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Bioinspired Activation of N 2 on Asymmetrical Coordinated Fe Grafted 1T MoS 2 at Room Temperature †
Author(s) -
Guo Jiaojiao,
Wang Maoyu,
Xu Liang,
Li Xiaomin,
Iqbal Asma,
Sterbinsky George E.,
Yang Hao,
Xie Miao,
Zai Jiantao,
Feng Zhenxing,
Cheng Tao,
Qian Xuefeng
Publication year - 2021
Publication title -
chinese journal of chemistry
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.28
H-Index - 41
eISSN - 1614-7065
pISSN - 1001-604X
DOI - 10.1002/cjoc.202000675
Subject(s) - chemistry , nitrogenase , raman spectroscopy , nitrogen , yield (engineering) , nitrogen fixation , ammonia , redox , electrochemistry , absorption spectroscopy , inorganic chemistry , analytical chemistry (journal) , organic chemistry , electrode , metallurgy , physics , materials science , quantum mechanics , optics
Main observation and conclusion Inspired by the nitrogen fixation process on MoFe nitrogenase, asymmetrical coordinated Fe grafted onto 1T MoS 2 were successfully synthesized. The unique electron‐rich structure with asymmetrical coordination made the 1T Fe 0.1 Mo 0.9 S 2 layered material actively react with water and dinitrogen at room temperature and atmosphere pressure. Subsequently, ammonia can be produced with a yield of ~800 μmol (NH 4 + ) g −1 (12.5% yield in mole). The activation, fixation and reduction of dinitrogen were confirmed by isotopically labeled experiments. The location and the specific coordination environment of grafted Fe in Fe‐Mo‐S were further determined by X‐ray absorption spectroscopy analysis. Our work demonstrates that the nitrogen fixation and reduction for ammonia at room temperature without any chemical and electrochemical assistance is distinctly different from traditional bionic‐inspired nitrogen fixation process. The mechanism of the activation and reduction of N 2 was further investigated by density functional theory calculation and Raman spectra. Compared with 1T MoS 2 , the enriched electron nature and asymmetrical coordination of Fe in Fe‐Mo‐S materials play a critical role in the bioinspired activation of N 2 at ambient condition.