期刊
CHEMPLUSCHEM
卷 86, 期 11, 页码 1511-1516出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cplu.202100349
关键词
ammonia oxidation; dinitrogen; electrochemical oxidation; heterogeneous catalysis; transition metal complexes
资金
- CREST, JST [JPMJCR1541]
- JSPS [20H05671, 20K21203, 20K05532]
- MEXT [20H05671, 20K21203, 20K05532]
- Leadership Development Program for Ph.D in the School of Engineering, the University of Tokyo
- JSPS
- Grants-in-Aid for Scientific Research [20H05671, 20K05532] Funding Source: KAKEN
The study presents a manganese-catalyzed oxidative conversion of ammonia into dinitrogen, which can be conducted under chemical or electrochemical conditions. Under chemical conditions, up to 17.1 equivalents of N-2 per catalyst are generated, while under electrochemical conditions, the reaction proceeds with 96% faradaic efficiency to give up to 6.56 equivalents of N-2 per catalyst.
Earth-abundant metal-catalyzed oxidative conversion of ammonia into dinitrogen is a promising process to utilize ammonia as a transportation fuel. Herein, we report the manganese-catalyzed ammonia oxidation under chemical or electrochemical conditions using a manganese complex bearing (1S,2S)-N,N '-bis(3,5-di-tert-butylsalicylidene)-1,2-cyclohexanediamine. Under chemical conditions using oxidant, up to 17.1 equivalents of N-2 per catalyst are generated. Also, mechanistic studies by stoichiometric reactions reveal that a nucleophilic attack of ammonia on manganese nitrogenous species occurs to form a nitrogen-nitrogen bond leading to dinitrogen. Moreover, we conduct density functional theory (DFT) calculations to confirm the plausible reaction mechanism. In addition, this reaction system is applicable under electrochemical conditions. The catalytic reaction proceeds with 96 % faradaic efficiency (FE) in bulk electrolysis to give up to 6.56 equivalents of N-2 per catalyst.
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