Low calcium content cementitious material

Abstract

Disclosed herein are compositions comprising CaO and SiO2 at varying ratios.

Description

[0001] NLH-00125 LOW CALCIUM CONTENT CEMENTITIOUS MATERIAL CROSS-REFERENCE TO RELATED APPLICATIONS

[0002] This application claims the benefit of U. S. Provisional Application No. 63 / 755,111 filed February 6, 2025, the contents of which is incorporated in its entirety by this reference.

[0003] BACKGROUND

[0004] The production of cementitious materials is traditionally highly energy and carbon intensive. Mechanochemical techniques (e.g., grinding and milling) represent a suitable alternative to traditional, thermal-based kiln techniques. However, there is a need for improved low-carbon cementitious compositions and methods for producing such materials.

[0005] SUMMARY OF THE INVENTION

[0006] In certain aspects, provided herein is a composition comprising a plurality of X(CaO) particles and a plurality of Y(SiO2) particles, wherein X: Y is from about 0.05 to about 5.

[0007] In certain aspects, provided herein is a method of preparing a composition comprising a plurality of first CaO particles and a plurality of first SiO2 particles, wherein the method comprises:

[0008] in a first milling step, milling a plurality of first SiO2 particles in a mill, thereby forming a plurality of first milled SiO2particles;

[0009] contacting the plurality of first milled SiO2particles with a plurality of first CaO particles in the mill, thereby forming a mixture of a plurality of remilled SiO2 particles and a plurality of first milled CaO particles; and

[0010] in a second milling step, milling the mixture of the plurality of remilled SiO2 particles and the plurality of first milled CaO particles, thereby forming the composition comprising the plurality of first CaO particles and the plurality of first SiO2 particles.

[0011] In certain aspects, provided herein is a method comprising:

[0012] 1) in a first milling step, milling a plurality of first particles SiO2 in a mill, thereby forming a plurality of first milled SiO2 particles;

[0013] 2) contacting the plurality of first milled SiO2 particles with a plurality of first CaO particles in the mill, thereby forming a mixture of a plurality of remilled SiO2 particles and a plurality of first milled CaO particles; and

[0014] 1

[0015] FH 13302371.4NLH-00125 3) in a second milling step, milling the mixture of the plurality of remilled SiO₂ particlesand the plurality of first milled CaO particles, thereby forming the composition comprising the plurality of first CaO particles and the plurality of first SiO₂ particles.

[0016] BRIEF DESCRIPTION OF THE FIGURES FIGURE 1 is a schematic representation of an exemplary cementitious material particle.

[0017] FIGURE 2 is a table showing the composition of an exemplary cementitious material, in accordance with the disclosure herein.

[0018] FIGURE 3 shows length change data of the cementitious materials described herein when exposed to a sulfate solution. Sulfate exposure was initiated 7-days after cast upon completion of saturated limewater bath cure at 38 °C. Exposure class SI: 0.10% at 6 months. Exposure class S2: 0.05% at 6 months, 0.10% at 12 months if the expansion exceeds the 6-month limit. Exposure class S3: 0.10% at 18 months. Flow of the test mixture was 112%.

[0019] FIGURE 4 is a table showing the ASTM Cl 157-23 Standard Physical Requirements.

[0020] FIGURE 5 shows a second set of length change data of the cementitious materials described herein when exposed to a sulfate solution. Sulfate exposure was initiated 7-days after cast upon completion of saturated limewater bath cure at 38 °C. Exposure class SI: 0.10% at 6 months. Exposure class S2: 0.05% at 6 months, 0.10% at 12 months if the expansion exceeds the 6-month limit. Exposure class S3: 0.10% at 18 months. Flow of the test mixture was 112%.

[0021] FIGURE 6 shows data from an isothermal conduction calorimetry analysis of the cementitious materials described herein. Testing was conducted at 23 °C for 168 hours using external mixing.

[0022] DETAILED DESCRIPTION OF THE INVENTION

[0023] The compositions and methods described herein provide a cementitious material produced through milling rather than high-temperature processing, thereby consuming far less energy and generating lower carbon emissions than traditional kiln-based routes. This approach to manufacturing enables decomposition and activation of ingredients that are conventionally thermally processed, such as limestone, through mechanical shock rather than heat. The composition described herein comprises calcium and silica compounds that, when subjected to controlled mechanical treatment, develop distinct reactive and structural features characteristic

[0024] 2

[0025] FH 13302371.4NLH-00125 of cementitious binders. The calcium and silica precursors may include CaO and SiO₂ and may be milled individually or together.

[0026] An influential aspect of the production methods described is the sequence of milling. The order in which the constituent compounds are introduced and processed, particularly milling SiO₂ first followed by the addition of CaO, may influence the structure and performance of the resulting material. Although calcium oxide might be expected to dominate process behavior, results indicate that this may not be the case. The mechanical parameters of the milling operation, including mill type and rotational speed, can be selected and adjusted to tune reaction kinetics and particle attributes.

[0027] The disclosed framework accommodates a broad range of calcium- and silica-containing compounds, with exemplary embodiments set forth herein. By manipulating the stiffness ratios of constituent phases, the compositions can be tailored to enhance targeted performance attributes. The compliance and compressibility of the resulting materials arise from the elastic stiffness, bulk modulus, and density of the selected precursors and their mechanically induced transformations. Collectively, these features yield cementitious compositions and processes that achieve desirable strength and durability while significantly reducing energy use and carbon intensity relative to kiln-based cement manufacture.

[0028] In certain aspects, a composition comprises a plurality of X(CaO) particles and a plurality of Y(SiO2) particles, wherein X: Y is from about 0.05 to about 5. In further embodiments, X: Y is about 0.05. In yet further embodiments, X: Y is about 0.10. In yet further embodiments, X: Y is about 0.15. In yet further embodiments, X: Y is about 0.20. In yet further embodiments, X: Y is about 0.25. In yet further embodiments, X: Y is about 0.30. In yet further embodiments, X: Y is about 0.35. In yet further embodiments, X: Y is about 0.40. In yet further embodiments, X: Y is about 0.45. In yet further embodiments, X: Y is about 0.50. In yet further embodiments, X: Y is about 0.55. In yet further embodiments, X: Y is about 0.60. In yet further embodiments, X: Y is about 0.65. In yet further embodiments, X: Y is about 0.70. In yet further embodiments, X: Y is about 0.75. In yet further embodiments, X: Y is about 0.80. In yet further embodiments, X: Y is about 0.85. In yet further embodiments, X: Y is about 0.90. In yet further embodiments, X: Y is about 0.95. In yet further embodiments, X: Y is about 1.00. In yet further embodiments, X: Y is about 1.05. In yet further embodiments, X: Y is about 1.10. In yet further embodiments, X: Y is about 1.15. In yet further embodiments, X: Y is about 1.20. In yet further embodiments, X: Y is about 1.25. In yet further embodiments, X: Y is about 1.30. In yet further embodiments, X: Y is about 1.35. In yet further embodiments, X: Y is about 1.40. In yet further 3

[0029] FH 13302371.4NLH-00125 embodiments, X: Y is about 1.45. In yet further embodiments, X: Y is about 1.50. In yet further embodiments, X: Y is about 1.55. In yet further embodiments, X: Y is about 1.60. In yet further embodiments, X: Y is about 1.65. In yet further embodiments, X:Y is about 1.70. In yet further embodiments, X:Y is about 1.75. In yet further embodiments, X:Y is about 1.80. In yet further embodiments, X:Y is about 1.85. In yet further embodiments, X:Y is about 1.90. In yet further embodiments, X:Y is about 1.95. In yet further embodiments, X:Y is about 2.00. In yet further embodiments, X:Y is about 2.05. In yet further embodiments, X:Y is about 2.10. In yet further embodiments, X:Y is about 2.15. In yet further embodiments, X:Y is about 2.20. In yet further embodiments, X:Y is about 2.25. In yet further embodiments, X:Y is about 2.30. In yet further embodiments, X:Y is about 2.35. In yet further embodiments, X:Y is about 2.40. In yet further embodiments, X:Y is about 2.45. In yet further embodiments, X:Y is about 2.50. In yet further embodiments, X:Y is about 2.55. In yet further embodiments, X:Y is about 2.60. In yet further embodiments, X:Y is about 2.65. In yet further embodiments, X:Y is about 2.70. In yet further embodiments, X:Y is about 2.75. In yet further embodiments, X:Y is about 2.80. In yet further embodiments, X:Y is about 2.85. In yet further embodiments, X:Y is about 2.90. In yet further embodiments, X:Y is about 2.95. In yet further embodiments, X:Y is about 3.00. In yet further embodiments, X:Y is about 3.05. In yet further embodiments, X:Y is about 3.10. In yet further embodiments, X:Y is about 3.15. In yet further embodiments, X:Y is about 3.20. In yet further embodiments, X:Y is about 3.25. In yet further embodiments, X:Y is about 3.30. In yet further embodiments, X:Y is about 3.35. In yet further embodiments, X:Y is about 3.40. In yet further embodiments, X:Y is about 3.45. In yet further embodiments, X:Y is about 3.50. In yet further embodiments, X:Y is about 3.55. In yet further embodiments, X:Y is about 3.60. In yet further embodiments, X:Y is about 3.65. In yet further embodiments, X:Y is about 3.70. In yet further embodiments, X:Y is about 3.75. In yet further embodiments, X:Y is about 3.80. In yet further embodiments, X:Y is about 3.85. In yet further embodiments, X:Y is about 3.90. In yet further embodiments, X:Y is about 3.95. In yet further embodiments, X:Y is about 4.00. In yet further embodiments, X:Y is about 4.05. In yet further embodiments, X:Y is about 4.10. In yet further embodiments, X:Y is about 4.15. In yet further embodiments, X:Y is about 4.20. In yet further embodiments, X:Y is about 4.25. In yet further embodiments, X:Y is about 4.30. In yet further embodiments, X:Y is about 4.35. In yet further embodiments, X:Y is about 4.40. In yet further embodiments, X:Y is about 4.45. In yet further embodiments, X:Y is about 4.50. In yet further embodiments, X:Y is about 4.55. In yet further embodiments, X:Y is about 4.60. In yet further embodiments, X:Y is about 4.65. In yet further embodiments, X:Y is about 4.70. In yet further 4

[0030] FH 13302371.4NLH-00125 embodiments, X:Y is about 4.75. In yet further embodiments, X:Y is about 4.80. In yet further embodiments, X:Y is about 4.85. In yet further embodiments, X:Y is about 4.90. In yet further embodiments, X:Y is about 4.95. In yet further embodiments, X:Y is about 5.00.

[0031] In certain embodiments, X:Y is from about 0.5 to about 4.5. In certain embodiments, X:Y is from about 1.0 to about 4.0. In certain embodiments, X:Y is from about 1.5 to about 3.5. In certain embodiments, X:Y is from about 2.0 to about 3.0.

[0032] In certain embodiments, the composition is cementitious.

[0033] In certain embodiments, the SiO₂ particles have an average particle size from about 10 nm to about 15 microns. In certain embodiments, the SiO₂ particles have an average particle size of about 10 microns. In certain embodiments, the SiO₂ particles have an average particle size of about 11 microns. In certain embodiments, the SiO₂ particles have an average particle size of about 12 microns. In certain embodiments the SiO₂ particles have an average particle size of about 13 microns. In certain embodiments, the SiO₂ particles have an average particle size of about 14 microns. In certain embodiments, the SiO₂ particles have an average particle size of about 15 microns.

[0034] In certain embodiments, the SiO₂ particles have an average particle size of about 100 nm to about 14000 nm. In certain embodiments, the SiO₂ particles have an average particle size of about 1000 nm to about 13000 nm. In certain embodiments, the SiO₂ particles have an average particle size of about 10000 nm to about 12000 nm.

[0035] In certain embodiments, the CaO particles have an average particle size from about 10 nm to about 15 microns. In certain embodiments, the CaO particles have an average particle size of about 10 microns. In further embodiments, the CaO particles have an average particle size of about 11 microns. In further embodiments, the CaO particles have an average particle size of about 12 microns. In further embodiments, the CaO particles have an average particle size of about 13 microns. In further embodiments, the CaO particles have an average particle size of about 14 microns. In further embodiments, the CaO particles have an average particle size of about 15 microns.

[0036] In certain embodiments, the CaO particles have an average particle size of about 100 nm to about 14000 nm. In further embodiments, the CaO particles have an average particle size of about 1000 nm to about 13000 nm. In further embodiments, the CaO particles have an average particle size of about 10000 nm to about 12000 nm.

[0037] In certain embodiments, the SiO2particles have a diameter 50 (D50) of from about 0.5 microns to about 50 microns In certain embodiments, the SiO2 particles have a D50 of about 5

[0038] 5

[0039] FH 13302371.4NLH-00125 microns. In certain embodiments, the SiO₂ particles have a D50 of about 10 microns. In certain embodiments, the SiO₂ particles have a D50 of about 15 microns. In certain embodiments, the SiO₂ particles have a D50 of about 20 microns. In certain embodiments, the SiO₂ particles have a D50 of about 25 microns. In certain embodiments, the SiO₂ particles have a D50 of about 30 microns. In certain embodiments, the SiO₂ particles have a D50 of about 35 microns. In certain embodiments, the SiO₂ particles have a D50 of about 40 microns. In certain embodiments, the SiO₂ particles have a D50 of about 45 microns. In certain embodiments, the SiO₂ particles have a D50 of about 50 microns.

[0040] In certain embodiments, the SiO₂ particles have a D50 of from about 10 microns to about 45 microns. In certain embodiments, the SiO₂ particles have a D50 of about 15 microns to about 40 microns. In certain embodiments, the SiO₂ particles have a D50 of about 20 microns to about 35 microns.

[0041] In certain embodiments, the CaO particles have a diameter 50 (D50) of from about 0.5 microns to about 50 microns. In certain embodiments, the CaO particles have a D50 of about 5 microns. In certain embodiments, the CaO particles have a D50 of about 10 microns. In certain embodiments, the CaO particles have a D50 of about 15 microns. In certain embodiments, the CaO particles have a D50 of about 20 microns. In certain embodiments, the CaO particles have a D50 of about 25 microns. In certain embodiments, the CaO particles have a D50 of about 30 microns. In certain embodiments, the CaO particles have a D50 of about 35 microns. In certain embodiments, the CaO particles have a D50 of about 40 microns. In certain embodiments, the CaO particles have a D50 of about 45 microns. In certain embodiments, the CaO particles have a D50 of about 50 microns.

[0042] In certain embodiments, the CaO particles have a D50 of from about 10 microns to about 45 microns. In certain embodiments, the CaO particles have a D50 of about 15 microns to about 40 microns. In certain embodiments, the CaO particles have a D50 of about 20 microns to about 35 microns.

[0043] In certain embodiments, the plurality of X(CaO) particles and the plurality of Y(SiO2) particles are arranged in a disordered structure. In alternative embodiments, the plurality of X(CaO) particles and the plurality of Y(SiO2) particles are arranged in an ordered structure. In certain embodiments, a composition is amorphous. In alternative embodiments, the composition is crystalline.

[0044] In certain embodiments, the SiO₂ is from a natural source (e.g., sand, such as quartz sand, quartzite, quartz, opal, agate, or granite). In certain embodiments, the SiO₂ is from rocks.

[0045] 6

[0046] FH 13302371.4NLH-00125 In certain embodiments, the SiO₂ is derived from a synthetic source (e.g., pyrogenic silica, precipitated silica, silica gel, colloidal silica, or silica glass). In certain embodiments, the SiO₂ is from fly ash.

[0047] In certain embodiments, the composition has a density from about 1.2 g / cm3to about 5 g / cm3. In certain embodiments, the composition has a density of about 1.2 g / cm3. In certain embodiments, the composition has a density of about 1.5 g / cm3. In certain embodiments, the composition has a density of about 1.8 g / cm3. In certain embodiments, the composition has a density of about 2.0 g / cm3. In certain embodiments, the composition has a density of about 2.2 g / cm3. In certain embodiments, the composition has a density of about 2.5 g / cm3. in certain embodiments, the composition has a density of about 2.8 g / cm3. In certain embodiments, the composition has a density of about 3.0 g / cm3. In certain embodiments, the composition has a density of about 3.2 g / cm3. In certain embodiments, the composition has a density of about 3.5 g / cm3. In certain embodiments, the composition has a density of about 3.8 g / cm3. In certain embodiments, the composition has a density of about 4.0 g / cm3. In certain embodiments, the composition has a density of about 4.2 g / cm3. In certain embodiments, the composition has a density of about 4.5 g / cm3. In certain embodiments, the composition has a density of about 4.8 g / cm3. In certain embodiments, the composition has a density of about 5.0 g / cm3.

[0048] In certain embodiments, the density of the composition is from about 1.5 g / cm3to about 4.5 g / cm3. In certain embodiments, the density of the composition is from about 2.0 g / cm3to about 4.0 g / cm3. In certain embodiments, the density of the composition is from about 2.5 g / cm3to about 3.5 g / cm3.

[0049] In certain embodiments, the composition can form a hydrate. In certain embodiments, the composition can form a hydrate in the presence of an alkaline composition (e.g., a carbonate or hydroxide base).

[0050] In certain preferred embodiments, the composition has a ratio of Ca:Si from about 0.05:1 to about 5:1 by wt%. In certain embodiments, the composition has a ratio of Ca: Si of about 0.25:1 wt%. In certain embodiments, the composition has a ratio of Ca:Si of about 0.5:1 wt%. In certain embodiments, the composition has a ratio of Ca:Si of about 0.75:1 wt%. In certain embodiments, the composition has a ratio of Ca:Si of about 1:1 wt%. In certain embodiments, the composition has a ratio of Ca:Si of about 1.25:1 wt%. In certain embodiments, the composition has a ratio of Ca:Si of about 1.5:1 wt%. In certain embodiments, the composition has a ratio of Ca:Si of about 1.75:1 wt%. In certain embodiments, the composition has a ratio of Ca:Si of about 2:1 wt%. In certain embodiments, the composition 7

[0051] FH 13302371.4NLH-00125 has a ratio of Ca:Si of about 2.25:1 wt%. In certain embodiments, the composition has a ratio of Ca:Si of about 2.5:1 wt%. In certain embodiments, the composition has a ratio of Ca:Si of about 2.75:1 wt%. In certain embodiments, the composition has a ratio of Ca:Si of about 3:1 wt%. In certain embodiments, the composition has a ratio of Ca:Si of about 3.25:1 wt%. In certain embodiments, the composition has a ratio of Ca:Si of about 3.5:1 wt%. In certain embodiments, the composition has a ratio of Ca:Si of about 3.75:1 wt%. In certain embodiments, the composition has a ratio of Ca:Si of about 4:1 wt%. In certain embodiments, the composition has a ratio of Ca:Si of about 4.25:1 wt%. In certain embodiments, the composition has a ratio of Ca:Si of about 4.5:1 wt%. In certain embodiments, the composition has a ratio of Ca:Si of about 4.75:1 wt%. In certain embodiments, the composition has a ratio of Ca: Si of about 5:1 wt%.

[0052] In certain embodiments, the composition has a ratio of Ca: Si from about 0.5:1 to about 4.5:1 by wt%. In certain embodiments, the composition has a ratio of Ca: Si from about 1:1 to about 4: 1 by wt%. In certain embodiments, the composition has a ratio of Ca: Si from about 2: 1 to about 3:1 by wt%.

[0053] In certain preferred embodiments, the composition has a ratio of Ca: Si from about 0.05:1 to about 5:1 by mol%. In certain embodiments, the composition has a ratio of Ca: Si of about 0.25: 1 mol%. In certain embodiments, the composition has a ratio of Ca:Si of about 0.5:1 mol%. In certain embodiments, the composition has a ratio of Ca:Si of about 0.75:1 mol%. In certain embodiments, the composition has a ratio of Ca:Si of about 1:1 mol%. In certain embodiments, the composition has a ratio of Ca:Si of about 1.25:1 mol%. In certain embodiments, the composition has a ratio of Ca:Si of about 1.5:1 mol%. In certain embodiments, the composition has a ratio of Ca:Si of about 1.75:1 mol%. In certain embodiments, the composition has a ratio of Ca: Si of about 2: 1 mol%. In certain embodiments, the composition has a ratio of Ca:Si of about 2.25:1 mol%. In certain embodiments, the composition has a ratio of Ca:Si of about 2.5:1 mol%. In certain embodiments, the composition has a ratio of Ca:Si of about 2.75:1 mol%. In certain embodiments, the composition has a ratio of Ca:Si of about 3:1 mol%. In certain embodiments, the composition has a ratio of Ca: Si of about 3.25: 1 mol%. In certain embodiments, the composition has a ratio of Ca:Si of about 3.5:1 mol%. In certain embodiments, the composition has a ratio of Ca:Si of about 3.75:1 mol%. In certain embodiments, the composition has a ratio of Ca:Si of about 4:1 mol%. In certain embodiments, the composition has a ratio of Ca:Si of about 4.25:1 mol%. In certain embodiments, the composition has a ratio of Ca:Si of about 4.5:1 mol%. In certain 8

[0054] FH 13302371.4NLH-00125 embodiments, the composition has a ratio of Ca:Si of about 4.75:1 mol%. In certain embodiments, the composition has a ratio of Ca: Si of about 5:1 mol%.

[0055] In certain embodiments, the composition has a ratio of Ca: Si from about 0.5:1 to about 4.5:1 by mol%. In certain embodiments, the composition has a ratio of Ca:Si from about 1:1 to about 4:1 by mol%. In certain embodiments, the composition has a ratio of Ca:Si from about 2:1 to about 3:1 by mol%.

[0056] In certain aspects, provided herein is method of preparing a composition comprising a plurality of first CaO particles and a plurality of first SiCb particles, wherein the method comprises:

[0057] in a first milling step, milling a plurality of first SiO2particles in a mill, thereby forming a plurality of first milled SiO2particles;

[0058] contacting the plurality of first milled SiO2particles with a plurality of first CaO particles in the mill, thereby forming a mixture of a plurality of remilled SiO2 particles and a plurality of first milled CaO particles; and

[0059] in a second milling step, milling the mixture of the plurality of remilled SiO2 particles and the plurality of first milled CaO particles, thereby forming the composition comprising the plurality of first CaO particles and the plurality of first SiO2 particles.

[0060] In certain aspects, provided herein is a method comprising:

[0061] 1) in a first milling step, milling a plurality of first particles SiO2 in a mill, thereby forming a plurality of first milled SiO2 particles;

[0062] 2) contacting the plurality of first milled SiO2 particles with a plurality of first CaO particles in the mill, thereby forming a mixture of a plurality of remilled SiO2 particles and a plurality of first milled CaO particles; and

[0063] 3) in a second milling step, milling the mixture of the plurality of remilled SiO2 particles and the plurality of first milled CaO particles, thereby forming the composition comprising the plurality of first CaO particles and the plurality of first SiO2 particles. In certain embodiments, the plurality of first particles of SiO2have an average particle size from about 100 nm to about 10 mm. In certain embodiments, the plurality of first particles of SiO2 have an average particle size from about 1000 nm to about 1 mm.

[0064] In certain embodiments, the plurality of first particles of SiO2 have an average particle size from about 10000 nm to about 0.5 mm.

[0065] 9

[0066] FH 13302371.4NLH-00125 In certain embodiments, the plurality of first particles of CaO have an average particle size from about 100 nm to about 10 mm. In certain embodiments, the plurality of first particles of CaO have an average particle size from about 1000 nm to about 1 mm. In certain embodiments, the plurality of first particles of CaO have an average particle size from about 10000 nm to about 0.5 mm.

[0067] In certain embodiments, the first milling step is performed from about 0.25 hours to about 6 hours. In certain embodiments, the first milling step is performed for from about 1 hour to about 4 hours.

[0068] In certain embodiments, the first milling step and second milling step are performed for a total of less than about 24 hours. In certain embodiments, the first milling step and second milling step are performed for a total of less than about 24 hours. In certain embodiments, the first milling step and second milling step are performed for a total of less than about 23 hours. In certain embodiments, the first milling step and second milling step are performed for a total of less than about 22 hours. In certain embodiments, the first milling step and second milling step are performed for a total of less than about 21 hours. In certain embodiments, the first milling step and second milling step are performed for a total of less than about 20 hours. In certain embodiments, the first milling step and second milling step are performed for a total of less than about 19 hours. In certain embodiments, the first milling step and second milling step are performed for a total of less than about 18 hours. In certain embodiments, the first milling step and second milling step are performed for a total of less than about 16 hours. In certain embodiments, the first milling step and second milling step are performed for a total of less than about 15 hours. In certain embodiments, the first milling step and second milling step are performed for a total of less than about 14 hours. In certain embodiments, the first milling step and second milling step are performed for a total of less than about 13 hours. In certain embodiments, the first milling step and second milling step are performed for a total of less than about 12 hours. In certain embodiments, the first milling step and second milling step are performed for a total of less than about 10 hours. In certain embodiments, the first milling step and second milling step are performed for a total of less than about 9 hours. In certain embodiments, the first milling step and second milling step are performed for a total of less than about 8 hours. In certain embodiments, the first milling step and second milling step are performed for a total of less than about 7 hours. In certain embodiments, the first milling step and second milling step are performed for a total of less than about 6 hours.

[0069] 10

[0070] FH 13302371.4NLH-00125 In certain embodiments, the mill further comprises a grinding media comprising a plurality of spherical particles. In certain preferred embodiments, the plurality of spherical particles have an average radii of less than about 10 cm. In further embodiments, the plurality of spherical particles have an average radii of less than about 9 cm. In yet further embodiments, the plurality of spherical particles have an average radii of less than about 8 cm. In yet other embodiments, the plurality of spherical particles have an average radii of less than about 7 cm. In yet further embodiments, the plurality of spherical particles have an average radii of less than about 6 cm. In yet further embodiments, the plurality of spherical particles have an average radii of less than about 5 cm.

[0071] In certain embodiments, the grinding media is about 10,000 times as large as the CaO and SiCh particles.

[0072] In certain embodiments, a method is performed at ambient temperature. In further embodiments, the method is performed at about 0 °C. In further embodiments, the method is performed at about 5 °C. In further embodiments, the method is performed at about 10 °C. In further embodiments, the method is performed at about 15 °C. In further embodiments, the method is performed at about 20 °C. In further embodiments, the method is performed at about 25 °C. In further embodiments, the method is performed at about 30 °C. In further embodiments, the method is performed at about 35 °C. In further embodiments, the method is performed at about 40 °C. In further embodiments, the method is performed at about 45 °C. In further embodiments, the method is performed at about 50 °C.

[0073] In certain embodiments, the method is performed at about 0 °C to about 50 °C. In certain embodiments, the method is performed at about 10 °C to about 40 °C. In certain embodiments, the method is performed at about 20 °C to about 30 °C.

[0074] In further embodiments, the weight percent of the grinding media in the mill is about 2 wt% as compared to the first SiCb particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 4.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 7 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 9.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 12 wt% as 11

[0075] FH 13302371.4NLH-00125 compared to the first S1O2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 14.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 17 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 19.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 22 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 24.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 27 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 29.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 32 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 34.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 37 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 39.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 42 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 44.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 47 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments,

[0076] 12

[0077] FH 13302371.4NLH-00125 the weight percent of the grinding media in the mill is about 49.5 wt% as compared to the first SiCh particles, the first CaO particles, or the first SiCb particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 52 wt% as compared to the first SiCb particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 54.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 57 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 59.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 62 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 64.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 67 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 69.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 72 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 74.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 77 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 79.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In further embodiments, the weight percent of the grinding media in the mill is about 80 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

[0078] 13

[0079] FH 13302371.4NLH-00125 In certain embodiments, the weight percent of the grinding media in the mill is from about 10 wt% to about 70 wt% as compared to the first SiCh particles, the first CaO particles, or the first SiCb particles and the first CaO particles. In certain embodiments, the weight percent of the grinding media in the mill is from about 20 wt% to about 60 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles. In certain embodiments, the weight percent of the grinding media in the mill is from about 30 wt% to about 50 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

[0080] In certain embodiments, the plurality of spherical particles comprises particles of iron, steel, or zirconia, or a combination thereof.

[0081] In certain embodiments, the density of each sphere in the plurality of spherical particles is from about 3 g / cm3to about 8 g / cm3. In certain embodiments, the density of each sphere in the plurality of spherical particles is about 3 g / cm3. In further embodiments, the density of each sphere in the plurality of spherical particles is about 4 g / cm3. In further embodiments, the density of each sphere in the plurality of spherical particles is about 5 g / cm3. In further embodiments, the density of each sphere in the plurality of spherical particles is about 6 g / cm3. In further embodiments, the density of each sphere in the plurality of spherical particles is about 7 g / cm3. In further embodiments, the density of each sphere in the plurality of spherical particles is about 8 g / cm3.

[0082] In certain embodiments, the density of each sphere in the plurality of spherical particles is from about 4 g / cm3to about 7 g / cm3. In certain embodiments, the density of each sphere in the plurality of spherical particles is from about 5 g / cm3to about 6 g / cm3.

[0083] In certain embodiments, the mill is operated from about 20 RPM to about 20,000 RPM. In further embodiments, the mill is operated at about 20 RPM. In further embodiments, the mill is operated at about 100 RPM. In further embodiments, the mill is operated at about 200 RPM. In further embodiments, the mill is operated at about 300 RPM. In further embodiments, the mill is operated at about 400 RPM. In further embodiments, the mill is operated at about 500 RPM. In further embodiments, the mill is operated at about 1,000 RPM. In further embodiments, the mill is operated at about 2,000 RPM. In further embodiments, the mill is operated at about 3,000 RPM. In further embodiments, the mill is operated at about 4,000 RPM. In further embodiments, the mill is operated at about 5,000 RPM. In further embodiments, the mill is operated at about 6,000 RPM. In further embodiments, the mill is operated at about 7,000 RPM. In further embodiments, the mill is operated at about 8,000 RPM. In further 14

[0084] FH 13302371.4NLH-00125 embodiments, the mill is operated at about 9,000 RPM. In further embodiments, the mill is operated at about 10,000 RPM. In further embodiments, the mill is operated at about 11,000 RPM. In further embodiments, the mill is operated at about 12,000 RPM. In further embodiments, the mill is operated at about 13,000 RPM. In further embodiments, the mill is operated at about 14,000 RPM. In further embodiments, the mill is operated at about 15,000 RPM. In further embodiments, the mill is operated at about 16,000 RPM. In further embodiments, the mill is operated at about 17,000 RPM. In further embodiments, the mill is operated at about 18,000 RPM. In further embodiments, the mill is operated at about 19,000 RPM. In further embodiments, the mill is operated at about 20,000 RPM.

[0085] In certain embodiments, the mill is operated from about 200 RPM to about 2,000 RPM. In further embodiments, the mill is operated from about 500 RPM to about 1,500 RPM. In further embodiments, the mill is operated from about 700 RPM to about 1,200 RPM.

[0086] In certain embodiments, the mill further comprises a grinding aid. In certain embodiments, the grinding aid comprises an amine, a glycol, or a carboxylic acid, or a combination thereof. In further embodiments, wherein the grinding aid is an amine, preferably the amine is diethanol isopropanolamine (DEPIA). In yet further embodiments, the grinding aid is carboxylic acid.

[0087] In certain embodiments, the mill is a planetary ball mill, an attritor ball mill, a vibratory ball mill, a horizontal ball mill, or a grate ball mill. In certain embodiments, the mill is a ball mill.

[0088] In other embodiments, the mill is a jet mill. In yet other embodiments, the mill is a vertical roller mill. In yet other embodiments, the mill is a stirred media mill.

[0089] In certain embodiments, the composition described above is formed by any one of the methods described above.

[0090] In certain embodiments, a construction material is provided comprising a composition of any one of the compositions described above.

[0091] In certain embodiments, a method of making a construction material is provided, comprising contacting any one of the described compositions with water.

[0092] 15

[0093] FH 13302371.4NLH-00125

[0094] ADDITIONAL EMBODIMENTS

[0095] 1. Overview

[0096] As shown in FIGURE 1, embodiments of the cementitious materials disclosed herein comprise particles having (sub-stoichiometric calcium content relative to silicon content. In some embodiments, the cementitious material comprises additives to improve resilience, chemical resistance (e.g., to sulfuric acid, chlorine, etc.), freeze-thaw behavior, coefficient of thermal expansion, mechanical strength, viscosity, slurry stability, and / or other properties of the cementitious material (e.g., before, during, and / or after setting).

[0097] In certain preferred embodiments, the cementitious materials are used to form cements with a compressive strength exceeding, for embodiment, about 5 MPa after about 28 days of curing. However, the cementitious material can additionally or alternatively be used for concrete, mortar, plaster, hydraulic cement, stucco, grout, screeds, insulation, fire protection, acid mine drainage remediation, sealants, agriculture (as a source of calcium and / or silicon), as a food additive, as a phosphate or other runoff trap, for cosmetics, for pharmaceuticals, and / or for other suitable purposes.

[0098] 2. Embodiments

[0099] In certain embodiments, the cementitious materials described herein comprise a calcium silicate with a ratio of calcium to silicon from about 0.1 to about 0.8. In certain embodiments, the cementitious material comprise silica (e.g., up to about 50 wt% silica to 50 wt% calcium silicate). In certain embodiments, the cementitious materials comprise alumina (e.g., the oxide content as measured for instance using XRF can include up to about 10 wt% aluminium oxides relative to calcium silicate, calcium oxide, silica, and / or other oxide species; where the aluminium oxides can include alumina, aluminosilicates, calcium aluminates, calcium alumininosilicates, etc.). In certain such embodiments, the cementitious material is a powder (e.g., comprising particles of calcium silicate). A characteristic size (e.g., D50 size) of the particles can be from about 100 nm to about 100 pm (e.g., about 200 nm, about 500 nm, about 1 pm, about 2 pm, about 5 pm, about 10 pm, about 20 pm, about 50 pm, values or ranges therebetween, etc.). In embodimentcertain preferred embodiments, a surface area of the particles is large (e.g., preferably about 500 m2 / kg, about 1000 m2 / kg, about 2000 m2 / kg, about 4000 m2 / kg, about 5000 m2 / kg, about 10000 m2 / kg, values or ranges therebetween, > about 10000 m2 / kg, etc.).

[0100] 16

[0101] FH 13302371.4NLH-00125 3. Exemplary Technical advantages

[0102] In certain embodiments, the technology and materials disclosed herein result in a lower carbon intensity cement compared to traditional cements. In some embodiments, the reduction in carbon intensity results from using a lower calcium content as the calcium in cement traditionally is produced by calcining limestone (e.g., calcium carbonate) which releases CO2 (concomitantly with producing CaO used to form the cementitious material). By using lower calcium content, less limestone is needed and thus less CO2 is released. In some embodiments, the reduction in carbon intensity results from processes used to produce such a material having a lower energy cost compared to traditional kiln firing at temperatures exceeding about 1000°C to activate the calcium silicate material. For instance, electrolytic processes (such as that described in US Patent Application 17 / 771,197 titled ‘ELECTROCHEMICAL SYNTHESIS OF CEMENTITIOUS COMPOUNDS’ filed 22-APR-2022 which is incorporated in its entirety by this reference) can be used to produce the cementitious material at temperatures closer to room temperature (e.g., at temperatures < about 200°C).

[0103] In certain embodiments, the technology and materials disclosed hereinresult in low calcium content hydraulically active cement. In certain embodiments, the properties of the hydraulically active cement on a crystallinity of the cementitious materials, a grain size of the cementitious materials, a composition (calcium content, ratio of calcium to silicon, presence or absence of residual or additive species, etc.) of the cementitious materials, a surface property of the cementitious material (or materials thereof such as a surface functionalization, surface termination, etc.), and / or other aspects of the cementitious material can modulate the hydraulic activity. In tcertain embodiments, the cementitious material has a compressive strength exceeding about 20 MPa after 7 days of curing. In certain embodiments, the cementitious material has a compressive strength exceeding about 28 MPa after 28 days of curing. In tcertain, the cementitious material has a compressive strength exceeding about 35 MPa after 90 days of curing. In certain embodiments, the cementitious material has a compressive strength exceeding about 5 MPa after 7 days of curing.

[0104] The embodiments set forth above are non-limiting and further advantages may be provided by the technology and materials disclosed herein.

[0105] 4. Cementitious material

[0106] 17

[0107] FH 13302371.4NLH-00125 As shown in FIGURE 1, embodiments of the cementitious materials comprise particles having (e.g., consisting of, composed of, consisting essentially of, composed essentially of, including predominantly, with a majority composition of, including, comprising, etc.) sub stoichiometric calcium content relative to silicon content.

[0108] In certain preferred embodiments, the cementitious materials disclosed herein comprise a calcium silicate. In certain preferred embodiments, the calcium silicate is sub stoichiometric in calcium relative to silicon. In certain preferred embodiments, the stoichiometric ratio of calcium to silicon is from about 0.1 to about 0.8. When the stoichiometric ratio of calcium is less than about 0.1, the resulting cementitious material can have a lower (e.g., less than a target value, insufficient, less than desirable, etc.) compressive strength. Relatedly, higher stoichiometric ratios can result in a high carbon intensity (e.g., CO2 emissions greater than about 1 kg CO2 emitted / kg of cementitious material produced).

[0109] In certain preferred embodiments, the calcium silicate is amorphous or nanocrystalline (e.g., has crystal grains with a characteristic size less than about 100 nm). For example, the calcium silicate can have a grain size from about 0.01 nm to about 100 nm (e.g., about 0.01 nm, about 0.1 nm, about 1 nm, about 10 nm, about 20 nm, about 30 nm, about 40 nm, about 50 nm, about 60 nm, about 70 nm, about 80 nm, about 90 nm, about 100 nm, and / or any value or range therebetween). However, the calcium silicate can have any suitable crystallinity and / or crystal grain size. In certain embodiments, the crystallinity (or lack thereof) can be measured using x-ray diffraction (e.g., based on a linewidth, peak position, etc. in x-ray diffraction scans), x-ray photoelectron spectroscopy, nuclear magnetic resonance spectroscopy, electron diffraction, scanning transmission electron micrographs (STEM), vibrational spectroscopy (e.g., resonant vibration transition frequencies, vibrational transition linewidths, etc. such as Raman, Fourier transform infrared spectroscopy, etc.), and / or other suitable techniques.

[0110] In certain preferred embodiments, The calcium silicate is particulate. A characteristic size (e.g., D50 size, diameter, hydrodynamic radius, Stokes radius, width, length, depth, etc.) of the particles can be from about 100 nm to about 100 pm (e.g., about 200 nm, about 500 nm, about 1 pm, about 2 pm, about 5 pm, about 10 pm, about 20 pm, about 50 pm, values or ranges therebetween, etc.). When particles are less than about 100 nm, forming a slurry of particles (e.g., to form cement) can be difficult (e.g., the viscosity, flow, etc. properties of the slurry can be inadequate for formation of cement, a curing time can be too long, etc.). Similarly, cements formed from cementitious material that includes calcium silicate with characteristic particle size greater than about 100 pm can have inadequate properties (e.g., low compressive strength)

[0111] 18

[0112] FH 13302371.4NLH-00125 from issues with curing, slurry stability, and / or other problems. The characteristic size can be measured using vibrational spectroscopy, x-ray diffraction, direct imaging (e.g., electron beam imaging, neutron imaging, etc.), dynamic light scattering, and / or using other suitable techniques.

[0113] The calcium silicate particles can exhibit a high specific surface area. In certain embodiments, the specific surface area of the calcium silicate particles can be from about 5 m2 / g to about 200 m2 / g (e.g., about 5 m2 / g, about 10 m2 / g, about 20 m2 / g, about 30 m2 / g, about 40 m2 / g, about 50 m2 / g, about 75 m2 / g, about 100 m2 / g, about 125 m2 / g, about 150 m2 / g, about 175 m2 / g, about 200 m2 / g, and / or any value or range therebetween). In certain embodiments, the specific surface area can be from about 200 m2 / g to about 10,000 m2 / kg (e.g., about 500 m2 / kg, about 1,000 m2 / kg, about 2,000 m2 / kg, about 4,000 m2 / kg, about 5,000 m2 / kg, about 7,500 m2 / kg, about 10,000 m2 / kg, and / or any value or range therebetween). In certain embodiments, the specific surface area can exceed about 10,000 m2 / kg. The specific surface area can be measured using Brunauer-Emmett-Teller (BET) nitrogen adsorption, krypton adsorption, water vapor adsorption, or other suitable gas adsorption techniques. A high specific surface area can enhance hydration kinetics, increase chemical reactivity, promote formation of binding phases during curing, and / or enable hydraulic activity even at reduced calcium-to-silicon ratios.

[0114] In certain embodiments, the cementitious material can be formed by mechanically activating a mixture of calcium oxide and silicon oxide. Mechanical activation comprises one or more of agitation, mixing, milling, grinding, attrition, shearing, impact milling, ball milling, planetary milling, vibratory milling, jet milling, stirred media milling, high-energy milling, and / or other suitable solid-state processing techniques. In certain embodiments, calcium oxide and silicon oxide are reacted in the solid state under mechanical energy to form calcium silicate phases. Mechanical activation can induce lattice strain, crystal defects, partial amorphization, increased defect density, and / or metastable bonding configurations within the calcium silicate. These effects can increase reactivity with water, enhance hydration kinetics, and enable formation of hydraulically active binding phases without requiring high-temperature kiln firing. In some embodiments, mechanical activation can occur at temperatures less than about 500°C (e.g., less than about 400°C, about 300°C, about 200°C, about 150°C, about 100°C, about 75°C, about 50°C, room temperature, and / or any value or range therebetween).

[0115] In embodiments where calcium oxide and / or calcium hydroxide and silicon oxide are mechanically reacted, the particle sizes of the calcium oxide and silicon oxide are selected to 19

[0116] FH 13302371.4NLH-00125 promote intimate mixing and efficient solid-state reaction. In some embodiments, the silicon oxide is milled to a characteristic particle size from about 0.1 pm to about 10 pm (e.g., about 0.1 pm, about 0.2 pm, about 0.3 pm, about 0.5 pm, about 0.7 pm, about 1 pm, about 2 pm, about 3 pm, about 5 pm, about 7 pm, about 10 pm, and / or any value or range therebetween). In some embodiments, the calcium oxide is milled to a characteristic particle size from about 0.1 pm to about 20 pm (e.g., about 0.1 pm, about 0.2 pm, about 0.5 pm, about 1 pm, about 2 pm, about 5 pm, about 7 pm, about 10 pm, about 15 pm, about 20 pm, and / or any value or range therebetween). In some embodiments, the calcium oxide and silicon oxide have substantially similar particle sizes prior to mechanical activation. Reducing the particle sizes of both reactants can increase contact area, reduce diffusion length scales, suppress formation of unreacted lime, improve reaction uniformity, and / or enhance formation of amorphous or nanocrystalline calcium silicate phases during mechanical activation.

[0117] In embodiments where the cementitious material is formed from calcium oxide and silicon oxide precursors, the relative amounts of calcium oxide and silicon oxide are selected to yield a desired calcium-to- silicon ratio in the resulting calcium silicate. In certain embodiments, the ratio of calcium oxide to silicon oxide is defined on a molar basis, a mass basis, a weight percent basis, a volume basis, and / or a stoichiometric basis. In some embodiments, the calcium oxide and silicon oxide are combined in relative molar amounts selected to yield a calcium-to-silicon atomic ratio from about 0.1 to about 0.8 (e.g., about 0.1, about 0.15, about 0.2, about 0.25, about 0.3, about 0.35, about 0.4, about 0.45, about 0.5, about 0.6, about 0.7, about 0.8, and / or any value or range therebetween). In certain embodiments, the calcium oxide is from about 5 wt% to about 60 wt% of the combined calcium oxide and silicon oxide (e.g., about 5 wt%, about 10 wt%, about 15 wt%, about 20 wt%, about 25 wt%, about 30 wt%, about 35 wt%, about 40 wt%, about 45 wt%, about 50 wt%, about 55 wt%, about 60 wt%, and / or any value or range therebetween), with the balance being silicon oxide. In some embodiments, the calcium oxide and silicon oxide are combined in non- stoichiometric proportions relative to crystalline calcium silicate phases, such that the resulting calcium silicate is amorphous or nanocrystalline. Selecting the relative amounts of calcium oxide and silicon oxide can control the phase composition, degree of polymerization of silicate units, defect density, surface chemistry, hydraulic reactivity, and / or carbon intensity of the resulting cementitious material.

[0118] In some embodiments, the cementitious material comprises additives and / or dopants to improve resilience, chemical resistance (e.g., to sulfuric acid, chlorine, etc.), freeze-thaw 20

[0119] FH 13302371.4NLH-00125 behavior, coefficient of thermal expansion, mechanical strength, viscosity, slurry stability, curing of (e.g., time to cure), compressive strength of the as cured cement, appearance (e.g., color) of the as cured cement, and / or other properties of the cementitious material (e.g., before, during, and / or after setting or curing). In certain embodiments, the additives, additionally or alternatively, comprise residual materials introduced in the formation of calcium silicate (e.g., silica, lime, calcium carbonate, calcium oxide, calcite, lime, quick lime, slaked lime, calcium hydroxide, silicon, carbon, gypsum, etc.). Exemplary additives include: aluminium oxide, iron oxide, sulfur oxide, magnesium oxide, chromium oxide, manganese oxide, titanium oxide, alkali metals (e.g., lithium, sodium, potassium, rubidium, caesium, etc. typically as an oxide), and / or other suitable oxides (e.g., metal oxides) or other materials. In certain embodiments, set modifiers, retarders (e.g., gypsum, calcium sulfate, lignosulfonates, citric acid, sugar, etc.), and / or accelerators (e.g., calcium chloride, sodium nitrate, sodium thiocyanate, etc.) can be included in the cementitious material (e.g., from about 0.5 to about 10%) to control the setting time. In certain embodiments, aggregates (e.g., sand, gravel, etc.), fillers (e.g., limestone, quartz, fly ash, metakaolin, etc.), fibers (e.g., steel fibers, glass fibers, etc.), plasticizers, and / or any other suitable additive are included in the cementitious material (e.g., to alter its physical properties, etc.).

[0120] In some embodiments, dopants are incorporated in small quantities to modify the chemical or crystalline structure of the cement, improve hydration kinetics, and / or enhance performance properties. Examples of dopants include alkaline oxides (e.g., Na2O, K2O), alkaline earth oxides (e.g., MgO, CaO, SrO), halogens (e.g., F, Cl−, Br−), transition metal oxides (e.g., Fe2O3, TiO2, MnO2), rare earth oxides, or any other suitable dopant. In certain preferred embodiments, the dopants are less than about 1 wt% of the cementitious material. The 1 wt% can refer to a total wt% of additives and / or a wt% of a specific additive (where each additive can contribute up to about 10 wt% each). However in some embodiments, the cementitious material has a composition with a dopant weight percentage greater than about 1 wt%.

[0121] In certain preferred embodiments, the additives and / or dopants are at most about 10 wt% of the cementitious material. The 10 wt% refers to a total wt% of additives or dopants and / or a wt% of a specific additive or dopants (where each additive or dopant contributes up to about 10 wt% each). In other embodiments, the cementitious material includes at most about 10 wt% impurities.

[0122] 21

[0123] FH 13302371.4NLH-00125 However, in some embodiments (particularly but not exclusively when the additives comprise silica or other silicon oxide species such as quartz), the additives are up to about 60 wt% of the cementitious material. In certain embodiments, cementitious materials comprise about 10 wt% aluminium oxide (or related aluminium minerals such as aluminosilicates, calcium aluminates, calcium aluminosilicates, etc.), about 50 wt% silica, and about 40 wt% calcium silicate (e.g., as described above). However, other compositions can be used (up to and including about 100 wt% calcium silicate).

[0124] The additives and / or dopant composition can be determined using x-ray fluorescence, particle-induced X-ray emission, X-ray photoelectron spectroscopy, Auger electron spectroscopy, mass spectrometry, energy-dispersive X-ray spectroscopy, cathodoluminescence, nuclear magnetic resonance spectroscopy, and / or using other suitable technique(s).

[0125] In use, the cementitious material can be mixed with water to initiate hydration and setting. The water- to-cementitious-material ratio can be from about 0.1 to about 1.0 by mass (e.g., about 0.1, about 0.15, about 0.2, about 0.25, about 0.3, about 0.35, about 0.4, about 0.45, about 0.5, about 0.6, about 0.7, about 0.8, about 0.9, about 1.0, and / or any value or range therebetween). Upon contact with water, the amorphous and / or nanocrystalline calcium silicate can undergo hydration through dissolution, surface hydration, and / or precipitation mechanisms to form binding phases (e.g., calcium-silicate-hydrate-like phases). In some embodiments, hydration proceeds without formation of substantial portlandite. In some embodiments, hydration occurs at ambient temperature and pressure. The hydration process can result in progressive densification of the cementitious matrix, development of mechanical strength, reduction of porosity, and / or improved durability over time.

[0126] After initial mixing with water, the cementitious material undergoes setting, which is the transition from a plastic, moldable state to a solid or semi-solid form. Under normal curing conditions, setting and / or curing can occur at ambient temperature and pressure over several hours to days (e.g., about 1 hour, about 2 hours, about 3 hours, about 4 hours, about 5 hours, about 6 hours, about 8 hours, about 10 hours, about 12 hours, about 24 hours, about 2 days, about 3 days, about 4 days, about 5 days, about 10 days, about 14 days, about 28 days, about 90 days, or any value therebetween), depending on the water-to-cementitious-material ratio, particle size, and chemical composition of the cementitious material. During this period, the progressive formation of binding phases, such as calcium-silicate-hydrate-like structures, gradually increases the mechanical strength and reduces porosity. In other embodiments,

[0127] 22

[0128] FH 13302371.4NLH-00125 setting and / or curing can involve maintaining appropriate moisture and temperature conditions to allow continued hydration, densification, and strength development. Conventional curing techniques include maintaining high relative humidity (e.g., above about 80%, above about 90%, above about 95%, above about 99%), covering the material with wet fabrics or plastic sheets, or submerging the material in water to prevent moisture loss. In some embodiments, accelerated curing methods are applied to achieve faster strength development or enhanced early-age performance. Such methods can include elevated temperature curing, such as steam curing (e.g., about 50 to about 90°C) or hot water immersion, autoclaving under pressurized conditions, or exposure to chemical accelerators. Additionally, techniques such as controlled curing chambers, microwave-assisted curing, or induction heating can provide rapid hydration and densification while still allowing the cementitious matrix to develop long-term mechanical properties. However, setting and / or curing can be otherwise performed.

[0129] In certain preferred embodiments, after setting and / or curing, the cementitious material as described above meets or exceeds the mechanical properties of other hydraulic cements (e.g., Portland cement, alite, belite, tricalcium aluminate, brownmillerite, etc.). For instance, after 7 days for setting (i.e., drying after being mixed with water), embodiments of the cementitious material can achieve a compressive strength exceeding about 3 MPa (e.g., about 5 MPa, about 7 MPa, about 8 MPa, about 10 MPa, about 12 MPa, about 15 MPa, about 20 MPa, about 25 MPa, about 28 MPa, about 30 MPa, about 40 MPa, etc.). Similarly, after 28 days for setting, embodiments of the cementitious material can achieve a compressive strength exceeding about 5 MPa (e.g., about 7 MPa, about 9 MPa, about 10 MPa, about 12 MPa, about 15 MPa, about 20 MPa, about 25 MPa, about 28 MPa, about 30 MPa, about 35 MPa, about 40 MPa, about 44 MPa, about 50 MPa, about 52 MPa, about 58 MPa, about 61 MPa, about 65 MPa, about 70 MPa, values or ranges therebetween, etc.). Similarly, after 90 days for setting, embodiments of the cementitious material can achieve a compressive strength exceeding about 7.5 MPa (e.g., about 10 MPa, about 12 MPa, about 15 MPa, about 20 MPa, about 25 MPa, about 28 MPa, about 30 MPa, about 33 MPa, about 35 MPa, about 36 MPa, about 40 MPa, about 44 MPa, about 50 MPa, about 52 MPa, about 58 MPa, about 61 MPa, about 65 MPa, about 70 MPa, about 77 MPa, about 82 MPa, about 85 MPa, about 90 MPa, about 93 MPa, about 96 MPa, about 98 MPa, about 100 MPa, about 110 MPa, values or ranges therebetween, etc.). However, the cementitious material can achieve other suitable compressive strength. For comparison, typical Portland cement concrete sets in approximately 6 hours and develops a compressive strength of about 8 MPa in 24 hours, rises to about 15 MPa at 3 days, about 23 MPa at 1 week,

[0130] 23

[0131] FH 13302371.4NLH-00125 about 35 MPa at 4 weeks, and approximately 41 MPa at 3 months. In this context, the cementitious materials described herein are capable of meeting or exceeding these standard performance benchmarks, demonstrating suitability for applications traditionally served by Portland cement and other conventional hydraulic cements.

[0132] Relatedly, embodiments of the cementitious material achieve comparable or superior chemical stability of cement, freeze-thaw behavior, and / or other suitable properties as compared to Portland cement (or other hydraulic cement). In certain preferred embodiments, cement formed using the cementitious materials described herein have superior stability to sulphate (e.g., sulfuric acid). One hypothesis as to the source of this improved chemical resistance is because of a reduced aluminium content in the cementitious material (as compared to Portland cement); however, other aspects of the cementitious material can additionally or alternatively contribute to or result in the improved chemical stability.

[0133] During and / or after setting and curing, the cementitious material can exhibit different structural states depending on composition, curing conditions, and reaction pathways. In some embodiments the cementitious material remains amorphous or nanocrystalline calcium silicate hydrate (C-S-H). In other embodiments, the hydration reaction results in the formation of partially or fully crystalline calcium silicate hydrate phases, including but not limited to tobermorite-type, xonotlite-type, jennite-type, gyrolite-type, afwillite-type, and / or thaumasite-type structures, depending on curing temperature, moisture availability, and ageing conditions. The relative proportion of crystalline versus amorphous or nanocrystalline phases can vary with factors such as temperature, curing duration, water availability, dopants, and / or additives. In contrast to conventional Portland cement systems, which typically produce significant quantities of calcium hydroxide (Ca(OH)2) during hydration, the cementitious materials described herein can, in some embodiments, form reduced amounts of Ca(OH)2and increased proportions of C-S-H-rich binding phases, consistent with its lower calcium content and mechanically enhanced reactivity. These hydration pathways can contribute to improved chemical stability, reduced susceptibility to acid or sulfate attack, and enhanced long-term durability. However, other hydration reactions and phase assemblages are also possible, and the cementitious material is not limited to any single crystallinity state or reaction mechanism. The hydration reactions can proceed through mechanically enabled or pozzolanic-type reaction pathways, wherein the mechanically activated silica reacts with calcium species to form binding hydrates. These hydration pathways can contribute to improved chemical stability, reduced susceptibility to acid or sulfate attack, and enhanced long-term durability. However,

[0134] 24

[0135] FH 13302371.4NLH-00125 other hydration reactions and phase assemblages are also possible, and the cementitious material is not limited to any single crystallinity state or reaction mechanism.

[0136] In certain embodiments, the cementitious material described herein can alternatively be formed using electrochemical processes (e.g., be formed using an electrolysis cell as described in US Patent Application 17 / 771,197 titled ‘ELECTROCHEMICAL SYNTHESIS OF CEMENTITIOUS COMPOUNDS’ filed 22- APR-2022 which is incorporated in its entirety by this reference). However, thermal chemical approaches (e.g., using flash freezing to form amorphous or nanocrystalline calcium silicate phases), high energy bombardment (e.g., gamma ray bombardment), and / or other processes can be used to achieve similar cementitious materials (e.g., where additives can be added separately).

[0137] 5. Exemplary Embodiments

[0138] Specific Embodiment 1. A cementitious material, comprising: a plurality of calcium silicate particles, wherein the calcium silicate particles have a sub stoichiometric calcium content relative to silicon, a nanocrystalline structure, and a specific surface area from about 1000 m2 / kg to about 10000 m2 / kg.

[0139] Specific Embodiment 2. The cementitious material of Specific Embodiment 1, wherein a calcium-to-silicon atomic ratio is from about 0.1 to about 0.8.

[0140] Specific Embodiment 3. The cementitious material of Specific Embodiment 2, wherein the calcium-to-silicon atomic ratio is from about 0.2 to about 0.75.

[0141] Specific Embodiment 4. The cementitious material of Specific Embodiment 1, wherein the calcium silicate particles have a crystal grain size of less than about 100 nm.

[0142] Specific Embodiment 5. The cementitious material of Specific Embodiment 1, wherein the plurality of calcium silicate particles has a D50 particle size from about 100 nm to about 100 μm.

[0143] Specific Embodiment 6. The cementitious material of Specific Embodiment 1, wherein the cementitious material is hydraulic, wherein after mixing with water and curing for 28 days, the cementitious material exhibits a compressive strength of at least about 5 MPa.

[0144] Specific Embodiment 7. The cementitious material of Specific Embodiment 1, further comprising additives, wherein a total amount of additives present in the cementitious material is from about 0.1 wt% to about 10 wt% of the cementitious material.

[0145] Specific Embodiment 8. The cementitious material of Specific Embodiment 7, wherein the additives comprise gypsum or calcium sulfate.

[0146] 25

[0147] FH 13302371.4NLH-00125 Specific Embodiment 9. The cementitious material of Specific Embodiment 7, wherein the additives comprise one or more metal oxides selected from the group consisting of aluminium oxide, iron oxide, magnesium oxide, sulfur oxide, titanium oxide, chromium oxide, manganese oxide, or alkali metal oxides.

[0148] Specific Embodiment 10. The cementitious material of Specific Embodiment 7, wherein the additives an alkali metal oxide selected from the group consisting of lithium oxide, sodium oxide, potassium oxide, or combinations thereof.

[0149] Specific Embodiment 11. The cementitious material of Specific Embodiment 7, wherein the additives comprise an aluminum-containing compound selected from the group consisting of aluminum oxide, aluminosilicates, calcium aluminates, calcium aluminosilicates, or combinations thereof.

[0150] Specific Embodiment 12. A composite material, comprising: a cementitious material consisting essentially of amorphous calcium silicate with a calcium-to- silicon atomic ratio of less than about 0.75; and a particulate morphology.

[0151] Specific Embodiment 13. The composite material of Specific Embodiment 12, wherein the calcium-to-silicon atomic ratio is from about 0.1 to about 0.75.

[0152] Specific Embodiment 14. The composite material of Specific Embodiment 12, wherein the calcium silicate has a D50 particle size from about 100 nm to about 100 μm.

[0153] Specific Embodiment 15. The composite material of Specific Embodiment 12, further comprising additives, wherein a total amount of additives present in the cementitious material is from about 0.1 wt% to about 10 wt% of the cementitious material.

[0154] Specific Embodiment 16. The composite material of Specific Embodiment 15, wherein the additives comprise an aluminum-containing compound selected from the group consisting of aluminum oxide, aluminosilicates, calcium aluminates, calcium aluminosilicates, or combinations thereof.

[0155] Specific Embodiment 17. The composite material of Specific Embodiment 15, wherein the additives comprise gypsum or calcium sulfate.

[0156] Specific Embodiment 18. The composite material of Specific Embodiment 15, wherein the additives comprise one or more metal oxides selected from the group consisting of aluminium oxide, iron oxide, magnesium oxide, sulfur oxide, titanium oxide, chromium oxide, manganese oxide, or alkali metal oxides.

[0157] 26

[0158] FH 13302371.4NLH-00125 Specific Embodiment 19. The composite material of Specific Embodiment 12, wherein the cementitious material is hydraulic, wherein after mixing with water and curing for 28 days, the cementitious material exhibits a compressive strength of at least about 5 MPa.

[0159] Specific Embodiment 20. The composite material of Specific Embodiment 12, wherein the amorphous calcium silicate has a specific surface area from about 1 m2 / g to about 100 m2 / g.

[0160] Specific Embodiment 21. A mechanically activated calcium silicate with a sub-stoichiometric calcium to silicon atomic ratio.

[0161] Specific Embodiment 22. The mechanically activated calcium silicate of Specific Embodiment 21 with any of the properties of a calcium silicate material of one or more of specific embodiments 1-20.

[0162] Embodiments of the system can include every combination and permutation of the various system components. Components of the preceding system can be used with, in addition to, in lieu of, or otherwise integrated with all or a portion of the systems and / or methods disclosed in the applications mentioned above, each of which are incorporated in their entirety by this reference.

[0163] As used herein, "substantially" or other words of approximation (e.g., “about,” “approximately,” etc.) can be within a predetermined error threshold or tolerance of a metric, component, or other reference (e.g., within 0.001%, 0.01%, 0.1%, 1%, 5%, 10%, 20%, 30% of a reference), or be otherwise interpreted.

[0164] As a person skilled in the art will recognize from the previous detailed description and from the figures and claims, modifications and changes can be made to the preferred embodiments of the invention without departing from the scope of this invention defined in the following claims.

[0165] EXAMPLES

[0166] The invention now being generally described, it will be more readily understood by reference to the following examples which are included merely for purposes of illustration of certain aspects and embodiments of the present invention and are not intended to limit the invention.

[0167] Example 1: Exemplary Preparation of a CaO: SiO2 Compositions

[0168] An exemplary CaO:SiO2was prepared according to the following procedure.

[0169] 27

[0170] FH 13302371.4NLH-00125 First, approximately 500 grams of SiO2particles (typically quartz) having an initial median particle size of approximately ~100 mm were charged into a planetary ball mill equipped with steel milling media. The SiO2particles were milled at a rotational speed of 400 rpm, with an approximate ball to powder ratio of 50, for an approximate period of 300 minutes resulting in SiO2particles having a reduced median particle size of approximately 1 pm.

[0171] Following the first milling step, approximately 140 grams of CaO particles having an initial median particle size of approximately 100 pm were added to the mill containing the milled SiO2particles. The mixture of particles was then milled for approximately 15 minutes to yield an exemplary composition.

[0172] INCORPORATION BY REFERENCE

[0173] All publications and patents mentioned herein are hereby incorporated by reference in their entirety as if each individual publication or patent was specifically and individually indicated to be incorporated by reference. In case of conflict, the present application, including any definitions herein, will control.

[0174] EQUIVALENTS

[0175] While specific embodiments of the subject invention have been discussed, the above specification is illustrative and not restrictive. Many variations of the invention will become apparent to those skilled in the art upon review of this specification and the claims below. The full scope of the invention should be determined by reference to the claims, along with their full scope of equivalents, and the specification, along with such variations.

[0176] 28

[0177] FH 13302371.4

Claims

NLH-00125 We claim:

1. A composition comprising a plurality of X(CaO) particles and a plurality of Y(SiO2) particles, wherein X: Y is from about 0.05 to about 5.

2. The composition of claim 1, wherein X: Y is about 0.05.

3. The composition of claim 1, wherein X: Y is about 0.10.

4. The composition of claim 1, wherein X: Y is about 0.15.

5. The composition of claim 1, wherein X: Y is about 0.20.

6. The composition of claim 1, wherein X: Y is about 0.25.

7. The composition of claim 1, wherein X: Y is about 0.30.

8. The composition of claim 1, wherein X: Y is about 0.35.

9. The composition of claim 1, wherein X: Y is about 0.40.

10. The composition of claim 1, wherein X: Y is about 0.45.

11. The composition of claim 1, wherein X: Y is about 0.50.

12. The composition of claim 1, wherein X: Y is about 0.55.

13. The composition of claim 1, wherein X: Y is about 0.60.

14. The composition of claim 1, wherein X: Y is about 0.65.

15. The composition of claim 1, wherein X: Y is about 0.70.

16. The composition of claim 1, wherein X: Y is about 0.75.29FH 13302371.4NLH-00125 17. The composition of claim 1, wherein X: Y is about 0.80.

18. The composition of claim 1, wherein X: Y is about 0.85.

19. The composition of claim 1, wherein X: Y is about 0.90.

20. The composition of claim 1, wherein X: Y is about 0.95.

21. The composition of claim 1, wherein X: Y is about 1.00.

22. The composition of claim 1, wherein X: Y is about 1.05.

23. The composition of claim 1, wherein X: Y is about 1.10.

24. The composition of claim 1, wherein X: Y is about 1.15.

25. The composition of claim 1, wherein X: Y is about 1.20.

26. The composition of claim 1, wherein X: Y is about 1.25.

27. The composition of claim 1, wherein X: Y is about 1.30.

28. The composition of claim 1, wherein X: Y is about 1.35.

29. The composition of claim 1, wherein X: Y is about 1.40.

30. The composition of claim 1, wherein X: Y is about 1.45.

31. The composition of claim 1, wherein X: Y is about 1.50.

32. The composition of claim 1, wherein X: Y is about 1.55.

33. The composition of claim 1, wherein X: Y is about 1.60.

34. The composition of claim 1, wherein X: Y is about 1.65.30FH 13302371.4NLH-00125 35. The composition of claim 1, wherein X:Y is about 1.70.

36. The composition of claim 1, wherein X:Y is about 1.75.

37. The composition of claim 1, wherein X:Y is about 1.80.

38. The composition of claim 1, wherein X:Y is about 1.85.

39. The composition of claim 1, wherein X:Y is about 1.90.

40. The composition of claim 1, wherein X:Y is about 1.95.

41. The composition of claim 1, wherein X:Y is about 2.00.

42. The composition of claim 1, wherein X:Y is about 2.05.

43. The composition of claim 1, wherein X:Y is about 2.10.

44. The composition of claim 1, wherein X:Y is about 2.15.

45. The composition of claim 1, wherein X:Y is about 2.20.

46. The composition of claim 1, wherein X:Y is about 2.25.

47. The composition of claim 1, wherein X:Y is about 2.30.

48. The composition of claim 1, wherein X:Y is about 2.35.

49. The composition of claim 1, wherein X:Y is about 2.40.

50. The composition of claim 1, wherein X:Y is about 2.45.

51. The composition of claim 1, wherein X:Y is about 2.50.

52. The composition of claim 1, wherein X:Y is about 2.55.31FH 13302371.4NLH-00125 53. The composition of claim 1, wherein X:Y is about 2.60.

54. The composition of claim 1, wherein X:Y is about 2.65.

55. The composition of claim 1, wherein X:Y is about 2.70.

56. The composition of claim 1, wherein X:Y is about 2.75.

57. The composition of claim 1, wherein X:Y is about 2.80.

58. The composition of claim 1, wherein X:Y is about 2.85.

59. The composition of claim 1, wherein X:Y is about 2.90.

60. The composition of claim 1, wherein X:Y is about 2.95.

61. The composition of claim 1, wherein X:Y is about 3.00.

62. The composition of claim 1, wherein X:Y is about 3.05.

63. The composition of claim 1, wherein X:Y is about 3.10.

64. The composition of claim 1, wherein X:Y is about 3.15.

65. The composition of claim 1, wherein X:Y is about 3.20.

66. The composition of claim 1, wherein X:Y is about 3.25.

67. The composition of claim 1, wherein X:Y is about 3.30.

68. The composition of claim 1, wherein X:Y is about 3.35.

69. The composition of claim 1, wherein X:Y is about 3.40.

70. The composition of claim 1, wherein X:Y is about 3.45.32FH 13302371.4NLH-00125 71. The composition of claim 1, wherein X:Y is about 3.50.

72. The composition of claim 1, wherein X:Y is about 3.55.

73. The composition of claim 1, wherein X:Y is about 3.60.

74. The composition of claim 1, wherein X:Y is about 3.65.

75. The composition of claim 1, wherein X:Y is about 3.70.

76. The composition of claim 1, wherein X:Y is about 3.75.

77. The composition of claim 1, wherein X:Y is about 3.80.

78. The composition of claim 1, wherein X:Y is about 3.85.

79. The composition of claim 1, wherein X:Y is about 3.90.

80. The composition of claim 1, wherein X:Y is about 3.95.

81. The composition of claim 1, wherein X:Y is about 4.00.

82. The composition of claim 1, wherein X:Y is about 4.05.

83. The composition of claim 1, wherein X:Y is about 4.10.

84. The composition of claim 1, wherein X:Y is about 4.15.

85. The composition of claim 1, wherein X:Y is about 4.20.

86. The composition of claim 1, wherein X:Y is about 4.25.

87. The composition of claim 1, wherein X:Y is about 4.30.

88. The composition of claim 1, wherein X:Y is about 4.35.33FH 13302371.4NLH-00125 89. The composition of claim 1, wherein X:Y is about 4.40.

90. The composition of claim 1, wherein X:Y is about 4.45.

91. The composition of claim 1, wherein X:Y is about 4.50.

92. The composition of claim 1, wherein X:Y is about 4.55.

93. The composition of claim 1, wherein X:Y is about 4.60.

94. The composition of claim 1, wherein X:Y is about 4.65.

95. The composition of claim 1, wherein X:Y is about 4.70.

96. The composition of claim 1, wherein X:Y is about 4.75.

97. The composition of claim 1, wherein X:Y is about 4.80.

98. The composition of claim 1, wherein X:Y is about 4.85.

99. The composition of claim 1, wherein X:Y is about 4.90.

100. The composition of claim 1, wherein X:Y is about 4.95.

101. The composition of claim 1, wherein X:Y is about 5.00.

102. The composition of claim 1, wherein X:Y is from about 0.5 to about 4.5.

103. The composition of claim 1, wherein X:Y is from about 1.0 to about 4.0.

104. The composition of claim 1, wherein X:Y is from about 1.5 to about 3.5.

105. The composition of claim 1, wherein X:Y is from about 2.0 to about 3.0.

106. The composition of any one of claims 1-105 wherein the composition is cementitious.34FH 13302371.4NLH-00125 107. The composition of any one of claims 1-106, wherein the SiO2particles have an average particle size from about 10 nm to about 15 microns.

108. The composition of any one of claims 1-107, wherein the SiO2particles have an average particle size of about 10 microns.

109. The composition of any one of claims 1-107, wherein the SiO2particles have an average particle size of about 11 microns.

110. The composition of any one of claims 1-107, wherein the SiO2particles have an average particle size of about 12 microns.

111. The composition of any one of claims 1-107, wherein the SiO2particles have an average particle size of about 13 microns.

112. The composition of any one of claims 1-107, wherein the SiO2particles have an average particle size of about 14 microns.

113. The composition of any one of claims 1-107, wherein the SiO2particles have an average particle size of about 15 microns.

114. The composition of any one of claims 1-107, wherein the SiO2particles have an average particle size of about 100 nm to about 14000 nm.

115. The composition of any one of claims 1-107, wherein the SiO2particles have an average particle size of about 1000 nm to about 13000 nm.

116. The composition of any one of claims 1-107, wherein the SiO2particles have an average particle size of about 10000 nm to about 12000 nm.

117. The composition of any one of claims 1-116, wherein the CaO particles have an average particle size from about 10 nm to about 15 microns.35FH 13302371.4NLH-00125 118. The composition of any one of claims 1-117, wherein the CaO particles have an average particle size of about 10 microns.

119. The composition of any one of claims 1-117, wherein the CaO particles have an average particle size of about 11 microns.

120. The composition of any one of claims 1-117, wherein the CaO particles have an average particle size of about 12 microns.

121. The composition of any one of claims 1-117, wherein the CaO particles have an average particle size of about 13 microns.

122. The composition of any one of claims 1-117, wherein the CaO particles have an average particle size of about 14 microns.

123. The composition of any one of claims 1-117, wherein the CaO particles have an average particle size of about 15 microns.

124. The composition of any one of claims 1-117, wherein the CaO particles have an average particle size of about 100 nm to about 14 pm.

125. The composition of any one of claims 1-117, wherein the CaO particles have an average particle size of about 1 pm to about 13 pm.

126. The composition of any one of claims 1-117, wherein the CaO particles have an average particle size of about 10 pm to about 12 pm.

127. The composition of any one of claims 1-126, wherein the SiO2particles have a diameter 50 (D50) of from about 0.5 microns to about 50 microns.

128. The composition of any one of claims 1-127, wherein the SiO2particles have a D50 of about 0.5 microns.36FH 13302371.4NLH-00125 129. The composition of any one of claims -127, wherein the SiO2particles have a D50 of about 5 microns.

130. The composition of any one of claims 1-127, wherein the SiO2particles have a D50 of about 10 microns.

131. The composition of any one of claims 1-127, wherein the SiO2particles have a D50 of about 15 microns.

132. The composition of any one of claims 1-127, wherein the SiO2particles have a D50 of about 20 microns.

133. The composition of any one of claims 1-127, wherein the SiO2particles have a D50 of about 25 microns.

134. The composition of any one of claims 1-127, wherein the SiO2particles have a D50 of about 30 microns.

135. The composition of any one of claims 1-127, wherein the SiO2particles have a D50 of about 35 microns.

136. The composition of any one of claims 1-127, wherein the SiO2particles have a D50 of about 40 microns.

137. The composition of any one of claims 1-127, wherein the SiO2particles have a D50 of about 45 microns.

138. The composition of any one of claims 1-127, wherein the SiO2particles have a D50 of about 50 microns.

139. The composition of any one of claims 1-127, wherein the SiO2particles have a D50 of from about 10 microns to about 45 microns.37FH 13302371.4NLH-00125 140. The composition of any one of claims 1-127, wherein the SiO2particles have a D50 of about 15 microns to about 40 microns.

141. The composition of any one of claims 1-127, wherein the SiO2particles have a D50 of about 20 microns to about 35 microns.

142. The composition of any one of claims 1-141, wherein the CaO particles have a diameter 50 (D50) of from about 0.5 microns to about 50 microns.

143. The composition of any one of claims 1-142, wherein the CaO particles have a D50 of about 0.5 microns.

144. The composition of any one of claims 1-142, wherein the CaO particles have a D50 of about 5 microns.

145. The composition of any one of claims 1-142, wherein the CaO particles have a D50 of about 10 microns.

146. The composition of any one of claims 1-142, wherein the CaO particles have a D50 of about 15 microns.

147. The composition of any one of claims 1-142, wherein the CaO particles have a D50 of about 20 microns.

148. The composition of any one of claims 1-142, wherein the CaO particles have a D50 of about 25 microns.

149. The composition of any one of claims 1-142, wherein the CaO particles have a D50 of about 30 microns.

150. The composition of any one of claims 1-142, wherein the CaO particles have a diameter 50 (D50) of about 35 microns.38FH 13302371.4NLH-00125 151. The composition of any one of claims 1-142, wherein the CaO particles have a D50 of about 40 microns.

152. The composition of any one of claims 1-142, wherein the CaO particles have a D50 of about 45 microns.

153. The composition of any one of claims 1-142, wherein the CaO particles have a D50 of about 50 microns.

154. The composition of any one of claims 1-142, wherein the CaO particles have a D50 of from about 10 microns to about 45 microns.

155. The composition of any one of claims 1-142, wherein the CaO particles have a D50 of about 15 microns to about 40 microns.

156. The composition of any one of claims 1-142, wherein the CaO particles have a D50 of about 20 microns to about 35 microns.

157. The composition of any one of claims 1-156, wherein the plurality of X(CaO) particles and the plurality of Y (SiO2) particles are arranged in a disordered structure.

158. The composition of any one of claims 1-156, wherein the plurality of X(CaO) particles and the plurality of Y (SiO2) particles are arranged in an ordered structure.

159. The composition of any one of claims 1-156, wherein the composition is amorphous.

160. The composition of any one of claims 1-156, wherein the composition is crystalline.

161. The composition of any one of claims 1-160, wherein the SiO2is from a natural source (e.g., sand, such as quartz sand, quartzite, quartz, opal, agate, or granite).

162. The composition of any one of claims 1-160, wherein the SiO2is from a synthetic source (e.g., pyrogenic silica, precipitated silica, silica gel, colloidal silica, or silica glass).39FH 13302371.4NLH-00125 163. The composition of any one of claims 1 -160, wherein the SiO2is from rocks.

164. The composition of any one of claims 1 -160, wherein the SiO2is from fly ash.

165. The composition of any one of claims 1 -164, wherein the density of the composition is from about 1.2 g / cm3to about 5 g / cm3.

166. The composition of any one of claims 1 -166, wherein the density of the composition is about 1.2 g / cm3.

167. The composition of any one of claims 1 -166, wherein the density of the composition is about 1.5 g / cm3.

168. The composition of any one of claims 1 -166, wherein the density of the composition is about 1.8 g / cm3.

169. The composition of any one of claims 1 -166, wherein the density of the composition is about 2.0 g / cm3.

170. The composition of any one of claims 1 -166, wherein the density of the composition is about 2.2 g / cm3.

171. The composition of any one of claims 1 -166, wherein the density of the composition is about 2.5 g / cm3.

172. The composition of any one of claims 1 -166, wherein the density of the composition is about 2.8 g / cm3.

173. The composition of any one of claims 1 -166, wherein the density of the composition is about 3.0 g / cm3.

174. The composition of any one of claims 1 -166, wherein the density of the composition is about 3.2 g / cm3.40FH 13302371.4NLH-00125 175. The composition of any one of claims 1-166, wherein the density of the composition is about 3.5 g / cm3.

176. The composition of any one of claims 1-166, wherein the density of the composition is about 3.8 g / cm3.

177. The composition of any one of claims 1-166, wherein the density of the composition is about 4.0 g / cm3.

178. The composition of any one of claims 1-166, wherein the density of the composition is about 4.2 g / cm3.

179. The composition of any one of claims 1-166, wherein the density of the composition is about 4.5 g / cm3.

180. The composition of any one of claims 1-166, wherein the density of the composition is about 4.8 g / cm3.

181. The composition of any one of claims 1-166, wherein the density of the composition is about 5.0 g / cm3.

182. The composition of any one of claims 1-166, wherein the density of the composition is from about 1.5 g / cm3to about 4.5 g / cm3.

183. The composition of any one of claims 1-166, wherein the density of the composition is from about 2.0 g / cm3to about 4.0 g / cm3.

184. The composition of any one of claims 1-166, wherein the density of the composition is from about 2.5 g / cm3to about 3.5 g / cm3.

185. The composition of any one of claims 1-184, wherein the composition can form a hydrate.41FH 13302371.4NLH-00125 186. The composition of any one of claims 1-184, wherein the composition can form a hydrate in the presence of an alkaline composition (e.g., a carbonate or hydroxide base).

187. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si from about 0.05:1 to about 5:1 by wt%.

188. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 0.25:1 by wt%.

189. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 0.5:1 wt%.

190. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 0.75:1 wt%.

191. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 1:1 wt%.

192. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 1.25:1 wt%.

193. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 1.5:1 wt%.

194. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 1.75:1 wt%.

195. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 2:1 wt%.

196. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 2.25:1 wt%.42FH 13302371.4NLH-00125 197. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 2.5:1 wt%.

198. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 2.75:1 wt%.

199. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 3:1 wt%.

200. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 3.25:1 wt%.

201. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 3.5:1 wt%.

202. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 3.75:1 wt%.

203. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 4:1 wt%.

204. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 4.25:1 wt%.

205. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 4.5:1 wt%.

206. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 4.75:1 wt%.

207. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 5:1 wt%.

208. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si from about 0.5:1 to about 4.5:1 by wt%.43FH 13302371.4NLH-00125 208. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si from about 1:1 to about 4:1 by wt%.

209. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si from about 2:1 to about 3:1 by wt%.

210. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si from about 0.05:1 to about 5:1 by mol%.

211. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 0.25:1 by mol%.

211. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 0.5:1 mol%.

212. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 0.75:1 mol%.

213. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 1:1 mol%.

214. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 1.25:1 mol%.

215. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 1.5:1 mol%.

216. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 1.75:1 mol%.

217. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 2:1 mol%.

218. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 2.25:1 mol%.44FH 13302371.4NLH-00125 219. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 2.5:1 mol%.

220. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 2.75:1 mol%.

221. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 3:1 mol%.

222. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 3.25:1 mol%.

223. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 3.5:1 mol%.

224. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 3.75:1 mol%.

225. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 4:1 mol%.

226. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 4.25:1 mol%.

227. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 4.5:1 mol%.

228. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 4.75:1 mol%.

229. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si of about 5:1 mol%.

230. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si from about 0.5:1 to about 4.5:1 by mol%.45FH 13302371.4NLH-00125 230. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si from about 1:1 to about 4:1 by mol%.

231. The composition of any one of claims 1-186, wherein the composition has a ratio of Ca:Si from about 2:1 to about 3:1 by mol%.

232. A method of preparing a composition comprising a plurality of first CaO particles and a plurality of first SiCb particles, wherein the method comprises:in a first milling step, milling a plurality of first SiO2particles in a mill, thereby forming a plurality of first milled SiO2particles;contacting the plurality of first milled SiO2particles with a plurality of first CaO particles in the mill, thereby forming a mixture of a plurality of remilled SiO2 particles and a plurality of first milled CaO particles; andin a second milling step, milling the mixture of the plurality of remilled SiO2 particles and the plurality of first milled CaO particles, thereby forming the composition comprising the plurality of first CaO particles and the plurality of first SiO2 particles.

233. The method of claim 232 comprising:1) in a first milling step, milling a plurality of first SiO2 particles in a mill, thereby forming a plurality of first milled SiO2 particles;2) contacting the plurality of first milled SiO2 particles with a plurality of first CaO particles in the mill, thereby forming a mixture of a plurality of remilled SiO2 particles and a plurality of first milled CaO particles; and3) in a second milling step, milling the mixture of the plurality of remilled SiO2 particles and the plurality of first milled CaO particles, thereby forming the composition comprising the plurality of first CaO particles and the plurality of first SiO2 particles.

234. The method of claim 232 or 233, wherein the composition is a composition of any one of claims 1-231.

235. The method of any one of claims 232-234, wherein the plurality of first particles of SiO2have an average particle size from about 100 nm to about 10 mm.46FH 13302371.4NLH-00125 236. The method of any one of claims 232-235, wherein the plurality of first particles of SiO2have an average particle size from about 1000 nm to about 1 mm.

237. The method of any one of claims 232-235, wherein the plurality of first particles of SiO2have an average particle size from about 10000 nm to about 0.5 mm.

238. The method of any one of claims 232-237, wherein the plurality of first particles of CaO have an average particle size from about 100 nm to about 10 mm.

239. The method of any one of claims 232-237, wherein the plurality of first particles of CaO have an average particle size from about 1000 nm to about 1 mm.

240. The method of any one of claims 232-237, wherein the plurality of first particles of CaO have an average particle size from about 10000 nm to about 0.5 mm.

241. The method of any one of claims 232-240, wherein the first milling step is performed from about 0.25 hours to about 6 hours.

242. The method of any one of claims 232-241, wherein the first milling step is performed from about 1 hour to about 4 hours.

243. The method of any one of claims 232-242, wherein the first milling step and second milling step are performed for a total of less than about 24 hours.

244. The method of any one of claims 232-243, wherein the first milling step and second milling step are performed for a total of less than about 23 hours.

245. The method of any one of claims 232-243, wherein the first milling step and second milling step are performed for a total of less than about 22 hours.

246. The method of any one of claims 232-243, wherein the first milling step and second milling step are performed for a total of less than about 21 hours.47FH 13302371.4NLH-00125 247. The method of any one of claims 232-243, wherein the first milling step and second milling step are performed for a total of less than about 20 hours.

248. The method of any one of claims 232-243, wherein the first milling step and second milling step are performed for a total of less than about 19 hours.

249. The method of any one of claims 232-243, wherein the first milling step and second milling step are performed for a total of less than about 18 hours.

250. The method of any one of claims 232-243, wherein the first milling step and second milling step are performed for a total of less than about 16 hours.

251. The method of any one of claims 232-243, wherein the first milling step and second milling step are performed for a total of less than about 15 hours.

252. The method of any one of claims 232-243, wherein the first milling step and second milling step are performed for a total of less than about 14 hours.

253. The method of any one of claims 232-243, wherein the first milling step and second milling step are performed for a total of less than about 13 hours.

254. The method of any one of claims 232-243, wherein the first milling step and second milling step are performed for a total of less than about 12 hours.

255. The method of any one of claims 232-243, wherein the first milling step and second milling step are performed for a total of less than about 10 hours.

256. The method of any one of claims 232-243, wherein the first milling step and second milling step are performed for a total of less than about 9 hours.

257. The method of any one of claims 232-243, wherein the first milling step and second milling step are performed for a total of less than about 8 hours.48FH 13302371.4NLH-00125 258. The method of any one of claims 232-243, wherein the first milling step and second milling step are performed for a total of less than about 7 hours.

259. The method of any one of claims 232-243, wherein the first milling step and second milling step are performed for a total of less than about 6 hours.

260. The method of any one of claims 232-259, wherein the mill further comprises a grinding media comprising a plurality of spherical particles.

261. The method of any one of claims 232-260, wherein the plurality of spherical particles have an average radii of about less than 10 cm.

262. The method of any one of claims 232-261, wherein the plurality of spherical particles have an average radii of less than about 9 cm.

263. The method of any one of claims 232-261, wherein the plurality of spherical particles have an average radii of less than about 8 cm.

264. The method of any one of claims 232-261, wherein the plurality of spherical particles have an average radii of less than about 7 cm.

265. The method of any one of claims 232-261, wherein the plurality of spherical particles have an average radii of less than about 6 cm.

266. The method of any one of claims 232-261, wherein the plurality of spherical particles have an average radii of less than about 5 cm.

267. The method of any one of claims 232-266, wherein the grinding media is about 10,000 times as large as the CaO and SiO2particles.

268. The method of any one of claims 232-267, wherein the method is performed at ambient temperature.49FH 13302371.4NLH-00125 269. The method of any one of claims 232-267, wherein the method is performed at about 0 °C to about 50 °C.

270. The method of any one of claims 232-267, wherein the method is performed at about 10 °C to about 40 °C.

271. The method of any one of claims 232-267, wherein the method is performed at about 20 °C to about 30 °C.

272. The method of any one of claims 232-267, wherein the method is performed at about 0 °C.

273. The method of any one of claims 232-267, wherein the method is performed at about 5 °C.

274. The method of any one of claims 232-267, wherein the method is performed at about 10 °C.

275. The method of any one of claims 232-267, wherein the method is performed at about 15 °C.

276. The method of any one of claims 232-267, wherein the method is performed at about 20 °C.

277. The method of any one of claims 232-267, wherein the method is performed at about 25 °C.

278. The method of any one of claims 232-267, wherein the method is performed at about 30279. The method of any one of claims 232-267, wherein the method is performed at about 3550FH 13302371.4NLH-00125 280. The method of any one of claims 232-267, wherein the method is performed at about 40281. The method of any one of claims 232-267, wherein the method is performed at about 45 °C.

282. The method of any one of claims 232-267, wherein the method is performed at about 50 °C.

283. The method of any one of claims 232-282, wherein the weight percent of the grinding media in the mill is from about 2 wt% to about 80 wt% as compared to the first SiCh particles, the first CaO particles, or the first SiCb particles and the first CaO particles.

284. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is from about 10 wt% to about 70 wt% as compared to the first SiCh particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

285. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is from about 20 wt% to about 60 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

286. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is from about 30 wt% to about 50 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

287. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 2 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

288. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 4.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.51FH 13302371.4NLH-00125 289. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 7 wt% as compared to the first SiCb particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

290. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 9.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

291. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 12 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

292. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 14.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

293. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 17 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

294. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 19.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

295. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 22 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

296. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 24.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.52FH 13302371.4NLH-00125 297. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 27 wt% as compared to the first SiCb particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

298. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill about 29.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

299. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 32 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

300. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 34.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

301. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 37 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

302. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 39.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

303. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 42 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

304. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 44.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.53FH 13302371.4NLH-00125 305. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill about 47 wt% as compared to the first SiCb particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

306. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 49.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

307. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 52 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

308. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 54.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

309. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 57 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

310. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 59.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

311. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 62 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

312. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 64.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.54FH 13302371.4NLH-00125 313. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 67 wt% as compared to the first SiCb particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

314. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 69.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

315. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 72 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

316. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 74.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

317. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 77 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

318. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 79.5 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

319. The method of any one of claims 232-283, wherein the weight percent of the grinding media in the mill is about 80 wt% as compared to the first SiO2 particles, the first CaO particles, or the first SiO2 particles and the first CaO particles.

320. The method of any one of claims 232-319, wherein the plurality of spherical particles comprises particles of iron, steel, or zirconia, or a combination thereof.

321. The method of any one of claims 232-320, wherein the density of each sphere in the plurality of spherical particles is from about 3 g / cm3to about 8 g / cm3.55FH 13302371.4NLH-00125 322. The method of any one of claims 232-321, wherein the density of each sphere in the plurality of spherical particles is from about 4 g / cm3to about 7 g / cm3.

323. The method of any one of claims 232-321, wherein the density of each sphere in the plurality of spherical particles is from about 5 g / cm3to about 6 g / cm3.

324. The method of any one of claims 232-321, wherein the density of each sphere in the plurality of spherical particles is from about 3 g / cm3.

325. The method of any one of claims 232-321, wherein the density of each sphere in the plurality of spherical particles is about 4 g / cm3.

326. The method of any one of claims 232-321, wherein the density of each sphere in the plurality of spherical particles is about 5 g / cm3.

327. The method of any one of claims 232-321, wherein the density of each sphere in the plurality of spherical particles is about 6 g / cm3.

328. The method of any one of claims 232-321, wherein the density of each sphere in the plurality of spherical particles is about 7 g / cm3.

329. The method of any one of claims 232-321, wherein the density of each sphere in the plurality of spherical particles is about 8 g / cm3.

330. The method of any one of claims 232-329, wherein the mill is operated from about 20 RPM to about 20,000 RPM.

331. The method of any one of claims 232-330, wherein the mill is operated from about 200 RPM to about 2,000 RPM.

332. The method of any one of claims 232-331, wherein the mill is operated from about 500 RPM to about 1,500 RPM.56FH 13302371.4NLH-00125 333. The method of any one of claims 232-331, wherein the mill is operated from about 700 RPM to about 1,200 RPM.

334. The method of any one of claims 232-331, wherein the mill is operated at about 20 RPM.

335. The method of any one of claims 232-331, wherein the mill is operated at about 100 RPM.

336. The method of any one of claims 232-331, wherein the mill is operated at about 200 RPM.

337. The method of any one of claims 232-331, wherein the mill is operated at about 300 RPM.

338. The method of any one of claims 232-331, wherein the mill is operated at about 400 RPM.

339. The method of any one of claims 232-331, wherein the mill is operated at about 500 RPM.

340. The method of any one of claims 232-331, wherein the mill is operated at about 1,000 RPM.

341. The method of any one of claims 232-331, wherein the mill is operated at about 2,000 RPM.

342. The method of any one of claims 232-331, wherein the mill is operated at about 3,000 RPM.

343. The method of any one of claims 232-331, wherein the mill is operated at about 4,000 RPM.57FH 13302371.4NLH-00125 344. The method of any one of claims 232-331, wherein the mill is operated at about 5,000 RPM.

345. The method of any one of claims 232-331, wherein the mill is operated at about 6,000 RPM.

346. The method of any one of claims 232-331, wherein the mill is operated at about 7,000 RPM.

347. The method of any one of claims 232-331, wherein the mill is operated at about 8,000 RPM.

348. The method of any one of claims 232-331, wherein the mill is operated at about 9,000 RPM.

349. The method of any one of claims 232-331, wherein the mill is operated at about 10,000 RPM.

350. The method of any one of claims 232-331, wherein the mill is operated at about 11,000 RPM.

351. The method of any one of claims 232-331, wherein the mill is operated at about 12,000 RPM.

352. The method of any one of claims 232-331, wherein the mill is operated at about 13,000 RPM.

353. The method of any one of claims 232-331, wherein the mill is operated at about 14,000 RPM.

354. The method of any one of claims 232-331, wherein the mill is operated at about 15,000 RPM.58FH 13302371.4NLH-00125 355. The method of any one of claims 232-331, wherein the mill is operated at about 16,000 RPM.

356. The method of any one of claims 232-331, wherein the mill is operated at about 17,000 RPM.

357. The method of any one of claims 232-331, wherein the mill is operated at about 18,000 RPM.

358. The method of any one of claims 232-331, wherein the mill is operated at about 19,000 RPM.

359. The method of any one of claims 232-331, wherein the mill is operated at about 20,000 RPM.

360. The method of any one of claims 232-359, wherein the mill is a planetary ball mill, an attritor ball mill, a vibratory ball mill, a horizontal ball mill, or a grate ball mill.

361. The method of any one of claims 323-360, wherein the mill further comprises a grinding aid.

362. The method of any one of claims 232-361, wherein the grinding aid comprises an amine, a glycol, or a carboxylic acid, or a combination thereof.

363. The method of claim 362, wherein the grinding aid is an amine, preferably the amine is diethanol isopropanolamine (DEPIA).

364. The method of claim 362, wherein the grinding aid is carboxylic acid.

365. The method of claim 360, wherein the mill is a ball mill.

366. The method of claim 360, wherein the mill is a jet mill.

367. A composition formed by the method of any one of claims 232-366.59FH 13302371.4NLH-00125 368. A construction material comprising the composition of any one of claims 1-231 and 367.

369. A method of making a construction material comprising contacting the composition of any one of claims 1-231 and 367 with water.

370. A cementitious material, comprising:a plurality of calcium silicate particles, wherein the calcium silicate particles have asub stoichiometric calcium content relative to silicon, a nanocrystalline structure, and a specific surface area between 1000 m2 / kg and 10000 m2 / kg.

371. The cementitious material of Claim 370, wherein a calcium-to-silicon atomic ratio is from about 0.1 to about 0.8.

372. The cementitious material of Claim 370, wherein the calcium-to-silicon atomic ratio is from about 0.2 to about 0.75.

373. The cementitious material of Claim 370, wherein the calcium silicate particles have a crystal grain size of less than 50 nm.

374. The cementitious material of Claim 370, wherein the plurality of calcium silicate particles has a D50 particle size from about 100 nm to about 100 pm.

375. The cementitious material of Claim 370, wherein the cementitious material is hydraulic, wherein after curing for 28 days, the cementitious material exhibits a compressive strength of at least 5 MPa.

376. The cementitious material of Claim 370, further comprising additives, wherein a total amount of additives present in the cementitious material is from about 0.1 wt% to about 10 wt% of the cementitious material.

377. The cementitious material of Claim 376, wherein the additives comprise gypsum or calcium sulfate.60FH 13302371.4NLH-00125 378. The cementitious material of Claim 376, wherein the additives comprise one or more metal oxides selected from the group consisting of aluminium oxide, iron oxide, magnesium oxide, sulfur oxide, titanium oxide, chromium oxide, manganese oxide, or alkali metal oxides.

379. The cementitious material of Claim 376, wherein the additives comprise one or more alkali metal oxide selected from the group consisting of lithium oxide, sodium oxide, potassium oxide, or combinations thereof.

380. The cementitious material of Claim 376, wherein the additives comprise an aluminium-containing compound selected from the group consisting of aluminium oxide, aluminosilicates, calcium aluminates, calcium aluminosilicates, or combinations thereof.

381. A composite material, comprising a cementitious material consisting essentially of amorphous calcium silicate with a calcium-to-silicon atomic ratio of less than 0.75 and a particulate morphology.

382. The composite material of Claim 381, wherein the calcium-to-silicon atomic ratio is from about 0.1 to about 0.75.

383. The composite material of Claim 381, wherein the calcium silicate has a D50 particle size from about 100 nm to about 100 pm.

384. The composite material of Claim 381, further comprising additives, wherein a total amount of additives present in the cementitious material is from about 0.1 wt% to about 10 wt% of the cementitious material.

385. The composite material of Claim 384, wherein the additives comprise an aluminium-containing compound selected from the group consisting of aluminium oxide, aluminosilicates, calcium aluminates, calcium aluminosilicates, or combinations thereof.

386. The composite material of Claim 384, wherein the additives comprise gypsum or calcium sulfate.61FH 13302371.4NLH-00125 387. The composite material of Claim 384, wherein the additives comprise one or more metal oxides selected from the group consisting of aluminium oxide, iron oxide, magnesium oxide, sulfur oxide, titanium oxide, chromium oxide, manganese oxide, or alkali metal oxides.

388. The composite material of Claim 381, wherein the cementitious material is hydraulic, wherein after curing for 28 days, the cementitious material exhibits a compressive strength of at least 5 MPa.

389. The composite material of Claim 381, wherein the amorphous calcium silicate has a specific surface area from about 1 m2 / g to about 100 m2 / g.62FH 13302371.4

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