Fine-tuned local coordination environment of Pt single atoms on ceria controls catalytic reactivity

Constructing single atom catalysts with fine-tuned coordination environments can be a promising strategy to achieve satisfactory catalytic performance. Herein, via a simple calcination temperature-control strategy, CeO 2 supported Pt single atom catalysts with precisely controlled coordination envir...

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Published in:Nature communications 2022-11, Vol.13 (1), p.7070-16, Article 7070
Main Authors: Tan, Wei, Xie, Shaohua, Le, Duy, Diao, Weijian, Wang, Meiyu, Low, Ke-Bin, Austin, Dave, Hong, Sampyo, Gao, Fei, Dong, Lin, Ma, Lu, Ehrlich, Steven N., Rahman, Talat S., Liu, Fudong
Format: Article
Language:English
Subjects:
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Ammonia
Catalysts
Catalytic oxidation
Cerium oxides
Coordination numbers
Desorption
Humanities and Social Sciences
MATERIALS SCIENCE
multidisciplinary
Oxidation
Science
Science (multidisciplinary)
Single atom catalysts
Theoretical analysis
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Summary:Constructing single atom catalysts with fine-tuned coordination environments can be a promising strategy to achieve satisfactory catalytic performance. Herein, via a simple calcination temperature-control strategy, CeO 2 supported Pt single atom catalysts with precisely controlled coordination environments are successfully fabricated. The joint experimental and theoretical analysis reveals that the Pt single atoms on Pt 1 /CeO 2 prepared at 550 °C (Pt/CeO 2 -550) are mainly located at the edge sites of CeO 2 with a Pt–O coordination number of ca . 5, while those prepared at 800 °C (Pt/CeO 2 -800) are predominantly located at distorted Ce substitution sites on CeO 2 terrace with a Pt–O coordination number of ca . 4. Pt/CeO 2 -550 and Pt/CeO 2 -800 with different Pt 1 -CeO 2 coordination environments exhibit a reversal of activity trend in CO oxidation and NH 3 oxidation due to their different privileges in reactants activation and H 2 O desorption, suggesting that the catalytic performance of Pt single atom catalysts in different target reactions can be maximized by optimizing their local coordination structures. CeO 2 -supported Pt single atoms with different coordination environments exhibit distinct behaviors in reactant adsorption/activation and product desorption, thus showing different catalytic performance for various catalytic oxidation reactions.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-022-34797-2