Tailoring the Local Environment of Platinum in Single-Atom Pt1/CeO2 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/anie.202108585

Tailoring the Local Environment of Platinum in Single-Atom Pt₁/CeO₂ Catalysts for Robust Low-Temperature CO Oxidation

Journal Article · Tue Aug 03 00:00:00 EDT 2021 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202108585· OSTI ID:1833382

^[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]

Washington State Univ., Pullman, WA (United States)
Univ. of Maryland, College Park, MD (United States); Huazhong Univ. of Science and Technology, Wuhan (China)
Univ. of Maryland, College Park, MD (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Univ. of New Mexico, Albuquerque, NM (United States)
Washington State Univ., Pullman, WA (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

A single-atom Pt₁/CeO₂ catalyst formed by atom trapping (AT, 800 degrees C in air) shows excellent thermal stability but is inactive for CO oxidation at low temperatures owing to over-stabilization of Pt²⁺ in a highly symmetric square-planar Pt₁O₄ coordination environment. Reductive activation to form Pt nanoparticles (NPs) results in enhanced activity; however, the NPs are easily oxidized, leading to drastic activity loss. In this work, we show that tailoring the local environment of isolated Pt²⁺ by thermal-shock (TS) synthesis leads to a highly active and thermally stable Pt₁/CeO₂ catalyst. Ultrafast shockwaves (>1200 degrees C) in an inert atmosphere induced surface reconstruction of CeO₂ to generate Pt single atoms in an asymmetric Pt₁O₄ configuration. Owing to this unique coordination, Pt₁^δ+ in a partially reduced state dynamically evolves during CO oxidation, resulting in exceptional low-temperature performance. CO oxidation reactivity on the Pt₁/CeO₂_TS catalyst was retained under oxidizing conditions.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC02-06CH11357; AC02-76SF00515; AC05-76RL01830; FG02-05ER15712

OSTI ID:: 1833382

Alternate ID(s):: OSTI ID: 1819402
OSTI ID: 1840960
OSTI ID: 1843415
OSTI ID: 1863235

Report Number(s):: PNNL-SA--164380; 171405

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 50 Vol. 60; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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