4.8 Article

Ni/Ce0.9Eu0.1O1.95 with enhanced coke resistance for dry reforming of methane

期刊

JOURNAL OF CATALYSIS
卷 407, 期 -, 页码 77-89

出版社

ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2022.01.020

关键词

Dry reforming of methane; Solid solution; Oxygen vacancy; Coke resistance

资金

  1. National Natural Science Founda-tion of China (NSFC) [21978148]

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In this study, Ni/Ce0.9Eu0.1O1.95 catalysts with better activity and enhanced stability were synthesized for dry reforming of methane. The catalysts exhibited stronger lattice oxygen mobility, higher oxygen storage capacity, and a strong metal-support interaction, which contributed to the reduction of carbon deposition and sintering. As a result, the catalyst achieved a balance between the rate of carbon generation and carbon consumption, leading to improved overall catalytic performance.
Methane reforming with carbon dioxide provides an environmentally friendly route for converting methane to synthesis gas while consuming two greenhouse gases. Large-scale implementation of this process has been stalled by the lack of stable catalysts owing to the rapid deactivation caused by carbon deposition and sintering. Ni/Ce0.9Eu0.1O1.95 catalysts with better activity and enhanced stability are synthesized for dry reforming of methane. This reaction is believed to occur via the direct C-H bond dissociation of CH4 to form surface carbon intermediates on metal sites followed by the oxidation of carbon intermediates to CO. Compared with CeO2, Ce0.9Eu0.1O1.95 with stronger lattice oxygen mobility and higher oxygen storage capacity generates more mobile active oxygen species that participate in eliminating the carbon deposition. Moreover, the particle size of Ni species decreases and Ni shifts to higher oxidation state as a result of the strong metal-support interaction over Ce0.9Eu0.1O1.95. The more surface oxygen species are involved in the reaction, the more methane can be converted to CO rather than surface carbon. As a consequence, the balance between the rate of carbon generation (i.e., the direct C-H bond dissociation of CH4) and the rate of carbon consumption (i.e., the oxidation of formed carbon intermediates) can be achieved for dry reforming of methane over Ni/Ce0.9Eu0.1O1.95, leading to less coke accumulation and thereafter an improved overall catalytic performance. (c) 2022 Elsevier Inc. All rights reserved.

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