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author:

Chen, Yang (Chen, Yang.) [1] | Wan, Qiang (Wan, Qiang.) [2] | Cao, Liru (Cao, Liru.) [3] | Gao, Zhe (Gao, Zhe.) [4] | Lin, Jian (Lin, Jian.) [5] | Li, Lin (Li, Lin.) [6] | Pan, Xiaoli (Pan, Xiaoli.) [7] | Lin, Sen (Lin, Sen.) [8] | Wang, Xiaodong (Wang, Xiaodong.) [9] | Zhang, Tao (Zhang, Tao.) [10]

Indexed by:

EI

Abstract:

Tuning the electronic state and local structure of single-atom dispersed metals is important to improve the performance of single-atom catalysts. Here, we find that the electronic structure of Pt single atoms (Pt1) depends on the facets of CeO2. Various characterizations and density functional theory calculations demonstrate that Pt1 anchored on the (1 1 0) facet of CeO2 nanorods exhibits a positively charged state, while it approaches the metallic state on the (1 0 0) facet of CeO2 nanocubes. The different Pt1 states on these facets are attributed to the Pt-O-Ce microstructures with different electron transfer patterns. The positively charged Pt1 shows much weaker adsorption of CO which is favorable for its complete oxidation at lower temperatures. In contrast, the metallic Pt1 can facilitate the activation of H2 in the form of dissociation. The activated H species on metallic Pt1 then promote the preferential oxidation of CO to a greater extent and significantly reduce the reaction barrier. This study provides important implications for tailoring the electronic structure of single-atom centers for heterogeneous catalysis by bonding to specific facet supports. © 2022 Elsevier Inc.

Keyword:

Atoms Catalysis Catalysts Cerium oxide Chemical bonds Density functional theory Electronic states Electronic structure Nanorods Oxidation Platinum Platinum compounds

Community:

  • [ 1 ] [Chen, Yang]Institute of Clean Energy Chemistry, College of Chemistry, Liaoning University, Shenyang; 110036, China
  • [ 2 ] [Chen, Yang]CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian; 116023, China
  • [ 3 ] [Wan, Qiang]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350002, China
  • [ 4 ] [Cao, Liru]CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian; 116023, China
  • [ 5 ] [Gao, Zhe]State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan; 030001, China
  • [ 6 ] [Lin, Jian]CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian; 116023, China
  • [ 7 ] [Li, Lin]CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian; 116023, China
  • [ 8 ] [Pan, Xiaoli]CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian; 116023, China
  • [ 9 ] [Lin, Sen]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350002, China
  • [ 10 ] [Wang, Xiaodong]CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian; 116023, China
  • [ 11 ] [Zhang, Tao]CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian; 116023, China

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Source :

Journal of Catalysis

ISSN: 0021-9517

Year: 2022

Volume: 415

Page: 174-185

7 . 3

JCR@2022

6 . 5 0 0

JCR@2023

ESI HC Threshold:74

JCR Journal Grade:1

CAS Journal Grade:2

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count: 19

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 3

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