Study Of The Fabrication Of MOF-Derived FeCu-C Cathode And Degradarion Of CAZ With Electro-Fentone

Electro-Fenton technology(EF)has been used widely to remove antibiotic pollutants due to the in-situ generation of H2O2,however,the narrow applicable scope of pH(2.8～3.5)and the production of iron sludge limit its further development.Meantime,cathode is the one of important factors of EF process,the selection of cathode plays an important role in the application of EF.MOFderived materials,obtained by carbonization,have been used for broadening the applied range of EF due to the intriguing features such as rich active sites,high electricity and excellent structural stability.In this study,MOFs was used a precursor to prepare nitrogen doped iron/copper porous carbon modified cathode(FeCu-CT),The property of catalysts were characterized.In addition,the study about the degradation of CAZ in hetero-EF technology with FeCu-CT cathode was concluded,and the degradation mechanisms were analyzed to supply a reference for the degradation of ceftazidime(CAZ)with MOF-derived cathode.The main experimental results as follows:1.FeCu-CT was successfully prepared through carbonizing Cu copper FeNH2-BDC precursor,and the effects of carbonization conditions and double metal doping on the physi-chemical characteristics and electrochemical property of FeCu-CT were investigated.Compared with other materials,FeCuC400Ar had a spindle-shaped structure,which is similar to the that of precursor.Argon promoted the formation of graphite N,surface oxygen(Osur)and Fe304.Furthermore,FeCu-C400Ar had the smallest lattice size(21.2 nm),the biggest electrochemical active surface(0.4083 cm2)and the largest corrosion potential(-181～-191mV),and the introduction of copper increased the material electricity;The pathway of ORR on the FeCu-C400Ar/CB composite cathode was dominated by 2 electrons,and the electron transfer number was 2.09～2.27.2.In the hetero-EF system,there was an excellent CAZ removal merely in acidic condition(pH=3)for the FeCu-C650Ar/CB cathode.However,FeCuC400Ar/CB cathode had a wide pH range(3～9)for the efficient degradation of CAZ,the removal process was in accord with the 1st order reaction kinetics,and the CAZ degradation rate achieved 98%in 60 min.Meantime,the lower metal leaching and repeated experiment showed the good stability of the FeCuC400Ar/CB cathode.3.In the hetero-EF system,the main active species was hydroxyl radical(·OH)by the analysis of fluorescence spectrum,EPR and radical quenching.The dissolved oxygen gained 2 electrons to produce H2O2 on the surface of the FeCu-C400Ar/CB cathode,and OH was generated by the reaction between with H2O2 and FeⅡ/CuⅠ.The recycle generation of FeⅡ/CuⅠ occurred on the cathode surface by the reduction of FeⅢ/CuⅡ,and the complexation of CuⅡcontributed to the efficient degradation of CAZ for the FeCu-C400Ar/CB cathode.4.FTIR,UV-vis and HPLC-MS were applied to investigated the intermediate products and degradation pathway of CAZ.The removal pathway in the hetero-EF system was speculated,the main degradation pathways included S atom oxidation of thiazine ring,fracture of pyridine ring and rid of thiazole ring.