Preparation Of Graphene-like Materials Doped Catalytic Particle Electrode And Study On The Efficiency Of Three-dimensional-Electro-Fenton In Treating Antiviral

New pollutants,PPCPs,have received more and more attention because of their potential threats to organisms and human health.PPCPs and their metabolites have adverse effects on the non-target organs of other organisms in human body or ecosystem.Long-term existence in the environment may lead to unprecedented serious consequences.However,the existing wastewater treatment process can not completely degrade it,and it is necessary to seek a new and efficient process to remove PPCP in the environment.The three-dimensional-electric Fenton process has attracted much attention due to its green,efficient and controllable characteristics.The catalytic particle electrode is the key to the process,but the existing catalytic particle electrode still has defects in corrosion resistance,specific surface area,cost and stability.It is necessary to study and prepare a new type of particle electrode.This thesis uses montmorillonite as carrier,graphene-like materials to improve conductivity,and iron as a catalytically active component.Two catalytic particle electrodes are prepared:MMT/rGO/Fe₃O₄ and MMT/GH/Fe₃O₄.They will be used in the three-dimensional-electric Fenton system to degrade antiviral drugs（acyclovir and arbidol）,and explore the influence of various factors in the degradation process and the influence of different particle electrodes on the system.The stability and superiority of the catalytic particle electrode and the degradation mechanism of acyclovir and arbidol were also studied.The specific research content is as follows:（1）The MMT/rGO/Fe₃O₄ catalytic particle electrode was prepared by using ethylene glycol as solvent and loading by hydrothermal method.The morphology,structure and composition were analyzed by SEM、BET、FT-IR、XRD、Raman and other characterization methods.After loading and hybrid reaction,its specific surface area increased.The characteristic peak of grapheme oxide appeared first and then disappeared,indicating that the graphene oxide was reduced during the preparation process.And the characteristic peak of Fe₃O₄ appeared,which proved the existence of Fe₃O₄ in the catalyst.With acyclovir and arbidol as the target pollutants,the effect of various operating conditions in the three-dimensional-electric Fenton system on the catalytic performance was studied.The results show that the applicable p H si very wide.The degradation rate of Acyclovir can reach 100%in 120 min under the optimal degradation conditions,and the degradation rate of Arbidol can reach 100%in 2 min under the optimal degradation conditions.At the same time,the stability of the catalytic particle electrode was investigated and the degradation rate under different catalytic particle electrodes and different reaction systems was compared.The results showed that the degradation rate can still reach more than 90%after ten cycles of the catalytic rate.Compared with other particle electrodes,the catalytic performance of MMT/rGO/Fe₃O₄ particle electrode is the best.Compared with different reaction systems,the three-dimensional electrode process and the electric Fenton method have a synergistic effect,and the degradation efficiency is greatly improved.（2）Using ethylene glycol as solvent,natural clay montmorillonite as hard template,sucrose as carbon source,assembling and synthesizing dopant materials with graphene-like morphology.MMT/GH/Fe₃O₄ catalytic particle electrode is prepard after granulating and debinding.The morphology,structure and composition were analyzed by SEM,BET,FT-IR,XRD and other characterization methods.After loading and hybridization reaction,the specific surface area increases,The characteristic peaks of graphene and Fe₃O₄ appear which proves that the catalyst has the structure of graphene-like and the presence of Fe₃O₄.Taking acyclovir and arbidol as the target pollutants,the effect of various operating conditions in the three-dimensional-electric Fenton system on the catalytic performance was studied,which showed that the catalytic particle electrode can be applied to a wide range of p H so that can be applied to various types of water bodies.The degradation rate of acyclovir can reach 97%in 120 minutes under the optimal degradation conditions,and the degradation rate of Arbidol can reach 100%in 6 minutes under the optimal degradation conditions.At the same time,the stability of the catalytic particle electrode and the degradation rate of different catalytic particle electrodes and different reaction systems were investigated.The results show that the degradation rate can still reach more than 90%after ten cycles of the catalytic rate,MMT/GH/Compared with other particle electrodes,the catalytic performance of Fe3O4 catalytic particle electrode has the best performance.Compared with different reaction systems,the three-dimensional electrode process and the electric Fenton method have a synergistic effect,and the degradation efficiency is greatly improved.（3）The mechanism of MMT/rGO/Fe₃O₄ and MMT/GH/Fe₃O₄ degradation with acyclovir and arbidol was studied.The content of active oxygen species in the system was measured by using quencher anhydrous methanol and capture agent salicylic acid.The results show that the contribution rate of hydroxyl radicals in the system to the degradation of pollutants was about 40%.The intermediate products of acyclovir and arbidol degraded by the catalytic particle electrode were measured and analyzed,and the possible degradation pathways were deduced.