期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 16, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202200899
关键词
C-C Bond Cleavage; Ethylene Glycol Oxidation Reaction; Pd-PdSe Heterostructural Nanosheets; Tensile Strain; p-d Hybridization
资金
- Natural Science Foundation of Henan Province [2023000410209]
- Key Research and Promotion Project of Henan Province [202102310267]
- Top-notch Personnel Fund of Henan Agricultural University [30500682]
In this study, highly efficient Pd-PdSe heterostructural nanosheets (Pd-PdSe HNSs) were successfully fabricated, showing unique electronic and geometrical structures with unconventional p-d hybridization interactions and tensile strain effect. Compared to commercial catalysts, Pd-PdSe HNSs exhibited significantly enhanced activity and selectivity for the oxidation of ethylene glycol.
Advanced electrocatalysts for complete oxidation of ethylene glycol (EG) in direct EG fuel cells are strongly desired owing to the higher energy efficiency. Herein, Pd-PdSe heterostructural nanosheets (Pd-PdSe HNSs) have been successfully fabricated via a one-step approach. These Pd-PdSe HNSs feature unique electronic and geometrical structures, in which unconventional p-d hybridization interactions and tensile strain effect co-exist. Compared with commercial Pd/C and Pd NSs catalysts, Pd-PdSe HNSs display 5.5 (6.6) and 2.5 (2.6) fold enhancement of specific (mass) activity for the EG oxidation reaction (EGOR). Especially, the optimum C1 pathway selectivity of Pd-PdSe HNSs reaches 44.3 %, illustrating the superior C-C bond cleavage ability. Electrochemical in situ FTIR spectroscopy and theoretical calculations demonstrate that the extraordinary p-d hybridization interaction and tensile strain effect could effectively reduce the activation energy of C-C bond breaking and accelerate CO* oxidation, boosting the complete oxidation of EG and improving the catalytic performance.
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