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Design, Synthesis And Studies Of Cobalt,iron And Copper Complexes With Electrocatalytic Or Photo-catalytic Water Splitting Properties

Posted on:2017-03-11Degree:MasterType:Thesis
Country:ChinaCandidate:L L ZhouFull Text:PDF
GTID:2271330503468872Subject:Inorganic Chemistry
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In 21 th, is the area of information and the technology. Along with science’s and technology’s swift development, the demand for energy is also growing, however, resource have been less and less. Development and utilization of new energy sources to become the problem of the moment.Hydrogen energy is the ideal energy in 21 th.Water splitting is composed of two parts,which are the oxidation and reduction of water, it demands 113.38 kcal/mol(4.92 eV) energy. From the point of thermodynamics,we can say that water is a relatively stable molecule. Electrolysis of water can get pure hydrogen and oxygen, but it has to consume a part of electrical power.Can we reduce the consumption of electrical energy from the chemical point. The activation energy required for the reaction can be reduced by the addition of a suitable catalyst. Similarly,searching for an efficient catalyst can also reduce the electrical energy required for the electrolysis of water. We also found, microorganism can produce hydrogen by catalytic pyrolysis of water under the action of photosynthesis. Although the biological environment of photosynthesis is not simulated, this phenomenon has led scientists to the study of molecular catalysis have a deeper thinking. Whether the hydrogen can be produced by light, which can reduce the consumption of electrical energy. So, searching for new catalysts of water splitting by designing new ligands and different types of transition metal complexes is an important work of this paper.This paper including:First, three organic ligands were synthesized: 1-[(2-methoxy)benzene]-3-[benzothiazole] Triazene(HLa),Dimethylaminoethylamino-N,N-bis(2-methylene-4-tert-butyl-6-methylphenol)(HLb),(2-aminomethylpyridine)-N-2-(2-methene-4-ethyl-6-tert-butylphenol),N-(2-methene-4-methyl-6-tert-butylphenol)(HLc).Second, five new complexes were prepared and characterized: complex [Co2(La)4] 1, complex [LbCoCl] 2, complex [LbCo(H2O)] 3, complex [LcFeCl] 4, and complex [CuMe2(oxpn)Cu(OH)2]5 and properties of complexes were characterized by X-ray crystallography and Uv-vis and so on.Third, one new complex was studied with electric water reduction and oxidation: complex [CuMe2(oxpn)Cu(OH)2] 5 processed both water reduction and oxidation, TOF is 654 h-1(pH 7.0) of hydrogen evolution, TOF is 2.56 s-1(pH 10.4) of oxygen evolution.Forth, two new complex was studied with elctrocatalytic and photo-catalytic properties: complex [Co2(La)4] 1, complex [Lb CoCl] 2 processed both elctrocatalytic and photo-catalytic properties, TOF is 223 h-1(pH 7.0), 162 h-1(pH 7.0) of electrocatalyst, TON is 4360, 4125 of photocatalyst.Fifth, primary studies of catalytic mechanisms were proposed.
Keywords/Search Tags:complexes, molecular catalysts, water reduction and oxidation, elctrocatalytic and photo-catalytic hydrogen evolution
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