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author:

Huang, Xing (Huang, Xing.) [1] (Scholars:黄兴) | Jones, Travis (Jones, Travis.) [2] | Fedorov, Alexey (Fedorov, Alexey.) [3] | Farra, Ramzi (Farra, Ramzi.) [4] | Coperet, Christophe (Coperet, Christophe.) [5] | Schloegl, Robert (Schloegl, Robert.) [6] | Willinger, Marc-Georg (Willinger, Marc-Georg.) [7]

Indexed by:

EI SCIE

Abstract:

Metal catalysts play an important role in industrial redox reactions. Although extensively studied, the state of these catalysts under operating conditions is largely unknown, and assignments of active sites remain speculative. Herein, an operando transmission electron microscopy study is presented, which interrelates the structural dynamics of redox metal catalysts to their activity. Using hydrogen oxidation on copper as an elementary redox reaction, it is revealed how the interaction between metal and the surrounding gas phase induces complex structural transformations and drives the system from a thermodynamic equilibrium toward a state controlled by the chemical dynamics. Direct imaging combined with the simultaneous detection of catalytic activity provides unparalleled structure-activity insights that identify distinct mechanisms for water formation and reveal the means by which the system self-adjusts to changes of the gas-phase chemical potential. Density functional theory calculations show that surface phase transitions are driven by chemical dynamics even when the system is far from a thermodynamic phase boundary. In a bottom-up approach, the dynamic behavior observed here for an elementary reaction is finally extended to more relevant redox reactions and other metal catalysts, which underlines the importance of chemical dynamics for the formation and constant re-generation of transient active sites during catalysis.

Keyword:

chemical dynamics metal catalysts oscillatory redox dynamics phase coexistence phase transitions structure-activity correlation

Community:

  • [ 1 ] [Huang, Xing]Swiss Fed Inst Technol, Sci Ctr Opt & Electron Microscopy, Otto Stern Weg 3, CH-8093 Zurich, Switzerland
  • [ 2 ] [Willinger, Marc-Georg]Swiss Fed Inst Technol, Sci Ctr Opt & Electron Microscopy, Otto Stern Weg 3, CH-8093 Zurich, Switzerland
  • [ 3 ] [Huang, Xing]Fuzhou Univ, Coll Chem, Fuzhou 350116, Peoples R China
  • [ 4 ] [Huang, Xing]Swiss Fed Inst Technol, Dept Chem & Appl Biosci, Vladimir Prelog Weg 1-5, CH-8093 Zurich, Switzerland
  • [ 5 ] [Coperet, Christophe]Swiss Fed Inst Technol, Dept Chem & Appl Biosci, Vladimir Prelog Weg 1-5, CH-8093 Zurich, Switzerland
  • [ 6 ] [Huang, Xing]Max Planck Gesell, Fritz Haber Inst, Faradayweg 4-6, D-14195 Berlin, Germany
  • [ 7 ] [Jones, Travis]Max Planck Gesell, Fritz Haber Inst, Faradayweg 4-6, D-14195 Berlin, Germany
  • [ 8 ] [Farra, Ramzi]Max Planck Gesell, Fritz Haber Inst, Faradayweg 4-6, D-14195 Berlin, Germany
  • [ 9 ] [Schloegl, Robert]Max Planck Gesell, Fritz Haber Inst, Faradayweg 4-6, D-14195 Berlin, Germany
  • [ 10 ] [Willinger, Marc-Georg]Max Planck Gesell, Fritz Haber Inst, Faradayweg 4-6, D-14195 Berlin, Germany
  • [ 11 ] [Fedorov, Alexey]Swiss Fed Inst Technol, Dept Mech & Proc Engn, Leonhardstr 21, CH-8092 Zurich, Switzerland
  • [ 12 ] [Schloegl, Robert]Max Planck Inst Chem Energy Convers, Dept Heterogeneous React, D-45470 Mulheim, Germany

Reprint 's Address:

  • 黄兴

    [Huang, Xing]Swiss Fed Inst Technol, Sci Ctr Opt & Electron Microscopy, Otto Stern Weg 3, CH-8093 Zurich, Switzerland;;[Willinger, Marc-Georg]Swiss Fed Inst Technol, Sci Ctr Opt & Electron Microscopy, Otto Stern Weg 3, CH-8093 Zurich, Switzerland;;[Huang, Xing]Fuzhou Univ, Coll Chem, Fuzhou 350116, Peoples R China;;[Huang, Xing]Swiss Fed Inst Technol, Dept Chem & Appl Biosci, Vladimir Prelog Weg 1-5, CH-8093 Zurich, Switzerland;;[Huang, Xing]Max Planck Gesell, Fritz Haber Inst, Faradayweg 4-6, D-14195 Berlin, Germany;;[Willinger, Marc-Georg]Max Planck Gesell, Fritz Haber Inst, Faradayweg 4-6, D-14195 Berlin, Germany

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Source :

ADVANCED MATERIALS

ISSN: 0935-9648

Year: 2021

Issue: 31

Volume: 33

3 2 . 0 8 6

JCR@2021

2 7 . 4 0 0

JCR@2023

ESI Discipline: MATERIALS SCIENCE;

ESI HC Threshold:142

JCR Journal Grade:1

CAS Journal Grade:1

Cited Count:

WoS CC Cited Count: 41

SCOPUS Cited Count: 37

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 0

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