Binuclear rhenium(I) complexes for the photocatalytic reduction of CO2

被引:79
|
作者
Bruckmeier, Christian [1 ]
Lehenmeier, Maximilian W. [1 ]
Reithmeier, Richard [1 ]
Rieger, Bernhard [1 ]
Herranz, Juan [2 ]
Kavakli, Cueneyt [2 ]
机构
[1] Tech Univ Munich, Catalysis Res Ctr, WACKER, Chair Macromol Chem, D-85748 Garching, Germany
[2] Tech Univ Munich, Dept Tech Electrochem, D-85748 Garching, Germany
关键词
CARBON-DIOXIDE; METAL-COMPLEXES; EXCITED-STATE; ELECTROCATALYTIC REDUCTION; ELECTROCHEMICAL REDUCTION; PHOTOINDUCED REDUCTION; CATALYSTS; LIGAND; REACTIVITY; PHOTOCHEMISTRY;
D O I
10.1039/c2dt30273j
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
Binuclear rhenium(I) complexes with 1,2-bis(4,4'-methyl-[2,2'] bipyridyl)-ethane and 1,2-bis(4,4'-methyl-[ 2,2'] bipyridyl)-dodecane as bridging ligands and their mononuclear analogues have been synthesized and characterized by their spectroscopic and electrochemical properties. First reduction potentials and luminescence properties as well as the reductive quenching of the emissive state with TEOA were not affected by the alkyl linker. By means of a detailed comparison of the photocatalytic CO2 reductions of the monometallic and the bimetallic complexes a great beneficial effect on the activity depending on the proximity of the centres was found. In high dilution the overall kinetics in the CO2 photoreduction of mononuclear complexes are clearly monometallic. If the proximity of the centres is adjusted according to the lifetime of the OER (one electron reduced species) the photocatalytic activity is greatly improved showing a clear bimetallic mechanism. In the binuclear rhenium complexes, both the facile generation of a free coordination site and binuclear interactions for effective two electron transfer can be realized.
引用
收藏
页码:5026 / 5037
页数:12
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