Reduction of Decabrominated Diphenyl Ether by Nanoscale Zero-valent Iron

碩士 === 中興大學 === 土壤環境科學系所 === 94 === Polybrominated diphenyl ethers (PBDEs) are widely used as flame retardants in inflammables to ensure the life and property safety by decreasing the risk of fire accidents. PBDEs have been detected in human, wildlife, marine, and freshwater sediments. PBDEs become...

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Main Authors: Yu-Tsung Tai, 戴侑宗
Other Authors: 施養信
Format: Others
Language:zh-TW
Published: 2006
Online Access:http://ndltd.ncl.edu.tw/handle/48297731697890544816
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spelling ndltd-TW-094NCHU50200122015-10-13T16:41:01Z http://ndltd.ncl.edu.tw/handle/48297731697890544816 Reduction of Decabrominated Diphenyl Ether by Nanoscale Zero-valent Iron 奈米零價鐵還原降解十溴聯苯醚之研究 Yu-Tsung Tai 戴侑宗 碩士 中興大學 土壤環境科學系所 94 Polybrominated diphenyl ethers (PBDEs) are widely used as flame retardants in inflammables to ensure the life and property safety by decreasing the risk of fire accidents. PBDEs have been detected in human, wildlife, marine, and freshwater sediments. PBDEs become important environmental organic pollutants but the degradation studies of PBDEs in the environment are still limited. In this study, the chemical debromination of DBDE (Decabrominated diphenyl ether) by zero-valent iron (ZVI) was studied. A scanning electron microscopy and a photon correlation spectroscopy were performed to characterize the surface properties and particle size of nanoscale ZVI, respectively. The nanoscale ZVI existed as spherical particles averaging 20~50 nm in diameter and its surface area was 52.0 m2/g. Within 40 minutes over 80 % of DBDE was transformed into lower bromo congeners by nanoscale ZVI under ambient conditions. During the initial reaction period (< 20 minutes), nonabromo BDEs were the most abundant products but hexa to heptabromo congeners were dominant after 130 minutes. The effects of particle sizes of zero-valent iron, temperature (5, 25, and 45 ℃), pH value (5, 7, 8, and 10), and the existence of inorganic anions (Cl-, HCO3-, and H2PO4-) and cations (Na+, Cu2+, and Fe3+) in solutions on the dehalogenation were evaluated. For nanoscale ZVI, the pseudo-first-order DBDE debromination rate constant (0.0583 min-1) was significantly faster than that of microscale ZVI (0.0077 min-1) due to the higher surface area and reactivity of nanoscale iron particles. The debromination rate constants of DBDE increased with the decreasing of aqueous pH values and with the increase of temperature. For anions, a high concentration of chloride ions enhanced the debromination of DBDE, whereas phosphate and carbonate ions hindered the debromination process. The cation species also affected the reduction reaction by ZVI except Na+. The debromination rate constants of DBDE increased in the presence of Cu2+ and decreased in the presence of Fe3+. Lugang and Longgang soil solutions and Lugang and Longgang soils were chose as soil systems to evaluate the debromination rate of DBDE by nanoscale ZVI. The reduction rates of DBDE by nanoscale ZVI in soil solutions and soils were slower than those in pure water. Comparing the reaction rates between Longgang and Lugang soils, the reduction rate of DBDE in Longgang soil was faster than that in Lugang soil probably due to the lower pH of Loggang soil. The debromination pathway of DBDE by nanoscale ZVI was proposed via the analysis of byproducts. Nanoscale ZVI has the high potential values to remediate PBDEs in the environment. 施養信 2006 學位論文 ; thesis 90 zh-TW
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description 碩士 === 中興大學 === 土壤環境科學系所 === 94 === Polybrominated diphenyl ethers (PBDEs) are widely used as flame retardants in inflammables to ensure the life and property safety by decreasing the risk of fire accidents. PBDEs have been detected in human, wildlife, marine, and freshwater sediments. PBDEs become important environmental organic pollutants but the degradation studies of PBDEs in the environment are still limited. In this study, the chemical debromination of DBDE (Decabrominated diphenyl ether) by zero-valent iron (ZVI) was studied. A scanning electron microscopy and a photon correlation spectroscopy were performed to characterize the surface properties and particle size of nanoscale ZVI, respectively. The nanoscale ZVI existed as spherical particles averaging 20~50 nm in diameter and its surface area was 52.0 m2/g. Within 40 minutes over 80 % of DBDE was transformed into lower bromo congeners by nanoscale ZVI under ambient conditions. During the initial reaction period (< 20 minutes), nonabromo BDEs were the most abundant products but hexa to heptabromo congeners were dominant after 130 minutes. The effects of particle sizes of zero-valent iron, temperature (5, 25, and 45 ℃), pH value (5, 7, 8, and 10), and the existence of inorganic anions (Cl-, HCO3-, and H2PO4-) and cations (Na+, Cu2+, and Fe3+) in solutions on the dehalogenation were evaluated. For nanoscale ZVI, the pseudo-first-order DBDE debromination rate constant (0.0583 min-1) was significantly faster than that of microscale ZVI (0.0077 min-1) due to the higher surface area and reactivity of nanoscale iron particles. The debromination rate constants of DBDE increased with the decreasing of aqueous pH values and with the increase of temperature. For anions, a high concentration of chloride ions enhanced the debromination of DBDE, whereas phosphate and carbonate ions hindered the debromination process. The cation species also affected the reduction reaction by ZVI except Na+. The debromination rate constants of DBDE increased in the presence of Cu2+ and decreased in the presence of Fe3+. Lugang and Longgang soil solutions and Lugang and Longgang soils were chose as soil systems to evaluate the debromination rate of DBDE by nanoscale ZVI. The reduction rates of DBDE by nanoscale ZVI in soil solutions and soils were slower than those in pure water. Comparing the reaction rates between Longgang and Lugang soils, the reduction rate of DBDE in Longgang soil was faster than that in Lugang soil probably due to the lower pH of Loggang soil. The debromination pathway of DBDE by nanoscale ZVI was proposed via the analysis of byproducts. Nanoscale ZVI has the high potential values to remediate PBDEs in the environment.
author2 施養信
author_facet 施養信
Yu-Tsung Tai
戴侑宗
author Yu-Tsung Tai
戴侑宗
spellingShingle Yu-Tsung Tai
戴侑宗
Reduction of Decabrominated Diphenyl Ether by Nanoscale Zero-valent Iron
author_sort Yu-Tsung Tai
title Reduction of Decabrominated Diphenyl Ether by Nanoscale Zero-valent Iron
title_short Reduction of Decabrominated Diphenyl Ether by Nanoscale Zero-valent Iron
title_full Reduction of Decabrominated Diphenyl Ether by Nanoscale Zero-valent Iron
title_fullStr Reduction of Decabrominated Diphenyl Ether by Nanoscale Zero-valent Iron
title_full_unstemmed Reduction of Decabrominated Diphenyl Ether by Nanoscale Zero-valent Iron
title_sort reduction of decabrominated diphenyl ether by nanoscale zero-valent iron
publishDate 2006
url http://ndltd.ncl.edu.tw/handle/48297731697890544816
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