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

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

186 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
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
Externally published	Yes

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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.\}",

note = "Publisher Copyright: {\textcopyright} 2021, The Author(s).",

year = "2021",

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

language = "English",

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issn = "2041-1723",

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TY - JOUR

T1 - Dynamic structure of active sites in ceria-supported Pt catalysts for the water gas shift reaction

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.

UR - https://www.scopus.com/pages/publications/85101018044

U2 - 10.1038/s41467-021-21132-4

DO - 10.1038/s41467-021-21132-4

M3 - Article

C2 - 33568629

AN - SCOPUS:85101018044

SN - 2041-1723

VL - 12

JO - Nature Communications

JF - Nature Communications

IS - 1

M1 - 914

ER -

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

Abstract

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