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个人信息Personal Information
教授
博士生导师
硕士生导师
主要任职：中国化学会创始会士、常务理事，中国化工学会会士
性别：男
毕业院校：大连理工大学
学位：博士
所在单位：化工学院
学科：应用化学. 精细化工. 化学生物学
办公地点：大连理工大学西部校区知顺楼F-202#
http://peng-group.dlut.edu.cn/
联系方式：大连理工大学西部校区知顺楼F-202 辽宁省大连市高新区凌工路2号，大连116024 课题组网址：http://peng-group.dlut.edu.cn/ E-mail: pengxj@dlut.edu.cn
电子邮箱：pengxj@dlut.edu.cn
Selenium-bridged diiron hexacarbonyl complexes as biomimetic models for the active site of Fe-Fe hydrogenases
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论文类型：期刊论文
发表时间：2008-04-28
发表刊物：DALTON TRANSACTIONS
收录刊物：SCIE、EI、PubMed
期号：16
页面范围：2128-2135
ISSN号：1477-9226
摘要：Three N-substituted selenium-bridged diiron complexes [{(mu-SeCH2)(2)NC6H4R}Fe-2(CO)(6)] (R= 4-NO2, 7; R = H, 8; R = 4-CH3, 9) were firstly prepared as biomimetic models for the Fe-Fe hydrogenases active site. Models 7-9 could be generated by the convergent reaction of [(mu-HSe)(2)Fe-2(CO)(6)] (6) with N,N-bis(hydroxymethyl)-4-nitroaniline ( 1), N, N-bis( hydroxymethyl) aniline ( 2), and N, N-bis( hydroxymethyl)-4-methylaniline ( 3) in 46-52% yields. All the new complexes 7-9 were characterized by IR, H-1 and C-13 NMR and HRMS spectra and their molecular structures were determined by single-crystal X-ray analysis. The redox properties of 7-9 and their dithiolate analogues [{(mu-SCH2)(2)NC6H4R}Fe-2(CO)(6)] (R= 4-NO2, 7s; R = H, 8s; R = 4-CH3, 9s) were evaluated by cyclic voltammograms. The electrochemical proton reduction by 9 and 9s were investigated in the presence of p-toluenesulfonic acid (HOTs) to evaluate the influence of changing the coordinating S atoms of the bridging ligands to Se atoms on the electrocatalytic activity for proton reduction.