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Title: A combined experimental and computational study of water-gas shift reaction over rod-shaped Ce 0.75 M 0.25O 2 (M=Ti, Zr, and Mn) supported Cu catalysts

Abstract

Water-gas shift (WGS) reaction over a series of ceria-based mixed oxides supported Cu catalysts was investigated using a combined experimental and theoretical method. The mixed rod-shaped Ce 0.75M 0.25O 2 (M = Ti 4+, Zr 4+, Mn 4+) solid solutions, which majorly expose the (110) and (100) facets, are synthesized by hydrothermal method and used to prepare supported Cu catalysts. We found that the Cu/Ce0.75Ti 0.25O 2 (Cu-CT) exhibits the highest CO conversion in the temperature range of 150-250 °C among all supported Cu catalysts. This is mainly attributed to (i) good dispersion of Cu; (ii) largest amount of moderate copper oxide; and (iii) strongest Cu-support interaction of Cu-CT. And compared to other mixed metals, periodic density functional theory calculations performed, this work further suggest that the introduction of Ti into CeO 2 not only promotes oxygen vacancy formation and CO adsorption, but also facilitates the carboxyl (COOH) formation at the interface of the Cu cluster and the support, which leads to the enhanced catalytic activity of the Cu-CT toward WGS reaction.

Authors:
; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1414536
Report Number(s):
PNNL-SA-129864
Journal ID: ISSN 0360-3199; 49734; KC0302010
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: International Journal of Hydrogen Energy; Journal Volume: 42; Journal Issue: 51
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; mixed ceria nanorods; Cu catalysts; water-gas shift reaction; Cu-support interaction; DFT calculation; Environmental Molecular Sciences Laboratory

Citation Formats

Ren, Zhibo, Peng, Fei, Chen, Biaohua, Mei, Donghai, and Li, Jianwei. A combined experimental and computational study of water-gas shift reaction over rod-shaped Ce0.75 M0.25O2 (M=Ti, Zr, and Mn) supported Cu catalysts. United States: N. p., 2017. Web. doi:10.1016/j.ijhydene.2017.10.047.
Ren, Zhibo, Peng, Fei, Chen, Biaohua, Mei, Donghai, & Li, Jianwei. A combined experimental and computational study of water-gas shift reaction over rod-shaped Ce0.75 M0.25O2 (M=Ti, Zr, and Mn) supported Cu catalysts. United States. doi:10.1016/j.ijhydene.2017.10.047.
Ren, Zhibo, Peng, Fei, Chen, Biaohua, Mei, Donghai, and Li, Jianwei. Thu . "A combined experimental and computational study of water-gas shift reaction over rod-shaped Ce0.75 M0.25O2 (M=Ti, Zr, and Mn) supported Cu catalysts". United States. doi:10.1016/j.ijhydene.2017.10.047.
@article{osti_1414536,
title = {A combined experimental and computational study of water-gas shift reaction over rod-shaped Ce0.75 M0.25O2 (M=Ti, Zr, and Mn) supported Cu catalysts},
author = {Ren, Zhibo and Peng, Fei and Chen, Biaohua and Mei, Donghai and Li, Jianwei},
abstractNote = {Water-gas shift (WGS) reaction over a series of ceria-based mixed oxides supported Cu catalysts was investigated using a combined experimental and theoretical method. The mixed rod-shaped Ce0.75M0.25O2 (M = Ti4+, Zr4+, Mn4+) solid solutions, which majorly expose the (110) and (100) facets, are synthesized by hydrothermal method and used to prepare supported Cu catalysts. We found that the Cu/Ce0.75Ti0.25O2 (Cu-CT) exhibits the highest CO conversion in the temperature range of 150-250 °C among all supported Cu catalysts. This is mainly attributed to (i) good dispersion of Cu; (ii) largest amount of moderate copper oxide; and (iii) strongest Cu-support interaction of Cu-CT. And compared to other mixed metals, periodic density functional theory calculations performed, this work further suggest that the introduction of Ti into CeO2 not only promotes oxygen vacancy formation and CO adsorption, but also facilitates the carboxyl (COOH) formation at the interface of the Cu cluster and the support, which leads to the enhanced catalytic activity of the Cu-CT toward WGS reaction.},
doi = {10.1016/j.ijhydene.2017.10.047},
journal = {International Journal of Hydrogen Energy},
number = 51,
volume = 42,
place = {United States},
year = {Thu Nov 02 00:00:00 EDT 2017},
month = {Thu Nov 02 00:00:00 EDT 2017}
}