催化作用
化学
电化学
Atom(片上系统)
法拉第效率
分子
铜
吸附
密度泛函理论
选择性
氧化还原
化学物理
纳米技术
无机化学
化学工程
材料科学
电极
计算化学
物理化学
有机化学
工程类
嵌入式系统
计算机科学
作者
Jiqing Jiao,Rui Lin,Shoujie Liu,Weng‐Chon Cheong,Chao Zhang,Zheng Chen,Yuan Pan,Jianguo Tang,Konglin Wu,Sung‐Fu Hung,Hao Ming Chen,Lirong Zheng,Qi Lu,Xuan Yang,Bingjun Xu,Hai Xiao,Jun Li,Dingsheng Wang,Qing Peng,Chen Chen,Yadong Li
出处
期刊:Nature Chemistry
[Springer Nature]
日期:2019-01-21
卷期号:11 (3): 222-228
被引量:633
标识
DOI:10.1038/s41557-018-0201-x
摘要
The electrochemical reduction of CO2 could play an important role in addressing climate-change issues and global energy demands as part of a carbon-neutral energy cycle. Single-atom catalysts can display outstanding electrocatalytic performance; however, given their single-site nature they are usually only amenable to reactions that involve single molecules. For processes that involve multiple molecules, improved catalytic properties could be achieved through the development of atomically dispersed catalysts with higher complexities. Here we report a catalyst that features two adjacent copper atoms, which we call an ‘atom-pair catalyst’, that work together to carry out the critical bimolecular step in CO2 reduction. The atom-pair catalyst features stable Cu10–Cu1x+ pair structures, with Cu1x+ adsorbing H2O and the neighbouring Cu10 adsorbing CO2, which thereby promotes CO2 activation. This results in a Faradaic efficiency for CO generation above 92%, with the competing hydrogen evolution reaction almost completely suppressed. Experimental characterization and density functional theory revealed that the adsorption configuration reduces the activation energy, which generates high selectivity, activity and stability under relatively low potentials. Anchored single-atom catalysts have recently been shown to be very active for various processes, however, a catalyst that features two adjacent copper atoms—which we call an atom-pair catalyst—is now reported. The Cu10–Cu1x+ pair structures work together to carry out the critical bimolecular step in CO2 reduction.
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