Synthesis Of Metal Copper And Cobalt Complexes And Their Electrocatalytic Hydrogen Production And Oxygen Production Properties

Human are facing major problems that over-exploitated and deterriorated the fossil energy,as a renewable resource,in the sustainable development of the contemporary society.One of the practical and promising technologies is to electrocatalytic water splitting into hydrogen.This process could be divided into two half reactions,namely oxidizing water and reducting water dedcomposition.Therefore,suitable for water splitting catalysts attract considering attention.In this dissertation,two kinds of Cu???and Co???mononuclear complex catalysts were prepared by using commercial or facilely prepared ligands.The electrocatalytic properties for water splitting were investigated,some interesting results were obtained as following:1.A self-assembly new-style copper???complex: [Cu?BHEED??H₂O?₂]SO4]?BHEED=N,N'-double?2-hydroxyethyl?ethylenediamine?,has already been simbly synthesized in deionized water.Its structure was determined by mass spectrometry and X-ray single crystal diffraction analysis,and the performance of electrocatalytic hydrogen evolution for the complex in 0.1M,pH=12.4 phosphate buffer solution was carried out.The over potential of 387 m V?1.1V vs.NHE?was observed,which is the lowest compared with those reported,and the catalytic current is equal 6 m A/cm².In the process of electrocatalysis,we found that the working electrode was coated with in situ brown film.The film was confirmed to be Cu₂O by electrochemical workstation?CHI-660E?test,SEM,EDX,XRD,and XPS analysis,and exhibits a high electrocatalytic activity in the same condition,the catalytic current is 3.5m A/cm²,over potential is 147 m V.2.Using the same catalyst [Cu?BHEED??H₂O?₂]SO4]?BHEED=N,N'-double?2-hydroxyethyl?ethylenediamine?,in the 0.1mol/L,SABS solution at the pH =12.4,a black film was formed at 1.35V?vs.NHE?.By electrochemical workstation?CHI-660E?test,SEM,EDX,XRD,and XPS analysis,formation of Cu O film was confirmed.Under the same condition,the catalytic current is 4.3m A/cm²,the Faradaic efficiency value is 100%.3.Cobalt porphyrin compounds with diethyl phosphate as axial ligands were synthesized and characterized by X-ray diffraction.The complex was coated as thin film on the ITO working electrode.which has efficiently activities in phosphate buffer solution at pH=9.24.The working electrode was investigated before and after electrocatalysis by ESI-MS,UV spectrum,SEM and EDX analysis,the result showed that it is a molecular catalyst,the catalytic current is 2 m A/cm²,and the Faradaic efficiency is 95.6%.