Extraordinary p–d Hybridization Interaction in Heterostructural Pd‐PdSe Nanosheets Boosts C?C Bond Cleavage of Ethylene Glycol Electrooxidation

作者：Qin Yuchen; Zhang Wenlong; Wang Fengqi; Li JunJun; Ye Jinyu; Sheng Xia; Li Chenxi; Liang Xiaoyu; Liu Pei; Wang Xiaopeng; Zheng Xin; Ren Yunlai; Xu Cuilian; Zhang Zhicheng

来源：Angewandte Chemie, 2022, 134(16).

DOI：10.1002/ANGE.202200899

• C?C Bond Cleavage
• Ethylene Glycol Oxidation Reaction
• Pd-PdSe Heterostructural Nanosheets
• Tensile Strain
• p–d Hybridization

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 ...

• 单位
  重庆师范大学; 固体表面物理化学国家重点实验室; 河南农业大学; 天津大学; 厦门大学