Mechanochemically activated materials and their uses

Abstract

A mechanochemically activated material obtainable by a process for the mechanochemical activation of kaolinite-poor starting materials, the process comprising the following steps: a) providing a solid starting material comprising a phyllosilicate mineral, the starting material having a kaolinite content of less than 50 wt% as determined by XRD, preferably less than 20 wt%, more preferably less than 10 wt%; b) providing a gas; c) introducing the feedstock and the gas into a mechanical agitation unit; and d) subjecting the starting material to mechanical agitation in the presence of the gas in the mechanical agitation unit; wherein the phyllosilicate mineral is selected from the kaolinite group, serpentinite group, mica group, chlorite group and combinations thereof, wherein the mechanochemically activated material has a Strength Activity Index (SAI) at Day 28 of at least 110%, the SAI being determined in accordance with ASTM C311 / C311 M-22.

Description

FIELD OF THE INVENTION

[0001] The present invention relates to mechanochemically activated materials that can be obtained from low-kaolinite starting materials. The invention further relates to compositions comprising the mechanochemically activated materials and another material, wherein the other material is selected from the group consisting of asphalt, cement, geopolymers, polymers, and combinations thereof. STATE OF THE ART

[0002] Concrete is a composite material comprising a matrix of aggregate (typically a rock material) and a binder (typically Portland cement or asphalt) that holds the matrix together. Concrete is one of the most widely used construction materials and is considered the second most used material on Earth after water.

[0003] To reduce the cost of concrete and CO 2To reduce CO2 emissions generated by global cement production, much research has been done to identify inexpensive materials that can be used as fillers or alternative binders to replace the binder component without adversely affecting the properties of concrete. Such secondary cementitious materials are an area of ​​broad industrial interest.

[0004] An example of a widely used cement filler is limestone. A comprehensive review of fillers in cementitious materials can be found in John, Vanderley M., et al., "Fillers in cementitious materials—Experience, recent advances, and future potential." Cement and Concrete Research 114 (2018): 65–78.

[0005] Portland cement production contributes to approximately 8% of global carbon dioxide emissions. According to Vanderley et al., traditional mitigation strategies for CO 2Emissions in the cement industry are not sufficient to ensure the necessary reduction in a scenario of increasing cement demand. Currently, cement production is increasing due to a combination of increasing urbanization and the replacement of old infrastructure.

[0006] Therefore, there is still a need to develop affordable filler technology that will lead to a reduction in CO 2 emissions through reduced cement production, which can be associated with low CO 2 footprint and which ideally does not adversely affect the properties of concrete.

[0007] Thermally activated kaolins have been used as supplementary cementitious materials (SCMs) in blended cements since the 1950s. Heat treatment transforms kaolin (also known as kaolinite - a clay mineral) into metakaolin, a highly reactive pozzolanic material. The process of thermal activation of clay minerals such as kaolin is commonly referred to as calcination. The activation temperature is typically in the range of 550-800 °C. Therefore, the production of calcined clays for use as SCMs for large CO 2 -emissions.

[0008] As an alternative to calcination, the so-called mechanochemical activation of kaolins has been investigated for some time. Instead of a heat treatment, this process is based on extensive grinding to convert the kaolin mineral into an amorphous water-containing material with a high specific surface area, which physically, chemically and structurally differs from the metakaolin obtained by thermal activation. See Souri, Alireza, et al. “Pozzolanic activity of mechanochemically and thermally activated kaolins in cement.” Cement and Concrete Research 77 (2015): 47-59 or Vizcayno C et al: “Pozzolan obtained by mechanochemical and thermal treatments of kaolin” Applied clay science, Elsevier, Amsterdam, nl, vol. 49 no. 4, 1 August 2010 pages 405-413, both of which describe the grinding of kaolin in an air atmosphere to increase its pozzolanic activity.

[0009] However, kaolin-rich rock formations are not always available locally, and there are many other uses for kaolin, so its mechanochemical treatment into a SCM is often not an economically viable or attractive option. Therefore, there is still a need to develop alternative SCMs.

[0010] It is an object of the present invention to provide alternative or improved fillers for cement, geopolymer or asphalt binder.

[0011] It is a further object of the present invention to provide alternative or improved fillers for cement, geopolymer or asphalt binders that are inexpensive to produce.

[0012] It is a further object of the present invention to provide alternative or improved fillers for cement, geopolymer or asphalt binders which have a low CO 2 -footprint can be produced.

[0013] It is a further object of the present invention to provide alternative or improved fillers for cement, geopolymer or asphalt binder that improve the properties of the resulting concrete, such as compressive strength, strength activity index and / or water demand. SUMMARY OF THE INVENTION

[0014] The present inventors have surprisingly discovered that low-kaolinite starting materials can be mechanochemically activated to convert other phyllosilicate mineral phases into amorphous phases exhibiting high reactivity and, consequently, strong pozzolanic activity when used as SCMs. To the best of the inventors' knowledge, they are the first to demonstrate the activation and pozzolanic activity of phyllosilicate minerals such as illite, muscovite, and chlorite.

[0015] In a first aspect, the present invention provides a mechanochemically activated material obtainable by a process for the mechanochemical activation of kaolinite-poor starting materials, the process comprising the following steps: a) providing a solid starting material comprising a phyllosilicate mineral, the starting material having a kaolinite content of less than 50 wt% as determined by XRD, preferably less than 20 wt%, more preferably less than 10 wt%; b) providing a gas; c) introducing the feedstock and the gas into a mechanical agitation unit; and d) subjecting the starting material to mechanical agitation in the presence of the gas in the mechanical agitation unit, wherein the phyllosilicate mineral is selected from the kaolinite group, serpentinite group, mica group, chlorite group, and combinations thereof, wherein the mechanochemically activated material has a Strength Activity Index (SAI) at day 28 of at least 110%, the SAI being determined in accordance with ASTM C311 / C311M-22.

[0016] The phyllosilicate mineral is preferably uncalcined, meaning it has not been calcined. Thus, the starting material is preferably uncalcined.

[0017] This process, by which the mechanochemically activated material of the present invention is obtainable, can be applied to various types of low-kaolinite phyllosilicate starting materials, advantageously resulting in unique mechanochemically activated materials.

[0018] As demonstrated in the accompanying examples, it has been found that when such mechanochemically activated materials described herein are used as fillers in cement, the compressive strength of the resulting concrete is surprisingly increased beyond the values ​​obtained for unactivated phyllosilicates, and in particular, far beyond the values ​​of pure Portland cement. In particular, the setting time for strength development is greatly improved (shortened) compared to the use of unactivated phyllosilicates as fillers. Furthermore, a much larger amount of this mechanochemically activated material can be used as fillers while still achieving acceptable or even improved concrete properties. Furthermore, the water requirement of cement mixtures is significantly reduced when the present mechanochemically activated materials are employed as supplemental cementitious materials.

[0019] In addition, the production of the mechanochemically activated materials of the invention is based on a cost-effective technology platform capable of reacting with diluted CO 2 streams, such as directly at a point source emission from an incinerator, thus providing a filler that can be produced in an economically viable manner and that both reduces the CO 2 -Emission reduction through reduced cement production as well as low production CO 2 footprint. Thus, the mechanochemically activated material of the present invention represents an excellent filler for many applications, combining distinct mechanical properties with a cost-effective production technology.

[0020] In another aspect, the invention provides a composition comprising a mechanochemically activated material as described herein and another material, wherein the another material is selected from the group consisting of asphalt, geopolymers, cement, polymers, and combinations thereof. SHORT DESCRIPTION OF THE CHARACTERS

[0021] The figures show the TGA curves determined for the following materials as described in the “Examples” section. Fig. 1: Example 1 raw Fig. 2: Sample 1 Fig. 3: Sample 2 Fig. 4: Sample 3 Fig. 5: Sample 4 Fig. 6: Sample 5 Fig. 7: Sample 6 Fig. 8: Example 2 Raw material Fig. 9: Sample 7 Fig. 10: Sample 8 Fig. 11: Sample 9 DESCRIPTION OF EMBODIMENTS

[0022] The term "comprise" and variations thereof, such as "comprises" and "comprising," as used herein, should be construed in an open, inclusive sense, meaning that the described embodiment includes the recited features but does not preclude the presence of other features as long as they do not render the embodiment unusable.

[0023] The terms "one embodiment," "one particular embodiment," etc., as used herein, should be construed to mean that a particular feature, structure, or characteristic described in connection with the embodiment is included in at least one embodiment. Thus, appearances of such terms at various points in this specification do not necessarily all refer to the same embodiment. Moreover, the particular features, structures, or characteristics may be combined in any suitable manner in one or more embodiments. For example, certain features of the disclosure described herein in connection with separate embodiments are also explicitly contemplated in combination in a single embodiment.

[0024] The singular forms "a," "an," "the," "the," and "the" as used herein should be construed to include plural references unless the content clearly dictates otherwise. It should also be noted that the term "or" is generally used in its broadest sense, that is, as "and / or," unless the content clearly dictates otherwise.

[0025] Whenever reference is made in this document to a compound that is a salt, this should be construed to include the anhydrous form as well as any solvates (especially hydrates) of that compound.

[0026] As is known to those skilled in the art, all naturally occurring phyllosilicate minerals are hydrated, with water or hydroxyl groups bound. It is known that calcination can dehydrate the minerals. In accordance with preferred embodiments of the invention, the phyllosilicate minerals mentioned herein are not calcined. Thus, they are in hydrated form when provided in step (a) of the process by which the mechanochemically activated material according to the invention is obtainable.

[0027] As is known to those skilled in the art, minerals can be classified according to various classification systems. References made herein to minerals or mineral groups should be interpreted according to the Dana Classification System as set forth in Dana's New Mineralogy, Eighth Edition, by Richard V. Gaines, H. Catherine Skinner, Eugene E. Foord, Brian Mason, and Abraham Rosenzweig, with sections by Vandall T. King, illustrations by Eric Dowty, (ISBN: 047119310-0). Copyright © 1997, John Wiley & Sons, Inc.

[0028] The term "mechanochemically activated material" is used herein to refer to the material of the starting material after it has been subjected to the process by which the mechanochemically activated material of the present invention is obtainable. As shown in the attached examples, the processes by which the mechanochemically activated material of the present invention is obtainable result in an amorphization of the phyllosilicate minerals contained in the material (as observed by XRD) and a destabilization of the hydrates (as observed by a lower dehydration onset temperature in TGA).

[0029] TGA, as used herein, refers to thermogravimetric analysis, a technique known to those skilled in the art. A preferred TGA setup for determining the water content of the starting materials and activated materials in the context of the present invention is Mettler Toledo TGA / DSC 3+ using a 30-40 mg sample. In accordance with the invention, TGA is performed under an inert atmosphere, such as nitrogen or argon. The dehydration start temperature referred to here refers to the dehydration start temperature determined by TGA using a temperature trajectory in which the temperature was increased from room temperature to 105°C and held at 105°C for 5 to 10 minutes before the temperature was increased to 1000°C at a ramp rate of 10°C / min.

[0030] In accordance with the invention, the particle size distribution characteristics recited herein, such as D10, D50, and D90, as well as the specific surface area, are determined by measurement with a laser diffraction particle size analyzer using the Fraunhofer theory of light scattering, such as the Brookhaven Laser Particle Sizer, Model Microbrook 2000LD, or another instrument with equal or better sensitivity, and the data are reported using a volume-equivalent sphere model. As is known to those skilled in the art, the D50 is the mass-median diameter, i.e., the diameter at which 50% of the mass of a sample consists of smaller particles. Similarly, D10 and D90 represent the diameter at which 10% and 90% of the mass of a sample consists of smaller particles, respectively.

[0031] In accordance with the invention, the compressive strength, strength activity index, and water demand referred to herein are determined according to ASTM C311 / C311M-22. As will be appreciated by those skilled in the art, the raw material precursor or activated material of the present invention was used in conducting these tests instead of the "fly ash or natural pozzolans" specified in the standard.

[0032] The mineralogical composition and amorphous content reported here are determined by XRD. Samples for XRD analysis were finely crushed and ground using an agate mortar and pestle. XRD data were collected using a PANalytical Aeris X-ray diffractometer. Corundum was used as an external standard and was measured with the same instrument configuration shortly after the sample was measured. The weight percentage of the amorphous content of the sample was determined using the K-factor of the external standard phase. The weight percentages of minerals and amorphous content used here in connection with the starting material or the activated material provided in step (a) refer to the total weight of the starting material or activated material, respectively, unless otherwise stated.

[0033] The elemental compositions reported here are determined by EDS. Samples for EDS analysis were finely crushed and ground using an agate mortar and pestle. EDS data were collected using a JEOL JED-2300 DRY SDD EDS detector.

[0034] The heat of hydration mentioned here is calculated according to a modified version of the R 3 -Tests of ASTM C 1897-20, referred to here as modified ASTM C 1897-20, where the modifications consist of • Use of a ratio of calcium hydroxide to the supplementary cementitious material to be tested of 3:1; • Using a liquid-solid ratio of 0.9, with 0.5 M KOH (pH 13.5); • Performing isothermal calorimetry at 50 °C for 10 days; and • Conduct thermogravimetric analysis after 10 days.

[0035] For the purposes of this disclosure, the ideal gas law is assumed, so that the vol% of a gas is considered equal to the mol%. Process for the mechanochemical activation of phyllosilicate minerals by which the mechanochemically activated material of the invention is obtainable

[0036] In one aspect, the invention provides a mechanochemically activated material obtainable by a process for the mechanochemical activation of kaolinite-poor starting materials, the process comprising the following steps: a) providing a solid starting material comprising a phyllosilicate mineral, the starting material having a kaolinite content of less than 50 wt% as determined by XRD, preferably less than 20 wt%, more preferably less than 10 wt%; b) providing a gas; c) introducing the feedstock and the gas into a mechanical agitation unit; and d) subjecting the starting material to mechanical agitation in the presence of the gas in the mechanical agitation unit, wherein the phyllosilicate mineral is selected from the kaolinite group, serpentinite group, mica group, chlorite group and combinations thereof, wherein the mechanochemically activated material has a Strength Activity Index (SAI) at day 28 of at least 110%, the SAI being determined in accordance with ASTM C311 / C311M-22. The source material

[0037] The term "starting material" is to be interpreted as a material consisting of or comprising a (preferably uncalcined) phyllosilicate mineral and having a kaolinite content of less than 50 wt.%, as determined by XRD. The phyllosilicate mineral typically occurs mixed with other minerals and / or amorphous inorganic phases to form the starting material. Typically, the starting material consists mainly or entirely of rock (such as igneous rock, sedimentary rock, or metamorphic rock) that has been ground to a particle size suitable for introduction into the process by which the mechanochemically activated material of the present invention is obtainable. Thus, the preferred compositions of the starting material described elsewhere herein (e.g.Indication of contents of various minerals), typically to the composition of such naturally occurring rock deposits which have been reduced in size to provide the starting material for the process by which the mechanochemically activated material of the present invention is obtainable.

[0038] In some embodiments of the invention, the phyllosilicate mineral is selected from dickite, halloysite, endellite, kaolinite, nacrite, odinite, antigorite, caryopilite, lizardite, nepouit, greenalith, amesite, berthierite, brindleyite, fraipontite, kellyite, manandonite, cronstedtite, chrysotile, clinochrysotile, orthochrysotile, parachrysotile, pecoraite, bismuthoferrite, chapmanite, allophane, hisingerite, imogolite, neotocite, muscovite, paragonite, chernykhite, roscoelith, glauconite, celadonite, ferroceladonite, ferro-aluminoceladonite, aluminoceladonite, chromceladonite, tobelite, nanpingite, boromuscovite, montdorite, chromphyllite, phlogopite, tetra-ferriphlogopite, biotite, annite, tetra-ferri-annite, siderophyllite, eastonite, hendricksite, lepidolite, polylithionite, trilithionite, Tainiolites, Zinnwaldites, Norrishites, Masutomilites, Aspidolites, Wonesites, Preiswerkites, Ephesites, Fluoranites, Margarites, Clintonites, Bitites, Anandites, Kinoshitalites, Ferrokinoshitalites, Hydrobiotes, Illites, Vermiculites, Brammallites, Baileychlor, Borocookeites,Chamosite, clinochlor, cookeite, donbassite, franklinfurnaceite, glagolevite, gonyerite, nimite, pennantite, sudoite and combinations thereof.

[0039] Preferably, the phyllosilicate mineral is selected from kaolinite, illite, chlorite, muscovite, montmorillonite, vermiculite, smectite, pyrophyllite, sepiolite, palygorskite, antigorite, chrysotile, lizardite, biotite, fuchsite, muscovite, phlogopite, lepidolite, margarite, glauconite, halloysite, dickite, nacrite, orthoclase, lepidocrite, goethite, albite and combinations thereof, more preferably the phyllosilicate mineral is selected from kaolinite, illite, chlorite, muscovite and combinations thereof, most preferably the phyllosilicate mineral is selected from illite, chlorite, muscovite and combinations thereof.

[0040] Most preferably, the phyllosilicate mineral is selected from the serpentinite group, mica group, chlorite group, and combinations thereof.

[0041] In preferred embodiments of the invention, the phyllosilicate mineral contained in the starting material is not calcined, which means that preferably the starting material provided in step (a) is not calcined. General mineralogical properties of the starting material

[0042] In preferred embodiments of the invention, the phyllosilicate mineral is selected from the kaolinite group, serpentinite group, mica group, chlorite group and combinations thereof, more preferably the phyllosilicate mineral is selected from the serpentinite group, mica group, chlorite group and combinations thereof.

[0043] Examples of suitable minerals in the kaolinite group include dickite, halloysite, endellite, kaolinite, nacrite, odinite, and combinations thereof. Examples of suitable minerals in the serpentine group include antigorite, caryopilite, lizardite, nepouite, greenalite, amesite, berthierine, brindleyite, fraipontite, kellyite, manandonite, cronstedtite, chrysotile, clinochrysotile, orthochrysotile, parachrysotile, pecoraite, bismuth ferrite, chapmanite, allophane, hisingerite, imogolite, neotocite, and combinations thereof.Examples of suitable minerals in the mica group are muscolite, paragonite, chernykhite, roscoelite, glauconite, celadonite, ferroceladonite, ferro-aluminoceladonite, aluminoceladonite, chromium celadonite, tobelite, nanpingite, boromuscovite, montdorite, chromphyllite, phlogopite, tetra-ferriphlogopite, biotite, annite, Tetra-Ferri-Annite, Siderophyllite, Eastonite, Hendricksite, Lepidolite, Polylithionite, Trilithionite, Tainiolite, Zinnwaldite, Norrishite, Masutomilite, Aspidolite, Wonesite, Preiswerkite, Ephesite, Fluorannite, Margarite, Clintonite, Bityite, Anandite, Kinoshitalite, Ferrokinoshitalite, Hydrobiotite, Illite, Vermiculite, brammallite and combinations thereof. Examples of suitable minerals in the chlorite group are baileychlor, borocookeite, chamosite, clinochlor, cookeite, donbassite, franklinfurnaceite, glagolevite, gonyerite, nimite, pennantite, sudoite and combinations thereof.

[0044] In some embodiments of the invention, the phyllosilicate mineral is selected from aluminosilicate phyllosilicates such as muscovite, biotite, members of the chlorite group, and combinations thereof. In other embodiments of the invention, the phyllosilicate mineral is selected from silicate-hydrate phyllosilicates such as kaolinite, halloysite, smectite, and combinations thereof.

[0045] In the Dana classification system, phyllosilicates are further classified according to their structural features: (i) layer types (i.e., trioctahedral or dioctahedral) and (ii) layer stacking (1:1 or 2:1). In accordance with preferred embodiments of the invention, the phyllosilicate mineral is selected from the group consisting of phyllosilicates having layers of 6-membered rings with 1:1 layers; phyllosilicates having layers of 6-membered rings with 2:1 layers; phyllosilicates having layers of six-membered rings interspersed with 1:1, 2:1, and octahedra; and combinations thereof. Preferably, the phyllosilicate mineral is selected from the group consisting of phyllosilicates having layers of 6-membered rings with 2:1 layers; Phyllosilicates with layers of six-membered rings interspersed with 1:1, 2:1, and octahedra; and combinations thereof.In some embodiments, the phyllosilicate mineral is selected from the kaolinite group, the serpentine group, the mica group, the chlorite group, and combinations thereof, preferably selected from the mica group, the chlorite group, and combinations thereof.

[0046] In some embodiments of the invention, the phyllosilicate mineral is selected from phyllosilicates having 6-membered ring layers with 1:1 plies. In preferred embodiments, the phyllosilicate mineral is selected from the serpentine group.

[0047] In other embodiments, the phyllosilicate mineral is selected from phyllosilicates having layers of 6-membered rings with 2:1 layers. In preferred embodiments, the phyllosilicate mineral is selected from the mica group, more preferably it is selected from illite, muscovite, and combinations thereof, preferably illite. In some embodiments of the invention, the starting material comprises at least 1 wt.% illite, more preferably at least 5 wt.% illite, and most preferably at least 10 wt.% illite. In some embodiments of the invention, the starting material comprises at least 50 wt.% illite, more preferably at least 70 wt.% illite, more preferably at least 85 wt.% illite. In some embodiments of the invention, the starting material comprises at least 1 wt.% muscovite, more preferably at least 5 wt.% muscovite, and most preferably at least 10 wt.% muscovite. In some embodiments of the invention, the starting material comprises at least 50 wt.%-% muscovite, more preferably at least 70 wt.% muscovite, more preferably at least 85 wt.% muscovite.

[0048] In other embodiments, the phyllosilicate mineral is selected from phyllosilicates having layers of six-membered rings interspersed with 1:1, 2:1, and octahedra. In preferred embodiments, the phyllosilicate mineral is selected from the chlorite group. In some embodiments of the invention, the starting material comprises at least 1 wt.% of a mineral species from the chlorite group, more preferably at least 5 wt.% of a mineral species from the chlorite group, and most preferably at least 10 wt.% of a mineral species from the chlorite group. In some embodiments of the invention, the starting material comprises at least 50 wt.% of a mineral species from the chlorite group, more preferably at least 70 wt.% of a mineral species from the chlorite group, more preferably at least 85 wt.% of a mineral species from the chlorite group.

[0049] In some embodiments, the phyllosilicate mineral is not talc, preferably the phyllosilicate mineral is not selected from the group consisting of talc, serpentine group minerals, olivine, and combinations thereof, more preferably the phyllosilicate mineral is not selected from magnesium silicates. In some embodiments, the starting material comprises less than 10 wt.%, preferably less than 5 wt.%, more preferably less than 1 wt.% talc. In some embodiments, the starting material comprises less than 10 wt.%, preferably less than 5 wt.%, more preferably less than 1 wt.% talc. In some embodiments, the combined amount of talc, serpentine, and olivine in the starting material is less than 10 wt.%, preferably less than 5 wt.%, more preferably less than 1 wt.%. In some embodiments, the starting material comprises less than 10 wt.%, preferably less than 5 wt.%, more preferably less than 1 wt.% magnesium silicates.

[0050] In some embodiments, the phyllosilicate is not selected from the pyrophyllite-talc group. In other embodiments, the phyllosilicate is not selected from pyrophyllite, ferripyrophyllite, talc, willemseite, minnesotaite, and combinations thereof; preferably, the phyllosilicate is not selected from talc.

[0051] In some embodiments of the invention, the starting material is not significantly carbonatable, for example, it comprises less than 0.5 wt%, preferably less than 0.1 wt%, more preferably less than 0.05 wt% of a calcium oxide or hydroxide. In some embodiments, it comprises less than 0.5 wt%, preferably less than 0.1 wt%, more preferably less than 0.05 wt% of the total combined amount of oxides and hydroxides of Ca or Mg, preferably oxides and hydroxides of Ca, Mg, K, or Na.

[0052] In preferred embodiments of the invention, the starting material provided in step (a) comprises at least 5 wt% of the phyllosilicate mineral, preferably at least 10 wt%, more preferably at least 15 wt%.

[0053] In preferred embodiments, the starting material provided in step (a) comprises at least 5 wt.% quartz, preferably at least 15 wt.% quartz, more preferably at least 30 wt.% quartz. In natural deposits, quartz typically occurs in association with the phyllosilicate mineral, so the starting material typically comprises at least some quartz.

[0054] In preferred embodiments, the starting material provided in step (a) has an amorphous content of at least 10 wt.%, more preferably at least 15 wt.%, most preferably at least 20 wt.%.

[0055] In some embodiments of the invention, the total combined amount of the phyllosilicate mineral and the kaolinite content in the starting material provided in step (a) is at least 15 wt%, more preferably at least 20 wt%. In some embodiments of the invention, the total combined amount of the phyllosilicate mineral, quartz, and kaolinite content in the starting material provided in step (a) is at least 25 wt%, more preferably at least 30 wt%, more preferably at least 35 wt%.

[0056] In other embodiments of the invention, the total combined amount of the phyllosilicate mineral and the amorphous portion in the starting material provided in step (a) is at least 80 wt.%, more preferably at least 40 wt.%, more preferably at least 45 wt.%. In some embodiments of the invention, the total combined amount of the phyllosilicate mineral, quartz, and the amorphous portion in the starting material provided in step (a) is at least 60 wt.%, more preferably at least 65 wt.%, more preferably at least 75 wt.%.

[0057] Thus, according to some embodiments of the invention, the starting material provided in step (a) comprises: • at least 5% by weight of the phyllosilicate mineral, preferably at least 10% by weight, more preferably at least 15% by weight; and • an amorphous content of at least 10 wt.%, more preferably at least 15 wt.%, most preferably at least 20 wt.%; and • a total combined amount of the phyllosilicate mineral and the amorphous portion being at least 80 wt%, more preferably at least 90 wt%, more preferably at least 95 wt%.

[0058] In some embodiments of the invention, the starting material provided in step (a) comprises: • at least 5% by weight of the phyllosilicate mineral, preferably at least 10% by weight, more preferably at least 15% by weight; • an amorphous portion of at least 10 wt%, more preferably at least 15 wt%, most preferably at least 20 wt%. • a total combined amount of the phyllosilicate mineral and the amorphous portion being at least 45 wt%, more preferably at least 50 wt%, more preferably at least 55 wt%.

[0059] In some embodiments of the invention, the starting material provided in step (a) comprises: • at least 5% by weight of the phyllosilicate mineral, preferably at least 10% by weight, more preferably at least 15% by weight; • a kaolinite content of less than 20% by weight, preferably less than 10% by weight; • an amorphous portion of at least 10 wt%, more preferably at least 15 wt%, most preferably at least 20 wt%. • a total combined amount of the phyllosilicate mineral and the amorphous portion being at least 45 wt%, more preferably at least 50 wt%, more preferably at least 55 wt%.

[0060] In some embodiments of the invention, the starting material provided in step (a) comprises: • at least 5% by weight of the phyllosilicate mineral, preferably at least 10% by weight, more preferably at least 15% by weight; • a kaolinite content of less than 20% by weight, preferably less than 10% by weight; • an amorphous portion of at least 10 wt%, more preferably at least 15 wt%, most preferably at least 20 wt%. • a total combined amount of the phyllosilicate mineral and the amorphous portion being at least 45 wt%, more preferably at least 50 wt%, more preferably at least 55 wt%;wherein the phyllosilicate mineral is selected from the serpentinite group, mica group, chlorite group and combinations thereof, preferably wherein the phyllosilicate mineral is selected from kaolinite, illite, chlorite, muscovite and combinations thereof.

[0061] In some embodiments of the invention, the starting material provided in step (a) comprises: • at least 5% by weight of the phyllosilicate mineral, preferably at least 10% by weight, more preferably at least 15% by weight; • a kaolinite content of less than 50 wt% as determined by XRD, preferably less than 20 wt%, more preferably less than 10 wt%; • preferably at least 5 wt% quartz, preferably at least 15 wt% quartz, more preferably at least 30 wt% quartz; and • an amorphous content of at least 10 wt.%, more preferably at least 15 wt.%, most preferably at least 20 wt.%; and • a total combined amount of the phyllosilicate mineral, quartz and the amorphous portion being at least 80 wt%, more preferably at least 90 wt%, more preferably at least 95 wt%.

[0062] In some embodiments of the invention, the starting material provided in step (a) comprises: • at least 1 wt% illite, more preferably at least 5 wt% illite and most preferably at least 10 wt% illite; • a kaolinite content of less than 50 wt% as determined by XRD, preferably less than 20 wt%, more preferably less than 10 wt%; • an amorphous content of at least 10% by weight, preferably at least 15% by weight, most preferably at least 20% by weight; and • a total combined amount of illite, kaolinite and the amorphous content that is at least 45% by weight, preferably at least 50% by weight, more preferably at least 55% by weight.

[0063] In some embodiments of the invention, the starting material provided in step (a) comprises: • at least 5% by weight of the phyllosilicate mineral, preferably at least 10% by weight, more preferably at least 15% by weight; and • preferably at least 5% by weight of quartz, preferably at least 15% by weight of quartz, more preferably at least 30% by weight of quartz; and • an amorphous content of at least 10% by weight, more preferably at least 15% by weight, most preferably at least 20% by weight; and • a total amount of the phyllosilicate mineral, quartz and amorphous portion of at least 80 wt%, more preferably at least 90 wt%, even more preferably at least 95 wt%.

[0064] In some embodiments of the invention, the starting material provided in step (a) comprises a kaolinite to amorphous fraction ratio of at least 1:1.5, more preferably 1:10, more preferably 1:20, more preferably 1:30, more preferably 1:40, and more preferably 1:50.

[0065] In some embodiments of the invention, the starting material comprises less than 10 wt.% kaolinite, preferably less than 5 wt.% kaolinite, and more preferably less than 3 wt.% kaolinite. These low-kaolinite starting materials preferably have an amorphous content of greater than 10 wt.%, preferably greater than 20 wt.%, more preferably greater than 25 wt.%. In such embodiments, the starting material may comprise at least 5 wt.%, preferably at least 10 wt.%, more preferably at least 15 wt.%, more preferably at least 20 wt.%, more preferably at least 25 wt.%, and most preferably at least 30 wt.% quartz. The phyllosilicate mineral is preferably present in the starting material in an amount of at least 5 wt.%, preferably at least 10 wt.%, more preferably at least 15 wt.%, wherein the phyllosilicate mineral is not kaolinite.Preferably, the phyllosilicate mineral is selected from the group consisting of phyllosilicates having layers of 6-membered rings with 2:1 plies; phyllosilicates having layers of six-membered rings interspersed with 1:1, 2:1, and octahedra; and combinations thereof. In some preferred embodiments of the low-kaolinite starting materials, the phyllosilicate mineral is selected from the serpentinite group, the mica group, the chlorite group, and combinations thereof, preferably selected from the mica group, the chlorite group, and combinations thereof. Most preferably, the phyllosilicate mineral is selected from the mica group, such as illite or muscovite.

[0066] As will be apparent from the above, in preferred embodiments of the invention, the starting material provided in step (a) comprises: • less than 10 wt% kaolinite, preferably less than 5 wt% kaolinite and more preferably less than 3 wt% kaolinite; and • an amorphous content of more than 10 wt.%, preferably more than 20 wt.%, more preferably more than 25 wt.%; and • preferably at least 5 wt% quartz, preferably at least 15 wt% quartz, more preferably at least 30 wt% quartz; and • at least 5 wt%, preferably at least 10 wt%, more preferably at least 15 wt% of the phyllosilicate mineral, wherein the phyllosilicate mineral is not kaolinite; wherein preferably the phyllosilicate mineral is selected from the mica group, the chlorite group and combinations thereof, preferably the phyllosilicate mineral is selected from the mica group, most preferably selected from illite, muscovite and combinations thereof.

[0067] In preferred embodiments of the invention, the starting material provided in step (a) comprises: • less than 5 wt% kaolinite and more preferably less than 3 wt% kaolinite; and • an amorphous content of more than 10 wt.%, preferably more than 20 wt.%, more preferably more than 25 wt.%; and • preferably at least 5 wt% quartz, preferably at least 15 wt% quartz, more preferably at least 30 wt% quartz; and • at least 10% by weight, more preferably at least 15% by weight of the phyllosilicate mineral, wherein the phyllosilicate mineral is not kaolinite; wherein the phyllosilicate mineral is selected from the mica group, the chlorite group, and combinations thereof, preferably the phyllosilicate mineral is selected from the mica group, most preferably from illite, muscovite, and combinations thereof.

[0068] In preferred embodiments of the invention, the starting material provided in step (a) comprises: • less than 5 wt% kaolinite and more preferably less than 3 wt% kaolinite; and • an amorphous content of more than 10 wt.%, preferably more than 20 wt.%, more preferably more than 25 wt.%; and • preferably at least 5 wt% quartz, preferably at least 15 wt% quartz, more preferably at least 30 wt% quartz; and • at least 10% by weight, more preferably at least 15% by weight of the phyllosilicate mineral, wherein the phyllosilicate mineral is not kaolinite; and • a total amount of the phyllosilicate mineral, quartz and amorphous portion of at least 80 wt%, preferably at least 90 wt%, more preferably at least 95 wt%, wherein the phyllosilicate mineral is selected from the mica group, the chlorite group and combinations thereof, preferably the phyllosilicate mineral is selected from the mica group, most preferably from illite, muscovite and combinations thereof;

[0069] As shown in the accompanying examples, the activated materials obtained from the low-kaolinite starting materials described here were found to exhibit surprisingly high pozzolanic reactivity, making them useful as SCMs. Other properties of the starting material

[0070] The solid starting material provided in step (a) preferably consists of particles having a largest dimension of less than 30 cm, such as less than 20 cm. In preferred embodiments of the present invention, the solid starting material provided in step (a) has a D10 that is less than 100 mm, preferably less than 50 mm, and / or a D50 that is less than 100 mm, preferably less than 50 mm. The D10 and D50 described in this paragraph refer to the mass-based D10 and D50 determined by sieve analysis.

[0071] The starting material preferably has a bulk density of more than 1.5 g / cm 3 , preferably more than 2.0 g / cm 3 , more preferably more than 2.3 g / cm 3 .

[0072] The total amount of Si and O in the starting material is preferably at least 60 wt%, preferably at least 65 wt%. As already explained, the starting material typically originates from natural deposits, so it may comprise carbon, typically 5-15 wt% carbon. The total amount of Si, O, C, Al, Fe, and K in the starting material is preferably at least 90 wt%, more preferably at least 92 wt%, most preferably at least 94 wt%.

[0073] Description of the process by which the mechanochemically activated material of the present invention is obtainable.

[0074] Step (c) of the process described herein by which the mechanochemically activated material of the present invention is obtainable may comprise the introduction into the mechanical agitation unit of additional solid materials, such as grinding aids and comminution media (discussed elsewhere herein), or further activatable starting materials other than the starting material provided in step (a).

[0075] The gas provided in step (b) may be any gas stream, such as normal air, a gas with high amounts of inert gas (such as gas with > 90 vol.% nitrogen or argon), or gas streams with elevated CO 2 -Contents compared to air, such as an exhaust stream with an increased but relatively low CO 2 -concentration, or concentrated CO 2 -currents.

[0076] In embodiments of the process described herein by which the mechanochemically activated material of the present invention is obtainable, the gas provided in step (b) is normal air.

[0077] The CO 2 However, the CO concentration in the gas provided in step (b) is preferably at least 0.1 vol%, more preferably at least 0.5 vol%. As shown in the accompanying examples, the present inventors have found that the mechanochemical activation is improved when carried out in the presence of such a CO 2 -rich gas. In particular, it was found that milling time can be significantly reduced and / or that improved products can be obtained when considering properties such as amorphous fraction, dehydration start temperature, pozzolanic reactivity, etc.

[0078] In highly preferred embodiments of the process described herein, by which the mechanochemically activated material of the present invention is obtainable, the gas provided in step (b) is a combustion exhaust gas, in particular an exhaust gas from fossil fuel combustion, wood pellet combustion, biomass combustion, or municipal waste combustion. Fossil fuel combustion may be coal, petroleum coke, crude oil, natural gas, shale oil, bitumen, tar sands oil, or heavy oil combustion, or any combination thereof. The combustion exhaust gas may optionally have been treated to reduce the water content, the SO 2 -content and / or the NOx content.

[0079] The CO 2 -Concentration in the gas provided in step (b) is preferably at least 0.1 vol.%, more preferably at least 0.5 vol.%. Typical CO 2Concentrations for combustion exhaust gas are in the range of 1-15 vol.%, such as 2-10 vol.%, so it is preferred that the gas provided in step (b) has a CO 2 concentration in the range of 1-15 vol.%, such as 2-10 vol.%. In alternative embodiments of the invention, the gas provided in step (b) comprises at least 80 vol.% CO 2 , preferably at least 95 vol.% CO 2 . In some embodiments of the invention, the gas provided in step (b) comprises at least 80 vol.% CO 2 , preferably at least 95 vol.% CO 2 and less than 1000 ppm (v / v) H 2 O, preferably less than 100 ppm (v / v) H 2 O. In some embodiments, the gas provided in step (b) comprises CO 2 in at least 0.1 vol.% and H 2 O in the range of 5-25 vol.%. For example, in the case of exhaust gas, the gas provided in step (b) preferably comprises CO 2in the range of 1-15 vol.%, such as 2-10 vol.% and H 2 O in the range of 5-25 vol%, such as 15-20 vol%. The gas is typically not in a supercritical state, as this is not necessary for the mild mechanochemical carbonation process of the present invention. Therefore, in any embodiment of the invention, it is highly preferred that the gas not be in a supercritical state.

[0080] In some embodiments of the invention, the process described herein by which the mechanochemically activated material of the present invention is obtainable is provided with the condition that the temperature and pressure during step (d) are selected such that the pressure is lower than the saturated vapor pressure of water at the temperature in the mechanical agitation unit.

[0081] The phrase "in the presence of said gas" in step (d) should be interpreted to mean that the atmosphere within the mechanical agitation unit consists essentially of the gas provided in step (b) when step (d) is initiated. It will be understood by those skilled in the art that the composition of the gas will change as the reaction progresses unless the reactor (the mechanical agitation unit) is continuously purged or replenished.

[0082] In general, step (d) can be carried out at atmospheric pressure, below atmospheric pressure, or above atmospheric pressure. However, it is preferred that step (d) be carried out at a pressure of less than 1000 kPa, preferably less than 500 kPa, more preferably less than 400 kPa, and even more preferably less than 300 kPa. The present inventors have found that higher pressures than this, while not excluded from the invention, are less optimal because they slow the mechanochemical activation process. The process can be carried out at pressures below atmospheric pressure, but this is typically not necessary, so the energy required to reduce the pressure below atmospheric pressure can be limited or eliminated.Therefore, it is preferred that step (d) be carried out at a pressure of at least 20 kPa, preferably at least 50 kPa, more preferably at least 80 kPa, most preferably at least 95 kPa, most preferably at least about atmospheric pressure. Overall, step (d) is preferably carried out at a pressure in the range of 20-500 kPa, preferably 50-400 kPa, most preferably 80-300 kPa. In some embodiments, step (d) is carried out at a pressure greater than 500 kPa, such as a pressure in the range of 500 kPa to 2500 kPa. In the embodiments of this paragraph, it is understood that the pressure within the mechanical agitation unit conforms to the specifications set forth herein when step (d) is initiated. It will be understood by those skilled in the art that the pressure of the gas (if not actively maintained) will change as the reaction progresses.In accordance with the invention, step (d) is carried out at pressures below the critical pressure of carbon dioxide. In the context of the present invention, it is understood that the pressure within the mechanical agitation unit conforms to the specifications set forth herein at at least one time during step (d), for example, when step (d) is initiated. In some embodiments, the pressure within the mechanical agitation unit conforms to the specifications set forth herein during most or substantially all of step (d).

[0083] In preferred embodiments of the process described herein, by which the mechanochemically activated material of the present invention is obtainable, step (d) is carried out at a temperature of at most 500°C, preferably at most 400°C, more preferably at most 300°C. In some embodiments of the process described herein, by which the mechanochemically activated material of the present invention is obtainable, step (d) is carried out at a temperature of less than 150°C, preferably less than 100°C, more preferably less than 80°C. Typically, the temperature is at least 10°C, preferably at least 20°C. The reaction temperature depends mainly on the incoming exhaust gas temperature if an exhaust gas is provided in step (b). Typical exhaust gas temperatures are 120-400°C.In preferred embodiments of the invention, no active heating is applied, and any temperature increase is attributed to the temperature of the gas provided in step (b), the friction caused by mechanical agitation, or exothermic reactions occurring during mechanochemical activation. The temperature referred to in step (d) is preferably determined on the solid material in the reactor (i.e., the mechanical agitation unit) during processing.

[0084] In embodiments of the invention, step (d) is carried out for at least 1 minute, preferably at least 30 minutes, such as at least 1 hour, at least 4 hours, or at least 8 hours. The actual time during which step (d) is carried out to achieve activation of the phyllosilicate minerals contained in the starting material depends on the mechanical agitation equipment used and the operating conditions, such as the rotation speed in the case of a ball mill. It is within the routine skills of one skilled in the art, based on the guidance provided herein, to determine a suitable operating time. For example, regular sampling of material and analysis by XRD allows monitoring of the evolution of the phyllosilicate mineral content and the amorphous fraction.

[0085] In preferred embodiments of the invention, the mechanical agitation of step (d) includes grinding, comminuting, mixing, stirring (such as slow stirring or rapid stirring), shearing (such as high torque shearing), shaking, mixing, pulverizing, atomizing, comminuting, crumbling, a fluidized bed or ultrasonic treatment, preferably grinding, mixing, stirring (such as slow stirring or rapid stirring), shearing (such as high torque shearing) or ultrasonic treatment, preferably grinding. The present inventors have found that the mechanochemical carbonation process is facilitated when the mechanical agitation of step (d) is carried out in the presence of grinding or comminuting bodies, preferably balls, bearings or beads. A preferred material is stainless steel, ceramic or alumina. In preferred embodiments of the invention, the grinding bodies are made of stainless steel.In such highly preferred embodiments of the invention, mechanical agitation may simply be the rotation of the mechanical agitation unit containing the solid feedstock, the grinding media, and the gas. For example, grinding media may be made of steel (e.g., AISI H13, modified H10), alumina, chromium white cast iron (e.g., ASTM A532), molybdenum steel (e.g., AISI M2, M4, M-42), chromium-based steels (e.g., H11, H12, H13 CPM V9, ZDP-189), or other media with a target HRC hardness of 60. Such grinding media may be used with or without surface treatments such as nitriding and carburizing. Calcination of the grinding media may also be performed. The use of grinding media can be conveniently carried out in a rotating drum.It is understood that the product obtainable by the process by which the mechanochemically activated material of the present invention is obtainable, when step (d) is carried out in a rotating drum, can also be obtained using alternative milling techniques known to those skilled in the art. Without wishing to be bound by theory, the present inventors believe that increased media density leads to improved particle size distribution and / or amorphization. Therefore, it is preferred that the media density be at least 6.5 g / cm. 3 , preferably at least 7.0 g / cm 3 and most preferably at least 7.5 g / cm 3 and more preferably at least 8.0 g / cm 3The present inventors have found that stainless steel grinding media outperform ceramic material when considering feedstock activation, such as amorphization. Without wishing to be bound by theory, it is believed that this may be due to the density and / or presence of iron oxide deposits, which act as catalysts for the mechanochemical activation of the feedstock.

[0086] In some embodiments of the invention, the mechanical agitation of step (d) is carried out in the presence of grinding aids such as dead-burned magnesia (raw magnesite sintered at a temperature of 1750°C), activated alumina powder (such as activated alumina powder, preferably with a D90 <10 nm or with a D90 <100 nm), carbon black (preferably with a D90 <60 nm), graphite nanoplatelets (GNP), activated silicon dioxide, magnesium hydroxide, or combinations thereof. In other embodiments, the mechanical agitation of step (d) is free of grinding aids except for the grinding or comminution media described herein.

[0087] In preferred embodiments, the mechanical agitation of step (d) comprises the use of grinding or comminuting media selected from stainless steel balls having a diameter of less than 20 mm, preferably less than 15 mm, more preferably less than 10 mm, and most preferably 6 mm or less. In other embodiments, the mechanical agitation of step (d) comprises the use of grinding or comminuting media selected from ceramic balls. In some embodiments, the ceramic balls are uncalcined. In other embodiments, the ceramic balls are calcined. In preferred embodiments, the ceramic balls have a diameter of less than 25 mm, preferably less than 20 mm, most preferably less than 15 mm, and even more preferably 10 mm or less.

[0088] Therefore, as will be understood from the above, in highly preferred embodiments of the invention, step (d) comprises grinding, comminuting, mixing, stirring (such as slow stirring or fast stirring), shearing (such as high torque shearing), shaking, mixing, pulverizing, pulverizing, comminuting, crumbling, a fluidized bed or ultrasonic treatment, preferably grinding, comminuting, mixing, stirring (such as slow stirring or fast stirring), shearing (such as high torque shearing) or ultrasonic treatment, most preferably grinding or comminuting, in the presence of grinding or comminuting media.

[0089] In preferred processes by which the mechanochemically activated material of the present invention is obtainable, the mechanical agitation of step (d) uses grinding or comminuting bodies, wherein the mass ratio of grinding or comminuting bodies to starting material is more than 5:1, preferably more than 10:1, more preferably more than 25:1. It has been found that such high relative amounts of grinding or comminuting bodies strongly improve the activation process.

[0090] In preferred processes by which the mechanochemically activated material of the present invention is obtainable, apart from optional grinding or comminuting bodies, the starting material provided in step (a) forms the major part of the material introduced into the agitation unit in step (c) of the process by which the mechanochemically activated material of the present invention is obtainable and thus, apart from optional grinding or comminuting bodies, forms the major part of the material present during step (d) of the process by which the mechanochemically activated material of the present invention is obtainable. Preferably, apart from optional grinding or comminuting bodies, the starting material provided in step (a) forms at least 90% by weight, preferably at least 95% by weight, more preferably about 100% by weight.-% of the material introduced into the agitation unit in step (c) of the process by which the mechanochemically activated material of the present invention is obtainable and thus constitutes, apart from optional grinding or comminuting media, at least 90 wt.%, preferably at least 95 wt.%, more preferably about 100 wt.% of the material present during step (d) of the process by which the mechanochemically activated material of the present invention is obtainable.

[0091] As will be clear from the present description, in highly preferred embodiments, step (d) is a substantially dry process. While some moisture is likely to be naturally present in the starting material (not to be confused with the hydrates that are part of the mineral structure), step (d) is most preferably not performed on an aqueous solution or slurry. The present inventors have found that performing step (d) on a solid greatly improves energy efficiency (since no water needs to be subsequently removed) and imparts unique properties to the resulting mechanochemically activated materials. In embodiments of the invention, the solid starting material provided in step (a) has a moisture content of less than 30 wt.% (based on the total weight of the solid starting material), preferably less than 20 wt.-%, where the moisture content is determined by weight loss during drying to constant weight at 120 °C.

[0092] The moisture content of the starting material can be adjusted before or during the process by which the mechanochemically activated material of the present invention is obtainable, for example by spraying the solid starting material with an aqueous composition such as water before and / or during step (d).

[0093] It is within the routine capabilities of one skilled in the art to adjust the moisture content of the starting material based on the instructions provided herein, for example by spraying the solid starting material with an aqueous composition such as water before and / or during step (d).

[0094] In particular, the present inventors have found it important that step (d) be carried out in such a way as to effect certain degrees of amorphization, size reduction, and / or decrease in the dehydration start temperature during step (d), i.e., during mechanical agitation. This is representative, among other things, of the time of mechanical agitation (such as milling), which depends strongly on the equipment used. However, as shown in the accompanying examples, the present inventors have found that these properties reach optimal values, after which further mechanical agitation (such as milling) will lead to one or more undesirable effects such as agglomeration (size increase), stabilization of the hydrates (increase in the dehydration start temperature), and recrystallization (decrease in the amorphous fraction).

[0095] Therefore, in highly preferred embodiments of the invention, the process by which the mechanochemically activated material of the present invention is obtainable is provided, wherein amorphization, size reduction, decrease in phyllosilicate mineral content and decrease in dehydration start temperature during step (d) are effected such that the process by which the mechanochemically activated material of the present invention is obtainable has one, two, three or all four, preferably all four, of the following properties • the ratio of the amorphous portion of the mechanochemically activated material obtained in step (d) to the amorphous portion of the starting material from step (a) is at least 1.1:1, preferably at least 1.15:1, preferably at least 1.2:1, more preferably at least 1.3:1, preferably at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1; • the ratio of the D50 of the mechanochemically activated material obtained in step (d) to the D50 of the starting material precursor from step (a) is less than 0.95:1, preferably less than 0.9:1, preferably less than 0.85:1, preferably less than 0.8:1, preferably less than 0.7:1, preferably less than 0.6:1, preferably less than 0.5:1, more preferably less than 0.4:1, even more preferably less than 0.3:1 and most preferably less than 0.2:1; • the ratio of the phyllosilicate content of the starting material from step (a) to the phyllosilicate content of the mechanochemically activated material obtained in step (d) is at least 1.1:1, preferably at least 1.15:1, preferably at least 1.2:1, more preferably at least 1.3:1, preferably at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1, even more preferably at least 4:1; • the dehydration start temperature of the mechanochemically activated material obtained in step (d) is less than 250 °C, preferably less than 200 °C, more preferably less than 150 °C, even more preferably less than 130 °C.

[0096] In preferred embodiments of the invention, the process by which the mechanochemically activated material of the present invention is obtainable is provided, wherein amorphization, size reduction, decrease in phyllosilicate mineral content and decrease in dehydration start temperature are effected during step (d) such that the process exhibits two, three or all four, preferably all four, of the following properties • the ratio of the amorphous portion of the mechanochemically activated material obtained in step (d) to the amorphous portion of the starting material from step (a) is at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1; • the ratio of the D50 of the mechanochemically activated material obtained in step (d) to the D50 of the starting material precursor from step (a) is less than 0.85:1, preferably less than 0.8:1, preferably less than 0.7:1, preferably less than 0.6:1, preferably less than 0.5:1, more preferably less than 0.4:1, even more preferably less than 0.3:1 and most preferably less than 0.2:1; • the ratio of the phyllosilicate content of the starting material from step (a) to the phyllosilicate content of the mechanochemically activated material obtained in step (d) is at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1, even more preferably at least 4:1; • the dehydration start temperature of the mechanochemically activated material obtained in step (d) is less than 250 °C, preferably less than 200 °C, more preferably less than 150 °C, even more preferably less than 130 °C.

[0097] In preferred embodiments of the invention, the method by which the mechanochemically activated material of the present invention is obtainable is provided, wherein amorphization, size reduction, decrease in phyllosilicate mineral content, and decrease in dehydration start temperature during step (d) are effected such that the method has two, three, or all four, preferably all four, of the following properties • the ratio of the amorphous fraction of the mechanochemically activated material obtained in step (d) to the amorphous fraction of the starting material of step (a) is at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1; • the ratio of the D50 of the mechanochemically activated material obtained in step (d) to the D50 of the starting material precursor from step (a) is less than 0.5:1, more preferably less than 0.4:1, even more preferably less than 0.3:1 and most preferably less than 0.2:1; • the ratio of the phyllosilicate content of the starting material from step (a) to the phyllosilicate content of the mechanochemically activated material obtained in step (d) is at least 3:1, more preferably at least 3.5:1, even more preferably at least 4:1; • the dehydration start temperature of the mechanochemically activated material obtained in step (d) is less than 250 °C, preferably less than 200 °C, more preferably less than 150 °C, even more preferably less than 130 °C.

[0098] In preferred embodiments of the invention, the process by which the mechanochemically activated material of the present invention is obtainable is provided, wherein amorphization, size reduction, decrease in phyllosilicate mineral content and decrease in dehydration start temperature are effected during step (d) such that the process exhibits one, two, three or all four, preferably all four, of the following properties • the ratio of the amorphous portion of the mechanochemically activated material obtained in step (d) to the amorphous portion of the starting material from step (a) is at least 1.1:1, preferably at least 1.15:1, preferably at least 1.2:1, more preferably at least 1.3:1, preferably at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1; • the ratio of the D50 of the mechanochemically activated material obtained in step (d) to the D50 of the starting material precursor from step (a) is less than 0.95:1, preferably less than 0.9:1, preferably less than 0.85:1, preferably less than 0.8:1, preferably less than 0.7:1, preferably less than 0.6:1, preferably less than 0.5:1, more preferably less than 0.4:1, even more preferably less than 0.3:1 and most preferably less than 0.2:1; • the ratio of the phyllosilicate content of the starting material from step (a) to the phyllosilicate content of the mechanochemically activated material obtained in step (d) is at least 1.1:1, preferably at least 1.15:1, preferably at least 1.2:1, more preferably at least 1.3:1, preferably at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1, even more preferably at least 4:1; • the dehydration start temperature of the mechanochemically activated material obtained in step (d) is less than 250°C, preferably less than 200°C, more preferably less than 150°C, even more preferably less than 130°C;wherein the starting material of step (a) comprises less than 10 wt% kaolinite, preferably less than 5 wt% kaolinite and more preferably less than 3 wt% kaolinite based on the total weight of the starting material.

[0099] In preferred embodiments of the invention, the process by which the mechanochemically activated material of the present invention is obtainable is provided, wherein amorphization, size reduction, decrease in phyllosilicate mineral content and decrease in dehydration start temperature are effected during step (d) such that the process exhibits two, three or all four, preferably all four, of the following properties • the ratio of the amorphous portion of the mechanochemically activated material obtained in step (d) to the amorphous portion of the starting material from step (a) is at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1; • the ratio of the D50 of the mechanochemically activated material obtained in step (d) to the D50 of the starting material precursor from step (a) is less than 0.85:1, preferably less than 0.8:1, preferably less than 0.7:1, preferably less than 0.6:1, preferably less than 0.5:1, more preferably less than 0.4:1, even more preferably less than 0.3:1 and most preferably less than 0.2:1; • the ratio of the phyllosilicate content of the starting material from step (a) to the phyllosilicate content of the mechanochemically activated material obtained in step (d) is at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1, even more preferably at least 4:1; • the dehydration start temperature of the mechanochemically activated material obtained in step (d) is less than 250°C, preferably less than 200°C, more preferably less than 150°C, even more preferably less than 130°C;wherein the starting material of step (a) comprises less than 10 wt% kaolinite, preferably less than 5 wt% kaolinite and more preferably less than 3 wt% kaolinite based on the total weight of the starting material.

[0100] In preferred embodiments of the invention, the process by which the mechanochemically activated material of the present invention is obtainable is provided, wherein amorphization, size reduction, decrease in phyllosilicate mineral content and decrease in dehydration start temperature are effected during step (d) such that the process exhibits one, two, three or all four, preferably all four, of the following properties • the ratio of the amorphous portion of the mechanochemically activated material obtained in step (d) to the amorphous portion of the starting material from step (a) is at least 1.1:1, preferably at least 1.15:1, preferably at least 1.2:1, more preferably at least 1.3:1, preferably at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1; • the ratio of the D50 of the mechanochemically activated material obtained in step (d) to the D50 of the starting material precursor from step (a) is less than 0.95:1, preferably less than 0.9:1, preferably less than 0.85:1, preferably less than 0.8:1, preferably less than 0.7:1, preferably less than 0.6:1, preferably less than 0.5:1, more preferably less than 0.4:1, even more preferably less than 0.3:1 and most preferably less than 0.2:1; • the ratio of the phyllosilicate content of the starting material from step (a) to the phyllosilicate content of the mechanochemically activated material obtained in step (d) is at least 1.1:1, preferably at least 1.15:1, preferably at least 1.2:1, more preferably at least 1.3:1, preferably at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1, even more preferably at least 4:1; • the dehydration start temperature of the mechanochemically activated material obtained in step (d) is less than 250 °C, preferably less than 200 °C, more preferably less than 150 °C, even more preferably less than 130 °C;wherein the starting material of step (a) has an amorphous fraction of more than 10 wt.%, preferably more than 20 wt.%, more preferably more than 25 wt.%, based on the total weight of the starting material.

[0101] In preferred embodiments of the invention, the process by which the mechanochemically activated material of the present invention is obtainable is provided, wherein amorphization, size reduction, decrease in phyllosilicate mineral content and decrease in dehydration start temperature are effected during step (d) such that the process has two, three or all four, preferably all four of the following features • the ratio of the amorphous portion of the mechanochemically activated material obtained in step (d) to the amorphous portion of the starting material from step (a) is at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1; • the ratio of the D50 of the mechanochemically activated material obtained in step (d) to the D50 of the starting material precursor from step (a) is less than 0.85:1, preferably less than 0.8:1, preferably less than 0.7:1, preferably less than 0.6:1, preferably less than 0.5:1, more preferably less than 0.4:1, even more preferably less than 0.3:1 and most preferably less than 0.2:1; • the ratio of the phyllosilicate content of the starting material from step (a) to the phyllosilicate content of the mechanochemically activated material obtained in step (d) is at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1, even more preferably at least 4:1; • the dehydration start temperature of the mechanochemically activated material obtained in step (d) is less than 250°C, preferably less than 200°C, more preferably less than 150°C, even more preferably less than 130°C; wherein the starting material of step (a) has an amorphous fraction of more than 10% by weight, preferably more than 20% by weight, more preferably more than 25% by weight, based on the total weight of the starting material.

[0102] In preferred embodiments of the invention, the process by which the mechanochemically activated material of the present invention is obtainable is provided, wherein amorphization, size reduction, decrease in phyllosilicate mineral content and decrease in dehydration start temperature are effected during step (d) such that the process has one, two, three or all four, preferably all four of the following features • the ratio of the amorphous portion of the mechanochemically activated material obtained in step (d) to the amorphous portion of the starting material from step (a) is at least 1.1:1, preferably at least 1.15:1, preferably at least 1.2:1, more preferably at least 1.3:1, preferably at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1; • the ratio of the D50 of the mechanochemically activated material obtained in step (d) to the D50 of the starting material precursor from step (a) is less than 0.95:1, preferably less than 0.9:1, preferably less than 0.85:1, preferably less than 0.8:1, preferably less than 0.7:1, preferably less than 0.6:1, preferably less than 0.5:1, more preferably less than 0.4:1, even more preferably less than 0.3:1 and most preferably less than 0.2:1; • the ratio of the phyllosilicate content of the starting material from step (a) to the phyllosilicate content of the mechanochemically activated material obtained in step (d) is at least 1.1:1, preferably at least 1.15:1, preferably at least 1.2:1, more preferably at least 1.3:1, preferably at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1, even more preferably at least 4:1; • the dehydration start temperature of the mechanochemically activated material obtained in step (d) is less than 250°C, preferably less than 200°C, more preferably less than 150°C, even more preferably less than 130°C;wherein the starting material of step (a) comprises at least 1 wt% illite, more preferably at least 5 wt% illite and most preferably at least 10 wt% illite based on the total weight of the starting material.

[0103] In preferred embodiments of the invention, the process by which the mechanochemically activated material of the present invention is obtainable is provided, wherein amorphization, size reduction, decrease in phyllosilicate mineral content and decrease in dehydration start temperature are effected during step (d) such that the process has two, three or all four, preferably all four of the following features • the ratio of the amorphous portion of the mechanochemically activated material obtained in step (d) to the amorphous portion of the starting material from step (a) is at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1; • the ratio of the D50 of the mechanochemically activated material obtained in step (d) to the D50 of the starting material precursor from step (a) is less than 0.85:1, preferably less than 0.8:1, preferably less than 0.7:1, preferably less than 0.6:1, preferably less than 0.5:1, more preferably less than 0.4:1, even more preferably less than 0.3:1 and most preferably less than 0.2:1; • the ratio of the phyllosilicate content of the starting material from step (a) to the phyllosilicate content of the mechanochemically activated material obtained in step (d) is at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1, even more preferably at least 4:1; • the dehydration start temperature of the mechanochemically activated material obtained in step (d) is less than 250°C, preferably less than 200°C, more preferably less than 150°C, even more preferably less than 130°C;wherein the starting material of step (a) comprises at least 1 wt% illite, more preferably at least 5 wt% illite and most preferably at least 10 wt% illite based on the total weight of the starting material.

[0104] In preferred embodiments of the invention, the process by which the mechanochemically activated material of the present invention is obtainable is provided, wherein amorphization, size reduction, decrease in phyllosilicate mineral content and decrease in dehydration start temperature are effected during step (d) such that the process has one, two, three or all four, preferably all four of the following features • the ratio of the amorphous portion of the mechanochemically activated material obtained in step (d) to the amorphous portion of the starting material from step (a) is at least 1.1:1, preferably at least 1.15:1, preferably at least 1.2:1, more preferably at least 1.3:1, preferably at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1; • the ratio of the D50 of the mechanochemically activated material obtained in step (d) to the D50 of the starting material precursor from step (a) is less than 0.95:1, preferably less than 0.9:1, preferably less than 0.85:1, preferably less than 0.8:1, preferably less than 0.7:1, preferably less than 0.6:1, preferably less than 0.5:1, more preferably less than 0.4:1, even more preferably less than 0.3:1 and most preferably less than 0.2:1; • the ratio of the phyllosilicate content of the starting material from step (a) to the phyllosilicate content of the mechanochemically activated material obtained in step (d) is at least 1.1:1, preferably at least 1.15:1, preferably at least 1.2:1, more preferably at least 1.3:1, preferably at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1, even more preferably at least 4:1; • the dehydration start temperature of the mechanochemically activated material obtained in step (d) is less than 250°C, preferably less than 200°C, more preferably less than 150°C, even more preferably less than 130°C;wherein the starting material of step (a) comprises at least 50 wt% illite, more preferably at least 70 wt% illite, more preferably at least 85 wt% illite based on the total weight of the starting material.

[0105] In preferred embodiments of the invention, the process by which the mechanochemically activated material of the present invention is obtainable is provided, wherein amorphization, size reduction, decrease in phyllosilicate mineral content and decrease in dehydration start temperature are effected during step (d) such that the process has two, three or all four, preferably all four of the following features • the ratio of the amorphous portion of the mechanochemically activated material obtained in step (d) to the amorphous portion of the starting material from step (a) is at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1; • the ratio of the D50 of the mechanochemically activated material obtained in step (d) to the D50 of the starting material precursor from step (a) is less than 0.85:1, preferably less than 0.8:1, preferably less than 0.7:1, preferably less than 0.6:1, preferably less than 0.5:1, more preferably less than 0.4:1, even more preferably less than 0.3:1 and most preferably less than 0.2:1; • the ratio of the phyllosilicate content of the starting material from step (a) to the phyllosilicate content of the mechanochemically activated material obtained in step (d) is at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1, even more preferably at least 4:1; • the dehydration start temperature of the mechanochemically activated material obtained in step (d) is less than 250 °C, preferably less than 200 °C, more preferably less than 150 °C, even more preferably less than 130 °C;wherein the starting material of step (a) comprises at least 50 wt% illite, more preferably at least 70 wt% illite, more preferably at least 85 wt% illite based on the total weight of the starting material.

[0106] In preferred embodiments of the invention, the process by which the mechanochemically activated material of the present invention is obtainable is provided, wherein amorphization, size reduction, decrease in phyllosilicate mineral content and decrease in dehydration start temperature are effected during step (d) such that the process has one, two, three or all four, preferably all four of the following features • the ratio of the amorphous portion of the mechanochemically activated material obtained in step (d) to the amorphous portion of the starting material from step (a) is at least 1.1:1, preferably at least 1.15:1, preferably at least 1.2:1, more preferably at least 1.3:1, preferably at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1; • the ratio of the D50 of the mechanochemically activated material obtained in step (d) to the D50 of the starting material precursor from step (a) is less than 0.95:1, preferably less than 0.9:1, preferably less than 0.85:1, preferably less than 0.8:1, preferably less than 0.7:1, preferably less than 0.6:1, preferably less than 0.5:1, more preferably less than 0.4:1, even more preferably less than 0.3:1 and most preferably less than 0.2:1; • the ratio of the phyllosilicate content of the starting material from step (a) to the phyllosilicate content of the mechanochemically activated material obtained in step (d) is at least 1.1:1, preferably at least 1.15:1, preferably at least 1.2:1, more preferably at least 1.3:1, preferably at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1, even more preferably at least 4:1; • the dehydration start temperature of the mechanochemically activated material obtained in step (d) is less than 250°C, preferably less than 200°C, more preferably less than 150°C, even more preferably less than 130°C;wherein the starting material of step (a) comprises at least 1 wt% of a mineral species from the chlorite group, more preferably at least 5 wt% of a mineral species from the chlorite group and most preferably at least 10 wt% of a mineral species from the chlorite group based on the total weight of the starting material.

[0107] In preferred embodiments of the invention, the process by which the mechanochemically activated material of the present invention is obtainable is provided, wherein amorphization, size reduction, decrease in phyllosilicate mineral content and decrease in dehydration start temperature are effected during step (d) such that the process has two, three or all four, preferably all four of the following features • the ratio of the amorphous portion of the mechanochemically activated material obtained in step (d) to the amorphous portion of the starting material from step (a) is at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1; • the ratio of the D50 of the mechanochemically activated material obtained in step (d) to the D50 of the starting material precursor from step (a) is less than 0.85:1, preferably less than 0.8:1, preferably less than 0.7:1, preferably less than 0.6:1, preferably less than 0.5:1, more preferably less than 0.4:1, even more preferably less than 0.3:1 and most preferably less than 0.2:1; • the ratio of the phyllosilicate content of the starting material from step (a) to the phyllosilicate content of the mechanochemically activated material obtained in step (d) is at least 1.5:1, preferably at least 2:1, more preferably at least 3:1, even more preferably at least 3.5:1, even more preferably at least 4:1; • the dehydration start temperature of the mechanochemically activated material obtained in step (d) is less than 250°C, preferably less than 200°C, more preferably less than 150°C, even more preferably less than 130°C;wherein the starting material of step (a) comprises at least 1 wt% of a mineral species from the chlorite group, more preferably at least 5 wt% of a mineral species from the chlorite group and most preferably at least 10 wt% of a mineral species from the chlorite group based on the total weight of the starting material.

[0108] It is preferred that step (d) be carried out such that the dehydration start temperature of the mechanochemically activated material obtained in step (d) is at least 50°C lower than the dehydration start temperature of the starting material provided in step (a), preferably at least 100°C lower, more preferably at least 175°C lower. As one skilled in the art will understand, this involves milling for a sufficient period of time. However, the inventors have found that excessive milling leads to reagglomeration and recrystallization and stabilization of hydrates, so the process should be terminated in a timely manner.

[0109] As will be understood by those skilled in the art, it is preferred that step (d) be terminated when the trends of amorphization, size reduction, and / or dehydration onset temperature begin to reverse. During step (d), the increase in specific surface area is proportional to the milling time until the specific surface area enters the agglomeration phase, i.e., where the specific surface area decreases and the particles become chemically bound into agglomerates. In preferred embodiments, step (d) is terminated before or shortly after the D10, D50, D90, and / or specific surface area begin to increase again after the initial reduction phase. For example, in some highly preferred embodiments, the activated material is recovered from step (d) when the D50 is less than 120% of the minimum D50 achieved during step (d).In some embodiments of the invention, the activated material is obtained from step (d) when the mechanochemically activated material has one, two or all of the following features:. • a D10 in the range of 0.005-3 µm, preferably 0.01-2 µm, most preferably 0.1-1.4 µm; • a D50 in the range of 0.1-30 µm, preferably 0.5-15 µm, most preferably 1-10 µm; • a D90 in the range of 0.5-100 µm, preferably 1-80 µm, most preferably 5-70 µm; • a dehydration start temperature of less than 250°C, preferably less than 200°C, more preferably less than 150°C, even more preferably less than 130°C, even more preferably less than 120°C and most preferably less than 110°C; • a phyllosilicate mineral content of less than 10 wt%, based on the total weight of the mechanochemically activated material, preferably less than 5 wt%.

[0110] In embodiments of the invention, the process described herein by which the mechanochemically activated material of the present invention is obtainable does not comprise a solid-liquid separation step selected from filtration, decantation and gravitational separation (e.g. using cyclones) after step (d), preferably the process by which the mechanochemically activated material of the present invention is obtainable does not comprise a solid-liquid separation step after step (d).

[0111] In embodiments of the invention, the process described herein by which the mechanochemically activated material of the present invention is obtainable does not comprise a size selection step, such as a sieving or screening step, after step (d). Properties of the mechanochemically activated material obtained in step (d)

[0112] Step (d) typically involves recovering the mechanochemically activated material. In practice, in batch operation, mechanical agitation is stopped and the activated material is removed from the mechanical agitation unit. In a continuous process, activated material can be recovered continuously.

[0113] In another aspect, the invention provides the mechanochemically activated material obtainable from the process described herein, by which the mechanochemically activated material of the present invention is obtainable. The properties of the mechanochemically activated material described herein in connection with step (d) of the process by which the mechanochemically activated material of the present invention is obtainable apply equally to the mechanochemically activated material obtainable from the process.

[0114] In some embodiments of the invention, the mechanochemically activated material obtainable from the process described herein by which the mechanochemically activated material of the present invention is obtainable has one, two, three or four, preferably all four of the following properties: • a D50 in the range of 0.1-30 µm, preferably 0.5-15 µm, most preferably 1-10 µm; • a dehydration start temperature of less than 250°C, preferably less than 200°C, more preferably less than 150°C, even more preferably less than 130°C; • an amorphous portion of at least 25% by weight, preferably at least 30% by weight and more preferably at least 35% by weight; • a phyllosilicate mineral content of less than 10 wt%, based on the total weight of the mechanochemically activated material, preferably less than 5 wt%.

[0115] In some embodiments, the mechanochemically activated material obtained from step (d) has a dehydration start temperature that is at least 50°C lower than the dehydration start temperature of the starting material provided in step (a), preferably at least 100°C lower, more preferably at least 175°C lower.

[0116] In some embodiments, the mechanochemically activated material obtained from step (d) has an amorphous content of at least 25 wt.%, preferably at least 30 wt.%, more preferably at least 35 wt.%, even more preferably at least 40 wt.%, and most preferably at least 50 wt.%.

[0117] Without wishing to be bound by theory, the inventors believe that milling breaks up the phyllosilicate layer stacks and leads to increased structural disorder, resulting in weaker bonding of OH groups and reduced dehydration temperatures. The hydroxyl sites in native phyllosilicate, as present in the starting material, have a dehydration temperature between 440-450°C, as observed by TGA. In some embodiments, mechanochemically activated material is provided, obtainable from the process described herein by which the mechanochemically activated material of the present invention is obtainable, having a dehydration onset temperature of less than 250°C, preferably less than 200°C, more preferably less than 150°C, even more preferably less than 130°C.In such embodiments, the inventors found that the resulting mechanochemically activated material results in reduced water requirements when used as a supplemental cementitious material.

[0118] In preferred embodiments, the mechanochemically activated material obtained from step (d) meets the strength requirements specified in ASTM C618-12a (2012). In particular embodiments, the process described herein by which the mechanochemically activated material of the present invention is obtainable does not include a size selection step, such as a screening or sieving step, after step (d), and the starting material obtained in step (d) meets the strength requirements specified in ASTM C618-12a (2012).

[0119] In embodiments of the invention, the mechanochemically activated material obtained in step (d) has a specific surface area of ​​less than 5 m 2 / g, preferably less than 3 m 2 / g, more preferably less than 2 m 2 / g on.

[0120] In embodiments of the invention, the mechanochemically activated material obtained in step (d) has one, two or three, preferably three, of the following properties: • a D10 in the range of 0.005-3 µm, preferably 0.01-2 µm, most preferably 0.1-1.4 µm; • a D50 in the range of 0.1-30 µm, preferably 0.5-15 µm, most preferably 1-10 µm; • a D90 in the range of 0.5-100 µm, preferably 1-80 µm, most preferably 5-70 µm.

[0121] According to the invention, the mechanochemically activated material obtained in step (d) typically has a Strength Activity Index (SAI) on day 7 of at least 80%, preferably at least 85%. The inventors have observed that the mechanochemical process by which the mechanochemically activated material of the present invention is obtainable makes it possible to obtain mechanochemically activated material with excellent SAI on day 7. Therefore, in preferred embodiments, the mechanochemically activated material obtained in step (d) has an SAI on day 7 of at least 105%, preferably at least 110%, even more preferably at least 125%.

[0122] In embodiments of the invention, the mechanochemically activated material obtained in step (d) has a strength activity index (SAI) on day 28 of at least 75%, preferably at least 95%, more preferably at least 100%. The inventors have observed that the mechanochemical process by which the mechanochemically activated material of the present invention is obtainable makes it possible to obtain mechanochemically activated material with excellent SAI on day 28. Therefore, in preferred embodiments, the mechanochemically activated material obtained in step (d) has an SAI on day 28 of at least 110%, preferably at least 115%, even more preferably at least 125%.

[0123] In some embodiments of the invention, the mechanochemically activated material obtained in step (d) has a heat of hydration after 12 hours, determined according to modified ASTM C 1897-20, of at least 100 J / g, preferably at least 150 J / g, more preferably at least 200 J / g. The mechanochemically activated material obtained in step (d) preferably has a heat of hydration after 72 hours, determined according to modified ASTM C 1897-20, of at least 150 J / g, preferably at least 200 J / g, more preferably at least 250 J / g.

[0124] In embodiments of the invention, the mechanochemically activated material obtained in step (d) has a water requirement of less than 97%, preferably less than 96%, more preferably less than 95%. The inventors have observed that the mechanochemical process by which the mechanochemically activated material of the present invention is obtainable makes it possible to obtain mechanochemically activated material with an extremely low water requirement. Therefore, in preferred embodiments, the mechanochemically activated material obtained in step (d) has a water requirement of less than 93%, preferably less than 91%. Composition comprising a mechanochemically activated material

[0125] The materials obtainable by the mechanochemical activation of the present invention are useful, among other things, as a supplemental cementitious material. Therefore, in another aspect, the invention provides a composition comprising a mechanochemically activated material as described herein and another material selected from the group consisting of asphalt, cement, geopolymers, polymers, and combinations thereof, preferably cement, more preferably Portland cement.

[0126] In embodiments of the invention, the further material is a polymer selected from thermoplastic polymers and thermosetting polymers. In preferred embodiments of the invention, the further component is a polymer selected from the group consisting of epoxy resin, phenol-formaldehyde resin, polyalkylene terephthalate (preferably polyethylene terephthalate), polyalkylene adipate terephthalate (preferably polybutylene adipate terephthalate), polyalkylene isosorbide terephthalate (preferably polyethylene isosorbide 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, poly-lactic 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 a polyolefin such as polypropylene, polyethylene, copolymers thereof, and combinations thereof. The term "polymer" as used herein includes copolymers, such as block copolymers.

[0127] In highly preferred embodiments, the further material is selected from cement, asphalt, geopolymers or combinations thereof.

[0128] According to the invention, the cement can be a hydraulic or non-hydraulic cement. In preferred embodiments of the invention, the cement is a hydraulic cement, such as Portland cement. In highly preferred embodiments of the invention, the cement is one of the cements defined in EN197-1 (2011), preferably Portland cement as defined in EN197-1 (2011).

[0129] In embodiments of the invention, the composition comprises at least 0.1 wt.% (based on the total weight of the composition), preferably at least 1 wt.%, more preferably more than 5 wt.% of the mechanochemically activated material and / or at least 0.1 wt.% (based on the total weight of the composition), preferably more than 1 wt.%, more preferably more than 20 wt.% of the further material.

[0130] In embodiments of the invention, the composition comprises less than 60 wt.% (based on the total weight of the composition), preferably less than 50 wt.%, more preferably less than 45 wt.% of the mechanochemically activated material and / or less than 95 wt.% (based on the total weight of the composition), preferably less than 90 wt.%, more preferably less than 80 wt.% of the further material.

[0131] In embodiments of the invention, the composition is provided wherein the weight:weight ratio of the mechanochemically activated material to the further material is in the range of 1:9 to 2:1, preferably in the range of 1:8 to 1:1, more preferably in the range of 1:6 to 5:6.

[0132] In embodiments of the invention, the composition comprises 5-70 wt% (based on the total weight of the composition), preferably 10-60 wt%, more preferably 20-50 wt% of the mechanochemically activated material and 30-95 wt% (based on the total weight of the composition), preferably 40-90 wt%, preferably 50-80 wt% of the further material.

[0133] In embodiments of the invention, the composition comprises less than 5 wt.% (based on the total weight of the composition) of water, preferably less than 1 wt.%, more preferably less than 0.1 wt.%. The amount of water can conveniently be determined as mass loss up to 120°C, measured by TGAMS using a temperature gradient in which the temperature was increased from room temperature to 800°C at a rate of 10°C / min. In embodiments of the invention, the composition consists of the mechanochemically activated material and the further material.

[0134] The mechanochemically activated material as described herein can be used, for example: • as a filler, preferably as a filler in a material selected from the group consisting of asphalt, cement, geopolymers, mortar, polymers and combinations thereof; • as a partial replacement for asphalt, geopolymer, clinker or cement in concrete or mortar; • to increase the compressive strength of concrete, cement or mortar; • to improve the durability of concrete or mortar; • to reduce the expansion of concrete; • to improve the durability of concrete or mortar by reducing chloride permeability and / or porosity; • to improve the strength activity index of concrete or mortar; and / or • to reduce the water requirement of concrete or mortar, preferably, • to simultaneously improve the strength activity index of concrete and reduce the water demand of concrete; or • to simultaneously improve the strength activity index of mortar and reduce the water requirement of mortar. Examples

[0135] Particle size distribution and specific surface area measurements were carried out on a Brookhaven laser particle size analyzer, model Microbrook 2000LD, using the Fraunhofer theory of light scattering, and the data were reported using a volume-equivalent sphere model.

[0136] The compressive strength, strength activity index, and water demand were measured according to ASTM C311 / C311M-22. As will be apparent to those skilled in the art, the clay precursor or carbonated clay of the present invention was used in place of the "fly ash or natural pozzolans" specified in the standard when conducting these tests.

[0137] XRD data were collected using a PANalytical Aeris X-ray diffractometer. Samples for XRD analysis were finely crushed and ground using an agate mortar and pestle. Corundum was used as an external standard and was measured with the same instrument configuration shortly after the sample was measured. The weight percentage of the amorphous portion of the sample was determined using the K-factor of the external standard phase.

[0138] The heat of hydration was measured according to modified ASTM C 1897-20.

[0139] The hydration start temperature and the wt.% hydrates were determined using a Mettler Toledo TGA / DSC 3+, with a 30 - 40 mg sample used, where the TGA was carried out under an inert atmosphere, using a temperature trajectory in which the temperature was increased from room temperature to 105 °C and held at 105 °C for 5 to 10 minutes before the temperature was increased to 1000 °C at a ramp rate of 10 °C / min. The wt.% hydrates is calculated based on the mass loss, as determined by TGA at different temperatures (105 °C and 1000 °C), according to the following formula: TGA mass loss(%)105−TGA mass loss(%)1000TGA mass loss(%)105

[0140] The elemental composition was determined by EDS. Samples for EDS analysis were finely crushed and ground using an agate mortar and pestle. EDS data were collected using a JEOL JED-2300 DRY SDD EDS detector.

[0141] In the following tables, where the gas Ar or CO 2 is 99 vol% or higher Ar or CO 2 .

[0142] The starting materials used in the examples were coarse materials with particles of size 1-10 cm. Example 1

[0143] Mechanochemically activated material was prepared by placing 50 g of starting material 1 (uncalcined shale containing 3.5 wt% kaolinite, 10.8 wt% chlorite, 20.4 wt% illite, 19.8 wt% quartz, and 33.9 wt% amorphous fraction) into a pressure cell containing 1.4 kg of primary grinding media (6 mm diameter stainless steel balls). The cell was pressurized with gas and rotated on rollers at 65 rpm to obtain mechanochemically activated material. The reaction was initiated at room temperature, and no heating or cooling was applied. Table 1: Conditions applied during the mechanochemical activation of the starting material Sample 1 Sample 2 Sample 3 Sample 4 Sample 5 Sample 6 gas Air Air Air CO 2 CO 2 CO 2 Pressure (PSIG) 0 0 0 65 65 65 Bullet stainless steel stainless steel stainless steel stainless steel stainless steel stainless steel Time (h) 24 48 72 24 48 72

[0144] The results of the mechanochemical activation are shown in the table below. Table 2: Results of mechanochemical activation of the starting material sample 1 sample 2 sample 3 sample 4 sample 5 sample 6 Amorphous fraction wt% 40,4 48,4 46,4 57,2 68,0 59,9 D10 (µm) 0,78 0,71 0,74 1,23 0,84 0,92 D50 (µm) 2,87 2,07 2,16 8,57 6,90 7,02 D90 (µm) 11,71 9,95 10,52 208,1 34,58 33,83 SSA (m 2 / g) 1,15 1,38 1,32 0,63 0,84 0,80 TGA mass loss @ 105 °C (%) 2 2 3 2,5 2,5 2,5 TGA mass loss @ 1000 °C (%) 8 8 10 12 10,5 12 Hydrates wt.% 6 6 7 10 8 10 Dehydration start temperature (°C) 110 110 110 130 110 110 Example 2

[0145] Mechanochemically activated material was prepared by placing 50 g of starting material 2 (uncalcined clay containing 6.4 wt% kaolinite, 10.8 wt% chlorite, 19 wt% illite, 31 wt% quartz, and 24.1 wt% amorphous fraction) into a pressure cell containing 1.4 kg of the first grinding media (10 mm diameter ceramic balls or 6 mm diameter stainless steel balls). The cell was pressurized with gas and rotated on rollers at 65 rpm to obtain mechanochemically activated material. The reaction was initiated at room temperature, and no heating or cooling was applied. Table 3: Conditions applied during the mechanochemical activation of the starting material Sample 7 Sample 8 Sample 9 gas Air CO 2 CO 2 Pressure (PSIG) 0 65 65 Bullet Ceramics Ceramics stainless steel Time (h) 48 48 48

[0146] The results of the mechanochemical activation are shown in the table below. Table 6: Results of the mechanochemical activation of the starting material Sample 7 Sample 8 Sample 9 Kaolinite wt.% 3,0 0,6 0,5 Illite wt% 18,8 10,8 4,8 Quartz wt% 30,7 27,4 28,2 Amorphous portion % by weight 31,3 51,3 59,8 D10 (µm) 0,8 0,74 0,73 D50 (µm) 3,2 2,44 2,89 D90 (µm) 462,8 8,93 10,89 SSA (m 2 / g) 1,1 1,30 1,27

[0147] The elemental composition of the starting material before and after mechanochemical activation is shown in Table 7. Table 7: Elemental composition of the starting material before and after treatment % by weight Source material 2 Sample 9 O 53,39 54,29 Si 17,90 16,94 C 8,44 10,62 Al 6,54 6,07 Fe 5,24 4,31 K 2,68 2,40 Ca 2,28 2,06 Mg 1,83 1,72 N / a 0,65 0,69 Ti 0,49 0,41 Cl 0,32 0,26 Cu 0,13 - S 0,12 0,13 Mn - 0,09 Cr - 0,03 No - - Example 3

[0148] Feedstock 1 (uncalcined shale containing 3.5 wt% kaolinite, 10.8 wt% chlorite, 20.4 wt% illite, 19.8 wt% quartz, and 33.9 wt% amorphous fraction) was subjected to a full-scale test using 5 kg of feedstock and 300 kg of grinding media (stainless steel balls). Ball milling was conducted for 48 hours at a flue gas pressure of 65 PSIG (approximately 4 vol% CO 2 ) to obtain sample 10.

[0149] The results of the mechanochemical activation are shown in the table below. Table 8: Results of mechanochemical activation of the starting material Source material 1 Sample 10 Kaolinite wt.% 3,5 0,5 Illite wt% 20,4 1,5 Chlorite wt.% 10,8 0,3 Quartz wt% 19,8 17,0 Amorphous fraction wt% 33,9 73,0 SAI 7 days (%) 101 132 SAI 28 days (%) 95 118 Hydration heat 12 h (J / g) 8,75 277,97 Heat of hydration 72 h (J / g) 22,36 323,26 CITATIONS CONTAINED IN THE DESCRIPTION

[0000] This list of documents cited by the applicant has been generated automatically and is included solely for the better information of the reader. The list is not part of the German patent or utility model application. The DPMA assumes no liability for any errors or omissions. Cited Non-Patent Literature

[0000] John, Vanderley M., et al. „Fillers in cementitious materials-Experience, recent advances and future potential.“ Cement and Concrete Research 114 (2018): 65-78

[0004] Souri, Alireza, et al. „Pozzolanic activity of mechanochemically and thermally activated kaolins in cement.“ Cement and Concrete Research 77 (2015): 47-59

[0008] Vizcayno C et al: „Pozzolan obtained by mechanochemical and thermal treatments of kaolin“ Applied clay science, Elsevier, Amsterdam, nl, vol. 49 no. 4, 1 August 2010 pages 405-413

[0008] Dana's New Mineralogy, Eighth Edition, von Richard V. Gaines, H. Catherine Skinner, Eugene E. Foord, Brian Mason und Abraham Rosenzweig, mit Abschnitten von Vandall T. King, Illustrationen von Eric Dowty, (ISBN: 047119310-0) Copyright © 1997, John Wiley &

[0027] ASTM C618-12a (2012

[0118] EN197-1 (2011

[0128]

Claims

[1] Mechanochemically activated material obtainable by a process for the mechanochemical activation of kaolinite-poor starting materials, the process comprising the following steps: a) providing a solid starting material comprising a phyllosilicate mineral, the starting material having a kaolinite content of less than 50 wt% as determined by XRD, preferably less than 20 wt%, more preferably less than 10 wt%; b) providing a gas; c) introducing the feedstock and the gas into a mechanical agitation unit; and d) subjecting the starting material to mechanical agitation in the presence of the gas in the mechanical agitation unit; wherein the phyllosilicate mineral is selected from the kaolinite group, serpentinite group, mica group, chlorite group and combinations thereof, wherein the mechanochemically activated material has a Strength Activity Index (SAI) at Day 28 of at least 110%, the SAI being determined in accordance with ASTM C311 / C311 M-22. [2] The mechanochemically activated material of claim 1, wherein the phyllosilicate mineral is selected from the serpentinite group, mica group, chlorite group, and combinations thereof. [3] The mechanochemically activated material according to claim 2, wherein the phyllosilicate mineral is selected from the serpentinite group. [4] The mechanochemically activated material according to claim 2, wherein the phyllosilicate mineral is selected from the mica group. [5] The mechanochemically activated material according to claim 2, wherein the phyllosilicate mineral is selected from the chlorite group. [6] The mechanochemically activated material of claim 2, wherein the phyllosilicate mineral is selected from illite, chlorite, muscovite, and combinations thereof. [7] The mechanochemically activated material of claim 6, wherein the phyllosilicate mineral is illite. [8] The mechanochemically activated material of claim 6, wherein the phyllosilicate mineral is chlorite. [9] The mechanochemically activated material of claim 6, wherein the phyllosilicate mineral is muscovite. [10] Mechanochemically activated material according to any one of claims 1-9, wherein the phyllosilicate mineral is present in an amount of at least 5 wt.% based on the total weight of the starting material. [11] Mechanochemically activated material according to any one of claims 1-9, wherein the phyllosilicate mineral is present in an amount of at least 10 wt% based on the total weight of the starting material. [12] A mechanochemically activated material according to any one of claims 1-9, wherein the phyllosilicate mineral is present in an amount of at least 15 wt% based on the total weight of the starting material. [13] A mechanochemically activated material according to any one of claims 1-12, wherein the phyllosilicate mineral is not kaolinite and the starting material from step (a) comprises less than 10 wt% kaolinite. [14] A mechanochemically activated material according to any one of claims 1-12, wherein the phyllosilicate mineral is not kaolinite and the starting material from step (a) comprises less than 5 wt% kaolinite. [15] A mechanochemically activated material according to any one of claims 1-12, wherein the phyllosilicate mineral is not kaolinite and the starting material from step (a) comprises less than 3 wt% kaolinite. [16] Mechanochemically activated material according to any one of claims 1-15, wherein the starting material comprises at least 10 wt% quartz based on the total weight of the starting material. [17] Mechanochemically activated material according to any one of claims 1-15, wherein the starting material comprises at least 15 wt% quartz based on the total weight of the starting material. [18] Mechanochemically activated material according to any one of claims 1-15, wherein the starting material comprises at least 20 wt% quartz based on the total weight of the starting material. [19] A mechanochemically activated material according to any one of claims 1-18, wherein the starting material has an amorphous content of at least 10 wt.% as determined by XRD. [20] A mechanochemically activated material according to any one of claims 1-18, wherein the starting material has an amorphous content of at least 15 wt.% as determined by XRD. [21] A mechanochemically activated material according to any one of claims 1-18, wherein the starting material has an amorphous content of at least 20 wt.% as determined by XRD. [22] Mechanochemically activated material according to any one of claims 1-21, wherein the total amount of Si and O in the starting material is at least 60 wt%. [23] Mechanochemically activated material according to any one of claims 1-21, wherein the total amount of Si and O in the starting material is at least 65 wt%. [24] A mechanochemically activated material according to any one of claims 1-23, which has a D50 in the range of 0.1 to 30 µm. [25] A mechanochemically activated material according to any one of claims 1-23, which has a D50 in the range of 0.5 to 15 µm. [26] A mechanochemically activated material according to any one of claims 1-23, which has a D50 in the range of 1 to 10 µm. [27] A mechanochemically activated material according to any one of claims 1-26, which has a dehydration start temperature of less than 250°C. [28] A mechanochemically activated material according to any one of claims 1-26, which has a dehydration start temperature of less than 200°C. [29] A mechanochemically activated material according to any one of claims 1-26, which has a dehydration start temperature of less than 150°C. [30] A mechanochemically activated material according to any one of claims 1-26, which has a dehydration start temperature of less than 130°C. [31] Mechanochemically activated material according to any one of claims 1-30, which has an amorphous content of at least 25 wt.%. [32] Mechanochemically activated material according to any one of claims 1-30, which has an amorphous content of at least 30 wt.%. [33] Mechanochemically activated material according to any one of claims 1-30, which has an amorphous content of at least 35 wt.%. [34] Mechanochemically activated material according to any one of claims 1-33, which has one, two, three or four, preferably all four of the following properties: • a D50 in the range of 0.1 to 30 µm, preferably 0.5 to 15 µm, most preferably 1 to 10 µm; • a dehydration start temperature of less than 250°C, preferably less than 200°C, more preferably less than 150°C, even more preferably less than 130°C; • an amorphous portion of at least 25% by weight, preferably at least 30% by weight and more preferably at least 35% by weight; • a phyllosilicate mineral content of less than 10 wt%, based on the total weight of the mechanochemically activated material, preferably less than 5 wt%. [35] A mechanochemically activated material according to any one of claims 1-34, which has a D90 in the range of 0.5 to 100 µm. [36] A mechanochemically activated material according to any one of claims 1-34, which has a D90 in the range of 1 to 80 µm. [37] A mechanochemically activated material according to any one of claims 1-34, which has a D90 in the range of 5 to 70 µm. [38] A mechanochemically activated material according to any one of claims 1-37, having a Strength Activity Index (SAI) at day 7 of at least 80%, wherein the SAI is determined according to ASTM C311 / C311 M-22. [39] A mechanochemically activated material according to any one of claims 1-37, having a Strength Activity Index (SAI) at day 7 of at least 85%, wherein the SAI is determined according to ASTM C311 / C311 M-22. [40] A mechanochemically activated material according to any one of claims 1-37, having a Strength Activity Index (SAI) at day 7 of at least 105%, wherein the SAI is determined according to ASTM C311 / C311 M-22. [41] A mechanochemically activated material according to any one of claims 1-37, having a Strength Activity Index (SAI) at day 7 of at least 110%, wherein the SAI is determined according to ASTM C311 / C311 M-22. [42] A mechanochemically activated material according to any one of claims 1-37, having a Strength Activity Index (SAI) at day 7 of at least 125%, wherein the SAI is determined according to ASTM C311 / C311 M-22. [43] A mechanochemically activated material according to any one of claims 1-42, having a Strength Activity Index (SAI) at day 28 of at least 115%, wherein the SAI is determined according to ASTM C311 / C311 M-22. [44] A mechanochemically activated material according to any one of claims 1-42, having a Strength Activity Index (SAI) at day 28 of at least 125%, wherein the SAI is determined according to ASTM C311 / C311 M-22. [45] A mechanochemically activated material according to any one of claims 1-44, which has a heat of hydration after 12 hours, determined according to modified ASTM C 1897-20 as defined in the description, of at least 100 J / g. [46] A mechanochemically activated material according to any one of claims 1-44, which has a heat of hydration after 12 hours, determined according to modified ASTM C 1897-20 as defined in the description, of at least 150 J / g. [47] A mechanochemically activated material according to any one of claims 1-44, which has a heat of hydration after 12 hours, determined according to modified ASTM C 1897-20 as defined in the description, of at least 200 J / g. [48] ​​A mechanochemically activated material according to any one of claims 1-47, which has a heat of hydration after 72 hours, determined according to modified ASTM C 1897-20 as defined in the description, of at least 150 J / g. [49] A mechanochemically activated material according to any one of claims 1-47, which has a heat of hydration after 72 hours, determined according to modified ASTM C 1897-20 as defined in the description, of at least 200 J / g. [50] A mechanochemically activated material according to any one of claims 1-47, which has a heat of hydration after 72 hours, determined according to modified ASTM C 1897-20 as defined in the description, of at least 250 J / g. [51] A mechanochemically activated material according to any one of claims 1-50, which has a water demand, determined according to ASTM C311 / C311M-22, of less than 97%. [52] A mechanochemically activated material according to any one of claims 1-50, which has a water demand, determined according to ASTM C311 / C311M-22, of less than 96%. [53] A mechanochemically activated material according to any one of claims 1-50, which has a water demand, determined according to ASTM C311 / C311M-22, of less than 95%. [54] A mechanochemically activated material according to any one of claims 1-50, which has a water demand, determined according to ASTM C311 / C311M-22, of less than 93%. [55] A mechanochemically activated material according to any one of claims 1-50, which has a water demand, determined according to ASTM C311 / C311M-22, of less than 91%. [56] A mechanochemically activated material according to any one of claims 1-55, wherein step (d) is carried out such that the dehydration start temperature of the mechanochemically activated material obtained in step (d) is at least 50 °C lower than the dehydration start temperature of the starting material provided in step (a). [57] A mechanochemically activated material according to any one of claims 1-55, wherein step (d) is carried out such that the dehydration start temperature of the mechanochemically activated material obtained in step (d) is at least 100 °C lower than the dehydration start temperature of the starting material provided in step (a). [58] A mechanochemically activated material according to any one of claims 1-55, wherein step (d) is carried out such that the dehydration start temperature of the mechanochemically activated material obtained in step (d) is at least 175 °C lower than the dehydration start temperature of the starting material provided in step (a). [59] A mechanochemically activated material according to any one of claims 1-58, wherein the gas provided in step (b) is air. [60] A mechanochemically activated material according to any one of claims 1-58, wherein the gas provided in step (b) is a gas containing at least 0.1 vol% CO 2 includes. [61] Mechanochemically activated material according to any one of claims 1-60, wherein step (d) is carried out at a temperature of at most 300°C. [62] A mechanochemically activated material according to any one of claims 1-60, wherein step (d) is carried out at a temperature of less than 150°C. [63] A mechanochemically activated material according to any one of claims 1-60, wherein step (d) is carried out at a temperature of less than 100°C. [64] A mechanochemically activated material according to any one of claims 1-63, wherein the mechanical agitation of step (d) comprises grinding or comminuting. [65] Mechanochemically activated material according to claim 64, wherein the grinding is carried out in the presence of grinding or comminuting bodies. [66] Mechanochemically activated material according to claim 65, wherein the grinding or comminuting bodies are selected from balls, bearings or beads. [67] Mechanochemically activated material according to claim 65 or 66, wherein the grinding or comminuting bodies are made of a material having an HRC hardness of 60 or higher. [68] Mechanochemically activated material according to any one of claims 65-67, wherein the grinding or comminuting bodies are made of steel, alumina, chromium with cast iron, molybdenum steel, chromium-based steels, stainless steel, ceramic or alumina. [69] Mechanochemically activated material according to any one of claims 65-68, wherein the grinding or comminuting bodies have a density of at least 6.5 g / cm 3 have. [70] Mechanochemically activated material according to any one of claims 65-68, wherein the grinding or comminuting bodies have a density of at least 7.0 g / cm3 have. [71] Mechanochemically activated material according to any one of claims 65-68, wherein the grinding or comminuting bodies have a density of at least 7.5 g / cm 3 have. [72] Mechanochemically activated material according to any one of claims 65-68, wherein the grinding or comminuting bodies have a density of at least 8.0 g / cm 3 have. [73] Mechanochemically activated material according to any one of claims 65-72, wherein the mass ratio of grinding or comminuting bodies to starting material is more than 5:

1. [74] Mechanochemically activated material according to any one of claims 65-72, wherein the mass ratio of grinding or comminuting bodies to starting material is more than 10:

1. [75] Mechanochemically activated material according to any one of claims 65-72, wherein the mass ratio of grinding or comminuting bodies to starting material is more than 25:

1. [76] A composition comprising the mechanochemically activated material of any one of claims 1-75 and another material selected from the group consisting of asphalt, geopolymers, cement, polymers and combinations thereof. [77] A composition comprising the mechanochemically activated material according to any one of claims 1-75 and a further material selected from cement. [78] A composition comprising the mechanochemically activated material according to any one of claims 1-75 and a further material selected from Portland cement.

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