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通过结构诱导抑制析氢制备具有增强电催化CO还原性能的有序银纳米针阵列

Ordered Ag Nanoneedle Arrays with Enhanced Electrocatalytic CO Reduction via Structure-Induced Inhibition of Hydrogen Evolution.

作者信息

Chen Qin, Liu Kang, Zhou Yajiao, Wang Xiqing, Wu Kuangzhe, Li Hongmei, Pensa Evangelina, Fu Junwei, Miyauchi Masahiro, Cortés Emiliano, Liu Min

机构信息

Hunan Joint International Research Center for Carbon Dioxide Resource Utilization, School of Physics and Electronics, Central South University, Changsha 410083, People's Republic of China.

School of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450002, People's Republic of China.

出版信息

Nano Lett. 2022 Aug 10;22(15):6276-6284. doi: 10.1021/acs.nanolett.2c01853. Epub 2022 Aug 1.

Abstract

Silver is an attractive catalyst for converting CO into CO. However, the high CO activation barrier and the hydrogen evolution side reaction seriously limit its practical application and industrial perspective. Here, an ordered Ag nanoneedle array (Ag-NNAs) was prepared by template-assisted vacuum thermal-evaporation for CO electroreduction into CO. The nanoneedle array structure induces a strong local electric field at the tips, which not only reduces the activation barrier for CO electroreduction but also increases the energy barrier for the hydrogen evolution reaction (HER). Moreover, the array structure endows a high surface hydrophobicity, which can regulate the adsorption of water molecules at the interface and thus dynamically inhibit the competitive HER. As a result, the optimal Ag-NNAs exhibits 91.4% Faradaic efficiency (FE) of CO for over 700 min at -1.0 V RHE. This work provides a new concept for the application of nanoneedle array structures in electrocatalytic CO reduction reactions.

摘要

银是一种将一氧化碳转化为二氧化碳的有吸引力的催化剂。然而,较高的一氧化碳活化能垒和析氢副反应严重限制了其实际应用和工业前景。在此,通过模板辅助真空热蒸发制备了有序银纳米针阵列(Ag-NNAs)用于将一氧化碳电还原为二氧化碳。纳米针阵列结构在尖端诱导出强局部电场,这不仅降低了一氧化碳电还原的活化能垒,还增加了析氢反应(HER)的能垒。此外,阵列结构赋予了高表面疏水性,这可以调节界面处水分子的吸附,从而动态抑制竞争性析氢反应。结果,最优的Ag-NNAs在 -1.0 V(相对于可逆氢电极,RHE)下700多分钟内对二氧化碳的法拉第效率(FE)达到91.4%。这项工作为纳米针阵列结构在电催化二氧化碳还原反应中的应用提供了一个新概念。

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