| 研究生: |
陳玫璇 Chen, Mei-Hsuan |
|---|---|
| 論文名稱: |
利用合成之銅鐵氧化物奈米顆粒探討溶液中鉛的吸附行為 Evaluation of Lead Adsorption Using Synthesized Copper Ferrite Magnetic Nano-particles |
| 指導教授: |
游鎮烽
You, Chen-Feng |
| 學位類別: |
碩士 Master |
| 系所名稱: |
理學院 - 地球科學系 Department of Earth Sciences |
| 論文出版年: | 2015 |
| 畢業學年度: | 103 |
| 語文別: | 英文 |
| 論文頁數: | 76 |
| 中文關鍵詞: | 鉛 、銅鐵氧化物奈米顆粒 、吸附 、脫附 、富集 |
| 外文關鍵詞: | Lead, copper ferrite nano–particles, adsorption, desorption, pre-concentration |
| 相關次數: | 點閱:121 下載:2 |
| 分享至: |
| 查詢本校圖書館目錄 查詢臺灣博碩士論文知識加值系統 勘誤回報 |
自十九世紀工業革命以來,金屬鉛已廣泛地使用於工業產品中,為不可或缺的原料之一。然而,由於含鉛廢棄物及工業廢水的不當處置,含高濃度鉛之廢液因而排放到自然界眾多水域之中。鉛為具毒性的無機污染物之一,即使在地表水中的濃度低(即26–100 μg L-1),仍對於生物體有非常大之危害。兒童體內中血液鉛的濃度一旦高於100 μg L-1,鉛之毒性即開始攻擊中樞神經系統,嚴重者則會影響心智功能的發展。因此,發展有效移除水體中鉛的技術為現今科學界關注之重要議題。本研究欲使用工業污泥所製成之銅鐵氧化物奈米顆粒,探討在不同酸鹼值、吸附時間、鉛之初使濃度及不同溶液基質下,水溶液鉛之移除效能;此外,本研究亦評估此合成材料是否可經由吸附–脫附的過程,將鉛自水體中富集、濃縮,並發展一全新鉛之純化技術。研究結果顯示,利用銅鐵氧磁體奈米顆粒進行鉛之吸附,在pH 4.5、溫度298 K下,其移除效率高達90%;其吸附過程皆符合擬二階動力吸附式及Langmuir等溫吸附模型,並由Langmuir吸附式可得在pH 4.5、溫度298 K下,鉛於銅鐵氧化物奈米顆粒之飽和吸附量為17.83 mg g-1。此外,由鉛之吸附量隨著溶液中離子強度增加而下降之情形推斷,鉛之吸附行為應屬外層錯合;並由模擬海水結果顯示,鉛之吸附量不隨溶液中陽離子競爭吸附效應而有顯著影響。在脫附實驗中,吾人使用濃度0.005 N硝酸為脫附試劑,得其平均脫附率約為75%;並由此材料之消化實驗,得鉛含量為0.314±0.003 mg g-1,因此推論在進行脫附實驗時,約有339.34±2.99 ng鉛由銅鐵氧化物奈米顆粒溶出。本研究使用工業汙泥製成之低成本材料,除了可同時處理、再生汙泥及廢水外,也可應用於鉛在自然界水體中之有效富集,為一具有前瞻性之技術。
Lead (Pb) has been used extensively for many industrial purposes since the 19th century industrial revolution. However, Pb pollution can be found in various aquatic systems due to improper management of Pb contained waste or waste water. Being one of the major toxic inorganic pollutants, Pb can pose serious threat to living creatures at rather low concentration of 26–100 μg L-1. Once the blood lead (PbB) level of children exceeds 100 μg L-1, the central nervous system would damage and the body function may exhibit anomalous. Therefore, development of Pb remediation for drinking waters is critical and required. In this study, copper ferrite nano–particles (CuFe2O4) manufactured from industrial sludge were employed to evaluate aqueous Pb adsorption–desorption under various pHs, duration, initial Pb concentrations and solution matrix. Furthermore, a prospective study will be evaluated for Pb pre–concentration through the adsorption and desorption procedure. Our results indicated that the function of pH in sorption capacity of CuFe2O4 nano–particles was insignificantly, and reached the value of up to 90% at pH of 4.5. The adsorption kinetics fit well with pseudo–second–order model which suggests that Pb adsorption is a fast kinetics. Furthermore, the sorption isotherm fits well with the Langmuir model, and the maximum adsorption capacity of Pb was estimated to be 17.83 mg per gram sorbent at pH of 4.5 and temperature of 298 K. On the other hand, the ionic strength and coexisting cation showed negligible effect on Pb adsorption under seawater–like matrix. In desorption experiments, 0.005N HNO3 was evaluated as the best condition for Pb desorption with recovery of 75% in average, which enables Pb recycled and regenerated. In addition, Pb contents in CuFe2O4 were estimated 0.314±0.003 mg g-1 by digestion, and we infer that approximately 339.34±2.99 ng of Pb contribute to solution during desorption process. Overall, the novel low–cost fabricated CuFe2O4 from industrial sludge waste can be applied effectively for Pb remediation in aqueous solutions, not only deal with the danger of sludge waste and waste water, but also be considered as a reusable and cost–effective technique. On the other hand, through adsorption–desorption process, it demonstrates a potential application in Pb enrichment through simple operation procedure of adsorption and desorption.
Aderhold, D., Williams, C. J. and Edyvean, R. G. J. (1996) The Removal of Heavy-metal Ions by Seaweeds and Their Derivatives. Bioresource Technology, 58, pp. 1-6.
Adiano, D. C. (2001) Trace Elements in Terrestrial Environments: biogeochemistry, bioavailability, and risks of metals. Springer-Verlag, New York, I, pp. 1-867.
Agelidis, T., Fytianos, K., Vasilikiotis, G. and Jannakoudakis, D. (1988) Lead Removal from Waste-water by Cementation Utilizing a Fixed-bed of Iron Sphere. Environmental Pollution, 50, pp. 243-251.
Ahmed, Y. M. Z., Hessien, M. M., Rashad, M. M. and Ibrahim, I. A. (2009) Nano-crystalline Copper Ferrites from Secondary Iron Oxide (mill scale). Journal of Magnetism and Magnetic Materials, 321, pp. 181-187.
Apak, R. (2002) Adsorption of Heavy metal Ions on Soil Surfaces and Similar Substances. In: Hubbard, A. T. (Ed.) Encyclopedia of Surface and Colloid Science.
Benjamin, M., M. and Leckie, J., O. (1981) Multiple-Site Adsorption of Cd, Cu, Zn, and Pb on Amorphous Iron Oxyhydroxide. Journal of colloid and interface science, 79, pp. 209-221.
Bhattacharyya, K. G. and Gupta, S. S. (2008) Adsorption of a Few Heavy Metals on Natural and Modified Kaolinite and Montmorillonite: a Review. Advances in colloid and interface science, 140, pp. 114-131.
Bollhöfer, A. and Rosman, K. J. R. (2001) Isotopic source signatures for atmospheric lead The Northern Hemisphere. Geochimica et Cosmochimica Acta, 65, pp. 1727-1740.
Bradl, H. B. (2004) Adsorption of Heavy Metal Ions on Soils and Soils Constituents. Journal of colloid and interface science, 277, pp. 1-18.
Brunauer, S. (1944) The Adsorption of Gases and Vapours. Oxford University Press, London, pp. 150.
Erdem, M. and Tumen, F. (2004) Chromium Removal from Aqueous Solution by Ferrite Process. Journal of Hazardous Materials, 109, pp. 71-77.
Fedje, K. K., Ekberg, C., Skarnemark, G. and Steenari, B. M. (2010) Removal of Hazardous Metals from MSW Fly Ash-An Evaluation of Ash Leaching Methods. Journal of Hazardous Materials, 173, pp. 310-317.
Freundlich, H. M. F. (1906) Over the Adsorption in Solution. Journal of Physical Chemistry, 57, pp. 385-470.
Fu, F. and Wang, Q. (2011) Removal of Heavy Metal Ions from Wastewaters: a Review. Journal of environmental management, 92, pp. 407-418.
Giles, C. H., Macewan, T. H., Nakhwa, S. N. and Smith, D. (1960) Studies in Adsorption. Part XI. A system of Classification of Solution Adsorption Isotherms, and its Diagnosis of Adsorption Mechanisms and in Measurement of Specific Surface Areas of Solids. Journal of the Chemical Society, pp. 3973-3993.
Goel, J., Kadirvelu, K., Rajagopal, C. and Garg, V. K. (2005) Removal of Lead(II) from Aqueous Solution by Adsorption on Carbon Aerogel Using a Response Surface Methodological Approach. Industrial and Engineering Chemistry Research, 44, pp. 1987-1994.
Gupta, V. K., Carrott, P. J. M., Ribeiro Carrott, M. M. L. and Suhas (2009) Low-Cost Adsorbents: Growing Approach to Wastewater Treatment—a Review. Critical Reviews in Environmental Science and Technology, 39, 783-842.
Herrera, P., Uchiyama, H., Igarashi, T., Asakura, K., Ochi, Y., Iyatomi, N. and Nagae, S. (2007) Treatment of Acid Mine Drainage through a Ferrite Formation Process in Central Hokkaido, Japan: Evaluation of Dissolved Silica and Aluminium Interference in Ferrite Formation. Minerals Engineering, 20, pp. 1255-1260.
Ho, Y. S. and McKay, G. (1998) Sorption of Dye from Aqueous Solution by Peat. Chemical Engineering Journal, 70, pp. 115-124.
Ho, Y. S. and McKay, G. (1999) Pseudo-second Order Model for Sorption Processes. Process Biochemistry, 34, pp. 451-465.
Hu, H., Wang, Z. and Pan, L. (2010) Synthesis of monodisperse Fe3O4@silica core–shell microspheres and their application for removal of heavy metal ions from water. Journal of Alloys and Compounds, 492, pp. 656-661.
Hua, M., Zhang, S., Pan, B., Zhang, W., Lv, L. and Zhang, Q. (2012) Heavy Metal Removal from Water/Wastewater by Nanosized Metal Oxides: a review. Journal of Hazardous Materials, 211-212, pp. 317-331.
Kurniawan, T. A., Chan, G. Y. S., Lo, W.-H. and Babel, S. (2006) Physico–chemical Treatment Techniques for Wastewater Laden with Heavy Metals. Chemical Engineering Journal, 118, pp. 83-98.
Lagergren, S. (1898) About the Theory of So-called Adsorption of Soluble Substances. Kungliga Svenska Vetenskapsakademiens. Handlingar, 24, pp. 1-39.
Lai, C. H. and Chen, C. Y. (2001) Removal of Metal Ions and Humic Acid from Water by Iron-coated Filter Media. Chemosphere, 44, pp.1177-1184.
Langmuir, I. (1918) The Adsorption of Gases on Plane Surfaces of Glass, Mica and Platinum. Journal of American Chemical Society, 40, pp. 1361-1408.
Li, N. H., Lo, S. L., Hu, C. Y., Hsieh, C. H. and Chen, C. L. (2011) Stabilization and Phase Transformation of CuFe2O4 Sintered from Simulated Copper-laden Sludge. Journal of Hazardous Materials, 190, pp. 597-603.
Li, Y. H. (1982) A brief discussion on the mean oceanic residence time of elements. Geochimica et Cosmochimica Acta, 46, pp. 671-675.
Li, Y. H., Di, Z., Ding, J., Wu, D., Luan, Z. and Zhu, Y. (2005) Adsorption Thermodynamic, Kinetic and Desorption Studies of Pb2+ on Carbon Nanotubes. Water research, 39, pp. 605-609.
Liu, J. F., Zhao, Z. S. and Jiang, G. B. (2008) Coating Fe3O4 Magnetic Nanoparticles with Humic Acid for High Efficient Removal of Heavy Metals in Water. Environmental Science & Technology, 42, pp. 6949-6954.
Madaeni, S. S. and Mansourpanah, Y. (2003) COD Removal from Concentrated Wastewater Using Membranes. Filtration & Separation, 40, pp. 41-46.
Mushak, P., Davis, J. M., Crocetti, A. F. and Grant, L. D. (1989) Prenatal and Postnatal Effects of Low-Level Lead Exposure: Integrated Summary of a Report to the U.S. Congress on Childhood Lead Poisoning. Environmental Research, 50, pp. 11-36.
Namasivayam, C. and Prathap, K. (2006) Uptake of Molybdate by Adsorption Onto Industrial Solid Waste Fe(III)/Cr(III) Hydroxide: Kinetic and Equilibrium Studies. Environmental technology, 27, pp. 923-932.
Nassar, N. N. (2010) Rapid Removal and Recovery of Pb(II) from Wastewater by Magnetic Nanoadsorbents. Journal of Hazardous Materials, 184, pp. 538-546.
Nojiri, N., Tanaka, N., Sato, K. and Sakai, Y. (1980) Electricity Ferrite Formation System for Heavy-metal Removal. Journal Water Pollution Control Federation, 52, pp. 1898-1906.
Nosier, S. A. and Sallam, S. A. (2000) Removal of Lead Ions from Wastewater by Cementation on a Gas-sparged Zinc Cylinder. Separation and Purification Technology, 18, pp. 93-101.
O'Connell, D. W., Birkinshaw, C. and O'Dwyer, T. F. (2008) Heavy Metal Adsorbents Prepared from The Modification of Cellulose: A Review. Bioresource Technology, 99, pp. 6709-6724.
Paul, M., Bridgestock, L., Rehkamper, M., van DeFlierdt, T. and Weiss, D. (2015) High-precision Measurements of Seawater Pb Isotope Compositions by Double Spike Thermal Ionization Mass Spectrometry. Analytica Chimuca Acta, 863, pp. 59-69.
Qin, J. J., Wai, M. N., Oo, M. H. and Wong, F. S. (2002) A Feasibility Study on The Treatment and Recycling of A Wastewater from Metal Plating. Journal of Membrane Science, 208, pp. 213-221.
Quinby-Hunt, M. S. and Turekian, K. K. (1983) Distribution of elements in sea water. EOS, Transactions of the American Geophysical Union, 64, pp. 130-132.
Roy, S. and Ghose, J. (2006) Möessbauer Study of Nanocrystalline Cubic CuFe2O4 Synthesized by Precipitation in Polymer Matrix. Journal of Magnetism and Magnetic Materials, 307, pp. 32-37.
Sayilgan, E., Kukrer, T., Yigit, N. O., Civelekoglu, G. and Kitis, M. (2010) Acidic Leaching and Precipitation of Zinc and Manganese from Spent Battery Powders using Various Reductants. Journal of Hazardous Materials, 173, pp. 137-143.
Selvan, R. K., Augustin, C. O., Berchmans, L. J. and Saraswathi, R. (2003) Combustion Synthesis of CuFe2O4. Materials Research Bulletin, 38, pp. 41-54.
Sen Gupta, S. and Bhattacharyya, K. G. (2005) Interaction of Metal Ions with Clays: I. a Case Study with Pb(II). Applied Clay Science, 30, pp. 199-208.
Shaheen, S. M., Tsadilas, C. D. and Rinklebe, J. (2013) A Review of the Distribution Coefficients of Trace Elements in Soils: Influence of Sorption System, Element Characteristics, and Soil Colloidal Properties. Advances in colloid and interface science, 201-202, pp. 43-56.
Sheng, G. D., Wang, S. W., Hu, J., Lu, Y., Li, J. X., Dong, Y. H. and Wang, X. K. (2009) Adsorption of Pb(II) on Diatomite as Affected via Aqueous Solution Chemistry and Temperature. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 339, pp. 159-166.
Sposito, G. (1984) The Surface Chemistry of Soils.
Sposito, G. (2004) The Surface Chemistry of Natural Particles.
Tamaura, Y., Katsura, T., Rojarayanont, S., Yoshida, T. and Abe, H. (1991) Ferrite Process - Heavy Metal Ions Treatment System. Water Science and Technology, 23, pp. 1893-1900.
Tao, S. W., Gao, F., Liu, X. Q. and Sorensen, O. T. (2000) Preparation and Gas-sensing Properties of CuFe2O4 at Reduced Temperature. Materials Science and Engineering B-Solid State Materials for Advanced Technology, 77, pp. 172-176.
Tu, Y. J., Chang, C. K., You, C. F. and Lou, J. C. (2010) Recycling of Cu Powder from Industrial Sludge by Combined Acid Leaching, Chemical Exchange and Ferrite Process. Journal of Hazardous Materials, 181, pp. 981-985.
Tu, Y. J. and You, C. F. (2014) Phosphorus Adsorption onto Green Synthesized Nano-bimetal Ferrites: Equilibrium, Kinetic and Thermodynamic Investigation. Chemical Engineering Journal, 251, pp. 285-292.
Tu, Y. J., You, C. F. and Chang, C. K. (2012a) Kinetics and Thermodynamics of Adsorption for Cd on Green Manufactured Nano-particles. Journal of Hazardous Materials, 235-236, pp. 116-122.
Tu, Y. J., You, C. F., Chang, C. K., Chan, T. S. and Li, S. H. (2014) XANES Evidence of Molybdenum Adsorption onto Novel Fabricated Nano-magnetic CuFe2O4. Chemical Engineering Journal, 244, pp. 343-349.
Tu, Y. J., You, C. F., Chang, C. K., Wang, S. L. and Chan, T. S. (2012b) Arsenate Adsorption from Water Using a Novel Fabricated Copper Ferrite. Chemical Engineering Journal, 198-199, pp. 440-448.
Veysseyre, A. M., Bollhöfer, A. F., Rosman, K. J. R., Ferrari, C. P. and Boutron, C. F. (2001) Tracing the origin of pollution in French Alpine snow and aerosols using lead isotopic ratios. Environmental Science & Technology, 35, pp. 4463-4469.
Wang, Y.-H., Lin, S.-H. and Juang, R.-S. (2003) Removal of HeavyMmetal Ions from Aqueous Solutions Using Various Low-cost Adsorbents. Journal of Hazardous Materials, 102, pp. 291-302.
Wu, Z., Gu, Z., Wang, X., Evans, L. and Guo, H. (2003) Effects of Organic Acids on Adsorption of Lead onto Montmorillonite, Goethite and Humic Acid. Environmental Pollution, 121, pp. 469-475.
Yu, B., Zhang, Y., Shukla, A., Shukla, S. S. and Dorris, K. L. (2001) The Removal of Heavy Metals from Aqueous Solutions by Sawdust Adsorption— Removal of Lead and Comparison of its Adsorption with Copper. Journal of Hazardous Materials, B84, pp. 83-94.
Yu, X., Tong, S., Ge, M., Wu, L., Zuo, J., Cao, C. and Song, W. (2013) Adsorption of heavy metal ions from aqueous solution by carboxylated cellulose nanocrystals. Journal of Environmental Sciences, 25, pp. 933-943.