| 膦配体取代的乙基乙撑双铁配合物的合成、晶体结构及电化学催化性能 |
| Diiron Butane-1,2-dithiolate Complexes with Phosphine Ligands: Preparation, Crystal Structures, and Electrochemical Catalytic Performance |
|
| 摘要: 以母体配合物[Fe2(CO)6(μ-SCH2CH (CH2CH3) S)](1)分别与三(2-呋喃基)膦、二苯基丙基膦、双(二苯基膦)乙炔、1，2-双(二苯基膦基)苯和脱羰试剂Me3NO · 2H2O反应，制备了单取代配合物[Fe2(CO)5(L)(μ-SCH2CH (CH2CH3) S](L=P (2-C4H3O)3，2；Ph2PCH2CH2CH3，3)、桥联配合物{[Fe2(CO)5(μ-SCH2CH (CH2CH3) S)]2(Ph2PC≡CPPh2)}(4)和螯合配合物[Fe2(CO)4(κ2-(Ph2P)2(1，2-C6H4))(μ-SCH2CH (CH2CH3) S)](5)。配合物2~5经元素分析、红外光谱、核磁共振氢谱和磷谱表征，并进一步得到单晶X射线衍射的确证。电化学研究表明，在弱酸HOAc作为质子源存在的情况下，这些配合物可以实现催化质子还原产生氢气的功能。 |
| 关键词: 铁铁氢化酶 乙基乙撑双铁 晶体结构 电化学催化产氢 |
| 基金项目: 浙江省自然科学基金(No.LY19B020002)、 钒钛资源综合利用四川省重点实验室项目(No.2021FTSZ07)、 化学合成与污染控制四川省重点实验室项目(No.CSPC201904)、 四川省人力资源社会保障厅项目和四川轻化工大学项目(No.CX2021055)资助。 |
| Abstract: Treatment of the parent complex [Fe2(CO)6( μ-SCH2CH(CH2CH3)S)] (1) with tri(2-furyl)phosphine, n-propyldiphenylphosphine, bis(diphenylphosphino)acetylene, or 1, 2-bis(diphenylphosphino)benzene and Me3NO · 2H2O as the decarbonylating agent yielded the monosubstituted complexes [Fe2(CO)5(L)( μ-SCH2CH(CH2CH3)S)] (L= P(2-C4H3O)3, 2; Ph2PCH2CH2CH3, 3), bridging complex {[Fe2(CO)5( μ-SCH2CH(CH2CH3)S)]2(Ph2PC≡CPPh2)} (4), and chelating complex [Fe2(CO)4(κ2-(Ph2P)2(1,2-C6H4))( μ-SCH2CH(CH2CH3)S)] (5), respectively. Complexes 2-5 have been characterized by elemental analysis, IR, and 1H (31P{1H}) NMR spectroscopy, as well as confirmed by single crystal X-ray diffraction analysis. Moreover, the electrochemistry of complexes 2-5 has been studied, showing that these complexes can catalyze the reduction of proton to H2 in the presence of a weak acid HOAc as a proton source. |
| Keywords: [FeFe]-hydrogenases diiron butane-1,2-dithiolate crystal structure electrocatalytic H2 production |
| 投稿时间：2022-06-12 修订日期：2022-09-03 |
| 摘要点击次数: 3915 |
| 全文下载次数: 351 |
| 刘旭锋,徐博,徐航,李玉龙.膦配体取代的乙基乙撑双铁配合物的合成、晶体结构及电化学催化性能[J].无机化学学报,2022,38(12):2521-2529. |
| 查看全文 查看/发表评论 下载PDF阅读器 |
| Support information: |
|
|
|
|
|
|
