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  1. NTU Theses and Dissertations Repository
  2. 工學院
  3. 環境工程學研究所
請用此 Handle URI 來引用此文件: http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/38851
完整後設資料紀錄
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dc.contributor.advisor駱尚廉(Shang-Lien Lo)
dc.contributor.authorPing-Ju Tsaien
dc.contributor.author蔡秉儒zh_TW
dc.date.accessioned2021-06-13T16:49:10Z-
dc.date.available2011-07-29
dc.date.copyright2011-07-29
dc.date.issued2011
dc.date.submitted2011-07-15
dc.identifier.citationAlejandre, A., Medina, F., Salagre, P., Fabregat, A., Sueiras, J.E., Characterization and activity of copper and nickel catalysts for the oxidation of phenol aqueous solutions. Applied catalysis B: Environmental 18 (1998) 307-315.
Bhattacharyya, A.A., Woltermann, G.M., Yoo, J.S., Karch, J.A., Cormier, W.E., Catalytic sox abatement-the role of magnesium aluminate spinel in the removal of sox from fluid catalytic cracking (FCC) flue-gas. Ind. Eng. Chem. Res. 27 (1988) 1356-1360.
Bonen, D., Sarker, S.L., The effect of simulated environmental attack on immobilization of heavy metal doped in cement-based materials. J. Hazard. Mater. 13 (1995) 545-552.
Cheeseman, C.R, Butcher, E.J., Sollars, C.J., Perry, R., Heavy metal leaching from hydroxide, sulphide and silicate stabilized/solidified wastes. Waste Manage. 13 (1993) 545-552.
Chen, C.L., Lo, S.L., Kuan, W.H., Hsieh, C.H., Stabilization of Cu in acid-extracted industrial sludge using a microwave process. J. Hazard. Mater. B123 (2005) 256-261.
Chen, Y.C., Titanate nanotubes synthesized by microwave hydrothermal method: study on their adsorption and photocatalytic potential. Ph.D. Dissertation, Graduate Institute of Environmental Engineering, National Taiwan University, R.O.C. (2011)
Cheng, Y.T., Spinel formation for stabilization of copper- and aluminum- containing sludge by high temperature process. Master thesis, Graduate Institute of Environmental Engineering, National Taiwan University, R.O.C. (2009)
Chiang, Y. M., Birnie, D.P., III, Kingery, W. D., Physical Ceramics. John Willy & Sons, Inc., United States (1997)
Ding, D., Long, M., Cai, W., Wu, Y., Wu, D., Chen, C., In-situ synthesis of photocatalytic CuAl2O4-Cu hybrid nanorod arrays. Chem. Commun. (2009) 3588-3590.
Fan, Y., Lu, X., Ni, Y., Zhang, H., Zhao, L., Chen, J., Sun, C., Destruction of polychlorinated aromatic compounds by spinel-type complex oxides. Environ. Sci Technol. 44 (2010) 3079-3084.
Faungnawakij, K., Fukunaga, T., Kikuchi, R., Eguchi, K., Deactivation and regeneration behaviors of copper spinel-alumina composite catalysts in steam reforming of dimethyl ether. J. Catalysis 256 (2008) 37-44.
Fogler, H.S., Elements of chemical reaction engineering. 4th Ed., Pearson education, the United States (2006) 650-651.
Foll, H., Ionic crystals: spinel structure. German, http://www.tf.uni-kiel.de/matwis/amat/def_en/index.html (Apr. 2011)
Gherbia, R., Nasrallah, N., Amrane, A., Maachi, R., Trari, M., Photocatalytic reduction of Cr(VI) on the new hetero-system CuAl2O4/TiO2. J. Hazard. Mater. 186 (2011) 1124-1130.
Hu, C.Y., Shih, K., Leckie, J.O., Formation of copper aluminate spinel and couprous aluminate delafossite to thermally stabilize simulated copper-laden sludge. J. Hazard. Mater. 181 (2010) 399-404.
Hsieh, C.H., Microwave enhanced reclamation of heavy metal sludge. Ph.D. Dissertation, Graduate Institute of Environmental Engineering, National Taiwan University, R.O.C. (2008)
Jebarathinam, N.J., Eswaramoorthy, M., Krishnasamy, V., Nonoxidative and oxidative dehydrogenation of ethylbenzene over Zn-Fe-Cr ternary spinel system. Appl. Catal., A 145 (1996) 57–74.
Jiang, Y.Y., Li, J.G., Sui, X.T., Ning, G.L., Wang, C.Y., Gu, X.M., CuAl2O4 powder synthesis by sol-gel method and its photodegradation property under visible light irradiation. J. Sol-Gel Sci. Techn. 42 (2007) 41-45.
Kebir, M., Chabani, M., Nasrallah, N., Bensmaili, A., Trari, M., Coupling adsorption with photocatalysis process for the Cr(VI) removal. J. Desal. 270 (2011) 166-173.
Lv, W., Liu, B., Qiu, Q., Wang, F., Lou, Z., Zhang, P., Wei, S., Synthesis, characterization and photocatalytic properties of spinel CuAl2O4 nanoparticals by a sonochemical method. J. Alloys and Compounds. 479 (2009) 480-483.
Mehandjiev, D., Naydenov, A., Ivanov, G., Ozone decomposition, benzene and CO oxidation over NiMnO3-ilmenite and NiMn2O4-spinel catalysts. Appl. Catal., A, 206 (2001) 13-18.
Park, D., Lee, D.S., Park, J.M., Chun, H.D., Park, S.K., Jitsuhara, I., Miki, O., Kato, T., Metal recovery from electroplating wastewater using acidophilic iron oxidizing bacteria: pilot-scale feasibility test. Ind. Eng. Chem. Res. 44 (2005) 1854-1859.
Saadi, S., Bouguelia, A., Trari, M., Photoassisted hydrogen evolution over spinel CuM2O4 (M = Al, Cr, Mn, Fe and Co). J. Renene. 31 (2006) 2245-2256.
Shang, W.T., Photocatalytic oxidation of methyl orange over boron-doped TiO2 nanotube arrays. Master thesis, Graduate Institute of Environmental Engineering, National Taiwan University, R.O.C. (2010)
Shangguan, W.F., Teraoka, Y., Kagawa, S., Simultaneous catalytic removal of NOx and diesel soot particulates over ternary AB2O4 spinel-type oxides. Appl. Catal., B ,8 (1996) 217-227.
Yang, H., Yan, J., Lu, Z., Cheng, X., Tang, Y., Photocatalytic activity evaluation of tetragonal CuFe2O4 nanoparticals for the H2 evolution under visible light irradiation. J. Alloys and Compounds. 476 (2009) 715-719.
Zhang, X., Huang, J., Ding, K., Hou, Y., Wang, X., Fu, X., Photocatalytic decomposition of benzene by porous nanocrystalline ZnGa2O4 with a high surface area. Environ. Sci Technol. 43 (2009) 5947-5951.
dc.identifier.urihttp://tdr.lib.ntu.edu.tw/jspui/handle/123456789/38851-
dc.description.abstract因為銅的易溶出性質,含銅污泥為有害事業廢棄物的一種。在含銅污泥的廢棄與再利用時,安定與穩定化是不可忽視的課題,而熱處理程序是相當重要的銅污泥安定穩定化技術之一。熱處理程序具有將含銅污泥轉化成銅鋁尖晶石的潛力,並藉此降低銅溶出的濃度,以達到安定穩定化之目的。
在材料的特性上,銅鋁尖晶石為近年來受到學界矚目的吸附劑與催化劑之一。本研究的目的即在探討藉熱處理技術資源化含銅污泥,並轉化成銅鋁尖晶石吸附劑與催化劑的可能性。研究中同時應用模擬污泥與實場污泥做為材料,探討尖晶石合成的最佳條件與特性。在尖晶石合成的實驗中,利用X光粉末繞射儀(XRD)鑑定產物晶型,以選擇由模擬污泥與實場污泥合成尖晶石的最佳熱處理條件。在吸附與光催化的能力鑑定上,選用甲基橙作為目標污染物,進行吸附與降解的實驗,並得到最佳的反應條件。
實驗結果顯示,在尖晶石的合成上,對於模擬污泥的最佳溫度及時間為1100℃及2小時;對於實場污泥之最佳溫度及時間為1200℃及8小時。在毒性溶出測試(TCLP)中,經過熱處理技術後的污泥,銅溶出量明顯下降,達到污泥安定穩定化的效果。在吸附與降解甲基橙的實驗上,最佳反應條件為pH 7.5,35℃。在125W水銀燈(波長大於400nm)的照射之下,在三小時內由模擬污泥合成的尖晶石對甲基橙的去除率可達67%,實場污泥所合成之尖晶石亦展現了去除效果,也藉此指出了含銅污泥轉換成吸附劑或可見光催化劑的潛力。
zh_TW
dc.description.abstractCopper-laden sludge is regarded as a hazardous solid waste. Therefore, stabilizing process for the sludge should be taken before disposal and reuse. Thermal process is one of the methods to stabilize the copper-laden sludge. This method has the potential to transform copper-laden sludge into copper aluminate spinel structure (CuAl2O4) in ceramic products to reduce the leaching concentration of copper. Besides, copper aluminate is also a candidate for adsorbent and photo-catalyst. The aim of this research was to investigate the feasibility of adsorbent and photo-catalyst transformed from copper-laden sludge by thermal treatment. Both the simulated sludge and field sludge were used in this study. X-ray diffraction (XRD) was applied to determine the optimum conditions for the thermal process to transform the sludge into CuAl2O4. The target pollutant was methyl orange (MO), which was used to determine the proper reaction circumstance for adsorption and photo-degradation by CuAl2O4. Results indicated that the optimum temperature and heating time for transforming the simulated sludge and field sludge into CuAl2O4 were 1100 ℃, 2 hours, and 1200 ℃, 8 hours, respectively. From the result of toxicity characteristic leaching procedure (TCLP), the leaching concentration of copper had significant reduce, which indicated the stabilizing ability of the thermal process. In adsorption and photo-catalyst experiment, under the optimal reaction, which were pH 7.5 and 35℃, the spinel synthesized from simulated sludge adsorbed or decomposed methyl orange to 67%, within three hours with a light source of the 125W mercury lamp (wavelength > 400 nm). Spinel synthesized from field sludge showed the MO removing ability also. This study demonstrated the potential that copper-laden sludge could be transformed into adsorbent or visible light photo-catalyst.en
dc.description.provenanceMade available in DSpace on 2021-06-13T16:49:10Z (GMT). No. of bitstreams: 1
ntu-100-R98541110-1.pdf: 3199428 bytes, checksum: a673f2a3c48663832c59b150213e1cba (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 ......................................................................................................................v
LIST OF FIGURES....................................................................................................... viii
LIST OF TABLES........................................................................................................... xi
Chapter 1 Introduction..............................................................................................1
1.1 Motivation.......................................................................................................1
1.2 Objective.........................................................................................................2
Chapter 2 Literature Review ....................................................................................4
2.1 Copper laden-sludge .......................................................................................4
2.2 Sludge treatment .............................................................................................4
2.3 Spinel ..............................................................................................................6
2.3.1 Characteristic.........................................................................................6
2.3.2 Synthesis methods .................................................................................6
2.3.3 Application............................................................................................7
2.4 Methyl orange.................................................................................................9
2.5 Adsorption ....................................................................................................11
2.6 Photolysis......................................................................................................13
2.6.1 Direct photolysis .................................................................................13
2.6.2 Indirect photolysis ...............................................................................14
Chapter 3 Methods and Materials..........................................................................16
3.1 Research framework .....................................................................................16
3.2 Field sludge analysis.....................................................................................18
3.2.1 Total digestion.....................................................................................18
3.2.2 Chemical sequential extraction ...........................................................19
3.3 Spinel synthesis ............................................................................................20
3.3.1 Sludge preparation ..............................................................................20
3.3.2 Thermal process ..................................................................................21
3.4 Pollutant removal experiments .....................................................................21
3.4.1 Physical and chemical properties of the spinels..................................21
3.4.2 Removal experiments of methyl orange .............................................25
3.4.3 Reaction kinetics models.....................................................................26
Chapter 4 Results and Discussions .........................................................................29
4.1 Optimization of thermal synthesis process ...................................................29
4.1.1 Composition of field sludge ................................................................29
4.1.2 Effect of sintering temperature............................................................30
4.1.3 Heating time ........................................................................................37
4.1.4 Physical and chemical properties of the spinel products ....................42
4.2 Optimization of methyl orange removal reaction.........................................49
4.2.1 Background experiment ......................................................................50
4.2.2 Effect of pH value ...............................................................................51
4.2.3 Effect of temperature...........................................................................56
4.3 Reaction kinetics...........................................................................................58
4.3.1 First order and second order reaction simulation................................58
4.3.2 Activation energy ................................................................................61
4.3.3 Application of optimal reaction conditions on spinels synthesized
from simulated sludge and field sludge ..............................................62
Chapter 5 Conclusion and Suggestion....................................................................64
5.1 Conclusion ....................................................................................................64
5.2 Suggestions for future work..........................................................................65
REFERENCE ..................................................................................................................66
APPENDIX .....................................................................................................................70
dc.language.isoen
dc.title以熱處理程序將含銅污泥轉化為吸附劑與光催化劑之研究zh_TW
dc.titleTransformation of Copper-laden Sludge into Photo-catalyst and Adsorbent by Thermal Treatmenten
dc.typeThesis
dc.date.schoolyear99-2
dc.description.degree碩士
dc.contributor.oralexamcommittee官文惠(Wen-Hui Kuan),胡景堯(Ching-Yao Hu)
dc.subject.keyword吸附劑,含銅污泥,甲基橙,光降解,尖晶石,zh_TW
dc.subject.keywordAdsorption,copper sludge,methyl orange,photo-degradation,spinel,en
dc.relation.page76
dc.rights.note有償授權
dc.date.accepted2011-07-15
dc.contributor.author-college工學院zh_TW
dc.contributor.author-dept環境工程學研究所zh_TW
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