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拉伸应变铜穿透电极促进酸性条件下安培级CO到C还原的不对称C-C偶联。

Tensile-Strained Cu Penetration Electrode Boosts Asymmetric C-C Coupling for Ampere-Level CO-to-C Reduction in Acid.

作者信息

Li Shoujie, Wu Gangfeng, Mao Jianing, Chen Aohui, Liu Xiaohu, Zeng Jianrong, Wei Yiheng, Wang Jiangjiang, Zhu Huanyi, Xia Jiayu, Wang Xiaotong, Li Guihua, Song Yanfang, Dong Xiao, Wei Wei, Chen Wei

机构信息

Low-Carbon Conversion Science and Engineering Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210, Shanghai, China.

State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210, Shanghai, China.

出版信息

Angew Chem Int Ed Engl. 2024 Oct 7;63(41):e202407612. doi: 10.1002/anie.202407612. Epub 2024 Sep 6.

Abstract

The synthesis of multicarbon (C) products remains a substantial challenge in sustainable CO electroreduction owing to the need for sufficient current density and faradaic efficiency alongside carbon efficiency. Herein, we demonstrate ampere-level high-efficiency CO electroreduction to C products in both neutral and strongly acidic (pH=1) electrolytes using a hierarchical Cu hollow-fiber penetration electrode (HPE). High concentration of K could concurrently suppress hydrogen evolution reaction and facilitate C-C coupling, thereby promoting C production in strong acid. By optimizing the K and H concentration and CO flow rate, a faradaic efficiency of 84.5 % and a partial current density as high as 3.1 A cm for C products, alongside a single-pass carbon efficiency of 81.5 % and stable electrolysis for 240 h were demonstrated in a strong acidic solution of HSO and KCl (pH=1). Experimental measurements and density functional theory simulations suggested that tensile-strained Cu HPE enhances the asymmetric C-C coupling to steer the selectivity and activity of C products.

摘要

在可持续的CO电还原中,由于需要足够的电流密度、法拉第效率以及碳效率,多碳(C)产物的合成仍然是一个重大挑战。在此,我们展示了使用分级铜中空纤维穿透电极(HPE)在中性和强酸性(pH = 1)电解质中实现安培级高效CO电还原为C产物。高浓度的K可以同时抑制析氢反应并促进C-C偶联,从而在强酸中促进C的生成。通过优化K和H的浓度以及CO流速,在HSO和KCl的强酸性溶液(pH = 1)中,实现了C产物的法拉第效率为84.5%,部分电流密度高达3.1 A cm,单程碳效率为81.5%,并能稳定电解240小时。实验测量和密度泛函理论模拟表明,拉伸应变的铜HPE增强了不对称C-C偶联,从而控制了C产物的选择性和活性。

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