期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 7, 期 30, 页码 17987-17994出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9ta04867g
关键词
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资金
- National Natural Science Foundation of China [21771067]
- Natural Science Foundation of Fujian Province [2017J06005]
- Program for New Century Excellent Talents in Fujian Province University
- Huaqiao University
Sluggish C-C bond cleavage during the ethanol oxidation reaction (EOR) in acidic media results in a lowered energy yield and gravely hinders the commercialization of direct ethanol fuel cells. Here we report an elaborate synthesis of sub-10 nm concavity-tunable Rh@Pt core-shell nanocubes with an engineered Rh-Pt interface and Pt atomic surface steps to facilitate the C-C bond cleavage in the EOR. Using a microsyringe pump, the surface concavity of the Rh@Pt core-shell nanocubes is successfully manipulated through kinetically adjusting the ratio of the atom deposition rate and surface diffusion rate (V-dep./V-diff.) during the overgrowth process. Compared to the samples with shallow surface concavity and a flat surface, the deeper concaved Rh@Pt core-shell nanocubes possess richer surface Pt atomic steps and exhibit a greater enhancement in EOR catalysis, achieving mass activity and specific activity that are 3.74 times and 6.89 times higher than those of the state-of-the-art Pt/C catalysts, respectively. Electrochemical in situ FTIR studies indicate that the Rh-Pt interfacial interaction and the surface Pt atomic steps on the Rh@Pt concave nanocubes can effectively facilitate the C-C bond cleavage towards the complete oxidation of ethanol to CO2.
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