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

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...

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Autores principales: Smith, Paul J., Kondrat, Simon A., Carter, James H., Chater, Philip A., Bartley, Jonathan K., Taylor, Stuart H., Spencer, Michael S., Hutchings, Graham J.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: John Wiley and Sons Inc. 2017
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5485020/
https://www.ncbi.nlm.nih.gov/pubmed/28706569
http://dx.doi.org/10.1002/cctc.201601603
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author Smith, Paul J.
Kondrat, Simon A.
Carter, James H.
Chater, Philip A.
Bartley, Jonathan K.
Taylor, Stuart H.
Spencer, Michael S.
Hutchings, Graham J.
author_facet Smith, Paul J.
Kondrat, Simon A.
Carter, James H.
Chater, Philip A.
Bartley, Jonathan K.
Taylor, Stuart H.
Spencer, Michael S.
Hutchings, Graham J.
author_sort Smith, Paul J.
collection PubMed
description 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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spelling pubmed-54850202017-07-11 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. ChemCatChem Full Papers 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. John Wiley and Sons Inc. 2017-04-07 2017-05-10 /pmc/articles/PMC5485020/ /pubmed/28706569 http://dx.doi.org/10.1002/cctc.201601603 Text en © 2017 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA. This is an open access article under the terms of the Creative Commons Attribution (http://creativecommons.org/licenses/by/4.0/) License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
spellingShingle Full Papers
Smith, Paul J.
Kondrat, Simon A.
Carter, James H.
Chater, Philip A.
Bartley, Jonathan K.
Taylor, Stuart H.
Spencer, Michael S.
Hutchings, Graham J.
Supercritical Antisolvent Precipitation of Amorphous Copper–Zinc Georgeite and Acetate Precursors for the Preparation of Ambient‐Pressure Water‐Gas‐Shift Copper/Zinc Oxide Catalysts
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
title_full Supercritical Antisolvent Precipitation of Amorphous Copper–Zinc Georgeite and Acetate Precursors for the Preparation of Ambient‐Pressure Water‐Gas‐Shift Copper/Zinc Oxide Catalysts
title_fullStr Supercritical Antisolvent Precipitation of Amorphous Copper–Zinc Georgeite and Acetate Precursors for the Preparation of Ambient‐Pressure Water‐Gas‐Shift Copper/Zinc Oxide Catalysts
title_full_unstemmed Supercritical Antisolvent Precipitation of Amorphous Copper–Zinc Georgeite and Acetate Precursors for the Preparation of Ambient‐Pressure Water‐Gas‐Shift Copper/Zinc Oxide Catalysts
title_short Supercritical Antisolvent Precipitation of Amorphous Copper–Zinc Georgeite and Acetate Precursors for the Preparation of Ambient‐Pressure Water‐Gas‐Shift Copper/Zinc Oxide Catalysts
title_sort supercritical antisolvent precipitation of amorphous copper–zinc georgeite and acetate precursors for the preparation of ambient‐pressure water‐gas‐shift copper/zinc oxide catalysts
topic Full Papers
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5485020/
https://www.ncbi.nlm.nih.gov/pubmed/28706569
http://dx.doi.org/10.1002/cctc.201601603
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