Multi-metal catalyst

Abstract

The present disclosure includes a catalyst, including an electrocatalyst. Mixed metal electrocatalyst materials may include Ru, W, Mo, and / or Pd, which may be applied to reduce the need for Ir while exhibiting desirable properties. Further, a method of catalytic reaction may include: providing a multi-metal material comprising at least two metals, where a first metal is Ir and one or more other metals are from the group consisting of W, Mo, Re, Ru, Fe, Pd, Rh, Mn, and Cr; the multi-metal material is used as a catalyst in the reaction.

Description

Technical Field

[0001] This disclosure relates to catalytic compounds. More specifically, this disclosure relates to electrocatalytic compounds. Summary of the Invention

[0002] This application discloses one or more features as described in the appended claims and / or the following features, which, individually or in any combination, may encompass patentable subject matter.

[0003] According to one aspect of this disclosure, the electrocatalyst may comprise a multimetallic material, including a first metal of Ir; and at least one other metal selected from the group consisting of W, Mo, Re, Ru, Fe, Pd, Rh, Mn, and Cr. In some embodiments, the composition of the catalyst and the atomic ratio of the metals may be provided in Tables 1-19 and Figure 2A-22 The set is defined by at least one of the components and atomic ratios disclosed in it.

[0004] In some embodiments, one or more metals in the catalyst may be oxidized. Whether or not oxidation occurs can affect the performance of the catalyst under different test conditions. The crystallinity of the oxide can vary from amorphous to fully crystalline. The crystallinity of the oxide can affect the performance of the catalyst under different test conditions. The ratio of oxide to metal can be fully oxidized, partially oxidized, or entirely metallic. The oxide can be prepared by thermal annealing, calcination, chemical methods, or electrochemical methods.

[0005] In some embodiments, the electrocatalyst may comprise a mixed single-crystal phase nanomaterial containing multiple elements. In other embodiments, the electrocatalyst material may comprise a multiphase mixed nanomaterial containing multiple elements.

[0006] In some embodiments, the catalyst may be supportless or supported on carbon, silicon carbide, alumina, silicon dioxide, titanium, titanium dioxide, tungsten, tungsten oxide, antimony, tantalum, platinum, niobium oxide, indium tin oxide, fluorine-doped tin oxide, or graphene. In some embodiments, the catalyst may contain up to 10 atomic% of additional elements such as Pt, Os, Ta, Ce, Ba, Hf, In, Sn, Sb, Au, Ag, Sr, Y, Sc, Nb, La, Pr, Sm, and Cu; in some embodiments, other elements may also be included. In some embodiments, the catalyst may contain up to 10 atomic% of additional elements such as Ni and Co, but not compositions consisting solely of Ir, Ru, Ni, and Co.

[0007] In some embodiments, the surface of the electrocatalyst can be a nanostructure. In some embodiments, the mixed metal or mixed metal oxide can be synthesized by at least one of melting and template thermal decomposition. In some embodiments, the catalyst can be synthesized by other methods, such as colloidal synthesis, polymer penlithography, sol-gel hydrolysis, electrodeposition, and / or spray pyrolysis.

[0008] According to another aspect of this disclosure, a method for catalyzing an electrochemical reaction may include: providing a multimetallic material comprising at least two metals, wherein the first metal is Ir, and one or more of the other metals are from the group consisting of W, Mo, Re, Ru, Fe, Pd, Rh, Mn, and Cr; and applying the multimetallic material as a catalyst in the reaction. In some embodiments, the composition of the catalyst and the atomic ratio of the metals may be provided in Tables 1-19 and Figure 2A-22 The set is defined by at least one of the components and atomic ratios disclosed in it.

[0009] In some embodiments, one or more metals in the catalyst may be oxidized. The crystallinity of the oxide may range from amorphous to fully crystalline. The ratio of oxide to metal may be fully oxidized, partially oxidized, or entirely metallic. The oxide may be prepared by thermal annealing, calcination, chemical methods, or electrochemical methods. In some embodiments, the catalyst may be supportless or supported on carbon, silicon carbide, alumina, silicon dioxide, titanium, titanium dioxide, tungsten, tungsten oxide, niobium, niobium oxide, indium tin oxide, zirconium, tantalum, antimony, platinum, fluorine-doped tin oxide, or graphene; in some embodiments, other elements may also be included.

[0010] In some embodiments, the catalyst may contain up to 10 atomic% of additional elements, such as Pt, Os, Ta, Ce, Ba, Hf, In, Sn, Sb, Au, Ag, Sr, Y, Sc, Nb, La, Pr, Sm, and Cu. The catalyst may contain up to 10 atomic% of additional elements, such as Ni and Co, but does not include compositions consisting solely of Ir, Ru, Ni, and Co.

[0011] In some embodiments, the surface of the catalyst may be a nanostructure. Mixed metals or mixed metal oxides can be synthesized via at least one of melt fusion and template thermal decomposition. In some embodiments, the catalyst can be synthesized via other methods, such as colloidal synthesis, polymer pen lithography, sol-gel hydrolysis, electrodeposition, and / or spray pyrolysis.

[0012] According to another aspect of this disclosure, a method for catalyzing an electrochemical reaction may include: providing a multimetallic material comprising at least two metals, wherein the first metal of the at least two metals is Ru, and one or more of the other metals are from the group consisting of W, Mo, Re, Ir, Fe, Pd, Rh, Mn, and Cr; and applying the multimetallic material as a catalyst in the reaction. In some embodiments, applying the catalyst to the reaction may include applying the catalyst to the oxygen evolution reaction (OER). The OER reaction may be an acidic OER. In some embodiments, the OER reaction may be a basic OER.

[0013] In some embodiments, applying a catalyst to the reaction may include applying the catalyst to hydrogen generation and / or oxidation. Applying a catalyst to the reaction may include applying the catalyst to oxygen generation and reduction. Applying a catalyst to the reaction may include applying the catalyst to CO2 conversion. For example, conversion may include converting CO2 into various products, including but not limited to carbon monoxide, ethylene, methanol, ethanol, urea, acetonitrile, cyanide, etc. Applying a catalyst to the reaction may include applying the catalyst to biomass conversion. For example, biomass conversion may include conversion into organic products, including but not limited to biomass-derived furfural conversion such as hydroxymethylfurfural oxidation, biomass-derived polyol conversion such as glycerol or glucose oxidation, or lignin derivative conversion such as lignin depolymerization.

[0014] In some embodiments, applying a catalyst to a reaction may include applying the catalyst to hydrogenation and / or dehydrogenation. Applying a catalyst to a reaction may include applying the catalyst to an organic oxidation reaction. Applying a catalyst to a reaction may include applying the catalyst to generate a halogen gas. For example, halogen gases may include chlorine, bromine, and / or iodine.

[0015] In some embodiments, applying a catalyst to a reaction may include applying the catalyst to the generation and / or conversion of ammonia. Applying a catalyst to a reaction may include applying the catalyst to gas purification. Applying a catalyst to a reaction may include applying the catalyst to deoxygenation, dehydrogenation, and / or CO2 purification.

[0016] In some embodiments, applying a catalyst to the reaction may include applying the catalyst to gas purification. Applying a catalyst to the reaction may include electroplating, electrowinning, or wastewater purification.

[0017] According to another aspect of this disclosure, a method for catalyzing a non-electrochemical reaction may include a multimetallic material of two or more elements, wherein the first metal is Ir, and one or more other metals are derived from the group consisting of W, Mo, Re, Ru, Fe, Pd, Rh, Mn, and Cr; and the application of a catalyst to the reaction. In some embodiments, the composition of the catalyst and the atomic ratio of the metals may be provided in Tables 1-19 and Figure 2A-22 The set is defined by at least one of the components and atomic ratios disclosed in it.

[0018] In some embodiments, one or more metals in the catalyst may be oxidized. The crystallinity of the oxide may vary from amorphous to fully crystalline. The ratio of oxide to metal may be fully oxidized, partially oxidized, or entirely metallic. The oxide may be prepared by thermal annealing, calcination, chemical methods, or electrochemical methods.

[0019] In some embodiments, the catalyst may be supportless, supported on carbon, silicon carbide, alumina, silicon dioxide, titanium, titanium dioxide, tungsten, tungsten oxide, niobium oxide, indium tin oxide, fluorine-doped tin oxide, or graphene. In some embodiments, the catalyst may contain up to 10 atomic% of additional elements, such as Pt, Os, Ta, Ce, Ba, Hf, In, Sn, Sb, Au, Ag, Sr, Y, Sc, Nb, La, Pr, Sm, and Cu; in some embodiments, other elements may also be included. The catalyst may contain up to 10 atomic% of additional elements, such as Ni and Co, but does not include compositions consisting solely of Ir, Ru, Ni, and Co.

[0020] In some embodiments, the surface of the catalyst may be a nanostructure. Mixed metals or mixed metal oxides can be synthesized via at least one of melt fusion and template thermal decomposition. In some embodiments, the catalyst can be synthesized via other methods, such as colloidal synthesis, polymer pen lithography, sol-gel hydrolysis, electrodeposition, and / or spray pyrolysis.

[0021] According to another aspect of this disclosure, a method for catalyzing a non-electrochemical reaction may include: providing a multimetallic material comprising two or more elements, wherein the first metal is Ru, and one or more other metal elements are derived from the group consisting of W, Mo, Re, Ir, Fe, Pd, Rh, Mn, and Cr; and applying a catalyst to the reaction. In some embodiments, applying the catalyst to the reaction may include applying the catalyst to CO2 or CO conversion. For example, CO2 or CO conversion may include conversion to various products, including but not limited to carbon monoxide, ethylene, methanol, ethanol, urea, acetonitrile, cyanide, methane, etc. Applying the catalyst to the reaction includes applying the catalyst to the conversion from biomass to organic products. For example, biomass conversion may include, but is not limited to, biomass-derived furfural conversion such as hydroxymethylfurfural oxidation, biomass-derived polyol conversion such as glycerol or glucose oxidation, or lignin derivative conversion such as lignin depolymerization.

[0022] In some embodiments, applying a catalyst to a reaction may include applying the catalyst to hydrogenation and / or dehydrogenation. Applying a catalyst to a reaction may include applying the catalyst to an organic oxidation reaction. Applying a catalyst to a reaction may include applying the catalyst to the generation and / or conversion of ammonia. In some embodiments, applying a catalyst to a reaction may include applying the catalyst to gas purification.

[0023] According to another aspect of this disclosure, the electrocatalyst may comprise a multimetallic material containing two or more metals, wherein the first metal of the two or more metals is Ru; and one or more of the other metals are selected from the group consisting of W, Mo, Re, Ir, Fe, Pd, Rh, Mn, and Cr. In some embodiments, the composition of the catalyst and the atomic ratio of the metals may be provided in Tables 1-19 and Figure 2A-22 The set is defined by at least one of the components and atomic ratios disclosed in it.

[0024] In some embodiments, one or more metals in the catalyst may be oxidized. The crystallinity of the oxide may vary from amorphous to fully crystalline. The ratio of oxide to metal may be fully oxidized, partially oxidized, or entirely metallic. The oxide may be prepared by thermal annealing, calcination, chemical methods, or electrochemical methods. The catalyst may be unsupported or supported on carbon, silicon carbide, alumina, silicon dioxide, titanium, titanium dioxide, tungsten, tungsten oxide, niobium oxide, indium tin oxide, fluorine-doped tin oxide, or graphene; in some embodiments, other elements may also be included.

[0025] In some embodiments, the catalyst may contain up to 10 atomic% of additional elements, such as Pt, Os, Ta, Ce, Ba, Hf, In, Sn, Sb, Au, Ag, Sr, Y, Sc, Nb, La, Pr, Sm, and Cu. The catalyst may contain up to 10 atomic% of additional elements, such as Ni and Co, but does not include compositions consisting solely of Ir, Ru, Ni, and Co.

[0026] In some embodiments, the surface of the catalyst may be a nanostructure. Mixed metals or mixed metal oxides can be synthesized via at least one of melt fusion and template thermal decomposition. In some embodiments, the catalyst can be synthesized via other methods, such as colloidal synthesis, polymer pen lithography, sol-gel hydrolysis, electrodeposition, and / or spray pyrolysis.

[0027] According to another aspect of this disclosure, an oxygen evolution reaction (OER) catalyst may include: a first metal, wherein the first metal is a platinum group metal; and one or more other metals, wherein the concentration of each of the one or more other metals is less than about 95% atomically. In some embodiments, the catalyst may be represented as M1XM2Y, wherein M1 represents the first metal, M2 represents the second metal among one or more other metals, X+Y=100%, and each of X and Y is equal to or less than about 95% atomically.

[0028] In some embodiments, the catalyst may be represented as M1XM2YM3Z, where M1 represents a first metal, M2 represents a second metal from one or more other metals, M3 represents a third metal from one or more other metals, X+Y+Z=100%, and each of X, Y, and Z has an atomic ratio of less than or equal to about 95%. In some embodiments, M1 may be Ir or Ru; and M2 may be selected from the group consisting of W, Mo, Re, Ru, Fe, Pd, Rh, Mn, and Cr.

[0029] In some embodiments, M1 can be Ir or Ru; M2 can be an element selected from the group consisting of W, Mo, Re, Ru, Fe, Pd, Rh, Mn, and Cr; and M3 can be selected from the group consisting of W, Re, Mo, Fe, Pd, Rh, Mn, and Cr. In some embodiments, M1 can be Ir; M2 can be Ru or Re; and M3 can be selected from the group consisting of Re, Mo, W, Fe, Pd, Cr, Mn, and Rh.

[0030] In some embodiments, the catalyst may be an acidic OER catalyst. The catalyst may also include a support. The support may be doped SiC.

[0031] According to another aspect of this disclosure, a method of catalytic reaction may include: providing a catalyst comprising: a first metal, wherein the first metal is a platinum group metal; and one or more other metals, wherein the concentration of each of the one or more other metals is less than about 95% atomically; and applying the catalyst to the reaction. In some embodiments, applying the catalyst to the reaction may include applying the catalyst to the oxygen evolution reaction (OER). The OER reaction may be an acidic OER. The OER reaction may be a basic OER.

[0032] In some embodiments, applying a catalyst to a reaction may include applying the catalyst to hydrogen generation and / or oxidation. Applying a catalyst to a reaction may include applying the catalyst to oxygen generation and reduction. Applying a catalyst to a reaction may include applying the catalyst to CO2 conversion. Applying a catalyst to a reaction may include applying the catalyst to biomass conversion. Applying a catalyst to a reaction may include applying the catalyst to hydrogenation and / or dehydrogenation.

[0033] In some embodiments, applying a catalyst to a reaction may include applying the catalyst to the generation and / or conversion of ammonia. Applying a catalyst to a reaction may include applying the catalyst to gas purification. Applying a catalyst to a reaction may include applying the catalyst to deoxygenation, dehydrogenation, and / or CO2 purification.

[0034] According to another aspect of this disclosure, the catalyst may include: a first metal, wherein the first metal is a platinum group metal excluding Ir; and one or more other metals, wherein the catalyst is designated M1. X M2 Y In this system, M1 represents the first metal, M2 represents the second metal consisting of one or more other metals, X+Y=100%, and each of X and Y has an atomic ratio equal to or less than approximately 95%. M2 can be freely selected from the group consisting of W, Mo, Re, Fe, Pd, Rh, Mn, and Cr.

[0035] According to another aspect of this disclosure, the catalyst may include: a first metal, wherein the first metal is a platinum group metal excluding Ir; and one or more other metals, wherein the catalyst is represented as M1XM2YM3Z, wherein M1 represents the first metal, M2 represents a second metal of one or more other metals, M3 represents a third metal of one or more other metals, X+Y+Z=100%, and each of X, Y, and Z has an atomic ratio equal to or less than about 95%. M2 may be an element selected from the group consisting of W, Mo, Re, Fe, Pd, Rh, Mn, and Cr, and wherein M3 may be selected from the group consisting of W, Re, Mo, Fe, Pd, Rh, Mn, and Cr.

[0036] Additional features, used alone or in combination with any one or more other features (including the features listed above and those listed in the claims), may comprise patentable subject matter and will be apparent to those skilled in the art upon consideration of the following detailed description of exemplary embodiments, which exemplifies the best mode for carrying out the invention as now understood. Attached Figure Description

[0037] A detailed description is provided, with particular reference to the accompanying drawings, in which: Figure 1 It is an example of a ternary graph.

[0038] Figure 2A and 2B The images are graphical descriptions of catalyst material sample combinations according to exemplary embodiments, shown in black and white and color respectively, indicating moderately high early lifetime (BOL) activity. Figure 3A and 3B These are graphic descriptions of catalyst material sample combinations according to exemplary embodiments, shown in black and white and color respectively, indicating high early lifetime (BOL) activity; Figure 4A and 4B The images are graphical descriptions of catalyst material sample combinations according to exemplary embodiments, shown in black and white and color respectively, indicating higher early lifetime (BOL) activity; Figure 5A and 5B These are graphic descriptions of catalyst material sample combinations according to exemplary embodiments, shown in black and white and color respectively, indicating moderately high end-of-life (EOL) activity. Figure 6A and 6B These are graphic descriptions of catalyst material sample combinations according to exemplary embodiments, shown in black and white and color respectively, indicating high end-of-life (EOL) activity; Figure 7A and 7B These are graphic descriptions of catalyst material sample combinations according to exemplary embodiments, shown in black and white and color respectively, indicating higher end-of-life (EOL) activity; Figure 8A and 8B These are graphic descriptions of catalyst material sample combinations according to exemplary embodiments, shown in black and white and color respectively, indicating moderately high stability; Figure 9A and 9B The images are graphical descriptions of catalyst material sample combinations according to exemplary embodiments, shown in black and white and color respectively, indicating high stability.

[0039] Figure 10A and 10B These are graphic descriptions of catalyst material sample combinations according to exemplary embodiments, shown in black and white and color respectively, indicating higher stability; Figure 11A and 11B These are graphic descriptions of catalyst material sample combinations according to exemplary embodiments, shown in black and white and color respectively, indicating moderately high overall performance; Figure 12A and 12B The images are graphical descriptions of catalyst material sample combinations according to exemplary embodiments, shown in black and white and color respectively, demonstrating high overall performance.

[0040] Figure 13A and 13B These are graphical descriptions of catalyst material sample combinations according to exemplary embodiments, shown in black and white and color respectively, demonstrating superior overall performance; and Figure 14A and 14B These are graphic descriptions of catalyst material sample combinations according to exemplary embodiments, shown in black and white and color respectively, demonstrating excellent overall performance.

[0041] Figure 15 This is a representative powder X-ray diffraction (PXRD) pattern of a representative novel catalyst sample according to an exemplary embodiment, calibrated for a single crystalline phase.

[0042] Figure 16 This is a graphical representation of the composition collected from a representative novel catalyst sample according to an exemplary embodiment by scanning electron microscopy coupled with energy-dispersive X-ray spectroscopy (SEM-EDS).

[0043] Figure 17 This is a graphical representation of the iridium (wt%) distribution from a representative novel catalyst sample according to an exemplary embodiment.

[0044] Figure 18 This is a graphical representation of the ruthenium (wt%) distribution from a representative novel catalyst sample according to an exemplary embodiment.

[0045] Figure 19 This is a graphical representation of the tungsten (wt%) distribution from a representative novel catalyst sample according to an exemplary embodiment.

[0046] Figure 20 This is a graphical representation of the effective circle diameter (ECD) (in µm) collected from a novel catalyst sample according to an exemplary embodiment using a scanning electron microscope (SEM).

[0047] Figure 21 It is a collection of PEM electrolyzer linear polarization curves from novel catalyst samples according to exemplary embodiments.

[0048] Figure 22 It is a collection of PEM electrolyzer degradation data from novel catalysts and reference samples according to exemplary embodiments. Detailed Implementation

[0049] With the rapid development of sustainable technologies, particularly renewable fuels and chemicals, green hydrogen is emerging as a highly attractive alternative to traditional hydrogen sources globally. One method for producing green hydrogen requires the use of polymer electrolyte membrane (PEM) electrolyzers, where a proton-conducting membrane serves as the electrolyte, separating the anode and cathode.

[0050] In such a reactor, the oxygen evolution reaction (OER) takes place at the anode, oxidizing water into O2 and H2. + Subsequently, protons move through the membrane to the cathode to carry out the subsequent hydrogen evolution reaction (HER). The low pH at the anode results in rather harsh conditions, which can benefit high-performance anode catalyst materials.

[0051] Few materials meet both of the following conditions: a) stability under low pH and oxidation potential (as shown in the Pourbaix diagram); and b) possess an active OER catalyst. In the PEM electrolysis industry, the standard anode material is iridium oxide (IrO₂). x Iridium is a suitable OER catalyst due to its reasonable activity and appropriate stability under harsh acidic and oxidative conditions. However, iridium is one of the most expensive raw materials in the world, and its annual production is far from meeting the anticipated growth demand of the current PEM water electrolysis market. Therefore, finding an iridium alternative with sufficient stability and activity in PEM water electrolyzers can ensure the development of PEM water electrolyzers and avoid serious obstacles caused by supply chain constraints.

[0052] Alloying metals with metal oxides is a promising strategy for improving the performance of electrocatalysts for OER (Oxygen Response). When two or more metals or oxides are alloyed, the geometry and / or electronic properties of the active sites can be altered. These changes can lower the binding energy of the intermediates, thereby reducing the overpotential required for the reaction and / or stabilizing the lattice under acidic conditions.

[0053] Platinum group metals (PGMs), such as iridium (Ir) and ruthenium (Ru), can serve as electrocatalysts for acidic OERs. IrO xWhile Ir exhibits relatively low electrocatalytic activity, it demonstrates significantly higher stability at low pH and high oxidation potential. Therefore, many alloy-type OER electrocatalysts are based on Ir or Ru.

[0054] One of the findings of this disclosure is that Ir and / or Ru can be combined with a wide range of elements having various electronic and / or geometric characteristics to form combinations of two, three, or more elements. Such combinations can yield low-iridium or iridium-free catalysts that exhibit similar activity, stability, or both, to IrO. x Comparable or improved performance. Traditional mixed-component electrocatalysts often consist of multiple phases, due to the fundamental principles of material formation and oxidation processes. Typically, one phase exhibits higher activity relative to a given reaction and is therefore the ideal target for formation. Examples of suitable elements for combination include W, Mo, Re, Fe, Pd, Mn, Rh, and Cr, collectively referred to herein as "other elements".

[0055] Using polymer pen lithography, bimetallic and trimetallic composites were synthesized: M1 X M2 Y and M1 X M2 Y M3 Z For these components, X, Y, and Z represent atomic percentages (M). i The atomic percentage of the total number of atoms (%), and the proportion of X+Y=100% in the bimetallic composition and X+Y+Z=100% in the trimetallic composition. Catalyst candidates are selected from the above elements with a step size variation of 1 atom%.

[0056] In an exemplary embodiment, the catalyst material is supported on doped SiC. However, in some embodiments, other supports may be used, such as carbon, alumina, silicon dioxide, titanium dioxide, tungsten oxide, niobium oxide, indium tin oxide, fluorine-doped indium tin oxide, etc., or no support may be used.

[0057] Furthermore, the catalyst material presented was first synthesized as a zero-valent metal nanostructure, followed by thermal oxidation. However, other synthetic methods can also be used to obtain materials with similar compositions. These compositionally similar materials may have the same or different oxidation states, shapes, phases, and / or nanostructures.

[0058] The OER activity of the catalyst material was tested at the beginning of its life (BOL) and the end of its life (EOL). In an exemplary embodiment, a high-throughput scanning electrochemical method was used to detect the material. However, the electrochemical performance of the synthesized material can also be measured by other means, such as rotating disk electrode (RDE) testing, half-cell testing, electrolyzer testing, etc.

[0059] In an exemplary embodiment, the catalyst's initial lifetime (BOL) activity for the acidic oxygen evolution reaction (OER) is measured (by chronoamperometry), i.e., the current generated when a constant voltage, for example 2 V, relative to the reversible hydrogen electrode (RHE) is applied to the catalyst in 0.3 M HClO4, and expressed as IrO. x Standards are normalized; however, in some implementations, other methods may be applied to determine the BOL of the catalyst.

[0060] In an exemplary embodiment, the end-of-life (EOL) activity of the catalyst for the acidic oxygen evolution reaction (OER) is measured (by chronoamperometry), i.e., the current generated when a constant voltage, for example 2 V, relative to the reversible hydrogen electrode (RHE) is applied to the catalyst in 0.3 M HClO4, and expressed as IrO. x The standard is normalized, and this measurement is performed after accelerated stress testing (AST) of the catalyst. For example, an AST protocol may involve applying a constant voltage of 1.8 V relative to the reversible hydrogen electrode (RHE) to the catalyst in 0.1 M HClO4 for 1 hour. However, in some embodiments, other EOL activity measurements and AST protocols may also be applied.

[0061] In an exemplary embodiment, the stability of the catalyst to the acidic oxygen evolution reaction (OER) is calculated as (EOL) 催化剂 -BOL 催化剂 ) / BOL 催化剂 Normalized (EOL) IrOx -BOL IrOx ) / BOL IrOx However, in some implementations, other formulas can be applied to determine the stability of the catalyst.

[0062] Bimetallic and trimetallic M1 were synthesized using melt fusion and / or template thermal decomposition. X M2 Y and M1 X M2 Y M3 Z The combination of X, Y, and Z. For these compositions, X, Y, and Z are atoms (M). i The percentage of atoms in the total number of atoms (%), in bimetallic compositions X+Y=100%, and in trimetallic compositions X+Y+Z+100%. These compositions were selected for gram-scale synthesis due to their promising high-throughput results.

[0063] In an exemplary embodiment, the electrocatalyst material is unsupported. However, in some embodiments, a support may be used, such as carbon, alumina, titanium, titanium dioxide, niobium, niobium oxide, zirconium, tantalum, antimony, silicon carbide, tungsten, or platinum; in some embodiments, the support may also include other elements.

[0064] Furthermore, the proposed catalyst material was first synthesized as a direct mixed metal oxide, followed by a zero-valent mixed metal nanostructure obtained through thermal oxidation. However, other synthetic methods can also be used to obtain materials with similar compositions. These compositionally similar materials may have the same or different oxidation states, overall morphologies, and / or nanostructures.

[0065] The catalyst material was tested for early life (BOL), accelerated stress test (AST), and end-of-life (EOL) OER activity. In an exemplary embodiment, the material was tested using a small electrolyzer. However, the electrochemical performance of the synthesized material can also be measured by other methods, such as rotating disk electrode (RDE) testing, half-cell testing, droplet electrochemical testing, etc.

[0066] In an exemplary embodiment, the initial lifetime (BOL) activity of the catalyst for the acidic oxygen evolution reaction (OER) is determined from PEM electrolyzer polarization data at the start of the OER after the break-in period, using IrOx as a benchmark. However, in some embodiments, other methods may be applied to establish the BOL of the electrocatalyst.

[0067] In an exemplary embodiment, square-wave cyclic voltammetry is used, with the potential held at 2V vs RHE, to measure the performance of the novel catalyst during accelerated stress testing (AST) for the acidic oxygen evolution reaction (OER). For example, the AST protocol may include applying square-wave cyclic potentials of 2V and 1.45V for 30 seconds, respectively. However, in some embodiments, other protocols and measurements may be applied to AST.

[0068] In some cases, different calcination conditions are applied to the same material composition to obtain different particle sizes, morphologies, crystallinity, etc.

[0069] In some cases, the compositional distribution can be wide or narrow, and the optimal distribution depends on the material composition.

[0070] In some cases, the size of the material can be very small (sub-100 nm particles) or very large (micrometer scale), and the particle size distribution can be very wide or very narrow. The optimal particle size distribution can vary depending on the material and other test parameters.

[0071] Each composition described herein can be prepared to form a single mixed phase comprising the elements. Each composition described herein can also be prepared to form multiple mixed phases. Each composition described herein can be prepared to not form any mixed (single-element) phase. Each composition described herein can also be prepared to include elements forming a mixed phase, accompanied by the presence of additional single-element phases.

[0072] A typical melt-fusion synthesis scheme is as follows: A catalyst precursor solution is prepared by dissolving the metal precursor powder in a desired organic solvent (isopropanol, chloroform, acetonitrile, etc.) to achieve the required proportion and concentration. This solution is then combined with a large excess of sodium nitrate (used alone or with an auxiliary salt, in an amount 1-100 times the mass of the catalyst precursor) to produce a slurry. This slurry is mixed and dried simultaneously, then transferred to a suitable furnace crucible / boat. The precursor / salt mixture is placed in a tube furnace and annealed in air at 350-600°C for 1-4 hours, then cooled to room temperature. The resulting crude catalyst powder is then processed by repeated ultrasonic treatment, centrifugation, and washing with ultrapure water to remove excess salt, followed by drying.

[0073] A typical templated thermal decomposition synthesis scheme is as follows: The metal precursor is dissolved in a desired organic solvent (isopropanol, chloroform, acetonitrile, etc.) to achieve the required ratio and concentration. Then, finely ground inorganic salt powder (potassium sulfate, potassium chloride, sodium chloride, etc.) in a proportion of 100-2000 times the mass of the dissolved metal precursor is added to the solution to form a slurry. The slurry is dried under mixing, transferred to a suitable furnace crucible / boat, and annealed in a tube furnace at 300-600°C for 0.5-6 hours under air or hydrogen, with optional subsequent calcination. The resulting crude catalyst powder is then processed by repeated ultrasonic treatment, centrifugation, and washing with ultrapure water to remove excess salt, followed by drying.

[0074] The electrocatalyst powders were characterized using scanning electron microscopy-energy dispersive X-ray spectroscopy (SEM-EDS) and powder X-ray diffraction (PXRD). SEM-EDS shows the material composition and homogeneity of each sample. PXRD shows the crystallographic characteristics of each powder sample.

[0075] The electrocatalyst powder was tested using an in-situ three-electrode method and a 5 cm² PEM electrolysis cell.

[0076] A typical off-site three-electrode testing scheme is as follows: The catalyst powder was dispersed in a mixture of water and alcohol solvent at a concentration of 0.5–4 mg / mL. Then, an ionomer dispersion was added at 0.1–12 wt% relative to the catalyst powder. The mixture was sonicated for 30–90 minutes and then coated onto electrodes (glassy carbon electrodes, gold electrodes, etc.) by ultrasonic spray deposition. The electrodes were then placed in a three-electrode electrolytic cell containing 0.1–1.0 M perchloric acid and vigorously stirred. Cyclic voltammetry was performed in the non-Radida potential region to measure capacitance, followed by linear sweep voltammetry at 1.1–1.8 V vs. RHE to measure OER activity. Chorometric voltammetry was then performed at 1.65 V vs. RHE for 5–800 minutes, followed by repeated linear sweep voltammetry. Electrochemically active surface area (ECSA) was determined by underpotential deposition of metals (Hg, Pb, etc.).

[0077] In some cases, alternative test schemes can be used instead of the chronoamperometry method, including the chronopotentialometry method and the cyclic voltammetry method.

[0078] A typical PEM electrolyzer test procedure is as follows: The catalyst powder was dispersed in a mixture of water and alcohol solvent at a concentration of 0.4–5 mg / mL. Then, 3–25 wt% of an ion-polymer dispersion relative to the catalyst powder was added. The mixture was sonicated for 30–90 minutes and then applied to an ion exchange membrane (the other side of the membrane was already loaded with Pt / C), with a catalyst powder loading of 0.1–1 mg / mL. 2 The catalyst-coated membrane was assembled into a PEM electrolyzer comprising a platinum-titanium porous transport layer (anode), a carbon paper porous transport layer (cathode), and a PTFE spacer layer. Ultrapure water (80°C) was then circulated through the anode flow field at 100 mL / min, and the assembled electrolyzer was pretreated: first, a constant current of 0.2 A / cm² was maintained for 1 hour, then a constant current of 1 A / cm² for 1 hour, and finally a constant potential of 2 V for 30 minutes. After pretreatment, polarization curves were acquired by maintaining the potential at 1.3–2 V in 0.1 V increments for 5 minutes. Square wave voltammetry was then performed using the following steps: maintaining the electrolyzer potential at 2 V for 30 seconds and at 1.45 V for 30 seconds, and repeating the process. Polarization curves were acquired every 12 hours.

[0079] In some cases, other accelerated stress testing methods can be used instead of the square wave voltammetry method, including constant voltage holding or triangular wave.

[0080] Using these methods, several promising samples for acidic OER were synthesized and validated in the combined material space of Ir-Cr-Ru-Rh-W-Mn-Mo-Fe-Pd-Re.

[0081] Table 1-19 and Figure 1-22 The electrocatalysts described herein have been synthesized at the chip-scale or gram-scale using a variety of techniques, including polymer pen lithography, melt fusion, or template thermal decomposition. Table 1-17 and Figure 2A-14B This involves chip-level data. Tables 18-19 and... Figure 15-22 This involves data at the gram level.

[0082] Table 1-1 and Figure 2A-14B The results of high-throughput chip-based experiments are summarized, which screened various example compositions in the aforementioned material space. Tables 18-19 and... Figure 15-22 This involves data at the gram level.

[0083] refer to Figure 1 A sample graph is provided to illustrate how to interpret the data in Figure 2-14. The graph shows each metal and its corresponding coordinate axis, with the values ​​on the axis representing the percentage of that metal's composition. Metals A, B, and C are represented in red, blue, and green, respectively. The internal grid lines also correspond to the coordinate axes of their colors. Four points are shown as examples. Point 1 represents a composition of 20% metal A, 20% metal B, and 60% metal C. Point 2 represents a composition of 20% metal A, 60% metal B, and 20% metal C. Point 3 represents a composition of 60% metal A, 20% metal B, and 20% metal C. Point 4 represents a composition where all metals are equally distributed, at 33.3% metal A, 33.3% metal B, and 33.3% metal C.

[0084] Table 1-13 shows the composition ranges used for each evaluation and their corresponding properties. Columns named "Metal A," "Metal B," and "Metal C" represent the metal names. The columns "Minimum Atom %," "Minimum Btom %," and "Minimum Ctom %" represent the lowest composition percentage ranges for Metal A, Metal B, and Metal C in the material space, respectively. The columns "Maximum Atom %," "Maximum Btom %," and "Maximum Ctom %" represent the highest composition percentage ranges for Metal A, Metal B, and Metal C in the material space, respectively.

[0085] Referring to Tables 1-3 and 10-13, the columns "Highest Relative BOL Activity of Metal A at the Lowest Atomic %", "Highest Relative BOL Activity of Metal B at the Lowest Atomic %", and "Highest Relative BOL Activity of Metal C at the Lowest Atomic %" represent the highest relative early lifetime (BOL) activities of metals A, B, and C within the lowest composition range, respectively. The columns "Highest Relative BOL Activity of Metal A at the Highest Atomic %", "Highest Relative BOL Activity of Metal B at the Highest Atomic %", and "Highest Relative BOL Activity of Metal C at the Highest Atomic %" represent the highest relative BOL activities of metals A, B, and C within the highest composition range, respectively. Higher values ​​indicate better relative BOL activity. For example, consider the values ​​in row 2 of Table 1. The composition range is iridium 2-86 atomic%, iron 3-88 atomic%, and ruthenium 2-87 atomic%. The highest relative BOL activity of metal A at the lowest atomic % is 1.3169, which is the highest relative BOL activity of a material containing 2 atomic% iridium. The highest relative BOL activity of metal A at the highest atomic percentage (2.2804) is the highest relative BOL activity of a material containing 86 atomic percent iridium. The highest relative BOL activity of metal B at the lowest atomic percentage (2.5291) is the highest relative BOL activity of a material containing 3 atomic percent iron. The highest relative BOL activity of metal B at the highest atomic percentage (0.8190) is the highest relative BOL activity of a material containing 88% iron. The highest relative BOL activity of metal C at the lowest atomic percentage (2.7708) is the highest relative BOL activity of a material containing 2 atomic percent ruthenium. The highest relative BOL activity of metal C at the highest atomic percentage (0.8058) is the highest relative BOL activity of a material containing 87 atomic percent ruthenium.

[0086] Referring to Table 4-6, the columns for "Highest Relative End-of-Life (EOL) Activity of Metal A at the Lowest Atom %", "Highest Relative EOL Activity of Metal B at the Lowest Atom %", and "Highest Relative EOL Activity of Metal C at the Lowest Atom %" represent the highest relative end-of-life (EOL) activities of metals A, B, and C at the lowest composition range, respectively. The columns for "Highest Relative EOL Activity of Metal A at the Highest Atom %", "Highest Relative EOL Activity of Metal B at the Highest Atom %", and "Highest Relative EOL Activity of Metal C at the Highest Atom %" represent the highest relative EOL activities of metals A, B, and C at the highest composition range, respectively. Higher values ​​indicate better relative EOL activity.

[0087] Referring to Table 7-9, the columns for "Highest Relative Stability of Metal A at the Lowest Atomic %", "Highest Relative Stability of Metal B at the Lowest Atomic %", and "Highest Relative Stability of Metal C at the Lowest %" represent the optimal relative stability of metals A, B, and C at their lowest compositional ranges, respectively. The columns for "Highest Relative Stability of Metal A at the Highest Atomic %", "Highest Stability Activity of Metal B at the Highest Atomic %", and "Highest Relative Stability of Metal C at the Highest Atomic %" represent the optimal relative stability of metals A, B, and C at their highest compositional ranges, respectively. Lower values ​​indicate better relative stability.

[0088] refer to Figure 2A-4B The diagram illustrates the early lifetime (BOL) activity of the samples, with shading or color representing the electrocatalytic activity level at a given proportion indicated by the corresponding range bars in Figures A and B, respectively. The BOL activity level is exemplified by the activity of the electrocatalyst for the acidic oxygen evolution reaction (OER), which is composed of one, two, or three elements mixed in a given proportion within the Ir-Cr-Ru-Rh-W-Mn-Mo-Fe-Pd material space, each combination defined by a triangle. Each triangle represents a specific metal composition space, with element labels at the vertices. The position of the data point within the triangle corresponds to the atomic percentage of each element in the tested material, while the shading or color of the data point corresponds to the activity of the given material measured by chronoamperometry (in units of current), based on IrO. x The standard is normalized, where a value of 1 indicates activity similar to IrO. x The same applies; a value >1 indicates higher activity than IrO. x A value <1 indicates that the activity is lower than that of IrO. x .exist Figure 2A , 3A In 4A, the black and white scale represents relative BOL performance, where white indicates higher relative performance and black indicates lower relative performance. Figure 2B , 3B In 4B, the black and orange color scale represents the relative performance of BOL, where orange indicates higher relative performance and black indicates lower relative performance. Figure 2A and 2B The study showcased a material ensemble with moderately high BOL activity, defined as ≥ pure IrO. x 75% of the BOL activity; Figure 3A and 3B This study showcased a material ensemble with high BOL activity, defined as ≥ pure IrO. x 100% of the BOL activity; Figure 4A and 4B The study showcased a material ensemble with higher BOL activity, defined as ≥ pure IrO. x125% of the BOL activity. Figure 2A The data shown in B, 3A and B, and 4A and B are summarized in Tables 1, 2 and 3, respectively, which summarize the composition ranges with moderately high, high and higher BOL activity, as well as the specific materials and material properties close to each range.

[0089] refer to Figure 5A-7B The diagram illustrates the end-of-life (EOL) activity of the samples, with shading or color representing the activity level at a given proportion indicated by the corresponding range bars in Figures A and B, respectively. The EOL activity level is exemplified by the activity of the electrocatalyst for the acidic oxygen evolution reaction (OER), which is composed of one, two, or three elements mixed in a given proportion within the Ir-Cr-Ru-Rh-W-Mn-Mo-Fe-Pd material space. Each triangle represents a specific metal composition space, with element labels at the vertices. The position of the data point within the triangle corresponds to the atomic percentage of each element in the tested material, while the shading or color of the data point corresponds to the activity of the given material measured by chronoamperometry (in units of current), based on IrO. x The standard is normalized, where a value of 1 indicates activity similar to IrO. x The same applies; a value >1 indicates higher activity than IrO. x A value <1 indicates that the activity is lower than that of IrO. x .exist Figure 5A , 6A In 7A, the black and white scale represents relative EOL performance, where white indicates higher relative performance and black indicates lower relative performance. Figure 5B , 6B In 7B, the black and orange color scale represents the relative EOL performance, where orange indicates higher relative performance and black indicates lower relative performance. Figure 5A B and B demonstrate a material combination with moderately high EOL activity, defined as ≥ pure IrO. x 75% of EOL activity; Figure 6A B and others demonstrated a combination of materials with high EOL activity, defined as ≥ pure IrO. x 100% of EOL activity; Figure 7A B and others demonstrated a combination of materials with higher EOL activity, defined as ≥ pure IrO. x 125% of the EOL activity. Figure 5A The data shown in B, 6A and B, and 7A and B are summarized in Tables 4, 5 and 6, which respectively summarize the composition ranges with moderately high, high and higher EOL activity, as well as the specific materials and material properties approaching each range.

[0090] After the material was subjected to accelerated stress testing (AST) conditions, its EOL activity was measured. While in the exemplary embodiment the AST protocol is a chronoamperometry test performed for a set time at the oxidation potential in an acidic electrolyte, in other embodiments any suitable AST protocol (e.g., chronopotentiometry, potential / current pulse method, square wave voltammetry, cyclic voltammetry, etc.) can be applied. Each measurement was performed using pure IrO synthesized and measured from the same batch of samples. x Based on.

[0091] Now for reference Figure 8A-10B The figures illustrate sample stability, with shading or color representing the activity level at a given proportion indicated by the corresponding range bars in Figures A and B, respectively. Stability is exemplified by the decrease in activity of the electrocatalyst in the acidic oxygen evolution reaction (OER), which is composed of one, two, or three elements mixed in a given proportion within the Ir-Cr-Ru-Rh-W-Mn-Mo-Fe-Pd material space. For example, a more stable material will maintain higher activity in measurements from BOL to EOL, while a less stable material will lose more activity in the same measurement. Figure 8A-10B In the diagram, each triangle represents a specific metallic composition space, with element labels at the vertices. The positions of the data points within the triangles are related to the atomic percentage of each element in the tested material. The shading or color of the data points corresponds to the relative stability of the given material measured by chronoamperometry (determined over a current change from BOL to EOL), based on IrO. x The standard is normalized, where a value of 1 indicates that it is similar to IrO. x The stability is the same, and a value >1 indicates that the stability is lower than that of IrO. x A value <1 indicates higher stability than IrO. x . Figure 8A B and B represent material combinations with moderate to high stability, defined as ≥ pure IrO. x 75%; Figure 9A and 9B It demonstrates a highly stable material combination, defined as ≥ pure IrO x 100%; Figure 10A and 10B It demonstrates a more stable material combination, defined as ≥ pure IrO x 125%. Figure 8A The data shown in B, 9A and B, and 10A and B are summarized in Tables 7, 8 and 9, respectively, which summarize the composition ranges with moderate to high, high and higher stability, as well as the specific materials and material properties close to each range.

[0092] While other elements are used in the exemplary embodiments, in some embodiments, other components may be added and / or substituted, such as Pt, Os, Ta, Ce, Ba, Hf, In, Sn, Sb, Au, Ag, Sr, Y, Sc, Nb, La, Pr, Sm, Cu, etc. In some embodiments, the catalyst material may be synthesized not by polymer pen lithography, but by other methods, such as Adams fusion, colloidal synthesis, spray pyrolysis, etc.

[0093] Figure 11A Tables 10, 11, and 12, along with B, 12A and B, and 13A and B, and their corresponding Tables 10, 11, and 12, indicate that the composition of multi-element nanocatalysts containing Ir and / or Ru is superior to that of IrO, at least in two dimensions. x .

[0094] refer to Figure 11A Figures A and B, 12A and B, and 13A and B, show samples with moderately high, high, and higher overall performance, respectively. The specific proportions of electrocatalytic activity levels indicated by the corresponding range bars in Figures A and B are shown by shading or color. The overall activity level is exemplified by the activity of the electrocatalyst for the acidic oxygen evolution reaction (OER), which is composed of one, two, or three elements mixed in a given proportion within the Ir-Cr-Ru-Rh-W-Mn-Mo-Fe-Pd material space, each combination defined by a triangle. Each triangle represents a specific metal composition space, with element labels at the vertices. The position of the data point within the triangle is related to the atomic percentage of each element in the tested material, while the shading or color of the data point corresponds to the activity of the given material (measured in units of current) determined by chronoamperometry, based on IrO. x Normalization is performed, where a value of 1 indicates activity or stability relative to IrO. x The same applies; a value >1 indicates higher activity than IrO. x Or its stability is lower than that of IrO x A value <1 indicates that the activity is lower than that of IrO. x Or its stability is higher than IrO x . Figure 11A B and B exhibit a material combination with moderately high overall performance, defined as: BOL activity ≥ pure IrO x It has 75% of the properties and its stability is ≥ that of pure IrO. x 75%. Figure 12A B and B demonstrate a material combination with high overall performance, defined as BOL activity ≥ pure IrO. x 100% of the purity, and stability ≥ pure IrO x 100%. Figure 13A and 13BThis demonstrates a material combination with superior overall performance, defined as BOL activity ≥ pure IrO. x 125% of the purity, and with stability ≥ pure IrO x 125%. Figure 11A The data shown in B, 12A and B, and 13A and B are summarized in Tables 10, 11 and 12, which summarize the composition ranges with moderately high, high and higher overall performance, respectively, as well as the specific materials and material properties close to each range.

[0095] refer to Figure 14A Figures A and B illustrate the activity of samples with excellent overall performance, showing the electrocatalytic activity level at a given proportion indicated by the corresponding range bars in Figures A and B, respectively, based on shading or color. The overall activity level is exemplified by the activity of the electrocatalyst for the acidic oxygen evolution reaction (OER), which is composed of one, two, or three elements mixed in a given proportion within the Ir-Cr-Ru-Rh-W-Mn-Mo-Fe-Pd material space, each combination defined by a triangle. Each triangle represents a specific metal composition space, with element labels at the vertices. The position of the data point within the triangle is related to the atomic percentage of each element in the tested material, while the shading or color of the data point corresponds to the activity of the given material (measured in units of current) determined by chronoamperometry, normalized according to the IrOx standard, where a value of 1 indicates activity or stability relative to IrO. x The same applies; a value >1 indicates higher activity than IrO. x Or its stability is lower than that of IrO x A value <1 indicates that the activity is lower than that of IrOx or the stability is higher than that of IrO. x . Figure 14A B and B exhibit a material combination with excellent overall performance, defined as BOL activity ≥ pure IrO. x 150% of that of pure IrO, and stability ≥ pure IrO x 150%. Figure 14A The data shown in B are summarized in Table 13, which summarizes the range of compositions with excellent overall performance, as well as the specific materials and material properties close to each range.

[0096] Table 14-17 lists those exhibiting moderately high, high, higher, and excellent overall performance, meaning they perform well or better than IrO in both BOL activity and stability. x The specific composition is listed in Table 14. Table 14 lists the components exhibiting moderately high overall performance, i.e., BOL activity ≥ pure IrO. x 75% and stability ≥ pure IrO x The specific composition is 75%. Table 15 lists the components with high overall performance, i.e., BOL activity ≥ pure IrO.x 100% and stability ≥ pure IrO x The specific composition is 100%. Table 16 lists the components with higher overall performance, i.e., BOL activity ≥ pure IrO. x 125% and stability ≥ pure IrO x The specific composition is 125% of the total. Table 17 lists the components exhibiting excellent overall performance, i.e., BOL activity ≥ pure IrO. x 150% and stability ≥ pure IrO x The specific composition of 150%.

[0097] The material composition listed in Table 1-9 and Figure 2A-10B The material compositions shown are grouped in 1% increments of atomic percentage; however, if the composition falls within a defined range, intermediate compositions within 1% increments are expected to have similar properties.

[0098] The material composition listed in Table 10-17 and Figure 11A-14B The material compositions shown are grouped in 2% increments of atomic percentage; however, if the composition falls within a defined range, intermediate compositions within 2% increments are expected to have similar properties.

[0099] Now for reference Figure 15 The standard powder X-ray diffraction (PXRD) pattern obtained from a representative sample of the novel catalyst is shown. PXRD is a powerful analytical technique used to identify the crystal phase of a material based on a unique combination of characteristic peaks. In other embodiments, other characterization techniques may also be used to determine the crystal phase of the material. The peak positions of the PXRD spectrum depend on the radiation source. A copper source is used in this embodiment. In other embodiments, other radiation sources may be used. The specific composition of this particular sample is Ir. 0.27 Ru 0.66 W 0.07 The values ​​are expressed as the molar ratio of the three metals. The peaks in the spectrum of this example have been analyzed and labeled as a single crystalline phase with space group P4_2 / mnm. These data correspond to the samples listed in row 80 of Table 19.

[0100] Referring now to Figure X, the figure shows the compositional distribution of a representative sample of the novel catalyst, expressed in wt%, obtained using scanning electron microscopy-energy dispersive X-ray spectroscopy (SEM-EDS). SEM-EDS is a coupled analytical technique that simultaneously provides information on the structure and chemical composition of a sample, and this technique is used in this embodiment. In other embodiments, other techniques or combinations of techniques may be used to obtain the structure and chemical composition of the catalyst material. In this embodiment, SEM-EDS is used automatically to acquire data from hundreds of features, thereby generating a compositional ternary diagram, such as an example (wt%). The specific composition of this particular sample is Ir. 0.27 Ru 0.66 W 0.07 The values ​​are expressed as molar ratios of the three metals. These data correspond to the samples listed in row 80 of Table 19.

[0101] Now for reference Figure 17-19 These figures show Figure 16 The compositional distribution of the catalyst sample is represented by the ternary plot. Specifically, Figure 17 X is a histogram showing the distribution (wt%) of Ir on hundreds of features in the catalyst sample. Figure 18 It is a histogram showing the distribution (wt%) of Ru on hundreds of features in the catalyst sample. Figure 19 This is a histogram showing the distribution (wt%) of W over hundreds of features in the catalyst sample. The overall composition (molar ratio) of this particular sample is Ir. 0.27 Ru 0.66 W 0.07 These data correspond to the samples listed in row 80 of Table 19.

[0102] See Figure 20 The figure shows the morphological features of a representative sample of the novel catalyst, measured by scanning electron microscopy (SEM) and expressed as the effective circle diameter (ECD) in µm. ECD is a method for representing the size of features in an image, such as one acquired via SEM. In any given image, the diameter of a theoretical circle of the same area can be calculated using the area of ​​irregularities within the frame; this value is the ECD (µm). In an exemplary embodiment, SEM is used automatically to acquire data from hundreds of features, thereby generating a structural ternary diagram, as in the example. These data correspond to the samples listed in row 79 of Table 19.

[0103] Now for reference Figure 21 The figure illustrates the performance of the novel catalyst PEM electrolyzer, where the initial lifetime (BOL activity) is represented by the A / cm² value at 2V vs RHE on a linear polarization curve. 2The figure shows two different commercially available membranes (Nafion 115 and Nafion 117) used as substrates for the preparation of novel catalysts and device testing. The top left figure illustrates two Ir solutions with compositions within their preferred ranges. x Ru y W z The average PEM electrolyzer BOL and EOL (after 600 hours accelerated stress testing) activities of the samples on a thin N115 ion exchange membrane. The lower left figure shows a comparison of the average PEM electrolyzer BOL activity of the aforementioned IrxRuyWz sample with its composition within the preferred range on a thin N115 ion exchange membrane with the BOL activity of a pure Ir reference catalyst (Umicore batch number 1029-29 / 13). The upper right figure shows two Ir catalysts with preferred compositions. x Ru y W z The average PEM electrolyzer BOL and EOL (after 200 hours accelerated stress test) activity of the samples on a thick N117 ion exchange membrane. The lower right figure shows the Ir content of the above-mentioned samples with compositions within the preferred range on a thick N117 ion exchange membrane. x Ru y W z The average BOL activity of the sample in the PEM electrolyzer is compared with the BOL activity of the pure Ir reference catalyst (Umicore batch number 1029-29 / 13). In all cases, the shading around the data line represents the standard deviation of the individual linear polarization curves used to generate the average performance line.

[0104] Now for reference Figure 22 This figure illustrates the performance of the novel catalyst in a PEM electrolyzer, where degradation rate is evaluated as a percentage of BOL current density loss per hour of testing. Duration is expressed in hours. Two different commercial membranes (Nafion 115 and Nafion 117) were used as substrates for the preparation of the novel catalyst and for device testing. The dark cyan line represents the average degradation rate of the pure Ir reference catalyst (Umicore batch number 1029-29 / 13) on a thick N117 ion exchange membrane. The yellow line represents Ir with the preferred composition. x Ru y W z The average degradation rate of the sample on a thick N117 ion exchange membrane. The red line represents the average degradation rate of pure Ir reference catalyst (Umicore batch number 1029-29 / 13) on a thin N115 ion exchange membrane. The orange line represents Ir with the preferred composition. x Ru y W z The average degradation rate of the sample on a thin N115 ion exchange membrane. In all cases, the shading around the data line represents the standard deviation of the degradation curve used to generate the average performance line.

[0105] Although the above material was found to be IrO x Promising catalyst alternatives, specifically designed for acidic OERs, but they can also be used in other applications.

[0106] Applications of novel catalysts in oxygen evolution reactions in other industrial electrochemical processes.

[0107] Oxygen evolution anodes are widely used in various industrial electrolysis applications, some of which are related to electrometallurgy and cover a wide range of applied current densities, from extremely low current densities (e.g., hundreds of A / m, such as in electrowinning processes) to extremely high current densities (e.g., in high-speed electroplating, where current densities exceeding 10 kA / m can be achieved at the anode surface). Another application area for oxygen evolution anodes is cathodic protection under impressed current.

[0108] Anode configurations suitable for oxygen evolution at the anode in many conventional industrial electrochemical processes include a titanium substrate and a catalytic coating composed of oxides of iridium and tantalum, with a molar composition of 60-70% iridium and 30-40% tantalum, respectively. In some cases (e.g., to enable operation in strongly acidic or other corrosive electrolytes), it may be advantageous to include an intermediate protective layer between the titanium substrate and the catalytic coating. For example, such a layer could comprise titanium oxide and tantalum oxide with molar compositions of 80% Ti and 20% Ta, respectively. This type of electrode can be prepared in various ways, for example, by thermal decomposition of the precursor solution at high temperatures, such as 400°C to 600°C. For mixed-element electrocatalysts, these preparation methods may result in the formation of a heterogeneous catalytic coating. In many such applications, the specific iridium loading in the catalytic layer exceeds 0.5 mg / cm³. 2 Typically reaches 5 mg / cm 2 It has a loading capacity up to 10 times higher than that used in PEM electrolysis.

[0109] Electrodes with compositions within specified preferred ranges can meet the needs of a variety of industrial applications, offering a reasonable lifespan regardless of current density. However, some manufacturing processes, particularly in the metallurgical field (e.g., copper deposition in electroplating processes used to produce printed circuits and copper foil), may require electrodes with longer lifespans for economic reasons, while also necessitating a suitable reduction in oxygen evolution potential even at higher current densities. In fact, oxygen evolution potential can be one of the main factors determining process operating voltage and the resulting total energy consumption.

[0110] Furthermore, the lifespan of anodes coated on a metal substrate with a noble metal or its oxide is significantly shortened in the presence of particularly corrosive contaminants, which accelerate corrosion or anode surface contamination. Therefore, oxygen-evolving anodes have proven to require characteristics such as low oxygen evolution overpotential, longer lifespan even under particularly harsh process conditions, such as high current densities and / or the presence of particularly corrosive electrolytes (e.g., due to the presence of contaminants), and low or no dependence on Ir.

[0111] For example, the electrode can be placed in 1-1.5 M H2SO4 at a temperature of 60 °C, with an A / cm² concentration. 2 Accelerated stress tests were performed on the oxygen evolution anode at a constant current density, and the deactivation time (the run time required for a potential increase of, for example, 1 V) was measured.

[0112] The similar severity of the operating conditions suggests that the discovered low-iridium oxygen evolution catalyst can replace or reduce Ir not only in PEM water electrolysis but also in the other industrial electrochemical applications mentioned above.

[0113] Although the above materials have been found to be promising alternatives to IrO3 specifically for acidic OERs. x The electrocatalysts of this invention, however, can also be used in other applications, such as: Electrode coating in electrodeposition process Electrodeposition is a well-established industrial tool, particularly in electrometallurgy, for the controlled extraction and electroplating of metals and alloys. The quality of electrodeposited films, including adhesion and uniformity, depends not only on the local morphology of the electrode but also on demanding operating conditions such as current density, pH, and temperature. Due to its durability, IrO... x It has been used as an electrode material in some industrial electrodeposition processes. Electrodes made from the novel electrocatalyst disclosed herein can replace IrO under appropriate conditions. x Or other precious metals / transition metals / platinum group metals are used in the electrodeposition process.

[0114] Electrode coating for electrodeposition Electrodeposition refers to the electrodeposition of metals from ore leachates containing metal ions. It is crucial for the industrial purification of metals but may require harsh conditions such as high current densities, high temperatures, and low pH. Due to its durability, IrO... x It has already been used as an electrode material in some industrial electrodeposition processes. Electrodes made from the novel electrocatalyst disclosed herein can replace IrO under appropriate conditions. x Other precious metals / transition metals / platinum group metals are used in the electrowinning process.

[0115] Electrode coating for electroplating Electroplating is a mature industrial tool, particularly in the field of electrometallurgy, used for the controlled extraction and electroplating of metals and alloys. The quality of the electroplated film, including adhesion and uniformity, is highly dependent on potentially harsh operating conditions, such as high current density, high temperature, and low pH. Due to its durability, IrO... x It has been used as an electrode material in some industrial electroplating processes. Electrodes made from the novel electrocatalyst disclosed herein can, under appropriate conditions, replace IrO. x Other precious metals / transition metals / platinum group metals are used in electroplating processes.

[0116] Electrode coating for chlorine production The chlorine evolution reaction (CER) is a key anolyte reaction in chlor-alkali electrolysis and has been applied on an industrial scale. Pure noble metal electrocatalysts are typically used. The reaction can be carried out at neutral and acidic pH, but both are prone to competing side reactions such as the oxygen evolution reaction (OER). Introducing other elements, such as those included in the novel catalyst disclosed herein, can help mitigate these factors. Electrodes made from the novel electrocatalyst disclosed herein can, under appropriate conditions, replace IrO. x Other precious metals / transition metals / platinum group metals are used in CER and other halogen generation applications.

[0117] Electrocatalysts for hydrogen generation and oxidation The hydrogen evolution reaction (HER) and the hydrogen oxidation reaction (HOR) are crucial for the future of hydrogen fuels. The HOR reaction rate is inhibited under alkaline conditions. Therefore, this reaction is typically carried out under acidic conditions and requires the use of stable and rare IrO. x Electrodes made from the novel electrocatalyst disclosed herein can replace IrO under appropriate conditions. x Other precious metals / transition metals / platinum group metals are used in HER / HOR reactions.

[0118] Electrocatalysts for oxygen generation and reduction The oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) are core steps in many energy conversion and storage systems, but they tend to be kineticly slow and involve multiple electron transfer processes. Platinum and other platinum group metal (PGM) based materials are commonly used for OER / ORR. Electrodes made from the novel electrocatalyst disclosed herein can replace IrO under appropriate conditions. x Other precious metals / transition metals / platinum group metals are used in the OER / ORR reaction.

[0119] Electrocatalysts for CO2 conversion Electrocatalytic conversion of CO2 is a potential pathway to reduce anthropogenic CO2 emissions and to store excess renewable electricity as chemical energy. Various noble metal and transition metal catalysts have been developed for electrocatalytic CO2 conversion, but their effectiveness is still limited by low energy efficiency, reaction selectivity, and overall conversion rate. The electrode prepared from the novel electrocatalyst disclosed in this paper can, under appropriate conditions, replace noble metals / transition metals / platinum group metals in electrocatalytic CO2 conversion reactions.

[0120] Electrocatalysts for biomass conversion The selective and efficient electrochemical conversion of biomass derivatives can provide an economically viable and scalable pathway for renewable energy storage. Both biomass conversion and OER (Organic Energy Transfer) involve nucleophilic reactions. Therefore, the selection of materials for biomass conversion is primarily based on highly efficient OER electrocatalysts, such as IrO2. Electrodes prepared from the novel electrocatalysts disclosed herein can, under appropriate conditions, replace noble metals / transition metals / platinum group metals in the electrocatalytic biomass conversion reaction.

[0121] Catalysts for hydrogenation and dehydrogenation Electrocatalytic hydrogenation (ECH) and dehydrogenation reactions prepare high-value chemicals from organic feedstocks and water. However, these reactions are limited by the low solubility of reagents in aqueous conditions and electrical losses under organic conditions. Typically, these reactions employ noble metals and platinum group metals. Electrodes prepared from the novel electrocatalysts disclosed herein can, where appropriate, replace noble metals / transition metals / platinum group metals in electrocatalytic hydrogenation / dehydrogenation reactions.

[0122] Catalysts used for ammonia generation and conversion Ammonia is a fundamental chemical used in numerous industrial applications and has historically been primarily produced through CO2 emission processes. Developing clean electrocatalytic ammonia production technologies offers a pathway for the decentralized production of ammonia from locally available renewable energy sources at room temperature. The nitrate reduction reaction (NRR) uses noble metal-based catalysts to produce ammonia from nitrate ions, which are abundant in contaminated groundwater and industrial wastewater. Electrodes made from the novel electrocatalysts disclosed herein can, where appropriate, replace noble metals / transition metals / platinum group metals in the electrocatalytic production and conversion of ammonia.

[0123] Catalysts used for gas purification (including deoxygenation, dehydrogenation, CO2 purification, etc.).

[0124] Electrocatalytic reactions as described above, as well as others, can be used for gas purification. For example, H2 streams from OERs typically contain unsafe levels of O2. Platinum group metal electrocatalysts can be used to selectively remove O2 from H2 streams. Furthermore, flue gas from industrial combustion may contain significant amounts of CO2, which is a target for capture and utilization. However, flue gas also contains significant impurities such as SO2, which can poison the active sites of ideal electrocatalysts. Electrodes made from the novel electrocatalysts disclosed herein can, where appropriate, replace noble metals / transition metals / platinum group metals in electrocatalytic gas purification reactions.

[0125] Electrocatalysts for organic oxidation reactions Electrooxidation of organic compounds can utilize local green electricity to produce high-value chemicals from organic feedstocks and water. These reactions are limited by the lack of stable and efficient electrocatalyst materials. Electrodes prepared from the novel electrocatalysts disclosed herein can, under appropriate conditions, replace noble metals / transition metals / platinum group metals in electrocatalytic hydrogenation / dehydrogenation reactions.

[0126] Specific material space for synthesis: ·IrW ·IrMo ·IrRe ·RuW ·RuMo ·RuRe ·IrRuW ·IrRuRe ·IrRuMo ·IrWRe ·RuWRe ·IrFe ·RuFe ·IrRuFe ·IrPd ·RuPd ·IrRuPd ·IrRh ·RuRh ·IrRuRh ·IrMn ·RuMn ·IrRuMn ·IrCr ·RuCr ·IrRuCr The following tables are provided: Table 1 is a description of catalyst material sample combinations that exhibit moderately high early life (BOL) activity according to exemplary embodiments. Table 2 is a description of catalyst material sample combinations exhibiting high early lifetime (BOL) activity according to exemplary embodiments; Table 3 is a description of catalyst material sample combinations that exhibit higher early life (BOL) activity according to exemplary embodiments; Table 4 is a description of catalyst material sample combinations that exhibit moderately high end-of-life (EOL) activity according to exemplary embodiments. Table 5 is a description of catalyst material sample combinations exhibiting high end-of-life (EOL) activity according to exemplary embodiments; Table 6 is a description of catalyst material sample combinations that exhibit higher end-of-life (EOL) activity according to exemplary embodiments; Table 7 is a description of catalyst material sample combinations that exhibit moderate to high stability according to exemplary embodiments; Table 8 is a description of catalyst material sample combinations exhibiting high stability according to exemplary embodiments; Table 9 is a description of catalyst material sample combinations that exhibit higher stability according to exemplary embodiments; Table 10 is a description of catalyst material sample combinations that exhibit moderate to high overall performance according to exemplary embodiments; Table 11 is a description of catalyst material sample combinations exhibiting high overall performance according to exemplary embodiments; Table 12 is a description of catalyst material sample combinations that exhibit higher overall performance according to exemplary embodiments; Table 13 is a description of catalyst material sample combinations that demonstrate excellent overall performance according to exemplary embodiments; Tables 14-17 describe the composition of specific catalyst material samples selected from the combinations shown in Tables 10-13 according to exemplary embodiments, exhibiting moderately high, high, higher, and excellent overall performance.

[0127] Table 18 shows a range of preferred catalyst material sample combinations based on gram-level sample performance according to exemplary embodiments. For each constituent element, the minimum (lowest atomic %) and maximum (highest atomic %) composition values ​​cover the preferred range. All atomic % values ​​were generated from hundreds of features measured by SEM-EDS.

[0128] Table 19 describes various individual novel catalyst material combinations, including samples whose PEM electrolyzer performance reaches or exceeds that of commercial Ir catalysts (Umicore Ir catalyst, batch number 1029-29 / 13). The average atomic % composition values ​​for each constituent element in each sample are listed. Deviations in these values ​​describe the average deviation for any given feature in the sample, and the minimum (lowest atomic %) and maximum (highest atomic %) composition values ​​for each element are reported (where applicable). All atomic % values ​​and deviations were generated from hundreds of features measured by SEM-EDS. Structural information for each sample was acquired via SEM and is expressed as the effective circle diameter (ECD). ECD represents the size of irregular objects in an image by calculating the diameter of a theoretical circle equal to the area of ​​the object. The catalyst powder was loaded onto a glassy carbon electrode, and OER activity was screened in a three-electrode test by linear sweep voltammetry (1.1–1.8 V vs. RHE, reported as µA / µg at 1.8 V vs. RHE) and durability was screened by chronoamperometry (1.65 V vs. RHE, duration 5–800 min, reported as percentage of activity loss after retention). Finally, the catalyst was applied as an anode material to an ion exchange membrane, where the concentration was expressed as mg / cm³. 2 Membrane resistance (HFR) was measured in mΩ to measure the load, followed by testing in a PEM electrolyzer apparatus. BOL activity in the PEM electrolyzer was determined by linear scan and reported as A / cm at 2.0V vs. RHE. 2 The degradation rate of the PEM electrolyzer will only be reported after the catalyst has been tested for more than 50 hours under the corresponding accelerated stress test conditions (i.e., square wave, SqW).

[0129]

[0130] Table 1: Moderately high BOL activity

[0131] Table 2: High BOL Activity

[0132] Table 3: Higher BOL activity

[0133] Table 4: Moderately High EOL Activity

[0134] Table 5: High EOL Activity

[0135] Table 6: Higher EOL Activity

[0136] Table 7: Moderately High Stability

[0137] Table 8: High Stability

[0138] Table 9: Higher Stability

[0139] Table 10: Overall Performance (Moderately High)

[0140] Table 11: High Overall Performance

[0141] Table 12: Improved Overall Performance

[0142] Table 13: Excellent Overall Performance

[0143] Table 14: Overall Performance Data (Moderately High)

[0144] Table 15: Overall Performance Data

[0145] Table 16: Higher Overall Performance Data

[0146] Table 17: Excellent Overall Performance Data

[0147] Table 18. Showing the atomic percentage range of catalyst materials for scale-up of preferred features.

[0148] Table 19. Catalyst Samples and Their Characteristics for Large-Scale Production Terms and conditions of this disclosure: Article [1]: A catalyst comprising: Multimetallic materials, including Ir as the first metal; and At least one other metal selected from the group consisting of W, Mo, Re, Ru, Fe, Pd, Rh, Mn and Cr.

[0149] Article [2]: The catalyst according to any of the preceding articles, wherein the composition of the catalyst and the atomic ratio of the metal are given in Tables 1-19 and Figure 2A-22 The set disclosed contains at least one composition and atomic ratio specification.

[0150] Article [3]: A catalyst according to any of the preceding articles, wherein one or more metals in the catalyst are oxidized.

[0151] Article [4]: ​​The catalyst according to any of the preceding articles, wherein the crystallinity of the oxide may vary from amorphous to fully crystalline.

[0152] Article [5]: The catalyst according to any of the preceding articles, wherein the ratio of oxide to metal is complete oxidation, partial oxidation or complete metal.

[0153] Article [6]: The catalyst according to any of the preceding articles, wherein the oxide is prepared by thermal annealing, calcination, chemical method or electrochemical method.

[0154] Article [7]: The catalyst according to any of the preceding articles, wherein the metal comprises a single phase.

[0155] Article [8]: A catalyst according to any of the preceding articles, wherein the metal comprises one or more mixed phases.

[0156] Article [9]: A catalyst according to any of the preceding articles, wherein the catalyst is unsupported or supported on carbon, silicon carbide, alumina, silicon dioxide, titanium, titanium dioxide, tungsten, tungsten oxide, niobium oxide, indium tin oxide, fluorine-doped tin oxide, graphene or the like.

[0157]

[10] : A catalyst according to any of the preceding clauses, wherein the catalyst contains up to 10 atomic percent of additional elements, such as Pt, Os, Ta, Ce, Ba, Hf, In, Sn, Sb, Au, Ag, Sr, Y, Sc, Nb, La, Pr, Sm, Cu.

[0158]

[11] : A catalyst according to any of the preceding clauses, wherein the catalyst contains up to 10 atomic percent of additional elements, such as Ni and Co, but does not include a composition consisting only of Ir, Ru, Ni and Co.

[0159] Article

[12] : The catalyst according to any of the preceding articles, wherein the surface of the catalyst is nanostructured.

[0160] Article

[13] : The catalyst according to any of the preceding articles, wherein the metal or metal oxide is deposited onto the template by at least one of electrodeposition, chemical vapor deposition, physical vapor deposition and atomic layer deposition.

[0161] Article

[14] : The catalyst according to any of the preceding articles, wherein the catalyst is synthesized by polymer pen lithography.

[0162] Article

[15] : A catalyst according to any of the preceding articles, wherein the synthesis of the catalyst includes one or more of the Adams melting process, colloidal synthesis, precipitation and spray pyrolysis.

[0163] Article

[16] : A method for catalyzing an electrochemical reaction, comprising: Provides a multimetallic material comprising at least two metals, wherein the first metal is Ir, and one or more of the other metals are derived from the group consisting of W, Mo, Re, Ru, Fe, Pd, Rh, Mn, and Cr; and The polymetallic material is used as a catalyst in the reaction.

[0164] Section

[17] : The method according to any of the preceding sections, wherein the composition of the catalyst and the atomic ratio of the metal are given by Tables 1-19 and Figure 2A-22 The set disclosed contains at least one composition and atomic ratio specification.

[0165] Article

[18] : In any of the preceding articles, one or more metals in the catalyst are oxidized.

[0166] Article

[19] : The method according to any of the preceding articles, wherein the crystallinity of the oxide can vary from amorphous to fully crystalline.

[0167] Article

[20] : The method according to any of the preceding articles, wherein the ratio of oxide to metal is complete oxidation, partial oxidation or complete metal.

[0168] Article

[21] : The method according to any of the preceding articles, wherein the oxide is prepared by thermal annealing, calcination, chemical method or electrochemical method.

[0169] Article

[22] : The method according to any of the preceding articles, wherein the catalyst is unsupported or supported on carbon, silicon carbide, alumina, silicon dioxide, titanium, titanium dioxide, tungsten, tungsten oxide, niobium oxide, indium tin oxide, fluorine-doped tin oxide, graphene or the like.

[0170]

[23] : The method according to any of the preceding paragraphs, wherein the catalyst contains up to 10 atomic percent of additional elements, such as Pt, Os, Ta, Ce, Ba, Hf, In, Sn, Sb, Au, Ag, Sr, Y, Sc, Nb, La, Pr, Sm, Cu.

[0171]

[24] : The method according to any of the preceding paragraphs, wherein the catalyst contains up to 10 atomic percent of additional elements, such as Ni and Co, but does not include a composition consisting only of Ir, Ru, Ni and Co.

[0172] Article

[25] : The method according to any of the preceding articles, wherein the surface of the catalyst is nanostructured.

[0173] Article

[26] : The method according to any of the preceding articles, wherein the metal or metal oxide is deposited onto the template by at least one of electrodeposition, chemical vapor deposition, physical vapor deposition and atomic layer deposition.

[0174] Article

[27] : The method according to any of the preceding articles, wherein the catalyst is synthesized by polymer pen lithography.

[0175] Article

[28] : The method according to any of the preceding articles, wherein the catalyst synthesis includes one or more of Adams melting, colloidal synthesis, precipitation and spray pyrolysis.

[0176] Article

[29] : A method for catalyzing an electrochemical reaction, comprising: Provides a multimetallic material comprising at least two metals, wherein the first metal of the at least two metals is Ru, and one or more other metals of the at least two metals are derived from the group consisting of W, Mo, Re, Ir, Fe, Pd, Rh, Mn, and Cr; and The polymetallic material is used as a catalyst in the reaction.

[0177] Article

[30] : The method according to any of the preceding articles, wherein applying the catalyst to the reaction includes applying the catalyst to the oxygen evolution reaction (OER).

[0178] Article

[31] : The method described in any of the preceding articles, wherein the OER reaction is an acidic OER.

[0179] Article

[32] : The method described in any of the preceding articles, wherein the OER reaction is an alkaline OER.

[0180] Article

[33] : The method according to any of the preceding articles, wherein applying the catalyst to the reaction includes applying the catalyst to hydrogen generation and / or oxidation.

[0181] Article

[34] : The method according to any of the preceding articles, wherein applying the catalyst to the reaction includes applying the catalyst to oxygen generation and reduction.

[0182] Article

[35] : The method according to any of the preceding articles, wherein applying the catalyst to the reaction includes applying the catalyst to CO2 conversion.

[0183] Article

[36] : The method according to any of the preceding articles, wherein applying the catalyst to the reaction includes applying the catalyst to the conversion of biomass into organic products.

[0184] Article

[37] : The method according to any of the preceding articles, wherein applying the catalyst to the reaction includes applying the catalyst to hydrogenation and / or dehydrogenation.

[0185] Article

[38] : The method according to any of the preceding articles, wherein applying the catalyst to the reaction includes applying the catalyst to an organic oxidation reaction.

[0186] Article

[39] : The method according to any of the preceding articles, wherein applying the catalyst to the reaction includes applying the catalyst to the generation of halogen gas.

[0187] Article

[40] : The method according to any of the preceding articles, wherein applying the catalyst to the reaction includes applying the catalyst to the generation and / or conversion of ammonia.

[0188] Article

[41] : The method according to any of the preceding articles, wherein applying the catalyst to the reaction includes applying the catalyst to gas purification.

[0189] Article

[42] : The method according to any of the preceding articles, wherein applying the catalyst to the reaction includes applying the catalyst to deoxygenation, dehydrogenation and / or CO2 purification.

[0190] Section

[43] : A method for catalyzing a non-electrochemical reaction, comprising: A multimetallic material of two or more elements, wherein the first metal is Ir, and one or more other metals are derived from the group consisting of W, Mo, Re, Ru, Fe, Pd, Rh, Mn, and Cr; and The catalyst is used in the reaction.

[0191] Section

[44] : The method according to any of the preceding sections, wherein the composition of the catalyst and the atomic ratio of the metal are given by Tables 1-19 and Figure 2A-22 The set disclosed contains at least one composition and atomic ratio specification.

[0192] Article

[45] : In any of the preceding articles, one or more metals in the catalyst are oxidized.

[0193] Article

[46] : The method according to any of the preceding articles, wherein the crystallinity of the oxide can vary from amorphous to fully crystalline.

[0194] Article

[47] : The method according to any of the preceding articles, wherein the ratio of oxide to metal is complete oxidation, partial oxidation or complete metal.

[0195] Article

[48] : The method according to any of the preceding articles, wherein the oxide is prepared by thermal annealing, calcination, chemical method or electrochemical method.

[0196] Article

[49] : The method according to any of the preceding articles, wherein the catalyst is unsupported and is supported on carbon, silicon carbide, alumina, silicon dioxide, titanium, titanium dioxide, tungsten, tungsten oxide, niobium oxide, indium tin oxide, fluorine-doped tin oxide, graphene or otherwise.

[0197]

[50] The method according to any of the preceding paragraph, wherein the catalyst comprises up to 10 atomic percent of one or more additional elements selected from the group consisting of Pt, Os, Ta, Ce, Ba, Hf, In, Sn, Sb, Au, Ag, Sr, Y, Sc, Nb, La, Pr, Sm, Cu.

[0198]

[51] The method according to any of the preceding paragraph, wherein the catalyst comprises up to 10 atomic percent of one or more additional elements selected from the group consisting of Ni and Co, but excluding the composition consisting only of Ir, Ru, Ni and Co.

[0199] Article

[52] : The method according to any of the preceding articles, wherein the surface of the catalyst is nanostructured.

[0200] Article

[53] : The method according to any of the preceding articles, wherein the metal or metal oxide is deposited onto the template by at least one of electrodeposition, chemical vapor deposition, physical vapor deposition and atomic layer deposition.

[0201] Article

[54] : The method according to any of the preceding articles, wherein the catalyst is synthesized by polymer pen lithography.

[0202] Article

[55] : The method according to any of the preceding articles, wherein the catalyst synthesis includes one or more of Adams melting, colloidal synthesis, precipitation and spray pyrolysis.

[0203] Article

[56] : A method for catalyzing a non-electrochemical reaction, comprising: Provide a multimetallic material comprising two or more elements, wherein the first metal is Ru, and one or more other metals are derived from the group consisting of W, Mo, Re, Ir, Fe, Pd, Rh, Mn, and Cr; and The catalyst is used in the reaction.

[0204] Article

[57] : The method according to any of the preceding articles, wherein applying the catalyst to the reaction includes applying the catalyst to CO2 or CO conversion.

[0205] Article

[58] : The method according to any of the preceding articles, wherein applying the catalyst to the reaction includes applying the catalyst to the conversion of biomass into organic products.

[0206] Article

[59] : The method according to any of the preceding articles, wherein applying the catalyst to the reaction includes applying the catalyst to hydrogenation and / or dehydrogenation.

[0207] Article

[60] : The method according to any of the preceding articles, wherein applying the catalyst to the reaction includes applying the catalyst to an organic oxidation reaction.

[0208] Article

[61] : The method according to any of the preceding articles, wherein applying the catalyst to the reaction includes applying the catalyst to the generation and / or conversion of ammonia.

[0209] Article

[62] : The method according to any of the preceding articles, wherein applying the catalyst to the reaction includes applying the catalyst to gas purification.

[0210] Section

[63] : An electrocatalyst comprising: Multimetallic materials containing two or more metals. Wherein, the first metal in the two or more metals is Ru; and One or more of the other metals are selected from the group consisting of W, Mo, Re, Ir, Fe, Pd, Rh, Mn, and Cr.

[0211] Section

[64] : An electrocatalyst according to any of the preceding sections, wherein the composition of the catalyst and the atomic ratio of the metal are given by Tables 1-19 and Figure 2A-22 The set disclosed contains at least one composition and atomic ratio specification.

[0212] Article

[65] : An electrocatalyst according to any of the preceding articles, wherein one or more metals in the catalyst are oxidized.

[0213] Article

[66] : An electrocatalyst according to any of the preceding articles, wherein the crystallinity of the oxide may vary from amorphous to fully crystalline.

[0214] Article

[67] : The electrocatalyst according to any of the preceding articles, wherein the ratio of oxide to metal is complete oxidation, partial oxidation or complete metal.

[0215] Article

[68] : An electrocatalyst according to any of the preceding articles, wherein the oxide is prepared by thermal annealing, calcination, chemical method or electrochemical method.

[0216] Article

[69] : An electrocatalyst according to any of the preceding articles, wherein the catalyst is unsupported or supported on carbon, silicon carbide, alumina, silicon dioxide, titanium, titanium dioxide, tungsten, tungsten oxide, niobium oxide, indium tin oxide, fluorine-doped tin oxide, graphene or the like.

[0217]

[70] : An electrocatalyst according to any of the preceding paragraphs, wherein the catalyst comprises up to 10 atomic percent of one or more additional elements selected from the group consisting of Pt, Os, Ta, Ce, Ba, Hf, In, Sn, Sb, Au, Ag, Sr, Y, Sc, Nb, La, Pr, Sm, and Cu.

[0218]

[71] : An electrocatalyst according to any of the preceding paragraph, wherein the catalyst contains up to 10 atomic percent of one or more additional elements selected from the group consisting of Ni and Co, but excluding a composition consisting only of Ir, Ru, Ni and Co.

[0219] Article

[72] : An electrocatalyst according to any of the preceding articles, wherein the surface of the catalyst is nanostructured.

[0220] Article

[73] : An electrocatalyst according to any of the preceding articles, wherein the metal or metal oxide is deposited onto the template by at least one of electrodeposition, chemical vapor deposition, physical vapor deposition and atomic layer deposition.

[0221] Article

[74] : The electrocatalyst according to any of the preceding articles, wherein the catalyst is synthesized by polymer pen lithography.

[0222] Article

[75] : An electrocatalyst according to any of the preceding articles, wherein the synthesis of the catalyst includes one or more of the Adams melting process, colloidal synthesis, precipitation and spray pyrolysis.

[0223] Article

[76] : The method according to any of the preceding articles, wherein applying the catalyst to the reaction includes applying the catalyst to a process of producing chlorine gas that results in anodic oxygen evolution at the electrode surface, such as cathode electrodeposition, electrodeposition, metal plating, or anodic oxygen evolution at the electrode surface.

[0224] Article

[77] : The catalyst or method according to any one of the preceding claims, wherein the concentration of one of Ir, Ru, W, Mo, Re, Fe, Pd, Rh, Mn and / or Cr is zero.

[0225] Article

[78] : A catalyst or method according to any one of the preceding claims, wherein the concentrations of Ir, Ru, W, Mo, Re, Fe, Pd, Rh, Mn and / or Cr are defined as the average concentrations within the catalyst.

[0226] Therefore, the various embodiments of the present invention disclosed above are intended to be illustrative and not to limit the invention. Various modifications can be made without departing from the spirit and scope of the invention. Therefore, those skilled in the art should understand that the described exemplary embodiments are merely examples, and various modifications can be made within the scope of the invention as defined in the appended claims.

Claims

1. A catalyst, comprising: Multimetallic materials, wherein the first metal is Ir; and At least one other metal selected from the group consisting of W, Mo, Re, Ru, Fe, Pd, Rh, Mn and Cr.

2. The catalyst according to claim 1, wherein, The composition of the catalyst and the atomic ratio of the metal are defined by at least one of those compositions and atomic ratios disclosed in the set of Tables 1-19 and Figures 2A-22.

3. The catalyst according to claim 1, wherein, One or more metals in the catalyst are oxidized.

4. The catalyst according to claim 3, wherein, The crystallinity of the oxide can vary from amorphous to fully crystalline.

5. The catalyst according to claim 3, wherein, The ratio of oxide to metal is either fully oxidized, partially oxidized, or entirely metallic.

6. The catalyst according to claim 3, wherein, The oxide is prepared by thermal annealing, calcination, chemical methods, or electrochemical methods.

7. The catalyst according to claim 1, wherein, The catalyst is unsupported or supported on carbon, silicon carbide, alumina, silicon dioxide, titanium, titanium dioxide, tungsten, tungsten oxide, niobium oxide, indium tin oxide, fluorine-doped tin oxide, graphene, or others.

8. The catalyst according to claim 1, wherein, The catalyst contains up to 10 atomic percent of additional elements, such as Pt, Os, Ta, Ce, Ba, Hf, In, Sn, Sb, Au, Ag, Sr, Y, Sc, Nb, La, Pr, Sm, Cu.

9. The catalyst according to claim 1, wherein, The catalyst contains up to 10 atomic percent of additional elements, such as Ni and Co, but does not include a composition consisting only of Ir, Ru, Ni and Co.

10. The catalyst according to claim 1, wherein, The surface of the catalyst is nanostructured.

11. The catalyst according to claim 1, wherein, The metal or metal oxide is deposited onto the template by at least one of electrodeposition, chemical vapor deposition, physical vapor deposition, and atomic layer deposition.

12. The catalyst according to claim 1, wherein, The catalyst was synthesized using polymer pen lithography.

13. The catalyst according to claim 13, wherein, The catalyst synthesis includes one or more of the Adams melting process, colloidal synthesis, precipitation, and spray pyrolysis.

14. A method for catalyzing an electrochemical reaction, comprising: Provides a multimetallic material comprising at least two metals, wherein the first metal is Ir, and one or more of the other metals are derived from the group consisting of W, Mo, Re, Ru, Fe, Pd, Rh, Mn, and Cr; and The polymetallic material is used as a catalyst in the reaction.

15. The method according to claim 14, wherein, The composition of the catalyst and the atomic ratio of the metal are defined by at least one of those compositions and atomic ratios disclosed in the set of Tables 1-19 and Figures 2A-22.

16. The method of claim 14, wherein, One or more metals in the catalyst are oxidized.

17. The method according to claim 16, wherein, The crystallinity of the oxide can vary from amorphous to fully crystalline.

18. The method according to claim 16, wherein, The ratio of oxide to metal is either fully oxidized, partially oxidized, or entirely metallic.

19. The method of claim 16, wherein, The oxide is prepared by thermal annealing, calcination, chemical methods, or electrochemical methods.

20. The method of claim 14, wherein, The catalyst is unsupported or supported on carbon, silicon carbide, alumina, silicon dioxide, titanium, titanium dioxide, tungsten, tungsten oxide, niobium oxide, indium tin oxide, fluorine-doped tin oxide, graphene, or others.

21. The method according to claim 14, wherein, The catalyst contains up to 10 atomic percent of additional elements, such as Pt, Os, Ta, Ce, Ba, Hf, In, Sn, Sb, Au, Ag, Sr, Y, Sc, Nb, La, Pr, Sm, Cu.

22. The method according to claim 11, wherein, The catalyst contains up to 10 atomic percent of additional elements, such as Ni and Co, but does not include a composition consisting only of Ir, Ru, Ni and Co.

23. The method according to claim 14, wherein, The surface of the catalyst is nanostructured.

24. The method according to claim 14, wherein, The metal or metal oxide is deposited onto the template by at least one of electrodeposition, chemical vapor deposition, physical vapor deposition, and atomic layer deposition.

25. The method according to claim 14, wherein, The catalyst was synthesized using polymer pen lithography.

26. The method according to claim 14, wherein, The catalyst synthesis includes one or more of the Adams melting process, colloidal synthesis, precipitation, and spray pyrolysis.

27. A method for catalyzing an electrochemical reaction, comprising: Provides a multimetallic material comprising at least two metals, wherein the first metal of the at least two metals is Ru, and one or more other metals of the at least two metals are derived from the group consisting of W, Mo, Re, Ir, Fe, Pd, Rh, Mn, and Cr; and The polymetallic material is used as a catalyst in the reaction.

28. The method according to claim 27, wherein, Applying the catalyst to a reaction includes applying the catalyst to the oxygen evolution reaction (OER).

29. The method according to claim 28, wherein, The OER reaction is an acidic OER.

30. The method according to claim 28, wherein, The OER reaction is an alkaline OER.

31. The method according to claim 27, wherein, Applying the catalyst to a reaction includes applying the catalyst to hydrogen generation and / or oxidation.

32. The method according to claim 27, wherein, Applying the catalyst to a reaction includes applying the catalyst to oxygen generation and reduction.

33. The method according to claim 27, wherein, Applying the catalyst to a reaction includes applying the catalyst to CO2 conversion.

34. The method according to claim 27, wherein, Applying the catalyst to a reaction includes applying the catalyst to the conversion of biomass into organic products.

35. The method according to claim 27, wherein, Applying the catalyst to a reaction includes applying the catalyst to hydrogenation and / or dehydrogenation.

36. The method according to claim 27, wherein, Applying the catalyst to a reaction includes applying the catalyst to an organic oxidation reaction.

37. The method of claim 27, wherein, Applying the catalyst to a reaction includes applying the catalyst to the generation of halogen gases.

38. The method according to claim 27, wherein, Applying the catalyst to a reaction includes applying the catalyst to the generation and / or conversion of ammonia.

39. The method according to claim 27, wherein, Applying the catalyst to a reaction includes applying the catalyst to gas purification.

40. The method of claim 27, wherein, Applying the catalyst to a reaction includes applying the catalyst to deoxygenation, dehydrogenation, and / or CO2 purification.

41. A method for catalyzing a non-electrochemical reaction, comprising: A multimetallic material of two or more elements, wherein the first metal is Ir, and one or more other metals are derived from the group consisting of W, Mo, Re, Ru, Fe, Pd, Rh, Mn, and Cr; and The catalyst is used in the reaction.

42. The method according to claim 41, wherein, The composition of the catalyst and the atomic ratio of the metal are defined by at least one of those compositions and atomic ratios disclosed in the set of Tables 1-19 and Figures 2A-22.

43. The method according to claim 42, wherein, One or more metals in the catalyst are oxidized.

44. The method according to claim 43, wherein, The crystallinity of the oxide can vary from amorphous to fully crystalline.

45. The method according to claim 43, wherein, The ratio of oxide to metal is either fully oxidized, partially oxidized, or entirely metallic.

46. ​​The method according to claim 43, wherein, The oxide is prepared by thermal annealing, calcination, chemical methods, or electrochemical methods.

47. The method according to claim 41, wherein, The catalyst is unsupported and is supported on carbon, silicon carbide, alumina, silicon dioxide, titanium, titanium dioxide, tungsten, tungsten oxide, niobium oxide, indium tin oxide, fluorine-doped tin oxide, graphene, or others.

48. The method according to claim 41, wherein, The catalyst contains up to 10 atomic percent of one or more additional elements selected from the group consisting of Pt, Os, Ta, Ce, Ba, Hf, In, Sn, Sb, Au, Ag, Sr, Y, Sc, Nb, La, Pr, Sm, and Cu.

49. The method according to claim 41, wherein, The catalyst contains up to 10 atomic percent of one or more additional elements selected from the group consisting of Ni and Co, but does not include a composition consisting only of Ir, Ru, Ni and Co.

50. The method according to claim 41, wherein, The surface of the catalyst is nanostructured.

51. The method according to claim 41, wherein, The metal or metal oxide is deposited onto the template by at least one of electrodeposition, chemical vapor deposition, physical vapor deposition, and atomic layer deposition.

52. The method according to claim 41, wherein, The catalyst was synthesized using polymer pen lithography.

53. The method according to claim 41, wherein, The catalyst synthesis includes one or more of the Adams melting process, colloidal synthesis, precipitation, and spray pyrolysis.

54. A method for catalyzing a non-electrochemical reaction, comprising: Provide a multimetallic material comprising two or more elements, wherein the first metal is Ru, and one or more other metals are derived from the group consisting of W, Mo, Re, Ir, Fe, Pd, Rh, Mn, and Cr; and The catalyst is used in the reaction.

55. The method according to claim 54, wherein, Applying the catalyst to a reaction includes applying the catalyst to CO2 or CO conversion.

56. The method according to claim 54, wherein, Applying the catalyst to a reaction includes applying the catalyst to the conversion of biomass into organic products.

57. The method according to claim 54, wherein, Applying the catalyst to a reaction includes applying the catalyst to hydrogenation and / or dehydrogenation.

58. The method according to claim 54, wherein, Applying the catalyst to a reaction includes applying the catalyst to an organic oxidation reaction.

59. The method according to claim 54, wherein, Applying the catalyst to a reaction includes applying the catalyst to the generation and / or conversion of ammonia.

60. The method according to claim 54, wherein, Applying the catalyst to a reaction includes applying the catalyst to gas purification.

61. An electrocatalyst, comprising: Multimetallic materials containing two or more metals. Wherein, the first metal in the two or more metals is Ru; and One or more of the other metals are selected from the group consisting of W, Mo, Re, Ir, Fe, Pd, Rh, Mn, and Cr.

62. The electrocatalyst according to claim 61, wherein, The composition of the catalyst and the atomic ratio of the metal are defined by at least one of those compositions and atomic ratios disclosed in the sets of Tables 1-17 and Figures 2A-14B.

63. The electrocatalyst according to claim 61, wherein, One or more metals in the catalyst are oxidized.

64. The electrocatalyst according to claim 63, wherein, The crystallinity of the oxide can vary from amorphous to fully crystalline.

65. The electrocatalyst according to claim 63, wherein, The ratio of oxide to metal is either fully oxidized, partially oxidized, or entirely metallic.

66. The electrocatalyst according to claim 63, wherein, The oxide is prepared by thermal annealing, calcination, chemical methods, or electrochemical methods.

67. The electrocatalyst according to claim 61, wherein, The catalyst is unsupported or supported on carbon, silicon carbide, alumina, silicon dioxide, titanium, titanium dioxide, tungsten, tungsten oxide, niobium oxide, indium tin oxide, fluorine-doped tin oxide, graphene, or others.

68. The electrocatalyst according to claim 61, wherein, The catalyst contains up to 10 atomic percent of one or more additional elements selected from the group consisting of Pt, Os, Ta, Ce, Ba, Hf, In, Sn, Sb, Au, Ag, Sr, Y, Sc, Nb, La, Pr, Sm, and Cu.

69. The electrocatalyst according to claim 61, wherein, The catalyst contains up to 10 atomic percent of one or more additional elements selected from the group consisting of Ni and Co, but does not include a composition consisting only of Ir, Ru, Ni and Co.

70. The electrocatalyst according to claim 61, wherein, The surface of the catalyst is nanostructured.

71. The electrocatalyst according to claim 61, wherein, The metal or metal oxide is deposited onto the template by at least one of electrodeposition, chemical vapor deposition, physical vapor deposition, and atomic layer deposition.

72. The electrocatalyst according to claim 61, wherein, The catalyst was synthesized using polymer pen lithography.

73. The electrocatalyst according to claim 61, wherein, The catalyst synthesis includes one or more of the Adams melting process, colloidal synthesis, precipitation, and spray pyrolysis.

74. The method according to claim 27, wherein, Applying the catalyst to reactions includes applying the catalyst to processes such as cathode electrodeposition, electrodeposition, metal plating, and the production of chlorine gas that leads to anodic oxygen evolution on electrode surfaces.

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