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author:

Qiao, Luyang (Qiao, Luyang.) [1] | Wang, Xiguang (Wang, Xiguang.) [2] | Zong, Shanshan (Zong, Shanshan.) [3] | Huang, Zhishen (Huang, Zhishen.) [4] | Zhou, Zhangfeng (Zhou, Zhangfeng.) [5] | Fan, Maohong (Fan, Maohong.) [6] | Yao, Yuangen (Yao, Yuangen.) [7]

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EI

Abstract:

The electronic and geometric robustness of active sites in catalysts determines their long-term efficiency in CO2 hydrogenation. One effective strategy to improve durability is rationalizing metal site charge distribution through strong metal-support interactions (SMSIs). We propose an effective approach that can modulate the SMSI between Pd and CeO2 by doping chlorine anions into the CeO2 lattice. The developed Pd@CeOCl/CeO2 catalyst exhibits sustainable activity (3150 mmol·gPd-1·h-1) and CO selectivity (99.7%) for at least 200 h, as well as enhanced resistance toward CO and H2O. Anion-doping-mediated SMSIs result in significant electronic perturbations in the Pdδ+-[Cl-Ce-O]δ− interface, which modulates the surface properties and the energy band of the catalyst. Combined spectroscopic and microscopic evidence unveils that a Clδ−-Cl- pair buffers the electron transfer in Pdδ+↔Pd0 and Ce4+↔Ce3+ cycles, which circumvents the further hydrogenation of CO and shields Pdδ+ sites from sintering in hydrogenation conditions. © 2024 American Chemical Society.

Keyword:

Catalyst selectivity Cerium oxide Hydrogenation Negative ions Palladium compounds Positive ions Semiconductor doping Sintering

Community:

  • [ 1 ] [Qiao, Luyang]Key Laboratory of Coal to Ethylene Glycol and Its Related Technology, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou; 350002, China
  • [ 2 ] [Wang, Xiguang]College of Chemistry, Fuzhou University, Fuzhou; 350108, China
  • [ 3 ] [Zong, Shanshan]Key Laboratory of Coal to Ethylene Glycol and Its Related Technology, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou; 350002, China
  • [ 4 ] [Huang, Zhishen]College of Chemistry and Materials Science, Fujian Normal University, Fuzhou; 350007, China
  • [ 5 ] [Zhou, Zhangfeng]Key Laboratory of Coal to Ethylene Glycol and Its Related Technology, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou; 350002, China
  • [ 6 ] [Fan, Maohong]Departments of Chemical and Petroleum Engineering, University of Wyoming, Laramie; WY; 82071, United States
  • [ 7 ] [Yao, Yuangen]Key Laboratory of Coal to Ethylene Glycol and Its Related Technology, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou; 350002, China

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Source :

ACS Catalysis

Year: 2024

Issue: 17

Volume: 14

Page: 13181-13194

1 1 . 7 0 0

JCR@2023

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SCOPUS Cited Count:

ESI Highly Cited Papers on the List: 0 Unfold All

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Chinese Cited Count:

30 Days PV: 0

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