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Degradation And Mechanism Of Typical Chlorinated Hydrocarbons Under Ultraviolet Irradiation

Posted on:2019-03-19Degree:DoctorType:Dissertation
Country:ChinaCandidate:W LiuFull Text:PDF
GTID:1311330542964980Subject:Environmental Science and Engineering
Abstract/Summary:PDF Full Text Request
As the important raw materials and solvents,chlorinated hydrocarbons are widely used in industry.Due to their great adverse effect on human health,efficient technologies for chlorinated hydrocarbons removal are urgent.In the present study,firstly,the photocatalytic degradation of C2HCl3 was carried out.Then photochemical reduction technology was utilized to decompose CCl4 and CHCl3,which possess strong recalcitrance to oxidation.C2HCl3,CCl4 and CHCl3 were degraded well and the main results are as follows.?1?Due to the higher migration ability of h+and e-,BiOCl-0.6 showed better photocatalytic performance than BiOCl-6.0 for C2HCl3 degradation under the irradiation of medium-pressure UV mercury lamp?UV?.The degradation rate descended with increasing pH and C2HCl3 concentration.Impurities such as SO42-,NO3-and NOM exerted adverse effects on C2HCl3 degradation except Cl-.The generation of·OH and O2·-in UV-BiOCl system was detected by ESR.Both·OH,O2·-and h+contributed to the degradation and C2HCl3?30 mg/L?was almost completely decomposed and dechlorinated in 120 minutes.?2?UV-BiOCl system was unable to decompose CCl4,however,CCl4?5 mg/L?was rapidly degraded with a removal efficiency of around 98.0%in 40 minutes when CH3CH2OH or HCOONa was added.The degradation of CCl4 was inhibited in aqueous solution with elevated pH and groundwater.BothCH3 C HOH and O2·-were involved in the degradation of CCl4 in UV-BiOCl-CH3CH2OH system and the lag phase was caused by the quenching effect of O2 toCH3 C HOH.CO2·-was the main specie that caused CCl4 degradation in UV-BiOCl-HCOONa system.The main product was CHCl3 with dechlorination efficiency of about 40.0%.?3?In UV254?the low-pressure UV mercury lamp with a maximum emission at254 nm?-Na2SO3 system,the elevated Na2SO3 concentration and pH accelerated the degradation of CCl4,while O2 and impurities inhibited the reaction.The removal efficiency of CCl4 was 31.7%in groundwater with other condition constant.The quenching experiment indicated that e-aq induced the degradation of CCl4.CCl4?10mg/L?was almost completely degraded and dechlorinated within 60 minutes with the generation of CHCl3,C2Cl4 and C2HCl3 during degradation process.Additionally,the removal efficiencies of 5 mg/L CHCl3 and CH2Cl2 in UV254-Na2SO3 system achieved 97.9%in 30 minutes.?4?The degradation rate of CHCl3 in UV254-Na2S system enhanced with increasing Na2S concentration and then slowed down.The high rate was observed at elevated initial pH and the removal efficiency of CHCl3 in groundwater was around1/3 folds that in deionized water.The degradation of CHCl3 was mainly caused by e-aq.The rate constant between e-aq and CHCl3 was determined to be 6.5×109 L/?mol·s?by competition kinetics.CHCl3?10 mg/L?was almost completely decomposed and dechlorinated within 60 minutes.The main intermediates were CH2Cl2 and cis-1,2-C2H2Cl2.
Keywords/Search Tags:photocatalytic, photochemical reduction, degradation, chlorinated hydrocarbons, mechanism
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