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用于提高电催化硝酸盐还原制氨性能的氧化铜/银异质结构

CuO/Ag Heterostructure for Boosting the Electrocatalytic Nitrate Reduction to Ammonia Performance.

作者信息

Liu Yang, Yao Xiao-Man, Liu Xu, Liu Zhiliang, Wang Yan-Qin

机构信息

Inner Mongolia Key Laboratory of Chemistry and Physics of Rare Earth Materials, College of Chemistry and Chemical Engineering, Inner Mongolia University, Huhhot 010021, China.

出版信息

Inorg Chem. 2023 May 15;62(19):7525-7532. doi: 10.1021/acs.inorgchem.3c00857. Epub 2023 May 3.

Abstract

Electrocatalytic nitrate reduction reaction (ENORR) is an alternative, sustainable, and environmentally friendly value-added NH synthesis method under ambient conditions relative to the traditional Haber-Bosch process; however, its low NH yield, low Faradaic efficiency (FE), low selectivity, and low conversion rate severely restrict the development. In this work, a CuO/Ag-CC heterostructured electrocatalyst was successfully fabricated by constructing a heterogeneous interface between CuO and Ag for selective electrochemical nitrate-to-ammonia conversion. The construction of the heterogeneous interface effectively promotes the synergistic effect of the catalytically active components CuO and Ag, which enhances the material conductivity, accelerates the interfacial electron transfer, and exposes more active sites, thus improving the performance of ENORR. Such CuO/Ag-CC manifests a high NH yield of 2.2 mg h cm and a notable ammonia FE of 85.03% at the optimal applied potential of -0.74 V vs RHE in a relatively low concentration of 0.01 M NO-containing 0.1 M KOH. Moreover, it shows excellent electrochemical stability during the cycle tests. Our study not only provides an efficient catalyst for ammonia electro-synthesis from ENORR but also an effective strategy for the construction of ENORR electrocatalysts for electrocatalytic applications.

摘要

与传统的哈伯-博施法相比,电催化硝酸盐还原反应(ENORR)是一种在环境条件下可替代的、可持续且环保的增值氨合成方法;然而,其低氨产率、低法拉第效率(FE)、低选择性和低转化率严重限制了该反应的发展。在这项工作中,通过在CuO和Ag之间构建异质界面,成功制备了一种CuO/Ag-CC异质结构电催化剂,用于选择性电化学硝酸盐制氨转化。异质界面的构建有效地促进了催化活性组分CuO和Ag的协同效应,提高了材料的导电性,加速了界面电子转移,并暴露出更多活性位点,从而提高了ENORR的性能。在相对低浓度的含0.01 M NO的0.1 M KOH溶液中,相对于可逆氢电极(RHE),在-0.74 V的最佳施加电位下,这种CuO/Ag-CC表现出2.2 mg h cm的高氨产率和85.03%的显著氨法拉第效率。此外,在循环测试中它表现出优异的电化学稳定性。我们的研究不仅为ENORR氨电合成提供了一种高效催化剂,也为构建用于电催化应用的ENORR电催化剂提供了一种有效策略。

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