| 研究生: |
黃烱秦 Huang, Chiung-Chin |
|---|---|
| 論文名稱: |
以鋇系化學過氧沉澱法結合流體化床均質顆粒化技術回收含硼廢水中的硼 Recovery of Boron from Synthetic Wastewater by integrating Barium-based Chemical Oxo-Precipitation with Fluidized-Bed Homogeneous Granulation |
| 指導教授: |
黃耀輝
Huang, Yao-Hui |
| 學位類別: |
碩士 Master |
| 系所名稱: |
工學院 - 化學工程學系 Department of Chemical Engineering |
| 論文出版年: | 2016 |
| 畢業學年度: | 104 |
| 語文別: | 中文 |
| 論文頁數: | 110 |
| 中文關鍵詞: | 化學過氧沉澱 、流體化床均質顆粒化 、流體化床串聯系統 、晶種(BaB(OH)2(OO)2B(OH)2) |
| 外文關鍵詞: | Chemical Oxo-Precipitaiton, Fludized-Bed Homogeneous Granulation, FBRs in series, BaB(OH)2(OO)2B(OH)2 |
| 相關次數: | 點閱:84 下載:11 |
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本研究嘗試將化學過氧沉澱法(COP)結合流體化床均質顆粒化技術(FBHG),將含硼廢水中的硼以低含水率高純度的過硼酸鹽類顆粒型態回收,而非傳統沉澱法所產生高含水率汙泥,同時達到改善水質及資源化含硼廢水中的硼的目標。在單一流體化床之系統,透過pHe、Ba/B、H2O2/B、床高、HRT等變因探討,針對硼濃度600~700 ppm的合成廢水,得以在最佳操作條件下(pHe=9.90、Ba/B=0.84、H2O2/B=1.71、HRT=18 min、靜置床高大於45cm),達到80%的硼總去除率與75%的硼顆粒化率;透過改變進料硼濃度可知單一流體化床除硼系統的最大截面積負荷量為1.6 kg-B/m2·hr;資源化之均質顆粒經由XRD、TEM、Raman交叉比對分析,推測其成分為非結晶相的Ba(B(OH)3OOH)2。流體化床串聯系統則具備處理高濃度含硼廢水(CB,in > 700 ppm)的能力,藉由鋇沉澱劑的分散進料,最終硼總去除率與硼顆粒化率分別可達到80~84%與78%;若於串聯之流體化床填入結晶相沉澱物BaB(OH)2(OO)2B(OH)2作為晶種使用,則可將單一流體化床出流水的殘餘硼溶液有效降至10 ppm以下,系統之硼總去除率(TR)達97.5%,硼顆粒化率(GR)達80%,水質濁度則低於5 NTU。
關鍵字:化學過氧沉澱、流體化床均質顆粒化、流體化床串聯系統、晶種(BaB(OH)2(OO)2B(OH)2)
This study investigated the boron recovery from wastewater as moisture content and high purity barium perborate particles by integrating Chemical Oxo-Precipitation with Fluidized-Bed Homogeneous Granulation methods. FBHG-COP could recover boron from wastewater and improve quality of water instead of chemical precipitation producing high moisture content sludge. At research of single FBR system, investigated effect of pHe, molar ratio of Ba/B and H2O2/B, height of column, and HRT for boron wastewater containing 600~700 ppm-B. When operated suitable conditions (pHe=9.90、Ba/B=0.84、H2O2/B=1.71、HRT=18 min、height of column > 45 cm) , the total boron removal ratio (TR) and boron granulation ratio (GR) would get 80% and 75%, respectively. The maximum surface loading of FBHG-COP was 1.6 kg-B/m2·hr by effect of CB,in on boron recovery experiment. The homogeneous particle was Ba(B(OH)3OOH)2 by XRD, TEM, and Raman analysis. The system of FBRs in series could efficiency treat CB,in > 700 ppm wastewater by dividing barium input into half to each reactor. The TR and GR were 80~84% and 78%, respectively. The boron concentration of final effluent water could effectively reduce lower than 10 ppm by adding BaB(OH)2(OO)2B(OH)2 into second FBR. The TR, GR, and turbidity were 97.5%, 80%, and lower than 5 NTU, respectively.
[1] D. M. Schubert and R. J. Brotherton, "Boron: Inorganic Chemistry," in Encylopedia of Inorganic Chemistry, R. A. Scott, Ed., ed John Wiley & Sons, Ltd, 2006.
[2] N. Hilal, G. J. Kim, and C. Somerfield, "Boron removal from saline water: A comprehensive review," Desalination, vol. 273, pp. 23-35, 2011.
[3] P. D. Howe, "A review of boron effects in the environment," Biological trace element research, vol. 66, pp. 153-166, 1998.
[4] M. Tagliabue, A. P. Reverberi, and R. Bagatin, "Boron removal from water: needs, challenges and perspectives," Journal of Cleaner Production, vol. 77, pp. 56-64, 2014.
[5] D. M. Schubert, "Borates in Industrial Use," in Group 13 Chemistry III, H. Roesky and D. Atwood, Eds., ed: Springer Berlin Heidelberg, 2003, pp. 1-40.
[6] J. Anderson, E. Eyring, and M. Whittaker, "Temperature Jump Rate Studies of Polyborate Formation in Aqueous Boric Acid1," The Journal of Physical Chemistry, vol. 68, pp. 1128-1132, 1964.
[7] P. Argust, "Distribution of boron in the environment," Biological trace element research, vol. 66, pp. 131-143, 1998.
[8] A. E. Yilmaz, R. Boncukcuoglu, and M. M. Kocakerim, "A quantitative comparison between electrocoagulation and chemical coagulation for boron removal from boron-containing solution," J Hazard Mater, vol. 149, pp. 475-81, Oct 22 2007.
[9] D. Mohapatra, G. R. Chaudhury, and K. H. Park, "Recovery of boron from wastewater using 2, 2, 4-trimethyl-1, 3-pentanediol in carbon tetrachloride," Indian Journal of Chemical Technology, vol. 15, p. 483, 2008.
[10] O. C. Türker, J. Vymazal, and C. Türe, "Constructed wetlands for boron removal: A review," Ecological Engineering, vol. 64, pp. 350-359, 2014.
[11] "Chemical econamic hand book," in Boron Minerals and Chemicals, 1990.
[12] "TURKEY AS THE GLOBAL LEADER IN BORON EXPORT & PRODUCTION," in European Association of Service Providers for Persons with Disabilities Annual Conference, 2013.
[13] T. Itakura, R. Sasai, and H. Itoh, "In situ solid/liquid separation effect for high-yield recovery of boron and fluorine from aqueous media containing borate or fluoroborate ions," Bulletin of the Chemical Society of Japan, vol. 80, pp. 2014-2018, 2007.
[14] E. J. Shin, W. S. Lyoo, and Y. H. Lee, "Effect of boric acid treatment method on the characteristics of poly (vinyl alcohol)/iodine polarizing film," Journal of Applied Polymer Science, vol. 123, pp. 672-681, 2012.
[15] 林孟儒, "以化學方法去除廢水中硼之研究," Master, 環境與安全工程所, 國立雲林科技大學, 2010.
[16] B. Chetelat and J. Gaillardet, "Boron isotopes in the Seine River, France: a probe of anthropogenic contamination," Environmental science & technology, vol. 39, pp. 2486-2493, 2005.
[17] K. Warington, "The effect of boric acid and borax on the broad bean and certain other plants," Annals of Botany, vol. 37, pp. 629-672, 1923.
[18] L. Bolanos, E. Esteban, C. de Lorenzo, M. Fernandez-Pascual, M. R. de Felipe, A. Garate, et al., "Essentiality of boron for symbiotic dinitrogen fixation in pea (Pisum sativum) rhizobium nodules," Plant physiology, vol. 104, pp. 85-90, 1994.
[19] Y. Xu and J.-Q. Jiang, "Technologies for boron removal," Industrial & Engineering Chemistry Research, vol. 47, pp. 16-24, 2008.
[20] F. H. Nielsen, "Update on human health effects of boron," J Trace Elem Med Biol, vol. 28, pp. 383-7, Oct 2014.
[21] J. Wolska and M. Bryjak, "Methods for boron removal from aqueous solutions — A review," Desalination, vol. 310, pp. 18-24, 2013.
[22] W. A. Robbins, L. Xun, J. Jia, N. Kennedy, D. A. Elashoff, and L. Ping, "Chronic boron exposure and human semen parameters," Reprod Toxicol, vol. 29, pp. 184-90, Apr 2010.
[23] WHO, "Chapter 8. Chemical aspects," in Guidelines for drinking-water quality, WHO, Ed., ed: WHO, 2011, pp. 155-201.
[24] C. Irawan, Y.-L. Kuo, and J. C. Liu, "Treatment of boron-containing optoelectronic wastewater by precipitation process," Desalination, vol. 280, pp. 146-151, 2011.
[25] D. Hasson, H. Shemer, I. Brook, I. Zaslavschi, R. Semiat, C. Bartels, et al., "Scaling propensity of seawater in RO boron removal processes," Journal of Membrane Science, vol. 384, pp. 198-204, 2011.
[26] E. Güler, C. Kaya, N. Kabay, and M. Arda, "Boron removal from seawater: State-of-the-art review," Desalination, vol. 356, pp. 85-93, 2015.
[27] B. Wang, X. Guo, and P. Bai, "Removal technology of boron dissolved in aqueous solutions – A review," Colloids and Surfaces A: Physicochemical and Engineering Aspects, vol. 444, pp. 338-344, 2014.
[28] P. Dydo and M. Turek, "Boron transport and removal using ion-exchange membranes: A critical review," Desalination, vol. 310, pp. 2-8, 2013.
[29] I. Kipcak and M. Ozdemir, "Boron recovery from clay waste using Diaion CRB-02 resin," Environ Technol, vol. 31, pp. 327-35, Mar 2010.
[30] C. Irawan, J. Liu, and C.-C. Wu, "Removal of boron using aluminum-based water treatment residuals (Al-WTRs)," Desalination, vol. 276, pp. 322-327, 2011.
[31] J. Liu, X. Guo, and J. Yuan, "Synthesis of Mg/Al double-layered hydroxides for boron removal," Desalination and Water Treatment, vol. 52, pp. 1919-1927, 2013.
[32] F. Fu and Q. Wang, "Removal of heavy metal ions from wastewaters: a review," Journal of environmental management, vol. 92, pp. 407-418, 2011.
[33] A. E. Yilmaz, R. Boncukcuoğlu, S. Bayar, B. A. Fil, and M. M. Kocakerim, "Boron removal by means of chemical precipitation with calcium hydroxide and calcium borate formation," Korean Journal of Chemical Engineering, vol. 29, pp. 1382-1387, 2012.
[34] P. Remy, H. Muhr, E. Plasari, and I. Ouerdiane, "Removal of boron from wastewater by precipitation of a sparingly soluble salt," Environmental progress, vol. 24, pp. 105-110, 2005.
[35] H. C. Tsai and S. L. Lo, "Boron removal and recovery from concentrated wastewater using a microwave hydrothermal method," J Hazard Mater, vol. 186, pp. 1431-7, Feb 28 2011.
[36] A. E. Yilmaz, R. Boncukcuoglu, M. M. Kocakerim, M. T. Yilmaz, and C. Paluluoglu, "Boron removal from geothermal waters by electrocoagulation," J Hazard Mater, vol. 153, pp. 146-51, May 1 2008.
[37] J.-Q. Jiang, N. Graham, C. André, G. H. Kelsall, and N. Brandon, "Laboratory study of electro-coagulation–flotation for water treatment," Water research, vol. 36, pp. 4064-4078, 2002.
[38] J.-Q. Jiang, Y. Xu, K. Quill, J. Simon, and K. Shettle, "Mechanisms of boron removal with electrocoagulation," Environmental Chemistry, vol. 3, pp. 350-354, 2006.
[39] M. H. Isa, E. H. Ezechi, Z. Ahmed, S. F. Magram, and S. R. Kutty, "Boron removal by electrocoagulation and recovery," Water Res, vol. 51, pp. 113-23, Mar 15 2014.
[40] Y. J. Shih, C. H. Liu, W. C. Lan, and Y. H. Huang, "A novel chemical oxo-precipitation (COP) process for efficient remediation of boron wastewater at room temperature," Chemosphere, vol. 111, pp. 232-7, Sep 2014.
[41] J.-Y. Lin, Y.-J. Shih, P.-Y. Chen, and Y.-H. Huang, "Precipitation recovery of boron from aqueous solution by chemical oxo-precipitation at room temperature," Applied Energy, 2015.
[42] M. E. Deary, M. C. Durrant, and D. M. Davies, "A kinetic and theoretical study of the borate catalysed reactions of hydrogen peroxide: the role of dioxaborirane as the catalytic intermediate for a wide range of substrates," Org Biomol Chem, vol. 11, pp. 309-17, Jan 14 2013.
[43] Y. S. Sadovskii, T. Solomoichenko, T. Prokop’eva, Z. P. Piskunova, N. Razumova, B. Panchenko, et al., "Reactivity of the H2O2/B (OH) 3/HO-system in the decomposition of 4-nitrophenyl esters of diethylphosphonic and diethylphosphoric acids," Theoretical and Experimental Chemistry, vol. 48, pp. 163-171, 2012.
[44] M. C. Durrant, D. M. Davies, and M. E. Deary, "Dioxaborirane: a highly reactive peroxide that is the likely intermediate in borate catalysed electrophilic reactions of hydrogen peroxide in alkaline aqueous solution," Org Biomol Chem, vol. 9, pp. 7249-54, Oct 21 2011.
[45] B. Chernyshov, "The formation, composition, structure, and identification of peroxoborates in solution," Russian journal of inorganic chemistry, vol. 35, pp. 1333-1335, 1990.
[46] 林睿彥, "鋇系化學過氧沉澱程序回收高濃度含硼廢水中的硼," Master, Chemical Engineering, National Cheng Kung University, 2015.
[47] C. W. Jones, Applications of hydrogen peroxide and derivatives vol. 2: Royal Society of Chemistry, 1999.
[48] 黃國豪等人, "含硼廢水的處理方法," Taiwan Patent, 2002.
[49] J. Flanagan, W. P. Griffith, R. D. Powell, and A. P. West, "Vibrational spectra of alkali metal peroxoborates," Spectrochimica Acta Part A: Molecular Spectroscopy, vol. 45, pp. 951-955, 1989.
[50] J. Flanagan, W. P. Griffith, R. D. Powell, and A. P. West, "Nature of peroxoborate species in aqueous solution: a study by boron-11 nuclear magnetic resonance and Raman spectroscopy," Journal of the Chemical Society, Dalton Transactions, pp. 1651-1655, 1989.
[51] R. van Lier, C. Buisman, and A. Giesen, "Crystalactor® technology and its applications in the mining and metallurgical industry," Paques B.V.2005.
[52] 陳政澤, "流體化床結晶反應槽回收廢水中重金屬鎘之研究," Master, 環境工程學系, 國立中央大學, 1995.
[53] K. N. Ohlinger, T. M. Young, and E. D. Schroeder, "Postdigestion struvite precipitation using a fluidized bed reactor," Journal of Environmental Engineering, vol. 126, pp. 361-368, 2000.
[54] 張華強, "以流體化床反應器開發均相成核與結晶之新穎除磷技術," Master, Chemical Engineering, National Cheng Kung University, 2012.
[55] C.-S. Chen, Y.-J. Shih, and Y.-H. Huang, "Remediation of lead (Pb(II)) wastewater through recovery of lead carbonate in a fluidized-bed homogeneous crystallization (FBHC) system," Chemical Engineering Journal, vol. 279, pp. 120-128, 2015.
[56] 劉佳勳, "以化學過氧沉澱(COP)技術回收含硼酸廢液研究," Master, Chemical Enginnering, National Cheng Kung University, 2013.
[57] J. Dirksen and T. Ring, "Fundamentals of crystallization: kinetic effects on particle size distributions and morphology," Chemical Engineering Science, vol. 46, pp. 2389-2427, 1991.
[58] 劉志忠, "流體化床結晶法去除水中磷酸鹽之研究," Master, 環境工程學系, 國立中央大學, 1998.
[59] 陳寶琪, "微溶物系之沉澱與結晶," PhD, 化學工程學系, 國立台灣大學, 1987.
[60] 李嘉宜, "以流體化床反應器處理含銅廢水之研究," PhD, 環境工程學系, 國立台灣大學, 2005.
[61] 石政怡, "次成核的機構和其在結晶程序上之應用," PhD, 化學工程學系, 國立台灣大學, 1996.
[62] K. L. Tu, L. D. Nghiem, and A. R. Chivas, "Boron removal by reverse osmosis membranes in seawater desalination applications," Separation and Purification Technology, vol. 75, pp. 87-101, 2010.
[63] 張鈞期, "不同金屬藥劑的流體化床結晶技術處理含磷廢水之研究," Mater, Chemical Engineering, National Cheng Kung University, 2009.
[64] C. J. Adams and I. E. Clark, "On the nature of the peroxoborate ion in solution," Polyhedron, vol. 2, pp. 673-675, 1983.