Mo2C embedded on nitrogen-doped carbon toward electrocatalytic nitrogen reduction to ammonia under ambient conditions
Mo2C embedded on nitrogen-doped carbon toward electrocatalytic nitrogen reduction to ammonia under ambient conditions
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Mo2C嵌入氮掺杂碳上，用于在环境条件下电催化氮还原为氨
DOI：
10.1016/j.ijhydene.2021.01.150
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发表时间：
2021
影响因子：
7.2
通讯作者：
Leung Michael K. H.
中科院分区：
文献类型：
--
作者：
Zhang Yizhen;Hu Jue;Zhang Chengxu;Cheung Altair T. F.;Zhang Yue;Liu Lifen;Leung Michael K. H.
电化学氮还原反应（e-NRR）对于利用可再生能源在温和条件下生产氨具有诱人的前景。然而，开发高效稳定的电催化剂来驱动 e-NRR 仍然是一个巨大的挑战。在此，受活性钼固氮酶生物固氮的启发，首次开发了源自Mo/Zn-ZIF的氮掺杂多孔碳（Mo2C/NC）上的碳化钼，作为环境条件下的高效e-NRR电催化剂。在 0.1 M Na2SO4 电解质中，Mo2C/NC 催化剂在 -0.2 V vs. RHE 下实现了 70.6 μmol h−1gcat.−1 的最大 NH3 产率和 12.3% 的法拉第效率。此外，由于Mo2C和ZIFs衍生的碳骨架的结构和电化学稳定性，Mo2C/NC在长时间电解过程中表现出良好的电化学选择性和耐久性。这项工作为金属碳化物及其化合物作为高效 e-NRR 催化剂提供了新的视角。
Electrochemical nitrogen reduction reaction (e-NRR) is an attractive prospect for ammonia production under mild conditions using renewable energy. However, developing efficient and stable electrocatalysts for driving e-NRR remains a great challenge. Herein, inspired by the biological nitrogen fixation via active Mo-nitrogenase, molybdenum carbide on N-doped porous carbon (Mo2C/NC) derived from Mo/Zn-ZIFs was developed for the first time, as an efficient e-NRR electrocatalyst under ambient conditions. In 0.1 M Na2SO4electrolyte, the Mo2C/NC catalyst achieved a maximum NH3yield rate of 70.6 μmol h−1gcat.−1and a faradaic efficiency of 12.3% at −0.2 V vs. RHE. Additionally, Mo2C/NC displayed favorable electrochemical selectivity and durability during the longtime electrolysis, attributed to the structural and electrochemical stability of Mo2C and ZIFs-derived carbon framework. This work provides new perspectives upon metal carbides and their compounds as catalysts for efficient e-NRR.