Adsorption of CH4 and SO2 on Unsupported Pd1−xMxO(101) Surface
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PdO is known to efficiently catalyze the oxidation of methane but suffers tremendously from sulfur poisoning that lowers its catalytic activity. In this paper, dispersion-corrected density functional theory based first principles calculations were performed to systematically screen the metal impurities M (where M is a transition metal) on a Pd1−xMxO catalyst that promote the desired adsorption energies for CH4 and SO2 to gain insights into the design of sulfation-resistant PdO-based methane oxidation catalysts. Specific Pd1−xMxO(101) catalyst was identified to thermodynamically avoid surface sulfation while maintaining the active sites for methane activation at typical experimental conditions. Results indicate a potential route of tuning the catalytic property of PdO by the introduction of a surface metal impurity.
KeywordsSulfur poisoning Methane oxidation Palladium oxide
This work is supported in part by JST ACCEL Grant Number JPMJAC1501 "Creation of the Functional Materials on the Basis of the Inter-Element-Fusion Strategy and their Innovative Applications", MEXT Grant-in-Aid for Scientific Research (16K04876), and JST CREST Innovative Catalysts and Creation Technologies for the Utilization of Diverse Natural Carbon Resources: In-situ atomic characterization of catalytic reactions for the development of Innovative Catalysts (No. 17942262). Some numerical calculations were done using the computer facilities at the following institutes: High Energy Accelerator Research Organization (KEK), Institute for Solid State Physics (ISSP, University of Tokyo), Yukawa Institute for Theoretical Physics (YITP, Kyoto University), and the National Institute for Fusion Science (NIFS). RLA acknowledges the Balik Scientist Program of the Department of Science and Technology, through the Philippine Council for Industry, Energy and Emerging Technology Research and Development.
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Conflict of interest
All authors declare that they have no conflict of interest.
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