用于高效电合成氨的氧配位钼单原子催化剂。

An oxygen-coordinated molybdenum single atom catalyst for efficient electrosynthesis of ammonia.

作者信息

Geng Jing, Zhang Shengbo, Xu Hui, Wang Guozhong, Zhang Haimin

机构信息

Key Laboratory of Materials Physics, Centre for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience, Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences, Hefei 230031, China.

出版信息

Chem Commun (Camb). 2021 Jun 1;57(44):5410-5413. doi: 10.1039/d1cc01455b.

DOI:10.1039/d1cc01455b

PMID:33949474

Abstract

Electrochemical nitrogen (N2) reduction has been regarded as a promising strategy for artificial ammonia (NH3) production under ambient conditions. Herein, we report the fabrication of molybdenum (Mo) single atoms anchored on activated carbon (Mo-SAs/AC) for the electrochemical N2 reduction to NH3. The surface-rich oxygen functional groups of activated carbon can effectively capture the Mo precursor, and concurrently act as the coordination sites to anchor Mo single atoms by forming Mo-Ox bonds. As a result, the Mo-SAs/AC as an electrocatalyst shows high activity toward the N2 reduction reaction (NRR), affording an NH3 yield rate of 2.55 ± 0.31 mg h-1 mgMo-1 and a faradaic efficiency (FE) of 57.54 ± 6.98% at -0.40 V (vs. RHE) in 0.1 M Na2SO4 electrolyte with good stability and durability. The constructed Mo-Ox sites are responsible for high NRR activity of Mo-SAs/AC.

摘要

电化学氮还原被认为是在环境条件下人工合成氨的一种有前景的策略。在此，我们报道了锚定在活性炭上的钼单原子（Mo-SAs/AC）用于电化学氮还原制氨的制备方法。活性炭表面丰富的氧官能团能够有效捕获钼前驱体，并同时作为配位位点通过形成Mo-Ox键来锚定钼单原子。结果，Mo-SAs/AC作为一种电催化剂对氮还原反应（NRR）表现出高活性，在0.1 M Na2SO4电解液中，于-0.40 V（相对于可逆氢电极）下，氨产率为2.55±0.31 mg h-1 mgMo-1，法拉第效率（FE）为57.54±6.98%，具有良好的稳定性和耐久性。所构建的Mo-Ox位点是Mo-SAs/AC具有高NRR活性的原因。