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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 陳柏翰(Po-Han Chen) | |
dc.contributor.author | Min-Fa Lin | en |
dc.contributor.author | 林銘發 | zh_TW |
dc.date.accessioned | 2021-06-17T02:24:56Z | - |
dc.date.available | 2021-02-20 | |
dc.date.copyright | 2021-02-20 | |
dc.date.issued | 2021 | |
dc.date.submitted | 2021-02-15 | |
dc.identifier.citation | 中文參考文獻 ‧工研院,三氧化二砷(Arsenic trioxide)危害特性,2018 ‧王雅靜,戴惠新,生物吸附法分離廢水中重金屬離子的研究進展,冶金分析,第二十六期第一卷第40~45頁,2006 ‧白雁斌,王天嬌,趙曉玉,重金屬廢水處理技術研究進展,污染防治技術,第26卷第3期,2013 ‧行政院環境保護署,污泥處理現況檢討及因應策略,2014 ‧行政院環境保護署毒災防救管理資訊,重鉻酸鉀安全資料表,2016 ‧行政院環境保護署環境檢驗所,毒性化學物質重金屬類物種鑑識技術研究報告,2006 ‧行政院環境保護署環境檢驗所,毒性化學物質重鉻酸鹽類物種鑑識技術,2007 ‧李中光,吳獻經,呂孟篤,由中孔洞純矽分子篩製備高選擇性吸附劑:以染料吸附為例,行政院國家科學委員會專題研究計畫成果報告,2006 ‧李中光,劉新校,邱惠敏,重金屬廢水處理技術之進展,環保簡訊,第23期,2014 ‧李安成,陳俊六,王豐傑,郭叮坤,陳柏宏,吸附在廢水處理之應用(II)-以陰離子交換樹脂去除廢水中的鉻離子,工程科技與教育學刊,第二卷第二期第266~275頁,2005 ‧李優平,鈦鹽混凝去除無機 As(III)的實驗研究,西安建築科技大學碩士學位論文,2014 ‧侯萬善,廢水金屬處理回收技術簡介,中技社通訊,第48期,2003 ‧柯以侃編,儀器分析,新文京開發出版社,2005 ‧洪儷瑋,以廢鑄鐵還原電鍍廢液中高濃度六價鉻之研究,碩士論文,2006 ‧袁濤,曾新,羅啟芳,對混凝沉澱法分散式飲水除砷的研究,衛生研究,第二十八期第六卷第331~333頁,1999 ‧高峰,賈永忠,孫進賀,除砷技術現狀與展望,鹽湖研究,第十八期第一卷第53~57頁,2010 ‧國家環境毒物研究中心,國家環境毒物研究中心整理口服六價鉻毒性資料,2014 ‧莊建東,田勤奮,劉平,Bi2Sn2O7的不同水熱法製備及其可見光光催化除As(III)性能分析,物理化學學報,第三十二卷第551~557頁,2016 ‧郭維華,費忠民,水中砷混凝去除機理的研究,蘇州城建環保學院學報,第八期第一卷第70~77頁,1995 ‧黃富昌,顏冠忠,林嘉鴻,以吸脫附動力曲線探討土壤吸附特性,2006年台灣環境資源永續發展研討會論文集,台灣環境資源永續發展協會,2006 ‧廖敏,謝正苗,王銳,菌藻共生體去除廢水中砷初討,環境污染與防治,第九期第二卷第11~12頁,1997 ‧劉旭倍,垃圾變黑金-台灣農業廢棄物應用於製作生物碳的可行性探討,E-SOC JOURNAL,第111期,2013 ‧劉芳,靜電紡絲製備複合納米纖維及其在廢水處理中的應用,碩士論文,2015 ‧劉瑞霞,王亞雄,湯鴻霄,新型離子交換纖維去除水中砷酸根離子的研究,環境科學學報,第二十三期第五卷第88~91頁,2002 ‧劉銳平,李星,夏聖驥,高錳酸鉀強化三氯化鐵共沉降法去除亞砷酸鹽的效能與機理,環境科學,第二十六期第一卷第72~75頁,2005 ‧潘易霜,金屬氧化物在氧化矽表面的修飾及中孔碳材合成,碩士論文,2006 ‧蔡孝鑫,利用廢棄氟化鈣研製中孔洞材料與觸媒處理含矽烷光阻劑與丙酮之研究,碩士論文,2015 ‧網路新聞1,https://news.ltn.com.tw/news/society/breakingnews/2485157,2018/07/11 ‧網路新聞2,https://udn.com/news/amp/story/7321/5133747,2020/12/30 英文參考文獻 ‧Aacharya N., Gaowa H., Ohashi D., Kawamoto T., Honma Y., Okaue T., Yokoyama. Adsorption behavior of arsenic to an isolated ferric ion combined on chelate resin. Bulletin of the Chemical Society of Japan, 90 (2017) 1372-1374. ‧Acikyildiz A., Gurses S., Karaca. Preparation and characterization of activated carbon from plant wastes with chemical activation. Microporous and Mesoporous Materials, 198 (2014) 45–49. ‧Adegoke I. H., Adekola F. A., Fatoki O. S. Sorptive interaction of oxyanions with iron oxides: a review. Polish Journal of Environmental Studies, 22 (1) (2013) 7-24. ‧Aghdasi R., Ansari S., Yousefi M., Goli. Structural and mechanical properties of pristine and adsorbed puckered arsenene nanostructures: A DFT study. Superlattices and Microstructures, 139 (2020) 106414. ‧Akin G., Arslan A., Tor M., Ersoz Y., Cengeloglu. Arsenic (V) removal from underground water by magnetic nanoparticles synthesized from waste red mud. Journal of Hazardous Materials, 235 (2012) 62–68. ‧Alvarez-Torrellas M., Munoz J.A., Zazo J.A., Casas J., Garcia. Research article Synthesis of high surface area carbon adsorbents prepared from pine sawdust-Onopordumacanthium L. for nonsteroidal anti - inflammatory drugs adsorption. Environmental Management, 183 (2016) 294–305. ‧Bandpei A.M., Mohseni S.M., Sheikhmohammadi A., Sardar M., Sarkhosh M., Almasian M. Optimization of Arsenite removal by adsorption onto organically modified montmorillonite clay: Experimental theoretical approaches. Korean Journal of Chemical Engineering, (2017) 1–8 (in press). ‧Batista A.P.L. and Ornellas F.R. CASSCF and MRMP2 investigation of the interaction of arsenic adatoms with carbon dimers on the diamond (100)-2×1 surface. Surface Science, 641 (2015) 159–165. ‧Bhowmick S., Chakraborty P., Mondal W., Van Renterghem S., Van den Berghe G., Roman-Ross, Chatterjee D., M. Iglesias. Montmorillonite-supported nanoscale zero-valent iron for removal of arsenic from aqueous solution: Kinetics and mechanism. Chemical Engineering Journal, 243 (2014) 14–23. ‧Bhuvaneswari V., Nagarajan R., Chandiramouli. Methyl and Ethyl mercaptan molecular adsorption studies on novel Kagome arsenene nanosheets - A DFT outlook. Physica B, 586 (2020) 412135. ‧Biswas P., Nath D., Sanyal P., Banerji. An alternative approach to investigate the origin of p-type conductivity in arsenic doped ZnO. Current Applied Physics, 15 (2015) 1256-1261. ‧Blanchard M., Alfredsson J., Brodholt K., Wright C.R., Catlow A. Arsenic incorporation into FeS2 pyrite and its influence on dissolution: A DFT study. Geo Chimicaet Cosmo Chimica Acta, 71 (2007) 624–630. ‧Charlet G., Morin J., Rose Y., Wang M., Auffan A., Burnol A., Martinez F. Reactivity at (nano) particle-water interfaces, redox processes, and arsenic transport in the environment. C. R. Geoscience, 343 (2011) 123–139. ‧Cheng H., Luo L., Hu B., Yu Z., Luo M., Cortalezzi F. Sludge carbonization and activation: From hazardous waste to functional materials for water treatment. Journal of Environmental Chemical Engineering, 4 (2016) 4574–4586. ‧Chutia P., Kato S., Kojima T. Arsenic adsorption from aqueous solution on synthetic zeolites. Journal of Hazardous Materials, 162 (1) 2009 440-47. ‧Demirbas N., Dizge, Sulak M. T., Kobya M. Adsorption kinetics and equilibrium of copper from aqueous solutions using hazelnut shell activated carbon. Chemical Engineering, 148 (2009) 480–487. ‧Giri K., Patel R., Mandal S. Removal of Cr (VI) from aqueous solution by Eichhorniacrassipes root biomass - derived activated carbon. Chemical Engineering, 185–186 (2012) 71–81. ‧Gueye M., Richardson Y., Kafack F. T., Blin J. High efficiency activated carbons from African biomass residues for the removal of Chromium (VI) from wastewater. Journal of Environmental Chemical Engineering, 2 (2014) 273–281. ‧Hamed M. M., Ali M. M. S., Holiel M. Preparation of activated carbon from doum stone and its application on adsorption of 60 Co and 152+154 Eu: Equilibrium, kinetic and thermodynamic studies. Journal of Environmental Radioactivity, 164 (2016) 113-124. ‧Jiang L., Zhang, Wang X., Holm N., Rajagopalan K., Chen F., Ma S. Highly ordered macroporous woody biochar with ultra-high carbon content as a supercapacitor electrodes. Electrochimica Acta, 113 (2013) 481–489. ‧Jin H., Capareda S., Chang Z., Gao J., Xu Y., Zhang J., Biochar pyrolytically produced from municipal solid wastes for aqueous As (V) removal: Adsorption property and its improvement with KOH activation. Bioresource Technology, 169 (2014) 622–629. ‧Jin X., Wang Z., Gu J., Polin, Carbon materials from high ash biochar for supercapacitor and improvement of capacitance with HNO3 surface oxidation. Power Sources, 236 (2013) 285–292. ‧Jung L. K., Boateng, Flora J. R. V., Oh J., Braswell M. C., Son A., Yoon Y. Competitive adsorption of selected non - steroidal anti - inflammatory drugs on activated biochars: Experimental and molecular modeling study. Chemical Engineering, 264 (2015) 1–9. ‧Kilic M., Apaydin-Varol E., Putun A. E. Adsorptive removal of phenol from aqueous solutions on activated carbon prepared from tobacco residues: Equilibrium, kinetics and thermodynamics. Hazardous Materials, 189 (2011) 397–403. ‧Kilic M., Apaydin-Varol E., Putun A. E. Adsorptive removal of phenol from aqueous solutions on activated carbon prepared from tobacco residues: Equilibrium, kinetics and thermodynamics.Hazardous Materials, 189 (2011) 397–403. ‧Kilic M., Apaydın-Varol E., Putun A. E. Preparation and surface characterization of activated carbons from Euphorbia rigida by chemical activation with ZnCl2, K2CO3, NaOH and H3PO4. Applied Surface Science, 261 (2012) 247– 254. ‧Kurniawan A., Sillanpaa M.E., Sillanpaa M. Nano adsorbents for remediation of aquatic environment: Local and practical solutions for global water pollution problems. Critical Reviews in Environmental Science and Technology, 42 (2012) 1233–1295. ‧Li Y., Shao J., Wang X., Deng Y., Yang H., Chen H. Characterization of modified biochars derived from bamboo pyrolysis and their utilization for target component (Furfural) adsorption. Energy Fuels, 28 (2014) 5119–5127 ‧Li Z., Deng S., Yu G., Huang J., Lima V.C. As (V) and As (III) removal from water by a Ce–Ti oxide adsorbent: Behavior and mechanism. Chemical Engineering Journal, 161 (2010) 106–113. ‧Ma J., Zhu Z., Chen B., Yang M., Zhou H., Li C., Yu F., Chen J. One-pot, large-scale synthesis of magnetic activated carbon nanotubes and their applications for arsenic removal. Journal of Materials Chemistry, A (1) (2013) 4662–4666. ‧Ma Y., Liu W.J., Zhang N., Li Y.S., Hong J., Sheng G.P. Polyethylenimine modified biochar adsorbent for hexavalent chromium removal from the aqueous solution. Bioresource Technology, 169 (2014) 403–408. ‧Mahmoud D. K., Salleha M.A.M., Karima W.A.W.A., Idris A., Abidin Z. Z. Batch adsorption of basic dye using acid treated kenaf fibre char: Equilibrium, kinetic and thermodynamic studies. Chemical Engineering, 181 (2012) 449–457. ‧Oliveira A. F., Ladeira A. C. Q., Ciminelli V. S. T., Heine T., Duarte H. A. Structural model of arsenic (III) adsorbed on gibbsite based on DFT calculations. Journal of Molecular Structure : THEOCHEM, 762 (2006) 17–23. ‧Owlad M., Aroua M.K., Daud W. M. A. W. Hexavalent chromium adsorption on impregnated palm shell activated carbon with polyethyleneimine. Bioresource Technology, 101 (2010) 5098–5103. ‧Pattanayak J., Mondal K., Mathew S. A parametric evaluation of the removal of As (V) and As (III) by carbon-based adsorbents. Carbon, 38 (4) (2000) 589-596. ‧Qian Q., Machida M., Tatsumoto H. Characteristics and methylene blue adsorption performance of activated carbon prepared from cattle – manure - compost by ZnCl2 activation. Tanso, 226 (2007) 25–31. ‧Qian Q., Machida M., Tatsumoto H. Preparation of activated carbons from cattle-manure compost by zinc chloride activation. Bioresource Technology, 98 (2007) 353–360. ‧Rajapaksha U., Vithanage M., Ahmad M., Seo D.C., Cho J. S., Lee S. E., Lee S. S., Ok Y. S. Enhanced sulfamethazine removal by steam-activated invasive plant derived biochar. Journal of Hazardous Materials, 290 (2015) 43–50. ‧Regmi J. L., Moscoso G., Kumar S., Cao X., Mao J. G. Schafran. Removal of copper and cadmium from aqueous solution using switch grass biochar produced via hydrothermal carbonization process. Environmental Management, 109 (2012) 61–69. ‧Rensburg A. J., Landman M., Rooyen P. H., Conradie M. M., Conradie J. Molybdenum (0) Fischer ethoxycarbene complexes: Synthesis, X-ray crystal structures and DFT study. Polyhedron, 121 (2017) 285–296. ‧Reynosa-Martinez A.C., Tovar G. N., Gallegos W.R., Rodriguez-Melendez H., Torres-Cadena Mondragon-Solorzano R., Barroso-Flores G. J., Alvarez-Lemus M.A., Montalvo V.G., Lopez-Honorato E. Effect of the degree of oxidation of graphene oxide on As (III) adsorption. Journal of Hazardous Materials, 384 (2020) 121440. ‧Sharma N., Verma A., Sharma D., Deva N. Sankararamakrishnan. Iron doped phenolic resin based activated carbon micro and nanoparticles by milling: Synthesis, characterization and application in arsenic removal. Chemical Engineering Science, 65 (2010) 3591–3601. ‧Sharma V. K., Sohn M. Aquatic arsenic: Toxicity, speciation, transformations, and remediation. Environment International, 35 (4) (2009) 743-59. ‧Shi Q., Sterbinsky G.E., Prigiobbe V., Meng X. Mechanistic study of lead adsorption on activated carbon. Langmuir, 34 (2018) 13565–13573. ‧Smith A.H., Lingas E.O., Rahman M. Contamination of drinking water by arsenic in Bangladesh: a public health emergency. Bulletin of the World Health Organization, 78 (2000) 1093–103. ‧Song S., Lopez V. A., Hernandez C. D. J. Arsenic removal from high-arsenic water by enhanced coagulation with ferric ions and coarse calcite. Water Research, 40 (2) (2006) 364-372. ‧Sutcu H., Demiral. Production of granular activated carbons from loquat stones by chemical activation. Pyrolysis, 84 (2009) 47–52. ‧Tan S., Zhang, Liu H., Qiang Y., Li W., Guo L., Chen S. Insights into the inhibition mechanism of three 5-phenyltetrazole derivatives for copper corrosion in sulfuric acid medium via experimental and DFT methods. Journal of the Taiwan Institute of Chemical Engineers, 102 (2019) 424–437. ‧Tsai T., Chang C.Y., Wang S.Y., Chang C.F., Chien S.F., Sun H.F. Preparation of activated carbons from corn cob catalyzed by potassium salts and subsequent gasification with CO2. Bioresource Technology, 78 (2001) 203–208. ‧Tseng R. L. Physical and chemical properties and adsorption type of activated carbon prepared from plum kernels by NaOH activation. Hazardous Materials, 147 (2007) 1020–1027. ‧Tuna A. O. A., Ozdemir E., Simsek E. B., Removal of As (V) from aqueous solution by activated carbon-based hybrid adsorbents: Impact of experimental conditions. Chemical Engineering Journal, 2013, (223) 116-28. ‧Vitela-Rodriguez A.V., Rangel-Mendez J.R. Arsenic removal by modified activated carbons with iron hydroxide (oxide) nanoparticles. Journal of Environmental Management, 114 (2013) 225–231. ‧Wang C., Li H., Liang. Short communication bioleaching of heavy metal from woody biochar using Acidithiobacillus Ferrooxidans and activation for adsorption. Bioresource Technology, 146 (2013) 803–806. ‧Wang N.Y., Shih C.H., Chiueh P. T., Huang Y.F. Environmental Effects of Sewage Sludge Carbonization and Other Treatment Alternatives. Energies, 6 (2013) 871-883. ‧Wang R., Zhang D., Liu C. DFT study of the adsorption of 2, 3, 7, 8 tetrachlorodibenzo-p-dioxin on pristine and Ni-doped boron nitride nanotubes. Chemosphere, 168 (2017) 18-24. ‧Weber W. J. and Morris J.C. Kinetics of adsorption on carbon from solution. Journal of the Sanitary Engineering Division, 89 (1963) 31-40. ‧Xiong Y., Tong Q., Shan W., Xing Z., Wang Y, Wen S., Lou Z. Arsenic transformation and adsorption by iron hydroxide/manganese dioxide doped straw activated carbon. Applied Surface Science, 416 (2017) 618–627. ‧Xue Y., Gao B., Yao Y., Inyang M., Zhang M., Zimmerman A.R., Ro K. S. Hydrogen peroxide modification enhances the ability of biochar (hydrochar) produced from hydrothermal carbonization of peanut hull to remove aqueous heavy metals: Batch and column tests. Chemical Engineering, 200 (2012) 673–680. ‧Yang B.Y., Cao Y., Qi F.F., Li X.Q., Xu Q. Atrazine adsorption removal with nylon6/polypyrrole core-shell nanofibers mat: possible mechanism and characteristics. Nanoscale Research Letters, 10 (2015) 207. ‧Yang G. X., Hong J. Amino modification of biochar for enhanced adsorption of copper ions from synthetic waste water. Water Research, 48 (2014) 396–405. ‧Yang G., Zhang, H. Wang. Current state of sludge production, management, treatment and disposal in China. Water Research, 78 (2015) 60–73. ‧Yang M., Sun Y., Zhang X., McCord B., McGoron A.J., Mebel A., Cai Y. Raman spectra of thiolated arsenicals with biological importance. Talanta, 179 (2018) 520–530. ‧Yang R., Su Y., Aubrecht K.B., Wang X., Ma H., Grubbs R.B., Hsiao B.S., Chu B. Thiol-functionalized chitin nanofibers for As (III) adsorption. Polymer, 60 (2015) 9-17. ‧Yang S., Adjaye J., McCaffrey W.C., Nelson A.E. Density-functional theory (DFT) study of arsenic poisoning of NiMoS. Journal of Molecular Catalysis A, Chemical, 321 (2010) 83–91. ‧Yorgun S., Vural N., Demiral H. Preparation of high – surface area activated carbons from paulownia wood by ZnCl2 activation. Microporous and Mesoporous Materials, 122 (2009) 189–194. ‧Zhang G. S., Liu H. J., Qu J. H. Arsenate uptake and arsenite simultaneous sorption and oxidation by Fe–Mn binary oxides: Influence of Mn/Fe ratio, pH, Ca2+, and humic acid. Journal of Colloid and Interface Science, 366 (2012), 141-146. ‧Zhang M., G. He, G. Pan. Binding mechanism of arsenate on rutile (110) and (001) planes studied using grazing-incidence EXAFS measurement and DFT calculation. Chemosphere, 122 (2015) 199–205. ‧Zhang S., X. Li, J.P. Chen. Preparation and evaluation of a magnetite-doped activated carbon fiber for enhanced arsenic removal. Carbon, 48 (2010) 60 – 67. ‧Zheng S., Jiang W., Cai Y., Dionysiou D.D., O’Shea K.E.. Adsorption and photocatalytic degradation of aromatic organoarsenic compounds in TiO2 suspension. Catalysis Today, 224 (4) (2014) 83–88. ‧Zhi M., Liu S., Hong Z., Wu N., Electrospun activated carbon nanofibers for supercapacitor electrodes, RSC 82 (2014) 43619–43623. | |
dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/68549 | - |
dc.description.abstract | 摘要
本研究以“以廢制廢”的概念進行研究,將利用特定樣本醫院污泥實驗製備成新型生質碳吸附材料,試驗捕捉水中有害之砷離子與鉻離子。其實驗方法首先,採用微波碳化技術對污泥進行碳化,然後用ZnCl2在高溫下進行化學活化,以提高污泥的孔隙率和表面積。然後添加氯化鐵進行二次活化成新型金屬摻雜生質碳(Fe-SBC)材料對水中無機砷與鉻進行吸附性能評估。並採用各項實驗儀器檢測新生質碳材料特性如氮氣等溫吸/脫附法(BET)測定其比表面積、孔徑分佈和孔徑體積。又通過掃描電子顯微鏡(SEM)和能譜分析(EDS)測定了生質碳的形態與化學成分。再用X-射線繞射分析儀(XRD)測定了生質碳的晶相。及用熱重分析儀(TGA)研究分析生質碳的重量損失。 經實驗儀器檢測特性分析結果顯示,50%ZnCl2-SBC的比表面積為525 m2 g−1,平均孔體積為0.35 cm3 g−1,孔徑為8.71 nm。SEM-EDS結果表明,新生質碳材料具有均勻的孔徑以及成分與活性碳非常相似,成分包括:C、O、K、Ca、Si和P。XRD分析結果表明,Fe-SBC在2θ= 36°和57°時可以觀察到FeOOH的Fe-O典型峰。運用傅立葉轉換紅外線光譜儀(Fourier-transform infrared spectroscopy;簡稱FT-IR)分析結果發現,生質碳在3400 cm-1處,對應O-H鍵和N-H鍵的彎曲振動,為胺基的特徵峰,在不同比例之ZnCl2的SBC也可發現,而且有明顯增強之特性相符趨勢。 新型金屬摻雜生質碳(Fe-SBC)對As(III)的最高去除效率為91%在pH 3條件下,吸附容量為2.9 mg g-1。Fe-SBC對As(V)的最高去除效率為97%,吸附容量為3.72 mg g-1。在陰離子與As(V)和As(III)競爭吸附影響的順序排列如PO43- > CO32- > SO42- > NO3- > Cl-。另外此新型金屬摻雜生質碳(Fe-SBC)對樣對於較低之pH值環境條件下,Cr(VI)吸附效率亦可達到近90%。且依實驗結果隨著Fe-SBC投加量的增加,其吸附效率越來越好,Cr(VI)吸附效率可達99%以上。Cr(VI)吸附能力可達到67.7 mg g-1。 另外在等溫吸附模擬結果可看出在砷吸附實驗中,用Langmuir模式(R2As(III) = 0.992; R2As(V) = 0.995)比Freundlich模式(R2As(III) = 0.894; R2As(V) = 0.891)適合;而在鉻吸附實驗中,亦是用Langmuir模式(R2Ct(VI) = 0.995)比Freundlich模式(R2Cr(VI) = 0.889)適合。動力學模擬結果顯示擬二階具有良好結果,As(III)線性圖的迴歸係數高於0.99;As(V)線性圖的迴歸係數高於0.98;Cr(VI)線性圖的迴歸係數高於0.99,證明本實驗新材料之可信賴度。而吸附過程可觀察到之實驗數據是由顆粒內擴散控制,並呈現吸附過程由兩個因素控制。第一條線性關係屬於材料之表面吸附;第二條線性關係是指污染物緩慢的向材料內部擴散。 由本研究所繪製的吸附反應機理可分為三個途徑,第一條途徑污染物被吸附是由羥基氧化鐵官能團在SBC材料表面的附著並被氧取代。第二種途徑是砷離子與鉻離子被吸附在材料表面,是因為SBC材料表面帶正電與負離子砷分子與鉻分子之間產生靜電作用。第三個途徑是砷離子與鉻離子通過物理吸附並附著在SBC材料上,然後逐漸擴散到材料孔洞中,這可能是(包括Freundlich模式和Langmuir模式)吸附作用所產生的結果。 本研究已利用特定樣本醫院生活污水處理廠產生之廢污泥材料,實驗將其碳化為新型生質碳吸附材料,試驗捕捉水中有害之砷離子與鉻離子有所成效。且因污泥取得成本極低,因此若有機會進一步工廠實地做小型研究測試,驗證可行之後對於處理有害廢水處理領域中將具有非常可觀的前景。 關鍵字:生質碳、表面活化、污泥、砷與鉻、吸附 | zh_TW |
dc.description.abstract | ABSTRACT
The utilization of domestic sludge, hospital sludge and aquatic product sludge form waste water treatment plants as biochar adsorbent was investigated. The sludge was carbonized using microwave carbonization and then chemically activated at high temperatures by using ZnCl2 to enhance porosity and surface area. A newly designed metal doped sludge biochar (such as Fe-SBC) presents effective inorganic arsenic adsorption in water. The specific surface area, pore size distribution and pore volume were determined by performing nitrogen adsorption-desorption measurements (BET). The morphology of the biochar carbon was measured through a scanning electron microscope (SEM) with energy-dispersive X-ray (EDS) analysis. The crystal phase of the biochar carbon was determined by an X-ray diffraction (XRD). The thermal properties of carbonized and biochar carbon were studied by a thermo gravimetric analysis (TGA) instrument. Results show that the surface area, average pore volume and pore size of 50%ZnCl2-SBC are 525 m2 g−1, 0.35 cm3 g−1and 8.71 nm, respectively. SEM results reveal that biochar carbon has uniform pore size. XRD results show Fe-O typical peak of FeOOH were observed for Fe-SBC at 2θ = 36° and 57°. The maximum removal efficiency of As(III) by Fe-SBC was 91% and the adsorption capacity was 2.9 mg g-1 at pH 3. The maximum removal efficiency of As(V) by Fe-SBC was 97%, and the adsorption capacity was 3.72 mg g-1. The order of competitive adsorption effect between anions and arsenic was PO43- > CO32- > SO42- > NO3- > Cl-. The adsorption efficiency of Cr(VI) reached nearly 90% at low pH. With the increase of the dosage of Fe-SBC, the adsorption efficiency becomes better and better, and the adsorption efficiency can reach more than 99%.The adsorption capacity can reach 67.7 mg g-1. The adsorption data could be described well by the Langmuir model (R2As(III) = 0.998; R2As(V) = 0.995) rather than by the Freundlich model (R2As(III) = 0.982; R2As(V) = 0.987); Langmuir model (R2Ct(VI) = 0.995) rather than by the Freundlich model (R2Cr(VI) = 0.889). These data indicate that the adsorption process was fitted to a monolayer adsorption on a homogeneous surface. The values of the rate constant (k2) were found to increase from2.9x10-3 to 4.1x10-3 with As(III), and 3.1 x10-4 to 10.3 x10-3 with As(V). The data shows good compliance with the pseudo second order equation and the regression coefficients for the linear plots were higher than 0.97. The reaction mechanism is divided into three pathways. The first pathway is the attachment of arsenic ions and chromium ions onto the biochar via physical adsorption, which may be attributed to van der Waals forces. The second pathway is the adsorption of arsenic species and chromium species, which depends largely on the surface chemistry of the adsorbent and on the chemistry of the aqueous phase. Furthermore, the activated carbon possesses both acidic and basic groups so that its surface charge density can be positive at low pH. The third pathway is the attachment of metal functional groups onto the surface of adsorbents and their replacement with oxygen groups, which is a modification method for producing strong adsorbents toward heavy metals. In this study, the waste sludge material produced by the domestic sewage treatment plant has been used to carbonize it into a new type of biomass carbon adsorption material, and the experiment has been effective in capturing the harmful arsenic and chromium ions in the water. And because the cost of obtaining sludge is extremely low, if there is an opportunity for further small-scale research and testing in the factory, it will have a very promising prospect for the treatment of hazardous wastewater after the verification is feasible. Keyword: Biochar Carbon, Surface activation, Sludge, Arsenic and Chromium, Adsorption | en |
dc.description.provenance | Made available in DSpace on 2021-06-17T02:24:56Z (GMT). No. of bitstreams: 1 U0001-0902202109401300.pdf: 6276019 bytes, checksum: 9f04afcaddce8d5f0eedd742a38959e0 (MD5) Previous issue date: 2021 | en |
dc.description.tableofcontents | 目錄 口試委員會審定書……………………………………………………………………………! 誌謝………………………………………………………….…………………………………I 摘要 II ABSTRACT VI 目錄 IX 圖目錄 XIII 表目錄 XV 第一章 緒論 1 1.1 研究緣起 1 1.2 研究問題 5 1.3 研究範疇 6 1.4 研究限制 6 1.5 論文架構 7 第二章 文獻回顧 9 2.1 介紹污泥之處理方式 9 2.2 生質碳定義與應用 10 2.2.1 生質碳之來源與製備 10 2.2.2 生質碳之特性與應用 11 2.3 砷與六價鉻的特性與處理技術 12 2.3.1 砷的特性 12 2.3.2 砷的處理技術 15 2.3.3 六價鉻之特性 20 2.3.4 六價鉻之處理技術 21 第三章 研究設計與實驗方法 25 3.1 實驗藥品及研究設備 25 3.1.1 實驗藥品 25 3.1.2 生質碳原料 26 3.1.3 實驗設備 26 3.1.4 實驗儀器 27 3.2 實驗步驟與方法 27 3.2.1 SBC材料製備方法 27 3.2.2 摻雜重金屬SBC材料的製備方法 28 3.3 材料特性分析 29 3.3.1 氮氣等溫吸/脫附儀 29 3.3.2 X光粉末繞射儀 31 3.3.3 熱重分析儀分析 33 3.3.4 掃描式電子顯微鏡/能量散射光譜儀 34 3.4 傅立葉紅外線光譜儀分析 34 3.5 吸附性能評估 35 3.6 等溫吸附模式 40 3.6.1 Freundlich吸附理論 40 3.6.2 Langmuir吸附理論 41 3.7 動力吸附模式 43 3.7.1 擬一階動力吸附模式 43 3.7.2 擬二階動力吸附模式 44 3.7.3 顆粒內部擴散模式 44 第四章 量測結果分析 46 4.1 重金屬溶出實驗 46 4.2 材料特性分析結果 47 4.2.1 氮氣等溫吸/脫附儀分析結果 47 4.2.2 熱重損失分析結果 48 4.2.3 SEM-EDS分析結果 48 4.2.4 FT-IR 分析結果 50 4.2.5 X-射線繞射分析結果 52 4.3 砷吸附測試結果 52 4.3.1 摻雜鐵含量的影響 52 4.3.2 不同pH值之影響 53 4.3.3 不同污染物濃度之影響 55 4.3.4 陰離子競爭吸附的影響 57 4.3.5 質量平衡實驗結果 58 4.4 鉻吸附測試結果 58 4.4.1 不同初始濃度的影響 58 4.4.2 不同pH值之影響 59 4.4.3 吸附劑投加量的影響 61 4.5 等溫吸附與動力學模式 63 4.5.1 等溫吸附模式 63 4.5.2 動力學吸附模式 65 4.5.3 內擴散模式 67 4.6 吸附機理 69 第五章 結論與建議 71 5.1 結論 71 5.1.1 材料特性分析結果 71 5.1.2 新生質材料之吸附性能評估結果 71 5.1.3 新生質材料之等溫吸附與動力學吸附模式結果 72 5.1.4 新生質材料之吸附機理結果 72 5.2 研究後建議 73 中文參考文獻 75 英文參考文獻 77 附錄一 物質安全資料表-重鉻酸鉀 87 附錄二 物質安全資料表-氯化鋅 96 附錄三 物質安全資料表-三氧化二砷 101 附錄四 檢測方法-酸消化法 106 附錄五 檢測方法-比色法 110 附錄六 製備材料之經濟效益計算 114 圖目錄 圖1.1 處理混凝土廠未依規定處理污泥相關新聞報導 3 圖1.2 千興公司涉把產出的有害事業廢棄物掩埋在廠區土地下方相關新聞報導 4 圖1.3 印刷廢液濫倒翡翠水庫水源地相關新聞報導 4 圖1.4 論文架構圖 8 圖2.1 不同pH條件下,(a) As(V)和(b) As(III)的型態分佈 15 圖3.1 SBC材料上摻雜重金屬的流程圖 28 圖3.2 等溫吸/脫附曲線六種型式 30 圖3.3 IUPAC四種遲滯曲線型式 31 圖3.4 布拉格定律 32 圖3.5 熱重曲線型式 33 圖3.6 水中As/Cr離子吸附實驗裝置圖 37 圖3.7 研究流程規劃圖 39 圖3.8 Freundlich等溫吸附曲線圖 41 圖3.9 Langmuir等溫飽和吸附曲線示意圖 42 圖4.1 提取毒性分析結果 46 圖4.2 原始污泥和生質碳的熱重分析 48 圖4.3 醫院污泥的(a) SEM形態和(b)元素分析圖 49 圖4.4 X%ZnCl2-SBC SEM分析結果 50 圖4.5 SBC與不同ZnCl2比例SBC之FT-IR分析圖 51 圖4.6 (a) SBC,(b) Fe-SBC和(c) Fe2O3 JCPDS的XRD分析結果 52 圖4.7 鐵負載量對吸附性能的影響 53 圖4.8 不同pH值對As(III)吸附性能的影響 54 圖4.9 不同pH值對As(V)吸附性能的影響 55 圖4.10 不同初始濃度對As(III)吸附性能的影響 56 圖4.11 不同初始濃度對As(V)吸附性能的影響 56 圖4.12 常見陰離子對Fe-SBC在水中吸附As的影響 57 圖4.13 質量平衡實驗原理圖 58 圖4.14 各種不同濃度下之Fe-SBC吸附效果 60 圖4.15 pH對Fe-SBC吸附60 ppm Cr(VI)離子之影響 60 圖4.16 pH對Fe-SBC之吸附與介面電位影響 61 圖4.17 不同投加量對Fe-SBC吸附Cr(VI)離子之影響 62 圖4.18 不同投加量對Fe-SBC吸附Cr(VI)離子之吸附能力 62 圖4.19 Fe-SBC對As(III)和As(V)的吸附等溫線 63 圖4.20 Fe-SBC對Cr(VI)的吸附等溫線 64 圖4.21 (a) As(III)和(b) As(V)的內擴散速率迴歸分析結果 68 圖4.22 Fe-SBC內擴散速率迴歸分析結果 69 圖4.23 SBC材料與砷的吸附機理 70 圖4.24 SBC材料與鉻的吸附機理 70 圖5.1 現有污泥處理程序 74 圖5.2 新污泥處理思維 74 表目錄 表2.1 歐美地區部分國家污泥產生量及最終處置占比 9 表2.2 使用不同化學活化劑製成之生質碳 11 表2.3 生質碳應用於吸附處理不同污染物 12 表2.4 三氧化二砷之特性 14 表2.5 三氧化二砷之危害 14 表2.6 重鉻酸鉀之特性 20 表2.7 重鉻酸鉀之危害 21 表3.1 化學藥品中英名稱與化學式 25 表3.2 氣體中英名稱、純度與化學式 26 表3.3 材料之來源與價格 26 表3.4 ICP-AES工作参数表 37 表3.5 實驗操作參數表 38 表4.1 各種材料之比表面積、孔體積和孔徑分析結果 47 表4.2 Fe-SBC去除As(III)和As(V)的各種等溫線參數 64 表4.3 Fe-SBC去除Cr(VI)的等溫線參數 65 表4.4 砷吸附的擬一階和擬二階比較 66 表4.5 鉻吸附的擬一階和擬二階比較 66 表4.6 內擴散模式的比較 67 | |
dc.language.iso | zh-TW | |
dc.title | 利用廢棄污泥製備環保吸附材並應用於重金屬吸附之研究 | zh_TW |
dc.title | Research into the preparation of environmentally friendly adsorption material using waste sludge and its application to heavy metal adsorption | en |
dc.type | Thesis | |
dc.date.schoolyear | 109-1 | |
dc.description.degree | 博士 | |
dc.contributor.oralexamcommittee | 張陸滿(luh-Maan chang),曾惠斌(Hui-Ping Tserng),張章堂(Chang-Tang Chang),胡石政(Shih-Cheng Hu),楊希文(S-W Yung) | |
dc.subject.keyword | 生質碳,表面活化,污泥,砷與鉻,吸附, | zh_TW |
dc.subject.keyword | Biohar Carbon,Surface activation,Sludge,Arsenic and Chromium,Adsorption, | en |
dc.relation.page | 115 | |
dc.identifier.doi | 10.6342/NTU202100689 | |
dc.rights.note | 有償授權 | |
dc.date.accepted | 2021-02-17 | |
dc.contributor.author-college | 工學院 | zh_TW |
dc.contributor.author-dept | 土木工程學研究所 | zh_TW |
顯示於系所單位: | 土木工程學系 |
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