程昉

个人信息Personal Information

教授

博士生导师

硕士生导师

性别:男

毕业院校:美国华盛顿大学

学位:博士

所在单位:化工学院

学科:药剂学. 药物工程. 精细化工

办公地点:大连理工大学西部校区化工实验楼G309

联系方式:0411-84986336 15941139319

电子邮箱:ffcheng@dlut.edu.cn

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Ammonia formation by a thiolate-bridged diiron amide complex as a nitrogenase mimic

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论文类型:期刊论文

发表时间:2013-04-01

发表刊物:NATURE CHEMISTRY

收录刊物:SCIE、PubMed、Scopus

卷号:5

期号:4

页面范围:320-326

ISSN号:1755-4330

摘要:Although nitrogenase enzymes routinely convert molecular nitrogen into ammonia under ambient temperature and pressure, this reaction is currently carried out industrially using the Haber-Bosch process, which requires extreme temperatures and pressures to activate dinitrogen. Biological fixation occurs through dinitrogen and reduced NxHy species at multi-iron centres of compounds bearing sulfur ligands, but it is difficult to elucidate the mechanistic details and to obtain stable model intermediate complexes for further investigation. Metal-based synthetic models have been applied to reveal partial details, although most models involve a mononuclear system. Here, we report a diiron complex bridged by a bidentate thiolate ligand that can accommodate HN=NH. Following reductions and protonations, HN=NH is converted to NH3 through pivotal intermediate complexes bridged by N2H3- and NH2- species. Notably, the final ammonia release was effected with water as the proton source. Density functional theory calculations were carried out, and a pathway of biological nitrogen fixation is proposed.