# US 9,873,107 B2 · Process for the production of a carbon supported catalyst > Agents: this data is available as JSON from the patentgrep API and MCP server — see https://patentgrep.com/llms.txt - Number: US 9,873,107 B2 - Document ID: US9873107B2 - Status: Granted - Kind: B2 - Application number: 15/126,801 - Filed: 2015-03-17 - Published: 2017-04-13 - Granted: 2018-01-23 - Earliest claimed: 2014-03-18 - Assignees: BASF SE - Applicants: BASF SE - Inventors: Andreas Hass; Ekkehard Schwab; Franz Weber; Nicole Becker - Web page: https://patentgrep.com/patent/US9873107B2 ## CPC - B01J 21/18: Carbon - B01J 23/63: with rare earths or actinides - B01J 23/6484: {Niobium} - B01J 23/6522: {Chromium} - B01J 23/89: combined with noble metals - B01J 35/33: Electric or magnetic properties - B01J 35/393: {Metal or metal oxide crystallite size} - B01J 35/399: {homogeneously throughout the support particle} - B01J 35/45: Nanoparticles - B01J 35/615: {100-500 m2/g} - B01J 35/617: {500-1000 m2/g} - B01J 35/618: {more than 1000 m2/g} - B01J 35/70: characterised by their crystalline properties, e.g. semi-crystalline (catalysts comprising carbon B01J21/18; molecular sieves B01J29/00) - B01J 37/0045: {Drying a slurry, e.g. spray drying} - B01J 37/0203: {the impregnation liquid containing organic compounds} - B01J 37/0221: {of particles} - B01J 37/035: {Precipitation on carriers} - B01J 37/08: Heat treatment {(B01J37/0009, B01J37/0018 take precedence)} - B01J 37/16: Reducing - B01J 2235/00: Indexing scheme associated with group B01J35/00, related to the analysis techniques used to determine the catalysts form or properties - B01J 2235/15: X-ray diffraction - B01J 2235/30: Scanning electron microscopy; Transmission electron microscopy - H01M 4/9083: {on carbon or graphite} - H01M 4/926: {on carbon or graphite} - Y02E 60/50: Fuel cells - B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS - H01M: PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY - Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION ## Abstract A process for the production of a carbon supported catalyst, which comprises the following steps: (a) precipitation of at least one metal oxide onto a surface of a carbon-comprising support by preparing an initial mixture, comprising the carbon-comprising support, at least one metal oxide precursor and an organic solvent, and spray-drying of the initial mixture to obtain an intermediate product, (b) loading of noble-metal-comprising particles onto the surface of the intermediate product in a liquid medium by deposition, precipitation and/or reduction of a noble-metal-comprising precursor with a reducing agent, (c) heat treatment of the catalyst precursor resulting from step (b) at a temperature higher than 400° C. ## Claims ### Claim 1 A process for the production of a carbon supported catalyst, which comprises the following steps: (a) precipitation of at least one metal oxide onto a surface of a carbon-comprising support by preparing an initial mixture, comprising the carbon-comprising support, at least one metal oxide precursor and an organic solvent, and spray-drying of the initial mixture to obtain an intermediate product, (b) loading of noble-metal-comprising particles onto the surface of the intermediate product in a liquid medium by deposition, precipitation and/or reduction of a noble-metal-comprising precursor with a reducing agent, (c) heat treating the catalyst precursor resulting from step (b) at a temperature higher than 400° C., wherein the spray-drying is carried out with a drying gas at a temperature between 60° C. and 300° C. ### Claim 2 (depends on 1) The process according to claim 1, wherein the at least one metal oxide precursor comprises niobium, titanium, tantalum, molybdenum, vanadium, tungsten, cerium, zirconium, tin, silicon, or mixtures thereof and the metal oxide precursor is an alcoholate or a halide. ### Claim 3 (depends on 1) The process according to claim 1, wherein the metal oxide precursor is an alcoholate selected from the group consisting of ethanolate, n-propanolate, iso-propanolate, n-butanolate, iso-butanolate and tert-butanolate, or the metal oxide precursor is a chloride. ### Claim 4 (depends on 1) The process according to claim 1, wherein the organic solvent is an alcohol, a carboxylate ester, acetone or tetrahydrofuran. ### Claim 5 (depends on 1) The process according to claim 1, wherein the initial mixture comprises less than 2% by weight of water. ### Claim 6 (depends on 1) The process according to claim 1, wherein the initial mixture comprises up to 20% by weight of water. ### Claim 7 (depends on 1) The process according to claim 1, wherein the carbon-comprising support has a BET surface area of at least 500m2/g. ### Claim 8 (depends on 1) The process according to claim 1, wherein the carbon-comprising support comprises carbon black, graphene, graphite, activated carbon or carbon nanotubes. ### Claim 9 (depends on 1) The process according to claim 1, wherein the loaded noble-metal-comprising particles comprise platinum and optionally cobalt, nickel, chromium, copper, palladium, gold, ruthenium, scandium, yttrium, lanthanium, niobium or titanium. ### Claim 10 (depends on 9) A carbon supported catalyst produced according to claim 9, wherein the carbon supported catalyst comprises between 2% by weight and 25% by weight of niobium oxide, a mass ratio of niobium comprised in the carbon supported catalyst and platinum comprised in the carbon supported catalyst is between 0.05 and 0.5, and at least 90% by number of platinum comprising particles comprised in the carbon supported catalyst have a diameter smaller than 20 nm. ### Claim 11 (depends on 1) The process according to claim 1, wherein the spray-drying is operated with a residence time of less than 3 minutes. ### Claim 12 (depends on 1) The process according to claim 1, wherein the heat treatment in step (c) is carried out in a reducing atmosphere. ### Claim 13 (depends on 12) The process according to claim 12, wherein the reducing atmosphere comprises up to 5% by volume of hydrogen. ### Claim 14 (depends on 1) The process according to claim 1, wherein a molar ratio of metal comprised in the at least one metal oxide precursor and carbon comprised in the carbon-comprising support in the initial mixture is between 0.00005 and 0.01, a carbon content in the initial mixture is between 1% and 30% by weight and a molar ratio of metal, originating from the at least one metal oxide precursor and comprised in the intermediate product, and the noble-metal-comprising particles comprise platinum and the platinum comprised in the liquid medium is between 0.05 and 0.8. ### Claim 15 A process for the production of a carbon supported catalyst, which comprises the following steps: (a) precipitation of at least one metal oxide onto a surface of a carbon-comprising support by preparing an initial mixture, comprising the carbon-comprising support, at least one metal oxide precursor and an organic solvent, and spray-drying of the initial mixture to obtain an intermediate product, (a) loading of noble-metal-comprising particles onto the surface of the intermediate product in a liquid medium by deposition, precipitation and/or reduction of a noble-metal-comprising precursor with a reducing agent, (b) heat treating the catalyst precursor resulting from step (b) at a temperature higher than 400° C. wherein the spray-drying is carried out in a countercurrent mode. ### Claim 16 A process for the production of a carbon supported catalyst, which comprises the following steps: (c) precipitation of at least one metal oxide onto a surface of a carbon-comprising support by preparing an initial mixture, comprising the carbon-comprising support, at least one metal oxide precursor and an organic solvent, and spray-drying of the initial mixture to obtain an intermediate product, (d) loading of noble-metal-comprising particles onto the surface of the intermediate product in a liquid medium by deposition, precipitation and/or reduction of a noble-metal-comprising precursor with a reducing agent, (e) heat treating the catalyst precursor resulting from step (b) at a temperature higher than 400° C., wherein the spray-drying is carried out with an inert drying gas.