Supercritical Antisolvent Precipitation of Amorphous Copper–Zinc Georgeite and Acetate Precursors for the Preparation of Ambient‐Pressure Water‐Gas‐Shift Copper/Zinc Oxide Catalysts

Smith, Paul J.; Kondrat, Simon A.; Carter, James H.; Chater, Philip A.; Bartley, Jonathan K.; Taylor, Stuart H.; Spencer, Michael S.; Hutchings, Graham J.

doi:10.1002/cctc.201601603

Title: Supercritical Antisolvent Precipitation of Amorphous Copper–Zinc Georgeite and Acetate Precursors for the Preparation of Ambient‐Pressure Water‐Gas‐Shift Copper/Zinc Oxide Catalysts

Journal Article · Fri Mar 31 00:00:00 EDT 2017 · ChemCatChem

DOI:https://doi.org/10.1002/cctc.201601603· OSTI ID:1357273

Smith, Paul J. ^[1]; Kondrat, Simon A. ^[1]; Carter, James H. ^[1]; Chater, Philip A. ^[2]; Bartley, Jonathan K. ^[1]; Taylor, Stuart H. ^[1]; Spencer, Michael S. ^[1];

^[1]

Cardiff Catalysis Institute, School of ChemistryCardiff University Main Building, Park Place Cardiff CF10 3AT UK
Diamond Light Source Didcot OX11 0DE UK

Abstract A series of copper–zinc acetate and zincian georgeite precursors have been produced by supercritical CO ₂ antisolvent (SAS) precipitation as precursors to Cu/ZnO catalysts for the water gas shift (WGS) reaction. The amorphous materials were prepared by varying the water/ethanol volumetric ratio in the initial metal acetate solutions. Water addition promoted georgeite formation at the expense of mixed metal acetates, which are formed in the absence of the water co‐solvent. Optimum SAS precipitation occurs without water to give high surface areas, whereas high water content gives inferior surface areas and copper–zinc segregation. Calcination of the acetates is exothermic, producing a mixture of metal oxides with high crystallinity. However, thermal decomposition of zincian georgeite resulted in highly dispersed CuO and ZnO crystallites with poor structural order. The georgeite‐derived catalysts give superior WGS performance to the acetate‐derived catalysts, which is attributed to enhanced copper–zinc interactions that originate from the precursor.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE; Engineering and Physical Sciences Research Council; European Research Council (ERC)

Grant/Contract Number:: AC02-06CH11357; 291319; EP/K014714/1; EP/K014668/1; EP/K014706/1; EP/H000925/1; EP/I019693/1; EP/L027240/1

OSTI ID:: 1357273

Alternate ID(s):: OSTI ID: 1356429; OSTI ID: 1786067

Journal Information:: ChemCatChem, Journal Name: ChemCatChem Vol. 9 Journal Issue: 9; ISSN 1867-3880

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: Germany

Language:: English

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Cited by: 17 works

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Title: Supercritical Antisolvent Precipitation of Amorphous Copper–Zinc Georgeite and Acetate Precursors for the Preparation of Ambient‐Pressure Water‐Gas‐Shift Copper/Zinc Oxide Catalysts

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