期刊
ACS CATALYSIS
卷 12, 期 15, 页码 9092-9100出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c02274
关键词
core-shell nanostructures; compressive lattice strain; electronic interaction; d-band center; ethanol oxidation reaction; oxygen reduction reaction
资金
- National Natural Science Foundation of China [22075290, 21972068]
- Beijing Natural Science Foundation [Z200012]
- State Key Laboratory of Multiphase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences [MPCS-2021-A-05]
- Nanjing IPE Institute of Green Manufacturing Industry [E0010725]
Geometric structure and chemical composition are critical factors determining the electronic properties of metal catalysts. The wet-chemistry method used in this study successfully constructed core-shell nanoentities with enhanced catalytic activity through lattice strain and electronic interaction. The optimized core-shell nanoparticles exhibited excellent catalytic performance in an alkaline medium.
Geometric structure and chemical composition are two critical factors that determine the electronic properties of an active metal favorable for a given catalytic reaction. In this scenario, we develop a wet-chemistry method to construct core-shell nanoentities consisting of a CuPd alloy core and a NiPd alloy shell, termed as CuPd@NiPd, which involves the synthesis of CuNi alloy seeds, and a subsequent galvanic replacement reaction with Pd2+ precursors in an organic medium at elevated temperature. In these unique core-shell nanostructures, the compressive lattice strain between core and shell regions and the electronic interaction between Pd and transitional elements could be coupled together to lead to a downshift of the d-band center of Pd sites, thus endowing them with good activity for catalyzing ethanol oxidation reaction (EOR) and oxygen reduction reaction (ORR). In particular, at an appropriate Pd/Cu precursor ratio of 1/1, the as-prepared core-shell CuPd@NiPd nanoparticles exhibit a mass activity of 5.1 A mg(-1) for EOR and a half-wave potential of 0.91 V for ORR at room temperature in an alkaline medium, outperforming alloy CuPd, NiPd counterparts, commercial Pd/C, and the vast majority of recently reported Pd-based electrocatalysts.
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