键裂
催化作用
化学
氧气
选择性
电化学
物理化学
电极
有机化学
作者
Yao Wang,Miao Zheng,Yunrui Li,Juan Chen,Jinyu Ye,Chenliang Ye,Shuna Li,Jin Wang,Yongfa Zhu,Shi‐Gang Sun,Dingsheng Wang
出处
期刊:Nano Letters
[American Chemical Society]
日期:2023-08-25
卷期号:23 (17): 8194-8202
被引量:2
标识
DOI:10.1021/acs.nanolett.3c02319
摘要
Optimizing the interatomic distance of dual sites to realize C-C bond breaking of ethanol is critical for the commercialization of direct ethanol fuel cells. Herein, the concept of holding long-range dual sites is proposed to weaken the reaction barrier of C-C cleavage during the ethanol oxidation reaction (EOR). The obtained long-range Rh-O-Pt dual sites achieve a high current density of 7.43 mA/cm2 toward EOR, which is 13.3 times that of Pt/C, as well as remarkable stability. Electrochemical in situ Fourier transform infrared spectroscopy indicates that long-range Rh-O-Pt dual sites can increase the selectivity of C1 products and suppress the generation of a CO intermediate. Theoretical calculations further disclose that redistribution of the surface-localized electron around Rh-O-Pt can promote direct oxidation of -OH, accelerating C-C bond cleavage. This work provides a promising strategy for designing oxygen-bridged long-range dual sites to tune the activity and selectivity of complicated catalytic reactions.
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