Tailoring the Local Environment of Platinum in Single‐Atom Pt 1 /CeO 2 Catalysts for Robust Low‐Temperature CO Oxidation

Jiang, Dong; Yao, Yonggang; Li, Tangyuan; Wan, Gang; Pereira‐Hernández, Xavier Isidro; Lu, Yubing; Tian, Jinshu; Khivantsev, Konstantin; Engelhard, Mark H.; Sun, Chengjun; García‐Vargas, Carlos E.; Hoffman, Adam S.; Bare, Simon R.; Datye, Abhaya K.; Hu, Liangbing; Wang, Yong

doi:10.1002/ange.202108585

Tailoring the Local Environment of Platinum in Single‐Atom Pt ₁ /CeO ₂ Catalysts for Robust Low‐Temperature CO Oxidation

Journal Article · Tue Sep 07 00:00:00 EDT 2021 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.202108585· OSTI ID:1819967

^[1]; Yao, Yonggang ^[2]; Li, Tangyuan ^[3]; Wan, Gang ^[4]; Pereira‐Hernández, Xavier Isidro ^[1]; Lu, Yubing ^[5]; Tian, Jinshu ^[5]; Khivantsev, Konstantin ^[5]; Engelhard, Mark H. ^[5]; Sun, Chengjun ^[6]; García‐Vargas, Carlos E. ^[1]; Hoffman, Adam S. ^[4]; Bare, Simon R. ^[4]; Datye, Abhaya K. ^[7]; Hu, Liangbing ^[3]; ^[8]

The Gene and Linda Voiland School of Chemical Engineering and Bioengineering Washington State University Pullman WA 99164 USA
Department of Materials Science and Engineering University of Maryland College Park MD 20742 USA, Current address: State Key Laboratory of Materials Processing and Die &, Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan 430074 China
Department of Materials Science and Engineering University of Maryland College Park MD 20742 USA
Stanford Synchrotron Radiation Lightsource SLAC National Accelerator Laboratory Menlo Park CA 94025 USA
Institute for Integrated Catalysis Pacific Northwest National Laboratory Richland WA 99354 USA
X-ray Science Division Advanced Photon Source Argonne National Laboratory Lemont IL 60439 USA
Department of Chemical and Biological Engineering and Center for Micro-Engineered Materials University of New Mexico Albuquerque NM 87131 USA
The Gene and Linda Voiland School of Chemical Engineering and Bioengineering Washington State University Pullman WA 99164 USA, Institute for Integrated Catalysis Pacific Northwest National Laboratory Richland WA 99354 USA

Abstract

A single‐atom Pt ₁ /CeO ₂ catalyst formed by atom trapping (AT, 800 °C in air) shows excellent thermal stability but is inactive for CO oxidation at low temperatures owing to over‐stabilization of Pt ²⁺ in a highly symmetric square‐planar Pt ₁ O ₄ coordination environment. Reductive activation to form Pt nanoparticles (NPs) results in enhanced activity; however, the NPs are easily oxidized, leading to drastic activity loss. Herein we show that tailoring the local environment of isolated Pt ²⁺ by thermal‐shock (TS) synthesis leads to a highly active and thermally stable Pt ₁ /CeO ₂ catalyst. Ultrafast shockwaves (>1200 °C) in an inert atmosphere induced surface reconstruction of CeO ₂ to generate Pt single atoms in an asymmetric Pt ₁ O ₄ configuration. Owing to this unique coordination, Pt ₁ ^δ+ in a partially reduced state dynamically evolves during CO oxidation, resulting in exceptional low‐temperature performance. CO oxidation reactivity on the Pt ₁ /CeO ₂ _TS catalyst was retained under oxidizing conditions.

View Accepted Manuscript (Publisher)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-06CH11357; AC02-76SF00515; FG02-05ER15712

OSTI ID:: 1819967

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 50 Vol. 133; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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