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
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.