Composition-dependent electrochemical activity of Ag-based alloy nanotubes for efficient nitrogen reduction under ambient conditions

Composition-dependent electrochemical activity of Ag-based alloy nanotubes for efficient nitrogen reduction under ambient conditions
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环境条件下银基合金纳米管高效氮还原的成分依赖性电化学活性

DOI:
10.1016/j.electacta.2019.134691
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发表时间:
2019-10
影响因子:
6.6
通讯作者:
Zhang Weiqing
Zhang Weiqing
中科院分区:
材料科学2区
文献类型:
--
作者:
Zhang Qiwen;Shen Yongli;Hou Yufan;Yang Liting;Chen Baili;Lei Zhen;Zhang Weiqing

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电催化氮还原反应(NRR)催化剂的组成-活性关系可以指导NRR催化剂的合理设计。本文系统地研究了银基合金纳米管的组成对电催化NRR活性的影响。结果表明,在原子比为8:1 ~ 1:2的AgAu纳米管中,Ag 2Au 1合金纳米管对NRR催化活性的增强作用最大.具体而言,在-0.30 V vs. RHE下,Ag 2Au 1纳米管的NH3产生速率和法拉第效率分别为21.7 μg h-1 mgcat-1和3.8%,分别是Ag纳米线的3.0倍和3.6倍。与Ag 2 Pd 1和Ag 2 Pt 1纳米管相比,Ag 2Au 1空心纳米管也表现出更好的NRR催化活性。理论计算结果表明,Ag 2Au 1合金中Au原子的负离子特性有利于N2的吸附和活化。此外,Ag 2Au 1纳米管在18 h内表现出稳定的NH3产率和法拉第效率,显示了其在NRR电催化方面的巨大潜力。
The composition-activity relationship is highly desirable for electrocatalytic nitrogen reduction reaction (NRR) because it could guide the rational design of efficient NRR catalysts. In this work, the composition effect of Ag-based alloy nanotubes on electrocatalytic NRR activity is systematically investigated. It is found that, among AgAu nanotubes with atomic ratio from 8:1 to 1:2, Ag2Au1alloy nanotubes achieve the largest enhancement for NRR catalytic activity. Specifically, the NH3production rate and faradaic efficiency of Ag2Au1nanotubes are 21.7 μg h−1mgcat−1and 3.8% at −0.30 V vs. RHE, respectively, which were 3.0 and 3.6 times higher than those of Ag nanowires. Compared with Ag2Pd1and Ag2Pt1nanotubes, Ag2Au1hollow nanotubes also exhibit a better NRR catalytic activity. Theoretical calculation results indicate that the negative ion characteristic of Au atoms in the Ag2Au1alloy is favorable for the adsorption and activation of N2. Moreover, Ag2Au1nanotubes showed stable NH3yield rate and faradaic efficiency up to 18 h, revealing its great potential for promising NRR electrocatalysis.
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