第五章 結論與建議
5.2 建議
1.本研究所利用的 Aero-EISA 方法製備金屬觸媒是以對於吸附丙酮效 率最佳之 Surf/Si 莫耳比例 0.18 為基礎配方，再搭配不同的金屬種 類與濃度進行比較，因此建議對於製程配方參數與減低配方的化學 材料費用同時進行後續的探討研究，如研究選用以較便宜甚至是光 電廠廢棄物的矽基質取代原配方中的TEOS，以及以價格便宜的另 類介面活性劑(如 P123)取代原配方中的 CTAB，以期達到催化 VOCs 的最佳效率與價格最便宜的雙重目標。
2.實驗所選用的 VOCs 為丙酮分子，其他如芳香族類的甲苯(toluene)、
含氯化合物等均是重要的VOCs 污染物種，此外還可再針對氧化還 原雙功能(Bifunction)的污染物進行去除探討，如同時去除丙酮與氮 氧化物的實驗，將更可以提升金屬觸媒的使用效率，因此建議未來 可選用不同種類與型式的空氣污染物再進行研究比較，以獲得有關 反應物的影響參數。
3.本研究所設計的 Aero-EISA 製程是以震盪噴霧的原理進行氣膠的合 成，雖然與水熱法等製備金屬觸媒的方式相比已經是簡單快速有效 的製程，但是對於製程更趨於簡單化的設計提升部分，還可以選用 工業界製造粉體廣為被選用的噴霧乾燥器來嘗試進行 Metal-MSPs 的合成，以期朝向後續具有量產的潛力開發市場。
4.本研究以 Aero-EISA 一步合成之 Ce/Al-MSPs 金屬觸媒具有低溫有 效催化丙酮之效果，主要是因為Al 金屬之吸附活性與 Ce 金屬的催 化活性所形成的協合效應(synergetic effect)所致，然而對於其中的 吸附與催化反應卻未進行進一步之分別探討，因此建議未來可選用 純氮氣或空氣各別進行 Ce/Al-MSPs 金屬觸媒吸附或催化丙酮的實 驗，或以求得動力方程式等方法來進行吸附或催化反應的進一步研 究討論。
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第六章 參考文獻
Abi-aad, E., Bechara, R., Grimblot, J., Aboukais, A. “Preparation and characterization of CeO2 under an oxidizing atmosphere. Thermal analysis, XPS, and EPR study”, Chemistry of Materials 1993, 5, 793-797.
Aguero, F.N., Barbero, B.P., Sanz, O., Lozano, F.J.E., Montes, M., Cadŭs, L.E. “Influence of the support on MnOx metallic monoliths for the combustion of Volatile Organic Compounds”, Industrial ＆ Engineering Chemistry Research 2010, 49, 1663-1668.
Alifanti, M., Florea, M., Paevulescu, V.I. “Ceria-based oxides as supports for LaCoO3 perovskite; catalysts for total oxidation of VOC”, Applied Catalysis B: Environmental 2007, 70, 400-405.
Angel, G.D., Padilla, J.M., Cuauhtemoc, I., Navarrete, J. “Toluene combustion on γ-Al2O3-CeO2 catalysts prepared from boehmite and cerium nitrate”, Journal of Molecular Catalysis A: Chemical 2008, 281, 173-178.
Araujo, A.S. Aquino, J.M.F.B., Souza, M.J.B., Silva, A.O.S. “Synthesis, characterization and catalytic application of cerium-modified MCM-41”, Journal of Solid State Chemistry 2003, 171, 371-374.
Argauer, R.J., Landolt, G.R. “Crystalline zeolite ZSM-5 and method of preparing the same”, U.S. Patent 1972, 3, 702, 889.
Atwood, G.A., Greene, H.L., Chintawar, P., Rachapudi, R., Ramachandran, B., Vogel, C.A. “Trichloroethylene sorption and oxidation using a dual function sorbent/catalyst in a falling furnace reactor”, Applied Catalysis B: Environmental 1998, 18, 51-61.
Baccile, N., Grosso, D., Sanchez, C.J. “Aerosol generated mesoporous silica particles”, Journal of Materials Chemistry 2003, 13, 3011-3016.
Barman, S., Pradhan, N.C., Basu, J.K. “Kinetics of alkylation of benzene with isopropyl alcohol over Ce-exchanged NaX zeolite”, Industrial ＆ Engineering Chemistry Research 2005, 44, 7313-7319.
Beck, J.S., Vartull, J.C., Roth, W.J., Leonowicz, M.E., Kresge, C.T., Schmitt, K.D., Chu, C.T.W., Olson, D.H., Sheppard, E.W., McCullen, S.B., Higgins, J.B., Schlenker, J.L. “A new family of mesoporous molecular sieves prepared with liquid crystal templates”, Journal of American Chemical Society 1992, 114, 10834-10843.
Blasin-Aube, V.B., Monceaux, B.L. “General study of catalytic oxidation of various La0.8Sr0.2MnO3+x perovskite catalyst-influence of mixture”,
123
Applied Catalysis B: Environmental 2003, 43, 175-186.
Bore, M.T., Rathod, S.B., Ward, T.L., Datye, A.K. “Hexagonal mesostructure in powders produced by evaporation-induced self-assembly of aerosols from aqueous tetraethoxysilane solutions”, Langmuir 2003, 19(2), 256-264.
Bore, M.T., Marzke, R.F., Ward, T.L., Datye, A.K. “Aerosol synthesized mesoporous silica containing high loading of alumina and ziroconia”, Journal of Materials Chemistry 2005, 15, 5022-5028.
Bore, M.T., Mokhonoana, M.P., Ward, T.L., Coville, N.J., Datye, A.K.
“Synthesis and reactivity of gold nanoparticles supported on transition metal doped mesoporous silica”, Microporous and Mesoporous Materials 2006, 95, 118-125.
Breck, D.W. “Zeolite molecular sieves”, Wiley, New York, 1974.
Brinker, C.J., Lu, Y.F., Sellinger, A., Fan, H. “Evaporation-induced self-assembly: Nanostructures made easy”, Advanced Materials 1999, 11(7), 579-585.
Carja, G., Kameshima, Y., Okada, K., Madhusoodana, C.D.
“Mn-Ce/ZSM-5 as a new superior catalyst for NO reduction with NH3”, Applied Catalysis B: Environmental 2007, 73, 60-64.
Chen, I.P., Lin, S.S., Wang, C.H., Chang, L., Chang, J.S. “Preparing and characterizing an optimal supported ceria catalyst for the catalytic wet air oxidation of phenol”, Applied Catalysis B: Environmental 2004, 50, 49-58.
Clausse, B., Garrot, B., Cornier, C., Paulin, C., Simonot-Grange, M.H., Boutros, F. “Adsorption of chlorinated volatile organic compounds on hydrophobic faujasite: correlation between the thermodynamic and kinetic properties and the prediction of air cleaning”, Microporous and Mesoporous Materials 1998, 25, 169-177.
Costa, C., Dzikh, I.P., Lopes, J.M., Lemos, F., Ribeiro, F.R.
“Activity-acidity relationship in zeolite ZSM-5. Application of Brønsted-type equations”, Journal of Molecular Catalysis A: Chemical 2000, 154, 193-201.
Dai, Q., Wang, X., Lu, G. “Low-temperature catalytic combustion of trichloroethylene over cerium oxide and catalyst deactivation”, Applied Catalysis B: Environmental 2008, 81, 192-202.
Degnan, T.F., Chitnis, G.K., Schipper, P.H. “History of ZSM-5 fluid
124
catalytic cracking additive development at Mobil”, Microporous and Mesoporous Materials 2000, 35-36, 245-252.
Delimaris, D., Loannades, T. “VOC oxidation over CuO-CeO2 catalysts prepared by a combustion method”, Applied Catalysis B:
Environmental 2009, 89, 295-302.
Deshpande, S., Patil, S., Kuchibhatla, S., Seal, S. “Size dependency variation in lattice parameter and valency states in nanocrystalline cerium oxide”, Applied Physics Letters 2005, 87, 133113-1-133113-3.
Gandia, L.M., Gil, A., Korili, S.A. “Effects of various Alkali-acid additives on the activity of a manganese oxide in the catalytic combustion of ketones”, Applied Catalysis B: Environmental 2001, 33, 1-8.
Gandia, L.M., Vicente, M.A., Gil, A. “Complete oxidation of acetone over manganese oxide catalyst supported on alumina- and zirconia-pillared clays”, Applied Catalysis B: Environmental 2002, 38, 295-307.
Garcia, T., Solsona, B., Taylor, S.H. “Nano-crystalline ceria catalysts for the abatement of polycyclic aromatic hydrocarbons”, Catalysis Letters 2005, 105(3-4), 183-189.
Garcia, T., Solsona, B., Taylor, S.H. “Naphthalene total oxidation over metal oxide catalysts”, Applied Catalysis B: Environmental 2006, 66, 92-99.
Ghiaci, M., Abbaspur, A., Kia, R., Seyedeyn-Azad, F. “Equilibrium isotherm studies for the sorption of benzene, toluene, and phenol onto organo-zeolites and as-synthesized MCM-41”, Separation and Purification Technology 2004, 40, 217-229.
Gil, A., Vicente, M.A., Toranzo, R., Banares, M.A., Gandia, L.M.
“Preparation, characterization and catalytic activity in the deep oxidation of acetone of Cr, Al-pillared saponites”, Journal of Chemical Technology and Biotechnology 1998, 72(2), 131-136.
Gil, A., Vicente, M.A., Lambert, J.F., Gandia, L.M. “Platinum catalysts supported on Al-pillared clays application to the catalytic combustion of acetone and methyl-ethyl-ketone”, Catalysis Today 2001, 68, 41-51.
Greene H. L., Prakash, D. S., Athota, K. V. “Combined sorbent/catalyst media for desorption of halogenerated VOCs”, Applied Catalysis B:
Environmental 1996, 7, 213-224.
Guillemot, M., Mijoin, J., Mignard, S., Magnoux, P. “Volatile organic
125
compounds (VOCs) removal over dual functional adsorbent/catalyst system”, Applied Catalysis B: Environmental 2007, 75, 249-255.
Gutierrez-Ortiz J.I., de Rivas, B., Lopez-Fonseca R., Gonzalez-Velasco J.R. “Catalytic purification of waste gases containing VOC mixtures with Ce/Zr solid solutions”, Applied Catalysis B: Environmental 2006, 65, 191-200.
Gutierrez-Ortiz J.I., de Rivas, B., Lopez-Fonseca R., Gonzalez-Velasco J.R. “Study of the temperature-programmed oxidative degradation of hydrocarbons over Ce-based catalysts by evolved gas analysis”, Journal of Thermal Analysis and Calorimetry 2007, 87(1), 55-60.
Haiyan, C., Sayari, A., Adnot, A., Larachi, F. “Composition-activity effects of Mn-Ce-O composites on phenol catalytic wet oxidation”, Applied catalysis B: Environmental 2001, 31, 195-204.
Hampsey, J.E., Arsenault, S., Hu, Q., Lu, Y.F. “One-step synthesis of mesoporous metal-SiO2 particles by an aerosol-assisted self-assembly process”, Chemisty of Materials 2005, 17, 2475-2480.
He, C., Li, J., Cheng, J., Li, L., Li, P., Hao, Z., Xu, Z.P. “Comparative studies on porous material-supported Pd catalysts for catalytic oxidation of benzene, toluene, and ethyl acetate”, Industrial＆Engineering Chemistry Research 2009, 48, 6930-6936.
Hollander, M.A. den, Wissink, M., Makkee, M., Moulijn, J.A. “Gasoline conversion: reactivity towards cracking with equilibrated FCC and ZSM-5 catalysts”, Applied Catalysis A: General 2002, 223, 85-102.
Hu, C., Zhu, Q., Jiang, Z., Chen, L., Wu, R. “Catalytic combustion of dilute acetone over Cu-doped ceria catalysts”, Chemical Engineering Journal 2009, 152, 583-590.
Hung, C.T., Bai, H.L. “Adsorption behaviors of organic vapors using mesoporous silica particles made by evaporation induced self-assembly method”, Chemical Engineering Science 2008, 63, 1997-2005.
Hung, C.T., Bai, H.L., Karthik, M. “Ordered mesoporous silica particles and Si-MCM-41 for the adsorption of acetone: A comparative study”, Separation and Purification Technology 2009, 64(3), 265-272.
Jone, J., Ross, J.R.H. “The development of supported vanadia catalysts for the combined catalytic removal of the oxides of nitrogen and chlorinated hydrocarbons from flue gases”, Catalysis Today 1997, 35, 97-105.
Kadgaonkar, M.D., Laha, S.C., Pandey, R.K., Kumar, P., Mirajkar, S. P.,
126
Kumar, R. “Cerium-containing MCM-41 materials as selective acylation and alkylation catalysts”, Catalysis Today 2004, 97, 225-231.
Kalita, P., Gupta, N. M., Kumar, R. “Synergistic role of acid sites in the Ce-enhanced activity of mesoporous Ce-Al-MCM-41 catalysts in alkylation reaction: FTIR and TPD-ammonia studies”, Journal of Catalysis 2007, 245, 338-347.
Karthik, M., Lin, L.Y., Bai, H.L. “Bifunctional mesoporous Cu-Al-MCM-41 materials for the simultaneous catalytic abatement of NOx and VOCs”, Microporous and Mesoporous Materials 2009, 117, 153-160.
Kawi, S., Te, M. “MCM-48 supported chromium catalyst for trichloroethylene oxidation”, Catalysis Today 1998, 44, 101-109.
Khaleel, A., Al-Nayli, A. “Supported and mixed oxide catalysts based on iron and titanium for the oxidative decomposition of chlorobenzene”, Applied Catalysis B: Environmental 2008, 80, 176-184.
Khan, F.I., Ghoshal, A.K. “Removal of volatile organic compounds from polluted air”, Journal of Loss Prevention in the Process Industries 2000, 13, 527-545.
Kim, S.C. “The catalytic oxidation of aromatic hydrocarbons over supported metal oxide”, Journal of Hazardous Materials 2002, B91, 285-299.
Kim, H.J., Choi, S.W., Inyang, H.I. “Catalytic oxidation of toluene in contaminant emission control system using Mn-Ce/γ-Al2O3”, Environmental Technology 2008, 29, 559-569.
Kladis, C., Bhargava, S.K., Foger, K., Akolekar, D.B. “Effects of air pollutants on the cerium exchanged high silica zeolite catalyst: a Fourier transform infrared study”, Journal of Molecular Catalysis A: Chemical 2001, 171, 243-249.
Klinghoffer A. A., Rossin, J. A. “Catalytic oxidation of chloroacetonitrile over a 1% platinum alumina catalyst”, Industrial ＆ Engineering Chemistry Research 1992, 31, 481-486.
Korsvik, C., Patil, S., Seal, S., Self, W.T. “Superoxide dismutase mimetic properties exhibited by vacancy engineered ceria nanoparticles”, Chemistry Communication 2007, 1056-1058.
Kosslick, H., Lischke, G., Parlitz, B., Fricke, R. “Acidity and active sites of Al-MCM-41”, Applied Catalysis A: General 1999, 184, 49-60.
127
Kresge, C.T., Leonowicz, M.E., Roth, W.J., Vartuli, J.C., Beck, J.S.
“Ordered mesoporous molecular sieve synthesized by a liquid-crystal template mechanism”, Nature 1992, 359(6397), 710-712.
Krishnamoorthy, S., Rivas, J.A., Amiridis, M.D. “Catalytic combustion of 1,2-dichlorobenzene over supported transition oxides”, Journal of Catalysis 2000, 193, 264-272.
Laachir, A., Perrichon, V., Badri, A., Lamotte, J., Catherine E., Lavalley J.C., Fallah, J.E., Hilaire, L., Normand F.I., Quemere, E, Sauvion, G.N., Tourel, O. “Reduction CeO2 by hydrogen magnetic susceptibility and Fourier-transform infrared, ultraviolet and X-ray photoelectron spectroscope measurements”, Journal of the Chemical Society, Faraday Transaction 1991, 87(10), 1601-1609.
Laha, S.C., Mukherjee, P., Sainkar, S.R., Kumar, R. “Cerium containing MCM-41-type mesoporous materials and their acidic and redox catalytic properties”, Journal of Catalysis 2002, 207, 213-223.
Li, W.B., Chu, W.B., Zhuang, M., Hua, J. “Catalytic oxidation of toluene on Mn-containing mixed oxides prepared in reverse microemulsions”, Catalysis Today 2004, 93-95, 205-209.
Li, W.B., Zhuang, M., Xiao, T.C., Green, M.L.H.J. “MCM-41 supported Cu-Mn catalysts for catalytic oxidation of toluene at low temperatures”, Journal of Physical Cheistry. B 2006, 110, 21568-21571.
Lin, Y.C., Bai, H.L., Chang, C.L. “Applying hexagonal nanostructured zeolite particles for acetone removal”, Journal of Air & Waste Management Association 2005, 55(6), 834-840.
Lu, Y.F., Fan, H., Stump, A., Ward, T.L., Rieker, T., Brinker, C.J.
“Aerosol-assisted self-assembly of mesostructured spherical nanoparticles”, Nature 1999, 398(6724), 223-226.
Minico, S., Sire, S., Crisafulli, C., Galvagno, S. “Influence of catalyst pretreatments on volatile organic compounds oxidation over gold/iron oxides”, Applied Catalysis B: Environmental 2001, 34, 277-285.
Mitsui, T., Matsui T. “Low-temperature complete oxidation of ethyl acetate over CeO2 supported precious metal catalysts”, Topics in Catalysis 2009, 52, 464-469.
Mu, Z., Li, J.J., Tian, H., Hao, Z.P., Qiao, S.Z. “Synthesis of mesoporous Co/Ce-SBA-15 materials and their catalytic performance in the catalytic oxidation of benzene”, Materials Research Bulletin 2008, 43, 2599-2606.
128
Musialik-Piotrowska, A., Syczewska, K. A. “Catalytic oxidation of trichloroethylene in two-component mixtures with selected volatile organic compounds”, Catalysis Today 2002, 73, 333-342.
Nevers, N. D. “Air Pollution Control Engineering”, McGraw-Hill, 2nd ed., 2001.
Ntainjua, E., Garcia, T., Solsona, B., Taylor, S.H. “The influence of cerium to urea preparation ratio of nanocrystalline ceria catalysts for the total oxidation of naphthalene”, Catalysis Today 2008, 137, 373-378.
Oumi, Y., Nemoto, S., Nawata, S., Fukushima, T., Teranishi, T., Sano, T.
“Effect of the framework structure on the dealumination-realumination behavior of zeolite”, Materials Chemistry and Physics 2002, 78, 551-557.
Papaefthimiou P., Ioannides, T., Verykios, X.E. “Catalytic incineration of volatile organic compounds present in industrial waste streams”, Applied Thermal Engineering 1998, 18, 105-1012.
Park, S.H., Song, B.Y., Lee, T.G. “Effects of surfactant/silica and silica/cerium ratios on the characteristics of mesoporous Ce-MCM-41”, Journal of Industrial and Engineering Chemistry 2008, 14, 261-264.
Paulis, M., Gandia, L.M., Gil, A., Sambeth, J., Odriozolo, J.A., Montes, M. “Influence of the surface adsorption-desorption process on the ignition curves of volatile organic compounds (VOCs) complete oxidation over supported catalysts”, Applied Catalysis B:
Environmental 2000, 26, 37-46.
Picasso, G., Gutierrez, M., Pina, M.P., Herguido, J. “Preparation and characterization of Ce/Zr and Ce/Mn based oxides for n-hexane combustion: Application to catalytic membrance reactors”, Chemical Engineering Journal 2007, 126, 119-130.
Pina, M.P., Irusta, S., Menendez, M., Santamaria, J. “Combustion of volatile organic compounds over platinum-based catalytic membrances”, Industrial ＆ Enineering Chemistry Research 1997, 36, 4557-4566.
Reddy, B.M., Khan, A., Lakshmanan, P., Aouine, M., Loridant, S., Volta, J.C. “Structurl characterizaction of nanosized CeO2/SiO2, CeO2/TiO2, and CeO2/ZrO2 catalysts by XRD, Raman, and HREM techniques”, Journal of Physical Chemistry B 2005, 109, 3355-3363.
Ruthven, D.M., Kaul, B.K. “Adsorption of aromatic hydrocarbons in NaX zeolite.2. Kinetics”, Industrial ＆ Engineering Chemistry
129
Research 1993, 32, 2053-2057.
Scire, S., Minico, S., Grisafulli, C., Satriano, C., Pistone A. “Catalytic combustion of volatile organic compounds on gold/cerium oxide catalysts”, Applied Catalysis B: Environmental 2003, 40, 43-49.
Shan, R.K., Thonon, B., Benforado, D.M. “Opportunities for heat exchange application in environmental system”, Applied Thermal Engineering 2000, 20, 631-650.
Spinicci, R., Faticanti, M., Marini, P., De Rossi, S., Porta, P. “Catalytic activity of LaMnO3 and LaCoO3 perovskites towards VOCs combustion”, Journal of Molecular Catalysis A: Chemicl 2003, 197, 147-155.
Song, Y.Q., Feng, Y.L., Liu, F., Kang, C.L., Zhou, X.L. ”Effect of variations in pore structure and acidity of alkali treated ZSM-5 on the isomerization performance”, Journal of molecular Catalysis A:
Chemical 2009, 310, 130-137.
Terasaki, O. “Electron Crystallography” Erice. Itally, 2004.
Trovarelli, A., Leitenburg, C., Boaro, M., Dolcetti, G. “The utilization of ceria in industrial catalysis”, Catalysis Today 1999, 50, 353-367.
Tuel, A. “Modification of mesoporous silicas by incorporation heteroelements in the framework”, Microporous and Mesoporous Materials 1999, 27, 151-169.
US EPA, Compendium of Method for the Determination of Toxic Organic Compounds in Ambient Air, Second Edition, TO-14A, EPA/625/R-96/010B, http://www.epa.gov/ttn/amtic/files/ambient/ airtox/
to-14ar.pdf.
Velev. O.D., Kaler, E.W. “Structured porous materials via colloidal crystal templating: from inorganic oxides to metals”, Advanced Materials 2000, 12(7), 531-534.
Wang, C.H., Li, S.S. “Preparation an actived cerium oxide catalyst for the catalytic incineration of aromatic hydrocarbons”, Applied Catalysis A: General 2004, 268, 227-233.
Wang, S.P., Zheng, X.C., Wang, X.Y., Wang, S.R., Zhang, S.M., Yu, L.H., Huang, W.P., Wu, S.H. “Comparison of CuO/Ce0.8Zr0.2O2 and CuO/CeO2 catalysts for low-temperature CO oxidation”, Catalysis Letters 2005, 105(3-4), 163-168.
Wang, X., Dai, Q., Yi, Z. “Low-temperature catalytic combustion of
130
trichloroethylene over La, Ce, and Pt catalysts supported on MCM-41”, Chinese Journal of Catalysis, 2006, 27(6), 468-470.
Wang, X., Kang, Q., Li, D. “Catalytic combustion of chlorobenzene over MnOx/CeO2 mixed oxide catalysts”, Applied Catalysis B:
Environmental 2009, 86, 166-175.
Webber, R. “Relevance of PCDD/PCDF formation for the evaluation of POPs destruction technologies-Review on current status and assessment gaps”, Chemosphere 2007, 67, S109-S117.
Woolery, G.L., Kuehl, G.H., Timken, H.C., Chester, A.W., Vartuli, J.C.
“On the nature of framework Brønsted and Lewis acid sites in ZSM-5”, Zeolites 1997, 19, 288-296.
Wu, J.C.S., Chang, T.Y. “VOC deep oxidation over Pt catalysts using hydrophobic supports”, Catalysis Today 1998, 44, 111-118.
Wu, Y., Zhang, Y., Liu, M., Ma, Z. “Complete catalytic oxidation of o-xylene over Mn-Ce oxides prepared using a redox-precipitation method”, Catalysis Today 2010, 153, 170-175.
Xia, Q.H., Hidajat, K., Kawi, S. “Adsorption and catalytic combustion of aromatics on platinum-supported MCM-41 materials”, Catalysis Today 2001, 68, 255-262.
Yuliati, L., Hamajima, T., Hattori, T., Yoshida, H. “Highly dispersed Ce(III) species on silica and alumina as new photocatalysts for non-oxidative direct methane coupling”, Chemistry Communication 2005, 4824-4826.
Zhao, X.S., Ma, Q., Lu, G.Q. “VOC removal: Comparison of MCM-41 with hydrophobic zeolites and activated carbon”, Energy & Fuels 1998, 12, 1051-1054.
台灣環保署，“空氣污染防制-揮發性有機物空氣污染管制及排放標 準”，2005，http://w3.epa.gov.tw/epalaw/search/LordiDispFull.aspx?ltype=
04&lname=0162
顏秀慧，沸石對揮發性有機物吸附行為之研究，博士論文，1997。