Dynamic structure of active sites in ceria-supported Pt catalysts for the water gas shift reaction

Yuanyuan Li; Matthew Kottwitz; Joshua L. Vincent; Michael J. Enright; Zongyuan Liu; Lihua Zhang; Jiahao Huang; Sanjaya D. Senanayake; Wei Chang D. Yang; Peter A. Crozier; Ralph G. Nuzzo; Anatoly I. Frenkel

doi:10.1038/s41467-021-21132-4

Dynamic structure of active sites in ceria-supported Pt catalysts for the water gas shift reaction

Yuanyuan Li, Matthew Kottwitz, Joshua L. Vincent, Michael J. Enright, Zongyuan Liu, Lihua Zhang, Jiahao Huang, Sanjaya D. Senanayake, Wei Chang D. Yang, Peter A. Crozier, Ralph G. Nuzzo, Anatoly I. Frenkel

Engineering, Ira A. Fulton Schools of (IAFSE)

Research output: Contribution to journal › Article › peer-review

107 Scopus citations

Abstract

Oxide-supported noble metal catalysts have been extensively studied for decades for the water gas shift (WGS) reaction, a catalytic transformation central to a host of large volume processes that variously utilize or produce hydrogen. There remains considerable uncertainty as to how the specific features of the active metal-support interfacial bonding—perhaps most importantly the temporal dynamic changes occurring therein—serve to enable high activity and selectivity. Here we report the dynamic characteristics of a Pt/CeO₂ system at the atomic level for the WGS reaction and specifically reveal the synergistic effects of metal-support bonding at the perimeter region. We find that the perimeter Pt⁰ − O vacancy−Ce³⁺ sites are formed in the active structure, transformed at working temperatures and their appearance regulates the adsorbate behaviors. We find that the dynamic nature of this site is a key mechanistic step for the WGS reaction.

Original language	English (US)
Article number	914
Journal	Nature communications
Volume	12
Issue number	1
DOIs	https://doi.org/10.1038/s41467-021-21132-4
State	Published - Dec 1 2021

ASJC Scopus subject areas

General Chemistry
General Biochemistry, Genetics and Molecular Biology
General Physics and Astronomy

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title = "Dynamic structure of active sites in ceria-supported Pt catalysts for the water gas shift reaction",

abstract = "Oxide-supported noble metal catalysts have been extensively studied for decades for the water gas shift (WGS) reaction, a catalytic transformation central to a host of large volume processes that variously utilize or produce hydrogen. There remains considerable uncertainty as to how the specific features of the active metal-support interfacial bonding—perhaps most importantly the temporal dynamic changes occurring therein—serve to enable high activity and selectivity. Here we report the dynamic characteristics of a Pt/CeO2 system at the atomic level for the WGS reaction and specifically reveal the synergistic effects of metal-support bonding at the perimeter region. We find that the perimeter Pt0 − O vacancy−Ce3+ sites are formed in the active structure, transformed at working temperatures and their appearance regulates the adsorbate behaviors. We find that the dynamic nature of this site is a key mechanistic step for the WGS reaction.",

author = "Yuanyuan Li and Matthew Kottwitz and Vincent, {Joshua L.} and Enright, {Michael J.} and Zongyuan Liu and Lihua Zhang and Jiahao Huang and Senanayake, {Sanjaya D.} and Yang, {Wei Chang D.} and Crozier, {Peter A.} and Nuzzo, {Ralph G.} and Frenkel, {Anatoly I.}",

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doi = "10.1038/s41467-021-21132-4",

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AU - Li, Yuanyuan

AU - Kottwitz, Matthew

AU - Vincent, Joshua L.

AU - Enright, Michael J.

AU - Liu, Zongyuan

AU - Zhang, Lihua

AU - Huang, Jiahao

AU - Senanayake, Sanjaya D.

AU - Yang, Wei Chang D.

AU - Crozier, Peter A.

AU - Nuzzo, Ralph G.

AU - Frenkel, Anatoly I.

PY - 2021/12/1

Y1 - 2021/12/1

N2 - Oxide-supported noble metal catalysts have been extensively studied for decades for the water gas shift (WGS) reaction, a catalytic transformation central to a host of large volume processes that variously utilize or produce hydrogen. There remains considerable uncertainty as to how the specific features of the active metal-support interfacial bonding—perhaps most importantly the temporal dynamic changes occurring therein—serve to enable high activity and selectivity. Here we report the dynamic characteristics of a Pt/CeO2 system at the atomic level for the WGS reaction and specifically reveal the synergistic effects of metal-support bonding at the perimeter region. We find that the perimeter Pt0 − O vacancy−Ce3+ sites are formed in the active structure, transformed at working temperatures and their appearance regulates the adsorbate behaviors. We find that the dynamic nature of this site is a key mechanistic step for the WGS reaction.

AB - Oxide-supported noble metal catalysts have been extensively studied for decades for the water gas shift (WGS) reaction, a catalytic transformation central to a host of large volume processes that variously utilize or produce hydrogen. There remains considerable uncertainty as to how the specific features of the active metal-support interfacial bonding—perhaps most importantly the temporal dynamic changes occurring therein—serve to enable high activity and selectivity. Here we report the dynamic characteristics of a Pt/CeO2 system at the atomic level for the WGS reaction and specifically reveal the synergistic effects of metal-support bonding at the perimeter region. We find that the perimeter Pt0 − O vacancy−Ce3+ sites are formed in the active structure, transformed at working temperatures and their appearance regulates the adsorbate behaviors. We find that the dynamic nature of this site is a key mechanistic step for the WGS reaction.

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JO - Nature communications

JF - Nature communications

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Dynamic structure of active sites in ceria-supported Pt catalysts for the water gas shift reaction

Abstract

ASJC Scopus subject areas

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