Zhang Longcheng, Liang Jie, Wang Yuanyuan, Mou Ting, Lin Yiting, Yue Luchao, Li Tingshuai, Liu Qian, Luo Yonglan, Li Na, Tang Bo, Liu Yang, Gao Shuyan, Alshehri Abdulmohsen Ali, Guo Xiaodong, Ma Dongwei, Sun Xuping
Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu, 610054, Sichuan, China.
School of Chemical Engineering, Sichuan University, Chengdu, 610065, Sichuan, China.
Angew Chem Int Ed Engl. 2021 Nov 22;60(48):25263-25268. doi: 10.1002/anie.202110879. Epub 2021 Oct 27.
Electrochemical reduction of NO not only offers an attractive alternative to the Haber-Bosch process for ambient NH production but mitigates the human-caused unbalance of nitrogen cycle. Herein, we report that MoS nanosheet on graphite felt (MoS /GF) acts as an efficient and robust 3D electrocatalyst for NO-to-NH conversion. In acidic electrolyte, such MoS /GF attains a maximal Faradaic efficiency of 76.6 % and a large NH yield of up to 99.6 μmol cm h . Using MoS nanosheet-loaded carbon paper as the cathode, a proof-of-concept device of Zn-NO battery was assembled to deliver a discharge power density of 1.04 mW cm and an NH yield of 411.8 μg h mg . Calculations reveal that the positively charged Mo-edge sites facilitate NO adsorption/activation via an acceptance-donation mechanism and disfavor the binding of protons and the coupling of N-N bond.
电化学还原NO不仅为环境条件下合成氨提供了一种有吸引力的替代哈伯-博施法的方法，还缓解了人为造成的氮循环失衡。在此，我们报道了石墨毡上的MoS纳米片（MoS /GF）作为一种高效且稳定的三维电催化剂用于NO到NH的转化。在酸性电解质中，这种MoS /GF实现了76.6%的最大法拉第效率和高达99.6 μmol cm h的高NH产率。使用负载MoS纳米片的碳纸作为阴极，组装了一个锌-NO电池的概念验证装置，其放电功率密度为 1.04 mW cm，NH产率为411.8 μg h mg 。计算表明，带正电的Mo边缘位点通过接受-给予机制促进NO的吸附/活化，不利于质子的结合和N-N键的偶联。
