Surface Lattice-Embedded Pt Single-Atom Catalyst on Ceria-Zirconia with Superior Catalytic Performance for Propane Oxidation

Tan, Wei; Xie, Shaohua; Cai, Yandi; Yu, Haowei; Ye, Kailong; Wang, Meiyu; Diao, Weijian; Ma, Lu; Ehrlich, Steven N.; Gao, Fei; Dong, Lin; Liu, Fudong

doi:10.1021/acs.est.3c03497

Surface Lattice-Embedded Pt Single-Atom Catalyst on Ceria-Zirconia with Superior Catalytic Performance for Propane Oxidation

Journal Article · Fri Aug 11 00:00:00 EDT 2023 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.3c03497· OSTI ID:2432575

^[1]; ^[2]; Cai, Yandi ^[3]; Yu, Haowei ^[3]; Ye, Kailong ^[2]; Wang, Meiyu ^[3]; Diao, Weijian ^[4]; Ma, Lu ^[5]; Ehrlich, Steven N. ^[5]; ^[3]; ^[3]; ^[2]

Univ. of Central Florida, Orlando, FL (United States); Nanjing Univ. (China)
Univ. of Central Florida, Orlando, FL (United States)
Nanjing Univ. (China)
Villanova Univ., PA (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

Tuning the metal–support interaction and coordination environment of single-atom catalysts can help achieve satisfactory catalytic performance for targeted reactions. Herein, via the facile control of calcination temperatures for Pt catalysts on pre-stabilized Ce_0.9Zr_0.1O₂ (CZO) support, Pt single atoms (Pt₁) with different strengths of Pt–CeO₂ interaction and coordination environment were successfully constructed. With the increase in calcination temperature from 350 to 750 °C, a stronger Pt–CeO₂ interaction and higher Pt-O-Ce coordination number were achieved due to the reaction between PtO_x and surface Ce³⁺ species as well as the migration of Pt₁ into the surface lattice of CZO. The Pt/CZO catalyst calcined at 750 °C (Pt/CZO-750) exhibited a surprisingly higher C₃H₈ oxidation activity than that calcined at 550 °C (Pt/CZO-550). Here, through systematic characterizations and reaction mechanism study, it was revealed that the higher concentration of surface Ce³⁺ species/oxygen vacancies and the stronger Pt–CeO₂ interaction on Pt/CZO-750 could better facilitate the activation of oxygen to oxidize C₃H₈ into reactive carbonate/carboxyl species and further promote the transformation of these intermediates into gaseous CO₂. The Pt/CZO-750 catalyst can be a potential candidate for the catalytic removal of hydrocarbons from vehicle exhaust.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: National Natural Science Foundation of China (NSFC); National Science Foundation (NSF); Natural Science Foundation of Jiangsu Province; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012704

OSTI ID:: 2432575

Report Number(s):: BNL--225954-2024-JAAM

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 33 Vol. 57; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
C3H8 oxidation reaction
Calcination temperature
Coordination environment
Pt single atom
Pt-CeO2 interaction

Surface Lattice-Embedded Pt Single-Atom Catalyst on Ceria-Zirconia with Superior Catalytic Performance for Propane Oxidation

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