Smith_et_al-1621-ChemCatChem.pdf (8.58 MB)
Download fileSupercritical antisolvent precipitation of amorphous copper–zinc georgeite and acetate precursors for the preparation of ambient-pressure water-gas-shift copper/zinc oxide catalysts
journal contribution
posted on 2018-03-08, 13:48 authored by Paul J. Smith, Simon KondratSimon Kondrat, James H. Carter, Philip A. Chater, Jonathan K. Bartley, Stuart H. Taylor, Michael S. Spencer, Graham J. Hutchings© 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim 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.
Funding
This research was supported by the UK Catalysis Hub, the EPSRC and ERC (grants EP/K014714/1, EP/K014714/1, EP/K014668/1, EP/K014706/ 1, EP/H000925/1, EP/I019693/1, EPSRC Grant EP/L027240/1 and “After the Goldrush” ERC-2011-AdG-291319) .
History
School
- Science
Department
- Chemistry
Published in
ChemCatChemVolume
9Issue
9Pages
1621 - 1631Citation
SMITH, P.J. ...et al., 2017. Supercritical antisolvent precipitation of amorphous copper–zinc georgeite and acetate precursors for the preparation of ambient-pressure water-gas-shift copper/zinc oxide catalysts. ChemCatChem, 9(9), pp. 1621-1631.Publisher
© The Authors. Published by WileyVersion
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Publisher statement
This work is made available according to the conditions of the Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International (CC BY-NC-ND 4.0) licence. Full details of this licence are available at: https://creativecommons.org/licenses/by-nc-nd/4.0/Publication date
2017-02-15Copyright date
2017Notes
This is an Open Access Article. It is published by Wiley under the Creative Commons Attribution 4.0 Unported Licence (CC BY). Full details of this licence are available at: http://creativecommons.org/licenses/by/4.0/ISSN
1867-3880eISSN
1867-3899Publisher version
Language
- en