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Title: Structure-activity relationship of Pt catalyst on engineered ceria-alumina support for CO oxidation

Abstract

In heterogeneous catalysis, the promotion of low temperature activity and enhancement of thermal stability simultaneously especially for precious metal catalysts is always highly demanded but very challenging. In this work, we report a novel Pt catalyst on ceria-alumina (CeO2/Al2O3) support (Pt/CA-T) engineered by a two-step ceria deposition strategy, exhibiting superior thermal stability and low-temperature carbon monoxide (CO) oxidation activity after activation. Pt single sites anchored to engineered CeO2 edge sites are much more stable than that to CeO2 (111) surface, and such stable single sites can be transformed into highly active Pt clusters for efficient low-temperature CO oxidation. Active site identification indicates that the CO oxidation activity of different Pt sites follows such sequence: Pt cluster step sites ≈ Pt cluster terrace sites > Pt cluster corner sites $$\gg$$ Pt single sites on CeO2. The excellent low temperature activity of activated Pt/CA-T catalyst for CO oxidation is associated with its abundant Pt cluster step and terrace sites as well as rich Pt-CeO2 interfaces, which facilitate the adsorption of active CO species and superior oxygen activation/transfer ability. The present study provides new insights into the structure–activity relationship of Pt-CeO2-Al2O3 catalyst, which can also guide the preparation of other highly robust supported catalysts for important industrial applications.

Authors:
 [1];  [2];  [3]; ORCiD logo [4]; ORCiD logo [4];  [5];  [5];  [6];  [3];  [3]; ORCiD logo [1];  [7]; ORCiD logo [1]
  1. Univ. of Central Florida, Orlando, FL (United States)
  2. Univ. of Central Florida, Orlando, FL (United States); Nanjing Univ. (China)
  3. Chinese Academy of Sciences (CAS), Xiamen (China)
  4. Univ. of Sydney, NSW (Australia)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  6. Chinese Academy of Sciences (CAS), Beijing (China)
  7. Beijing University of Technology (China)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1836797
Alternate Identifier(s):
OSTI ID: 1862563
Report Number(s):
BNL-222478-2021-JAAM
Journal ID: ISSN 0021-9517
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Catalysis
Additional Journal Information:
Journal Volume: 405; Journal ID: ISSN 0021-9517
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Platinum catalyst; Support engineering; CO oxidation; Thermal stability; Active sites

Citation Formats

Xie, Shaohua, Tan, Wei, Wang, Chunying, Arandiyan, Hamidreza, Garbrecht, Magnus, Ma, Lu, Ehrlich, Steven N., Xu, Peng, Li, Yaobin, Zhang, Yan, Collier, Samantha, Deng, Jiguang, and Liu, Fudong. Structure-activity relationship of Pt catalyst on engineered ceria-alumina support for CO oxidation. United States: N. p., 2021. Web. doi:10.1016/j.jcat.2021.12.002.
Xie, Shaohua, Tan, Wei, Wang, Chunying, Arandiyan, Hamidreza, Garbrecht, Magnus, Ma, Lu, Ehrlich, Steven N., Xu, Peng, Li, Yaobin, Zhang, Yan, Collier, Samantha, Deng, Jiguang, & Liu, Fudong. Structure-activity relationship of Pt catalyst on engineered ceria-alumina support for CO oxidation. United States. https://doi.org/10.1016/j.jcat.2021.12.002
Xie, Shaohua, Tan, Wei, Wang, Chunying, Arandiyan, Hamidreza, Garbrecht, Magnus, Ma, Lu, Ehrlich, Steven N., Xu, Peng, Li, Yaobin, Zhang, Yan, Collier, Samantha, Deng, Jiguang, and Liu, Fudong. Thu . "Structure-activity relationship of Pt catalyst on engineered ceria-alumina support for CO oxidation". United States. https://doi.org/10.1016/j.jcat.2021.12.002. https://www.osti.gov/servlets/purl/1836797.
@article{osti_1836797,
title = {Structure-activity relationship of Pt catalyst on engineered ceria-alumina support for CO oxidation},
author = {Xie, Shaohua and Tan, Wei and Wang, Chunying and Arandiyan, Hamidreza and Garbrecht, Magnus and Ma, Lu and Ehrlich, Steven N. and Xu, Peng and Li, Yaobin and Zhang, Yan and Collier, Samantha and Deng, Jiguang and Liu, Fudong},
abstractNote = {In heterogeneous catalysis, the promotion of low temperature activity and enhancement of thermal stability simultaneously especially for precious metal catalysts is always highly demanded but very challenging. In this work, we report a novel Pt catalyst on ceria-alumina (CeO2/Al2O3) support (Pt/CA-T) engineered by a two-step ceria deposition strategy, exhibiting superior thermal stability and low-temperature carbon monoxide (CO) oxidation activity after activation. Pt single sites anchored to engineered CeO2 edge sites are much more stable than that to CeO2 (111) surface, and such stable single sites can be transformed into highly active Pt clusters for efficient low-temperature CO oxidation. Active site identification indicates that the CO oxidation activity of different Pt sites follows such sequence: Pt cluster step sites ≈ Pt cluster terrace sites > Pt cluster corner sites $\gg$ Pt single sites on CeO2. The excellent low temperature activity of activated Pt/CA-T catalyst for CO oxidation is associated with its abundant Pt cluster step and terrace sites as well as rich Pt-CeO2 interfaces, which facilitate the adsorption of active CO species and superior oxygen activation/transfer ability. The present study provides new insights into the structure–activity relationship of Pt-CeO2-Al2O3 catalyst, which can also guide the preparation of other highly robust supported catalysts for important industrial applications.},
doi = {10.1016/j.jcat.2021.12.002},
journal = {Journal of Catalysis},
number = ,
volume = 405,
place = {United States},
year = {Thu Dec 09 00:00:00 EST 2021},
month = {Thu Dec 09 00:00:00 EST 2021}
}

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