Extraction of base from silicate

Abstract

A method of extracting a base from a silicate under carbon neutral conditions is described. The method includes providing a reaction mixture comprising a base-containing aluminosilicate composition and a base-based composition. The reaction mixture is treated with a combined activation and leaching process to form a concentrated alkali-silicate solution and an alkaline aluminosilicate solid residue wherein carbon dioxide is generated from the activation as a reusable by-product carbon dioxide. The alkali aluminosilicate solid residue is reacted with a first portion of a reusable by-product carbon dioxide to form an alkali leached aluminosilicate composition to extract alkali from the alkali-containing aluminosilicate composition. Methods of preparing inorganic polymer cement and concrete from the products and / or by-products produced by the extraction process are also described.

Description

Cross-references to related applications

[0001] This application claims priority to U.S. Provisional Patent Application Serial No. 63 / 573,752, filed April 3, 2024, and U.S. Provisional Patent Application Serial No. 63 / 514,370, filed July 19, 2023, the disclosures of which are incorporated herein by reference in their entirety. Technical Field

[0002] This disclosure generally relates to methods for extracting alkalis, particularly from silicates, and their uses, including, for example, the preparation of inorganic polymer cement and inorganic polymer concrete. Background Technology

[0003] Inorganic polymer chemistry is a viable global pathway to decarbonize cement used in concrete. However, such cements require adequate amounts of basic elements (such as Na and K), rather than the relatively large amounts of calcium required by traditional Portland cement. Obtaining the necessary sodium and potassium from existing sources (e.g., the chlor-alkali process, the Solvay process, the Houbauer process, mined sodium carbonate, etc.) is possible but impractical. Of these sources, only mined sodium carbonate can provide enough alkali to support the global demand for inorganic polymer concrete (typically used in the form of liquid basic silicate hardeners). Potassium carbonate cannot be obtained in a similar manner from such deposits and is typically synthesized via the electrolysis of potassium salts, leading to its higher cost.

[0004] Unfortunately, sodium carbonate releases fossil CO2 when heated or decomposed to produce basic silicates. This is problematic for zero-CO2 production and requires a net-zero CO2 alkali metal source to enable complete decarbonization of inorganic polymer concrete.

[0005] If inorganic polymer cement is to compete as an alternative to Portland cement, all raw material inputs must adhere to the principles of sustainable chemistry, large-scale global production, and stringent price affordability. A major bottleneck for the future production of inorganic polymer cement is the production of abundant alkali-curing agents without generating process CO2. Inorganic polymer cement is typically a two-component system. The solid components of aluminosilicate reagents are suitable for large-scale global production; however, the production pathways and supply chains for alkali-silicate curing agents require particularly detailed examination regarding raw material availability, energy use, byproducts / residues, and CO2 footprint.

[0006] Currently, the supply of alkaline silicates is insufficient to support any major transition to inorganic polymer cement, inorganic polymer blended cement, or alkali-activated cement. More importantly, the input of alkali raw materials (such as mined sodium carbonate) is insufficient in quantity or distribution for a global transition, as sodium carbonate deposits are not even available on all continents, let alone in most regional markets.

[0007] The entire silicate production supply chain may require radical overhaul to meet the economic, logistical, and low greenhouse gas (GHG) emission requirements of a sustainable global inorganic polymer cement industry. The hardeners for inorganic polymers are almost entirely derived from sodium carbonate or salts with chloride byproducts, while most silicate crusts are rich in untapped alkalis.

[0008] One advantage of Portland cement is that it only requires water to harden the concrete mixture. Inorganic polymer cement is different because it requires a second agent, much like the catalytic polymerization of organic resins. While water is generally readily available globally, this is not the case for technical agents such as soluble basic silicates. If inorganic polymer cement is to become viable beyond niche applications, we must consider whether the modern basic silicate (hardener) supply chain is suited to leap from a relatively small-scale and high-purity agent to a ubiquitous commodity. The requirements for a viable cement silicate industry are simple: the cost of silicate hardeners must allow inorganic polymer concrete to compete with current alternatives, and the silicate industry must be able to grow in tandem with inorganic polymer cement production—this growth must be feasible, sustainable, and ideal. If global cement production (approximately 4000 Mt / a) were to transition to inorganic polymer cement, it would require basic silicate hardener production in the order of 100 to 1000 Mt / a. Current global production is approximately 25 Mt / a; therefore, growing the existing industry by several orders of magnitude is a significant undertaking.

[0009] The supply of SiO2 (quartz) used in the production of basic silicates is not a problem. Quartz is the second most abundant mineral in the continental crust, and it can be found in many rock types, usually with relatively pure production on each continent.

[0010] Because of the ease of processing relatively pure natural soda ash, mined sodium carbonate is the most obvious option for expanding supply (US reserves are 23 billion tons; USGS 2022). However, if carbon dioxide emissions are taxed in the future, GHG emissions from further sodium carbonate decomposition in cement production would be highly undesirable and potentially costly (there may be ways to mitigate this at significant additional cost, such as carbon capture, utilization, and storage (CCUS)). Another important question is whether it is feasible or wise to deplete a finite, valuable, and not globally ubiquitous strategic resource.

[0011] Seawater, brine, or mined evaporite-derived NaCl are abundant and readily apparent second-choice alkali sources. Sodium in seawater (3.5% NaCl w / w, 28.7 kg / ton NaCl equivalent) is primarily provided by continental weathering, a natural chemical leaching process that has spanned much of Earth's history. The abundance of seawater and mined NaCl globally is a good first step. Unfortunately, NaCl encounters the common problem found in available alkali salts, with the accompanying anions limiting further scaling. At current levels, chlorine production is not only useful but is often the primary byproduct of brine electrolysis. Current global chlorine production capacity is approximately 58 Mt / a. This is primarily used for sanitation and the production of polyvinyl chloride (PVC, approximately 59 Mt / a). Assuming there is no shortage of renewable energy sources to scale up brine electrolysis, finding a useful application for several orders of magnitude more chlorine seems to rule out brine electrolysis as a general solution for scaling up alkali production. Clearly, alternative production routes are needed if inorganic polymer cement is to achieve commercial success.

[0012] The supply of basic silicate hardeners is exacerbated by the desire to reduce the impact of CO2. From a sustainable chemistry perspective, this additional requirement is challenging for several reasons:

[0013] Alkaline elements on the Earth's surface are typically associated with carbonate anions (or similar problematic sulfate, chloride, and fluoride ions).

[0014] Calcium carbonate is abundant and inexpensive globally, and provides a readily available source of exchangeable cations that can be used for in-situ leaching of basic elements in high-pH aqueous solutions of cement mixtures (e.g., in Roman marine concrete) or for use when calcined into oxide forms. However, it is desirable to avoid the release of fossil CO2 from calcium carbonate, which is often necessary for utilizing its calcium cations in chemical processes.

[0015] The most readily conceivable chemical processes that effectively circumvent the alkali supply problem (reagent production or in-situ processes within cement) either come at the cost of releasing large amounts of CO2 from abundant calcium carbonate or utilize less reactive mixtures that require long curing times (e.g., other soluble alkali salts at various pore solution pH levels). A major bottleneck for the future of inorganic polymer cement production is the production of alkali salt solution hardeners without generating CO2.

[0016] This disclosure is intended to overcome these and other deficiencies in the art. Summary of the Invention

[0017] This disclosure generally relates to methods, particularly the following: extracting an alkali from a silicate, preparing an alkali-silicate composition from the extracted alkali, preparing an activated kaolinite composition, preparing inorganic polymer cement from the alkali-silicate and activated kaolinite composition, and preparing inorganic polymer concrete from the inorganic polymer cement. This disclosure also relates to products and byproducts produced by the methods described herein. This disclosure relates to the use of alkali-silicate compositions prepared according to the methods disclosed herein as reagents for the preparation of cement (including, but not limited to, inorganic polymer cement).

[0018] In one aspect, this disclosure relates to a method for extracting potassium, sodium, or both potassium and sodium from silicates under carbon-neutral conditions. The method comprises: (a) providing a reaction mixture comprising a first reactant and a second reactant, wherein the first reactant comprises a potassium-containing aluminosilicate composition, a sodium-containing aluminosilicate composition, or a mixture thereof, and wherein the second reactant comprises a corresponding potassium-based composition, a sodium-based composition, or a mixture thereof; (b) treating the reaction mixture with a combined activation and leaching process to form a concentrated potassium silicate solution, a sodium silicate solution, or a mixture thereof, and corresponding potassium aluminosilicate solid residues, sodium aluminosilicate solid residues, or a mixture thereof, wherein carbon dioxide is generated by activation as a reusable byproduct carbon dioxide; and (c) reacting the potassium aluminosilicate solid residues, sodium aluminosilicate solid residues, or a mixture thereof with a first portion of the reusable byproduct carbon dioxide to form a potassium-leached aluminosilicate composition, a sodium-leached aluminosilicate composition, or a mixture thereof, thereby extracting potassium, sodium, or a mixture thereof from the corresponding potassium-containing aluminosilicate composition, sodium-containing aluminosilicate composition, or a mixture thereof.

[0019] In another aspect, this disclosure relates to a composition comprising a potassium, sodium, or potassium and sodium leached aluminosilicate composition produced according to a method described herein for extracting potassium, sodium, or both potassium and sodium from silicates under carbon-neutral conditions.

[0020] In another aspect, this disclosure relates to a composition comprising a potassium, sodium, or a potassium and sodium composition produced according to a method for extracting potassium, sodium, or both potassium and sodium from silicates under carbon-neutral conditions as described herein.

[0021] In another aspect, this disclosure relates to a composition comprising an alkaline product produced according to a method for extracting potassium, sodium, or both potassium and sodium from silicates under carbon-neutral conditions as described herein, wherein the alkaline product is selected from the group consisting of alkaline carbonates, alkaline silicates, etc.

[0022] In another aspect, this disclosure relates to a method for extracting an alkali from a silicate under carbon-neutral conditions, while simultaneously forming an activated synthetic kaolinite composition. The method comprises: (a) providing a reaction mixture comprising an alkali-containing aluminosilicate composition and a base composition; (b) treating the reaction mixture with a combined activation and leaching process to form a concentrated alkali-silicate solution and an alkaline aluminosilicate solid residue, wherein carbon dioxide is generated by activation as a reusable byproduct carbon dioxide; (c) reacting the alkaline aluminosilicate solid residue with a first portion of the reusable byproduct carbon dioxide to form an alkali-leached aluminosilicate composition, thereby extracting the alkali from the alkali-containing aluminosilicate composition; and (d) activating the alkali-leached aluminosilicate composition to form an activated synthetic kaolinite composition.

[0023] In another aspect, this disclosure relates to a composition comprising an activated synthetic kaolinite composition produced according to a method disclosed herein for extracting a base from a silicate under carbon-neutral conditions while forming an activated synthetic kaolinite composition.

[0024] In another aspect, this disclosure relates to a composition comprising an alkaline carbonate liquid produced according to a method disclosed herein for extracting a base from a silicate under carbon-neutral conditions while forming an activated synthetic kaolinite composition.

[0025] In another aspect, this disclosure relates to a composition comprising a solid product produced according to a method disclosed herein for extracting a base from a silicate under carbon-neutral conditions while forming an activated synthetic kaolinite composition.

[0026] In another aspect, this disclosure relates to a composition comprising an alkali-silicate liquid produced according to a method disclosed herein for extracting an alkali from a silicate under carbon-neutral conditions while forming an activated synthetic kaolinite composition.

[0027] In another aspect, this disclosure relates to a composition comprising an alkali-silicate solid product produced according to a method disclosed herein for extracting an alkali from a silicate under carbon-neutral conditions while forming an activated synthetic kaolinite composition.

[0028] In another aspect, this disclosure relates to a composition comprising an optionally activated synthetic aluminosilicate having an aluminum to silicon ratio of about 1:1, produced according to a method disclosed herein for extracting a base from a silicate under carbon-neutral conditions while forming an optionally activated synthetic aluminosilicate composition.

[0029] In another aspect, this disclosure relates to a method for preparing inorganic polymer cement. The method includes: providing an activated synthetic kaolinite composition produced according to various methods of this disclosure; and using the activated synthetic kaolinite composition as a reagent to form inorganic polymer cement.

[0030] In another aspect, this disclosure relates to a composition comprising inorganic polymer cement produced according to the method for preparing inorganic polymer cement as described herein.

[0031] In another aspect, this disclosure relates to a method for preparing inorganic polymer concrete. The method includes: providing an inorganic polymer cement according to this disclosure; and combining the inorganic polymer cement with a solid aggregate composition and optionally a filler composition to form inorganic polymer concrete, wherein, based on the inorganic polymer concrete, the inorganic polymer is present in an amount ranging from 1 to 44 wt%, the solid aggregate composition is present in an amount ranging from 55 to 95 wt%, and the optional filler composition is present in an amount ranging from 1 to 20 wt%.

[0032] In another aspect, this disclosure relates to a composition comprising inorganic polymer concrete produced according to the method for preparing inorganic polymer concrete as described herein.

[0033] In one aspect, this disclosure relates to a method for extracting an alkali from an alkaline silicate under carbon-neutral conditions. The method comprises: (a) providing a reaction mixture comprising an alkaline aluminosilicate composition and a base composition, the base composition containing an alkali contained in the alkaline aluminosilicate; (b) treating the reaction mixture with a combined activation and leaching process to form a concentrated alkali-silicate solution and an alkaline aluminosilicate solid residue, wherein carbon dioxide is generated by activation as a reusable byproduct carbon dioxide; and (c) reacting the alkaline aluminosilicate solid residue with a first portion of the reusable byproduct carbon dioxide to form an alkali-leached aluminosilicate composition, thereby extracting the alkali from the alkaline aluminosilicate composition.

[0034] In another aspect, this disclosure relates to a composition comprising an alkali-leached aluminosilicate composition produced according to a method for extracting alkali from an alkali-containing silicate under carbon-neutral conditions as described herein.

[0035] As described herein, in some aspects, the methods and compositions of this disclosure involve using a base composition matched to the feedstock (e.g., β-spodumene in this embodiment), such that a portion of the resulting basic carbonate product can be recycled back to the first step, thereby eliminating the need to freshly feed the basic carbonate into the process. Therefore, in various respects, the methods of this disclosure are superior to the prior art, at least in that they generate little or no waste carbon dioxide or process carbon dioxide emissions, and the basic aluminosilicate byproducts can be further utilized in other aspects of the methods and products of this disclosure.

[0036] Unlike existing processes (such as those that merely aim to replace lithium in spodumene with cheaper alkali), the method disclosed herein is capable of efficiently recovering lithium using lithium carbonate. This method has the unique advantage of significantly reducing waste, as a portion of the recovered lithium carbonate can be reused to leach more material from the spodumene feedstock.

[0037] As shown in Table 1 below, the method disclosed herein is superior to existing methods in the art.

[0038] Additional aspects, advantages, and features of this disclosure will become more apparent upon reading the following non-limiting description of preferred embodiments, which are exemplary and should not be construed as limiting the scope of this disclosure. Brief Description of the Drawings

[0039] A better understanding of the features, advantages, and principles of this disclosure will be obtained by referring to the following detailed description and accompanying drawings illustrating illustrative embodiments, wherein:

[0040] Figure 1A illustrates an example of an albite-based binder system according to one embodiment as a ring-open, fully utilized green process solution;

[0041] Figure 1B illustrates an example of an albite-based binder system as a closed-loop, fully recyclable green process according to one embodiment.

[0042] Figure 1C illustrates an example of a potassium feldspar-based binder system according to one embodiment as a ring-open, fully utilized green process solution.

[0043] Figure 1D illustrates an example of a potassium feldspar-based binder system as a closed-loop, fully recyclable green process according to one embodiment.

[0044] Figure 2 is a flowchart illustrating the production of Na2CO3 from alkali feldspar and the synthesis of metakaolin according to one embodiment;

[0045] Figure 3 is a flowchart illustrating the production of alkali-silicates from feldspar-derived alkalis according to one embodiment;

[0046] Figure 4 is a flowchart illustrating the production of an alkali feldspar-derived inorganic polymer according to one embodiment;

[0047] Figure 5 shows the residue remaining after calcining potassium feldspar with the following substances at 900°C and leaching with water according to one embodiment: A) 1.2 equivalents (eq.) of Na2CO3; B) 2.2 equivalents of Na2CO3; and C) 3.0 equivalents of Na2CO3;

[0048] Figure 6 shows the scanning electron microscope-energy dispersive X-ray spectroscopy (SEM-EDX) data of the residue remaining after calcination of potassium feldspar with 3.0 equivalents of Na2CO3 at 900°C and water leaching according to one embodiment.

[0049] Figure 7 shows the degree of alkali leaching after CO2 bubbling at high temperature according to one embodiment;

[0050] Figure 8 shows the extent of alkaline leaching after CO2 bubbling, according to one embodiment, under optimized flow rate and temperature.

[0051] Figure 9 shows SEM-EDX data of the residue (synthetic kaolinite) from CO2 leaching of hydroxycancrinite in a trickle bed reactor according to one embodiment;

[0052] Figure 10 shows SEM-EDX data of the residue (synthetic kaolinite) after carbonation of calcium hydroxyl nepheline in a stirred reactor at high temperature using a CO2 flow rate of 5 L / min, according to one embodiment.

[0053] Figure 11 shows a comparison of XRD data for hydroxyl calcium nepheline starting material (blue), alkali leaching residue after CO2 carbonation in a stirred reactor (green), and alkali leaching residue after calcination (pink) according to one embodiment.

[0054] Figure 12 shows a comparison of XRD data for hydroxyl calcium nepheline starting material (green), alkaline leaching residue after CO2 carbonation in a trickle bed reactor (blue), and calcined synthetic kaolinite material (purple) according to one embodiment.

[0055] Figure 13 shows a comparison of XRD data for commercial metakaolin (red), synthetic metakaolin (blue) produced by CO2 leaching of calcium hydroxyl nepheline in a trickle bed reactor, and synthetic metakaolin (pink) produced by CO2 leaching in a stirred reactor, according to one embodiment.

[0056] Figure 14 shows the scanning electron microscope-energy dispersive X-ray spectroscopy (SEM-EDX) data of the residue remaining after calcination of sodium feldspar (albite) with 3.0 equivalents of Na2CO3 at 950°C and subsequent water leaching, according to one embodiment.

[0057] Figure 15 shows scanning electron microscopy-energy dispersive X-ray spectroscopy (SEM-EDX) data of the residue (synthetic kaolinite) remaining after high-pressure CO2 leaching of hydroxyl calcium nepheline (from albite) in a 2L reactor according to one embodiment.

[0058] Figure 16 shows the XRD patterns of Na feldspar (sodium feldspar) (blue) and the water leaching residue (calcium hydroxyl nepheline) (orange) after calcination of sodium feldspar with 3.0 equivalents of Na2CO3, and the CO2 leaching residue (synthetic kaolinite) (pink) after the calcination and water leaching steps, according to one embodiment.

[0059] Figure 17 shows a comparison of X-ray diffraction (XRD) data of the residue remaining after calcination and leaching of α-spodumene with 3 equivalents of Li2CO3 according to one embodiment.

[0060] Figure 18 shows the XRD pattern of the residue (bottom) remaining after the hydrothermal reaction between NaOH and potassium feldspar according to one embodiment, compared with the residue (top - Example 1) formed during the calcination of potassium feldspar with 3.0 equivalents of Na2CO3.

[0061] Figure 19 shows a scanning electron microscope (SEM) image of the residue (calcium hydroxide nepheline) formed by the hydrothermal reaction between NaOH and potassium feldspar according to one embodiment.

[0062] Figure 20 shows the XRD patterns of the residue (potassium nepheline) (pink) remaining after the hydrothermal reaction between KOH and potassium feldspar, and the residue (synthetic kaolinite) (blue) formed by leaching potassium nepheline with CO2, according to one embodiment.

[0063] Figure 21 shows SEM-EDX data of the residue (potassium nepheline) formed by the hydrothermal reaction between KOH and potassium feldspar according to one embodiment;

[0064] Figure 22 shows SEM-EDX data of the residue (synthetic kaolinite) from CO2 leaching of potassium nepheline in a trickle bed reactor according to one embodiment;

[0065] Figure 23 shows the XRD of the residue (synthetic kaolinite) remaining after leaching calcium hydroxyl nepheline with different nitric acid concentrations (from top to bottom: 1.1 M, 0.8 M and 0.5 M nitric acid) according to one embodiment;

[0066] Figure 24 shows SEM-EDX data of the residue (synthetic kaolinite) formed by leaching calcium hydroxide nepheline with 0.8 M nitric acid according to one embodiment;

[0067] Figure 25 shows the XRD of calcined kaolinite (synthetic metakaolin) according to one embodiment;

[0068] Figure 26 shows the XRD of the residue (synthetic kaolinite) remaining after leaching calcium hydroxide nepheline with 1 M nitric acid according to one embodiment;

[0069] Figure 27 shows SEM-EDX data of the residue (synthetic kaolinite) formed by leaching calcium hydroxide nepheline with 1 M nitric acid according to one embodiment;

[0070] Figure 28 shows the XRD of the residue (synthetic kaolinite) remaining after leaching potassium nepheline with 0.8 M nitric acid according to one embodiment;

[0071] Figure 29 shows SEM-EDX data of the residue (synthetic kaolinite) formed by leaching potassium nepheline with 0.8 M nitric acid according to one embodiment;

[0072] Figure 30 shows the cumulative heat released at 40°C when the following metakaolin samples are mixed with potassium silicate (Kasil - 1.7 MR) to form an inorganic binder according to one embodiment: commercial metakaolin (blue), synthetic metakaolin produced by CO2 leaching in a trickle bed reactor (purple), and synthetic metakaolin produced by CO2 leaching in a stirred reactor (red).

[0073] Figure 31 shows the cumulative heat released at 40°C when synthetic metakaolin and synthetic kaolinite samples are mixed with potassium silicate (Kasil-1.7 MR) to form an inorganic binder according to one embodiment.

[0074] Figure 32 shows 27 Aluminum magic angle rotating solid-state nuclear magnetic resonance (NMR) spectroscopy, showing the similarity of aluminum coordination between synthetic metakaolinite (left and middle) produced by the TerraCO2 process and commercial metakaolinite (right);

[0075] Figure 33 illustrates an approximate material flow of one embodiment of a process for producing dry tons of inorganic polymer cement using typical granite as a raw material; and

[0076] Figure 34 illustrates an approximate material flow of one embodiment of integrating inorganic polymer cement production with existing granite aggregate mines.

[0077] Further details of this disclosure and its advantages will become apparent from the detailed description below. Detailed Implementation

[0078] The following detailed description provides a better understanding of the features and advantages of the aspects described in this disclosure based on the embodiments disclosed herein. While the detailed description includes many specific embodiments, these are provided by way of example only and should not be construed as limiting the scope of the aspects disclosed herein.

[0079] In the following description of embodiments, reference is made to the accompanying drawings to illustrate examples of embodiments in which various aspects of this disclosure can be practiced. It should be understood that other embodiments may be made without departing from the scope of the disclosed aspects.

[0080] This application is intended to describe one or more embodiments of this disclosure. It should be understood that the use of absolute terms such as "must," "will," and specific quantities should be interpreted as applicable to one or more such embodiments, but not necessarily to all such embodiments. Therefore, embodiments of this disclosure may omit or include modifications to one or more features or functions described in the context of such absolute terms. Furthermore, the headings in this application are for reference only and should not in any way affect the meaning or interpretation of this disclosure.

[0081] In one aspect, this disclosure relates to a method for extracting potassium, sodium, or both potassium and sodium from silicates under carbon-neutral conditions. The method comprises: (a) providing a reaction mixture comprising a first reactant and a second reactant, wherein the first reactant comprises a potassium-containing aluminosilicate composition, a sodium-containing aluminosilicate composition, or a mixture thereof, and wherein the second reactant comprises a corresponding potassium-based composition, a sodium-based composition, or a mixture thereof; (b) treating the reaction mixture with a combined activation and leaching process to form a concentrated potassium silicate solution, a sodium silicate solution, or a mixture thereof, and corresponding potassium aluminosilicate solid residues, sodium aluminosilicate solid residues, or a mixture thereof, wherein carbon dioxide is generated by activation as a reusable byproduct carbon dioxide; and (c) reacting the potassium aluminosilicate solid residues, sodium aluminosilicate solid residues, or a mixture thereof with a first portion of the reusable byproduct carbon dioxide to form a potassium-leached aluminosilicate composition, a sodium-leached aluminosilicate composition, or a mixture thereof, thereby extracting potassium, sodium, or a mixture thereof from the corresponding potassium-containing aluminosilicate composition, sodium-containing aluminosilicate composition, or a mixture thereof.

[0082] In some implementations, the activation process is selected from the group consisting of: thermal activation, hydrothermal activation, chemical activation, mechanochemical activation, radiation activation (e.g., microwave irradiation), electromagnetic activation, electrochemical activation, etc.

[0083] In some embodiments, heating includes heating at temperatures ranging from about 850°C to 1100°C, about 900°C to 1050°C, or about 950°C to 1000°C, with residence times ranging from about 0.25 to 4 hours, about 0.5 to 1.5 hours, or about 0.75 to 1.25 hours. In some embodiments, heating may be carried out, for example, in a ceramic or high-alloy stainless steel container. In some embodiments, heating may be carried out, for example, in a static or flowing process. Examples of heating may include, but are not limited to, calcination processes as understood in the art.

[0084] In some embodiments, the activation process is a hydrothermal process, wherein the hydrothermal process includes heating at a temperature in the range of about 150°C-275°C, about 175°C-250°C, or about 200°C-225°C, with a residence time ranging from about 1-72 hours, about 8-24 hours, or about 12-18 hours. In some embodiments, the hydrothermal process may be carried out, for example, in a sealed autoclave lined with polytetrafluoroethylene (PTFE) or under similar conditions as understood in the art.

[0085] In some embodiments, the potassium-containing aluminosilicate composition and the sodium-containing aluminosilicate composition contain feldspar. In some embodiments, the feldspar may include, but is not limited to, alkali feldspar, plagioclase feldspar, etc. In some embodiments, the feldspar may include, but is not limited to, orthoclase, sanidine, microcline, anorthoclase, albite, oligoclase, andesine, labradorite, bytownite, anorthite, and mixtures thereof or solid solutions thereof.

[0086] In some embodiments, the potassium-containing aluminosilicate composition and the sodium-containing aluminosilicate composition comprise feldspathoid minerals selected from the group consisting of nepheline, potassium nepheline, sodalite, leucite, haüyne, cancrinite, etc.

[0087] In some embodiments, the potassium-containing aluminosilicate composition and the sodium-containing aluminosilicate composition comprise zeolite supergroup minerals, which include zeolites selected from the group consisting of: analcime, chabazite, clinoptilolite, erionite, mordenite, phillipsite, ferrierite, natrolite, faujasite, etc.

[0088] In some embodiments, the potassium-containing aluminosilicate composition and the sodium-containing aluminosilicate composition comprise mica and clay minerals, wherein the mica and clay minerals are selected from the group consisting of: muscovite, biotite, phlogopite, smectite, illite, vermiculite, saponite, lepidolite, hectorite, etc.

[0089] In some embodiments, the potassium-based composition comprises potassium (K), potassium hydroxide (KOH), potassium carbonate (K2CO3), potassium oxide (K2O), and mixtures thereof.

[0090] In some embodiments, the sodium-based composition comprises sodium (Na), sodium hydroxide (NaOH), sodium carbonate (Na2CO3), sodium oxide (Na2O), and mixtures thereof.

[0091] In some embodiments, the mixture of potassium-based and sodium-based compositions comprises a mixture of two or more compositions selected from the group consisting of: potassium (K), potassium hydroxide (KOH), potassium carbonate (K2CO3), potassium oxide (K2O), sodium (Na), sodium hydroxide (NaOH), sodium carbonate (Na2CO3), sodium oxide (Na2O), and mixtures thereof.

[0092] In some embodiments, the potassium aluminosilicate solid residue, sodium aluminosilicate solid residue, or mixture thereof produced by the processing steps have a silicon / aluminum (Si:Al) ratio in the range of about 0.8 to 1.8.

[0093] In some embodiments, the reaction steps are carried out at temperatures ranging from about 150°C to 500°C, about 175°C to 225°C, or about 185°C to 210°C, and at pressures ranging from about 0 to 1500 psig, about 50 to 600 psig, or about 100 to 300 psig for a duration sufficient to leach substantially all of the remaining alkali into an alkali metal solution having the formula M2CO3, where M is the corresponding alkali metal.

[0094] In some implementations, the carbon dioxide produced by this method is essentially reused.

[0095] In another aspect, this disclosure provides a composition comprising a potassium, sodium, or potassium and sodium leached aluminosilicate composition produced according to a method for extracting potassium, sodium, or both potassium and sodium from silicates under carbon-neutral conditions as described herein.

[0096] In another aspect, this disclosure provides a composition comprising potassium, sodium, or a combination of potassium and sodium produced according to a method for extracting potassium, sodium, or both potassium and sodium from silicates under carbon-neutral conditions as described herein.

[0097] In another aspect, this disclosure provides a composition comprising an alkaline product produced according to a method for extracting potassium, sodium, or both potassium and sodium from silicates under carbon-neutral conditions as described herein, wherein the alkaline product is selected from the group consisting of alkaline carbonates, alkaline silicates, etc.

[0098] In another aspect, this disclosure provides a method for extracting an alkali from a silicate under carbon-neutral conditions, while simultaneously forming an activated synthetic kaolinite composition. The method comprises: (a) providing a reaction mixture comprising an alkali-containing aluminosilicate composition and a base composition; (b) treating the reaction mixture with a combined activation and leaching process to form a concentrated alkali-silicate solution and an alkaline aluminosilicate solid residue, wherein carbon dioxide is generated by activation as a reusable byproduct carbon dioxide; (c) reacting the alkaline aluminosilicate solid residue with a first portion of the reusable byproduct carbon dioxide to form an alkali-leached aluminosilicate composition, thereby extracting the alkali from the alkali-containing aluminosilicate composition; and (d) activating the alkali-leached aluminosilicate composition to form an activated synthetic kaolinite composition.

[0099] In some embodiments of this method, activation includes processes that increase reactivity, including those selected from the group consisting of: thermal activation, hydrothermal activation, chemical activation, mechanochemical activation, radiation activation (e.g., microwave irradiation), electromagnetic activation, electrochemical activation, mechanical energy treatment, etc.

[0100] In some embodiments of this method, the activated synthetic kaolinite composition comprises metakaolinite, vitrified kaolinite, calcined kaolinite, rapidly calcined kaolinite, activated clay with a Si:Al ratio in the range of about 0.5-1.5, or combinations thereof. In some embodiments, the activated clay may have a Si:Al ratio close to 1.0.

[0101] In some embodiments of this method, the carbon dioxide produced by the method is essentially reused.

[0102] In some embodiments of the method, the reaction steps are carried out at temperatures ranging from about 150°C to 500°C, about 175°C to 225°C, or about 185°C to 210°C, and at pressures ranging from about 0 to 1500 psig, about 50 to 600 psig, or about 100 to 300 psig for a duration sufficient to leach substantially all of the remaining alkali into an alkali metal solution having a composition selected from the group consisting of M2CO3, MOH, and M2O, where M is the corresponding alkali metal.

[0103] In some embodiments of this method, the method further includes: concentrating, crystallizing, separating, and / or converting the alkali metal solution to form an alkali metal solid having a formula selected from the group consisting of M₂CO₃, MOH, and M₂O, wherein M is the corresponding alkali metal. According to this disclosure, in some embodiments, those skilled in the art can use techniques and solutions in related fields, and further in conjunction with this disclosure, to perform the steps as described herein of concentrating, crystallizing, separating, and / or converting the alkali metal solution to form an alkali metal solid.

[0104] In some embodiments of the method, the method further includes reintroducing at least a portion of the alkali metal solid as a base composition into the processing step, thereby forming a continuous loop of base composition production and consumption.

[0105] In some embodiments of the method, the method further includes reacting a concentrated alkali-silicate solution with a second portion of reusable byproduct carbon dioxide to form solid silica gel and an alkali-carbonate solution.

[0106] In some embodiments of the method, the solid silica gel comprises silicon dioxide (SiO2) at a concentration ranging from about 75 to 100 wt%. In some embodiments, the solid silica gel comprises silicon dioxide (SiO2) at a concentration ranging from about 75 to 100 wt%, wherein the remainder is alkaline carbonate.

[0107] In some embodiments of the method, solid silica gel is repeatedly used to react or combine with a base composition to form an alkaline silicate or as an activated silica source for the production of inorganic polymer cement, or the solid silica gel is repeatedly used to react or combine with an alkaline silicate composition.

[0108] In some embodiments of the method, the alkali-carbonate solution contains M2CO3, the concentration of M2CO3 in water ranging from 1 to 40 wt / wt%, where M is the corresponding alkali metal.

[0109] In some embodiments of the method, the method further includes: separating an alkaline carbonate composition from an alkaline-carbonate solution; and combining solid silica gel and the separated alkaline carbonate composition to form an alkaline-silicate liquid.

[0110] In some embodiments of the method, the alkali-silicate liquid contains silicon dioxide (SiO2) in a concentration range of about 10-50 wt%, and the SiO2:M2O weight ratio ranges from about 1.0 to 4.0.

[0111] In some embodiments of the method, the method further includes treating the alkali-silicate liquid to form a separated alkali-silicate solid product. In some embodiments, the treatment can be carried out by, but is not limited to, evaporation and recrystallization. In some embodiments, the treatment can be carried out by, but is not limited to, evaporation and recrystallization, wherein the alkali-silicate solid product can be dried and maintained in a form including, for example, hydrated crystals, anhydrous crystals, etc.

[0112] In another aspect, this disclosure provides a composition comprising an activated synthetic kaolinite composition produced according to a method disclosed herein for extracting a base from a silicate under carbon-neutral conditions while forming an activated synthetic kaolinite composition.

[0113] In another aspect, this disclosure provides a composition comprising an alkaline carbonate liquid produced according to a method disclosed herein for extracting a base from a silicate under carbon-neutral conditions while forming an activated synthetic kaolinite composition.

[0114] In another aspect, this disclosure relates to providing a composition comprising a solid product produced according to a method disclosed herein for extracting a base from a silicate under carbon-neutral conditions while forming an activated synthetic kaolinite composition.

[0115] In another aspect, this disclosure provides a composition comprising an alkali-silicate liquid produced according to a method disclosed herein for extracting an alkali from a silicate under carbon-neutral conditions while forming an activated synthetic kaolinite composition.

[0116] In another aspect, this disclosure provides a composition comprising an alkali-silicate solid product produced according to a method disclosed herein for extracting an alkali from a silicate under carbon-neutral conditions while forming an activated synthetic kaolinite composition.

[0117] In another aspect, this disclosure provides a composition comprising an optionally activated synthetic aluminosilicate having an aluminum to silicon ratio of about 1:1, produced according to a method disclosed herein for extracting a base from a silicate under carbon-neutral conditions while forming an optionally activated synthetic aluminosilicate composition.

[0118] In another aspect, this disclosure provides a method for preparing inorganic polymer cement. The method includes: providing an activated synthetic kaolinite composition produced according to various methods of this disclosure; and using the activated synthetic kaolinite composition as a reagent to form inorganic polymer cement.

[0119] In another aspect, this disclosure provides a composition comprising inorganic polymer cement produced according to the method for preparing inorganic polymer cement as described herein.

[0120] In another aspect, this disclosure provides a method for preparing inorganic polymer concrete. The method includes: providing an inorganic polymer cement according to this disclosure; and combining the inorganic polymer cement with a solid aggregate composition and optionally a filler composition to form inorganic polymer concrete, wherein, based on the inorganic polymer concrete, the inorganic polymer is present in an amount ranging from 1 to 44 wt%, the solid aggregate composition is present in an amount ranging from 55 to 95 wt%, and the optional filler composition is present in an amount ranging from 1 to 20 wt%.

[0121] In some embodiments, the optional packing composition is selected from the group consisting of reactive packings, inert packings, and combinations thereof.

[0122] In some embodiments, the solid aggregate composition is selected from the group consisting of: coarse aggregate, medium aggregate, fine aggregate, lightweight aggregate, engineered aggregate, artificial aggregate, angular aggregate, round aggregate, water-worn aggregate, recycled aggregate, stone, sand, natural rock, industrial by-products, alkaline aluminosilicate, feldspar, etc.

[0123] In another aspect, this disclosure provides a composition comprising inorganic polymer concrete produced according to the method for preparing inorganic polymer concrete as described herein.

[0124] In one aspect, this disclosure provides a method for extracting an alkali from an alkaline silicate under carbon-neutral conditions. The method comprises: (a) providing a reaction mixture comprising an alkaline aluminosilicate composition and a base composition, the base composition containing an alkali contained in the alkaline aluminosilicate; (b) treating the reaction mixture with a combined activation and leaching process to form a concentrated alkali-silicate solution and an alkaline aluminosilicate solid residue, wherein carbon dioxide is generated by activation as a reusable byproduct carbon dioxide; and (c) reacting the alkaline aluminosilicate solid residue with a first portion of the reusable byproduct carbon dioxide to form an alkali-leached aluminosilicate composition, thereby extracting the alkali from the alkaline aluminosilicate composition.

[0125] In some embodiments of this method, activation includes processes that increase reactivity, including those selected from the group consisting of: thermal activation, hydrothermal activation, chemical activation, mechanochemical activation, radiation activation (e.g., microwave irradiation), electromagnetic activation, electrochemical activation, mechanical energy treatment, etc.

[0126] In some embodiments of the method, heating includes heating at a temperature in the range of about 850°C-1100°C, about 900°C-1050°C, or about 950°C-1000°C, with a dwell time in the range of about 0.25-4 hours, about 0.5-1.5 hours, or about 0.75-1.25 hours.

[0127] In some embodiments of the method, the activation process is a hydrothermal process, wherein the hydrothermal process includes heating at a temperature in the range of about 150°C-275°C, about 175°C-250°C, or about 200°C-225°C, with a residence time in the range of about 1-72 hours, about 8-24 hours, or about 12-18 hours.

[0128] In some embodiments of the method, the alkaline aluminosilicate composition contains feldspar.

[0129] In some embodiments of this method, the feldspar is selected from the group consisting of alkali feldspar and plagioclase.

[0130] In some embodiments of the method, the feldspar is selected from the group consisting of: orthoclase, sancite, microcline, anisoclase, albite, orthoclase, andesine, labradorite, dalite, anorthite, and mixtures or solid solutions thereof.

[0131] In some embodiments of the method, the alkaline aluminosilicate composition comprises feldspar-like minerals selected from the group consisting of: nepheline, potassium nepheline, sodalite, leucite, lapis lazuli, calcium nepheline, etc.

[0132] In some embodiments of the method, the alkali-containing aluminosilicate composition comprises a zeolite supergroup mineral, which includes zeolites selected from the group consisting of: analcime, chalcogenide, clinoptilolite, mordenite, mordenite, calcium cross-shaped zeolite, magnesium alkali zeolite, sodium zeolite, octahedral zeolite, etc.

[0133] In some embodiments of the method, the alkaline aluminosilicate composition comprises mica and clay minerals, wherein the mica and clay minerals are selected from the group consisting of: muscovite, biotite, phlogopite, montmorillonite, illite, vermiculite, saponite, lepidolite, hydropyrite, etc.

[0134] In some embodiments of the method, the alkaline aluminosilicate composition comprises spodumene, petalite, hydropyrite, eucryptite, and / or jadarite.

[0135] In some embodiments of the method, the base composition comprises an alkali metal selected from the group consisting of sodium (Na), potassium (K), lithium (Li), and mixtures thereof.

[0136] In some embodiments of this method, the base composition is selected from the group consisting of sodium hydroxide (NaOH), potassium hydroxide (KOH), lithium hydroxide (LiOH), and mixtures thereof.

[0137] In some embodiments of the method, the base composition is selected from the group consisting of sodium carbonate (Na2CO3), potassium carbonate (K2CO3), lithium carbonate (Li2CO3), and mixtures thereof.

[0138] In some embodiments of this method, the base composition is selected from the group consisting of sodium oxide (Na2O), potassium oxide (K2O), lithium oxide (Li2O), and mixtures thereof.

[0139] In some embodiments of the method, the base composition is selected from the group consisting of sodium bicarbonate (NaHCO3), potassium bicarbonate (KHCO3), lithium bicarbonate (LiHCO3), and mixtures thereof.

[0140] In some embodiments of the method, the alkaline aluminosilicate solid residue produced by the processing steps has a silicon / aluminum (Si:Al) ratio in the range of about 0.8-1.8.

[0141] In some embodiments of the method, the reaction steps are carried out at temperatures ranging from about 150°C to 500°C, about 175°C to 225°C, or about 185°C to 210°C, and at pressures ranging from 0 to 1500 psig, about 50 to 600 psig, or about 100 to 300 psig for a duration sufficient to leach substantially all of the remaining alkali into an alkali metal solution having a composition selected from the group consisting of M2CO3, MOH, and M2O, where M is the corresponding alkali metal.

[0142] In some embodiments of this method, the carbon dioxide produced by the method is essentially reused.

[0143] In some embodiments, the alkaline aluminosilicate composition contains feldspar.

[0144] In some embodiments, the feldspar is selected from the group consisting of alkali feldspar ((K,Na)AlSi3O8) and plagioclase (NaAlSi3O8-CaAl2Si2O8). Examples of such feldspars include, but are not limited to, orthoclase (KAlSi3O8), sananoclase ((K,Na)AlSi3O8), microcline (KAlSi3O8), anisoclase ((Na,K)AlSi3O8), and albite ((Ab... 90 - Ab 100 NaAlSi3O8), austenite (Ab) 70 - Ab 90 ), andesite (Ab) 50 - Ab 70 Labradorite (Ab) 30 - Ab 50 ), Ab 10 - Ab 30 ), anorthite (Ab0 - Ab) 10 (CaAl2Si2O8) and mixtures or solid solutions thereof. Examples of feldspar may include, but are not limited to, those feldspars known in the art that are characterized by a ternary classification diagram of feldspars.

[0145] In some embodiments, the alkali-containing aluminosilicate composition comprises feldspar-like minerals. Examples of feldspar-like minerals may include, but are not limited to, nepheline, potassium nepheline, sodalite, leucite, lapis lazuli, and calcium nepheline.

[0146] In some embodiments, the alkali-containing aluminosilicate composition comprises amorphous alkali materials, such as soda-lime glass, aluminosilicate glass, volcanic glass, glass fiber, and metallurgical slag.

[0147] In some embodiments, the alkali-containing aluminosilicate composition comprises a zeolite supergroup mineral. Examples of zeolites may include, but are not limited to, analcime, chalcogenide, clinoptilolite, mordenite, mordenite, calcium cruciformite, magnesium alkali zeolite, sodium zeolite, and octahedralite.

[0148] In some embodiments, the alkali-containing aluminosilicate composition comprises mica and clay minerals. Examples of mica and clay minerals include, but are not limited to, muscovite, biotite, phlogopite, montmorillonite, illite, vermiculite, saponite, lepidolite, and hydropyrite.

[0149] In some embodiments, the alkaline aluminosilicate composition includes, but is not limited to, spodumene, petalite, hydropyrite, nepheline, and / or jadalite.

[0150] In some embodiments, the base composition comprises an alkali metal selected from the group consisting of sodium (Na), potassium (K), lithium (Li), and mixtures thereof.

[0151] In some embodiments, the base composition is selected from the group consisting of sodium hydroxide (NaOH), potassium hydroxide (KOH), lithium hydroxide (LiOH), and mixtures thereof.

[0152] In some embodiments, the base composition is selected from the group consisting of sodium carbonate (Na2CO3), potassium carbonate (K2CO3), lithium carbonate (Li2CO3), and mixtures thereof.

[0153] In some embodiments, the base composition is selected from the group consisting of sodium bicarbonate (NaHCO3), potassium bicarbonate (KHCO3), lithium bicarbonate (LiHCO3), and mixtures thereof.

[0154] In some embodiments, the base composition is selected from the group consisting of sodium oxide (Na2O), potassium oxide (K2O), lithium oxide (Li2O), and mixtures thereof.

[0155] In some embodiments, the base composition comprises sodium, potassium, or a combination of sodium and potassium. In some embodiments, the sodium content of the base composition ranges from 0-100%, the potassium content ranges from 0-100%, or any combination of sodium and potassium content.

[0156] In some embodiments, the alkaline aluminosilicate solid residue produced by the processing step has a silicon / aluminum (Si:Al) ratio in the range of about 0.8 to 1.8. In some embodiments, the alkaline aluminosilicate solid residue produced by the processing step may have a silicon / aluminum (Si:Al) ratio close to 1.0.

[0157] In some embodiments, the reaction steps are carried out at temperatures ranging from about 150°C to 500°C, about 175°C to 225°C, or about 185°C to 210°C, and at pressures ranging from about 0 to 1500 psig, about 50 to 600 psig, or about 100 to 300 psig for a duration sufficient to leach substantially all of the remaining alkali into an alkali metal solution having the formula M2CO3, where M is the corresponding alkali metal.

[0158] In some implementations, the carbon dioxide produced by this method is essentially reused.

[0159] In another aspect, this disclosure provides a composition comprising an alkali-leached aluminosilicate composition produced according to a method for extracting alkali from silicates under carbon-neutral conditions as described herein.

[0160] In another aspect, this disclosure provides a composition comprising an alkali-leached aluminosilicate composition produced according to a method for extracting alkali from an alkali-containing silicate under carbon-neutral conditions as described herein.

[0161] One or more embodiments include a method for deriving alkali salts from alkali-containing aluminosilicate materials and advantageously utilizing the byproducts. In the most known embodiments, feldspar minerals are the source of the alkali, although only the chemical properties of the material are important, and a wide range of alkali-containing silicate materials may be suitable.

[0162] One or more embodiments include a method for deriving basic salts from an alkaline aluminosilicate material containing a mixture of various basic elements, including but not limited to sodium, potassium, and lithium.

[0163] One embodiment of this disclosure includes a method for obtaining alkali from an alkali-containing feedstock using mild conditions. This method can provide a near-complete yield of useful products from the feedstock. For example, since one unit of feed can be converted into approximately one unit of useful cementitious agent and optional aggregate, all of which are used to produce concrete almost entirely from feldspar rock starting materials, there is no significant waste. Known processes for extracting elements from highly coordinated silicate minerals use strong acids to break down the crystal structure without regard to the recycling or regeneration of the acid reagent. Byproducts or tailings from conventional processes are also often difficult to find valuable uses for. The method of this disclosure can be carried out with relatively mild reagents that can be recycled / regenerated for further use, while the byproducts are useful and intentionally added to low-CO2 cement and concrete. Although the extraction of alkali from silicate minerals has been industrially valuable for at least a century, few economical methods have been able to achieve this due to the inherent difficulties in decomposing silicates (i.e., previously requiring harsh reagents). This method utilizes readily available starting materials, mild reagents, and processing conditions that avoid the handling of harmful reagents and chemicals, and the raw material inputs are abundant and widely distributed globally.

[0164] The method for extracting alkali from alkali-containing aluminosilicates is shown as an open-loop system in Figures 1A and 1C, and as a closed-loop system in Figures 1B and 1D. As an example, a closed-loop scheme for a sodium feldspar-based closed-loop system according to one embodiment of the method for extracting alkali from alkali-containing aluminosilicates of this disclosure is summarized in the process flow diagram of Figure 2, which uses feldspar as an example. Overall, this scheme conforms to the practices of green, closed-loop chemistry. Most importantly, the CO2 generated during roasting is recovered and used in subsequent carbonation steps. Byproducts (such as silica gel) are readily used in the alkali-silicate binder production step, thus significantly reducing energy consumption when silica gel is used instead of quartz in conventional quartz and Na2CO3 roasting. Finally, any mineral byproducts, such as non-feldspar gangue generated during the concentration of alkali-rich feldspar from feldspar ore (e.g., granite), can be used as aggregate in concrete production. Such byproducts should be well characterized and controlled, contributing to a robust, vertically integrated supply chain for cementitious products and aggregate materials. This could be one way to optimize the production value of aggregate mines.

[0165] In the first step, existing mining and metallurgical processes, such as flotation, classification, and magnetic separation, are used to purify and / or enrich alkali-containing aluminosilicates (e.g., potassium feldspar in the most well-known example) from other minerals. If appropriate, the material removed from this process can be used as aggregate.

[0166] In the next step, the alkali-containing aluminosilicate (alkaline feldspar) is calcined with a base (hydroxides, carbonates, bicarbonates, etc. of Na, Li, or K), with Na₂CO₃ being used under optimal conditions. The same results can also be obtained under hydrothermal conditions in a strongly alkaline solution containing the alkali feldspar. After calcination with the alkaline carbonate, a concentrated alkali-silicate solution is obtained by hydrothermal leaching of the solid product and subsequent liquid-solid separation. With two-thirds of the silicon atoms removed, the solid residue has an ideal Si:Al ratio (close to 1), suitable for inorganic polymers; however, aluminum is still bound to an equivalent of the base (i.e., the molar ratio of the base element to aluminum is approximately 1), which can be further extracted to increase the alkali yield.

[0167] Solid alkaline aluminosilicate (Si:Al approximately 1) is bubbled with CO2 at high temperature and pressure until the remaining alkali contained therein is leached into the solution as M2CO3 (where M represents one or more alkali metals), which can be blended with and recovered from the M2CO3 stream formed below. As shown in Figure 2, the final solid residue (which is now kaolinite-like in composition (Al2[Si2O5](OH)4)) is further activated by calcination to produce synthetic metakaolin, which is beneficial for use in concrete (especially inorganic polymer concrete).

[0168] The alkali-silicate solution formed after previous roasting and leaching is then completely leached with CO2 to form solid silica gel, and in the case of a sodium system, Na2CO3 / NaHCO3 is formed in solution. After another solid-liquid separation, the Na2CO3 solution is concentrated and the product is separated by, for example, evaporation crystallization. Most of this Na2CO3 is reintroduced into the roasting step, thus forming a continuous loop of Na2CO3 production and consumption. The collected silica gel can be reacted and combined with the remaining Na2CO3 from the process (i.e., excess Na2CO3 contributed by feldspar) in a roasting and hydrothermal reaction at 175°C–225°C to form basic silicates, or it can be used as an activated silica source in the final cement or concrete, as shown in Figure 4. In some other embodiments, the hydrothermal reaction can be carried out at temperatures in the range of about 150°C–500°C, about 175°C–225°C, or about 185°C–210°C.

[0169] Furthermore, the basic carbonates and basic silicates produced by this method provide valuable raw material sources for other commercial materials, such as glass. These basic silicates and basic carbonates can be used directly as direct substitutes for existing commercial alkali sources. The manufacturing process of soda-lime glass consists of melting raw materials (sodium carbonate, silica, lime, and other magnesium and aluminum minerals) in a glass furnace at a temperature of approximately 1500°C–1700°C. To reduce costs, pure chemicals are often replaced by relatively inexpensive sources such as natural soda ash and quartz sand. However, the method described in this application simultaneously provides silica (SiO2) and sodium carbonate (Na2CO3) as byproducts. In addition, existing soda-lime glass production is also severely affected by the availability of alkali from mining or synthesis processes. Furthermore, both mining and synthesizing soda ash generate significant raw material process CO2 emissions, while this method has the potential to produce scalable, carbon-neutral glass.

[0170] The method described in this paper can also use atmospheric CO2 and / or other CO2 sources as process inputs, thereby sequestering CO2 as a basic carbonate product (if desired). Given that basic carbonates are used as commodity inputs in a variety of downstream products, this could be useful in applications where CO2 in sodium carbonate or potassium carbonate can serve as a long-term carbon sink. In this way, basic carbonates produced using this method can provide pathways for carbon-neutral or carbon-negative derivatives downstream in the supply chain.

[0171] For example, sodium carbonate or potassium carbonate produced by this method can be used to decarbonize certain methods for producing lithium carbonate or lithium hydroxide, such as the analcime process for producing lithium from silicate ores, which is an improvement over previous methods but still incurs one mole of CO2 pollution per mole of lithium produced (due to the use of calcined Ca(OH)2, typically derived from CaCO3). If such methods use CO2-negative sodium carbonate as a feedstock (as is the case with methods applicable herein), it is possible to make the analcime lithium process carbon-neutral. In this case, synthetic analcime waste from lithium production can be treated according to this disclosure to provide a carbon-neutral or carbon-negative source of sodium carbonate, thereby potentially making the lithium extraction process carbon-neutral.

[0172] In some respects, the methods and compositions of this disclosure are suitable for the preparation and use of green commercial alkaline materials. In some embodiments, the green commercial alkaline materials may include, but are not limited to, glass, alkali-silicates, alkali-carbonates, alkali-hydroxides, alkali-oxides, etc. Example

[0173] The following examples are intended to illustrate specific implementations of this disclosure, but are in no way intended to limit the scope of this disclosure. Example 1 Roasting of potassium feldspar with Na2CO3 followed by CO2 leaching of calcium hydroxyl nepheline

[0174] Commercially available potassium feldspar (Custer) is ground to D. 50 The sample was 8 μm thick and thoroughly mixed with Na₂CO₃ (>99.5% purity, 3 molar equivalents), and heated to 900 °C for 2 hours in a furnace on a Hastelloy tray. The resulting molten product was coarsely ground and extracted in an autoclave with deionized (DI) water (liquid-to-solid ratio range of 1–5) at 240 °C for 6 hours. The residue was washed with twice the volume of DI water, and the solids were oven-dried overnight at 105 °C, then characterized by XRD (see Figure 5), SEM-EDX (see Figure 6), and X-ray fluorescence (XRF) (see Table 2 below). The liquid extract (sodium silicate) was quantitatively characterized by ICP (see Table 3), with a total dissolved solids value of 25.6%.

[0175] The solid residue was wet-milled to an average particle size of 10-15 μm, then dissolved in DI water at a liquid-to-solid ratio of 5 (L / S) and placed in a stirred pressure reactor. The slurry was heated to 150-200 °C under stirring (400-1100 rpm) with CO2 at 50-200 psig and continuously bubbled with CO2. Water was continuously introduced to maintain a constant L / S. After a predetermined time, the solids were filtered, washed, dried, and the alkali content was analyzed by SEM-EDX. The leachate from this step was combined and treated with the alkali-silicate leachate from below. Variations in temperature, reaction time, and CO2 pressure were considered during the optimized reaction process (see Figures 7 and 8).

[0176] In another embodiment of alkaline extraction via carbonation, the solid residue discussed above was loaded into a continuous flow (trickling bed) reactor (TBR), and extraction was performed using various parameters. Variations in temperature (150–225 °C), reaction time (6–24 h), water flow rate (0.5–5 ml / min), and CO2 pressure (100–1500 psig) were considered during the optimized reaction process.

[0177] The primary objective of CO2 carbonation is to remove alkali in the form of carbonates for further processing. Surprisingly, the remaining residue is very similar to kaolinite minerals and can be further modified for use as an additive in inorganic polymer cements. Mined kaolinite is typically almost alkali-free, with a Si:Al ratio close to 1. Therefore, the alkali:Al and Si:Al ratios in the leaching residue were used as indicators of carbonation reaction efficiency. As shown in Figure 7, a 12-hour carbonation reaction at 150°C in a stirred reactor resulted in a 90% reduction in alkali content in the residue, as determined by SEM / EDX, while a 17-hour reaction at 150°C resulted in a 91% reduction. No significant difference was observed between the reactions conducted at 150°C and 200°C. The increased pressure input at 200°C was necessary due to the design of the water displacement unit, not due to increased CO2 demand. Preliminary evidence suggests that shorter reactions initially proceed faster than longer reactions. As shown in Figure 8, carbonation in a trickle bed reactor for 24 hours at 200 °C, 400 psi CO2 and a flow rate of 3 ml / min resulted in a 97% reduction in the alkali content of the residue as determined by SEM / EDX (see Figure 9).

[0178] Increasing the CO2 flow rate through the stirred tank reactor resulted in a greater leaching rate, as shown in Figure 8. Increasing the gas flow rate to 5 L / min at 175 °C resulted in leaching 95% of the alkali from the residue within 12 hours. SEM-EDX data showed an alkali:Al ratio of 0.08 (Figure 10), which was confirmed by inductively coupled plasma optical emission spectroscopy (ICP-OES) experiments on a large sample.

[0179] In another embodiment, the calcium hydroxyl nepheline residue was rapidly ground by hand into a coarse powder and placed in a 2L stainless steel reactor equipped with a gas inlet pipe, a top stirrer, and a thermocouple. The residue was suspended in deionized water (0.5–1.5 L), and CO2 was introduced into the reactor under vigorous stirring at a pressure of 100–250 psi. The reactor was heated to 190°C for 4–24 hours. After the reaction was complete, the reactor was cooled to room temperature and the suspension was removed. Aliquots of the sample were filtered through a Buchner funnel, washed with hot deionized water, dried at 100°C, and then analyzed by SEM / EDX. Larger portions of the residue sample could then be decanted and used in further carbonation steps to increase alkali yield, if desired. No further processing of the residue, such as grinding or drying, was required. Figure 8 provides examples of these reactions (curves S and X), showing a high degree of leaching achieved only after three consecutive leaching attempts.

[0180] The residues obtained from the CO2 leaching process were analyzed by SEM-EDX and XRD to verify the presence of synthetic kaolinite as a byproduct of the alkaline leaching reaction (see Figures 10 and 11). The XRD patterns showed the disappearance of the starting material peaks and the appearance of a very broad, amorphous peak at 23°, indicating a kaolinite-like material. Furthermore, no crystalline quartz or nepheline phase was identified in the residues.

[0181] The fully leached solid residues (synthetic kaolinite) from either CO2 leaching process were milled to an average particle size of 10 μm and then further activated by calcination in a furnace at 775 °C for 1.5 h, with heating and cooling times of 1.5 h. Alternatively, the kaolinite could be activated by ultrafast vitrification, with residence times on the order of milliseconds and temperatures ranging from 1000 °C to 1700 °C. These products were characterized by XRD (see Figures 11 and 12) and can be used as a source of metakaolinite for inorganic polymer applications without further processing. The XRD shown in Figure 13 is intended to demonstrate that both calcined CO2 leaching residues possess an amorphous phase similar to high-quality commercial metakaolinite (OptiPozz).

[0182] The liquid sodium silicate formed in the first step is leached by bubbling and stirring the solution with CO2 to remove the alkali until the pH drops from 13 to 9. The first batch of silica is filtered out, rinsed, and the carbonation process is repeated to obtain a second batch at pH 8. The combined silica fraction is dried at 105°C for 3 hours, then heated to 500°C, at which point the water associated with the gel is removed.

[0183] The filtrates from the above steps (a mixture of Na₂CO₃ and NaHCO₃) are combined and concentrated by thermal evaporation to a near-dry slurry, then collected by vacuum filtration and subsequently oven-dried. Alternatively, if a very high purity product is required, the mixture of Na₂CO₃ and NaHCO₃ can be evaporated to a total solids content of 50% (or until the solution is slightly turbid). The warm solution is cooled to 5–10°C, the mixture of Na₂CO₃ and NaHCO₃ is filtered off, and then the evaporation and recrystallization are repeated twice. The composition of the product was analyzed by XRF (see Table 4), and the overall yield was 95%. The loss on ignition (LOI) value likely corresponds to CO₂ and is very close to the expected value assuming equal concentrations of Na₂CO₃ and NaHCO₃. The final liquid containing a small amount of Na₂CO₃ / NaHCO₃ can be used as a flushing stream in accordance with green, closed-loop chemistry practices. The Na₂CO₃ / NaHCO₃ is recycled to the initial feldspar roasting step, and the excess is combined with the silica gel formed above for industrially known alkali-silicate liquid production.

[0184] Finally, inorganic polymer cement can be prepared by combining the alkali-silicate liquid (or derivative) formed in the above steps with synthetic metakaolin. Alternatively, concrete can be formed by adding byproducts or other aggregates to the above-mentioned cementitious agent. Example 2 Roasting of sodium feldspar (Na+) with Na2CO3 followed by CO2 leaching of calcium hydroxyl nepheline

[0185] Albite minerals, measured to be 5-10 cm in size, were pulverized to < 1 mm and mixed with Na₂CO₃ (>99.5% purity, 3 molar equivalents). The mixture was then heated in a furnace on a Hastelloy tray to 950 °C for 1.5 hours. The resulting melt was coarsely ground and extracted in an autoclave with DI water (liquid-to-solid ratio range 1-5) at 225 °C for 12 hours. The residue was washed with twice the volume of DI water, and the solid was oven-dried overnight at 105 °C. The residue was characterized by SEM-EDX (Figure 14).

[0186] The solid residue (approximately 10 g) was coarsely crushed in a mortar and pestle, then dissolved in DI water (750 mL) and placed in a stirred pressure reactor. The slurry was placed under approximately 100 psig CO2 with vigorous stirring (approximately 1000 rpm) and heated to 190°C under CO2 static pressure. After a predetermined time, the solid was filtered, washed with hot deionized water, dried, and the alkali content was analyzed by SEM-EDX (Figure 15), and the present mineral phases were determined by XRD (Figure 16). The leachate from this step was combined and treated with the alkali-silicate leachate from the following examples.

[0187] The residues obtained from the CO2 leaching process were analyzed by SEM-EDX and XRD to verify the presence of kaolinite as a byproduct of the alkaline leaching reaction (see Figure 16). The XRD pattern showed the disappearance of the starting material peaks and the appearance of a very broad, amorphous peak at 23°, indicating a kaolinite sample. Furthermore, no crystalline quartz or nepheline phases were identified in the residues.

[0188] Similar to Example 1, the fully leached solid residue (synthetic kaolinite) from the CO2 leaching process can be activated by calcination in a furnace at 775°C for 1.5 hours, with heating and cooling times of 1.5 hours. Alternatively, kaolinite can be activated by ultrafast vitrification, with residence times on the order of milliseconds and temperatures ranging from 1000°C to 1700°C. These products can be used as a metakaolinite source for inorganic polymer applications without further processing.

[0189] Similar to Example 1, the liquid sodium silicate formed in the first step can be leached with alkali in two stages using low-pressure CO2 to collect silica gel, which is then washed and dried overnight at 200°C.

[0190] The filtrate (a mixture of Na2CO3 and NaHCO3) from the above steps can be concentrated to a nearly dry slurry by thermal evaporation, collected by vacuum filtration, and then dried in an oven.

[0191] Finally, inorganic polymer cement can be prepared by combining the alkali-silicate liquid (or derivative) formed in the above steps with synthetic metakaolin. Alternatively, concrete can be formed by adding byproducts or other aggregates to the above-mentioned cementitious agent. Example 3 Li2CO3 was roasted with α-spodumene and then CO2 was leached.

[0192] Fine, commercially available α-spodumene was thoroughly mixed with Li₂CO₃ (>99.5% purity, 3 molar equivalents) and heated in a furnace on a Hastelloy tray to 900°C for 2 hours. The resulting melt was coarsely ground and extracted in an autoclave with DI water (liquid-to-solid ratio range 1–5) at 240°C for 12 hours. The residue was washed with twice the volume of DI water, and the solid was oven-dried overnight at 105°C and then characterized by XRD (see Figure 17).

[0193] As in Example 1

[0115] , the solid residue discussed above was loaded into a continuous flow trickle-bed reactor (TBR) and extracted under conditions of 225°C, reaction time (18 hours), water flow rate (3 ml / min), and CO2 pressure (600 psig). The residue and starting material were analyzed by peroxide melting ICP-ES and XRD (see Table 5 and Figure 17). A lithium extraction rate of 75% from α-spodumene was achieved through a sequential calcination and high-pressure CO2 process. One reason for the lower-than-quantitative lithium extraction rate is the reported low water solubility of lithium silicate. This step not only limits the initial lithium removal, but incomplete desilication will further limit the extraction of lithium as Li2CO3 during the TBR step. Another potential reason for the lower-than-normal alkali extraction rate is the low solubility of the Li2CO3 product that may remain in the residue. Example 4 Potassium feldspar was hydrothermally leached with NaOH, followed by hydroxyl calcium nepheline leaching with CO2.

[0194] Commercially available potassium feldspar (Custer) is ground to D. 50The sample, with a particle size of 8 μm, was mixed with a solution of NaOH particles (>97.0% purity, 8.5 molar equivalents) dissolved in DI water (L / S ratio of 2). The suspension was heated to 250 °C for 3 hours in a PTFE-lined autoclave, then the mixture was cooled to 50 °C and the residue was filtered off. The resulting solid (calcium hydroxynepheline) was washed with 2 volumes of DI water and dried overnight in an oven at 105 °C, and then characterized by XRD (see Figure 18), SEM (see Figure 19), and SEM-EDX (see Table 6 below).

[0195] The solid residue (calcium hydroxynepheline) was briefly wet-milled to an average particle size of 10 μm, and then the same carbonation step was continued to form kaolinite, followed by metakaolinite. The recovery and utilization of the alkali carbonates will be carried out using the carbonation steps outlined in Example 1. In this case, nitric acid can also be used to form alkali nitrates to achieve the recovery of alkali from the alkali-silicate – thus, (Na,K)OH and nitric acid will be electrochemically regenerated using known methods.

[0196] Finally, inorganic polymer cement and concrete can be formed using aggregates, alkali-silicates, and the synthetic metakaolin formed in the above steps. Example 5 Potassium feldspar was hydrothermally leached with KOH, followed by potassium nepheline leaching with CO2.

[0197] Commercially available potassium feldspar (Custer) is ground to D. 50 The sample, 8 μm in size, was mixed with a solution of KOH particles (>85% purity, 8.5 molar equivalents) dissolved in DI water (L / S ratio 2). The suspension was heated to 250 °C for 3 hours in a PTFE-lined autoclave, then cooled to 50 °C. The resulting residue was filtered off and washed with twice the volume of DI water. The resulting solid (potassium nepheline) was oven-dried overnight at 105 °C and characterized by XRD (see Figure 20) and SEM-EDX (see Figure 21).

[0198] The solid residue (potassium nepheline) was briefly wet-milled to an average particle size of 10 μm, and then the carbonation step employed in Example 1 was continued to form synthetic kaolinite, which in turn formed metakaolinite. In an example of potassium extraction via carbonation, the solid residue discussed above

[0060] was loaded into a continuous flow (trickling bed) reactor (TBR) and extracted using various parameters: temperature 150-225 °C, reaction time (6-24 h), water flow rate (0.5-5 ml / min), and CO2 pressure (200-1500 psig). The resulting solid was oven-dried overnight at 105 °C and then characterized by XRD (see Figure 20) and SEM-EDX (see Figure 22). The recovery and utilization of the alkali carbonate will be carried out as outlined in Example 2. In this case, nitric acid can also be used to form alkali nitrate to recover the alkali from the alkali-silicate – thus, (Na,K)OH and nitric acid will be electrochemically regenerated using known methods.

[0199] Finally, inorganic polymer cement and concrete can be formed using aggregates, alkali-silicates, and metakaolin formed in the above steps. Example 6 Leaching of calcium hydroxyl nepheline (calcined product) with nitric acid and recovery of acid via electrochemical process

[0200] As in Example 1, commercially available potassium feldspar (Custer) was ground to D... 50 The sample was 8 μm thick and thoroughly mixed with Na₂CO₃ (>99.5% purity, 3 molar equivalents), and heated to 900 °C for 2 hours in a furnace on a Hastelloy tray. The resulting melt was coarsely ground and extracted in an autoclave with DI water (liquid-to-solid ratio range 1-5) at 240 °C for 6 hours. The residue was washed with twice the volume of DI water, and the solid was oven-dried overnight at 105 °C, then characterized by XRD, SEM-EDX, and XRF (Example 1). The liquid extract (sodium silicate) was quantitatively characterized by ICP (Example 1).

[0201] The solid residue was dissolved in 0.8 M (1.6 equivalents) nitric acid (L / S ratio 12) and placed in an autoclave at 240 °C for 15 hours. After cooling to 50 °C, the resulting residue was filtered and washed with twice the volume of warm DI water. The resulting solid (synthetic kaolinite) was oven-dried overnight at 105 °C and then characterized by XRD (see Figure 23) and SEM-EDX (see Figure 24 and Table 7 below). Under these conditions, the total alkali remaining in the leaching residue was found to be 0.2%, indicating almost complete alkali extraction.

[0202] As described in Example 1, the fully leachable solid residue (synthetic kaolinite) was ground to an average particle size of 10 μm and then further activated by calcination in a furnace at 775 °C for 1.5 hours, wherein the heating and cooling times were 1.5 hours. The product was characterized by XRD (see Figure 25) and can be used as a metakaolinite source for inorganic polymer applications without further processing.

[0203] In this case, nitric acid can also be used to form alkali nitrate to recover alkali from alkali-silicates - thus (Na,K)OH and nitric acid will be electrochemically regenerated using known methods.

[0204] Finally, inorganic polymer cement and concrete can be formed using aggregates, alkali-silicates, and metakaolin formed in the above steps. Example 7 Leaching of calcium hydroxyl nepheline (a hydrothermal product) with nitric acid and recovery of acid via electrochemical methods

[0205] As in Example 2, commercially available potassium feldspar (Custer) was ground to D... 50 The sample, with a particle size of 8 μm, was mixed with a solution of NaOH particles (>97.0% purity, 8.5 molar equivalents) dissolved in DI water (L / S ratio of 2). The suspension was heated to 250°C for 3 hours in a PTFE-lined autoclave, then the mixture was cooled to 50°C. The resulting residue was filtered off and washed with twice the volume of DI water. The resulting solid was oven-dried overnight at 105°C and characterized by XRD and SEM-EDX (see Example 2).

[0206] The solid residue was dissolved in 1 M (2 equivalents) nitric acid (L / S ratio 12) and placed in an autoclave at 240°C for 15 hours. After cooling to 50°C, the resulting residue was filtered and washed with twice the volume of warm DI water. The resulting solid was oven-dried overnight at 105°C and then characterized by XRD (see Figure 26) and SEM-EDX (see Figure 27). In this case, no residual total alkali was detected (i.e., 0%). Metakaolin can be formed by calcining this residue, as described in Example 1.

[0207] In this case, nitric acid can also be used to form alkali nitrate to recover alkali from alkali-silicates - thus (Na,K)OH and nitric acid will be electrochemically regenerated using known methods.

[0208] Finally, inorganic polymer cement and concrete can be formed using aggregates, alkali-silicates, and metakaolin formed in the above steps. Example 8 Leaching potassium nepheline (a hydrothermal product) with nitric acid and recovering acid via electrochemical methods

[0209] As in Example 3, commercially available potassium feldspar (Custer) was ground to D... 50 The sample was 8 μm thick and mixed with a solution of KOH particles (>85% purity, 8.5 molar equivalents) dissolved in DI water (L / S ratio 2). The suspension was heated to 250°C for 3 hours in a PTFE-lined autoclave, then the mixture was cooled to 50°C, and the resulting residue was filtered off and washed with twice the volume of DI water. The resulting solid was oven-dried overnight at 105°C and then characterized by XRD and SEM-EDX (see Example 2).

[0210] The solid residue was dissolved in 0.8 M (1.6 equivalent) nitric acid (L / S ratio 12) and placed in an autoclave at 240°C for 15 hours. After cooling to 50°C, the resulting residue was filtered and washed with twice the volume of warm DI water. The resulting solid was oven-dried overnight at 105°C and characterized by XRD (see Figure 28) and SEM-EDX (see Figure 29). In this case, the remaining total alkali was 0.82%. Metakaolin can be formed by calcining this residue as described in Example 1.

[0211] In this case, nitric acid can also be used to form alkali nitrate to recover alkali from alkali-silicates - thus (Na / K)OH and nitric acid will be electrochemically regenerated using known methods.

[0212] Finally, inorganic polymer cement and concrete can be formed using aggregates, alkali-silicates, and metakaolin formed in the above steps. Example 9 A highly reactive binder formed from commercial potassium silicate and synthetic metakaolin produced via the TerraCO2 process.

[0213] One g of metakaolin produced by CO2 leaching (e.g., those formed in Example 1) (calcined at 775°C) was vortexed with 1.8 g of potassium silicate (1.7 molar ratio) for 30 seconds, and its heat release was then measured by isothermal calorimetry at 40°C. For comparison, commercially available metakaolin (OptiPozz), known to perform well in inorganic polymer binders, was also prepared and measured in the same manner. The total heat released over time for these CO2 leaching samples is shown in Figure 30. As expected, after calcination at 775°C, both the stirred-reactor and trickle-bed reactor synthesized metakaolin samples produced in Example 1 exhibited comparable or higher total heat release compared to commercial metakaolin (OptiPozz).

[0214] One g of synthetic kaolinite or metakaolinite produced by acid leaching (e.g., those formed in Example 4) (calcined at 600°C or 775°C) was vortexed with 1.8 g of potassium silicate (1.7 molar ratio) for 30 seconds, and its heat release was then measured by isothermal calorimetry at 40°C. For comparison, commercially available metakaolinite (OptiPozz), known for its good performance in inorganic polymer binders, was also prepared and measured in the same manner. The total heat released over time for these acid-leached samples is shown in Figure 31. As expected, both metakaolinite samples produced in Example 4 had a higher total heat release than the precursor synthetic kaolinite, with the sample calcined at 775°C having a higher total heat release than the sample calcined at 600°C. It should also be noted that the synthetic metakaolinite calcined at 775°C had a slightly higher total heat release when compared to commercial metakaolinite. To further demonstrate that the synthetic metakaolinite produced in this example has an atomic structure similar to OptiPozz, 27-aluminum magic angle rotating solid-state NMR (Al0.05) was used. 27 The two samples were compared using MAS SS NMR. Figure 32 shows the 27-Al NMR spectrum, which indicates a similar distribution of Al coordination (Note: the chemical shifts (in ppm) of coordination states IV, V and VI are approximately 57 ppm, 28 ppm and 0 ppm, respectively).

[0215] Advantages of one or more implementation methods include, but are not limited to:

[0216] The widespread availability of feldspar raw materials allows for dispersed production in most parts of the world, while natural sodium carbonate deposits are geographically isolated and strictly controlled, requiring long-distance transportation.

[0217] The original alkali silicate raw material (instead of alkali carbonate raw material) will not generate process CO2.

[0218] Closed-loop process, in line with green chemistry: acids are regenerated (e.g., CO2 / carbonate ring and nitrate / nitrate ring).

[0219] The byproduct Al-Si (synthetic kaolinite or metakaolinite) is also a valuable reagent for inorganic polymers.

[0220] Excess silica gel is a valuable byproduct.

[0221] Electrification or other zero-CO2 energy sources can also be used to power the processes described in these embodiments. The use of green energy, including but not limited to hydropower, solar, and wind power, significantly reduces GHG emissions throughout the process. This energy can be used to power various aspects of the supply chain, including transportation, potentially leading to the complete decarbonization of the production process.

[0222] In one implementation, all components of inorganic polymer concrete can be efficiently produced using granite (or any feldspar-containing rock) (Figure 1). In such an example, cement production and aggregate production can be integrated into a single operation if locally advantageous, and because aggregate is the primary component of concrete, the amount of aggregate produced will always significantly exceed the amount of cement required. The amount of aggregate diverted to cement production needs to be only a small fraction of the existing mine output. Furthermore, the processes of crushing and grading aggregates in mines rarely produce an optimal balance of graded products suitable for the local market—partly due to limitations in crushing equipment. This process can provide an opportunity to increase the value of a portion of the lower-value aggregate fines stream, thereby maximizing the value of the mined material from the aggregate operation.

[0223] For example, to produce 1 m from typical granite 3 The concrete may require 4.6 tons of granite (approximately 1.7 m³). 3 Using natural resources as raw materials, 1.85 tons of graded fine and coarse concrete aggregates, approximately 0.37 tons of cementitious materials (according to this method), and 2.4 tons of additional aggregate products not used in concrete are produced. This is an example of how to produce concrete using minimal amounts of natural resources.

[0224] Considering only cement production (Figure 33), inputting 4.2 tons of typical granite will produce approximately 3.2 tons of aggregate products (mainly the non-alkali portion) and 1 dry ton of inorganic polymer cement.

[0225] A typical input of 1 ton of albite yields approximately 0.46 tons of kaolinite, 0.20 tons of sodium carbonate, and 1.8 tons of silica (in gel or other forms).

[0226] In one implementation, the feedstock can be an alkali-rich product of another industrial process. For example, an analcime-rich waste byproduct from lithium extraction from lithium silicate minerals.

[0227] In one embodiment, the raw material used to prepare the inorganic polymer cement is an inorganic polymer cement (or concrete) of a suitable alkali-aluminosilicate composition. In one type, the concrete aggregate has a composition similar to that of the binder. In another type, the aggregate and binder compositions differ but can be separated during recycling to form two waste streams (one primarily binder, the other primarily aggregate). In this way, the raw material for the cement can consist of recycled cement or concrete from construction and demolition waste. Thus, concrete production can be a fully circular process that uses minimal energy and resources to demolish, regenerate, and recast structures as needed. A non-limiting example of such a system is shown in Figure 34, which reinforces the circular potential of the process; the same concept applies to potassium-based systems and hybrid sodium-potassium systems.

[0228] In one embodiment, the alkali, silica, and kaolinite-like product are used to prepare inorganic polymer cement, which is used for ready-mixed concrete, precast concrete, road surfaces, waste encapsulation or stabilization, cementing, or physical and chemical stabilization of waste materials.

[0229] In one embodiment, the product of this process is used to prepare concrete:

[0230] Various aspects of this disclosure are also described in the following numbered clauses:

[0231] Clause 1. A method for extracting potassium, sodium, or both potassium and sodium from silicates under carbon-neutral conditions, the method comprising: (a) providing a reaction mixture comprising a first reactant and a second reactant, wherein the first reactant comprises a potassium-containing aluminosilicate composition, a sodium-containing aluminosilicate composition, or a mixture thereof, and wherein the second reactant comprises a corresponding potassium-based composition, a sodium-based composition, or a mixture thereof; (b) treating the reaction mixture with a combined activation and leaching process to form a concentrated potassium silicate solution, a sodium silicate solution, or a mixture thereof, and corresponding potassium aluminosilicate solid residues, sodium aluminosilicate solid residues, or a mixture thereof, wherein carbon dioxide is generated by activation as a reusable byproduct carbon dioxide; and (c) reacting the potassium aluminosilicate solid residues, sodium aluminosilicate solid residues, or a mixture thereof with a first portion of the reusable byproduct carbon dioxide to form a potassium-leached aluminosilicate composition, a sodium-leached aluminosilicate composition, or a mixture thereof, thereby extracting potassium, sodium, or a mixture thereof from the corresponding potassium-containing aluminosilicate composition, sodium-containing aluminosilicate composition, or a mixture thereof.

[0232] Clause 2. The method according to Clause 1, wherein the activation process is selected from the group consisting of: thermal activation, hydrothermal activation, chemical activation, mechanochemical activation, radiation activation, electromagnetic activation and electrochemical activation.

[0233] Clause 3. The method according to Clause 2, wherein heating includes heating at a temperature in the range of about 850°C-1100°C, about 900°C-1050°C, or about 950°C-1000°C, and the dwell time is in the range of about 0.25-4 hours, about 0.5-1.5 hours, or about 0.75-1.25 hours.

[0234] Clause 4. The method according to Clause 2, wherein the activation process is a hydrothermal process, and wherein the hydrothermal process includes heating at a temperature in the range of about 150°C-275°C, about 175°C-250°C, or about 200°C-225°C, with a residence time in the range of about 1-72 hours, about 8-24 hours, or about 12-18 hours.

[0235] Clause 5. The method according to Clause 1, wherein the potassium-containing aluminosilicate composition and the sodium-containing aluminosilicate composition contain feldspar.

[0236] Clause 6. The method according to Clause 5, wherein the feldspar is selected from the group consisting of alkali feldspar and plagioclase.

[0237] Clause 7. The method according to Clause 5, wherein the feldspar is selected from the group consisting of: orthoclase, sancite, microcline, anisoclase, albite, orthoclase, andesine, labradorite, dextrose, anorthoclase, and aorthite, and mixtures or solid solutions thereof.

[0238] Clause 8. The method according to Clause 1, wherein the potassium-containing aluminosilicate composition and the sodium-containing aluminosilicate composition comprise feldspar-like minerals selected from the group consisting of: nepheline, potassium nepheline, sodalite, leucite, lapis lazuli, calcium nepheline, etc.

[0239] Clause 9. The method according to Clause 1, wherein the potassium-containing aluminosilicate composition and the sodium-containing aluminosilicate composition comprise a zeolite supergroup mineral comprising zeolites selected from the group consisting of: analcime, chalcogenide, clinoptilolite, mordenite, mordenite, calcium cross-shaped zeolite, magnesium alkali zeolite, sodium zeolite, octahedral zeolite, etc.

[0240] Clause 10. The method according to Clause 1, wherein the potassium-containing aluminosilicate composition and the sodium-containing aluminosilicate composition comprise mica and clay minerals, wherein the mica and clay minerals are selected from the group consisting of: muscovite, biotite, phlogopite, montmorillonite, illite, vermiculite, saponite, lepidolite, hydropyrite, etc.

[0241] Clause 11. The method according to Clause 1, wherein the potassium-based composition comprises potassium (K), potassium hydroxide (KOH), potassium carbonate (K2CO3), potassium oxide (K2O) and mixtures thereof.

[0242] Clause 12. The method according to Clause 1, wherein the sodium-based composition comprises sodium (Na), sodium hydroxide (NaOH), sodium carbonate (Na2CO3), sodium oxide (Na2O), and mixtures thereof.

[0243] Clause 13. The method according to Clause 1, wherein the mixture of potassium-based composition and sodium-based composition comprises a mixture of two or more compositions selected from the group consisting of: potassium (K), potassium hydroxide (KOH), potassium carbonate (K2CO3), potassium oxide (K2O), sodium (Na), sodium hydroxide (NaOH), sodium carbonate (Na2CO3), sodium oxide (Na2O), and mixtures thereof.

[0244] Clause 14. The method according to Clause 1, wherein the potassium aluminosilicate solid residue, sodium aluminosilicate solid residue, or mixture thereof produced by the processing step has a silicon / aluminum (Si:Al) ratio in the range of about 0.8 to 1.8.

[0245] Clause 15. The method according to Clause 1, wherein the reaction steps are carried out at a temperature in the range of about 150°C to 500°C, about 175°C to 225°C, or about 185°C to 210°C, at a pressure in the range of about 0 to 1500 psig, about 50 to 600 psig, or about 100 to 300 psig, for a time sufficient to leach substantially all of the remaining alkali into an alkali metal solution having the formula M2CO3, wherein M is the corresponding alkali metal.

[0246] Clause 16. The method of Clause 1, wherein the carbon dioxide produced by the method is substantially reused.

[0247] Clause 17. A composition comprising a potassium, sodium, or potassium and sodium leached aluminosilicate composition produced by any one of Clauses 1-16.

[0248] Clause 18. A composition comprising potassium, sodium, or a combination of potassium and sodium produced by any one of Clauses 1-16.

[0249] Clause 19. A composition comprising an alkaline product produced by any one of Clauses 1-16, wherein the alkaline product is selected from the group consisting of alkaline carbonates, alkaline silicates, etc.

[0250] Clause 20. A method for extracting an alkali from a silicate under carbon-neutral conditions while forming an activated synthetic kaolinite composition, the method comprising: (a) providing a reaction mixture comprising an alkali-containing aluminosilicate composition and an alkali composition; (b) treating the reaction mixture with a combined activation and leaching process to form a concentrated alkali-silicate solution and an alkaline aluminosilicate solid residue, wherein carbon dioxide is generated by activation as a reusable byproduct carbon dioxide; (c) reacting the alkaline aluminosilicate solid residue with a first portion of the reusable byproduct carbon dioxide to form an alkali-leached aluminosilicate composition, thereby extracting the alkali from the alkali-containing aluminosilicate composition; and (d) activating the alkali-leached aluminosilicate composition to form an activated synthetic kaolinite composition.

[0251] Clause 21. The method according to Clause 20, wherein activation includes a process of increasing reactivity selected from the group consisting of: thermal activation, chemical activation, radiation activation, electromagnetic activation, electrochemical activation, and mechanical energy treatment.

[0252] Clause 22. The method according to Clause 20, wherein the activated synthetic kaolinite composition comprises metakaolinite, vitrified kaolinite, calcined kaolinite, rapidly calcined kaolinite, activated clay or a combination thereof with a Si:Al ratio in the range of about 0.5 to 1.5.

[0253] Clause 23. The method described in accordance with Clause 20, wherein the carbon dioxide produced by the method is substantially reused.

[0254] Clause 24. The method according to Clause 20, wherein the reaction steps are carried out at a temperature in the range of about 150°C to 500°C, about 175°C to 225°C, or about 185°C to 210°C, at a pressure in the range of about 0 to 1500 psig, about 50 to 600 psig, or about 100 to 300 psig, for a duration sufficient to leach substantially all of the remaining alkali into an alkali metal solution having a formula selected from the group consisting of M2CO3, MOH, and M2O, wherein M is the corresponding alkali metal.

[0255] Clause 25. The method according to Clause 24 further comprises: concentrating, crystallizing, separating and / or converting the alkali metal solution to form an alkali metal solid having a formula selected from the group consisting of M2CO3, MOH and M2O, wherein M is the corresponding alkali metal.

[0256] Clause 26. The method according to Clause 25 further comprises: reintroducing at least a portion of the alkali metal solid as a base composition into the processing step, thereby forming a continuous loop of base composition production and consumption.

[0257] Clause 27. The method according to Clause 20 further comprises: reacting a concentrated alkali-silicate solution with a second portion of reusable byproduct carbon dioxide to form solid silica gel and an alkali-carbonate solution.

[0258] Clause 28. The method according to Clause 27, wherein the solid silica gel comprises silica (SiO2) in a concentration range of about 75-100 wt%.

[0259] Clause 29. The method according to Clause 27, wherein the solid silica gel is repeatedly used to react or combine with a base composition to form an alkaline silicate or as an activated silica source for the production of inorganic polymer cement, or wherein the solid silica gel is repeatedly used to react or combine with an alkaline-silicate composition.

[0260] Clause 30. The method according to Clause 27, wherein the alkali-carbonate solution contains M2CO3, the concentration of M2CO3 in water being in the range of 1-40 wt / wt%, where M is the corresponding alkali metal.

[0261] Clause 31. The method according to Clause 27 further comprises: separating an alkaline carbonate composition from an alkaline-carbonate solution; and combining solid silica gel and the separated alkaline carbonate composition to form an alkaline-silicate liquid.

[0262] Clause 32. The method according to Clause 31, wherein the alkali-silicate liquid comprises silicon dioxide (SiO2) in a concentration range of about 10-50 wt%, and comprises SiO2:M2O in a weight ratio range of about 1.0-4.0.

[0263] Clause 33. The method according to Clause 31 further comprises: treating the alkali-silicate liquid to form a separated alkali-silicate solid product.

[0264] Clause 34. A composition comprising an activated synthetic kaolinite composition produced according to any one of Clauses 20-23.

[0265] Clause 35. A composition comprising an alkaline carbonate liquid produced according to any one of Clauses 20-23.

[0266] Clause 36. A composition comprising a solid product produced according to any one of Clauses 20-23.

[0267] Clause 37. A composition comprising an alkali-silicate liquid produced by any one of Clauses 31-32.

[0268] Clause 38. A composition comprising an alkali-silicate solid product produced according to the method described in Clause 33.

[0269] Clause 39. A method for preparing inorganic polymer cement, comprising: providing an activated synthetic kaolinite composition produced according to the method of Clause 20; and using the activated synthetic kaolinite composition as a reagent to form inorganic polymer cement.

[0270] Clause 40. A composition comprising an inorganic polymer cement produced according to the method described in Clause 39.

[0271] Clause 41. A method for preparing inorganic polymer concrete, the method comprising: providing inorganic polymer cement according to Clause 40; and combining the inorganic polymer cement with a solid aggregate composition and an optional filler composition to form inorganic polymer concrete, wherein, based on the inorganic polymer concrete, the inorganic polymer is present in an amount ranging from 1 to 44 wt%, the solid aggregate composition is present in an amount ranging from 55 to 95 wt%, and the optional filler composition is present in an amount ranging from 1 to 20 wt%.

[0272] Clause 42. The method according to Clause 41, wherein the optional packing composition is selected from the group consisting of: reactive packings, inert packings, and combinations thereof.

[0273] Clause 43. The method according to Clause 41, wherein the solid aggregate composition is selected from the group consisting of: coarse aggregate, medium aggregate, fine aggregate, lightweight aggregate, engineered aggregate, artificial aggregate, angular aggregate, round aggregate, water-worn aggregate, recycled aggregate, stone, sand, natural rock, industrial by-products, alkaline aluminosilicate, feldspar, etc.

[0274] Clause 44. A composition comprising inorganic polymer concrete produced according to any one of Clauses 41-43.

[0275] Clause 45. A method for extracting an alkali from an alkaline silicate under carbon-neutral conditions, the method comprising: (a) providing a reaction mixture comprising an alkaline aluminosilicate composition and a base composition, the base composition containing an alkali contained in the alkaline aluminosilicate; (b) treating the reaction mixture with a combined activation and leaching process to form a concentrated alkali-silicate solution and an alkaline aluminosilicate solid residue, wherein carbon dioxide is generated by activation as a reusable byproduct carbon dioxide; and (c) reacting the alkaline aluminosilicate solid residue with a first portion of the reusable byproduct carbon dioxide to form an alkali-leached aluminosilicate composition, thereby extracting the alkali from the alkaline aluminosilicate composition.

[0276] Clause 46. The method according to Clause 45, wherein the activation process is selected from the group consisting of: thermal activation, hydrothermal activation, chemical activation, mechanochemical activation, radiation activation, electromagnetic activation and electrochemical activation.

[0277] Clause 47. The method according to Clause 46, wherein heating comprises heating at a temperature in the range of about 850°C-1100°C, about 900°C-1050°C, or about 950°C-1000°C, with a dwell time in the range of about 0.25-4 hours, about 0.5-1.5 hours, or about 0.75-1.25 hours.

[0278] Clause 48. The method according to Clause 46, wherein the activation process is a hydrothermal process, and wherein the hydrothermal process includes heating at a temperature in the range of about 150°C-275°C, about 175°C-250°C, or about 200°C-225°C, with a residence time in the range of about 1-72 hours, about 8-24 hours, or about 12-18 hours.

[0279] Clause 49. The method according to Clause 45, wherein the alkali-containing aluminosilicate composition comprises feldspar.

[0280] Clause 50. The method according to Clause 49, wherein the feldspar is selected from the group consisting of alkali feldspar and plagioclase.

[0281] Clause 51. The method according to Clause 49, wherein the feldspar is selected from the group consisting of: orthoclase, sancite, microcline, anisoclase, albite, orthoclase, andesine, labradorite, dextrose, anorthoclase, and anorthoclase, and mixtures or solid solutions thereof.

[0282] Clause 52. The method according to Clause 45, wherein the alkali-containing aluminosilicate composition comprises feldspar-like minerals selected from the group consisting of: nepheline, potassium nepheline, sodalite, leucite, lapis lazuli, calcium nepheline, etc.

[0283] Clause 53. The method according to Clause 45, wherein the alkali-containing aluminosilicate composition comprises a zeolite supergroup mineral, the zeolite supergroup mineral comprising zeolites selected from the group consisting of: analcime, chalcogenide, clinoptilolite, mordenite, mordenite, calcium cross-shaped zeolite, magnesium alkali zeolite, sodium zeolite, octahedral zeolite, etc.

[0284] Clause 54. The method according to Clause 45, wherein the alkali-containing aluminosilicate composition comprises mica and clay minerals, wherein the mica and clay minerals are selected from the group consisting of: muscovite, biotite, phlogopite, montmorillonite, illite, vermiculite, soapstone, lepidolite, hydropyrite, etc.

[0285] Clause 55. The method according to Clause 45, wherein the alkali-containing aluminosilicate composition comprises spodumene, lepidolite, hydropyrite, nepheline, and / or jadalite.

[0286] Clause 56. The method according to Clause 45, wherein the base composition comprises an alkali metal selected from the group consisting of sodium (Na), potassium (K), lithium (Li), and mixtures thereof.

[0287] Clause 57. The method according to Clause 45, wherein the base composition is selected from the group consisting of sodium hydroxide (NaOH), potassium hydroxide (KOH), lithium hydroxide (LiOH), and mixtures thereof.

[0288] Clause 58. The method according to Clause 45, wherein the base composition is selected from the group consisting of sodium carbonate (Na2CO3), potassium carbonate (K2CO3), lithium carbonate (Li2CO3), and mixtures thereof.

[0289] Clause 59. The method according to Clause 45, wherein the base composition is selected from the group consisting of sodium oxide (Na2O), potassium oxide (K2O), lithium oxide (Li2O), and mixtures thereof.

[0290] Clause 60. The method according to Clause 45, wherein the base composition is selected from the group consisting of sodium bicarbonate (NaHCO3), potassium bicarbonate (KHCO3), lithium bicarbonate (LiHCO3), and mixtures thereof.

[0291] Clause 61. The method according to Clause 45, wherein the alkaline aluminosilicate solid residue produced by the processing step has a silicon / aluminum (Si:Al) ratio in the range of about 0.8 to 1.8.

[0292] Clause 62. The method according to Clause 45, wherein the reaction steps are carried out at a temperature in the range of about 150°C to 500°C, about 175°C to 225°C, or about 185°C to 210°C, at a pressure in the range of 0 to 1500 psig, about 50 to 600 psig, or about 100 to 300 psig, for a duration sufficient to leach substantially all remaining alkali into an alkali metal solution having a composition selected from the group consisting of M2CO3, MOH, and M2O, wherein M is the corresponding alkali metal.

[0293] Clause 63. The method described in accordance with Clause 45, wherein the carbon dioxide produced by the method is substantially reused.

[0294] Clause 64. A composition comprising an alkaline-leached aluminosilicate composition produced by any one of Clauses 45-63.

[0295] This document contains headings for reference and to help locate certain sections. These headings are not intended to limit the scope of the concepts described herein, and these concepts may be applicable throughout other parts of the specification. Therefore, this disclosure is not intended to be limited to the embodiments shown herein, but should be given the widest scope consistent with the principles and novel features disclosed herein.

[0296] Unless the context clearly indicates otherwise, the singular forms “a / an” and “the” include the corresponding plural references.

[0297] Unless otherwise stated, all figures representing amounts of components, reaction conditions, concentrations, properties, etc., as used in this specification and claims should be understood to be modified by the term "about" in all cases. At a minimum, each numerical parameter should be interpreted based on at least the number of significant figures reported and by applying conventional rounding techniques. Therefore, unless stated to the contrary, the numerical parameters set forth in this specification and the appended claims are approximate values ​​and may vary depending on the properties sought. Although the numerical ranges and parameters illustrating a broad range of embodiments are approximate, the values ​​set forth in specific embodiments are reported as accurately as possible. However, any numerical value inherently contains some error due to differences in experimental, test measurements, statistical analyses, etc.

[0298] It should be understood that the embodiments and implementations described herein are for illustrative purposes only, and those skilled in the art will make various modifications or changes based on them, which will be included within the scope of this disclosure and the appended claims. Those skilled in the art will recognize that any process or method disclosed herein can be modified in many ways. The process parameters and order of steps described and / or illustrated herein are given by way of example only and can be varied as needed. For example, although the steps shown and / or described herein may be shown or discussed in a particular order, these steps do not necessarily need to be performed in the order shown or discussed.

[0299] The various exemplary methods described and / or illustrated herein may omit one or more of the steps described or illustrated herein, or include additional steps beyond those disclosed. Furthermore, the steps of any method disclosed herein may be combined with any one or more steps of any other method disclosed herein.

[0300] Unless otherwise stated, the terms “connected to” and “coupled to” (and their derivatives) as used in this specification and claims shall be construed as allowing both direct and indirect (i.e., via other elements or components) connections. Furthermore, the term “a (or an)” as used in this specification and claims shall be construed as meaning “at least one”. Finally, for ease of use, the terms “comprising” and “having” (and their derivatives) as used in this specification and claims are interchangeable and shall have the same meaning as the word “including”.

[0301] The processor disclosed herein can be configured to perform one or more steps of any of the methods disclosed herein via instructions.

[0302] As used in this article, the term “or” is used in an inclusive sense, referring to any one of a number of options or a combination thereof.

[0303] As used in this article, characters such as numbers refer to similar elements.

[0304] Embodiments of this disclosure have been shown and described herein, and are provided by way of example only. Many modifications, alterations, variations, and substitutions will be recognized by those skilled in the art without departing from the scope of this disclosure. Several alternatives and combinations of the embodiments disclosed herein may be utilized without departing from the scope of this disclosure and the invention disclosed herein. Therefore, the scope of the invention currently disclosed should be defined only by the scope of the appended claims and their equivalents.

Claims

1. A method for extracting potassium, sodium, or both potassium and sodium, from silicates under carbon-neutral conditions, the method comprising: (a) A reaction mixture comprising a first reactant and a second reactant, wherein the first reactant comprises a potassium-containing aluminosilicate composition, a sodium-containing aluminosilicate composition or a mixture thereof, and wherein the second reactant comprises a corresponding potassium-based composition, a sodium-based composition or a mixture thereof; (b) The reaction mixture is treated with a combined activation and leaching process to form a concentrated potassium silicate solution, a sodium silicate solution, or a mixture thereof, and corresponding potassium aluminosilicate solid residues, sodium aluminosilicate solid residues, or mixtures thereof, wherein carbon dioxide is generated by activation as a reusable byproduct; and (c) Reacting a potassium aluminosilicate solid residue, a sodium aluminosilicate solid residue, or a mixture thereof with a first portion of the reusable byproduct carbon dioxide to form a potassium-leached aluminosilicate composition, a sodium-leached aluminosilicate composition, or a mixture thereof, thereby extracting potassium, sodium, or a mixture thereof from the respective potassium-containing aluminosilicate composition, sodium-containing aluminosilicate composition, or a mixture thereof.

2. The method according to claim 1, wherein the activation process is selected from the group consisting of: thermal activation, hydrothermal activation, chemical activation, mechanochemical activation, radiation activation, electromagnetic activation, and electrochemical activation.

3. The method according to claim 2, wherein the heating comprises heating at a temperature in the range of about 850°C-1100°C, about 900°C-1050°C, or about 950°C-1000°C, and the dwell time is in the range of about 0.25-4 hours, about 0.5-1.5 hours, or about 0.75-1.25 hours.

4. The method according to claim 2, wherein the activation process is a hydrothermal process, and wherein the hydrothermal process includes heating at a temperature in the range of about 150°C-275°C, about 175°C-250°C, or about 200°C-225°C, and the residence time is in the range of about 1-72 hours, about 8-24 hours, or about 12-18 hours.

5. The method according to claim 1, wherein the potassium-containing aluminosilicate composition and the sodium-containing aluminosilicate composition comprise feldspar.

6. The method according to claim 5, wherein the feldspar is selected from the group consisting of alkali feldspar and plagioclase.

7. The method according to claim 5, wherein the feldspar is selected from the group consisting of: orthoclase, sancite, microcline, anisoclase, albite, orthoclase, andesine, labradorite, dalite, anorthoclase, and albite, and mixtures thereof or solid solutions thereof.

8. The method according to claim 1, wherein the potassium-containing aluminosilicate composition and the sodium-containing aluminosilicate composition comprise feldspar-like minerals selected from the group consisting of: nepheline, potassium nepheline, sodalite, leucite, lapis lazuli, calcium nepheline, etc.

9. The method according to claim 1, wherein the potassium-containing aluminosilicate composition and the sodium-containing aluminosilicate composition comprise zeolite supergroup minerals, wherein the zeolite supergroup minerals comprise zeolites selected from the group consisting of: analcime, chalcogenide, clinoptilolite, mordenite, mordenite, calcium cruciformite, magnesium alkali zeolite, sodium zeolite, octahedralite, etc.

10. The method according to claim 1, wherein the potassium-containing aluminosilicate composition and the sodium-containing aluminosilicate composition comprise mica and clay minerals, wherein the mica and clay minerals are selected from the group consisting of: muscovite, biotite, phlogopite, montmorillonite, illite, vermiculite, saponite, lepidolite, hydropyrite, etc.

11. The method of claim 1, wherein the potassium-based composition comprises selected from the group consisting of potassium (K), potassium hydroxide (KOH), potassium carbonate (K2CO3), potassium oxide (K2O), and mixtures thereof.

12. The method of claim 1, wherein the sodium-based composition comprises sodium selected from the group consisting of sodium (Na), sodium hydroxide (NaOH), sodium carbonate (Na2CO3), sodium oxide (Na2O), and mixtures thereof.

13. The method of claim 1, wherein the mixture of the potassium-based composition and the sodium-based composition comprises a mixture of two or more compositions selected from the group consisting of: potassium (K), potassium hydroxide (KOH), potassium carbonate (K2CO3), potassium oxide (K2O), sodium (Na), sodium hydroxide (NaOH), sodium carbonate (Na2CO3), sodium oxide (Na2O), and mixtures thereof.

14. The method of claim 1, wherein the potassium aluminosilicate solid residue, sodium aluminosilicate solid residue, or mixture thereof produced by the processing step has a silicon / aluminum (Si:Al) ratio in the range of about 0.8-1.

8.

15. The method of claim 1, wherein the reaction steps are carried out at a temperature in the range of about 150°C-500°C, about 175°C-225°C, or about 185°C-210°C, at a pressure in the range of about 0-1500 psig, about 50-600 psig, or about 100-300 psig, for a duration sufficient to leach substantially all remaining alkali into an alkali metal solution having the formula M2CO3, wherein M is the corresponding alkali metal.

16. The method of claim 1, wherein the carbon dioxide produced by the method is substantially reused.

17. A composition comprising a potassium, sodium, or potassium and sodium leached aluminosilicate composition produced by any one of claims 1-16.

18. A composition comprising potassium, sodium, or a combination of potassium and sodium produced by the method according to any one of claims 1-16.

19. A composition comprising an alkaline product produced by the method according to any one of claims 1-16, wherein the alkaline product is selected from the group consisting of alkaline carbonates, alkaline silicates, etc.

20. A method for extracting an alkali from a silicate under carbon-neutral conditions, simultaneously forming an activated synthetic kaolinite composition, the method comprising: (a) A reaction mixture comprising an alkaline aluminosilicate composition and a base composition; (b) The reaction mixture is treated with a combination of activation and leaching processes to form a concentrated alkali-silicate solution and an alkaline aluminosilicate solid residue, wherein carbon dioxide is generated by activation as a reusable byproduct. (c) The alkaline aluminosilicate solid residue is reacted with a first portion of the reusable byproduct carbon dioxide to form an alkaline-leached aluminosilicate composition, thereby extracting alkali from the alkaline-containing aluminosilicate composition; as well as (d) Activate the alkaline-leached aluminosilicate composition to form an activated synthetic kaolinite composition.

21. The method of claim 20, wherein activation comprises a process of increasing reactivity selected from the group consisting of: thermal activation, hydrothermal activation, chemical activation, mechanochemical activation, radiation activation, electromagnetic activation, and electrochemical activation.

22. The method of claim 20, wherein the activated synthetic kaolinite composition comprises metakaolinite, vitrified kaolinite, calcined kaolinite, rapidly calcined kaolinite, activated clay or a combination thereof with a Si:Al ratio in the range of about 0.5-1.

5.

23. The method of claim 20, wherein the carbon dioxide produced by the method is substantially reused.

24. The method of claim 20, wherein the reaction steps are carried out at a temperature in the range of about 150°C-500°C, about 175°C-225°C, or about 185°C-210°C, at a pressure in the range of about 0-1500 psig, about 50-600 psig, or about 100-300 psig, for a duration sufficient to leach substantially all remaining alkali into an alkali metal solution having a formula selected from the group consisting of M2CO3, MOH, and M2O, wherein M is the corresponding alkali metal.

25. The method of claim 24, further comprising: The alkali metal solution is concentrated, crystallized, separated and / or transformed to form an alkali metal solid having a formula selected from the group consisting of M2CO3, MOH and M2O, where M is the corresponding alkali metal.

26. The method of claim 25, further comprising: At least a portion of the alkali metal solid is reintroduced into the processing step as the base composition, thereby forming a continuous loop of base composition production and consumption.

27. The method of claim 20, further comprising: The concentrated alkali-silicate solution is reacted with a second portion of the reusable byproduct carbon dioxide to form solid silica gel and an alkali-carbonate solution.

28. The method of claim 27, wherein the solid silica gel comprises silicon dioxide (SiO2) in a concentration range of about 75-100 wt%.

29. The method of claim 27, wherein the solid silica gel is repeatedly used to react or combine with the base composition to form an alkaline silicate or as an activated silica source for the production of inorganic polymer cement, or wherein the solid silica gel is repeatedly used to react or combine with the alkali-silicate composition.

30. The method of claim 27, wherein the alkali-carbonate solution comprises M2CO3, the concentration of M2CO3 in water being in the range of 1-40 wt / wt%, wherein M is the corresponding alkali metal.

31. The method of claim 27, further comprising: Separate the alkaline carbonate composition from the alkaline-carbonate solution; as well as The solid silica gel and the separated alkaline carbonate composition are combined to form an alkaline silicate liquid.

32. The method of claim 31, wherein the alkali-silicate liquid comprises silicon dioxide (SiO2) in a concentration range of about 10-50 wt%, and comprises SiO2:M2O in a weight ratio range of about 1.0-4.

0.

33. The method of claim 31, further comprising: The alkali-silicate liquid is processed to form a separated alkali-silicate solid product.

34. A composition comprising an activated synthetic kaolinite composition produced by any one of claims 20-23.

35. A composition comprising an alkaline carbonate liquid produced according to any one of claims 20-23.

36. A composition comprising the solid product produced according to any one of claims 20-23.

37. A composition comprising an alkali-silicate liquid produced by the method according to any one of claims 31-32.

38. A composition comprising an alkali-silicate solid product produced by the method according to claim 33.

39. A method for preparing inorganic polymer cement, comprising: Provides an activated synthetic kaolinite composition produced by the method according to claim 20; as well as An activated synthetic kaolinite composition was used as a reagent to form inorganic polymer cement.

40. A composition comprising an inorganic polymer cement produced by the method according to claim 39.

41. A method for preparing inorganic polymer concrete, the method comprising: Provide the inorganic polymer cement according to claim 40; as well as The inorganic polymer cement is combined with a solid aggregate composition and an optional filler composition to form inorganic polymer concrete. The inorganic polymer concrete is provided in an amount ranging from 1 to 44 wt%, the solid aggregate composition is provided in an amount ranging from 55 to 95 wt%, and the optional filler composition is provided in an amount ranging from 1 to 20 wt%.

42. The method of claim 41, wherein the optional filler composition is selected from the group consisting of reactive fillers, inert fillers, and combinations thereof.

43. The method according to claim 41, wherein the solid aggregate composition is selected from the group consisting of: coarse aggregate, medium aggregate, fine aggregate, lightweight aggregate, engineered aggregate, artificial aggregate, angular aggregate, round aggregate, water-worn aggregate, recycled aggregate, stone, sand, natural rock, industrial by-products, alkaline aluminosilicate, feldspar, etc.

44. A composition comprising inorganic polymer concrete produced by the method according to any one of claims 41-43.

45. A method for extracting a base from a base-containing silicate under carbon-neutral conditions, the method comprising: (a) A reaction mixture comprising an alkaline aluminosilicate composition and a base composition, wherein the base composition comprises an alkaline substance contained in the alkaline aluminosilicate; (b) The reaction mixture is treated with a combined activation and leaching process to form a concentrated alkali-silicate solution and an alkaline aluminosilicate solid residue, wherein carbon dioxide is generated by activation as a reusable byproduct; and (c) The alkaline aluminosilicate solid residue is reacted with a first portion of the reusable byproduct carbon dioxide to form an alkaline-leached aluminosilicate composition, thereby extracting alkali from the alkaline-containing aluminosilicate composition.

46. ​​The method according to claim 45, wherein the activation process is selected from the group consisting of: thermal activation, hydrothermal activation, chemical activation, mechanochemical activation, radiation activation, electromagnetic activation, and electrochemical activation.

47. The method of claim 46, wherein heating comprises heating at a temperature in the range of about 850°C-1100°C, about 900°C-1050°C, or about 950°C-1000°C, and the dwell time is in the range of about 0.25-4 hours, about 0.5-1.5 hours, or about 0.75-1.25 hours.

48. The method of claim 46, wherein the activation process is a hydrothermal process, and wherein the hydrothermal process comprises heating at a temperature in the range of about 150°C-275°C, about 175°C-250°C, or about 200°C-225°C, and a residence time in the range of about 1-72 hours, about 8-24 hours, or about 12-18 hours.

49. The method of claim 45, wherein the alkali-containing aluminosilicate composition comprises feldspar.

50. The method according to claim 49, wherein the feldspar is selected from the group consisting of alkali feldspar and plagioclase.

51. The method according to claim 49, wherein the feldspar is selected from the group consisting of: orthoclase, sancite, microcline, anisoclase, albite, orthoclase, andesine, labradorite, dalite, anorthoclase, and mixtures or solid solutions thereof.

52. The method according to claim 45, wherein the alkali-containing aluminosilicate composition comprises feldspar-like minerals selected from the group consisting of: nepheline, potassium nepheline, sodalite, leucite, lapis lazuli, calcium nepheline, etc.

53. The method according to claim 45, wherein the alkali-containing aluminosilicate composition comprises a supergroup of zeolites, the supergroup of zeolites comprising zeolites selected from the group consisting of: analcime, chalcogenide, clinoptilolite, mordenite, mordenite, calcium cruciformite, magnesium alkali zeolite, sodium zeolite, octahedralite, etc.

54. The method according to claim 45, wherein the alkali-containing aluminosilicate composition comprises mica and clay minerals, wherein the mica and clay minerals are selected from the group consisting of: muscovite, biotite, phlogopite, montmorillonite, illite, vermiculite, saponite, lepidolite, hydropyrite, etc.

55. The method of claim 45, wherein the alkaline aluminosilicate composition comprises spodumene, lepidolite, hydropyrite, nepheline, and / or jadalite.

56. The method of claim 45, wherein the base composition comprises an alkali metal selected from the group consisting of sodium (Na), potassium (K), lithium (Li), and mixtures thereof.

57. The method according to claim 45, wherein the base composition is selected from the group consisting of sodium hydroxide (NaOH), potassium hydroxide (KOH), lithium hydroxide (LiOH), and mixtures thereof.

58. The method according to claim 45, wherein the base composition is selected from the group consisting of sodium carbonate (Na2CO3), potassium carbonate (K2CO3), lithium carbonate (Li2CO3), and mixtures thereof.

59. The method according to claim 45, wherein the base composition is selected from the group consisting of sodium oxide (Na2O), potassium oxide (K2O), lithium oxide (Li2O), and mixtures thereof.

60. The method according to claim 45, wherein the base composition is selected from the group consisting of sodium bicarbonate (NaHCO3), potassium bicarbonate (KHCO3), lithium bicarbonate (LiHCO3), and mixtures thereof.

61. The method of claim 45, wherein the alkaline aluminosilicate solid residue produced by the processing step has a silicon / aluminum (Si:Al) ratio in the range of about 0.8 to 1.

8.

62. The method of claim 45, wherein the reaction steps are carried out at a temperature in the range of about 150°C-500°C, about 175°C-225°C, or about 185°C-210°C, at a pressure in the range of 0-1500 psig, about 50-600 psig, or about 100-300 psig, for a duration sufficient to leach substantially all remaining alkali into an alkali metal solution having a formula selected from the group consisting of M2CO3, MOH, and M2O, wherein M is the corresponding alkali metal.

63. The method of claim 45, wherein the carbon dioxide produced by the method is substantially reused.

64. A composition comprising an alkaline-leached aluminosilicate composition produced by any one of claims 45-63.

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