Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 51, Pages 61047-61054Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c17205
Keywords
atomic interface; single-atom catalysts; benzene oxidation; catalytic performance; theoretical simulations
Funding
- National Natural Science Foundation of China [21971002]
- Natural Science Foundation of Anhui province [1908085QB45, 2008085QB81]
- Education Department of Anhui Province Foundation [KJ2019A0503]
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The study demonstrates the effectiveness of the atomic interface strategy in improving catalytic performance through the design of Cu-1/B-N with a Cu-N2B1 atomic interface. The enhanced catalytic activity is attributed to the optimized adsorption of intermediates resulting from the manipulation of the electronic structure of Cu single atoms in the Cu-N2B1 atomic interface. This approach provides an innovative method for the rational design of high-performance heterogeneous catalytic materials at the atomic level.
Development of high-performance heterogeneous catalytic materials is important for the rapid upgrade of chemicals, which remains a challenge. Here, the benzene oxidation reaction was used to demonstrate the effectiveness of the atomic interface strategy to improve catalytic performance. The developed B,N-cocoordinated Cu single atoms anchored on carbon nanosheets (Cu-1/B-N) with the Cu-N2B1 atomic interface was prepared by the pyrolysis of a precoordinated Cu precursor. Benefiting from the unique atomic Cu-N2B1 interfacial structure, the designed Cu-1/B-N exhibited considerable activity in the oxidation of benzene, which was much higher than Cu-1/N-C, Cu NPs/N-C, and N-C catalysts. A theoretical study showed that the enhanced catalytic performance resulted from the optimized adsorption of intermediates, which originated from the manipulation of the electronic structure of Cu single atoms induced by B atom coordination in the Cu-N2B1 atomic interface. This study provides an innovative approach for the rational design of high-performance heterogeneous catalytic materials at the atomic level.
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