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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]

Indexed by:

EI Scopus SCIE

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 mmolg(Pd)(-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 Pd delta+-[Cl-Ce-O](delta-) interface, which modulates the surface properties and the energy band of the catalyst. Combined spectroscopic and microscopic evidence unveils that a Cl delta--Cl- pair buffers the electron transfer in Pd delta+<-> Pd-0 and Ce4+<-> Ce3+ cycles, which circumvents the further hydrogenation of CO and shields Pd delta+ sites from sintering in hydrogenation conditions.

Keyword:

anion doping CeO2 CO2 hydrogenation electronic perturbation Pd catalyst

Community:

  • [ 1 ] [Qiao, Luyang]Chinese Acad Sci, Fujian Inst Res Struct Matter, Key Lab Coal Ethylene Glycol & Its Related Techno, Fuzhou 350002, Peoples R China
  • [ 2 ] [Zong, Shanshan]Chinese Acad Sci, Fujian Inst Res Struct Matter, Key Lab Coal Ethylene Glycol & Its Related Techno, Fuzhou 350002, Peoples R China
  • [ 3 ] [Zhou, Zhangfeng]Chinese Acad Sci, Fujian Inst Res Struct Matter, Key Lab Coal Ethylene Glycol & Its Related Techno, Fuzhou 350002, Peoples R China
  • [ 4 ] [Yao, Yuangen]Chinese Acad Sci, Fujian Inst Res Struct Matter, Key Lab Coal Ethylene Glycol & Its Related Techno, Fuzhou 350002, Peoples R China
  • [ 5 ] [Wang, Xiguang]Fuzhou Univ, Coll Chem, Fuzhou 350108, Peoples R China
  • [ 6 ] [Huang, Zhishen]Fujian Normal Univ, Coll Chem & Mat Sci, Fuzhou 350007, Peoples R China
  • [ 7 ] [Fan, Maohong]Univ Wyoming, Dept Chem, Laramie, WY 82071 USA
  • [ 8 ] [Fan, Maohong]Univ Wyoming, Dept Petr Engn, Laramie, WY 82071 USA

Reprint 's Address:

  • [Zhou, Zhangfeng]Chinese Acad Sci, Fujian Inst Res Struct Matter, Key Lab Coal Ethylene Glycol & Its Related Techno, Fuzhou 350002, Peoples R China;;[Yao, Yuangen]Chinese Acad Sci, Fujian Inst Res Struct Matter, Key Lab Coal Ethylene Glycol & Its Related Techno, Fuzhou 350002, Peoples R China;;

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Source :

ACS CATALYSIS

ISSN: 2155-5435

Year: 2024

Issue: 17

Volume: 14

Page: 13181-13194

1 1 . 7 0 0

JCR@2023

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count:

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 2

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