Supplementary cementitious materials comprising inosilicates

Abstract

The present disclosure relates to supplementary cementitious materials (SCMs) comprising inosilicates. The present disclosure also relates to methods of forming the supplementary cementitious materials (SCMs) comprising inosilicates.

Description

[0001] Title: Supplementary Cementitious Materials Comprising Inosilicates

[0002] FIELD OF THE INVENTION

[0003] The present disclosure relates to supplementary cementitious materials (SCMs) comprising inosilicates. The present disclosure also relates to methods of forming the supplementary cementitious materials (SCMs) comprising inosilicates.

[0004] BACKGROUND OF THE INVENTION

[0005] Cement based materials make up more than half of all the materials used by humankind worldwide and account for approximately eight percent of global carbon dioxide emissions. There is a need to reduce global carbon dioxide emissions associated with cement based materials.

[0006] An example of a cement based material is concrete. Concrete traditionally comprises cement, aggregates and water. Concrete is a fundamental building material and is a widely used man-made material. The cement in the concrete is the mineral glue that binds the different components in the concrete together. Some types of cement, such as Ordinary Portland cement (also known as CEM I), contain a material called “clinker”. Clinker is usually present at a high amount in the cement. For example, Ordinary Portland cement contains more than 90 percent by weight of clinker. The clinker production process requires grinding and calcining up to a temperature of 1450 °C a mixture of limestone, clays and other minor components. The mixture is then mixed with 3 to 5 percent by weight of gypsum to form cement. The predominant source of carbon dioxide emissions in the production of cement (and cement based materials generally) is the production of the clinker. For example, clinker production typically generates approximately 850 Kg of carbon dioxide per ton of clinker produced. The high carbon dioxide emissions can be attributed to the combustion of fuel and the decomposition of limestone into calcium oxide and carbon dioxide during the production of the clinker.

[0007] In recent years, supplementary cementitious materials (SCMs) have been used in addition to or as a partial replacement of the clinker to reduce the carbon dioxideemissions associated with cement based materials. SCMs include materials such as ground granulated blast furnace slag, fly ash, glass powder, natural pozzolana, calcined clays, silica fume, pumice, opaline rock, metakaolin and burnt shale. The use of SCMs is advantageous from an environmental and energy conservation viewpoint. By partly replacing clinker with SCMs, the environmental impact of cement based materials is improved. This is because the carbon dioxide emissions associated with clinker production, and thus cement based material production, is reduced. SCMs can also be formed as byproducts in industrial processes, and the reuse of SCMs further improves the energy efficiency of the cement based materials.

[0008] The use of SCMs in cement based materials is further advantageous because SCMs improve the durability, reduce the permeability and enhance the strength of cement based materials. For example, SCMs contribute to the properties of cement based materials through hydraulic or pozzolanic activity. The pozzolanic reaction is a chemical reaction that can take place between calcium and a silicate, such as calcium hydroxide and silica oxide, in the presence of water to form calcium silicate hydrate. Calcium silicate hydrate has favourable cementitious properties and can be the main binding phase in cement based materials. As a further example, SCMs also affect the chemical and physical properties of cement based materials. SCMs improve the physical properties of cement based materials by reducing the water absorption and apparent porosity, thus increasing the durability of the cement based materials.

[0009] Furthermore, there is an increasing demand for SCMs and decreasing availability of some SCMs. There is therefore a need for finding new types and sources of SCMs.

[0010] Furthermore, the presence of SCMs with an elongated particle shape can advantageously contribute to the flexural strength of the final hardened cement based material.

[0011] There is a continued need to provide an improved SCM. In particular, there is a need to provide an improved SCM that promotes pore discontinuity in cement based materials (thereby reducing the amount of water absorbed by cement based materials).SUMMARY OF THE INVENTION

[0012] The present disclosure relates to supplementary cementitious materials (SCMs) comprising inosilicates. The present disclosure also relates to methods of forming the supplementary cementitious materials (SCMs) comprising inosilicates.

[0013] Representative features of the present invention are set out in the following clauses, which stand alone or may be combined, in any combination, with one or more features disclosed in the text of the specification.

[0014] The present invention is as set out in the following clauses:

[0015] 1. A supplementary cementitious material (SCM) comprising an inosilicate.

[0016] 2. The supplementary cementitious material (SCM) of clause 1 , wherein the inosilicate is present at: from 0.5 to 20 weight percent; or, from 0.75 to 15 weight percent; or, from 1 to 10 weight percent of the total weight of the supplementary cementitious material (SCM).

[0017] 3. The supplementary cementitious material (SCM) of clause 1 or clause 2, wherein the inosilicate is: a pyroxene; and / or, an amphibole; and / or, a chlorite; and / or, a combination thereof.

[0018] 4. The supplementary cementitious material (SCM) of clause 3, wherein the pyroxene is: clinopyroxene; and / or, orthopyroxene; and / or, a combination thereof.

[0019] 5. The supplementary cementitious material (SCM) of clause 4, wherein the clinopyroxene is: Diopside; and / or, Hedenbergite; and / or, Augite; and / or, Jadeite; and / or, Aegirine; and / or, Omphacite; and / or, a combination thereof.

[0020] 6. The supplementary cementitious material (SCM) of clause 4 or clause 5, wherein the orthopyroxene is: Enstatite; and / or, Ferrosilite; and / or, Bronzite; and / or, Hypersthene; and / or, a combination thereof.7. The supplementary cementitious material (SCM) of clause 3, wherein the amphibole is: a calcium amphibole; and / or, a sodium amphibole; and / or, a sodiumcalcium amphibole; and / or, a lithium-(magnesium-iron-manganese) amphibole; and / or, a lithium amphibole; and / or, a sodium-(magnesium-iron-manganese) amphibole, a magnesium-iron-manganese amphibole, and / or, a lithium-calcium amphibole; and / or, an alkali amphibole; and / or, a combination thereof.

[0021] 8. The supplementary cementitious material (SCM) of clause 7, wherein the calcium amphibole is: Tremolite; and / or, Magnesio-hornblende; and / or, Edenite; and / or, Pargasite; and / or, Ferro-actinolite; and / or, Hastingsite; and / or, a combination thereof.

[0022] 9. The supplementary cementitious material (SCM) of clause 7 or clause 8, wherein the sodium amphibole is: Glaucophane; and / or, Eckermannite; and / or, Leakeite; and / or, Riebeckite; and / or, Arfvedsonite; and / or, a combination thereof.

[0023] 10. The supplementary cementitious material (SCM) of any one of clauses 7 to 9, wherein the sodium-calcium amphibole is: Winchite; and / or, Richterite; and / or, Ferro-winchite; and / or, a combination thereof.

[0024] 11. The supplementary cementitious material (SCM) of any one of clauses 7 to 10, wherein the magnesium-iron-manganese amphibole is: Cummingtonite; and / or, Grunerite; and / or, Anthophyllite; and / or, Gedrite; and / or, a combination thereof.

[0025] 12. The supplementary cementitious material (SCM) of any one of clauses 7 to 11, wherein the lithium amphibole is: Holmquistite; and / or, Ferri-pedrizite; and / or, a combination thereof.

[0026] 13. The supplementary cementitious material (SCM) of any one of clauses 7 to 12, wherein the alkali amphibole is: K-richterite; and / or, Eckerite; and / or, a combination thereof.14. The supplementary cementitious material (SCM) of clause 3, wherein the chlorite is: Clinochlore; and / or, Chamosite; optionally, wherein the Clinochlore is Kammererite.

[0027] 15. The supplementary cementitious material (SCM) of any one of clauses 1 to 14, wherein the inosilicate comprises, or consists of, Enstatite.

[0028] 16. The supplementary cementitious material (SCM) of any one of clauses 1 to 14, wherein the inosilicate comprises, or consists of, Anthophyllite.

[0029] 17. The supplementary cementitious material (SCM) of any one of clauses 1 to 16, wherein the supplementary cementitious material (SCM) is: ground granulated blast furnace slag; and / or, fly ash; and / or, burnt shale; and / or, glass powder; and / or, silica fume; and / or, natural pozzolana; and / or, calcined clays; and / or, pumice; and / or, opaline rock; and / or, metakaolin; and / or, olivine; and / or, carbonated olivine; and / or, a combination thereof.

[0030] 18. The supplementary cementitious material (SCM) of any one of clauses 1 to 17, wherein the supplementary cementitious material (SCM) comprises, or consists of, carbonated olivine.

[0031] 19. The supplementary cementitious material (SCM) of any one of clauses 1 to 18, wherein the supplementary cementitious material (SCM) comprises, or consists of, carbonated olivine and the inosilicate comprises, or consists of, Enstatite.

[0032] 20. The supplementary cementitious material (SCM) of any one of clauses 1 to 18, wherein the supplementary cementitious material (SCM) comprises, or consists of, carbonated olivine and the inosilicate comprises, or consists of, Anthophyllite.

[0033] 21. The supplementary cementitious material (SCM) of any one of clauses 1 to 17, wherein the supplementary cementitious material (SCM), comprises, or consists of, olivine and carbonated olivine.22. The supplementary cementitious material (SCM) of clause 21 , wherein the olivine is present at: from 0.01 to 60 weight percent; or, from 0.05 to 55 weight percent; or, from 0.1 to 50 weight percent of the total weight of the supplementary cementitious material (SCM).

[0034] 23. The supplementary cementitious material (SCM) of clause 21 or clause 22, wherein the carbonated olivine is present at: from 1 to 99 weight percent; or, from 35 to 97 weight percent; or, from 40 to 95 weight percent of the total weight of the supplementary cementitious material (SCM).

[0035] 24. The supplementary cementitious material (SCM) of any one of clauses 1 to 17 and 21 to 23, wherein the supplementary cementitious material (SCM), comprises, or consists of, olivine and carbonated olivine and the inosilicate comprises, or consists of, Enstatite.

[0036] 25. The supplementary cementitious material (SCM) of any one of clauses 1 to 17 and 21 to 23, wherein the supplementary cementitious material (SCM), comprises, or consists of, olivine and carbonated olivine and the inosilicate comprises, or consists of, Anthophyllite.

[0037] 26. A method of preparing the supplementary cementitious material (SCM) of any one of clauses 1 to 25, the method comprising the steps of:

[0038] (a) providing a supplementary cementitious material (SCM),

[0039] (b) providing an inosilicate, and

[0040] (c) combining the supplementary cementitious material and the inosilicate.

[0041] 27. The method of clause 26, wherein the supplementary cementitious material (SCM) comprises, or consists of, carbonated olivine.

[0042] 28. The method of clause 26, wherein the supplementary cementitious material (SCM) comprises, or consists of, olivine and carbonated olivine.29. The method of clause 28, wherein the olivine is present at: from 0.01 to 60 weight percent; or, from 0.05 to 55 weight percent; or, from 0.1 to 50 weight percent of the total weight of the supplementary cementitious material (SCM).

[0043] 30. The method of clause 28 or clause 29, wherein the carbonated olivine is present at: from 1 to 99 weight percent; or, from 35 to 97 weight percent; or, from 40 to 95 weight percent of the total weight of the supplementary cementitious material (SCM).

[0044] 31. The method of any one of clauses 26 to 30, wherein the carbonated olivine is prepared by reacting olivine with carbon dioxide in the presence of water; optionally,

[0045] (a) wherein the olivine is reacted with the carbon dioxide in the presence of water at a pressure of from 10 to 300 bar; or, from 25 to 250 bar; or, from 50 to 200 bar; and / or,

[0046] (b) wherein the olivine is reacted with the carbon dioxide in the presence of water at a temperature of from 100 to 350 °C; or, from 125 to 325 °C; or, from 150 to 300 °C; and / or,

[0047] (c) wherein the olivine is reacted with the carbon dioxide in the presence of water at a pressure of from 50 to 200 bar and a temperature of 150 to 300 °C.

[0048] 32. A composite cement comprising the supplementary cementitious material (SCM) of any one of clauses 1 to 25.

[0049] 33. The composite cement of clause 32, wherein the composite cement comprises:

[0050] the supplementary cementitious material (SCM) at: from 1 to 95 weight percent; or, from 3 to 75 weight percent; or, from 10 to 60 weight percent of the total weight of the composite cement.

[0051] 34. A cement based material comprising the composite cement of clause 32 or clause 33, wherein the cement based material further comprises:

[0052] an aggregate, and

[0053] water.35. The cement based material of clauses 34, wherein the cement based material comprises:

[0054] the composite cement and water at a ratio of: from 0.1 :0.1 to 1 : 1 ; or, from 0.25:0.50 to 0.50:0.85; or, 0.35:0.65 of water to composite cement by weight; and the composite cement and aggregate at a ratio of: from 2:1 to 10:1 ; or, 3:1 to 6:1 of aggregate to composite cement by weight;

[0055] wherein any remainder is unavoidable impurities.

[0056] 36. Use of the supplementary cementitious material (SCM) of any one of clauses 1 to 25 for promoting pore discontinuity in cement based materials.

[0057] The present invention is also as set out in the following clauses:

[0058] 1A. A supplementary cementitious material (SCM) comprising carbonated olivine and an inosilicate.

[0059] 2A. The supplementary cementitious material (SCM) of clause 1 A, wherein the inosilicate is present at: from 0.5 to 50 weight percent; or, from 0.5 to 20 weight percent; or, from 0.75 to 15 weight percent; or, from 1 to 10 weight percent; or, from 10 to 45 weight percent; or, from 15 to 42 weight percent; or, from 20 to 40 weight percent of the total weight of the supplementary cementitious material (SCM).

[0060] 3A. The supplementary cementitious material (SCM) of clause 1 A or clause 2A, wherein the inosilicate is: a pyroxene; and / or, an amphibole; and / or, a combination thereof; and / or optionally further comprising a phyllosilicate selected from chlorite minerals; and / or optionally,

[0061] wherein:

[0062] (i) the pyroxene is: clinopyroxene; and / or, orthopyroxene; and / or, a combination thereof; optionally,wherein the clinopyroxene is: Diopside; and / or, Hedenbergite; and / or, Augite; and / or, Jadeite; and / or, Aegirine; and / or, Omphacite; and / or, a combination thereof; and / or,

[0063] wherein the orthopyroxene is: Enstatite; and / or, Ferrosilite; and / or, Bronzite; and / or, Hypersthene; and / or, a combination thereof; or,

[0064] (ii) the amphibole is: a calcium amphibole; and / or, a sodium amphibole; and / or, a sodium-calcium amphibole; and / or, a lithium-(magnesium-iron-manganese) amphibole; and / or, a lithium amphibole; and / or, a sodium-(magnesium-iron-manganese) amphibole, a magnesium-iron-manganese amphibole, and / or, a lithiumcalcium amphibole; and / or, an alkali amphibole; and / or, a combination thereof; optionally,

[0065] wherein the calcium amphibole is: Tremolite; and / or, Magnesio-hornblende; and / or, Edenite; and / or, Pargasite; and / or, Ferro-actinolite; and / or, Hastingsite; and / or, a combination thereof; and / or,

[0066] wherein the sodium amphibole is: Glaucophane; and / or, Eckermannite; and / or, Leakeite; and / or, Riebeckite; and / or, Arfvedsonite; and / or, a combination thereof; and / or,

[0067] wherein the sodium-calcium amphibole is: Winchite; and / or, Richterite; and / or, Ferro-winchite; and / or, a combination thereof; and / or,

[0068] wherein the magnesium-iron-manganese amphibole is: Cummingtonite; and / or, Grunerite; and / or, Anthophyllite; and / or, Gedrite; and / or, a combination thereof; and / or,

[0069] wherein the lithium amphibole is: Holmquistite; and / or, Ferri-pedrizite; and / or, a combination thereof; and / or,

[0070] wherein the alkali amphibole is: K-richterite; and / or, Eckerite; and / or, a combination thereof; or,(iii) the chlorite is: Clinochlore; and / or, Chamosite; optionally, wherein the Clinochlore is Kammererite.

[0071] 4A. The supplementary cementitious material (SCM) of any one of clauses 1 A to 3A, wherein the inosilicate comprises, or consists of, Enstatite; or,

[0072] wherein the inosilicate comprises, or consists of, Anthophyllite.

[0073] 5A. The supplementary cementitious material (SCM) of any one of clauses 1 A to 4A, wherein the supplementary cementitious material (SCM) is, or, further comprises: ground granulated blast furnace slag; and / or, fly ash; and / or, burnt shale; and / or, glass powder; and / or, silica fume; and / or, natural pozzolana; and / or, calcined clays; and / or, pumice; and / or, opaline rock; and / or, metakaolin; and / or, olivine; and / or, a combination thereof.

[0074] 6A. The supplementary cementitious material (SCM) of any one of clauses 1 A to 5A, wherein the supplementary cementitious material (SCM) comprises, or consists of:

[0075] (a) carbonated olivine and olivine, optionally, wherein the carbonated olivine and olivine are a mixture; and,

[0076] (b) an inosilicate.

[0077] 7A. The supplementary cementitious material (SCM) of clause 6A, wherein the supplementary cementitious material (SCM) comprises, or consists of:

[0078] (a) carbonated olivine and olivine; optionally, wherein the carbonated olivine and olivine are a mixture; and

[0079] (b) Enstatite and / or Anthophyllite.

[0080] 8A. The supplementary cementitious material (SCM) of clause 6A or clause 7A wherein the olivine is present at: from 0.01 to 60 weight percent; or, from 0.05 to 55 weight percent; or, from 0.1 to 50 weight percent of the total weight of the supplementary cementitious material (SCM); and / or,wherein the carbonated olivine is present at: from 1 to 99 weight percent; or, from 35 to 97 weight percent; or, from 40 to 95 weight percent of the total weight of the supplementary cementitious material (SCM).

[0081] 9A. A method of preparing the supplementary cementitious material (SCM) of any one of clauses 1 A to 8A, the method comprising the steps of:

[0082] (a) providing a supplementary cementitious material (SCM) comprising carbonated olivine, (b) providing an inosilicate, and

[0083] (c) combining the supplementary cementitious material comprising carbonated olivine and the inosilicate.

[0084] 10A. The method of clause 9A, wherein the supplementary cementitious material (SCM) comprises, or consists of, olivine and carbonated olivine; optionally,

[0085] wherein the supplementary cementitious material (SCM) comprises, or consists of, a mixture of olivine and carbonated olivine; and / or,

[0086] wherein the olivine is present at: from 0.01 to 60 weight percent; or, from 0.05 to 55 weight percent; or, from 0.1 to 50 weight percent of the total weight of the supplementary cementitious material (SCM); and / or,

[0087] wherein the carbonated olivine is present at: from 1 to 99 weight percent; or, from 35 to 97 weight percent; or, from 40 to 95 weight percent of the total weight of the supplementary cementitious material (SCM).

[0088] 11A. The method of clause 9A or 10A, wherein the inosilicate is present at: from 0.5 to 50 weight percent; or from 10 to 45 weight percent; or, from 15 to 42 weight percent; or, from 20 to 40 weight percent of the total weight of the supplementary cementitious material (SCM).

[0089] 12A. The method of any one of clauses 9A to 11 A, wherein the carbonated olivine is prepared by reacting olivine with carbon dioxide in the presence of water; optionally,(a) wherein the olivine is reacted with the carbon dioxide in the presence of water at a pressure of from 10 to 300 bar; or, from 25 to 250 bar; or, from 50 to 200 bar; and / or,

[0090] (b) wherein the olivine is reacted with the carbon dioxide in the presence of water at a temperature of from 100 to 350 °C; or, from 125 to 325 °C; or, from 150 to 300 °C; or, from 100 to 300 °C; or, from 100 to 250 °C; and / or,

[0091] (c) wherein the olivine is reacted with the carbon dioxide in the presence of water at a pressure of from 50 to 200 bar and a temperature of 150 to 300 °C.

[0092] 13A. The method of any one of clauses 9A to 12A, wherein the olivine carbonation has a carbonation degree of carbonated olivine of: from 10 to 100 weight percent; or, from 40 to 90 weight percent; or, from 60 to 95 weight percent; or from 75 to 90 weight percent of the total weight of the carbonated olivine based on the total amount of carbon dioxide released during thermal decomposition of the carbonated product as determined by thermogravimetric analysis (TGA).

[0093] 14A. A composite cement comprising the supplementary cementitious material (SCM) of any one of clauses 1 A to 8A.

[0094] 15A. The composite cement of clause 14A, wherein the composite cement comprises:

[0095] the supplementary cementitious material (SCM) at: from 1 to 95 weight percent; or, from 3 to 75 weight percent; or, from 10 to 60 weight percent of the total weight of the composite cement.

[0096] 16A. A cement based material comprising the composite cement of clause 14A or clause 15A, wherein the cement based material further comprises:

[0097] an aggregate, and

[0098] water.

[0099] 17A. The cement based material of clause 16A, wherein the cement based material comprises:the composite cement and water at a ratio of: from 0.1 :0.1 to 1 : 1 ; or, from 0.25:0.50 to 0.50:0.85; or, 0.35:0.65 of water to composite cement by weight; and the composite cement and aggregate at a ratio of: from 2:1 to 10:1 ; or, 3:1 to 6:1 of aggregate to composite cement by weight;

[0100] wherein any remainder is unavoidable impurities.

[0101] 18A. Use of the supplementary cementitious material (SCM) of any one of clauses 1 A to 8A for promoting pore discontinuity in cement based materials.

[0102] DETAILED DESCRIPTION

[0103] Embodiments of the invention are described below with reference to the accompanying drawings. The accompanying drawings illustrate various embodiments of systems, methods, and embodiments of various other aspects of the disclosure. Any person with ordinary skills in the art will appreciate that the illustrated element boundaries (e.g., boxes, groups of boxes, or other shapes) in the figures represent one example of the boundaries. It may be that in some examples one element may be designed as multiple elements or that multiple elements may be designed as one element. In some examples, an element shown as an internal component of one element may be implemented as an external component in another and vice versa. Furthermore, elements may not be drawn to scale. Nonlimiting and non-exhaustive descriptions are described with reference to the following drawings. The components in the figures are not necessarily to scale, emphasis instead being placed upon illustrating principles.

[0104] Figure 1 is an X-ray Diffraction (XRD) analysis of Enstatite.

[0105] Figures 2A and 2B are Enstatite images from a Scanning Electron Microscope (SEM) in different magnifications (x1 000 and x1 500 respectively).

[0106] Figure 3 is an elemental mapping of Enstatite obtained from a Scanning Electron Macroscopy (SEM) equipped with an Energy-Dispersive X-ray Spectroscopy (EDS) detector.Figure 4 shows flexural strength at 7 and 28 days for mortars containing 15 weight percent of carbonated olivine and 5 or 10 weight percent of Enstatite or quartz (with weight percent relative to the total weight of the mortar).

[0107] Figure 5 shows capillary absorption curves of mortars with 15 weight percent of carbonated olivine and 10 weight percent of Enstatite or quartz (with weight percent relative to the total weight of the mortar).

[0108] Figure 6 shows capillary absorption curves of mortars comprising 35 weight percent of carbonated olivine, wherein 0 or 10 weight percent of the carbonated olivine is Enstatite (with weight percent relative to the total weight of the mortar).

[0109] Figure 7 shows flexural strength at 7 and 28 days for mortars comprising 35 weight percent carbonated olivine, wherein 0 or 20 weight percent of the carbonated olivine is Enstatite (with weight percent relative to the total weight of the mortar).

[0110] Embodiments of the present disclosure will be described more fully hereinafter with reference to the accompanying drawings, and in which example embodiments are shown. Embodiments of the claims may, however, be embodied in many different forms and should not be construed as limited to the embodiments set forth herein.

[0111] The words "comprising," "having," "containing," and "including," and other forms thereof, are intended to be equivalent in meaning and be open ended in that an item or items following any one of these words is not meant to be an exhaustive listing of such item or items or meant to be limited to only the listed item or items. It must also be noted that as used herein and in the appended claims, the singular forms "a," "an," and "the" include plural references unless the context clearly dictates otherwise. Although any systems and methods similar or equivalent to those described herein can be used in the practice or testing of embodiments of the present disclosure, the preferred systems and methods are now described.

[0112] Some of the terms used to describe the present invention are set out below:“Alkali amphiboles” refers to a form of amphibole. Alkali amphiboles contain alkali metals such as lithium, sodium, potassium and / or combinations thereof. Examples of alkali amphiboles include, but are not limited to, K-richterite and Eckerite.

[0113] “Amphibole” refers to a chain silicate that can comprise linked double chains of SiC tetrahedra with the basic structural unit of [Si40n]6’. Amphiboles have the general chemical formula of: A0-1B2C5T8O22W2, wherein A is, but not limited to, large cations such as: Na+, K+, Ca2+, Pb2+, and / or, Li+; B is, but not limited to, octahedral coordination sites such as: Na+, Ca2+, Mn2+, Fe2+, Mg2+, and / or, Li+; C is, but not limited to, octahedral coordination sites such as: Mg2+, Fe2+, Mn2+, Al3+, Fe3+, Mn3+, Ti4+, and / or, Li+; T is, but not limited to, tetrahedral coordination sites such as: Si4+, Al3+, Ti4+, and / or, Be2+; and, W is, but not limited to, (OH) F; Cl and / or, O2’.

[0114] Amphiboles can additionally comprise Zn2+, Ni2+, Co2+, V3+, Sc3+and / or Zr4+as the “C” component. In some examples, amphiboles can be categorised according to IMA2012 reports. In some examples, amphiboles are categorised into two groups, depending on the “W’ component. The two groups are (1) W-dominant amphiboles (when W is (OH); F’ and / or Cl’), and (2) WO-dominant amphiboles (oxoamphiboles). The first group, W-dominant amphiboles, is divided into eight subgroups according to the dominant charge and the “B” component. The eight subgroups are: magnesium-iron-manganese amphiboles, calcium amphiboles, sodium-calcium amphiboles, sodium amphiboles, lithium amphiboles, sodium-(magnesium-iron-manganese) amphiboles, lithium-(magnesium-iron-manganese) amphiboles, and lithium-calcium amphiboles. The second group, WO-dominant amphiboles, includes oxo-amphiboles and is not divided into subgroups.

[0115] “Calcium amphiboles” refers to a subgroup of the W-dominant amphiboles. Calcium amphiboles have the general chemical formula: B(Ca2++ ZM2+) / ZB > 0.75, BCa2+ / ZB > BZM2+ / ZB), wherein BZM2+is the sum of the divalent B cations (as described in the definition of “amphiboles”) and is calculated with the following equation: BZM2+= BCa2++ BMn2++ BFe2++ BMg2+, and, wherein ZB is the sum of all B cations (as described in the definition of “amphiboles”) and is calculated with the following equation: ZB = BLi++ BNa++ BCa2++ BMn2++ BFe2++ BMg2+. Non-limiting examples of calcium amphiboles include, but are not limited to, Tremolite, Magnesio-hornblende, Edenite, Pargasite, Ferro-actinolite and Hastingsite.“Capillary pore discontinuity” refers to a condition within a cementitious matrix in which the originally interconnected capillary pore network becomes sufficiently segmented or interrupted such that fluid transport no longer follows the flow behaviour associated with a continuous capillary system. In this condition, the pathways that enable the movement of water or other deleterious substances through the material are substantially obstructed. As discussed in the literature (e.g. Nokken and Hooton, Discontinuous Capillary Porosity in Concrete PCA R&D Serial No. 2861b, which is hereby incorporated by reference in its entirety), the development of a discontinuous capillary pore system is considered beneficial for durability, because disruption of the capillary pore network limits the ingress of harmful agents.

[0116] “Carbonated olivine” refers to a mix of magnesium carbonate defined by the chemical formula MgCOsand amorphous silica defined by the chemical formula SiO2. For example, carbonated olivine is a material obtained from the carbonation of natural olivine, as defined in the following description. During the carbonation, part of the magnesium in the natural olivine reacts with carbon dioxide to form magnesium carbonate (MgCOs) and part of the silica from the crystal structure in the natural olivine is released to form amorphous silica (SiCh). Carbonated olivine may contain residual unreacted olivine.

[0117] “Carbonation” refers to a wet process of introducing carbon dioxide, within a high-pressure reactor, to transform magnesium and silica present in natural olivine into magnesium carbonate (MgCO3) and amorphous silica (SiO2), wherein the combination of the magnesium carbonate and amorphous silica is carbonated olivine. When the carbonation reaction does not reach full conversion, the resulting material contains unreacted olivine.

[0118] “Carbonation degree” refers to the proportion of a starting material (natural olivine) that is converted into carbonate-containing phases during reaction with carbon dioxide. The carbonation degree of olivine feedstock is determined by thermogravimetric analysis (TGA) based on the mass loss recorded between approximately 450 °C and 900 °C with release of carbon dioxide. Owing to themagnitude of the mass loss being directly proportional to the quantity of carbonate formed, the mass loss provides a quantitative measure of the extent of carbonation. For example, a carbonated olivine having a carbonation degree of 90 weight percent indicates that approximately 90 weight percent of the carbonated product is composed of magnesium carbonate (MgCO3) and amorphous silica (SiO2) and the remaining fraction consists of unreacted or partially reacted constituents such as magnesium orthosilicate (Mg2SiO4) and iron oxide (FeO and / or Fe2O3).

[0119] “Cement based materials” refers to a material that comprises cement and water. Cement based materials can further comprise aggregates (such as sand, gravel, crushed rocks, lightweight aggregates and / or a combination thereof), admixtures (such as water reducing agents, plasticizers, air entering agents, retarders, setting accelerators, rheology modifiers and / or a combination thereof), additives (such as pigments, fibers, fillers, reinforcing elements, self-healing agents and / or a combination thereof) and / or a combination thereof. Examples of cement based materials include, but are not limited to, concrete, mortars, plasters and known construction chemical products such as screed and / or tile adhesives.

[0120] “Clinopyroxene” refers to a form of pyroxene that crystallises in the monoclinic system and includes ions such as, but not limited to, Ca2+, Na+, Mg2+, Fe2+, Al3+and / or Ti4+. Non-limiting examples of clinopyroxene include, but are not limited to, Diopside, Hedenbergite, Augite, Jadeite, Aegirine and Omphacite.

[0121] “Chlorite” refers to a form of pyroxene. Chlorite is formed from sheet silicate (phyllosilicate) minerals characterised by their layered structure, with silica tetrahedral sheets bonded to octahedral sheets of Al3+, Fe2+and Mg2+ions. The general chemical formula for chlorite is: A5-6T4Z18, wherein A is, but not limited to, Al3+, Fe2+, Fe3+, Li+, Mg2+, Mn2+and / or Ni2+; T is, but not limited to, Al3+, Fe3+, Si4+, and / or a combination thereof; and, Z is, but not limited to, O2’ and / or (OH)’. Nonlimiting examples of chlorite include, but are not limited to, Clinochlore and Chamosite. A non-limiting example of Clinochlore is Kammererite.

[0122] “Composite cement” refers to a cement that comprises a supplementary cementitious material. The cement may be Ordinary Portland Cement (also knownas CEM I). The composite cement may be used in cement based materials such as, but not limited to, concrete, mortars and known construction chemical products such as screed and / or tile adhesives. The composite cement may be mixed with aggregates (such as sand, gravel, crushed rocks, lightweight aggregates and / or a combination thereof), water, admixtures (such as water reducing agents, plasticizers, air entering agents, retarders, setting accelerators, rheology modifiers and / or a combination thereof), additives (such as pigments, fibers, fillers, reinforcing elements, self-healing agents and / or a combination thereof) and / or a combination thereof to form a cement based material.

[0123] “Inosilicate” refers to a subclass of silicate minerals. Inosilicates have a chain-like structure formed by linking S iC tetrahedra. The tetrahedra share oxygen atoms in a way that creates either single chains, giving single-chain inosilicates (such as pyroxenes) or double chains, giving double-chain inosilicates (such as amphiboles).

[0124] “Lithium amphiboles” refers to a subgroup of W-dominant amphiboles and are defined by the general chemical formula: B(Na++ Li+) / ZB > 0.75, BLi+ / ZB > BNa+ / ZB, wherein ZB is the sum of the “B” cations (as described in the definition of “amphiboles”), for example, ZB = BLi++ BNa++ BCa2++ BMn2++ BFe2++ BMg2+. Lithium amphiboles can be orthorhombic (having the space group of Pnma) or monoclinic (having the space group C2 / m). Non-limiting examples of lithium amphiboles include, but are not limited to, Holmquistite and Ferri-pedrizite.

[0125] “Lithium-calcium amphiboles” refers to a subgroup of W-dominant amphiboles and are defined by the general chemical formulas: 0.75 > B(Ca2++ ZM2+) / ZB > 0.25, BCa2+ / ZB > BZM2+ / ZB and 0.75 > B(Na++ Li+) / ZB > 0.25, BLi+ / ZB > BNa+ / ZB, wherein BZM2+is the sum of the “B” divalent cations (as described in the definition of “amphiboles”), for example, BZM2+= BMn2++ BFe2++ BMg2+and ZB is the sum of the B cations (as described in the definition of “amphiboles”), for example, ZB = BLi++ BNa++ BCa2++ BMn2++ BFe2++ BMg2+. Lithium-calcium amphiboles are the lithium analogue of sodium-calcium amphiboles, wherein sodium is replaced by lithium.“Lithium-(magnesium-iron-manganese) amphiboles” refers to a subgroup of W-dominant amphiboles and are defined by the general chemical formulas: 0.75 > B(Ca2++ ZM2+) / ZB > 0.25, BZM2+ / ZB > BCa2+ / ZB and 0.75 > B(Na++ Li+) / ZB > 0.25, BLi+ / ZB > BNa+ / ZB, wherein BZM2+is the sum of the “B” divalent cations (as described in the definition of “amphiboles”), for example, BZM2+= BMn2++ BFe2++ BMg2+and ZB is the sum of the B cations (as described in the definition of “amphiboles”), for example, ZB = BLi++ BNa++ BCa2++ BMn2++ BFe2++ BMg2+. Lithium-(magnesium-iron-manganese) amphiboles are the lithium analogues of sodium-(magnesium-iron-manganese) amphiboles, wherein sodium is replaced by lithium. These amphiboles are only known as synthetic phases.

[0126] “Magnesium-iron-manganese amphiboles” refers to a subgroup of W-dominant amphiboles and are defined by the general chemical formula: B(Ca2++ ZM2+) / ZB > 0.75, BZM2+ / ZB > BCa2+ / ZB, wherein BZM2+is the sum of the “B” divalent cations (as described in the definition of “amphiboles”), for example, BZM2+= BMn2++ BFe2++ BMg2+and ZB is the sum of the B cations (as described in the definition of “amphiboles”), for example, ZB = BLi++ BNa++ BCa2++ BMn2++ BFe2++ BMg2+. Magnesium-iron-manganese amphiboles can be orthorhombic (having the space group Pnma or Pnmn) or monoclinic (having the space groups C2 / m or P21 / m). Nonlimiting examples of magnesium-iron-manganese amphiboles include, but are not limited to, Anthophyllite, Gedrite, Cummingtonite and Grunerite.

[0127] “Olivine” refers to a magnesium iron silicate and is defined by the chemical formula: (Mg,Fe)2SiO4. The ratio of magnesium to iron varies between the two endmembers of the solid solution states for olivine: forsterite (Mg endmember: Mg2SiO4) and fayalite (Fe endmember: Fe2SiO4). Other names for olivine include chrysolite, serpentine, dunite, forsterite, magnesium iron silicate, magnesium iron solid solution silicate, forsterite-fayalite solid solution, nesosilicate, orthosilicate, ultramafic, alkali earth silicate, and, magnesium silicate.

[0128] “Orthopyroxene” refers to a form of pyroxene that crystallises in the orthorhombic system and that includes Mg2+and Fe2+. Orthopyroxene can additionally include Ca2+and Al3+, but generally at lower amounts than Mg2+and Fe2+. Non-limitingexamples of orthopyroxene include, but are not limited to, Enstatite, Ferrosilite, Bronzite and Hypersthene.

[0129] “Oxo-amphiboles” refers to a subgroup of WO-dominant amphiboles. Non-limiting examples of oxo-amphiboles include, but are not limited to, Dellaventuraite, Obertiite, Ungarettiite and Kaersutite.

[0130] “Portland cement” refers to a finely ground hydraulic binder made exclusively from Portland cement clinker and a small, controlled amount of calcium sulfate (such as gypsum) added only to regulate the setting time. In its 100% pure form, it contains no fillers, supplementary cementitious materials, pigments, or chemical additives, consisting solely of the characteristic clinker minerals — tricalcium silicate (C3S), dicalcium silicate (C2S), tricalcium aluminate (C3A), and tetracalcium aluminoferrite (C4AF) — formed by heating a precise mixture of limestone and clay-derived materials to clinkering temperature.

[0131] “Pozzolanic activity” refers to how quicky a mineral, such as a silicate (such as silica and / or alumina), reacts with calcium (Ca2+) or calcium hydroxide (Ca(OH)2) in the presence of water to form compounds having cementitious properties. The compounds having cementitious properties include, but are not limited to, calcium silicate hydrates, calcium aluminate hydrates and calcium silicate aluminate hydrates. Pozzolanic activity can be measured by any method known in the art, such as the “activity index test” or the “ Frattini test”.

[0132] “Pyroxene” refers to a group of chain silicates that are characterised by a single chain of S iC tetrahedra, with the basic structural unit [Si20e]4'. Pyroxenes are defined by the general chemical formula: XY(Si20e), wherein X is large cations such as, but not limited to, Ca2+and Na+; and, Y is a cation smaller than X such as, but not limited to, Mg2+, Fe2+and Al3+. Pyroxenes are categorised into two-subgroups based on crystal system, the two subgroups being clinopyroxenes (monoclinic system) and orthopyroxenes (orthorhombic crystal system).“Sodium amphiboles” refers to a subgroup of W-dominant amphiboles and are defined by the chemical formula: B(Na++ Li+) / ZB > 0.75, BNa+ / ZB > BLi+ / ZB, wherein ZB is the sum of the B cations (as described in the definition of “amphiboles”), for example, ZB = BLi++ BNa++ BCa2++ BMn2++ BFe2++ BMg2+. Non-limiting examples of sodium amphiboles include, but are not limited to, Glaucophane, Eckermannite, Leakeite, Riebeckite and Arfvedsonite.

[0133] “Sodium-(magnesium-iron-manganese) amphiboles” refers to a subgroup of W-dominant amphiboles and are defined by the chemical formulas: 0.75 > B(Ca + ZM2+) / ZB > 0.25, BZM2+ / ZB > BCa2+ / ZB, and, 0.75 > B(Na++ Li+) / ZB > 0.25, BNa+ / ZB > BLi+ / ZB, wherein BZM2+is the sum of the “B” divalent cations (as described in the definition of “amphiboles”), for example, BZM2+= BMn2++ BFe2++ BMg2+and ZB is the sum of the B cations (as described in the definition of “amphiboles”), for example, ZB = BLi++ BNa++ BCa2++ BMn2++ BFe2++ BMg2+.

[0134] “Sodium-calcium amphiboles” refers to a subgroup of WO-dominant amphiboles and are defined by the chemical formulas: 0.75 > B(Ca2++ ZM2+) / ZB > 0.25, BCa2+ / ZB > BZM2+ / ZB, and, 0.75 > B(Na++ Li+) / ZB > 0.25, BNa+ / ZB > BLi+ / ZB, wherein BZM2+is the sum of the “B” divalent cations (as described in the definition of “amphiboles”), for example, BZM2+= BMn2++ BFe2++ BMg2+and ZB is the sum of the B cations (as described in the definition of “amphiboles”), for example, ZB = BLi++ BNa++ BCa2++ BMn2++ BFe2++ BMg2+. Non-limiting examples of sodium-calcium amphiboles include, but are not limited to, Winchite, Richterite, and Ferro-winchite.

[0135] “Supplementary cementitious materials” or “SCMs” refers to a material that partially replaces clinker in cement. SCMs can have pozzolanic properties. Materials with pozzolanic properties are characterised by a content of reactive silica and / or alumina which form strength providing calcium silicate hydrates, calcium hydrates and / or calcium silicate aluminate hydrates when water is added. SCMs includes both latent hydraulic and pozzolanic materials. However, unreactive or only slightly reactive materials, such as but not limited to limestone, are differentiated from SCMs. SCMs improve the durability and strength of the final product and reduce the permeability of the final product. Examples of SCMs include, but are not limited to, ground granulated blast furnace slag, fly ash, burnt shale, glass powder, silica fume, naturalpozzolana, calcined clays, pumice, opaline rock, metakaolin, olivine and / or carbonated olivine.

[0136] Supplementary cementitious materials (SCMs) comprising inosilicates

[0137] In one example of the present disclosure, a SCM comprises an inosilicate. The SCM can additionally comprise carbonated olivine.

[0138] The inosilicate may be present at: from 0.5 to 20 weight percent; or, from 0.75 to 15 weight percent; or, from 1 to 10 weight percent of the total weight of the SCM.

[0139] Preferably, the inosilicate is present at from 1 to 10 weight percent of the total weight of the SCM. The inosilicate may be present at: from 0.5 to 50 weight percent; or, from 10 to 45 weight percent; or, from 15 to 42 weight percent; or, from 20 to 40 weight percent of the total weight of the SCM. Preferably, the inosilicate is present at from 20 to 40 weight percent of the total weight of the SCM.

[0140] The inosilicate may be: a pyroxene; and / or, an amphibole; and / or, a combination thereof; and / or, optionally further comprising a phyllosilicate selected from chlorite minerals.

[0141] The pyroxene may be: clinopyroxene; and / or, orthopyroxene; and / or, a combination thereof.

[0142] The clinopyroxene may be: Diopside; and / or, Hedenbergite; and / or, Augite; and / or, Jadeite; and / or, Aegirine; and / or, Omphacite; and / or, a combination thereof.

[0143] The orthopyroxene may be: Enstatite; and / or, Ferrosilite; and / or, Bronzite; and / or, Hypersthene; and / or, a combination thereof.

[0144] Preferably, the inosilicate is pyroxene. More preferably, the inosilicate is orthopyroxene. Even more preferably, the inosilicate is Enstatite.

[0145] The amphibole may be: a calcium amphibole; and / or, a sodium amphibole; and / or, a sodium-calcium amphibole; and / or, a lithium-(magnesium-iron-manganese)amphibole; and / or, a lithium amphibole; and / or, a sodium-(magnesium-iron-manganese) amphibole; and / or, a magnesium-iron-manganese amphibole, and / or, a lithium-calcium amphibole; and / or, an alkali amphibole; and / or, a combination thereof.

[0146] The calcium amphibole may be: Tremolite; and / or, Magnesio-hornblende; and / or, Edenite; and / or, Pargasite; and / or, Ferro-actinolite; and / or, Hastingsite; and / or, a combination thereof.

[0147] The sodium amphibole may be: Glaucophane; and / or, Eckermannite; and / or, Leakeite; and / or, Riebeckite; and / or, Arfvedsonite; and / or, a combination thereof.

[0148] The sodium-calcium amphibole may be: Winchite; and / or, Richterite; and / or, Ferro-winchite; and / or, a combination thereof.

[0149] The magnesium-iron-manganese amphibole may be: Cummingtonite; and / or, Grunerite; and / or, Anthophyllite; and / or, Gedrite; and / or, a combination thereof.

[0150] The lithium amphibole may be: Holmquistite; and / or, Ferri-pedrizite; and / or, a combination thereof.

[0151] The alkali amphibole may be: K-richterite; and / or, Eckerite; and / or, a combination thereof.

[0152] The amphibole may be an oxo-amphibole. The oxo-amphibole may be:

[0153] Dellaventuraite; and / or, Obertiite; and / or, Ungarettiite; and / or, Kaersutite; and / or, a combination thereof.

[0154] Preferably, the inosilicate is an amphibole. More preferably, the inosilicate is a magnesium-iron-manganese amphibole. Even more preferably, the inosilicate is Anthophyllite.

[0155] The chlorite may be Clinochlore; and / or, Chamosite. The Clinochlore may be Kammererite.The SCM may be: ground granulated blast furnace slag; and / or, fly ash; and / or, burnt shale; and / or, glass powder; and / or, silica fume; and / or, natural pozzolana; and / or, calcined clays; and / or, pumice; and / or, opaline rock; and / or, metakaolin; and / or, olivine; and / or, carbonated olivine; and / or, a combination thereof.

[0156] The SCM may be a material with pozzolanic properties. The material with pozzolanic properties may be: ground granulated blast furnace slag; and / or, fly ash; and / or, burnt shale; and / or, glass powder; and / or, silica fume; and / or, natural pozzolana; and / or, calcined clays; and / or, pumice; and / or, opaline rock; and / or, metakaolin; and / or, carbonated olivine; and / or, a combination thereof.

[0157] Preferably, the SCM is carbonated olivine. Alternatively, the SCM additionally comprises carbonated olivine.

[0158] Preferably, the SCM is olivine and carbonated olivine. Preferably, the SCM is a mixture of olivine and carbonated olivine. When the SCM is olivine and carbonated olivine, the olivine may be present at: from 0.01 to 60 weight percent; or, from 0.05 to 55 weight percent; or, from 0.1 to 50 weight percent of the total weight of the SCM and the carbonated olivine may be present at: from 1 to 99 weight percent; or, from 35 to 97 weight percent; or, from 40 to 95 weight percent of the total weight of the SCM, wherein any remainder is inosilicates and / or unavoidable impurities.

[0159] Preferably, the olivine is present at from 0.1 to 50 weight percent of the total weight of the SCM and the carbonated olivine is present at from 40 to 95 weight percent of the total weight of the SCM, wherein any remainder is inosilicates and / or unavoidable impurities.

[0160] In one example of the present disclosure, the SCM is carbonated olivine and the inosilicate is Enstatite. Preferably, the inosilicate is present at from 1 to 10 weight percent of the total weight of the SCM. Alternatively, the inosilicate is present at from 20 to 40 weight percent of the total weight of the SCM.

[0161] In one example of the present disclosure, the SCM is carbonated olivine and the inosilicate is Anthophyllite. Preferably, the inosilicate is present at from 1 to 10weight percent of the total weight of the SCM. Alternatively, the inosilicate is present at from 20 to 40 weight percent of the total weight of the SCM.

[0162] In one example of the present disclosure, the SCM is olivine and carbonated olivine and the inosilicate is Enstatite. Preferably, the SCM is a mixture of olivine, carbonated olivine and the inosilicate is Enstatite. Preferably, the olivine is present at from 0.1 to 50 weight percent of the total weight of the SCM, the carbonated olivine is present at from 40 to 95 weight percent of the total weight of the SCM and the inosilicate is present at from 1 to 10 weight percent of the total weight of the SCM, wherein any remainder is unavoidable impurities. Preferably, the olivine is present at from 0.1 to 50 weight percent of the total weight of the SCM, the carbonated olivine is present at from 40 to 95 weight percent of the total weight of the SCM and the inosilicate is present at from 20 to 40 weight percent of the total weight of the SCM, wherein any remainder is unavoidable impurities.

[0163] In one example of the present disclosure, the SCM is olivine and carbonated olivine and the inosilicate is Anthophyllite. Preferably, the SCM is a mixture of olivine, carbonated olivine and the inosilicate is Anthophyllite. Preferably, the olivine is present at from 0.1 to 50 weight percent of the total weight of the SCM, the carbonated olivine is present at from 40 to 95 weight percent of the total weight of the SCM and the inosilicate is present at from 1 to 10 weight percent of the total weight of the SCM, wherein any remainder is unavoidable impurities. Preferably, the olivine is present at from 0.1 to 50 weight percent of the total weight of the SCM, the carbonated olivine is present at from 40 to 95 weight percent of the total weight of the SCM and the inosilicate is present at from 20 to 40 weight percent of the total weight of the SCM, wherein any remainder is unavoidable impurities.

[0164] In the examples set out above, the SCM may comprise another inosilicate.

[0165] The SCM comprising an inosilicate may be used to promote pore discontinuity in cement based materials, such as concrete. Advantageously, the inosilicate contains microfibers that promote the discontinuity of pores in cement based materials, such as concrete. Further advantageously, the inosilicates have pozzolanic activity. Both the presence of microfibers and the pozzolanic activity of the inosilicates improvesthe compactness of the cement based materials, such as concrete in which the SCM is included, which in turn reduces the amount of water absorbed by the cement based materials, such as concrete.

[0166] Method of making the supplementary cementitious material (SCM) carbonated olivine

[0167] In one example of the present disclosure, the SCM comprises, or consists of, carbonated olivine. The carbonated olivine is prepared by reacting olivine with carbon dioxide in the presence of water. The reaction can be represented with the following equation:

[0168] Mg2SiO4 + 2CO2 — 2MgCOs + SiO2

[0169] Preferably, the olivine is reacted with the carbon dioxide in the presence of water at a pressure of: from 10 to 300 bar; or, from 25 to 250 bar; or, from 50 to 200 bar.

[0170] Preferably, the olivine is reacted with the carbon dioxide in the presence of water at a temperature of: from 100 to 350 °C; or, from 125 to 325 °C; or, from 150 to 300 °C. Preferably, the olivine is reacted with the carbon dioxide in the presence of water at a temperature of: from 100 to 350 °C; or, from 100 to 300 °C; or, from 100 to 250 °C.

[0171] Preferably, the olivine is reacted with the carbon dioxide in the presence of water at a pressure of from 50 to 200 bar and a temperature of from 150 to 300 °C.

[0172] Preferably, the olivine is reacted with the carbon dioxide in the presence of water at a pressure of from 50 to 200 bar and a temperature of from 100 to 250 °C.

[0173] Preferably, the olivine carbonation has a carbonation degree of carbonated olivine of: from 10 to 100 weight percent; or, from 40 to 99 weight percent; or from 60 to 95 weight percent; or, from 75 to 90 weight percent of the total weight of the carbonated olivine based on the total amount of carbon dioxide released during thermal decomposition of the carbonated product as determined by thermogravimetric analysis (TGA).Preferably, the olivine is crushed and milled into fine particles prior to the reaction with the carbon dioxide in the presence of water. Preferably, the olivine is milled to a particle size of: from 700 mesh (20 pm) to 50 mesh (300 pm); or, from 600 mesh (23 pm) to 100 mesh (150 pm); or, from 500 mesh (25 pm) to 170 mesh (90 pm).

[0174] Preferably, the olivine is crushed to a particle size of from 500 mesh (25 pm) to 170 mesh (90 pm), wherein the particle size is determined with a laser diffraction technique with a Sympatec Helos equipment for particle size analysis.

[0175] The olivine may be reacted with the carbon dioxide in the presence of water and a catalyst. The catalyst may be a chelating agent. The chelating agent may be: oxalic acid; and / or, citric acid; and / or, fulvic acid; and / or, ethylenediaminetetraacetic acid (EDTA); and / or, nitrilotriacetic acid (NTA); and / or, a combination thereof. Preferably, the chelating agent is oxalic acid.

[0176] The olivine may be reacted with the carbon dioxide in the presence of water and a salt. The salt may act as a catalyst. The salt may be: sodium bicarbonate; and / or, sodium carbonate; and / or, sodium chloride; and / or a combination thereof.

[0177] In one example of the present disclosure, the SCM carbonated olivine is prepared by a method set out in the paper titled “Kinetics and mechanism of mineral carbonation of olivine for CO2 sequestration” by F. Wang etal., Minerals Engineering 131 (2019), 185-197, which is hereby incorporated by reference in its entirety.

[0178] Method of making supplementary cementitious materials (SCMs) comprising inosilicates

[0179] In one example of the present disclosure, the SCM is made by a method that comprises the following steps:

[0180] (a) providing a SCM,

[0181] (b) providing an inosilicate, and

[0182] (c) combining the SCM and the inosilicate.In another example of the present disclosure, the SCM is made by a method that comprises the following steps:

[0183] (a) providing a SCM, wherein the SCM is or comprises carbonated olivine, (b) providing an inosilicate, and

[0184] (c) combining the SCM and the inosilicate.

[0185] Composite cement comprising the supplementary cementitious materials (SCMs) comprising inosilicates

[0186] In one example of the present disclosure, composite cement comprises a SCM comprising an inosilicate. The SCM can additionally comprise carbonated olivine.

[0187] The inosilicate may be present in the SCM at: from 0.5 to 20 weight percent; or, from 0.75 to 15 weight percent; or, from 1 to 10 weight percent of the total weight of the SCM. Preferably, the inosilicate is present in the SCM at from 1 to 10 weight percent of the total weight of the SCM. The inosilicate may be present in the SCM at: from 0.5 to 50 weight percent; or, from 10 to 45 weight percent; or, from 15 to 42; or, from 20 to 40 weight percent of the total weight of the SCM. Preferably, the inosilicate is present in the SCM at from 20 to 40 weight percent of the total weight of the SCM.

[0188] The inosilicate may be: a pyroxene; and / or, an amphibole; and / or, a combination thereof; and / or optionally further comprising a phyllosilicate selected from chlorite minerals.

[0189] The pyroxene may be: clinopyroxene; and / or, orthopyroxene; and / or, a combination thereof.

[0190] The clinopyroxene may be: Diopside; and / or, Hedenbergite; and / or, Augite; and / or, Jadeite; and / or, Aegirine; and / or, Omphacite; and / or, a combination thereof.

[0191] The orthopyroxene may be: Enstatite; and / or, Ferrosilite; and / or, Bronzite; and / or, Hypersthene; and / or, a combination thereof.Preferably, the inosilicate is pyroxene. More preferably, the inosilicate is orthopyroxene. Even more preferably, the inosilicate is Enstatite.

[0192] The amphibole may be: a calcium amphibole; and / or, a sodium amphibole; and / or, a sodium-calcium amphibole; and / or, a lithium-(magnesium-iron-manganese) amphibole; and / or, a lithium amphibole; and / or, a sodium-(magnesium-iron-manganese) amphibole; and / or, a magnesium-iron-manganese amphibole; and / or, a lithium-calcium amphibole; and / or, an alkali amphibole; and / or, a combination thereof.

[0193] The calcium amphibole may be: Tremolite; and / or, Magnesio-hornblende; and / or, Edenite; and / or, Pargasite; and / or, Ferro-actinolite; and / or, Hastingsite; and / or, a combination thereof.

[0194] The sodium amphibole may be: Glaucophane; and / or, Eckermannite; and / or, Leakeite; and / or, Riebeckite; and / or, Arfvedsonite; and / or, a combination thereof.

[0195] The sodium-calcium amphibole may be: Winchite; and / or, Richterite; and / or, Ferro-winchite; and / or, a combination thereof.

[0196] The magnesium-iron-manganese amphibole may be: Cummingtonite; and / or, Grunerite; and / or, Anthophyllite; and / or, Gedrite; and / or, a combination thereof.

[0197] The lithium amphibole may be: Holmquistite; and / or, Ferri-pedrizite; and / or, a combination thereof.

[0198] The alkali amphibole may be: K-richterite; and / or, Eckerite; and / or, a combination thereof.

[0199] The amphibole may be an oxo-amphibole. The oxo-amphibole may be Dellaventuraite; and / or, Obertiite; and / or, Ungarettiite; and / or, Kaersutite; and / or, a combination thereof.Preferably, the inosilicate is an amphibole. More preferably, the inosilicate is a magnesium-iron-manganese amphibole. Even more preferably, the inosilicate is Anthophyllite.

[0200] The chlorite may be Clinochlore; and / or, Chamosite. The Clinochlore may be Kammererite.

[0201] The SCM may be: ground granulated blast furnace slag; and / or, fly ash; and / or, burnt shale; and / or, glass powder; and / or, silica fume; and / or, natural pozzolana; and / or, calcined clays; and / or, pumice; and / or, opaline rock; and / or, metakaolin; and / or, olivine; and / or, carbonated olivine; and / or, a combination thereof.

[0202] The SCM may be a material with pozzolanic properties. The material with pozzolanic properties may be: ground granulated blast furnace slag; and / or, fly ash; and / or, burnt shale; and / or, glass powder; and / or, silica fume; and / or, natural pozzolana; and / or, calcined clays; and / or, pumice; and / or, opaline rock; and / or, metakaolin; and / or, carbonated olivine; and / or, a combination thereof.

[0203] Preferably, the SCM is carbonated olivine. Alternatively, the SCM additionally comprises carbonated olivine.

[0204] Preferably, the SCM is olivine and carbonated olivine. Preferably, the SCM is a mixture of olivine and carbonated olivine. When the SCM is olivine and carbonated olivine, or a mixture of olivine and carbonated olivine, the olivine may be present at: from 0.01 to 60 weight percent; or, from 0.05 to 55 weight percent; or, from 0.1 to 50 weight percent of the total weight of the SCM and the carbonated olivine may be present at: from 1 to 99 weight percent; or, from 35 to 97 weight percent; or, from 40 to 95 weight percent of the total weight of the SCM, wherein any remainder is inosilicates and / or unavoidable impurities. Preferably, the olivine is present at from 0.1 to 50 weight percent of the total weight of the SCM and the carbonated olivine is present at from 40 to 95 weight percent of the total weight of the SCM, wherein any remainder is inosilicates and / or unavoidable impurities.

[0205] In the examples set out above, the SCM may comprise another inosilicate.The composite cement may comprise the SCM at: from 1 to 95 weight percent; or, from 3 to 75 weight percent; or, from 10 to 60 weight percent of the total weight of the composite cement. Preferably, the composite cement comprises the SCM at from 10 to 60 weight percent of the total weight of the composite cement. The SCM includes an inosilicate as set out above.

[0206] When the SCM is carbonated olivine, the composite cement may comprise the SCM at from: 1 to 80 weight percent; or, from 5 to 70 weight percent; or, from 10 to 60 weight percent of the total weight of the composite cement. Preferably, the composite cement comprises the SCM at from 10 to 60 weight percent of the total weight of the composite cement. The SCM includes an inosilicate as set out above.

[0207] When the SCM is olivine and carbonated olivine, or a mixture of olivine and carbonated olivine, the composite cement may comprise the SCM at from: 1 to 80 weight percent; or, from 5 to 70 weight percent; or, from 10 to 60 weight percent of the total weight of the composite cement. Preferably, the composite cement comprises the SCM at from 10 to 60 weight percent of the total weight of the composite cement. The SCM includes an inosilicate as set out above.

[0208] The cement in the composite cement may be: Ordinary Portland cement; and / or, Portland pozzolana cement; and / or, rapid-hardening cement; and / or, quick-setting cement; and / or, low-heat cement; and / or, sulfate-resisting cement; and / or, blast furnace slag cement; and / or, high-alumina cement; and / or, white cement; and / or, coloured cement; and / or, air-entraining cement; and / or, expansive cement; and / or, hydrographic cement; and / or, Portland-limestone cement; and / or, a combination thereof. Preferably, the cement is Ordinary Portland cement.

[0209] The composite cement may comprise the cement at: from 1 to 95 weight percent; or, from 30 to 90 weight percent; or, from 40 to 85 weight percent of the total weight of the composite cement. Preferably, the composite cement comprises the cement at from 40 to 85 weight percent of the total weight of the composite cement.Preferably, the composite cement comprises the SCM at from 10 to 60 weight percent of the total weight of the composite cement and cement at from 40 to 85 weight percent of the total weight of the composite cement, wherein the remainder is unavoidable impurities. The SCM includes an inosilicate as set out above.

[0210] When the SCM is carbonated olivine, the composite cement preferably comprises the SCM at from: 10 to 60 weight percent of the total weight of the composite cement and cement at from 40 to 85 weight percent of the total weight of the composite cement, wherein the remainder is unavoidable impurities. The SCM includes an inosilicate as set out above.

[0211] When the SCM is olivine and carbonated olivine; or, a mixture of olivine and carbonated olivine, the composite cement preferably comprises the SCM at from: 10 to 60 weight percent of the total weight of the composite cement and cement at from 40 to 85 weight percent of the total weight of the composite cement, wherein the remainder is unavoidable impurities. The SCM includes an inosilicate as set out above.

[0212] The composite cement may be mixed with aggregates and water to form a cement based material. Typically, the composite cement is mixed with water to form a cement paste and the cement paste is then mixed with aggregate(s) to generate a cement based material such as mortar and / or concrete.

[0213] The aggregate may be: gravel; and / or, sand; and / or, slag; and / or, recycled concrete; and / or, crushed rock; and / or, ballast; and / or, lightweight aggregates; and / or, any combination thereof. Preferably, the aggregate is sand or gravel.

[0214] The cement based material may comprise the composite cement and aggregate at a ratio of: from 2:1 to 10: 1 ; or, 3: 1 to 6: 1 of aggregate to composite cement by weight. Preferably, the cement based material comprises the composite cement and aggregate at a ratio of 3:1 to 6:1 of aggregate to composite cement by weight.

[0215] The cement based material may comprise the composite cement and water at a ratio of: from 0.1 :0.1 to 1:1; or, from 0.25:0.50 to 0.50:0.85; or, 0.35:0.65 of water tocomposite cement by weight. Preferably, the cement based material comprises the composite cement and water at a ratio of 0.35:0.65 of water to composite cement by weight.

[0216] Preferably, the cement based material comprises the composite cement and aggregate at a ratio of 3:1 to 6:1 of aggregate to composite cement by weight and composite cement and water at a ratio of 0.35:0.65 of water to composite cement by weight, wherein any remainder is unavoidable impurities. The composite cement comprises a SCM as set out above.

[0217] The cement based material may additionally comprise admixtures and / or additives. Preferably, the admixtures are: water reducing agents; and / or, plasticizers; and / or, air entering agents; and / or, retarders; and / or setting accelerators; and / or, rheology modifiers; and / or, a combination thereof. Preferably, the additives are: pigments; and / or, fibers; and / or, fillers; and / or, reinforcing elements; and / or, self-healing agents; and / or a combination thereof.

[0218] In one example, the composite cement is used to produce the cement based material mortar.

[0219] In one example of the present disclosure, the cement based material, mortar, comprises:

[0220] a composite cement that comprises SCM at from 10 to 60 weight percent of the total weight of the composite cement and cement at from 40 to 85 weight percent of the total weight of the composite cement,

[0221] an aggregate at a ratio of 3:1 of aggregate to composite cement by weight, water at a ratio of 0.35:0.65 of water to composite cement by weight, wherein any remainder is unavoidable impurities, and

[0222] wherein the SCM comprises an inosilicate and wherein the SCM is carbonated olivine and the inosilicate is Enstatite; or, wherein the SCM comprises carbonated olivine and an inosilicate and the inosilicate is Enstatite.

[0223] Preferably, the cement is Ordinary Portland cement (CEM I) and the aggregate is sand or gravel.Preferably, the Enstatite is present at from 1 to 10 weight percent of the total weight of the SCM. Preferably, the Enstatite is present at from 20 to 40 weight percent of the total weight of the SCM.

[0224] In one example of the present disclosure, the cement based material, mortar, comprises:

[0225] a composite cement that comprises SCM at from 10 to 60 weight percent of the total weight of the composite cement and cement at from 40 to 85 weight percent of the total weight of the composite cement,

[0226] an aggregate at a ratio of 3:1 of aggregate to composite cement by weight, water at a ratio of 0.35:0.65 of water to composite cement by weight, wherein any remainder is unavoidable impurities, and

[0227] wherein the SCM comprises an inosilicate and wherein the SCM is carbonated olivine and the inosilicate is Anthophyllite; or, wherein the SCM comprises carbonated olivine and an inosilicate and the inosilicate is Anthophyllite.

[0228] Preferably, the cement is Ordinary Portland cement (CEM I) and the aggregate is sand or gravel.

[0229] Preferably, the Anthophyllite is present at from 1 to 10 weight percent of the total weight of the SCM. Preferably, the Anthophyllite is present at from 20 to 40 weight percent of the total weight of the SCM.

[0230] In one example of the present disclosure, the cement based material, mortar, comprises:

[0231] a composite cement that comprises SCM at from 10 to 60 weight percent of the total weight of the composite cement and cement at from 40 to 85 weight percent of the total weight of the composite cement

[0232] an aggregate at a ratio of 3:1 of aggregate to composite cement by weight, water at a ratio of 0.35:0.65 of water to composite cement by weight, wherein any remainder is unavoidable impurities, and

[0233] wherein the SCM comprises an inosilicate and wherein the SCM is olivine and carbonated olivine and the inosilicate is Enstatite; or, wherein the SCM comprises amixture of carbonated olivine and olivine and an inosilicate and the inosilicate is Enstatite.

[0234] Preferably, the cement is Ordinary Portland cement (CEM I) and the aggregate is sand or gravel.

[0235] Preferably, the Enstatite is present at from 1 to 10 weight percent of the total weight of the SCM. Preferably, the Enstatite is present at from 20 to 40 weight percent of the total weight of the SCM.

[0236] Preferably, the olivine is present at from 0.1 to 50 weight percent of the total weight of the SCM and the carbonated olivine is present at from 40 to 95 weight percent of the total weight of the SCM and any remainder is unavoidable impurities.

[0237] In one example of the present disclosure, the cement based material, mortar, comprises:

[0238] a composite cement that comprises SCM at from 10 to 60 weight percent of the total weight of the composite cement and cement at from 40 to 85 weight percent of the total weight of the composite cement,

[0239] an aggregate at a ratio of 3:1 of aggregate to composite cement by weight, water a ratio of 0.35:0.65 of water to composite cement by weight, wherein any remainder is unavoidable impurities, and

[0240] wherein the SCM comprises an inosilicate and wherein the SCM is olivine and carbonated olivine and the inosilicate is Anthophyllite; or, wherein the SCM comprises a mixture of carbonated olivine and olivine and an inosilicate and the inosilicate is Anthophyllite.

[0241] Preferably, the cement is Ordinary Portland cement (CEM I) and the aggregate is sand or gravel.

[0242] Preferably, the Anthophyllite is present at from 1 to 10 weight percent of the total weight of the SCM. Preferably, the Anthophyllite is present at from 20 to 40 weight percent of the total weight of the SCM.Preferably, the olivine is present at from 0.1 to 50 weight percent of the total weight of the SCM and the carbonated olivine is present at from 40 to 95 weight percent of the total weight of the SCM and any remainder is unavoidable impurities.

[0243] In one example, the composite cement is used to produce the cement based material concrete.

[0244] In one example of the present disclosure, the cement based material, concrete, comprises:

[0245] a composite cement that comprises SCM at from 10 to 60 weight percent of the total weight of the composite cement and cement at from 40 to 85 weight percent of the total weight of the composite cement,

[0246] an aggregate at a ratio of 6:1 of aggregate to composite cement by weight, water at a ratio of 0.35:0.65 of water to composite cement by weight, wherein any remainder is unavoidable impurities, and

[0247] wherein the SCM comprises an inosilicate and wherein the SCM is carbonated olivine and the inosilicate is Enstatite; or, wherein the SCM comprises carbonated olivine and an inosilicate and the inosilicate is Enstatite.

[0248] Preferably, the cement is Ordinary Portland cement (CEM I) and the aggregate is sand.

[0249] Preferably, the Enstatite is present at from 1 to 10 weight percent of the total weight of the SCM. Preferably, the Enstatite is present at from 20 to 40 weight percent of the total weight of the SCM.

[0250] In one example of the present disclosure, the cement based material, concrete, comprises:

[0251] a composite cement that comprises SCM at from 10 to 60 weight percent of the total weight of the composite cement and cement at from 40 to 85 weight percent of the total weight of the composite cement,

[0252] an aggregate at a ratio of 6:1 of aggregate to composite cement by weight, water at a ratio of 0.35:0.65 of water to composite cement by weight, wherein any remainder is unavoidable impurities, andwherein the SCM comprises an inosilicate and wherein the SCM is carbonated olivine and the inosilicate is Anthophyllite; or, wherein the SCM comprises carbonated olivine and an inosilicate and the inosilicate is Anthophyllite.

[0253] Preferably, the cement is Ordinary Portland cement (CEM I) and the aggregate is sand.

[0254] Preferably, the Anthophyllite is present at from 1 to 10 weight percent of the total weight of the SCM. Preferably, the Anthophyllite is present at from 20 to 40 weight percent of the total weight of the SCM.

[0255] In one example of the present disclosure, the cement based material, concrete, comprises:

[0256] a composite cement that comprises SCM at from 10 to 60 weight percent of the total weight of the composite cement and cement at from 40 to 85 weight percent of the total weight of the composite cement

[0257] an aggregate at a ratio of 6:1 of aggregate to composite cement by weight, water at a ratio of 0.35:0.65 of water to composite cement by weight, wherein any remainder is unavoidable impurities, and

[0258] wherein the SCM comprises an inosilicate and wherein the SCM is olivine and carbonated olivine and the inosilicate is Enstatite; or, wherein the SCM comprises a mixture of carbonated olivine and olivine and an inosilicate and the inosilicate is Enstatite.

[0259] Preferably, the cement is Ordinary Portland cement (CEM I) and the aggregate is sand.

[0260] Preferably, the Enstatite is present at from 1 to 10 weight percent of the total weight of the SCM. Preferably, the Enstatite is present at from 20 to 40 weight percent of the total weight of the SCM.

[0261] Preferably, the olivine is present at from 0.1 to 50 weight percent of the total weight of the SCM and the carbonated olivine is present at from 40 to 95 weight percent of the total weight of the SCM and any remainder is unavoidable impurities.In one example of the present disclosure, the cement based material, concrete, comprises:

[0262] a composite cement that comprises SCM at from 10 to 60 weight percent of the total weight of the composite cement and cement at from 40 to 85 weight percent of the total weight of the composite cement,

[0263] an aggregate at a ratio of 6:1 of aggregate to composite cement by weight, water a ratio of 0.35:0.65 of water to composite cement by weight, wherein any remainder is unavoidable impurities, and

[0264] wherein the SCM comprises an inosilicate and wherein the SCM is olivine and carbonated olivine and the inosilicate is Anthophyllite; or, wherein the SCM comprises a mixture of carbonated olivine and olivine and an inosilicate and the inosilicate is Anthophyllite.

[0265] Preferably, the cement is Ordinary Portland cement (CEM I) and the aggregate is sand.

[0266] Preferably, the Anthophyllite is present at from 1 to 10 weight percent of the total weight of the SCM. Preferably, the Anthophyllite is present at from 20 to 40 weight percent of the total weight of the SCM.

[0267] Preferably, the olivine is present at from 0.1 to 50 weight percent of the total weight of the SCM and the carbonated olivine is present at from 40 to 95 weight percent of the total weight of the SCM and any remainder is unavoidable impurities.

[0268] In the examples set out above, the SCM may comprise another inosilicate.

[0269] EXAMPLES

[0270] The following are non-limiting examples that discuss, with reference to tables and figures, the advantages of the present invention. The examples set forth herein are merely examples among other possible examples.Example 1: Mineral and morphological composition of Enstatite

[0271] 1. Mineral composition

[0272] In this non-limiting example, the mineral composition of Enstatite was analysed using X-ray Diffraction (XRD) analysis (such as on a Broker D2 Phaser instrument). The results are shown in Figure 1.

[0273] As shown in Figure 1 , the Enstatite is 90.10 percent pure with other species such as Clinochlore, Hornblende and Talc present.

[0274] 2. Morphological composition

[0275] In this non-limiting example, the morphological composition of Enstatite was analysed using scanning electron microscopy (SEM) (instrument: JEOL JSM-6010 Plus / LV) equipped with an Energy-Dispersive X-ray Spectroscopy (EDS) detector (Oxford Ultirn Max 170)). The results are shown in Figures 2A and 2B.

[0276] As shown in Figures 2A and 2B, the Enstatite exhibited elongated particle morphologies with characteristic lengths in the range of approximately 8-15 pm. Enstatite with this elongated particle morphology contributed to improved flexural strength in the final hardened cement-based material.

[0277] Figure 3 is an elemental mapping of the Enstatite. As shown in Figure 3, the elongated particles of Enstatite were magnesium silicate rich. The spectrum points of 111, 112 and 113 taken on the surface of the elongated particle of Enstatite show that the Enstatite had an oxide composition comprising approximately 34-37 weight percent of magnesium oxide (MgO), 52-56 weight percent of iron oxide (Fe2Os) of the total weight of the Enstatite, which is consistent with Fe-bearing Enstatite.

[0278] Example 2: Measuring flexural strength of cement based materials

[0279] In this non-limiting example, the flexural strength of a cement based material (mortar) comprising carbonated olivine and Enstatite was measured.Preparation

[0280] Mortar samples were produced and tested following the EN 196-1 : 2016 standard to evaluate the improvement of the flexural strength provided by the Enstatite in a cement-based material with carbonated olivine as a supplementary cementitious material.

[0281] The starting material (olivine) had a magnesium oxide (MgO) content of 49.3 weight percent, a silica (SiCh) content of 41.6 weight percent and an iron oxide (FeO) content of 7.6 weight percent of the total weight of the starting material (olivine) measured by XRF analysis (Axios, Malvern Panalytical). The starting material (olivine) had an olivine content of 89.4 weight percent of the total weight of the starting material (olivine), as measured by XRD analysis (Bruker D2 Phaser instrument). The starting material (olivine) had a D50 of 7pm (measured by laser diffraction, Sympatec Helos).

[0282] The starting material (olivine) was subjected to a carbonation reaction in the presence of carbon dioxide. The carbonation reaction was undertaken via a wet process using a high-pressure reactor. The carbonation reaction was performed using a carbon dioxide purity of 99.7 percent for four hours at 200 °C and 180 bar in the presence of sodium bicarbonate (NaHCOs).

[0283] Analysis of the resulting carbonated product, carbonated olivine, indicated a carbonation degree of 90 weight percent of the total weight of the carbonated olivine. In particular, the 90 weight percent of the product consisted of magnesium carbonate (MgCO3) and silicon dioxide (SiO2). The remaining 10 weight percent of the resulting carbonated product comprised unreacted or partially reacted components, including magnesium silicate (Mg2SiO4) and minor metal oxide constituents such as ferric oxide (FeO).

[0284] The carbonation degree was calculated based on mass loss determined by Thermogravimetric analysis (TGA-Mettler Toledo TGA / DSC 3+) in the temperaturerange 450 °C to 900 °C. In this temperature range, magnesium carbonate in the solid carbonated product decomposes and carbon dioxide was released:

[0285] 2MgCOs + SiO2 -> 2MgO+ SiO2 + 2CO2

[0286] The release of carbon dioxide from the solid carbonated product resulted in a loss in mass of the solid material. The magnitude of the mass loss was directly proportional to the amount of carbonate formed, thereby providing a quantitative measure of the extent of carbonation.

[0287] The carbonated olivine had a magnesium carbonate (MgCOs) content of 60.0 weight percent and an amorphous silica (SiCh) content of 28.6 weight percent of the total weight of the carbonated olivine, measured by XRD analysis (Bruker D2 Phaser instrument). The remaining part of the carbonated olivine included unreacted materials.

[0288] Mineralogical measurements were performed with XRD analysis using the Rietveld quantification method.

[0289] Four mortar samples were prepared by replacing 20 and 25 weight percent of cement with the carbonated olivine and quartz or Enstatite. The cement used was a commercial ordinary Portland cement Cem I 52.5 R.

[0290] In the mortar samples, the proportion of carbonated olivine was fixed at 15 weight percent of the total weight of the mortar sample. The additional 5 or 10 weight percent (to achieve the abovementioned 20 and 25 weight percent) was achieved by incorporating quartz or Enstatite powders (weight percent being of the total weight of the mortar sample).

[0291] Quartz was selected as reference, since it is a commonly used supplementary material. The two minerals, quartz and Enstatite, were milled and sieved below 100 pm and both had a D50 of 25 pm (determined with a laser diffraction technique a Sympatec Helos equipment for particle size analysis). The compositions are shown in Table 1.Table 1. Mortar samples with 15 weight percent of carbonated olivine and 5 or 10 weight percent of Enstatite or quartz addition, wherein wt% is weight percent of the total weight of the mortar sample.

[0292] 5 (wt%) 10(wt%) 5 (wt%) 10(wt%) Component

[0293] Enstatite Enstatite Quartz Quartz Portland

[0294] cement 360 337.5 360 337.5

[0295] (Cem I) (g)

[0296] Carbonated

[0297] 67.5 67.5 67.5 67.5 olivine (g)

[0298] Enstatite

[0299] 22.5 45 - - powder (g)

[0300] Quartz

[0301] - - 22.5 45

[0302]

[0303] powder (g)

[0304] The four mortar samples produced with the blended cement composition, as described in Table 1 , were tested for flexural strength using a Tonitechnick bench press (Tonitrol v.1) after 7 and 28 days of curing. For each curing age, the measurement was performed on two prisms.

[0305] Results

[0306] The results of the flexural strength test of mortars with 15 weight percent of carbonated olivine and 5 or 10 weight percent of Enstatite or quartz are shown in Figure 4. The flexural strength results indicate that the blends containing Enstatite exhibited both at 7 and 28 days superior flexural performance compared to those incorporating quartz, showing increases of +9.8 percent (5 weight percent Enstatite compared to 5 weight percent of quartz) and +7.8 percent (10 weight percent of Enstatite compared to 10 weight percent of quartz) at 28 days. This improvement is attributed to the characteristic elongated morphology of Enstatite particles.

[0307] Example 3: Measuring pore discontinuity in mortars that include the addition of 10 weight percent of Enstatite (of the total weight of the mortar)

[0308] In this non-limiting example, capillary water absorption and bulk resistivity measurements were performed to demonstrate the impact of Enstatite in increasingthe pore tortuosity and discontinuity, generating a cementitious matrix with reduced improved durability.

[0309] 3.1 - 25 weight percent SCM replacement

[0310] Preparation

[0311] Standard mortars were produced and tested following the EN 196-1 : 2016 standard. Three mortars were produced that had a total cement replacement of 25 weight percent of the total weight of each mortar. For one mortar, 25 weight percent of the total weight of the cement was replaced with carbonated olivine (OC). In the other two mortars, 15 weight percent of the total weight of the cement was replaced with carbonated olivine (OC) and 10 weight percent of the total weight of the cement was replaced with quartz or Enstatite, wherein the quartz and Enstatite represented 40 percent of the SCM content.

[0312] As in Example 2, quartz was selected as reference, since it is a commonly used supplementary material. The two minerals, quartz and Enstatite, were milled and sieved below 100pm and both had a D50 of 25 pm (determined with a laser diffraction technique with a Sympatec Helos equipment for particle size analysis). The compositions are shown in Table 2.

[0313] Table 2. Mortar samples with carbonated olivine (OC), Enstatite and quartz substitution, wherein wt% is weight percent of the total weight of the mortar sample.

[0314] 15 (wt%) OC and 15 (wt%) OC and Components 25 (wt%) OC

[0315] 10 (wt%) Enstatite 10 (wt%) Quartz Portland cement

[0316] 337.5 337.5 337.5 (Cem I) (g)

[0317] Carbonated olivine

[0318] 112.5 67.5 67.5

[0319] (g)

[0320] Enstatite powder - 45 - (g)

[0321] Quartz powder (g) - - 45

[0322]

[0323] Capillary water absorptionThe capillary water absorption was determined following the standard EN 1015-18: 2002 on standard prisms, at the age of 28 days, after recommended curing resume and conditioning. The sides of each mortar sample analysed were covered with an aluminium tape to force the water absorption only from the side exposed to the water.

[0324] During the measurements, the mortar samples were placed in a shallow flatbottomed trays on knife-edge supports to achieve a depth of water immersion of (2.0 ± 1.0) mm. The mass of the specimens was measured immediately before their exposure to the clean water at the beginning of the measurement and then at various time intervals throughout the measurement. Before measurement the surface water was wiped off the mortar samples with a damp cloth. Between measurements, the tray was covered with a lid, and after the weight of each mortar sample was measured, the water level was checked and corrected if necessary.

[0325] The cumulative water absorption per unit area, i(t)(in kg / m2), was calculated using Equation (Eq.) 1 :

[0326]

[0327] where Am represents the increase in the specimen mass (kg) and A is the exposed surface area (m2).

[0328] The absorption coefficient C(sorptivity) was determined from the slope of the linear portion of the plot of i(t) versus Vt, where t is the time in seconds (s). The initial linear region was used for regression analysis, as this period corresponds to capillary-driven absorption. The coefficient C is expressed in units of kg / m2.s0-5.

[0329] Electrical bulk resistivity

[0330] The electrical bulk resistivity was measured with the two-point probe method, conceptually based on ASTM C1760-12 “Standard test method for bulk electricalconductivity of hardened concrete", with prismatic samples (with dimensions 4 x 4 cm).

[0331] The mortar samples were separately placed between two electrodes (parallel metal plates) with moist sponge contacts in electrochemical impedance spectroscopy (EIS) mode. Bulk impedance measurements were performed using an IviumStat 24-bit CompactStat potentiostat (Ivium Technologies, Netherlands). Alternating Current (AC) signal of 10 mV was applied over a frequency range of 100 kHz to 0.1 Hz. The separation distance between the electrodes was fixed at 16 cm.

[0332] Prior to each measurement, the sponge was soaked in a low conductivity electrolyte solution comprising NaOH 7.6 g / L, KOH 10.64 g / L and Ca(OH)22 g / L (which is commonly used), to ensure stable and reproducible ionic contact, prevent drying during the test, and reduce contact impedance effects. Excess liquid was gently removed to achieve a moist, but not dripping, interface.

[0333] Resistivity was calculated using the following Equation 2: p = /

[0334]

[0335] ?bulk|

[0336] where:

[0337] p - electrical resistivity (Q m);

[0338] buik- high-frequency intercept on the Nyquist diagram (Q);

[0339] S - electrode area (m2);

[0340] L - specimen thickness (m).

[0341] Results: Capillary water absorption

[0342] The results from the capillary water absorption are shown in Table 3.

[0343] Table 3. Sorptivity coefficients

[0344] Mortar sample Initial sorptivity (0-5 h) (mm-s"1 / 2)

[0345] 15 wt% CO + 10 wt% quartz 0.01224

[0346] 15 wt% CO + 10 wt% Enstatite 0.00858

[0347]

[0348] The presence of Enstatite lead to a pronounced increase in pore network discontinuity, as demonstrated consistently by multiple independent transport parameters measured at the mortar scale.

[0349] The capillary absorption curves for both modified mortar samples exhibited a nearly linear relationship with the square root of time during the early stage of testing (Figure 5). This linearity is characteristic of capillary-controlled water uptake, confirming that the regime of interest was governed primarily by capillary suction rather than diffusion or permeation.

[0350] The regression lines determined for the 0-5 h interval revealed a steeper slope for the mortar sample comprising 10 weight percent quartz mixture compared with the mortar sample comprising 10 weight percent Enstatite, indicating faster early-time infiltration in the quartz system. This is consistent with the measured sorptivity coefficients presented in Table 3.

[0351] As shown in Table 3, the initial sorptivity — which reflects the ease of water ingress driven by capillarity and depends strongly on capillary pore size and connectivity in the near-surface region — was approximately 30% lower in the Enstatite-containing mortar sample (0.00858 mm s-1 / 2) relative to the quartz-modified mortar sample (0.01224 mm s-1 / 2). This reduction clearly indicates reduced capillary continuity. The presence of Enstatite increases pore tortuosity and disrupts the connectivity of the capillary structure, thereby slowing early-age water uptake. Therefore, this behaviour can be beneficial from a durability standpoint by reducing the ingress of aggressive agents and lowering the material’s susceptibility to moisture fluctuations and wetting cycles.Results: Electrical bulk resistivity

[0352] The electrical bulk resistivity results are shown in Table 4.

[0353] Table 4. Bulk resistivity measurements

[0354] Sample Bulk resistivity (Qm)

[0355] 25 wt% CO 109

[0356] 15 wt% CO + 10 wt% quartz 60

[0357] 15 wt% CO + 10 wt% Enstatite 126

[0358]

[0359] The bulk resistivity test provided a complementary macroscopic measure of pore connectivity. The resistivity results in Table 4 clearly mirror the behaviour observed in the sorptivity results, since the mortar sample comprising Enstatite exhibited a bulk resistivity of 126 O m, which is 110% higher than observed for the mortar sample comprising quartz (60 O m) and 16% higher than the mortar sample comprising 25 weight percent of carbonated olivine (109 O m). Higher resistivity directly implies greater disruption of continuous conductive paths, confirming a more tortuous pore structure that hinders ionic transport.

[0360] Conclusion

[0361] Taken together, the sorptivity and resistivity data results give a coherent picture: the mortar samples that comprised carbonated olivine and Enstatite exhibited less connected capillary pathways and a more tortuous pore system than the mortar sample that comprised quartz. These changes manifest as both lower sorptivity and higher resistivity, providing converging evidence of enhanced pore discontinuity.

[0362] The underlying mechanism driving these observations was the microstructural disruption of continuous flow paths, particularly within and around the interfacial transition zone (ITZ). This microstructural modification lead directly to the observed reductions in capillary-driven absorption and ionic conduction.3.2- 35 weight percent SCM replacement

[0363] Preparation

[0364] Standard mortars were produced and tested following the EN 196-1 : 2016 standard. Three mortars were produced that had a total cement replacement of 35 weight percent of the total weight of each mortar. For one mortar, 35 weight percent of the total weight of the cement was replaced with carbonated olivine (OC). In another mortar, 25 weight percent of the total weight of the cement was replaced with carbonated olivine and 10 weight percent of the total weight of the cement was replaced with Enstatite. The compositions are shown in Table 5.

[0365] Table 5. Composition for the tested mortar samples, wherein wt% is weight percent of the total weight percent of the mortar sample.

[0366] Components 0 wt % Enstatite 10 wt% Enstatite Portland cement (Cem I) (g) 292.5 292.5

[0367] Carbonated olivine (g) 157.5 141.75

[0368] Enstatite powder (g) 0 15.75

[0369]

[0370] Capillary water absorption

[0371] The capillary water absorption was determined following the standard EN 1015-18: 2002 on standard prisms, at the age of 28 days, after recommended curing resume and conditioning. The sides of each mortar sample analysed were covered with an aluminium tape to force the water absorption only from the side exposed to the water. The tests were conducted like in Example 3.1.

[0372] Capillary water absorption results

[0373] The results from the capillary water absorption are shown in Table 6.Table 6. Sorptivity coefficients.

[0374] Mortar sample Initial sorptivity Secondary sorptivity (0-5 h) (0-48 h) (kg / m2-s"1 / 2) (kg / m2-s"1 / 2)

[0375] 0 wt% Enstatite 0.01518 0.00462

[0376] 10 wt% Enstatite 0.01225 0.00359

[0377]

[0378] Comparison of the data presented in Figure 6 demonstrates that the mixture containing 10 weight percent Enstatite consistently outperformed the reference mixture (where the mortar sample comprises 35 weight percent carbonated olivine and 0 weight percent Enstatite) at all stages of the capillary water absorption test. At 5 hours, the sample with Enstatite addition of 10 weight percent exhibited approximately 13% lower water uptake, and at 48 hours, the reduction remained significant at 11%.

[0379] As evidenced by the results in Table 6, substituting 10 weight percent of the supplementary cementitious material with Enstatite lead to a pronounced reduction in early-time capillary absorption (approximately -19%), indicating the formation of a denser and more tortuous near-surface pore network. This reduced permeability persisted throughout the test duration: at later times, the Enstatite -containing mixture continued to absorb water more slowly (approximately -22% relative to the Enstatite-free sample). This sustained reduction suggests that the incorporation of Enstatite promotes a refined and more uniformly compact pore structure throughout the matrix, not only at the exposed surface.

[0380] As seen in Example 3.1 , in over extended curing periods up to 200 days, the SCM-containing mortar samples reached sorptivity values comparable to the reference cement, confirming that long-term moisture transport resistance was fully recovered despite clinker reduction.

[0381] Taken together, the results from Examples 3.1 and 3.2 clearly demonstrate that, in addition to the beneficial effect attributed to the 10 weight percent Enstatite substitution, the higher overall SCM replacement level (increasing carbonated olivine from 25 weight percent to 35 weight percent) also contributes to reduced sorptivity.This further enhancement indicates that both the increased carbonated olivine content and the inclusion of Enstatite act synergistically to disrupt capillary pathways and refine the pore structure.

[0382] Example 4: Enhancing the flexural strength of mortars with 35 weight percent of SCM replacement and higher Enstatite content.

[0383] In this non-limiting example, flexural strength of mortars was measured.

[0384] Preparation

[0385] Standard mortars were produced and tested following the EN 196-1 : 2016 standard with a total Portland cement replacement of 35 mass percent of the total mass of each mortar. For one mortar, 35 mass percent of the total mass of the Portland Cement was replaced with carbonated olivine (OC). In another example, 15 mass percent of the Portland cement was replaced with carbonated olivine (OC) and 20 mass percent of the Portland cement was replaced with Enstatite (with the mass percent being of the total mass of the mortar). To evaluate the influence of the mineralogical composition of the SCM, the Enstatite content within the SCM was varied.

[0386] The mortar samples had Enstatite levels of 0 mass percent and 20 mass percent of the total SCM mass, enabling direct assessment of the effect of controlled Enstatite additions on hydration behaviour and performance of the blended binder. The compositions of the two mortar samples are shown in Table 7.Table 7. Mortar sample composition, wherein wt% is weight percent of the total weight of the mortar sample.

[0387] Component 35 wt% SCM 15 wt% SCM 0 wt% Enstatite 20% Enstatite Portland cement (Cem I) (g) 292.5 292.5

[0388] Carbonated olivine (g) 157.5 126

[0389] Enstatite powder (g) 0 31.5

[0390]

[0391] The mortar samples were tested for flexural strength using a Tonitechnick bench press (Tonitrol v.1 ) after 7 and 28 days of curing. For each curing age, the measurement was performed on two prisms.

[0392] Resu / ts

[0393] Figure 7 shows the flexural strength development at 7 and 28 days for mortar samples incorporating 35 mass percent of the carbonated olivine, with and without the addition of 20 mass percent Enstatite within the carbonated olivine fraction. The data shows that the presence of Enstatite produced a measurable and consistent enhancement of both early-age and later-age flexural performance.

[0394] At 7 days, the reference mixture (OC 35 mass percent - Enstatite 0 mass percent) reached a flexural strength of 6.24 MPa, whereas the mortar containing 15 mass percent OC and 20 mass percent Enstatite achieved an improvement of approximately 7.7%. This early-age gain indicated that Enstatite contributed positively to the initial mechanical development of the matrix.

[0395] At 28 days, both systems exhibited significant strength growth. The reference mortar (OC 35 mass percent - Enstatite 0 mass percent) attained 10.905 MPa, while the mortar containing 15 mass percent OC and 20 mass percent Enstatite reached an 8.3% increase relative to the reference mortar. The similarity in improvement at bothcuring ages indicated that the primary mechanism by which Enstatite enhanced flexural performance is physical rather than chemical.

[0396] Overall, the combined data demonstrates that optimised SCM blends incorporating Enstatite can deliver superior flexural performance relative to the reference mortars particularly when carbonated olivine and Enstatite are used together in balanced proportions.

[0397] The features disclosed in the foregoing description, or the following claims, or the accompanying drawings, expressed in their specific forms or in terms of a means for performing the disclosed function, or a method or process for attaining the disclosed result, as appropriate, may, separately, or in any combination of such features, be utilized for realising the invention in diverse forms thereof.

[0398] Although certain example aspects of the invention have been described, the scope of the appended claims is not intended to be limited solely to these examples. The claims are to be construed literally, purposively, and / or to encompass equivalents.

Claims

CLAIMS1. A supplementary cementitious material (SCM) comprising carbonated olivine and an inosilicate.

2. The supplementary cementitious material (SCM) of claim 1, wherein the inosilicate is present at: from 0.5 to 50 weight percent; or, from 0.5 to 20 weight percent; or, from 0.75 to 15 weight percent; or, from 1 to 10 weight percent; or, from 10 to 45 weight percent; or, from 15 to 42 weight percent; or, from 20 to 40 weight percent of the total weight of the supplementary cementitious material (SCM).

3. The supplementary cementitious material (SCM) of claim 1 or claim 2, wherein the inosilicate is: a pyroxene; and / or, an amphibole; and / or, a combination thereof; and / or optionally further comprising a phyllosilicate selected from chlorite minerals; and / or optionally,wherein:(i) the pyroxene is: clinopyroxene; and / or, orthopyroxene; and / or, a combination thereof; optionally,wherein the clinopyroxene is: Diopside; and / or, Hedenbergite; and / or, Augite; and / or, Jadeite; and / or, Aegirine; and / or, Omphacite; and / or, a combination thereof; and / or,wherein the orthopyroxene is: Enstatite; and / or, Ferrosilite; and / or, Bronzite; and / or, Hypersthene; and / or, a combination thereof; or,(ii) the amphibole is: a calcium amphibole; and / or, a sodium amphibole; and / or, a sodium-calcium amphibole; and / or, a lithium-(magnesium-iron-manganese) amphibole; and / or, a lithium amphibole; and / or, a sodium-(magnesium-iron-manganese) amphibole, a magnesium-iron-manganese amphibole, and / or, a lithiumcalcium amphibole; and / or, an alkali amphibole; and / or, a combination thereof;optionally,wherein the calcium amphibole is: Tremolite; and / or, Magnesio-hornblende; and / or, Edenite; and / or, Pargasite; and / or, Ferro-actinolite; and / or, Hastingsite; and / or, a combination thereof; and / or,wherein the sodium amphibole is: Glaucophane; and / or, Eckermannite; and / or, Leakeite; and / or, Riebeckite; and / or, Arfvedsonite; and / or, a combination thereof; and / or,wherein the sodium-calcium amphibole is: Winchite; and / or, Richterite; and / or, Ferro-winchite; and / or, a combination thereof; and / or,wherein the magnesium-iron-manganese amphibole is: Cummingtonite; and / or, Grunerite; and / or, Anthophyllite; and / or, Gedrite; and / or, a combination thereof; and / or,wherein the lithium amphibole is: Holmquistite; and / or, Ferri-pedrizite; and / or, a combination thereof; and / or,wherein the alkali amphibole is: K-richterite; and / or, Eckerite; and / or, a combination thereof; or,(iii) the chlorite is: Clinochlore; and / or, Chamosite; optionally, wherein the Clinochlore is Kammererite.

4. The supplementary cementitious material (SCM) of any one of claims 1 to 3, wherein the inosilicate comprises, or consists of, Enstatite; or,wherein the inosilicate comprises, or consists of, Anthophyllite.

5. The supplementary cementitious material (SCM) of any one of claims 1 to 4, wherein the supplementary cementitious material (SCM) is, or, further comprises: ground granulated blast furnace slag; and / or, fly ash; and / or, burnt shale; and / or, glass powder; and / or, silica fume; and / or, natural pozzolana; and / or, calcined clays;and / or, pumice; and / or, opaline rock; and / or, metakaolin; and / or, olivine; and / or, a combination thereof.

6. The supplementary cementitious material (SCM) of any one of claims 1 to 5, wherein the supplementary cementitious material (SCM) comprises, or consists of:(a) carbonated olivine and olivine, optionally, wherein the carbonated olivine and olivine are a mixture; and,(b) an inosilicate.

7. The supplementary cementitious material (SCM) of claim 6, wherein the supplementary cementitious material (SCM) comprises, or consists of:(a) carbonated olivine and olivine; optionally, wherein the carbonated olivine and olivine are a mixture; and(b) Enstatite and / or Anthophyllite.

8. The supplementary cementitious material (SCM) of claim 6 or claim 7 wherein the olivine is present at: from 0.01 to 60 weight percent; or, from 0.05 to 55 weight percent; or, from 0.1 to 50 weight percent of the total weight of the supplementary cementitious material (SCM); and / or,wherein the carbonated olivine is present at: from 1 to 99 weight percent; or, from 35 to 97 weight percent; or, from 40 to 95 weight percent of the total weight of the supplementary cementitious material (SCM).

9. A method of preparing the supplementary cementitious material (SCM) of any one of claims 1 to 8, the method comprising the steps of:(a) providing a supplementary cementitious material (SCM) comprising carbonated olivine, (b) providing an inosilicate, and(c) combining the supplementary cementitious material comprising carbonated olivine and the inosilicate.

10. The method of claim 9, wherein the supplementary cementitious material (SCM) comprises, or consists of, olivine and carbonated olivine; optionally,wherein the supplementary cementitious material (SCM) comprises, or consists of, a mixture of olivine and carbonated olivine; and / or,wherein the olivine is present at: from 0.01 to 60 weight percent; or, from 0.05 to 55 weight percent; or, from 0.1 to 50 weight percent of the total weight of the supplementary cementitious material (SCM); and / or,wherein the carbonated olivine is present at: from 1 to 99 weight percent; or, from 35 to 97 weight percent; or, from 40 to 95 weight percent of the total weight of the supplementary cementitious material (SCM).

11. The method of claim 9 or 10, wherein the inosilicate is present at: from 0.5 to 50 weight percent; or from 10 to 45 weight percent; or, from 15 to 42 weight percent; or, from 20 to 40 weight percent of the total weight of the supplementary cementitious material (SCM).

12. The method of any one of claims 9 to 11 , wherein the carbonated olivine is prepared by reacting olivine with carbon dioxide in the presence of water; optionally,(a) wherein the olivine is reacted with the carbon dioxide in the presence of water at a pressure of from 10 to 300 bar; or, from 25 to 250 bar; or, from 50 to 200 bar; and / or,(b) wherein the olivine is reacted with the carbon dioxide in the presence of water at a temperature of from 100 to 350 °C; or, from 125 to 325 °C; or, from 150 to 300 °C; or, from 100 to 300 °C; or, from 100 to 250 °C; and / or,(c) wherein the olivine is reacted with the carbon dioxide in the presence of water at a pressure of from 50 to 200 bar and a temperature of 150 to 300 °C.

13. The method of any one of claims 9 to 12, wherein the olivine carbonation has a carbonation degree of carbonated olivine of: from 10 to 100 weight percent; or, from 40 to 90 weight percent; or, from 60 to 95 weight percent; or from 75 to 90 weight percent of the total weight of the carbonated olivine based on the total amount ofcarbon dioxide released during thermal decomposition of the carbonated product as determined by thermogravimetric analysis (TGA).

14. A composite cement comprising the supplementary cementitious material (SCM) of any one of claims 1 to 8.

15. The composite cement of claim 14, wherein the composite cement comprises:the supplementary cementitious material (SCM) at: from 1 to 95 weight percent; or, from 3 to 75 weight percent; or, from 10 to 60 weight percent of the total weight of the composite cement.

16. A cement based material comprising the composite cement of claim 14 or claim 15, wherein the cement based material further comprises:an aggregate, andwater.

17. The cement based material of claim 16, wherein the cement based material comprises:the composite cement and water at a ratio of: from 0.1 :0.1 to 1 : 1 ; or, from 0.25:0.50 to 0.50:0.85; or, 0.35:0.65 of water to composite cement by weight; and the composite cement and aggregate at a ratio of: from 2:1 to 10:1 ; or, 3:1 to 6:1 of aggregate to composite cement by weight;wherein any remainder is unavoidable impurities.

18. Use of the supplementary cementitious material (SCM) of any one of claims 1 to 8 for promoting pore discontinuity in cement based materials.

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