期刊
NANO LETTERS
卷 22, 期 17, 页码 7144-7150出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.2c02290
关键词
Single-atom-kernelled nanocluster; antigalvanic reduction; active site; Pd based trimetal nanocluster; CO2 electroreduction; metal utilization efficiency
类别
资金
- National Natural Science Foundation of China [21905284, 21829501, 21925303, 22075291, 21771186, 21222301, 21171170, 21528303]
- China Postdoctoral Science Foundation [Y94G4E356B]
- Key Program of 13th five-year plan, CASHIPS [KP-2017-16]
- Collaborative Innovation Program of Hefei Science Center, CAS [2020HSC-CIP005]
- Center for Mesoscience, Institute of Process Engineering, Chinese Academy of Sciences, State Key Laboratory of Multiphase Complex Systems [MPCS- 2019-A-09]
This study proposes the concept of single-atom-kernelled nanoclusters and synthesizes a Pd-based trimetal nanocluster with a single-Ag atom-kernel using an alloying strategy. The nanoclusters with single-silver atom kernels exhibit higher activity and selectivity compared to the bimetal precursor nanoclusters. The single atoms in the kernel have significant influence on catalytic performance by affecting the electronic configuration.
To propose the concept of single-atom-kernelled nanocluster, we synthesized a Pd-based trimetal nanocluster with a single-Ag atom-kernel for the first time by introducing some steric hindrance factors and employing a joint alloying strategy that combines the coreduction with an antigalvanic reduction (AGR). Although the AGR-derived Pd-based trimetal nanoclusters with single-silver atom kernels have low contents of gold, they show higher activity and selectivity than those of the bimetal precursor nanocluster in the electrocatalytical reduction of CO2 to CO. Furthermore, it is revealed that the kernel single atoms from both Au4Pd6(TBBT)(12) and Au3AgPd6(TBBT)(12) are not the active sites for catalysis, but greatly influence the catalytical performance by effecting the electronic configuration. Thus, it is demonstrated that the single-atom-kernelled nanocluster can not only improve the precious metal utilization (even to 100%) but also better the properties and provide insight into the structure-property correlation for metal nanoclusters.
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