Study On Properties And Analysis Of Environmental Pollutants Polybrominated Diphenyl Ethers And Its Metabolites

Persistent organic pollutants,polybrominated diphenyl ethers(PBDEs),are brominated flame retardants,it have been widely added to industrial products and daily necessities.Because of its mass production and widespread use,PBDEs had a tremendous impact on the environment,food,and human health.This paper aims to establish a modern analysis method for the quantitative detection of PBDEs and their derivatives;explore the interaction between PBDEs and their derivatives and biomolecules,and study the degradate technology of PBDEs in water and soil.The paper is divided into four parts:In part one,the basic properties of PBDEs and their derivatives as well as their pollution in the environment and organisms are described in detail.The current progress in the research on toxicology,pretreatment techniques,detection and analysis methods,and degradation technologies are outlined.At the same time,the research purpose and main research contents of this paper are briefly described.In part two,combined novel pretreatment materials with chromatography-mass spectrometry techniques,we established three methods for the quantitative analysis of PBDEs and their derivatives in the environment and food.This part mainly includes the following three chapters:1)Two-dimensional sheet material cobalt oxyhydroxide were used as a dispersive solid-phase extraction material to extract PBDEs in water samples,gas chromatography was used for analysis and detection,external standard method was used for quantitative analysis.2)A solid phase extraction cartridge was prepared by using a carbon nitride nanosheet(g-C3N4)as a filler to purify algae extracts.The purified liquid was analyzed by gas chromatography and external standard method was used for quantitative analysis.3)Using ultrasonic-assisted extraction technology to extract OH-PBDEs in shellfish samples,QuEChERS EMR-Lipid was used to purify the extract and LC/MS/MS was used to separate and detect the target.In part three,the interaction between PBDEs and three biomolecules were studied via fluorescence spectroscopy.The main three chapters were as follows:1)4-OH-BDE-42 is taken as a representative to study the interaction between PBDEs and human serum albumin(HSA).The binding constants,binding sites,binding sites number,and binding modes of PBDEs-HSA was obtained by fluorescence spetral method.The effect of interaction on the conformation and physiological functions of HSA were also investigated.2)Fluorescence spectroscopy was employed to study the interaction of hydroxypolybrominated diphenyl ethers(OH-PBDEs)with protein disulfide isomerases(PDI)by using isothiocyanate fluorescence-triiodothyronine(F-T3)as a probe molecule.3)The interaction between PBDE-QS and glutathione(GSH)was studied using DNA-AgNCs.as fluorescent probes.Mass spectrometry was used to study the mechanism and the structure and stability of PBDE-Qs binding with GSH.Part four was divided into two chapters.Nano-zero-valent iron immobilizilized in carbon nitride nanosheets(nZVI@C3N4)was prepared and ultilized to remove decabromodiphenyl ether(DBDE)from water and soil,respectively.The effect of nZVI@C3N4 amount,DBDE initial concentration,solution pH and temperature on the debromination efficiency werer investigated.The results indicated that the degradation rate of DBDE increased with increasing the amount of nZVI@C3N4,DBDE initial concentration,solution pH and temperature within a certain scope.