A photo- and electrochemical investigation of BODIPY-cobaloxime complexes for hydrogen production, coupled with quantum chemical calculations

被引：28

作者：

Manton, Jennifer C. ^{[1
]}

Long, Conor ^{[1
]}

Vos, Johannes G. ^{[1
]}

Pryce, Mary T. ^{[1
]}

机构：

[1] Dublin City Univ, Sch Chem Sci, SRC Solar Energy Convers, Dublin 9, Ireland

来源：

PHYSICAL CHEMISTRY CHEMICAL PHYSICS | 2014年 / 16卷 / 11期

关键词：

DENSITY-FUNCTIONAL THEORY; KINETIC-ENERGY DENSITY; SET MODEL CHEMISTRY; GAUSSIAN-BASIS SETS; PHOTOPHYSICAL PROPERTIES; MOLECULAR CALCULATIONS; SEPARATION; EVOLUTION; LIGANDS; COBALT;

D O I：

10.1039/c3cp55347g

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Two BODIPY-cobaloxime complexes; [{Co(dmgH)(2)Cl}{3-[bis-(4-ethyl-3,5-dimethyl-1H-pyrrol-2-yl)-methyl]-pyridine- borondiflouride}] (1a) and [{Co(dmgH)(2)Cl}{4-[bis-(4-ethyl-3,5-dimethyl-1H-pyrrol-2-yl)-methyl]-pyridine- borondiflouride}] (2a) (BODIPY = boron dipyrromethene), (dmgH = dimethylglyoxime) have been synthesised and studied as model catalytic systems for the generation of hydrogen gas in aqueous media. Under photochemical conditions, neither complex catalysed the reduction of water to hydrogen. However, both complexes showed considerable activity under electrochemical conditions. Turn-over-numbers for hydrogen production of 1.65 x 10(4) and 1.08 x 10(4) were obtained for 1a and 2a respectively following potentiostatic electrolysis at -1.2 V vs. Ag/AgCl after 1 hour. Quantum chemical calculations were performed to provide an explanation for the lack of photochemical activity.

引用

页码：5229 / 5236

页数：8

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