催化作用
材料科学
电化学
选择性
吸附
氧化物
纳米片
电流密度
法拉第效率
化学工程
电极
金属
铜
选择性催化还原
纳米技术
物理化学
化学
有机化学
冶金
物理
量子力学
工程类
作者
Ruian Du,Qiqi Wu,Shiyi Zhang,Peng Wang,Zheng Jian Li,Yongcai Qiu,Keyou Yan,Geoffrey I.N. Waterhouse,Pei Wang,Jia Li,Yun Zhao,Weiwei Zhao,Xue Wang,Guangxu Chen
出处
期刊:Small
[Wiley]
日期:2023-03-28
卷期号:19 (28)
被引量:11
标识
DOI:10.1002/smll.202301289
摘要
Abstract The electrocatalytic CO 2 reduction reaction (CO 2 RR) is an attractive technology for CO 2 valorization and high‐density electrical energy storage. Achieving a high selectivity to C 2+ products, especially ethylene, during CO 2 RR at high current densities (>500 mA cm −2 ) is a prized goal of current research, though remains technically very challenging. Herein, it is demonstrated that the surface and interfacial structures of Cu catalysts, and the solid–gas–liquid interfaces on gas‐diffusion electrode (GDE) in CO 2 reduction flow cells can be modulated to allow efficient CO 2 RR to C 2+ products. This approach uses the in situ electrochemical reduction of a CuO nanosheet/graphene oxide dots (CuOC(O)) hybrid. Owing to abundant CuOC interfaces in the CuOC(O) hybrid, the CuO nanosheets are topologically and selectively transformed into metallic Cu nanosheets exposing Cu(100) facets, Cu(110) facets, Cu[ n (100) × (110)] step sites, and Cu + /Cu 0 interfaces during the electroreduction step, the faradaic efficiencie (FE) to C 2+ hydrocarbons was reached as high as 77.4% (FE ethylene ≈ 60%) at 500 mA cm −2 . In situ infrared spectroscopy and DFT simulations demonstrate that abundant Cu + species and Cu 0 /Cu + interfaces in the reduced CuOC(O) catalyst improve the adsorption and surface coverage of *CO on the Cu catalyst, thus facilitating CC coupling reactions.
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