期刊
JOURNAL OF CATALYSIS
卷 404, 期 -, 页码 400-410出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2021.10.018
关键词
Methane oxidation; Palladium; Active support; Metal-support interaction; Lattice oxygen
资金
- Nanjing Tech University Research Start-up Fund [38274017111]
- Zhongyan Jilantai Chlor-Alkali Chemical Co., Ltd. [FZ2019-RWS-027]
- National Research Foundation, Prime Minister's Office, Singapore
- Ministry of National Development, Singapore
- National Environment Agency, Ministry of the Environment and Water Resource, Singapore under the Closing the Waste Loop R&D Initiative as part of the Urban Solutions and Sustainability Integration Fund [USS-IF-2019-4]
- Singapore Ministry of Education [RG3/18 (S), MOE2018-T2-2-027]
Palladium-based catalysts are effective but expensive and scarce, necessitating the design of improved catalysts; Pd-NiCo2O4 spinel catalysts obtained via thermal decomposition method exhibit unique structure and high activity; Enhanced activity mainly comes from Pd ions substituting into the structure of NiCo2O4.
While palladium-based catalysts are effective in low-temperature methane combustion, their high cost and scarcity render them unsuitable to fulfil the growing demand. The design of improved catalysts which can more efficiently utilize this precious metal is required. Here, by using a facile one-pot thermal decomposition method Pd-NiCo2O4 spinel catalysts with a unique structure are obtained, in which the majority of Pd incorporated into the bulk spinel structure of NiCo2O4 with limited highly dispersed PdOx species on the surface at an atomic scale. The robust 1 %Pd-NiCo2O4 spinel catalyst exhibits comparable activity in methane oxidation to that of the conventional incipient wetness impregnation 2 %Pd/NiCo2O4. Theoretical calculations and catalyst characterizations (SEM, HRTEM, XRD, XPS, XAS, ICP-OES, etc.) revealed that the enhanced activity is mainly originated from having the O p-band center closer to the Fermi level, with Pd ions incorporated into the bulk NiCo2O4 via substituting for the octahedral coordinated Ni3+/Co3+. (C) 2021 Published by Elsevier Inc.
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