材料科学
催化作用
选择性
纳米颗粒
铜
电化学
氢
制氢
钯
法拉第效率
化学工程
无机化学
纳米技术
电极
化学
物理化学
有机化学
冶金
工程类
作者
Xianmeng Song,Wanfeng Xiong,Hao He,Duan‐Hui Si,Linzhe Lü,Yuhang Peng,Qiaorong Jiang,Yanjie Wang,Yanping Zheng,Zi‐Ang Nan,Qiuxiang Wang,Mingshu Chen,Rong Cao,Feng Ru Fan
出处
期刊:Nano Energy
[Elsevier]
日期:2024-04-01
卷期号:122: 109275-109275
标识
DOI:10.1016/j.nanoen.2024.109275
摘要
Direct electrochemical conversion of CO2 to C2H4 is a promising technology for high-value chemical synthesis. However, challenges arise from competing hydrogen evolution reactions (HER) and the formation of undesired C1 products. In this study, we successfully engineered palladium nanoparticles (Pd NPs) with hydrogen storage capabilities on the Cu2O interface. This strategic modification effectively controls hydrogen states at the interface, leading to simultaneous HER inhibition and a significant increase in C2H4 selectivity. Detailed insights into the reaction mechanism were obtained through in-situ infrared spectroscopy, in-situ X-ray diffraction (XRD) and controlled experiments, offering a molecular-level understanding of the reaction mechanism. The interface-modified Pd NPs provided stable *H intermediates during the reaction process, effectively suppressing HER. Furthermore, the direct bonding between Pd and Cu interfaces increases charge density at the copper sites. These copper sites, in conjunction with the Pd-H sites, activate *CO at the Pd-Cu interface, forming stable *CHO intermediates. This enhances the coupling of *CHO and *CO intermediates, resulting in a remarkable increase in the C2H4/H2 production rate from 0.4 to 2.0 after Pd NPs modification, with a high faradaic efficiency of up to 46%. Our work presents a promising approach for designing copper-based CO2 reduction catalysts with outstanding activity and selectivity.
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