Generation Of High-valent Metal-oxo Species In Ligand-Modulated Catalytic System For Oxidizing Organic Pollutants

As an indispensable material in human life,the water in human tissue is accounted for 60 to 70 percent of body weight.And it is also accounted for more than five percent in other animals or plants,shows that water is an essential material.In addition,water is also a necessary condition for national economic development,because it is demanded in business activities,industrial development,agricultural operations,water development and the aquaculture.However,with the rapid development,the water pollution problem has become an increasingly prominent problem,mainly from in the process of production of some toxic organic pollutants,for instance,dyes,pesticides and antibiotics,causing serious environmental harm.These pollutants are complex and high chemical oxygen demanded,and they are difficult to be degraded by the traditional biological and physical methods.The pollutants can be degraded into small-molecule matters or be complete mineralization by the advanced oxidation technology(AOPs)in the process of generating strong oxidizing species.From the point of view of atom economy and environment friendliness,it is very important to use hydrogen peroxide as the oxidizing agent because it is green,non-pollution chemical agent.The non-toxic metal ion copper and iron are used as active centers,which are meaningful in the cheap and large-scale synthesis of catalyst.In this work,we designed and synthesized a series of coordination compounds,which generating high-valent metal-oxygen species.This series of complexes catalyzed the oxidation of dyes and antibiotics with high selectivity and high selectivity.The results showed that the effect of 4-aminopyridine in the reactions and the difference of catalytic activities of different metal-catalyzed species.This paper includes the following aspects: Firstly,the homogeneous catalytic system IDA/Cu(?)/4-ampy was synthesized and its catalytic activity and reaction mechanism were investigated.Homogeneous catalysts have attracted much attention because of their high catalytic activity and they can be widely used in the degradation of organic pollutants.However,the homogeneous catalysts are difficult to be recycled and may generate a new pollution.The problem can be solved by the use of carrier materials.The ion-exchange resin-chlorine sphere(PS)has an excellent chemical stability and a good adsorption property after being modified,it can be used as the carrier of catalyst and it can promote the enrichment of organic contaminants in the solution.Secondly,a supported catalyst was prepared by loading a homogeneous catalyst onto PS,and the catalytic activities were studied.Lastly,PS-IDA/Fe(?)/4-ampy was synthesized by the change of the active centre metal.The catalytic activity and reaction mechanism were investigated.A series of characterization experiments were also carried out.The experiment results showed that 4-aminopyridine had a great effect on the catalytic activity,and all the catalytic systems showed high catalytic efficiency.The results of EPR tests showed that all the systems were not the ·OH reaction mechanism,and the possible mechanism was that high-valent metal-oxygen species were produced.