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author:

Yan, Dongxu (Yan, Dongxu.) [1] | Gao, Yanxia (Gao, Yanxia.) [2] | Qi, Ming-Yu (Qi, Ming-Yu.) [3] | Jia, Hongpeng (Jia, Hongpeng.) [4] | Xu, Yi-Jun (Xu, Yi-Jun.) [5] (Scholars:徐艺军)

Abstract:

The dynamic evolution of active site coordination structure during a high-temperature reaction is critically significant but often difficult for the research of efficient single-atom catalysts (SACs). Herein, we for the first time report the in situ activation behaviors of the local coordination structure of Pt single atoms (Pt-1) during the high-temperature oxidation of light alkanes. The distinctly enhanced activity of the catalyst is attributed to the in situ evolved Pt-1-oxygen vacancy (Pt-1-OV) combination ensemble as an efficient and stable active site. Theoretical calculations reveal that the lattice oxygen adjacent to Pt-1 and the H dissociated from CH4 constitute the lattice hydroxyl, which is the initial step in the formation of the Pt-1-OV combination. Pt-1 and nearby unsaturated Mn can donate the charge back to O-O to promote the dissociation of O-2. This work provides molecular-level insight into the in situ reaction-induced evolution of a single-atom coordination environment for designing efficient SACs under harsh conditions.

Keyword:

alkane coordination structure high temperature in situ reaction Pt single atom

Community:

  • [ 1 ] [Yan, Dongxu]Chinese Acad Sci, Inst Urban Environm, Xiamen Key Lab Mat Gaseous Pollutant Control, Xiamen 361021, Peoples R China
  • [ 2 ] [Gao, Yanxia]Chinese Acad Sci, Inst Urban Environm, Xiamen Key Lab Mat Gaseous Pollutant Control, Xiamen 361021, Peoples R China
  • [ 3 ] [Jia, Hongpeng]Chinese Acad Sci, Inst Urban Environm, Xiamen Key Lab Mat Gaseous Pollutant Control, Xiamen 361021, Peoples R China
  • [ 4 ] [Yan, Dongxu]Univ Chinese Acad Sci, Beijing 100049, Peoples R China
  • [ 5 ] [Gao, Yanxia]Univ Chinese Acad Sci, Beijing 100049, Peoples R China
  • [ 6 ] [Jia, Hongpeng]Univ Chinese Acad Sci, Beijing 100049, Peoples R China
  • [ 7 ] [Qi, Ming-Yu]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China
  • [ 8 ] [Xu, Yi-Jun]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China

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Source :

PRECISION CHEMISTRY

Year: 2023

Issue: 5

Volume: 1

Page: 299-308

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count: 6

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 1

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