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

Yuanyuan Li(Stony Brook University), Matthew Kottwitz(University of Illinois Urbana-Champaign), Joshua Vincent(Arizona State University), Michael J. Enright(University of Illinois Urbana-Champaign), Zongyuan Liu(Brookhaven National Laboratory), Lihua Zhang(Brookhaven National Laboratory), Jiahao Huang(Stony Brook University), Sanjaya D. Senanayake(Brookhaven National Laboratory), Wei‐Chang Yang(National Institute of Standards and Technology), Peter A. Crozier(Arizona State University), Ralph G. Nuzzo(University of Illinois Urbana-Champaign), Anatoly I. Frenkel(Brookhaven National Laboratory)
Nature Communications
February 10, 2021
Cited by 226Open Access
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Abstract

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/CeO 2 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 Pt 0 − O vacancy−Ce 3+ 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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