异硫氰酸荧光素后修饰的金属有机三元环光解水制氢 |
Photocatalytic Hydrogen Production Based on Metal-Organic Triangle Modified by Fluorescein Isothiocyanate |
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摘要: 将具有N、O、P三齿配位点的直线型双臂席夫碱配体L1与钴离子配位自组装得到一例[3+3]金属-有机三元环Co-L1。在该配体的苯环侧链上引入易于修饰的NH2基团,通过组装后修饰的方法把光活性的异硫氰酸荧光素(FITC)分子以共价键方式键合到金属-有机三元环上,并将其用于可见光下的光解水制氢。该体系属于无须引入额外光敏剂的双组分放氢体系。与传统的三组分体系相比,在同等金属催化剂和光敏剂浓度下,组装后修饰的金属配合物催化剂Co-L3具有更高的光催化活性,转换数(TON)可以达到80,大约是Co-L1光催化效率的30倍。 |
关键词: 金属有机大环 钴 光催化产氢 组装后修饰 |
基金项目: 国家自然科学基金(No.21971030)和大连理工大学基本科研业务费(No.DUT20ZD218)资助项目 |
Abstract: A cobalt based metal-organic[3+3] self-assembly macrocycle was constructed by tridentate Schiff base ligand L1 with N, O and P atoms (L1=1,1'-biphenyl-4,4'-di-carbohydrazide-bis-(2-diphenyphosphinobenzaldehyde)). The functionalized metal-organic triangle with amino groups was connected to photoactive fluorescein isothiocyanate (FITC) via post-assembly modification reaction. This modified complex Co-L3 was used as photocatalyst for hydrogen evolution from water splitting. It was a two-component system for hydrogen production without extra photosensitizer. Besides, compared with the three-component system, the metallosupramolecular catalyst Co-L3 underwent post-assembly modification reactions exhibited higher photocatalytic activity at the same metal catalyst and photosensitizer concentration with a turnover number (TON) of 80, which was approximately 30 times the photocatalytic efficiency of complex Co-L1. |
Keywords: metal-organic macrocycle cobalt light-driven H2 production post-assembly modification |
投稿时间:2020-05-19 修订日期:2020-06-17 |
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张文言,杨阳,黄慧琳,景旭,段春迎.异硫氰酸荧光素后修饰的金属有机三元环光解水制氢[J].无机化学学报,2020,36(10):1988-1996. |
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