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

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

doi:10.1038/s41467-021-21132-4

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

Journal Article · Wed Feb 10 00:00:00 EST 2021 · Nature Communications

DOI:https://doi.org/10.1038/s41467-021-21132-4· OSTI ID:1766166

^[1]; Kottwitz, Matthew ^[2]; Vincent, Joshua L. ^[3]; Enright, Michael J. ^[2]; Liu, Zongyuan ^[4]; Zhang, Lihua ^[5];

^[1]; Senanayake, Sanjaya D. ^[4];

^[6]; Crozier, Peter A. ^[3]; Nuzzo, Ralph G. ^[7];

^[8]

Stony Brook Univ., NY (United States)
Univ. of Illinois at Urbana, IL (United States)
Arizona State Univ., Tempe, AZ (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States); Univ. of Maryland, College Park, MD (United States)
Univ. of Illinois at Urbana, IL (United States); KTH Royal Inst. of Technology, Stockholm (Sweden)
Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)

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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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF); National Institute of Standards and Technology (NIST)

Grant/Contract Number:: FG02-03ER15476; SC0012704; AC02-06CH11357; CBET-1604971; 70NANB14H209

OSTI ID:: 1766166

Alternate ID(s):: OSTI ID: 1772732

Report Number(s):: BNL-221190-2021-JAAM; APS_261220

Journal Information:: Nature Communications, Vol. 12, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: ENGLISH

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