Achieving a Record-High Yield Rate of 120.9 μgNH3 mgcat-1. h-1 for N2 Electrochemical Reduction over Ru Single-Atom Catalysts
Achieving a Record-High Yield Rate of 120.9 μgNH3 mgcat-1. h-1 for N2 Electrochemical Reduction over Ru Single-Atom Catalysts
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DOI：
10.1002/adma.201803498
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发表时间：
2018-10-04
影响因子：
29.4
通讯作者：
Zeng, Jie
中科院分区：
文献类型：
--
作者：
Geng, Zhigang;Liu, Yan;Zeng, Jie
在环境条件下电化学还原N-2生成NH3代表了固定N-2的诱人前景。然而，该方法的缺点是在报道的电催化剂上NH3的产率低。在这项工作中，N-2的电化学还原Ru单原子分布在氮掺杂碳（Ru SAs/N-C）的记录高的活性。在-0.2V（相对于可逆氢电极）下，Ru SA/N-C在-0.13mA cm（-2）的电流密度下，法拉第效率为29.6%。值得注意的是，Ru SAs/N-C的产率达到120.9 μ g（NH3）mg（cat）（-1）·h（-1），这比以往报道的最高值高一个数量级。本工作不仅开发了一种上级电催化剂，而且为合理设计高活性和稳定的单原子催化剂提供了指导。
The electrochemical reduction of N-2 into NH3 production under ambient conditions represents an attractive prospect for the fixation of N-2. However, this process suffers from low yield rate of NH3 over reported electrocatalysts. In this work, a record-high activity for N-2 electrochemical reduction over Ru single atoms distributed on nitrogen-doped carbon (Ru SAs/N-C) is reported. At -0.2 V versus reversible hydrogen electrode, Ru SAs/N-C achieves a Faradaic efficiency of 29.6% for NH3 production with partial current density of -0.13 mA cm(-2). Notably, the yield rate of Ru SAs/N-C reaches 120.9 mu g(NH3) mg(cat)(-1).h(-1), which is one order of magnitude higher than the highest value ever reported. This work not only develops a superior electrocatalyst for NH3 production, but also provides a guideline for the rational design of highly active and robust single-atom catalysts.