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Ethanol electro-oxidation on the PdSn-TaN/C catalyst in alkaline media: Making TaN capable of splitting CC bond

Journal 2022 · IF 24.319 · 发表于 2022 年 5 月 10 日
作者: Na Ye,Pengcheng Zhao,Xiaoying Qi,Wenchao Sheng,Zhao Jiang,Tao Fang
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摘要

The C C bond cleavage remains a main challenge for alkaline EOR (ethanol oxidation reaction). In this work, we report an efficient PdSn-TaN/C electrocatalyst to split the C C bonds in ethanol. Structurally, a series of characterization results confirm the presence of the low-coordinated Pd sites on the PdSn-TaN/C interface. The PdSn-TaN/C catalyst exhibits very high activity (almost 26.9 times of commercial Pd/C), good durability and high selectivity to CO 2 (20.5%) towards alkaline EOR. Specifically, in-situ ATR-SEIRAS (Attenuated total reflection-surface enhanced infrared absorption spectroscopy) results indicate that TaN facilitates the cleavage of C C bonds, whereas Sn promotes the further oxidation of ethanol fragments. DFT (density functional theory) calculations indicate the activation barriers of the C H bond cleavage in CH 3 CH 2 OH, CH 3 CHOH, CH 3 CHO, CH 3 CO, CH 2 CO and the C C bond cleavage in CH 3 CO, CH 2 CO, CHCO are reduced evidently and the removal of adsorbed CH 3 CO and CO becomes easier on the PdSn-TaN/C catalyst surface.