 wt % (based on the total weight of the composition) of mechanochemical graphite oxide, preferably less than 30 wt % of mechanochemical graphite oxide, for example less than 20 wt % of mechanochemical graphite oxide.

[0147] In a preferred embodiment of the present invention, a composition is provided, which comprises a mechanochemical carbide magnesium silicate and a polymer as described above and further comprises 0.1 to 40 wt % (based on the total weight of the composition) of mechanochemical graphite oxide, preferably 1 to 30 wt % of mechanochemical graphite oxide, more preferably 5 to 25 wt % of mechanochemical graphite oxide, and at least 50 wt % (based on the total weight of the composition) of the polymer, preferably at least 55 wt % of the polymer, more preferably at least 60 wt % of the polymer.

[0148] The mechanochemical carbide magnesium silicate and mechanochemical graphite oxide are preferably included in the composition in a combined amount in the range of 0.1 to 40 wt% (based on the total weight of the composition), preferably 1 to 30 wt%, more preferably 5 to 25 wt%. The mechanochemical carbide magnesium silicate and mechanochemical graphite oxide are preferably included in the composition in a ratio (w / w) mechanochemical carbide magnesium silicate: mechanochemical graphite oxide in the range of 1:10 to 10:1, preferably in the range of 6:1 to 1:6, preferably in the range of 3:1 to 1:3.

[0149] According to the present invention, the mechanochemically oxidized graphite preferably has

[0150] At least 50m 2 / g, preferably at least 100m 2 / g, most preferably at least 150m 2 / g range, and

[0151] a CO2 content in the range of at least 2 wt.-%, preferably at least 4 wt.-%, more preferably at least 5 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min, and

[0152] • D50 in the range of 0.01 to 50 μm, preferably 0.1 to 25 μm, most preferably 0.2 to 20 μm.

[0153] According to a preferred embodiment of the present invention, the mechanochemical graphite oxidation has

[0154] · Between 50 and 2000m 2 / g, preferably 100 to 1500m 2 / g, most preferably at least 150 to 1000 m 2 / g range, and

[0155] a CO2 content in the range of 3 to 40 wt.-%, preferably 4 to 30 wt.-%, more preferably 5 to 25 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min, and

[0156] • D50 in the range of 0.01 to 50 μm, preferably 0.1 to 25 μm, most preferably 0.2 to 20 μm.

[0157] According to a specific embodiment of the present invention, the mechanochemically oxidized graphite is a mildly mechanochemically oxidized graphite having

[0158] · Between 50 and 300m 2 / g, preferably 150 to 250m 2 / g range, and

[0159] a CO2 content in the range of 3 to 15 wt.-%, preferably 5 to 10 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min, and

[0160] • D50 in the range of 1 to 20 μm.

[0161] Such mechanochemical graphite oxide typically has a D10 in the range of 0.2 to 5 μm and a D90 in the range of 25 to 50 μm.

[0162] According to a specific embodiment of the present invention, the mechanochemical graphite oxide is a broad mechanochemical graphite oxide having

[0163] · Between 400 and 1300 m 2 / g, preferably 600 to 900m 2 / g range, and

[0164] a CO2 content in the range of 16 to 30 wt.-%, preferably 18 to 25 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min, and

[0165] • D50 in the range of 0.1 to 0.8 μm.

[0166] The mechanochemical graphite oxide described herein can be obtained by a method for producing mechanochemical graphite oxide, the method comprising the following steps:

[0167] a) providing a solid raw material comprising graphite;

[0168] b) providing a gas comprising CO2;

[0169] c) introducing the solid raw material and the gas into a mechanical stirring unit; and

[0170] d) subjecting the solid raw material to a mechanical stirring operation in the presence of the gas at a pressure of at least 1 atm in the mechanical stirring unit to obtain mechanochemical graphite oxidation.

[0171] The embodiments described in the present invention with respect to the method for producing mechanochemical magnesium carbide silicate apply mutatis mutandis to the mechanochemical graphite oxide obtainable by the method for producing mechanochemical graphite oxide. For example, the various embodiments as described herein in the background of the method for producing mechanochemical magnesium carbide silicate with respect to the identity of the gas provided in step (b) and with respect to the mechanical stirring operation of step (d) (particularly, including the presence of inert grinding or grinding media and catalyst) are equally applicable to the mechanochemical graphite oxide obtainable by the method for producing mechanochemical graphite oxide described herein and included in the composition according to various embodiments of the present invention together with the polymer.

[0172] Without wishing to be bound by any theory, the inventors believe that the CO sequestration process involved when subjecting graphite to mechanical agitation in the presence of CO generally results in the formation of graphite oxide (i.e., enriching the graphite with oxygen, thereby increasing the O / C ratio of the graphite), for example in the form of carbonyl, carboxyl, epoxy, hydroxyl, etc.

[0173] In fact, as described herein before, the gas provided in step (b) may be any gas stream containing CO2, such as ordinary air, an exhaust gas stream with a low CO2 concentration, or a concentrated CO2 stream. In an embodiment, the gas stream containing CO2 is ordinary air. In a very preferred embodiment, the gas stream containing CO2 is a combustion flue gas, in particular a flue gas from the combustion of fossil fuels, the combustion of wood particles, the combustion of biomass or the combustion of municipal waste. The fossil fuel combustion may be coal, petroleum, petroleum coke, natural gas, shale oil, asphalt, tar sand oil, or heavy oil combustion or any combination thereof. The combustion flue gas may optionally be treated to reduce the water content, SO2 content and / or NO x content.

[0174] Typical CO2 concentrations of such combustion flue gases are in the range of 1 to 15 vol%, such as 1 to 10 vol% or 2 to 10 vol%, so that preferably, the gas provided in step (b) has a CO2 concentration in the range of 1 to 15 vol%, such as 2 to 10 vol%.

[0175] In an embodiment of the present invention, the gas provided in step (b) contains less than 80% by volume of CO2, preferably less than 50% by volume of CO2. In such embodiments, the CO2 concentration in the gas can be extremely low, such as less than 1% by volume, or less than 0.1% by volume. The CO2 concentration in the gas provided in step (b) is preferably at least 0.1% by volume, more preferably at least 0.5% by volume. Typically and preferably, the low-enriched gas stream is a combustion flue gas having a CO2 concentration in the range of 1 to 15% by volume, such as 1 to 10% by volume or 2 to 10% by volume, or 2 to 5% by volume. In an alternative embodiment of the present invention, the gas provided in step (b) contains at least 80% by volume of CO2, preferably at least 95% by volume of CO2.

[0176] In some embodiments of the present invention, the gas provided in step (b) contains less than 1000 ppm (v / v) of H2O, preferably less than 100 ppm (v / v) of H2O. In a more preferred embodiment of the present invention, the gas provided in step (b) contains more than 1000 ppm (v / v) of H2O, preferably more than 10000 ppm (v / v) of H2O.

[0177] In some embodiments of the present invention, the gas provided in step (b) comprises at least 80% by volume of CO2, preferably at least 95% by volume of CO2 and less than 1000 ppm (v / v) of H2O, preferably less than 100 ppm (v / v) of H2O. In a more preferred embodiment of the present invention, the gas provided in step (b) comprises at least 80% by volume of CO2, preferably at least 95% by volume of CO2 and greater than 1000 ppm (v / v) of H2O, preferably greater than 10000 ppm (v / v) of H2O.

[0178] In some embodiments of the present invention, the gas provided in step (b) comprises 1 to 15% by volume of CO2 and less than 1000 ppm (v / v) of H2O, preferably less than 100 ppm (v / v) of H2O. In a more preferred embodiment of the present invention, the gas provided in step (b) comprises 1 to 15% by volume of CO2, and greater than 1000 ppm (v / v) of H2O, preferably greater than 10000 ppm (v / v) of H2O.

[0179] In any embodiment of the present invention, the gas provided in step (b) is generally not in a supercritical state, as this is not necessary for the mild mechanochemical carbonization process of the present invention. Therefore, in any embodiment of the present invention, it is very preferred that the gas is not in a supercritical state in any step of the process.

[0180] In an embodiment of the present invention, step (d) is carried out at a pressure of at least 3 atm, preferably at least 6 atm. In an embodiment of the present invention, step (d) is carried out at a temperature of less than 150°C, preferably less than 100°C, preferably less than 90°C, more preferably less than 80°C, most preferably less than 75°C. In a very preferred embodiment of the present invention, step (d) is carried out at a temperature in the range of 45 to 85°C, preferably 55 to 70°C. In a preferred embodiment of the present invention, active heating is not applied and any increase in temperature is attributed to friction due to mechanical stirring or to exothermic reactions occurring during mechanochemical carbonization. The temperature is preferably determined according to the solid material in the reactor (i.e., the mechanical stirring unit) during the treatment.

[0181] The low temperature requirement of the process means that fossil fuels are not required, and in case the friction caused by mechanical stirring is not sufficient to reach the desired temperature (e.g. greater than 45°C), it is practical to use electric heating elements (or low calorific value green fuel sources) to provide heat. In this way, fossil fuels can be avoided throughout the entire production chain.

[0182] In an embodiment of the present invention, step (d) is performed for at least 1 hour, preferably at least 4 hours, more preferably at least 8 hours.

[0183] As with any chemical process, suitable reaction times are highly dependent on the degree of carbonization desired, the surface area desired, and the pressure, temperature, and mechanochemical agitation applied and can be readily determined by periodically sampling the material and monitoring the progress of the reaction, for example by BET analysis, particle size analysis, amorphous content, and / or CO2 content determination as described herein.

[0184] In addition, the inventors have found that the mechanochemical carbonization method described herein can be advantageously carried out without using an additional oxidant (such as an acid). Therefore, the mechanochemical carbonization method described herein is preferably carried out without using a strong acid, preferably without using any other oxidant other than the gas provided in step (b).

[0185] In a preferred embodiment of the present invention, the mechanical stirring operation of step (d) includes milling, grinding, mixing, stirring (slow speed stirring or high speed stirring), shearing (high torque shearing), shaking, blending, fluidized bed or ultrasonic treatment, preferably milling, grinding, mixing, stirring (slow speed stirring or high speed stirring), shearing (high torque shearing) or ultrasonic treatment. The inventors have found that if the mechanochemical stirring operation of step (d) is carried out in the presence of inert milling or grinding media (preferably inert balls or beads), the mechanochemical carbonization process is convenient to carry out. A preferred inert medium is stainless steel. In such highly preferred embodiments, the mechanical stirring operation can be simply rotating a mechanical stirring unit containing solid raw materials, inert milling or grinding media and gas. This can be easily carried out in a rotating drum.

[0186] In a preferred embodiment of the present invention, step (d) is carried out in the presence of a catalyst, preferably a transition metal oxide catalyst, more preferably a transition metal dioxide catalyst, most preferably a transition metal dioxide catalyst selected from the group consisting of iron oxide, cobalt oxide, ruthenium oxide, titanium oxide, nickel oxide and a combination thereof.

[0187] Thus, as will be understood from the above, in a highly preferred embodiment of the present invention, step (d) comprises a mechanical agitation operation in the presence of an inert grinding medium and a transition metal oxide catalyst, preferably milling, grinding, mixing, stirring (slow speed stirring or high speed stirring), shearing (high torque shearing), shaking, blending, fluidized bed or ultrasonic treatment. The inventors have found that it is advantageous to use an inert medium as described above with a view to the efficiency of mechanochemical carbonization (e.g., reaction time, CO2 absorption and particle size reduction), wherein the inert medium is coated with the transition metal oxide catalyst. As described elsewhere herein, the mechanical agitation operation may be simply rotating a mechanical agitation unit containing a solid feedstock, an inert milling or grinding medium, a transition metal oxide catalyst and a gas. This can be conveniently performed in a rotating drum.

[0188] The solid starting material provided in step (a) is typically a particulate material.

[0189] Thus, as will be appreciated by the skilled artisan in view of the various preferred embodiments set out above, in a particular embodiment, the present invention provides a composition comprising:

[0190] a) a polymer, preferably a polymer selected from the group consisting of epoxy resins, phenol-formaldehyde resins, polyalkylene terephthalates (preferably polyethylene terephthalate), polyalkylene adipate terephthalates (preferably polybutylene adipate terephthalate), polyisosorbide terephthalates (preferably polyisosorbide terephthalate), polyalkylene aromatic polyamides (preferably polyethylene aromatic polyamides), polyacrylonitrile, polyacetal, polyimide, aromatic polyester, poly Isoprene (preferably cis-1,4-polyisoprene), polyethylene, polypropylene, polyurethane, polyisocyanurate, polyamide, polyether, polyester, polyhydroxyalkanoate, polylactic acid, polylactic acid-co-glycolic acid, polyvinylidene fluoride, polyvinyl acetate, polyvinyl chloride, polystyrene, polytetrafluoroethylene, acrylonitrile-butadiene-styrene, nitrile rubber, styrene-butadiene, ethylene vinyl acetate, copolymers thereof and combinations thereof, more preferably polyolefins such as polypropylene, polyethylene, copolymers thereof and combinations thereof; and

[0191] b) Mechanochemical carbide magnesium silicate having

[0192] · Between 20 and 100m 2 / g, preferably 30 to 80m 2 / g, more preferably 40 to 70m 2 / g, more preferably 45 to 65m 2 / g, and / or an amorphous content of at least 30 wt.-%, preferably at least 40 wt.-%, more preferably at least 50 wt.-%, more preferably at least 60 wt.-% as determined by XRD; and

[0193] a CO2 content of at least 3 wt.-%, preferably at least 6 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min; and

[0194] preferably a D50 in the range of 0.1 to 50 μm, preferably 1 to 25 μm, most preferably 2 to 10 μm; and

[0195] c) Mechanochemical oxidation of graphite.

[0196] The mechanochemical magnesium carbide silicate is preferably obtainable by the method for producing a mechanochemical magnesium carbide silicate as described herein.

[0197] The mechanochemical graphite oxide preferably has

[0198] · Between 50 and 2000m 2 / g, preferably 100 to 1500m 2 / g, most preferably at least 150 to 1000 m 2 / g range, and

[0199] a CO2 content in the range of 3 to 40 wt.-%, preferably 4 to 30 wt.-%, more preferably 5 to 25 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min, and

[0200] • D50 in the range of 0.01 to 50 μm, preferably 0.1 to 25 μm, most preferably 0.2 to 20 μm.

[0201] In certain embodiments, the present invention provides a composition comprising:

[0202] a) a polymer, preferably a polymer selected from the group consisting of epoxy resins, phenol-formaldehyde resins, polyalkylene terephthalates (preferably polyethylene terephthalate), polyalkylene adipate terephthalates (preferably polybutylene adipate terephthalate), polyisosorbide terephthalates (preferably polyisosorbide terephthalate), polyalkylene aromatic polyamides (preferably polyethylene aromatic polyamides), polyacrylonitrile, polyacetal, polyimide, aromatic polyester, poly Isoprene (preferably cis-1,4-polyisoprene), polyethylene, polypropylene, polyurethane, polyisocyanurate, polyamide, polyether, polyester, polyhydroxyalkanoate, polylactic acid, polylactic acid-co-glycolic acid, polyvinylidene fluoride, polyvinyl acetate, polyvinyl chloride, polystyrene, polytetrafluoroethylene, acrylonitrile-butadiene-styrene, nitrile rubber, styrene-butadiene, ethylene vinyl acetate, copolymers thereof and combinations thereof, more preferably polyolefins such as polypropylene, polyethylene, copolymers thereof and combinations thereof; and

[0203] b) Mechanochemical carbide magnesium silicate having

[0204] · Between 20 and 100m 2 / g, preferably 30 to 80m 2 / g, more preferably 40 to 70m 2 / g, more preferably 45 to 65m 2 / g, and / or an amorphous content of at least 30 wt.-%, preferably at least 40 wt.-%, more preferably at least 50 wt.-%, more preferably at least 60 wt.-% as determined by XRD; and

[0205] a CO2 content of at least 3 wt.-%, preferably at least 6 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min; and

[0206] preferably a D50 in the range of 0.1 to 50 μm, preferably 1 to 25 μm, most preferably 2 to 10 μm; and

[0207] c) mechanochemical graphite oxidation;

[0208] wherein the composition comprises at least 0.1 wt. % (based on the total weight of the composition) of mechanochemical carbide magnesium silicate, preferably at least 1 wt. % of mechanochemical carbide magnesium silicate, more preferably at least 5 wt. % of mechanochemical carbide magnesium silicate, and

[0209] wherein the composition comprises at least 0.1 wt. % (based on the total weight of the composition) of mechanochemical graphite oxide, preferably at least 1 wt. % of mechanochemical graphite oxide, more preferably at least 5 wt. % of mechanochemical graphite oxide, and

[0210] Therein, the composition comprises at least 50 wt% (based on the total weight of the composition) of the polymer, preferably at least 55 wt% of the polymer, more preferably at least 60 wt% of the polymer.

[0211] The mechanochemical magnesium carbide silicate is preferably obtainable by the method for producing a mechanochemical magnesium carbide silicate as described herein.

[0212] The mechanochemical graphite oxide preferably has

[0213] · Between 50 and 2000m 2 / g, preferably 100 to 1500m 2 / g, most preferably 150 to 1000m 2 / g range, and

[0214] a CO2 content in the range of 3 to 40 wt.-%, preferably 4 to 30 wt.-%, more preferably 5 to 25 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min, and

[0215] • D50 in the range of 0.01 to 50 μm, preferably 0.1 to 25 μm, most preferably 0.2 to 20 μm.

[0216] In certain embodiments, the present invention provides a composition comprising:

[0217] a) a polymer, preferably a polymer selected from the group consisting of epoxy resins, phenol-formaldehyde resins, polyalkylene terephthalates (preferably polyethylene terephthalate), polyalkylene adipate terephthalates (preferably polybutylene adipate terephthalate), polyisosorbide terephthalates (preferably polyisosorbide terephthalate), polyalkylene aromatic polyamides (preferably polyethylene aromatic polyamides), polyacrylonitrile, polyacetal, polyimide, aromatic polyester, poly Isoprene (preferably cis-1,4-polyisoprene), polyethylene, polypropylene, polyurethane, polyisocyanurate, polyamide, polyether, polyester, polyhydroxyalkanoate, polylactic acid, polylactic acid-co-glycolic acid, polyvinylidene fluoride, polyvinyl acetate, polyvinyl chloride, polystyrene, polytetrafluoroethylene, acrylonitrile-butadiene-styrene, nitrile rubber, styrene-butadiene, ethylene vinyl acetate, copolymers thereof and combinations thereof, more preferably polyolefins such as polypropylene, polyethylene, copolymers thereof and combinations thereof; and

[0218] b) Mechanochemical carbide magnesium silicate having

[0219] · Between 20 and 100m 2 / g, preferably 30 to 80m 2 / g, more preferably 40 to 70m 2 / g, more preferably 45 to 65m 2 / g, and / or an amorphous content of at least 30 wt.-%, preferably at least 40 wt.-%, more preferably at least 50 wt.-%, more preferably at least 60 wt.-% as determined by XRD; and

[0220] a CO2 content of at least 3 wt.-%, preferably at least 6 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min; and

[0221] preferably a D50 in the range of 0.1 to 50 μm, preferably 1 to 25 μm, most preferably 2 to 10 μm; and

[0222] c) mechanochemical graphite oxidation;

[0223] wherein the mechanochemical carbide magnesium silicate and the mechanochemical graphite oxide are contained in the composition in a combined amount of 0.1 to 40 wt % (based on the total weight of the composition), preferably 1 to 30 wt %, more preferably 5 to 25 wt %,

[0224] and

[0225] wherein the composition comprises at least 50 wt% (based on the total weight of the composition) of polymer, preferably at least 55 wt% of polymer, more preferably at least 60 wt% of polymer, and

[0226] The mechanochemical magnesium silicate carbide and the mechanochemical graphite oxide are preferably contained in the composition in a ratio (w / w) mechanochemical magnesium silicate carbide: mechanochemical graphite oxide in the range of 1:10 to 10:1, preferably in the range of 6:1 to 1:6, preferably in the range of 3:1 to 1:3.

[0227] The mechanochemical magnesium carbide silicate is preferably obtainable by the method for producing a mechanochemical magnesium carbide silicate as described herein.

[0228] The mechanochemical graphite oxide preferably has

[0229] · Between 50 and 2000m 2 / g, preferably 100 to 1500m 2 / g, most preferably at least 150 to 1000 m 2 / g range, and

[0230] a CO2 content in the range of 3 to 40 wt.-%, preferably 4 to 30 wt.-%, more preferably 5 to 25 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min, and

[0231] • D50 in the range of 0.01 to 50 μm, preferably 0.1 to 25 μm, most preferably 0.2 to 20 μm.

[0232] The luggage item or luggage accessory comprises a hardware component, wherein the hardware component comprises a hardware composition comprising a mechanochemical magnesium carbide silicate as described herein and / or a mechanochemical graphite oxide as described herein.

[0233] The present inventors have identified the importance of considering the environment in all aspects of material development and design in response to the changing needs of consumers. Current consumption patterns are changing as people want to know the origin and sustainability behind the products they buy. This brings new opportunities but also new challenges. There is a need to consider how to meet consumer expectations and in some cases how to challenge and drive new attitudes without compromising product performance.

[0234] One challenge is to address the impact of carbon emissions on our planet. Increasing CO2 levels result in air pollution and play a significant role in climate change. The inventors have developed a way to capture and store CO2 in a composition (hardware composition) used in a hardware component of a luggage article or luggage accessory using an effective and energy-efficient mechanochemical process, thereby reducing the environmental impact of the luggage article or luggage accessory. As the hardware component removes CO2 from the environment, the hardware component acts as a carbon sink. Therefore, the present invention provides a luggage article or luggage accessory comprising a hardware component, wherein the hardware component contains a hardware composition comprising stored CO2.

[0235] Another aspect of the present invention provides a luggage item or luggage accessory comprising a hardware component, wherein the hardware component contains a hardware composition comprising a mechanochemical magnesium carbide silicate as described herein and / or a mechanochemical graphite oxide as described herein. The hardware composition may be any composition as defined herein, including: a composition comprising a mechanochemical magnesium carbide silicate and a polymer as defined herein; a composition comprising a mechanochemical magnesium carbide silicate and a polymer as defined herein, which further comprises a mechanochemical graphite oxide; and a hardware composition as defined herein. For example, the hardware composition may comprise a mechanochemical magnesium carbide silicate as described herein and / or a mechanochemical graphite oxide as described herein and further comprises a polymer as described herein. In some embodiments, the hardware component consists essentially of a hardware composition as defined herein, for example, the hardware composition may be a hardware component consisting of a hardware composition as defined herein.

[0236] Waste of natural resources is also a problem to be solved. The development of consumption patterns such as the so-called fast way has driven the production of large quantities of goods using processes selected for speed, often with little consideration for material quality or sustainability. It is necessary to find a new model that breaks away from the existing model. However, there is no clear consensus on what the new model should be. One problem to be solved is that products such as luggage supplies or luggage accessories often have a variety of different uses. For example, an average consumer may have a first bag for transporting a laptop to and from a meeting, a second bag for socializing with friends, a third bag for use when going out with family, and a fourth bag for outdoor exploration. Replacing the first, second, third, and fourth bags with a multi-purpose bag reduces waste. However, the multi-purpose bag must be suitable for all intended uses, suitable for a variety of different environments (e.g., from offices to extreme temperatures and moisture levels) and strong enough to withstand more frequent use from replacing multiple bags with a single multi-purpose bag. It is applicable to any type of luggage supplies and luggage accessories and hardware components adopted according to the luggage supplies or luggage accessories. The present invention solves this point by providing hardware components as disclosed herein. Surprisingly, the inventors have found that the hardware components disclosed herein are suitable for use in a range of different scenarios and different environments and provide good material properties (such as tensile modulus, impact strength, yield stress or crystallization temperature) and good overall mechanical properties. The inventors have found that the hardware components disclosed herein are stronger and less likely to break than known hardware components used in luggage items and luggage accessories.

[0237] The inventors have also discovered that the hardware compositions disclosed herein can include recycled materials. Surprisingly, the use of recycled materials has no significant detrimental effect on the material properties (e.g., tensile modulus, impact strength, yield stress, crystallization temperature, and wear resistance) and overall mechanical properties of the hardware components. In some embodiments, the use of recycled materials improves the material properties (e.g., tensile modulus, impact strength, yield stress, crystallization temperature, and wear resistance) and overall mechanical properties of the hardware components.

[0238] Therefore, another aspect of the present invention is the use of recycled materials, such as recycled polymers and / or fillers comprising recycled rubber (e.g., recycled tire rubber), in hardware compositions, wherein the hardware compositions are as defined herein. The hardware compositions are used in hardware components as defined herein and the hardware components are used in luggage articles or luggage accessories as defined herein. Typically, the recycled material is a recycled polymer, wherein the polymer is as defined herein. Also described herein is a use of a luggage article or luggage accessory comprising a hardware component, wherein the hardware component contains a hardware composition comprising recycled materials. The recycled materials may be recycled polymers and / or fillers comprising recycled rubber.

[0239] By taking CO2 capture into account, by providing hardware components suitable for a variety of different scenarios and environments, and by using recycled materials, embodiments of the present invention provide a holistic and integrated approach to address changing consumer expectations without compromising product performance. The hardware components disclosed herein are more environmentally friendly products that will be preferred by environmentally conscious consumers.

[0240] As used herein, the term "luggage items or luggage accessories" includes backpacks, tote bags, camera bags, laptop bags, travel wallets, card holders, key chains, accessory bags, covers, inserts, notepads, sleeves, cases (including wheeled cases such as wheeled luggage cases), accessories for bags, cell phone cases, slings, raincovers, field organizers, packing cubes, camera inserts, sunglasses cases, removable watch straps for bags, camera cases, wash bags, shoe bags / bags, tech pouches, laptop sleeves, pencil cases, key chains, and bottle bags.

[0241] As used herein, the term "hardware components" includes buckles, standard buckles, magnetic snap buckles, belt pin buckles, double tongue buckles, heel bar buckles, roller bar buckles, side squeeze buckles, side release buckles, swivel snaps, o-rings, triangular loops, rectangular loops, D-rings, heavy duty D-rings, double D-rings, sewable D-rings, square double D-rings, snap loops, strap slides, loops, sewable loops, snap hook loops, adjustable slick clips, rope end hooks, adjustable hidden clips, tension hooks, hanging clips, safety triangular hooks, swiveltactical hooks, gate holders, snap hooks, triangular hooks, single gate holders, double gate holders, stable key hooks, webbing adjusters, weblocks, standard weblocks, heavy duty weblocks, webbing single bar locks, tension locks, name tags, tags, zippers, zip pullers, zip clips, zip cords, bell stoppers, webbing handles, chest clips, pipe clips and webbing ends.

[0242] Luggage articles or luggage accessories may include one or more hardware components, such as at least one, two, three, four or five hardware components. The one or more hardware components may be any hardware components as defined herein. The luggage articles or luggage accessories may, for example, include a woven or nonwoven fabric substrate and one or more hardware components, such as at least one, two, three, four or five hardware components. For example, luggage articles such as bags generally include a woven textile substrate that substantially forms a closed wall of the bag, and the bag also includes one or more hardware components, wherein the one or more hardware components (e.g., at least one, two, three, four or five hardware components) are as defined herein, such as selected from zippers, chain pull tab devices, buttons and name tags. For example, luggage articles or luggage accessories may include two or more zipper pulls and name tags. As an alternative to a woven or nonwoven fabric substrate, the luggage articles or luggage accessories may, for example, include a hard shell case.

[0243] The hardware components described herein contain a hardware composition comprising mechanochemical graphite oxide and / or mechanochemical magnesium carbide silicate. In some embodiments, the hardware composition comprises mechanochemical magnesium carbide silicate, wherein the mechanochemical magnesium carbide silicate is as described herein. The hardware composition may comprise at least 1 wt % (based on the total weight of the hardware composition) of mechanochemical magnesium carbide silicate, preferably at least 5 wt % of mechanochemical magnesium carbide silicate. In other embodiments, the hardware composition comprises mechanochemical graphite oxide, wherein the mechanochemical graphite oxide is as described herein. The hardware composition may comprise at least 1 wt % (based on the total weight of the hardware composition) of mechanochemical graphite oxide, preferably at least 5 wt % of mechanochemical graphite oxide.

[0244] Preferably, the hardware composition comprises a mechanochemical carbide magnesium silicate as described herein, wherein the hardware composition optionally further comprises a mechanochemical graphite oxide as described herein, for example, the hardware composition may comprise a mechanochemical carbide magnesium silicate as described herein and a polymer as described herein, and optionally may further comprise a mechanochemical graphite oxide as described herein.

[0245] Typically, the hardware composition comprises mechanochemical carbide magnesium silicate and mechanochemical graphite oxide, wherein the mechanochemical graphite oxide is as described herein and the mechanochemical carbide magnesium silicate is as described herein. For example, the hardware composition may comprise mechanochemical carbide magnesium silicate and mechanochemical graphite oxide, wherein the hardware composition comprises a combined amount of mechanochemical carbide magnesium silicate and mechanochemical graphite oxide of at least 1 wt % (based on the total weight of the hardware composition), preferably at least 5 wt %. Preferably, the hardware composition comprises at least 1 wt % (based on the total weight of the hardware composition) of mechanochemical graphite oxide and at least 1 wt % (based on the total weight of the hardware composition) of mechanochemical carbide magnesium silicate, more preferably at least 5 wt % of mechanochemical carbide magnesium silicate and at least 5 wt % of mechanochemical graphite oxide.

[0246] Increasing the amount of mechanochemical carbide magnesium silicate and / or mechanochemical graphite oxide in the hardware composition provides the benefit of increasing the CO2 stored in the hardware composition. The increased amount of mechanochemical carbide magnesium silicate and / or mechanochemical graphite oxide in the hardware composition can also lead to optimization of the material and mechanical properties of the hardware components comprising the hardware composition. In some embodiments, the hardware composition comprises at least 10% by weight (based on the total weight of the hardware composition) of mechanochemical carbide magnesium silicate; at least 10% by weight (based on the total weight of the hardware composition) of mechanochemical graphite oxide; or at least 10% by weight (based on the total weight of the hardware composition) of a combined amount of mechanochemical carbide magnesium silicate and mechanochemical graphite oxide. The combined amount of mechanochemical carbide magnesium silicate and mechanochemical graphite oxide employed in the hardware composition may be at least 15% by weight (based on the total weight of the hardware composition), for example, at least 20% by weight.

[0247] Preferably, the hardware composition comprises a mechanochemical carbide magnesium silicate as described herein and / or a mechanochemical graphite oxide as described herein and further comprises a polymer as described herein. The hardware composition may comprise: a mechanochemical carbide magnesium silicate and a polymer, wherein the mechanochemical carbide magnesium silicate is as described herein and the polymer is as described herein; a mechanochemical graphite oxide and a polymer, wherein the mechanochemical graphite oxide is as described herein and the polymer is as described herein; or a mechanochemical carbide magnesium silicate and a mechanochemical graphite oxide and a polymer, wherein the mechanochemical carbide magnesium silicate is as described herein, the mechanochemical graphite oxide is as described herein and the polymer is as described herein.

[0248] The hardware composition may comprise: (a) at least 1 wt % (based on the total weight of the hardware composition) of mechanochemical carbide magnesium silicate, preferably at least 5 wt % of mechanochemical carbide magnesium silicate; and / or (b) at least 1 wt % (based on the total weight of the hardware composition) of mechanochemical graphite oxide, preferably at least 5 wt % of mechanochemical graphite oxide; and (c) at least 50 wt % (based on the total weight of the hardware composition) of polymer, preferably at least 55 wt % of polymer, more preferably at least 60 wt % of polymer. Typically, the hardware composition comprises: (a) at least 1 wt % (based on the total weight of the hardware composition) of mechanochemical carbide magnesium silicate, preferably at least 5 wt % of mechanochemical carbide magnesium silicate; and (b) at least 1 wt % (based on the total weight of the hardware composition) of mechanochemical graphite oxide, preferably at least 5 wt % of mechanochemical graphite oxide; and (c) at least 50 wt % (based on the total weight of the hardware composition) of polymer, preferably at least 55 wt % of polymer, more preferably at least 60 wt % of polymer.

[0249] The hardware composition may comprise (a) 1 to 40 wt % (based on the total weight of the hardware composition) of mechanochemical carbide magnesium silicate, preferably 5 to 30 wt % of mechanochemical carbide magnesium silicate; and / or (b) 1 to 40 wt % (based on the total weight of the hardware composition) of mechanochemical graphite oxide, preferably 5 to 30 wt % of mechanochemical graphite oxide; and (c) at least 50 wt % (based on the total weight of the hardware composition) of polymer, preferably at least 55 wt % of polymer. Typically, the hardware composition comprises (a) 1 to 40 wt % (based on the total weight of the hardware composition) of mechanochemical carbide magnesium silicate, preferably 5 to 30 wt % of mechanochemical carbide magnesium silicate; and (b) 1 to 40 wt % (based on the total weight of the hardware composition) of mechanochemical graphite oxide, preferably 5 to 30 wt % of mechanochemical graphite oxide; and (c) at least 50 wt % (based on the total weight of the hardware composition) of polymer, preferably at least 55 wt % of polymer.

[0250] Preferably, the polymer is a recycled polymer. The polymer can be recycled using any known recycling technology. Preferred recycled polymers include recycled polyacetal, recycled polyethylene terephthalate, recycled polypropylene, recycled polyethylene and recycled polybutylene adipate terephthalate, copolymers thereof and combinations thereof. Highly preferred recycled polymers are recycled polyolefins, such as recycled polypropylene, recycled polyethylene, copolymers thereof and combinations thereof, particularly polypropylene. Recycled polyethylene includes recycled HDPE, recycled LDPE, recycled LLDPE, etc.

[0251] In a specific embodiment of the present invention, the hardware composition comprises mechanochemical carbide magnesium silicate and / or mechanochemical graphite oxide and a preferred polymer, and further comprises a filler selected from rubber (preferably selected from styrene-butadiene rubber, polyisoprene, chloroprene, nitrile rubber, polyisobutylene, polybutadiene and combinations thereof, preferably styrene-butadiene rubber). An example of a suitable and preferred rubber filler is recycled rubber, such as recycled tire rubber, in particular styrene-butadiene rubber from recycled tires. The rubber can be recycled using any known recycling technology. In a preferred embodiment of the present invention, the hardware composition comprises a filler selected from rubber (preferably recycled tire rubber as described herein) in an amount of at least 0.1% by weight (based on the total weight of the hardware composition), preferably at least 1% by weight. Typically, the filler selected from rubber is present in an amount of 0.1 to 10% by weight (based on the total weight of the hardware composition), preferably 1 to 8% by weight, and more preferably 4 to 6% by weight.

[0252] The hardware composition may comprise (a) at least 1 wt % (based on the total weight of the hardware composition) of mechanochemical carbide magnesium silicate, preferably at least 5 wt % of mechanochemical carbide magnesium silicate; and / or (b) at least 1 wt % (based on the total weight of the hardware composition) of mechanochemical graphite oxide, preferably at least 5 wt % of mechanochemical graphite oxide; and (c) at least 50 wt % (based on the total weight of the hardware composition) of polymer, preferably at least 55 wt % of polymer, more preferably at least 60 wt % of polymer; and (d) at least 0.1 wt % (based on the total weight of the hardware composition) of a filler selected from rubber, preferably at least 1 wt % of a filler selected from rubber Fillers of glue, for example: (a) at least 1 weight % (based on the total weight of the hardware composition) of mechanochemical carbide magnesium silicate, preferably at least 5 weight % of mechanochemical carbide magnesium silicate; and (b) at least 1 weight % (based on the total weight of the hardware composition) of mechanochemical graphite oxide, preferably at least 5 weight % of mechanochemical graphite oxide; and (c) at least 50 weight % (based on the total weight of the hardware composition) of polymer, preferably at least 55 weight % of polymer, more preferably at least 60 weight % of polymer; and (d) at least 0.1 weight % (based on the total weight of the hardware composition) of filler selected from rubber, preferably at least 1 weight % of filler selected from rubber.

[0253] In some embodiments, the hardware composition comprises (a) 1 to 40 wt % (based on the total weight of the hardware composition) of mechanochemical carbide magnesium silicate, preferably 5 to 30 wt % of mechanochemical carbide magnesium silicate; and / or (b) 1 to 40 wt % (based on the total weight of the hardware composition) of mechanochemical graphite oxide, preferably 5 to 30 wt % of mechanochemical graphite oxide; and (c) at least 50 wt % (based on the total weight of the hardware composition) of polymer, preferably at least 55 wt % of polymer; and (d) 0.1 to 10 wt % (based on the total weight of the hardware composition), preferably 1 to 8 wt %, more preferably 4 to 6 wt % of fillers selected from rubber, for example, (a) 1 to 40 wt % (based on the total weight of the hardware composition) of mechanochemical carbide magnesium silicate, preferably 5 to 30 wt % of mechanochemical carbide magnesium silicate; and (b) 1 to 40 wt % (based on the total weight of the hardware composition) of mechanochemical graphite oxide, preferably 5 to 30 wt % of mechanochemical graphite oxide; (c) at least 50 wt % (based on the total weight of the hardware composition) of polymer, preferably at least 55 wt % of polymer; and (d) 0.1 to 10 wt % (based on the total weight of the hardware composition), preferably 1 to 8 wt %, more preferably 4 to 6 wt % of fillers selected from rubber.

[0254] Preferably, the filler selected from rubber comprises recycled rubber, more preferably recycled tire rubber. In a particularly environmentally friendly embodiment of the present invention, the hardware composition comprises a recycled polymer as defined herein and a recycled rubber as defined herein (eg recycled tire rubber).

[0255] Examples of hardware components containing a hardware composition comprising a mechanochemical carbide magnesium silicate as described and a polymer as described herein and a mechanochemical graphite oxide as described herein include:

[0256] A hardware component, such as a nameplate, comprising a hardware composition comprising about 10 wt % (based on the total weight of the hardware composition) of mechanochemical carbide magnesium silicate; about 20 wt % (based on the total weight of the hardware composition) of mechanochemical graphite oxide; about 65 wt % (based on the total weight of the hardware composition) of polyethylene (such as HDPE); and about 5 wt % (based on the total weight of the hardware composition) of a rubber as described herein, preferably recycled tire rubber.

[0257] A hardware component, such as a zip-puller, comprising a hardware composition comprising about 15 wt % (based on the total weight of the hardware composition) of mechanochemical carbide magnesium silicate; about 10 wt % (based on the total weight of the hardware composition) of mechanochemical graphite oxide; about 70 wt % (based on the total weight of the hardware composition) of polyethylene; and about 5 wt % (based on the total weight of the hardware composition) of a rubber as described herein, preferably recycled tire rubber.

[0258] A hardware component, such as a zipper pull, comprising a hardware composition comprising about 15 wt % (based on the total weight of the hardware composition) of mechanochemical carbide magnesium silicate; about 10 wt % (based on the total weight of the hardware composition) of mechanochemical graphite oxide; about 67 wt % (based on the total weight of the hardware composition) of polyethylene; and about 5 wt % (based on the total weight of the hardware composition) of a rubber as described herein, preferably recycled tire rubber.

[0259] A particularly preferred example of the hardware components is:

[0260] A hardware component, such as a zipper pull, comprising a hardware composition comprising about 15 wt % (based on the total weight of the hardware composition) of mechanochemical carbide magnesium silicate; about 10 wt % (based on the total weight of the hardware composition) of mechanochemical graphite oxide; about 67 wt % (based on the total weight of the hardware composition) of polyethylene; and about 5 wt % (based on the total weight of the hardware composition) of a rubber as described herein, preferably recycled tire rubber.

[0261] Method for the co-production of mechanochemical magnesium carbide silicate and mechanochemical graphite oxide

[0262] As described elsewhere herein, the present inventors have found that it is desirable to provide a composition comprising a mechanochemical magnesium carbide silicate, a mechanochemical graphite oxide and a polymer. Such compositions have been described in detail in the previous paragraphs. The present inventors have also found that it is advantageous if the mechanochemical magnesium carbide silicate and the mechanochemical graphite oxide are co-produced, thereby obtaining a mixture of the mechanochemical magnesium carbide silicate and the mechanochemical graphite oxide. Such a mixture can be used in a polymer composition as described above.

[0263] Thus, in another aspect, the present invention provides a mixture of mechanochemically carbided magnesium silicate and mechanochemically graphite oxide. The mechanochemically carbided magnesium silicate and mechanochemically graphite oxide preferably have the properties described elsewhere herein.

[0264] In another aspect, the present invention provides a method for co-manufacturing a mixture of mechanochemical carbide magnesium silicate and mechanochemical graphite oxide as described herein, comprising the steps of:

[0265] a) providing a solid raw material comprising magnesium silicate and graphite;

[0266] b) providing a gas comprising CO2;

[0267] c) introducing the solid raw material and the gas into a mechanical stirring unit; and

[0268] d) subjecting the solid raw material to a mechanical stirring operation in the presence of the gas at a pressure of at least 1 atm in the mechanical stirring unit to obtain a mixture of mechanochemical magnesium carbide silicate and mechanochemical graphite oxide.

[0269] Those skilled in the art can adjust the relevant process parameters according to the guidance provided in the present invention to obtain mechanochemical magnesium carbide silicate and mechanochemical graphite oxide having the properties listed in this article.

[0270] The embodiments described in the present invention with respect to the method for producing mechanochemical magnesium carbide silicate apply mutatis mutandis to the method for co-producing mechanochemical magnesium carbide silicate and mechanochemical graphite oxide. For example, the various embodiments as described herein in the background of the method for producing mechanochemical magnesium carbide silicate with respect to the identity of the gas provided in step (b) and with respect to the mechanical stirring operation of step (d) (particularly, including the presence of inert grinding or grinding media and catalyst) are also applicable to the method for co-producing mechanochemical magnesium carbide silicate and mechanochemical graphite oxide described herein and included in the composition according to various embodiments of the present invention together with the polymer.

[0271] In an embodiment of the present invention, the magnesium silicate contained in the solid raw material (preferably the entire solid raw material) has a moisture content of less than 3 wt%, preferably less than 2 wt%, more preferably less than 1 wt% and / or a D50 in the range of 0.1 to 500 μm, preferably in the range of 0.2 to 50 μm.

[0272] The gas provided in step (b) may be any gas stream containing CO2, such as normal air, a waste gas stream with a low CO2 concentration, or a concentrated CO2 stream. In an embodiment, the gas stream containing CO2 is normal air. In a very preferred embodiment, the gas stream containing CO2 is a combustion flue gas, in particular a flue gas from the combustion of fossil fuels, the combustion of wood particles, the combustion of biomass or the combustion of municipal waste. The fossil fuel combustion may be coal, petroleum, petroleum coke, natural gas, shale oil, asphalt, tar sand oil, or heavy oil combustion or any combination thereof. The combustion flue gas may optionally be treated to reduce the water content, SO2 content and / or NO x content.

[0273] Typical CO2 concentrations of such combustion flue gases are in the range of 1 to 15 vol%, such as 1 to 10 vol% or 2 to 10 vol%, so that preferably, the gas provided in step (b) has a CO2 concentration in the range of 1 to 15 vol%, such as 2 to 10 vol%.

[0274] In an embodiment of the present invention, the gas provided in step (b) contains less than 80% by volume of CO2, preferably less than 50% by volume of CO2. In such embodiments, the CO2 concentration in the gas can be extremely low, such as less than 1% by volume, or less than 0.1% by volume. The CO2 concentration in the gas provided in step (b) is preferably at least 0.1% by volume, more preferably at least 0.5% by volume. Typically and preferably, the low-enriched gas stream is a combustion flue gas having a CO2 concentration in the range of 1 to 15% by volume, such as 1 to 10% by volume or 2 to 10% by volume, or 2 to 5% by volume. In an alternative embodiment of the present invention, the gas provided in step (b) contains at least 80% by volume of CO2, preferably at least 95% by volume of CO2.

[0275] In some embodiments of the present invention, the gas provided in step (b) contains less than 1000 ppm (v / v) of H2O, preferably less than 100 ppm (v / v) of H2O. In a more preferred embodiment of the present invention, the gas provided in step (b) contains more than 1000 ppm (v / v) of H2O, preferably more than 10000 ppm (v / v) of H2O.

[0276] In some embodiments of the present invention, the gas provided in step (b) comprises at least 80% by volume of CO2, preferably at least 95% by volume of CO2 and less than 1000 ppm (v / v) of H2O, preferably less than 100 ppm (v / v) of H2O. In a more preferred embodiment of the present invention, the gas provided in step (b) comprises at least 80% by volume of CO2, preferably at least 95% by volume of CO2 and greater than 1000 ppm (v / v) of H2O, preferably greater than 10000 ppm (v / v) of H2O.

[0277] In some embodiments of the present invention, the gas provided in step (b) comprises 1 to 15% by volume of CO2 and less than 1000 ppm (v / v) of H2O, preferably less than 100 ppm (v / v) of H2O. In a more preferred embodiment of the present invention, the gas provided in step (b) comprises 1 to 15% by volume of CO2, and greater than 1000 ppm (v / v) of H2O, preferably greater than 10000 ppm (v / v) of H2O.

[0278] In any embodiment of the present invention, the gas provided in step (b) is generally not in a supercritical state, as this is not necessary for the mild mechanochemical carbonization process of the present invention. Therefore, in any embodiment of the present invention, it is very preferred that the gas is not in a supercritical state in any step of the process.

[0279] In an embodiment of the present invention, step (d) is carried out at a pressure of at least 3 atm, preferably at least 6 atm. In an embodiment of the present invention, step (d) is carried out at a temperature of less than 150°C, preferably less than 100°C, preferably less than 90°C, more preferably less than 80°C, most preferably less than 75°C. In a very preferred embodiment of the present invention, step (d) is carried out at a temperature in the range of 45 to 85°C, preferably 55 to 70°C. In a preferred embodiment of the present invention, active heating is not applied and any increase in temperature is attributed to friction due to mechanical stirring or to exothermic reactions occurring during mechanochemical carbonization. The temperature is preferably determined according to the solid material in the reactor (i.e., the mechanical stirring unit) during the treatment.

[0280] The low temperature requirement of the process means that fossil fuels are not required, and in case the friction caused by mechanical stirring is not sufficient to reach the desired temperature (e.g. greater than 45°C), it is practical to use electric heating elements (or low calorific value green fuel sources) to provide heat. In this way, fossil fuels can be avoided throughout the entire production chain.

[0281] In an embodiment of the present invention, step (d) is performed for at least 1 hour, preferably at least 4 hours, more preferably at least 8 hours.

[0282] As with any chemical process, suitable reaction times are highly dependent on the degree of carbonization desired, the surface area desired, and the pressure, temperature, and mechanochemical agitation applied and can be readily determined by periodically sampling the material and monitoring the progress of the reaction, for example by BET analysis, particle size analysis, and CO2 content determination as described herein.

[0283] In addition, the inventors have found that the mechanochemical carbonization method described herein can be advantageously carried out without using an additional oxidant such as an acid. Therefore, the mechanochemical carbonization method described herein is preferably carried out without using a strong acid, preferably without using any other oxidant other than the gas provided in step (b).

[0284] In a preferred embodiment of the present invention, the mechanical stirring operation of step (d) comprises milling, grinding, mixing, stirring (slow speed stirring or high speed stirring), shearing (high torque shearing), oscillation, blending, fluidized bed or ultrasonic treatment, preferably milling, grinding, mixing, stirring (slow speed stirring or high speed stirring), shearing (high torque shearing) or ultrasonic treatment. The inventors have found that if the mechanochemical stirring operation of step (d) is carried out in the presence of inert milling or grinding media (preferably inert balls or beads), the mechanochemical carbonization process is convenient to carry out. A preferred inert medium is stainless steel. In such a very preferred embodiment, the mechanical stirring operation can be simply rotating a mechanical stirring unit containing solid raw materials, inert milling or grinding media and gas. This can be easily carried out in a rotating drum.

[0285] In a preferred embodiment of the present invention, step (d) is carried out in the presence of a catalyst, preferably a transition metal oxide catalyst, more preferably a transition metal dioxide catalyst, most preferably a transition metal dioxide catalyst selected from the group consisting of iron oxide, cobalt oxide, ruthenium oxide, titanium oxide, nickel oxide and a combination thereof.

[0286] Thus, as will be understood from the above, in a very preferred embodiment of the present invention, step (d) comprises a mechanical agitation operation in the presence of an inert grinding medium and a transition metal oxide catalyst, preferably milling, grinding, mixing, stirring (slow speed stirring or high speed stirring), shearing (high torque shearing), shaking, blending, fluidized bed or ultrasonic treatment. The inventors have found that it is advantageous to use an inert medium as described above with a view to the efficiency of mechanochemical carbonization (e.g., reaction time, CO2 absorption and particle size reduction), wherein the inert medium is coated with the transition metal oxide catalyst. As described elsewhere herein, the mechanical agitation operation may be simply rotating a mechanical agitation unit containing a solid feedstock, an inert milling or grinding medium, a transition metal oxide catalyst and a gas. This can be conveniently performed in a rotating drum.

[0287] The solid starting material provided in step (a) is typically a particulate material.

[0288] In a very preferred embodiment of the present invention, the mechanochemical carbide magnesium silicate and the mechanochemical graphite oxide are contained in the mixture obtained in step (d) in a ratio (w / w) mechanochemical carbide magnesium silicate: mechanochemical graphite oxide in the range of 1:10 to 10:1, preferably in the range of 6:1 to 1:6, preferably in the range of 3:1 to 1:3. The combined amount of the mechanochemical carbide magnesium silicate and the mechanochemical graphite oxide in the mixture obtained in step (d) is preferably at least 80% by weight (based on the total weight of the mixture), more preferably at least 90% by weight, most preferably at least 95% by weight.

[0289] The mechanochemical magnesium carbide silicate contained in the mixture obtained in step (d) preferably has

[0290] · Between 20 and 100m 2 / g, preferably 30 to 80m 2 / g, more preferably 40 to 70m 2 / g, more preferably 45 to 65m 2 / g, and / or an amorphous content of at least 30 wt.-%, preferably at least 40 wt.-%, more preferably at least 50 wt.-%, more preferably at least 60 wt.-% as determined by XRD; and

[0291] a CO2 content of at least 3 wt.-%, preferably at least 6 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min; and

[0292] Preferably, a D50 in the range of 0.1 to 50 μm, preferably 1 to 25 μm, most preferably 2 to 10 μm;

[0293] and

[0294] The mechanochemical graphite oxide contained in the mixture obtained in step (d) preferably has

[0295] · Between 50 and 2000m 2 / g, preferably 100 to 1500m 2 / g, most preferably at least 150 to 1000 m 2 / g range, and

[0296] a CO2 content in the range of 3 to 40 wt.-%, preferably 4 to 30 wt.-%, more preferably 5 to 25 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min, and

[0297] • D50 in the range of 0.01 to 50 μm, preferably 0.1 to 25 μm, most preferably 0.2 to 20 μm.

[0298] In another aspect, the present invention provides a mixture of mechanochemical magnesium carbide silicate and mechanochemical graphite oxide obtainable by a method for co-manufacturing a mixture of mechanochemical magnesium carbide silicate and mechanochemical graphite oxide as described herein. The mechanochemical magnesium carbide silicate is preferably obtainable by a method for manufacturing a mechanochemical magnesium carbide silicate as described herein, wherein the process is performed such that the mechanochemical magnesium carbide silicate contained in the mixture obtained in step (d) has

[0299] · Between 20 and 100m 2 / g, preferably 30 to 80m 2 / g, more preferably 40 to 70m 2 / g, more preferably 45 to 65m 2 / g, and / or an amorphous content of at least 30 wt.-%, preferably at least 40 wt.-%, more preferably at least 50 wt.-%, more preferably at least 60 wt.-% as determined by XRD; and

[0300] a CO2 content of at least 3 wt.-%, preferably at least 6 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min; and

[0301] Preferably, a D50 in the range of 0.1 to 50 μm, preferably 1 to 25 μm, most preferably 2 to 10 μm;

[0302] and

[0303] The mechanochemical graphite oxide contained in the mixture obtained in step (d) has

[0304] · Between 50 and 2000m 2 / g, preferably 100 to 1500m 2 / g, most preferably at least 150 to 1000 m 2 / g range, and

[0305] a CO2 content in the range of 3 to 40 wt.-%, preferably 4 to 30 wt.-%, more preferably 5 to 25 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min, and

[0306] • D50 in the range of 0.01 to 50 μm, preferably 0.1 to 25 μm, most preferably 0.2 to 20 μm.

[0307] Process for preparing a composition comprising mechanochemical magnesium carbide silicate and a polymer

[0308] In another aspect, the present invention provides a method for preparing a composition as described herein, comprising the steps of:

[0309] (i) providing a mechanochemical magnesium carbide silicate as described herein;

[0310] (ii) providing a polymer as described herein;

[0311] (iii) optionally providing mechanochemical graphite oxidation as described herein; and

[0312] (iv) combining the mechanochemical carbide magnesium silicate of step (i) with the polymer of step (ii) and optionally the mechanochemical graphite oxide of step (iii).

[0313] In an embodiment, step (iv) comprises dry blending the materials of steps (i) to (iii) and extruding the resulting mixture. In such a method, simultaneous co-extrusion of the mechanochemical carbide magnesium silicate of step (i) with the polymer of step (ii) and optionally with the mechanochemical graphite oxide of step (iii) can be achieved.

[0314] In an alternative embodiment, the polymer provided in step (ii) may be extruded first, such that step (iv) comprises adding the materials of step (i) and optionally step (iii) to the plasticized polymer.

[0315] The additives (such as fillers, light stabilizers, heat stabilizers, compatibilizers, antioxidants, rheology modifiers (such as plasticizers), impact modifiers, flame retardants, lubricants and / or antistatic agents) can be added at any point throughout the process, typically, they are added in step (iv) together with the materials of steps (i) to (iii). Preferably, a rubber filler as previously described herein is added.

[0316] The skilled person will appreciate that the embodiments of the invention described herein in the context of the composition of the invention, in particular with respect to the characteristics of the mechanochemical magnesium carbide silicate, the mechanochemical graphite oxide, the polymer or with respect to the amounts of each material used, are equally applicable to the method for preparing the composition described herein.

[0317] Method for preparing a luggage article or accessory

[0318] The present invention also provides a method for preparing a luggage item or luggage accessory as defined herein comprising a hardware component as defined herein, wherein the hardware component comprises a hardware composition as defined herein, the method comprising the steps of:

[0319] (i) providing a mechanochemical magnesium silicate carbide as described herein; or providing a mechanochemical graphite oxide as described herein; or providing a mechanochemical magnesium silicate carbide as described herein and a mechanochemical graphite oxide as described herein;

[0320] (ii) providing a polymer as described herein;

[0321] (iii) optionally providing a filler selected from rubbers as described herein; and

[0322] (iv) combining the mechanochemical carbide magnesium silicate and / or mechanochemical graphite oxide of step (i) with the polymer of step (ii) and optionally a filler selected from rubber of step (iii), thereby obtaining a hardware composition comprising the mechanochemical carbide magnesium silicate and / or mechanochemical graphite oxide, the polymer and optionally a filler selected from rubber;

[0323] (v) using the hardware composition obtained in step (iv) in a hardware component of a luggage item or luggage accessory.

[0324] Preferably, the method comprises the following steps:

[0325] (i) providing a mechanochemical carbide magnesium silicate as described herein and optionally a mechanochemical graphite oxide as described herein;

[0326] (ii) providing a polymer as described herein;

[0327] (iii) optionally providing a filler selected from rubbers as described herein; and

[0328] (iv) combining the mechanochemical carbide magnesium silicate and optionally mechanochemical graphite oxide of step (i) with the polymer of step (ii) and optionally a filler selected from rubber of step (iii), thereby obtaining a hardware composition comprising: mechanochemical carbide magnesium silicate and optionally mechanochemical graphite oxide; polymer; and optionally a filler selected from rubber;

[0329] (v) using the hardware composition obtained in step (iv) in a hardware component of a luggage item or luggage accessory.

[0330] In an embodiment, step (iv) comprises dry blending the materials of steps (i) to (iii) and extruding the resulting mixture. In this method, simultaneous co-extrusion of the mechanochemical carbide magnesium silicate and / or mechanochemical graphite oxide of step (i) with the polymer of step (ii) and optionally with the filler of step (iii) can be achieved.

[0331] In an alternative embodiment, the polymer provided in step (ii) may be extruded first, such that step (iv) comprises adding the materials of step (i) and optionally step (iii) to the plasticized polymer.

[0332] Additives (such as additional fillers, light stabilizers, heat stabilizers, compatibilizers, antioxidants, rheology modifiers (such as plasticizers), impact modifiers, flame retardants, lubricants and / or antistatic agents) may be added at any point throughout the process, typically, they are added in step (iv) together with the materials of steps (i) to (iii).

[0333] It will be understood by those skilled in the art that the embodiments of the invention described herein in the context of the compositions of the invention (including hardware compositions), particularly with respect to the characteristics of the mechanochemical carbide magnesium silicate, the mechanochemical graphite oxide, the polymers, or with respect to the amounts of each material used, are equally applicable to the methods for preparing the hardware compositions described herein.

[0334] Mechanochemical Uses of Magnesium Carbide Silicate

[0335] In another aspect, the present invention provides a use of a mechanochemical carbide magnesium silicate as described herein:

[0336] Used as filler in polymers;

[0337] Increase the crystallization temperature of the polymer;

[0338] Increase the tensile modulus of the polymer;

[0339] Increase the yield stress of the polymer; and / or

[0340] Increase the impact strength of polymers.

[0341] Preferably, the use of the present invention is provided, wherein the polymer is selected from the group consisting of: epoxy resins, phenol-formaldehyde resins, polyalkylene terephthalates (preferably polyethylene terephthalate), polyalkylene adipate terephthalates (preferably polybutylene adipate terephthalate), polyisosorbide terephthalates (preferably polyisosorbide terephthalate), polyalkylene aromatic polyamides (preferably polyethylene aromatic polyamides), polyacrylonitrile , polyacetal, polyimide, aromatic polyester, polyisoprene (preferably cis-1,4-polyisoprene), polyethylene, polypropylene, polyurethane, polyisocyanurate, polyamide, polyether, polyester, polyhydroxyalkanoate, polylactic acid, polylactic acid-co-glycolic acid, polyvinylidene fluoride, polyvinyl acetate, polyvinyl chloride, polystyrene, polytetrafluoroethylene, acrylonitrile-butadiene-styrene, nitrile rubber, styrene-butadiene, ethylene vinyl acetate, copolymers thereof and combinations thereof. Notably, the copolymer is a homogeneous or heterogeneous PE-PP copolymer. The polymer is preferably selected from polyacetal, polyethylene terephthalate, polypropylene, polyethylene and polybutylene adipate terephthalate, copolymers thereof and combinations thereof. Very preferably, polyolefins such as polypropylene, polyethylene, copolymers thereof and combinations thereof, in particular polypropylene. Polyethylene includes HDPE, LDPE, LLDPE, etc.

[0342] In a particular embodiment of the present invention, the use of the present invention is provided, comprising the use of a mechanochemical magnesium carbide silicate in a composition comprising a mechanochemical magnesium carbide silicate and a polymer, wherein the mechanochemical magnesium carbide silicate is present in an amount of at least 0.1 wt.-% (based on the total weight of the composition), preferably at least 1 wt.-%, more preferably at least 5 wt.-% and / or wherein the polymer is present in an amount of at least 50 wt.-% (based on the total weight of the composition), preferably at least 60 wt.-%, more preferably at least 70 wt.-%.

[0343] In a particular embodiment of the present invention, there is provided the use of a mechanochemical magnesium carbide silicate as described herein to increase the crystallization temperature of a polymer, comprising the use of a mechanochemical magnesium carbide silicate in a composition comprising a mechanochemical magnesium carbide silicate and a polymer, wherein the mechanochemical magnesium carbide silicate is present in an amount of at least 3% by weight (based on the total weight of the composition), preferably at least 4% by weight. Preferably, the use increases the crystallization temperature of the polymer by at least 2.5°C compared to the same composition without the mechanochemical magnesium carbide silicate.

[0344] In a particular embodiment of the present invention, there is provided the use of a mechanochemical magnesium carbide silicate as described herein to increase the tensile modulus of a polymer, comprising the use of a mechanochemical magnesium carbide silicate in a composition comprising a mechanochemical magnesium carbide silicate and a polymer, wherein the mechanochemical magnesium carbide silicate is present in an amount of at least 13% by weight (based on the total weight of the composition), preferably at least 14% by weight. Preferably, the use increases the tensile modulus of the polymer by at least 30%, preferably at least 40%, compared to the same composition without the mechanochemical magnesium carbide silicate.

[0345] In a particular embodiment of the present invention, there is provided the use of a mechanochemical magnesium carbide silicate as described herein to increase the tensile modulus of a polymer without reducing the impact strength, comprising the use of a mechanochemical magnesium carbide silicate in a composition comprising a mechanochemical magnesium carbide silicate and a polymer, wherein the mechanochemical magnesium carbide silicate is present in an amount of 3 to 13 wt % (based on the total weight of the composition), preferably 4 to 12 wt %. Preferably, the use increases the tensile modulus of the polymer by at least 30% and increases the impact strength by at least 10% compared to the same composition without the mechanochemical magnesium carbide silicate.

[0346] In a preferred embodiment of the present invention, there is provided a use of a combination of a mechanochemical carbide magnesium silicate as described herein and a mechanochemical graphite oxide as described herein:

[0347] Used as filler in polymers;

[0348] Increase the crystallization temperature of the polymer;

[0349] Increase the tensile modulus of the polymer;

[0350] Increase the yield stress of the polymer; and / or

[0351] Increase the impact strength of polymers.

[0352] In a preferred embodiment of the present invention, there is provided a use of a combination of a mechanochemical magnesium carbide silicate as described herein and a mechanochemical graphite oxide as described herein as a filler in a polymer to provide a dark color, such as to provide a black polymer composition.

[0353] In some embodiments of the present invention, there is provided a use of a mechanochemical carbide magnesium silicate as described herein for reducing the CO2 impact of a polymer, for providing carbon storage in a polymer, or for use as a CO2-negative emission filler.

[0354] In particularly preferred embodiments, the mechanochemical magnesium carbide silicate is used as a filler for a polymer which is a hardware composition employed in the manufacture of a hardware component for a luggage piece or luggage accessory, wherein the hardware component is as defined herein and the luggage piece or luggage accessory is as defined herein.

[0355] The skilled person will appreciate that embodiments of the invention described herein in the context of the composition of the invention, in particular with respect to the characteristics of the mechanochemical magnesium carbide silicate, the mechanochemical graphite oxide, the polymer or with respect to the amounts of each material used, are equally applicable to the uses described herein.

[0356] In another aspect, the present invention provides a method of:

[0357] Increase the crystallization temperature of the polymer;

[0358] Increase the tensile modulus of the polymer;

[0359] Increase the yield stress of the polymer; and / or

[0360] Increase the impact strength of polymers,

[0361] wherein the method comprises adding a mechanochemical magnesium carbide silicate as described herein to the polymer.

[0362] Preferably, the method of the present invention is provided, wherein the polymer is selected from the group consisting of: epoxy resin, phenol-formaldehyde resin, polyalkylene terephthalate (preferably polyethylene terephthalate), polyalkylene adipate terephthalate (preferably polybutylene adipate terephthalate), polyisosorbide terephthalate (preferably polyisosorbide terephthalate), polyalkylene aromatic polyamide (preferably polyethylene aromatic polyamide), polyacrylonitrile , polyacetal, polyimide, aromatic polyester, polyisoprene (preferably cis-1,4-polyisoprene), polyethylene, polypropylene, polyurethane, polyisocyanurate, polyamide, polyether, polyester, polyhydroxyalkanoate, polylactic acid, polylactic acid-co-glycolic acid, polyvinylidene fluoride, polyvinyl acetate, polyvinyl chloride, polystyrene, polytetrafluoroethylene, acrylonitrile-butadiene-styrene, nitrile rubber, styrene-butadiene, ethylene vinyl acetate, copolymers thereof and combinations thereof. Notably, the copolymer is a homogeneous or heterogeneous PE-PP copolymer. The polymer is preferably selected from polyacetal, polyethylene terephthalate, polypropylene, polyethylene and polybutylene adipate terephthalate, copolymers thereof and combinations thereof. Very preferably, polyolefins such as polypropylene, polyethylene, copolymers thereof and combinations thereof, in particular polypropylene. Polyethylene includes HDPE, LDPE, LLDPE, etc.

[0363] In a particular embodiment of the present invention, a method according to the present invention is provided, which comprises adding the mechanochemical magnesium carbide silicate to a polymer, thereby obtaining a composition comprising the mechanochemical magnesium carbide silicate and a polymer, wherein the mechanochemical magnesium carbide silicate is present in an amount of at least 0.1 wt.-% (based on the total weight of the composition), preferably at least 1 wt.-%, more preferably at least 5 wt.-% and / or wherein the polymer is present in an amount of at least 50 wt.-% (based on the total weight of the composition), preferably at least 55 wt.-%, more preferably at least 60 wt.-%.

[0364] In a particular embodiment of the present invention, there is provided a method of increasing the crystallization temperature of a polymer according to the present invention, comprising adding the mechanochemical magnesium carbide silicate to a polymer, thereby obtaining a composition comprising the mechanochemical magnesium carbide silicate and a polymer, wherein the mechanochemical magnesium carbide silicate is present in an amount of at least 3% by weight (based on the total weight of the composition), preferably at least 4% by weight. Preferably, the method increases the crystallization temperature of the polymer by at least 2.5°C compared to the same composition without the mechanochemical magnesium carbide silicate.

[0365] In a particular embodiment of the present invention, there is provided a method of increasing the tensile modulus of a polymer according to the present invention, comprising adding the mechanochemical magnesium carbide silicate to a polymer, thereby obtaining a composition comprising the mechanochemical magnesium carbide silicate and a polymer, wherein the mechanochemical magnesium carbide silicate is present in an amount of at least 13% by weight (based on the total weight of the composition), preferably at least 14% by weight. Preferably, the method increases the tensile modulus of the polymer by at least 30%, preferably at least 40%, compared to the same composition without the mechanochemical magnesium carbide silicate.

[0366] In a particular embodiment of the present invention, there is provided a method of the present invention for increasing the tensile modulus of a polymer without reducing the impact strength, comprising adding the mechanochemical magnesium carbide silicate to a polymer, thereby obtaining a composition comprising the mechanochemical magnesium carbide silicate and a polymer, wherein the mechanochemical magnesium carbide silicate is present in an amount of 3 to 13 wt % (based on the total weight of the composition), preferably 4 to 12 wt %. Preferably, the method increases the tensile modulus of the polymer by at least 30% and increases the impact strength by at least 10% compared to the same composition without the mechanochemical magnesium carbide silicate.

[0367] In a preferred embodiment of the present invention, a following method is provided:

[0368] Increase the crystallization temperature of the polymer;

[0369] Increase the tensile modulus of the polymer;

[0370] Increase the yield stress of the polymer;

[0371] Increase the impact strength of polymers,

[0372] The method comprises adding a combination of mechanochemical carbide magnesium silicate and mechanochemical graphite oxide as described herein to the polymer.

[0373] In a preferred embodiment of the present invention, there is provided a method of providing a dark color to a polymer comprising adding a combination of a mechanochemically carbided magnesium silicate as described herein and a mechanochemically oxidized graphite as described herein to the polymer.

[0374] In some embodiments of the present invention, there is provided a method for reducing the CO2 shock of a polymer, or for providing carbon storage in a polymer, the method comprising adding a mechanochemical carbide magnesium silicate as described herein to the polymer.

[0375] In a particularly preferred embodiment, a method for providing a luggage item or luggage accessory is provided, wherein the luggage item or luggage accessory is as defined herein, the method comprising adding a mechanochemical magnesium carbide silicate as described herein and / or a mechanochemical graphite oxide as described herein to a polymer, thereby obtaining a hardware composition comprising a mechanochemical magnesium carbide silicate and / or a mechanochemical graphite oxide and a polymer, and using the hardware composition as a hardware component of the luggage item or luggage accessory, wherein the hardware component is as defined herein. Preferably, the material properties (e.g., tensile modulus, impact strength, yield stress, crystallization temperature, and abrasion resistance) and overall mechanical properties of the hardware component are substantially the same as those seen for the virgin polymer. In some embodiments, the material properties (e.g., tensile modulus, impact strength, yield stress, crystallization temperature, and abrasion resistance) and overall mechanical properties of the hardware component are improved when compared to the virgin polymer.

[0376] The skilled person will appreciate that embodiments of the invention described herein in the context of the compositions of the invention, in particular with respect to the characteristics of the mechanochemical magnesium carbide silicate, the mechanochemical graphite oxide, the polymer or with respect to the amounts of each material used, are equally applicable to the methods described herein.

[0377] Examples

[0378] BET surface area, BJH desorption cumulative pore surface area and desorption average pore width (4 V / A by BET) were determined using nitrogen at 77 K using 0.5 to 1 g of sample mass spectrometry, where the sample was heated to 400° C. for desorption cycles prior to surface area analysis.

[0379] Amorphous content by X-ray diffraction (XRD) was performed using corundum standards. XRD data were collected using a PANalyticalAeris X-ray diffractometer. XRD analysis and Rietveld refinement were performed using HighScore Plus XRD analysis software.

[0380] Particle size distribution measurements were performed on a Fritsch Analysette 22 Nanotec using Fraunhofer diffraction theory.

[0381] The CO2 content was determined as the mass loss above 200°C measured by TGA using a temperature trace, where the temperature was increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min using a Setaram TAG 16 TGA / DSC dual chamber balance with 0.1 to 2 mg sample.

[0382] The tensile modulus is measured as Young's modulus according to ASTM 638 (2014).

[0383] The yield stress is determined as the pressure exhibited at yield as determined according to ASTM 638 (2014).

[0384] The impact strength is measured according to the Sandvik impact test of ASTM D6110 (2018).

[0385] Example 1

[0386] Mechanochemical carbide magnesium silicate was produced by inserting a 20 gram sample of hydrated magnesium silicate powder into a pressure cell with 1400 grams of inert medium (stainless steel ball) coated with titanium dioxide. The pressure cell was pressurized to 0.27 MPa (4.08 atm) using a gas composition consisting of 80 mol % CO2 and 20 mol % air, placed in a high energy ball mill and rotated at 65 RPM for 72 hours. The reaction was initiated at room temperature and no heating or cooling was applied.

[0387] The native magnesium silicate (ie before it was subjected to mechanochemical carbonisation) had a mass loss above 200°C of less than 2 wt% as measured by TGA as described herein (the inventors assume that the mass loss may be mainly water loss).

[0388] Example 2

[0389] The polymer composition was prepared by dry blending the mechanochemical magnesium carbide silicate of Example 1 with injection grade homogeneous polypropylene. The solid mixture was fed into the hopper section of a co-rotating twin-screw extruder. The extruder was operated with a temperature gradient of 210° C. to 120° C. from the die to the throat section, respectively. The engine RPM was set to 100 RPM and the feed was set to 6 RPM. The polymer and mechanochemical magnesium carbide silicate mixture were conveyed to the extruder and melt mixed throughout the extruder to produce a continuous solid strand leaving the extruder. The extrudate was then passed through a water cooling tank, followed by a vacuum / blower drying tube, and finally granulated. The properties of the resulting material are as follows.

[0390]

[0391] Example 3

[0392] The polymer composition was prepared by dry blending the mechanochemical magnesium carbide silicate of Example 1 with post-industrial recycled high density polyethylene. The solid mixture was fed into the hopper section of a co-rotating twin-screw extruder. The extruder was operated with a temperature gradient of 180° C. to 100° C. from the die to the throat section, respectively. The engine RPM was set to 100 RPM and the feed was set to 6 RPM. The polymer and mechanochemical magnesium carbide silicate mixture were conveyed into the extruder and melt mixed throughout the extruder to produce a continuous solid strand exiting the extruder. The extrudate was then passed through a water cooling tank, followed by a vacuum / blower drying tube, and finally granulated.

[0393]

[0394] Example 4

[0395] The surface modified mechanochemical carbide magnesium silicate is produced by reacting the mechanochemical carbide magnesium silicate of Example 1 with a metal organic compatibilizer in ethanol and removing the solvent. The polymer composition is prepared by dry blending the obtained surface modified mechanochemical carbide magnesium silicate with post-industrial recycled high-density polyethylene. The solid mixture is fed into the hopper section in a co-rotating twin-screw extruder. The extruder is operated with a temperature gradient of 180° C. to 100° C. from the die to the throat section, respectively. The engine RPM is set to 100 RPM and the feed is set to 6 RPM. The polymer and magnesium silicate mixture are conveyed to the extruder and melt mixed throughout the extruder to produce a continuous solid strand leaving the extruder. Then, the extrudate is passed through a water cooling tank, followed by a vacuum / blower drying tube, and finally granulated.

[0396]

[0397] Example 5

[0398] Mechanochemical graphite oxide is produced by inserting 10 kg of a sample of 325 mesh graphite of >98% purity into a manometer with 200 kg of inert medium (ceramic balls) coated with titanium dioxide. The manometer is pressurized to 0.689 MPa (6.8 atm) using a gas composition consisting of 99% mole % CO2 and <1% nitrogen and oxygen, placed in a high energy ball mill and rotated for 128 hours. The reaction is initiated at room temperature and no heating or cooling is applied. The resulting mechanochemical graphite oxide has a CO2 content of about 5.4 wt% and a carbon dioxide content of 210 m 2 / g and a BET surface area of ​​2.21, 10.67, and 31.92 μm, respectively.

[0399] Example 6

[0400] The branded luggage hardware components were made from 5 wt% recycled styrene-butadiene tires (20 mesh), 10 wt% mechanochemical carbide magnesium silicate of Example 1, 20 wt% mechanochemical graphite oxide of Example 5, and the balance HDPE.

[0401] The luggage hardware component in the form of a zipper pull was made from 5 wt% recycled styrene-butadiene tire (20 mesh), 15 wt% mechanochemical carbide magnesium silicate of Example 1, 10 wt% mechanochemical graphite oxide of Example 5, and the remainder recycled PP.

[0402] Both hardware components exhibit excellent mechanical properties.

[0403] Example 7

[0404] Mechanochemical carbide of magnesium silicate was prepared by mixing 10 kg of magnesium silicate powder sample ( Median particle size D50 is 15 microns, loose bulk density is 33 lbs / ft 3 , capture volume density 77lbs / ft 3 ) is inserted into a pressure gauge with 150kg grinding media (12mm ceramic ball bearings) to generate. The pressure gauge is pressurized to 0.45MPa (4.42atm) using industrial grade carbon dioxide, placed in a high energy ball mill and rotated at 38RPM for 48 hours. The reaction is initiated at room temperature without applying heating or cooling. After 48 hours, the reactor is allowed to cool and decompressed, and the product is separated by a vibrating separator to separate the product from the grinding media.

[0405] The XRD of the native magnesium silicate (ie before it was subjected to mechanochemical carbonization) and the treated magnesium silicate were recorded in order to determine the amorphous content. The results are shown in the table below.

[0406] Quantitative weight % Primary magnesium silicate Treated magnesium silicate Amorphous 10.3 54.2

[0407] Energy dispersive X-ray spectroscopy (EDS) was recorded for the raw and treated magnesium silicate samples and showed the weight % of carbon to be 9.14 and 20.78 respectively.

[0408] The obtained mechanochemical carbide magnesium silicate has a CO2 content of about 4.3% by weight and a carbon dioxide content of 572810 cm 2 / g(=57.28m 2 / g) of BET surface area.

[0409] Example 8

[0410] The magnesium silicate in the receiving state ( P200, median particle size D50 is 8.5 microns, loose bulk density is 28 lbs / ft 3 , capture volume density 48lbs / ft 3 ) was loaded into the reactor in 20 to 35 gram quantities without further treatment. The grinding media (5 mm steel bearings) were loaded into the reactor containing the sodium magnesium silicate. The reactor was pressurized to 0.68 MPa (6.8 atm) with industrial grade CO2 gas and sealed. The reactor was rotated at 65 RPM to allow for grinding and carbonization. Sample 8-A was ground for 3 days and sample 8-B was ground for 4 days. At the end of the run time, the reactor was depressurized and the product was separated into a wire mesh separator to separate the product from the grinding media.

[0411] Sample ID <![CDATA[CO2 absorption and drying (%)]]> <![CDATA[g CO2 / kg sample]]> 8-A 11.1％ 110.8 8-B 11.2％ 111.7

[0412] Aspects of the Invention

[0413] 1. A mechanochemical carbide magnesium silicate having

[0414] · Between 20 and 100m 2 / g, preferably 30 to 80m 2 / g, more preferably 40 to 70m 2 / g, more preferably 45 to 65m 2 / g, and / or an amorphous content of at least 30 wt.-%, preferably at least 40 wt.-%, more preferably at least 50 wt.-%, more preferably at least 60 wt.-% as determined by XRD; and

[0415] · A CO2 content of at least 3 wt.-%, preferably at least 6 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min.

[0416] 2. The mechanochemical carbide magnesium silicate according to aspect 1, which has:

[0417] · Between 20 and 100m 2 / g, preferably 30 to 80m 2 / g, more preferably 40 to 70m 2 / g, most preferably 45 to 65m 2 BET surface area in the range of 1000 Å / g; and

[0418] a CO2 content in the range of 3 to 40 wt.-%, preferably 5 to 35 wt.-%, more preferably 7 to 30 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min; and

[0419] - An amorphous content of at least 30 wt.-%, preferably at least 40 wt.-%, more preferably at least 50 wt.-%, even more preferably at least 60 wt.-%, as determined by XRD.

[0420] 3. The mechanochemical carbide magnesium silicate according to aspect 1 or aspect 2, which has one, two or all (preferably all) of the following characteristics:

[0421] D10 in the range of 0.01 to 5 μm, preferably 0.1 to 3 μm, most preferably 0.5 to 1.5 μm;

[0422] D50 in the range of 0.1 to 50 μm, preferably 1 to 25 μm, most preferably 2 to 10 μm;

[0423] • D90 in the range of 5 to 150 μm, preferably 10 to 100 μm, most preferably 15 to 40 μm.

[0424] 4. A method for producing the mechanochemical carbide magnesium silicate according to any one of aspects 1 to 3, comprising the following steps:

[0425] a) providing a solid raw material comprising magnesium silicate;

[0426] b) providing a gas comprising CO2;

[0427] c) introducing the solid raw material and the gas into a mechanical stirring unit; and

[0428] d) subjecting the solid raw material to a mechanical stirring operation in the presence of the gas at a pressure of at least 1 atm in the mechanical stirring unit to obtain mechanochemical magnesium carbide silicate.

[0429] 5. The method according to aspect 4, wherein the solid feedstock has a D50 in the range of 0.1 to 500 μm, preferably in the range of 0.2 to 50 μm, more preferably in the range of 0.5 to 15 μm.

[0430] 6. A method according to aspect 4 or aspect 5, wherein the solid raw material comprises 80%, preferably at least 90%, more preferably at least 95% of hydrated magnesium silicate measured by X-ray diffraction and optionally comprises at least 1% of a mineral selected from magnesite, dolomite and / or chlorite measured by X-ray diffraction.

[0431] 7. The method according to any one of aspects 4 to 6, wherein the gas provided in step (b) is combustion flue gas.

[0432] 8. The method according to any one of aspects 4 to 7, wherein step (d) is performed

[0433] at a pressure of at least 3 atm, preferably at least 6 atm;

[0434] at a temperature of less than 150°C, preferably less than 100°C, preferably less than 90°C; and / or

[0435] • Lasts for at least 1 hour, preferably at least 4 hours, more preferably at least 8 hours.

[0436] 9. According to the method described in any one of aspects 4 to 8, the mechanochemical stirring operation in step (d) includes mixing, stirring (low-speed stirring or high-speed stirring), shearing (high-torque shearing), oscillation, blending, fluidized bed or ultrasonic treatment, preferably mixing, stirring (low-speed stirring or high-speed stirring), shearing (high-torque shearing) or ultrasonic treatment.

[0437] 10. The method according to any one of aspects 4 to 9, wherein step (d) is carried out in the presence of a catalyst, preferably a transition metal oxide catalyst, more preferably a transition metal dioxide catalyst, most preferably a transition metal dioxide catalyst selected from the group consisting of iron oxides, cobalt oxides, ruthenium oxides, titanium oxides, nickel oxides and combinations thereof.

[0438] 11. A mechanochemical magnesium carbide silicate obtainable by a method according to any one of aspects 4 to 10.

[0439] 12. A composition comprising the mechanochemical carbide magnesium silicate according to any one of aspects 1 to 3 or 11 and a polymer, preferably a polyolefin.

[0440] 13. A composition according to aspect 12, wherein the composition comprises at least 1 wt%, preferably at least 5 wt%, more preferably at least 10 wt% of the mechanochemical carbide magnesium silicate.

[0441] 14. The composition according to aspect 12 or aspect 13, further comprising mechanochemically carbonized fly ash.

[0442] 15. Use of the mechanochemical carbide magnesium silicate according to any one of aspects 1 to 3 or 11:

[0443] Used as filler in polymers;

[0444] Increase the crystallization temperature of the polymer

[0445] Increase the tensile modulus of the polymer;

[0446] Increase the yield stress of the polymer; and / or

[0447] Increase the impact strength of polymers.

Claims

1. A luggage item or luggage accessory comprising a hardware component, wherein the hardware component comprises a hardware composition, wherein the hardware composition comprises: (a) a mechanochemical carbide magnesium silicate, wherein the mechanochemical carbide magnesium silicate has ●20 to 100m 2 / g, preferably 30 to 80m 2 / g, more preferably 40 to 70m 2 / g, more preferably 45 to 65m 2 / g, and / or an amorphous content of at least 30 wt.-%, preferably at least 40 wt.-%, more preferably at least 50 wt.-%, more preferably at least 60 wt.-% as determined by XRD; and a CO2 content of at least 3 wt.-%, preferably at least 6 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min; and / or (b) mechanochemically oxidized graphite, wherein the mechanochemically oxidized graphite has at least 50 m 2 / g and a BET surface area of ​​at least 2 wt. % CO2 content, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min.

2. The luggage piece or luggage accessory of claim 1, wherein the hardware composition further comprises a polymer.

3. The luggage item or luggage accessory of claim 1 or claim 2, wherein the hardware composition comprises at least 1 wt% of the mechanochemical carbide magnesium silicate, preferably at least 5 wt% of the mechanochemical carbide magnesium silicate.

4. The luggage piece or luggage accessory according to any one of claims 1 to 3, wherein the hardware composition comprises at least 1 wt% of the mechanochemical graphite oxide, preferably at least 5 wt% of the mechanochemical graphite oxide.

5. The luggage piece or luggage accessory of any one of claims 1 to 4, wherein the hardware composition comprises the mechanochemical carbide magnesium silicate and the mechanochemical graphite oxide, and optionally, wherein the composition comprises a combined amount of at least 5% by weight of the mechanochemical carbide magnesium silicate and the mechanochemical graphite oxide.

6. The luggage item or luggage accessory of any one of claims 1 to 5, wherein the mechanochemical magnesium carbide silicate has: a) Between 20 and 100 m 2 / g, preferably 30 to 80m 2 / g, more preferably 40 to 70m 2 / g, more preferably 45 to 65m 2 / g, and / or an amorphous content of at least 30 wt.-%, preferably at least 40 wt.-%, more preferably at least 50 wt.-%, more preferably at least 60 wt.-% as determined by XRD; and b) a CO2 content of at least 3 wt.-%, preferably at least 6 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min; and c) one, two or all, preferably all of the following characteristics: o D10 of 0.01 to 5 μm, preferably 0.1 to 3 μm, most preferably 0.5 to 1.5 μm; o D50 of 0.1 to 50 μm, preferably 1 to 25 μm, most preferably 2 to 10 μm; o D90 of 5 to 150 μm, preferably 10 to 100 μm, most preferably 15 to 40 μm.

7. The luggage item or luggage accessory of any one of claims 1 to 6, wherein the mechanochemically oxidized graphite has: a) 50 to 2000 m 2 / g, preferably 100 to 1500m 2 / g, most preferably 150 to 1000m 2 / g BET surface area; and / or b) a CO2 content of 3 to 40 wt.-%, preferably 4 to 30 wt.-%, more preferably 5 to 25 wt.-%, wherein the CO2 content is determined as the mass loss above 200°C measured by TGA using a temperature trace, wherein the temperature is increased from room temperature to 800°C at a rate of 10°C / min and then decreased to room temperature at a rate of 10°C / min; and / or c) D50 of 0.01 to 50 μm, preferably 0.1 to 25 μm, most preferably 0.2 to 20 μm.

8. The luggage article or luggage accessory of any one of claims 2 to 7, wherein the polymer is selected from epoxy resins, phenol-formaldehyde resins, polyalkylene terephthalates, polyalkylene adipate terephthalates, polyisosorbide terephthalates, polyalkylene aromatic polyamides, polyacrylonitrile, polyacetals, polyimides, aromatic polyesters, polyisoprene, polyethylene, polypropylene, polyurethanes, polyisocyanurates, polyamides, polyethers, polyesters, polyhydroxyalkanoates, polylactic acid, polylactic-co-glycolic acid, polyvinylidene fluoride, polyvinyl acetate, polyvinyl chloride, polystyrene, polytetrafluoroethylene, acrylonitrile-butadiene-styrene, nitrile rubber, styrene-butadiene, ethylene-vinyl acetate, copolymers thereof and combinations thereof, preferably polyolefins such as polypropylene, polyethylene, copolymers thereof and combinations thereof.

9. The luggage piece or luggage accessory according to any one of claims 2 to 8, wherein the hardware composition comprises greater than 50% by weight of the polymer, preferably greater than 55% by weight of the polymer, more preferably greater than 60% by weight of the polymer.

10. The luggage item or luggage accessory according to any one of claims 1 to 9, wherein the hardware composition further comprises a filler in an amount of at least 0.1 wt%, preferably at least 1 wt%, selected from rubbers, preferably rubbers selected from styrene-butadiene rubber, polyisoprene, chloroprene, nitrile rubber, polyisobutylene, polybutadiene and combinations thereof.

11. The luggage piece or luggage accessory of any one of claims 2 to 10, wherein the hardware composition comprises: (a) at least 1 wt% of said mechanochemical carbide magnesium silicate, preferably at least 5 wt% of said mechanochemical carbide magnesium silicate; and (b) at least 1 wt% of said mechanochemically oxidized graphite, preferably at least 5 wt% of said mechanochemically oxidized graphite; and (c) greater than 50% by weight of said polymer, preferably greater than 55% by weight of said polymer, more preferably greater than 60% by weight of said polymer, And optionally further comprises a filler in an amount of at least 0.1 wt%, preferably at least 1 wt%, selected from rubbers, preferably rubbers selected from styrene-butadiene rubber, polyisoprene, chloroprene, nitrile rubber, polyisobutylene, polybutadiene and combinations thereof.

12. The luggage piece or luggage accessory of any one of claims 2 to 11, wherein the hardware composition comprises: (a) 1 to 40 wt % of said mechanochemical carbide magnesium silicate, preferably 5 to 30 wt % of said mechanochemical carbide magnesium silicate; and (b) 1 to 40 wt% of said mechanochemical graphite oxidation, preferably 5 to 30 wt% of said mechanochemical graphite oxidation; and (c) greater than 50% by weight of said polymer, preferably greater than 55% by weight of said polymer, And optionally further comprises a filler in an amount of 0.1 to 10 wt %, preferably 1 to 8 wt %, more preferably 4 to 6 wt %, wherein the filler is selected from rubber, preferably a rubber selected from styrene-butadiene rubber, polyisoprene, chloroprene, nitrile rubber, polyisobutylene, polybutadiene and combinations thereof.

13. The luggage piece or luggage accessory of any one of claims 2 to 12, wherein the polymer is a recycled polymer.

14. The luggage piece or luggage accessory of any one of claims 10 to 13, wherein the filler selected from rubber comprises recycled rubber.

15. A method for manufacturing a luggage article or luggage accessory according to any one of claims 1 to 14, comprising the steps of: i) providing mechanochemical magnesium carbide silicate; providing mechanochemical graphite oxide; or providing mechanochemical magnesium carbide silicate and mechanochemical graphite oxide; ii) providing a polymer; iii) optionally providing a filler selected from rubber, preferably selected from styrene-butadiene rubber, polyisoprene, chloroprene, nitrile rubber, polyisobutylene, polybutadiene and combinations thereof; iv) combining the mechanochemical carbide magnesium silicate and / or the mechanochemical graphite oxide of step (i) with the polymer of step (ii) and optionally the filler selected from rubber of step (iii), thereby obtaining a hardware composition comprising the mechanochemical carbide magnesium silicate and / or the mechanochemical graphite oxide, a polymer and optionally the filler selected from rubber; v) using the hardware composition obtained in step (iv) as a hardware component of a luggage item or luggage accessory.

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