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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
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dc.contributor.advisor | 林郁真 | |
dc.contributor.author | Wei-Chieh Chang | en |
dc.contributor.author | 張瑋潔 | zh_TW |
dc.date.accessioned | 2021-05-20T20:51:55Z | - |
dc.date.available | 2014-01-01 | |
dc.date.available | 2021-05-20T20:51:55Z | - |
dc.date.copyright | 2011-08-12 | |
dc.date.issued | 2011 | |
dc.date.submitted | 2011-08-06 | |
dc.identifier.citation | A.Gulkowska, Yuhe He, M.K. So, Leo W.Y. Yeung, H.W. Leung, J.P. Giesy, Paul K.S. Lam , Michael Martin, Bruce J. Richardson, 2007. The occurrence of selected antibiotics in Hong Kong coastal waters. Marine Pollution Bulletin 54, 1287-1306.
Antibiotics, N., 2006. National Antibiotics Usage Survey Project Department of Health. in: Yuan, E. (Ed.), Taiwan. Balistrieri, L.S., Murray, J.W., 1982. The surface chemistry of [delta]MnO2 in major ion sea water. Geochimica et Cosmochimica Acta 46, 1041-1052. Balistrieri, L.S., Murray, J.W., 1987. The influence of the major ions of seawater on the adsorption of simple organic acids by goethite. Geochimica et Cosmochimica Acta 51, 1151-1160. Barrett, K.A., McBride, M.B., 2005. Oxidative Degradation of Glyphosate and Aminomethylphosphonate by Manganese Oxide. Environmental Science & Technology 39, 9223-9228. Brenda Crompton, M.J., Kathleen Crawford, G. G. F. Newton, and E. P. Abraham 1962. Behaviour of some derivatives of 7-aminocephalosporanic acid and 6-aminopenicillanic acid as substrates, inhibitors and inducers of penicillinases. Biochem. J. 83, 52-63. Cha, J.M., Yang, S., Carlson, K.H., 2006. Trace determination of [beta]-lactam antibiotics in surface water and urban wastewater using liquid chromatography combined with electrospray tandem mass spectrometry. Journal of Chromatography A 1115, 46-57. Chen, W.-R., Huang, C.-H., 2011. Transformation kinetics and pathways of tetracycline antibiotics with manganese oxide. Environmental Pollution 159, 1092-1100. Cherry, D.S., Currie, R.J., Soucek, D.J., Latimer, H.A., Trent, G.C., 2001. An integrative assessment of a watershed impacted by abandoned mined land discharges. Environmental Pollution 111, 377-388. Daryl D. DePestel , Michael S. Benninger , Larry Danziger , Kerry L. LaPlante , Chandler May , Allan Luskin , Michael Pichichero , Hadley, J.A., 2008. Cephalosporin use in treatment of patients with penicillin allergies. Journal of the American Pharmacists Association 48, 530-540. Davis, J.L., Salmon, J.H., Papich, M.G., 2005. Pharmacokinetics and tissue fluid distribution of cephalexin in the horse after oral and i.v. administration. Journal of Veterinary Pharmacology and Therapeutics 28, 425-431. Demain, A.L., Elander, R.P., 1999. The β-lactam antibiotics: past, present, and future. Antonie van Leeuwenhoek 75, 5-19. Filipek, L.H., Nordstrom, D.K., Ficklin, W.H., 1987. Interaction of acid mine drainage with waters and sediments of West Squaw Creek in the West Shasta Mining District, California. Environmental Science & Technology 21, 388-396. Gáspár, A., Andrási, M., Kardos, S., 2002. Application of capillary zone electrophoresis to the analysis and to a stability study of cephalosporins. Journal of Chromatography B 775, 239-246. Indelicato, J.M., Norvilas, T.T., Pfeiffer, R.R., Wheeler, W.J., Wilham, W.L., 1974. Substituent effects upon the base hydrolysis of penicillins and cephalosporins. Competitive intramolecular nucleophilic amino attack in cephalosporins. Journal of Medicinal Chemistry 17, 523-527. Jaudon, P., Massiani, C., Galea, J., Rey, J., Vacelet, E., 1989. Groundwater pollution by manganese. Manganese speciation: Application to the selection and discussion of an in situ groundwater treatment. Science of The Total Environment 84, 169-183. Kelkar, P.S., Li, J.T.C., 2001. Cephalosporin Allergy. New England Journal of Medicine 345, 804-809. Klausen, J., Haderlein, S.B., Schwarzenbach, R.P., 1997. Oxidation of Substituted Anilines by Aqueous MnO2: Effect of Co-Solutes on Initial and Quasi-Steady-State Kinetics. Environmental Science & Technology 31, 2642-2649. Krauskopf, K.B. (Ed.), 1967. Introduction to Geochemistry. McGraw-Hill, New York. Kummert, R., Stumm, W., 1980. The surface complexation of organic acids on hydrous [gamma]-Al2O3. Journal of Colloid and Interface Science 75, 373-385. Laha, S., Luthy, R.G., 1990. Oxidation of aniline and other primary aromatic amines by manganese dioxide. Environmental Science & Technology 24, 363-373. Lai, Y.-C., 2003. Geochemistry of Major and Trace Elements in the Kaoping River: Weathering and Human Influences. Institute of Marine Geology and Chemistry. National Sun Yat-sen University Taiwan. Larson, R.A., Hufnal, J.M., Jr., 1980. Oxidative Polymerization of Dissolved Phenols by Soluble and Insoluble Inorganic Species. Limnology and Oceanography 25, 505-512. Li, H., Lee, L.S., Schulze, D.G., Guest, C.A., 2003. Role of Soil Manganese in the Oxidation of Aromatic Amines. Environmental Science & Technology 37, 2686-2693. Lien, K.-L., 2009. Spatial and Temporal Variations and Flux of Dissolved Inorganic Components in the Small Mountainous Rivers of Taiwan Institute of Oceanography, College of Science. National Taiwan University, Taiwan. Lin, A.Y.-C., Yu, T.-H., Lateef, S.K., 2009a. Removal of pharmaceuticals in secondary wastewater treatment processes in Taiwan. Journal of Hazardous Materials 167, 1163-1169. Lin, A.Y.-C., Yu, T.-H., Lin, C.-F., 2008. Pharmaceutical contamination in residential, industrial, and agricultural waste streams: Risk to aqueous environments in Taiwan. Chemosphere 74, 131-141. Lin, K., Liu, W., Gan, J., 2009b. Oxidative Removal of Bisphenol A by Manganese Dioxide: Efficacy, Products, and Pathways. Environmental Science & Technology 43, 3860-3864. McArdell, C.S., Stone, A.T., Tian, J., 1998. Reaction of EDTA and Related Aminocarboxylate Chelating Agents with CoIIIOOH (Heterogenite) and MnIIIOOH (Manganite). Environmental Science & Technology 32, 2923-2930. Murray, J.W., 1974. The surface chemistry of hydrous manganese dioxide. Journal of Colloid and Interface Science 46, 357-371. Peterson, J., O’Meara, T., Seymour, M., 2008. Experimental investigation of cephapirin adsorption to quartz filter sands and dune sands. Hydrogeology Journal 16, 879-892. Pichichero, M.E., 2005. A Review of Evidence Supporting the American Academy of Pediatrics Recommendation for Prescribing Cephalosporin Antibiotics for Penicillin-Allergic Patients. Pediatrics 115, 1048-1057. Rubert, Pedersen, J.A., 2006. Kinetics of Oxytetracycline Reaction with a Hydrous Manganese Oxide†. Environmental Science & Technology 40, 7216-7221. Rudder, J.d., Wiele, T.V.d., Dhooge, W., Comhaire, F., Verstraete, W., 2004. Advanced water treatment with manganese oxide for the removal of 17[alpha]-ethynylestradiol (EE2). Water Research 38, 184-192. Stone, A.T., 1987a. Reductive Dissolution of Manganese(III/Iv) Oxides by Substituted Phenols. Environmental Science & Technology 21, 979-988. Stone, A.T., 1987b. Microbial metabolites and the reductive dissolution of manganese oxides: Oxalate and pyruvate. Geochimica et Cosmochimica Acta 51, 919-925. Stone, A.T., Morgan, J.J., 1984a. Reduction and dissolution of manganese(III) and manganese(IV) oxides by organics. 1. Reaction with hydroquinone. Environmental Science & Technology 18, 450-456. Stone, A.T., Morgan, J.J., 1984b. Reduction and dissolution of manganese(III) and manganese(IV) oxides by organics: 2. Survey of the reactivity of organics. Environmental Science & Technology 18, 617-624. Stumm, W., Morgan, J.J. (Eds.), 1996. Aquatic chemistry, New York. Sukul, P., Lamshöft, M., Zühlke, S., Spiteller, M., 2008. Sorption and desorption of sulfadiazine in soil and soil-manure systems. Chemosphere 73, 1344-1350. Sunda, W.G., Huntsman, S.A., Harvey, G.R., 1983. Photoreduction of manganese oxides in seawater and its geochemical and biological implications. Nature 301, 234-236. Theis, T.L., Singer, P.C., 1974. Complexation of iron(II) by organic matter and its effect on iron(II) oxygenation. Environmental Science & Technology 8, 569-573. Xu, L., Xu, C., Zhao, M., Qiu, Y., Sheng, G.D., 2008. Oxidative removal of aqueous steroid estrogens by manganese oxides. Water Research 42, 5038-5044. Yamana, T., Tsuji, A., 1976. Comparative stability of cephalosporins in aqueous solution: Kinetics and mechanisms of degradation. Journal of Pharmaceutical Sciences 65, 1563-1574. Zhang, H., Chen, W.-R., Huang, C.-H., 2008. Kinetic Modeling of Oxidation of Antibacterial Agents by Manganese Oxide. Environmental Science & Technology 42, 5548-5554. Zhang, H., Huang, C.-H., 2003. Oxidative Transformation of Triclosan and Chlorophene by Manganese Oxides. Environmental Science & Technology 37, 2421-2430. Zhang, H., Huang, C.-H., 2005. Oxidative Transformation of Fluoroquinolone Antibacterial Agents and Structurally Related Amines by Manganese Oxide. Environmental Science & Technology 39, 4474-4483. | |
dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/9958 | - |
dc.description.abstract | 民眾錯誤的用藥觀念及任意拋棄藥物的習慣,導致藥物進入環境中造成生態系統的衝擊,進而對人類健康產生潛在的風險。其中抗生素是許多研究關注的議題,尤其台灣民眾廣泛地使用以及在自然水體中檢測出較高濃度。本研究目的為探討三種頭孢子類抗生素 (cephalexin (CFX), cefazolin (CFZ), cephapirin (CFP))於不同環境因子下(二氧化錳濃度、目標污染物初始濃度、pH、水體溶氧量、水中陽離子及溶解性有機物(HA)),經由兩種不同型態的二氧化錳(δ-MnO2和c-MnO2)之化學氧化反應及轉換作用的宿命研究。批次實驗結果顯示,CFZ (100 μg/L)於合成水樣中不會被兩種二氧化錳氧化降解。反之CFX (100 μg/L)與CFP (100 μg/L)於酸性環境(pH = 5)下,經過48小時後分別被4 mg/L δ-MnO2氧化降解30 ± 2%、90 ± 1%,其CFP的半生期為13.9小時;中性環境(pH = 7)下則無任何的降解情況(≤5%);鹼性環境(pH = 9)下,CFP有明顯的水解現象。另外,水中二氧化錳濃度上升會加速CFX與CFP反應速率。若CFP的初始濃度提高 (500 μg/L),其反應速率則呈現減緩的情形。再者,水體中存在二價(Mn2+. Ca2+, Mg2+),三價(Fe3+)陽離子和HA會抑制反應,其陽離子抑制能力的權重為Mn2+ > Fe3+> Ca2+ > Mg2+,伴隨二、三價陽離子與HA的濃度提高,其氧化反應抑制的情形也會隨之上升。本研究亦發現水中溶氧不會造成反應速率的改變。於CFP降解機制中遵循擬一階模式(R2 = 0.929-0.994)。環境水體批次實驗中,發現二氧化錳對於目標污染物之氧化反應並不顯著,推測由於水體pH、水體二價陽離子和溶解性有機碳所造成之抑制情形。綜合以上結果,證實水中pH及基質對於二氧化錳之氧化反應具有影響性,由於環境水體的差異性甚大,二氧化錳氧化頭孢子類抗生素仍可能為自然淨化的一環,未來其降解機制亦可應用於廢污水處理程序。 | zh_TW |
dc.description.abstract | Incorrect practices of disposing residual medicine cause potential risk for ecosystem and human health. Antibiotics, in particular, are of significant concern. This study used batch experiments to investigate the transformation of three cephalosporin antibiotics (cephalexin (CFX), cefazolin (CFZ), cephapirin (CFP)) by manganese dioxides (δ-MnO2 and c-MnO2) in aquatic environments and to study the effect of different environmental factors such as MnO2 loading, initial cephalosporin concentration, pH, presence of dissolved oxygen, humic acid (HA) and cations on the transformation rates. In the synthetic water experiments, CFZ (100 μg/L) cannot be degraded by MnO2 while CFX (100 μg/L) and CFP (100 μg/L) can be dagraded by 4 mg/L δ-MnO2 to 30 ± 2% and 90 ± 1% respectively after 48 hours reaction at pH 5. The half life of CFP is 13.9 hours. Higher MnO2 concentration increased the reaction rate of CFX and CFP. On the other hand, the reaction rate decreased as initial concentration of CFP increased to 500 μg/L. The reaction rate increases with decreasing pH from 7 to 5. The presence of dissolved cations and HA could cause inhibitive effects, and the inhibitive capacity is Mn2+ >Fe3+ > Ca2+ > Mg2+. Dissolved oxygen has no significant effect in this reaction. In the river water system, MnO2 doesn’t play a major role to degrade selected cephalosporins due to the inhibitory effects from dissolved cations and humic acid. These results demonstrated that the degradation of cephalosporins by MnO2 could be affected by pH and matrix in the aqueous environment; therefore, according to the differences of natural water, MnO2 may facilitate, to various degrees, transformation of cephalosporin antibiotics in the natural environment. | en |
dc.description.provenance | Made available in DSpace on 2021-05-20T20:51:55Z (GMT). No. of bitstreams: 1 ntu-100-R98541103-1.pdf: 22085482 bytes, checksum: d96fd7523ebd0dd05d92f70f9d5f06a5 (MD5) Previous issue date: 2011 | en |
dc.description.tableofcontents | 口試委員會審定書 #
誌謝 i 中文摘要 ii ABSTRACT iii CONTENTS iv LIST OF FIGURES vii LIST OF TABLES ix Chapter 1 Introduction 1 1.1 Background 1 1.2 Hypotheses and Objectives 3 Chapter 2 Literature Review 4 2.1 Cephalosporin Antibiotics 4 2.2 Manganese Oxides 8 2.2.1 Manganese Oxides 8 2.2.2 Reaction mechanism 11 2.2.3 Environmental factors 13 Chapter 3 Materials and Methods 16 3.1 Description of the sampling site 16 3.2 Experimental methods 18 3.2.1 MnO2 synthesis and comparison between commercial c-MnO2 and synthesized δ-MnO2 22 3.2.2 Hydrolysis of cephalosporins 25 3.2.3 Selection of reductants 26 3.2.4 MnO2 oxidation and adsorption of cephalosporins 27 3.2.5 Redox reaction kinetics 28 3.2.6 River water degradation 29 Chapter 4 Results and discussion 30 4.1 δ-MnO2 and c-MnO2 comparison 30 4.1.1 Morphology 31 4.1.2 Particle size 33 4.1.3 Surface area 34 4.1.4 Crystallography 35 4.2 Hydrolysis and reductant interference on cephalosporins stability 37 4.2.1 Cephalosporins hydrolysis 37 4.2.2 Reductant selection 39 4.3 MnO2 oxidation and adsorption of cephalosporins 41 4.3.1 MnO2 loading and initial target compound concentration 41 4.3.2 Influence of pH 45 4.3.3 Effect of dissolved oxygen 48 4.3.4 Presence of dissolved cations 50 4.3.5 Presence of humic acid 53 4.4 Reaction kinetics of CFP oxidation with MnO2 55 4-5 River water 60 Chapter 5 Conclusions 65 5.1 Conclusions 65 5.2 Recommendations for future work 67 REFERENCE 68 Appendix A | |
dc.language.iso | en | |
dc.title | 水體環境中二氧化錳氧化降解頭孢子類抗生素之研究 | zh_TW |
dc.title | Oxidative Transformation of Cephalosporin Antibiotics by Manganese Dioxides in Aquatic Environments | en |
dc.type | Thesis | |
dc.date.schoolyear | 99-2 | |
dc.description.degree | 碩士 | |
dc.contributor.oralexamcommittee | 林正芳,康佩群 | |
dc.subject.keyword | 頭孢子類抗生素,二氧化錳,氧化降解, | zh_TW |
dc.subject.keyword | cephalosporins,manganese oxides,oxidation degradation, | en |
dc.relation.page | 74 | |
dc.rights.note | 同意授權(全球公開) | |
dc.date.accepted | 2011-08-08 | |
dc.contributor.author-college | 工學院 | zh_TW |
dc.contributor.author-dept | 環境工程學研究所 | zh_TW |
顯示於系所單位: | 環境工程學研究所 |
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