Design,Synthesis And Studies Of Cobalt,Iron Complexes With Electrocatalytic Water Splitting Properties

With the rapid development, the demand for energy increasing.However, fossil energy is limited, the development of renewable energy becomes imminent. The hydrogen is becoming a hot study spot of today’s scientists due to its advantages.In nature, microbes meet its energy needs via hydrogenase catalytic pyrolysis water to generate hydrogen, but the biological environment is simulated. The revelation opened the prelude to scientist research on molecular catalyst.This work is devoted to designing ligand and assembing complexes with different transition metel, looking for new catalyst for cracking water.This paper including:1) Explore different substituents which effect on the properties of complexes electric catalytic hydrogen production, this paper design and synthesis two similar ligand 2-pyridine amino-N,N-2（2-methyl-4, 6-dimethyl phenol）（H₂L_A） and 2-pyridine amino-N,N-2（2-methyl-4, 6-dichlorophenol）（H₂L_B）, and synthesis complexes[Co^â…¢₂L_ACl₂] 1 å’Œ[Co^â…¢₂L_BCl₂] 2 by the two ligands.Electric catalytic performance, measured TOF under the two complexes in p H 7.0（turnover frequency） values were 457.4（1）,454.6 h-1（2）, show that ligand substituent effect on the properties of complexes electric catalytic hydrogen production is not obvious.2) Explore different center metal which effect on the properties of complexes electriccatalytic hydrogen production, this paper synthesis two different complexes [Co^â…¢₂L_ACl₂] 1 å’Œ [Fe^â…¢₂L_A（HO）₂] 3 by the ligand 2-pyridine amino-N,N-2（2-methyl-4,6-dimethyl phenol）（H₂L_A）.Electric catalytic performance, measured TOF under the two complexes in p H 7.0（turnover frequency） values were 457.4（1）,1076 h-1（3）, shows when H₂L_A as ligand, the electric catalytic hydrogen production performance of complex 3 is better than complex 1.3) There are two possibilities of catalyzed hydrogen activation point for the complexes, one kind of activation point at the metal, another one at N atoms.In this paper, for vertify the attitude, design and synthesis two ligands 2,6-2 amino-3-[（2-methoxy）benzene azo group] pyridine（H₂LC）, 1-[2-carboxy methyl phenyl]-3-（2-pyridine） three nitrogen（HLD）, and synthesis two complexes[Co^â…¡₂LCCl₃]Cl 4, [Co^â…¢L_D3] 5 by the two ligands.Two complexes have good electric catalytic hydrogen production performance, at p H 7.0 TOF（turnover frequency） value 1332（4）, 1990 h- 1（5）.Complex 5 may well prove N atom also can be used as catalytic activation point.4) In this paper, complex [Co^â…¡A₂（H₂O）₂] 6（A: picolinate ion） which structure is simple was synthesised, found that the complex also has electric catalytic hydrogen production performance, at p H 7.0 TOF（turnover frequency） value were 722.1 h-1（6）.