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用于高效稳定电化学将CO还原为C的多孔铜电催化剂上的余氯诱导阳离子活性物种

Residual Chlorine Induced Cationic Active Species on a Porous Copper Electrocatalyst for Highly Stable Electrochemical CO Reduction to C.

作者信息

Li Minhan, Ma Yuanyuan, Chen Jun, Lawrence Robert, Luo Wei, Sacchi Marco, Jiang Wan, Yang Jianping

机构信息

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, International Joint Laboratory for Advanced Fiber and Low-dimension Materials, College of Materials Science and Engineering, Donghua University, Shanghai, 201620, P. R. China.

ARC Centre of Excellence for Electromaterials Science, Intelligent Polymer Research Institute, Australian Institute of Innovative Materials, Innovation Campus, University of Wollongong, Wollongong, NSW, 2522, Australia.

出版信息

Angew Chem Int Ed Engl. 2021 May 10;60(20):11487-11493. doi: 10.1002/anie.202102606. Epub 2021 Apr 8.

Abstract

Electrochemical carbon dioxide (CO ) reduction reaction (CO RR) is an attractive approach to deal with the emission of CO and to produce valuable fuels and chemicals in a carbon-neutral way. Many efforts have been devoted to boost the activity and selectivity of high-value multicarbon products (C ) on Cu-based electrocatalysts. However, Cu-based CO RR electrocatalysts suffer from poor catalytic stability mainly due to the structural degradation and loss of active species under CO RR condition. To date, most reported Cu-based electrocatalysts present stabilities over dozens of hours, which limits the advance of Cu-based electrocatalysts for CO RR. Herein, a porous chlorine-doped Cu electrocatalyst exhibits high C Faradaic efficiency (FE) of 53.8 % at -1.00 V versus reversible hydrogen electrode (V ). Importantly, the catalyst exhibited an outstanding catalytic stability in long-term electrocatalysis over 240 h. Experimental results show that the chlorine-induced stable cationic Cu /Cu species and the well-preserved structure with abundant active sites are critical to the high FE of C in the long-term run of electrochemical CO reduction.

摘要

电化学二氧化碳(CO₂)还原反应(CO₂RR)是一种有吸引力的方法,可用于处理CO₂排放,并以碳中和方式生产有价值的燃料和化学品。人们已做出许多努力来提高铜基电催化剂上高价值多碳产物(C₂+)的活性和选择性。然而,铜基CO₂RR电催化剂的催化稳定性较差,主要原因是在CO₂RR条件下结构降解和活性物种损失。迄今为止,大多数报道的铜基电催化剂的稳定性在数十小时以上,这限制了铜基电催化剂在CO₂RR方面的进展。在此,一种多孔氯掺杂铜电催化剂在相对于可逆氢电极(V)为-1.00 V时表现出53.8%的高C₂+法拉第效率(FE)。重要的是,该催化剂在超过240小时的长期电催化中表现出出色的催化稳定性。实验结果表明,氯诱导的稳定阳离子Cu⁺/Cu²⁺物种以及具有丰富活性位点的良好保存结构对于电化学CO₂还原长期运行中C₂+的高FE至关重要。

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