Photocatalytic Hydrogen Production from Water by Noble-Metal-Free Molecular Catalyst Systems Containing Rose Bengal and the Cobaloximes of BFx-Bridged Oxime Ligands

被引:148
作者
Zhang, Pan [1 ]
Wang, Mei [1 ]
Dong, Jingfeng [1 ]
Li, Xueqiang [1 ]
Wang, Feng [2 ]
Wu, Lizhu [2 ]
Sun, Licheng [1 ,3 ]
机构
[1] Dalian Univ Technol, State Key Lab Fine Chem, DUT KTH Joint Educ & Res Ctr Mol Devices, Dalian 116012, Peoples R China
[2] Tech Inst Phys & Chem, Key Lab Photochem Convers & Optoelect Mat, Beijing 100190, Peoples R China
[3] Royal Inst Technol, Dept Chem, S-10044 Stockholm, Sweden
基金
瑞典研究理事会;
关键词
ELECTRON-TRANSFER REACTIONS; COBALT; COMPLEXES; REDUCTION; PHOTOREDUCTION; GENERATION; IRIDIUM; EVOLUTION; DIIMINE; MODELS;
D O I
10.1021/jp106512a
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
Hydrogen evolution was observed from the noble-metal-free catalyst systems, comprising Rose Bengal, BFx-bridged cobaloximes, and triethylamine, in an aqueous solution under irradiation of visible light. Two types of BFx-bridged cobaloximes namely, the annulated cobaloximes [Co(dmgBF(2))(2)(H2O)(2)] (1, dmgBF(2) = (difluoroboryl)dimethylglyoximate anion) and [Co(dpgBF(2))(2)(H2O)(2)] (2, dpgBF(2) =(difluoroboryl)diphenylglyoximate anion), and the clathrochelated cobaloximes [Co(dmg(BF)(2/3))(3)](BF4) (3) and [Co(dpg(BF)(2/3))(3)](BF4) (4)-were used as catalysts. Among the four cobalt complexes, complex 1 displayed the highest hydrogen-evolving efficiency, with turnovers up to 327. Complexes 2 and 4 that bear the diphenylglyoximate ligands exhibited much lower efficiencies as compared with their analogues 1 and 3 that have the dimethylglyoximate ligands. The hydrogen-evolving efficiency of the annulated cobalt(II) complex 1 that contains two labile axial ligands is more than three times as high as that of the encapsulated cobalt(III) complex 3 that has a single macrobicyclic ligand. The different pathways for formation of the cobalt(I) species from these two types of cobaloximes are discussed on the basis of the results obtained from fluorescence and laser flash photolysis spectroscopic studies.
引用
收藏
页码:15868 / 15874
页数:7
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