Study On Activation Persulfate Degradation Of Organic Pollutants By ZIFs Derived Carbon Skeleton Materials

In recent years,more and more attention has been paid to the research on water quality safety at home and abroad.In fact,water containing organic pollutants is a kind of wastewater pollutant with unusually complex composition,which may seriously threaten the urban water environment safety in China.Tetracycline antibiotics are widely used in China’s pharmaceutical industry and aquaculture industry.Tetracycline content in water is relatively high,and due to its solubility,stability and difficulty in degradation,tetracycline will cause harm to human health through drinking water and biological chain.Therefore,the development of low-cost,high-efficiency degradation of organic matter technology is extremely urgent.In this paper,at the same time in the preparation of materials dissolved into a transition metal to metal nodes and rich in MOFs materials of N elements（M-ZIFs）,formed by carbonization technology in high pressure under the action of carbon materials,then calcined under N2 protection in the process of the carbon materials doped N elements,the resulting a N doped carbon containing transition metal catalytic materials（M-N-C）,through a series of characterization methods for the analysis of microstructure and macro properties of catalysts,and by using the M-N-C activation persulfate degradation of organic matter,study different material effect on the degradation of organic matter,get the following results and conclusions:1.Study on activation of perosulfate to degradation of organic pollutants by Fe-N-C Materials.Preparation of a Fe,N co-doped mesoporous material Fe-N-C,by simple hydrothermal method and coprecipitation method Characterization results show that Fe,N heteroatoms are successfully doped into carbon materials,High crystallinity,dodecahedral shape in a regular shape,The contents of Fe,N and C were 21.6%,3.9%and 75.5%,respectively;The material has good catalytic performance,0.4 g/L,in catalyst dosage Initial concentration of tetracycline mg/L,40 PS concentration g/L,0.04 At 7 p H,the degradation rate of tetracycline was 86.8%,The existence of C₂O₄^2-and CO₃^2-degradation effect interference;According to the free radical quenching experiment,Active oxidizing substances that play a leading role in the whole degradation system are O₂^-·radicals,There are a small amount of SO₄^-·and OH·free radicals;Meanwhile,Fe-N-C showed good stability,The degradation rate of tetracycline was 72.8%after 4 cycles;The degradation effect of ciprofloxacin hydrochloride,methylene blue and chloroquine phosphate is still good,65%,99%and 70%,respectively..2.Study on activation of perosulfate to degradation of organic pollutants by Fe Cu-N-C Materials.Based on Fe-N-C materials,Fe Cu-N-C,of mesoporous catalytic materials Fe,Cu bimetallic doped N by introducing appropriate copper ions The characterization results show that the materials have a regular arrangement of polyhedron structure,High crystallinity,The Fe,Cu,N and C elements are uniformly distributed on the surface of the material,The contents of each element were 0.1%,0.2%,1.6%and 98.1%respectively;The catalytic performance of the material is strong,0.4 g/L,in catalyst dosage Initial concentration of tetracycline mg/L,40 PS concentration g/L,0.08 At p H 8,the degradation rate of tetracycline was 90.5%,C₂O₄^2-and CO₃^2-have more inhibitory effect on degradation effect;In the catalytic degradation of tetracycline,Active oxidizing substances in the whole system are O₂^-·free radicals;Meanwhile,Fe Cu-N-C after four cycles,the degradation rate of tetracycline was still 70.5%,showing good stability;The degradation effect of ciprofloxacin hydrochloride,methylene blue and chloroquine phosphate is still good,67%,98%and 75%,respectively.3.Study on activation of perosulfate to degradation of organic pollutants by FeCuCo-N-C Materials.In the preparation of materials and the introduction of appropriate amount of transition metal ions,Preparation of a Mesoporous Catalytic Material Fe、Cu、Co Polymetallic Doped N The characterization results show that the materials are arranged in clusters,The contents of Fe,Cu,Co,N and C were 0.1%,0.3%,0.2%,1.4%and 97.8%respectively;Before and after degradation,XRD characteristic peaks decreased,may be due to the reaction is residue or intermediate product occupied the active site;The material has excellent catalytic performance,0.4 g/L,in catalyst dosage Initial concentration of tetracycline mg/L,40 PS concentration g/L,0.08 At p H time,the degradation rate of tetracycline was 99.1%,The presence of C₂O₄^2-and CO₃^2-inhibited the degradation of tetracycline;According to the free radical quenching experiment,Active oxidizing substances that play a leading role in the whole degradation system are O₂^-·radicals,There are a small amount of SO₄^-·and OH·free radicals;Meanwhile,FeCuCo-N-C showed good stability,The degradation rate of tetracycline was 75.3%after 4 cycles;The degradation effect of ciprofloxacin hydrochloride,methylene blue and chloroquine phosphate is still good.The Fe-N-C、Fe Cu-N-C and FeCuCo-N-C of ZIFs derived carbon skeleton materials showed good catalytic activity in the experiment of activating persulfate to degrade organic pollutants,the degradation effect of Fe Cu-N-C and FeCuCo-N-C on organic pollutants is stronger than that of Fe-N-C,it can be seen that polymetallic doped activity efficiently,70%,99% and 80%,respectively.