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在具有可调壳层厚度的Cu@Ag核壳串联催化剂上,CO向含碳产物的电化学还原反应

Electrochemical Reduction of CO Toward C Valuables on Cu@Ag Core-Shell Tandem Catalyst with Tunable Shell Thickness.

作者信息

Zhang Shuaishuai, Zhao Shulin, Qu Dongxue, Liu Xiaojing, Wu Yuping, Chen Yuhui, Huang Wei

机构信息

State Key Laboratory of Materials-Oriented Chemical Engineering, School of Energy Science and Engineering, Nanjing Tech University, Nanjing, 211816, China.

Key Laboratory of Flexible Electronics (KLOFE)Institute of Advanced Materials (IAM), Nanjing Tech University, Nanjing, 210009, China.

出版信息

Small. 2021 Sep;17(37):e2102293. doi: 10.1002/smll.202102293. Epub 2021 Aug 3.

Abstract

Electrochemical CO reduction reaction (CO RR) is critical to converting CO to high-value multicarbon chemicals. However, the Cu-based catalysts as the only option to reduce CO into C products suffer from poor selectivity and low activity. Tandem catalysis for CO reduction is an efficient strategy to overcome such problems. Here, Cu@Ag core-shell nanoparticles (NPs) with different silver layer thicknesses are fabricated to realize the tandem catalysis for CO conversion by producing CO on Ag shell and further achieving C-C coupling on Cu core. It is found that Cu@Ag-2 NPs with the proper thickness of Ag shell exhibit the Faradaic efficiency (FE) of total C products and ethylene as high as 67.6% and 32.2% at -1.1 V (versus reversible hydrogen electrode, RHE), respectively. Moreover, it exhibits remarkably electrocatalytic stability after 14 h. Based on electrochemical tests and CO adsorption capacity analyses, the origin of the enhanced catalytic performance can be attributed to the synergistic effect between Ag shell and Cu core, which strengthens the bonding strength of CO on Cu/Ag interfaces, expedites the charge transfer, increases the electrochemical surface areas (ECSAs). This report provides a Cu-based catalyst to realize efficient C generation via a rationally designed core-shell structured catalyst.

摘要

电化学CO还原反应(CO RR)对于将CO转化为高价值的多碳化学品至关重要。然而,作为将CO还原为含碳产物的唯一选择,铜基催化剂存在选择性差和活性低的问题。用于CO还原的串联催化是克服这些问题的有效策略。在此,制备了具有不同银层厚度的Cu@Ag核壳纳米颗粒(NPs),以通过在Ag壳上产生CO并进一步在Cu核上实现C-C偶联来实现CO转化的串联催化。研究发现,具有适当Ag壳厚度的Cu@Ag-2 NPs在-1.1 V(相对于可逆氢电极,RHE)下,总含碳产物和乙烯的法拉第效率(FE)分别高达67.6%和32.2%。此外,在14小时后它表现出显著的电催化稳定性。基于电化学测试和CO吸附容量分析,催化性能增强的原因可归因于Ag壳和Cu核之间的协同效应,这种效应增强了CO在Cu/Ag界面上的键合强度,加快了电荷转移,增加了电化学表面积(ECSAs)。本报告提供了一种铜基催化剂,通过合理设计的核壳结构催化剂实现高效的碳生成。

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