Please use this identifier to cite or link to this item: http://hdl.handle.net/11455/90131
DC FieldValueLanguage
dc.contributor鄒裕民zh_TW
dc.contributor.authorRung-Rung Changen_US
dc.contributor.author張容蓉zh_TW
dc.contributor.other土壤環境科學系所zh_TW
dc.date2014zh_TW
dc.date.accessioned2015-12-09T02:25:10Z-
dc.identifier.citation陳楷岳。2012。不同炭化溫度導致土壤組成的變化及其對 Cr(VI)轉移的影響,碩士論文,國立中興大學,台中,台灣。 Aiken, G.R., D.M. McKnight, R.L. Wershaw, and P. MacCarthy. 1985. An introduction to humic substances in soil sediment and water. In: G. R. Aiken, D. M. McKnight, R. L. Wershaw and P. MacCarthy, editors, Humic substances in soil, sediment and water: Geochemistry, isolation and characterization. John Wiley and Sons, New York. p. 1-9. Aimin, L., X. Minjuan, L. Wenhui, W. Xuejun, and D. Jingyu. 2008. Adsorption characterizations of fulvic acid fractions onto kaolinite. J. Entomol. Sci. 20: 528-535. Allison, L.E. 1965. Organic carbon. In: C. A. Black, D. D. Evans, J. L. White, L. E. Ensminger and F. E. Clark, editors, Methods of Soil Analysis, Part 2. Chemical and Microbiological Properties. American Society of Agronomy, Madison, WI Balcke, G.U., N.A. Kulikova, S. Hesse, F.-D. Kopinke, I.V. Perminova, and F.H. Frimmel. 2002. Adsorption of humic substances onto kaolin clay related to their structural features. Soil Sci. Soc. Am. J. 66: 1805-1812. Baldock, J.A., and J.O. Skjemstad. 2000. Role of the soil matrix and minerals in protecting natural organic materials against biological attack. Org. Geochem. 31: 697-710. Basile-Doelscha, I., R. Amundson, W.E.E. Stone, D. Borschneck, J.Y. Bottero, S. Moustier, F. Masin, and F. Colin. 2007. Mineral control of carbon pools in a volcanic soil horizon. Geoderma 137: 477-489. Burdon, J. 2001. Are the traditional concepts of the structures of humic substances realistic? Soil Sci. 166: 752-769. Chai, X., S. Takayuki, Q. Guo, and Y. Zhao. 2008. Characterization of humic and fulvic acids extracted from landfill by elemental composition,13 C CP/MAS NMR and TMAH-Py-GC/MS. Waste Manage. 28: 896-903. Chen, K., J. Liu, P. Chiang, S. Wang, W. Kuan, Y. Tzou, Y. Deng, K. Tseng, C. Chen, and M. Wang. 2012. Chromate removal as influenced by the structural changes of soil components upon carbonization at different temperatures. Environ. Pollut. 162: 151-158. Chen, S.Y., S.W. Huang, P.N. Chiang, J.C. Liu, W.H. Kuan, J.H. Huang, and J.T. Hung. 2011. Influence of chemical compositions and molecular weights of humic acids on Cr(VI) photo-reduction. J. Hazard. Mater. 197: 337-344. Chen, Y., N. Senesi, and M. Schnitzer. 1977. Information provided on humic substances by E4/E6 ratios. Soil Sci. Soc. Am. J. 41: 352-358. Clapp, C.E., and M.H.B. Hayes. 1999. Size and shapes of humic substances. Soil Sci. 164: 777-789. Clapp, C.E., M.H.B. Hayes, A.J. Simpson, and W.L. Kingery. 2005. The chemistry of soil organic matter. In: A. Tabatabai and D. L. Sparks, editors, Chemical processes in soils. Soil Sci. Soc. Am., Madison, WI. p. 1-150. Davis, J.A., and R. Gloor. 1981. Adsorption of dissolved organics in lake water by aluminium oxide: Effect of molecular weight. Environ. Sci. Technol. 15: 1223-1229. Derenne, S., and C. Largeau. 2001. A review of some important families of refractory macromolecules: Composition, origin, and fate in soils and sediments. Soil Sci. 166: 833-847. Deshmukh, A.P., A.J. Simpson, C.M. Hadad, and P.G. Hatcher. 2005. Insights into the structure of cutin and cutan from Agave americana leaf cuticle using HRMAS NMR spectroscopy. Org. Geochem. 36: 1072-1085. Ekschmitta, K., M. Liub, S. Vettera, O. Foxa, and V. Wolters. 2005. Strategies used by soil biota to overcome soil organic matter stability-why is dead organic matter left over in the soil? Geoderma 128: 167-176. Filius, J.D., D.D. Lumsdon, J.C.L. Meeussen, T. Hiemstra, and W.H.V. Riemsdijk. 2000. Adsorption of fulvic acid on goethite. Geochim. Cosmochim. Acta 64: 61-60. Flaig, W. 1966. The chemistry of humic substances. In The Use of Isotopes in Soil Organic Matter Studies. Report of FAO/IAEA Technical Meeting. Pergamon, Elmsford, NY. p. 103-127. Gu, B., J. Schmitt, Z. Chen, L. Liang, and J.F. McCarthy. 1995. Adsorption and desorption of different organic matter fractions on iron oxide. Geochim. Cosmochim. Acta 59: 219-229. Gu, B., J. Schmltt, Z. Chen, L. Liang, and F. McCarthy. 1994. Adsorption and desorption of natural organic matter on iron oxide: Mechanisms and models.Environ. Sci. Technol. 28: 38-46. Hatcher, P., I. Breger, G. Maciel, and N. Szeverenyi. 1985. Geochemistry of humin. In: G. R. Aiken, D. M. McKnight, R. L. Wershaw and P. MacCarthy, editors, Humic Substances in Soil, Sediment, and Water. John Wiley and Sons, New York. p. 275-302 Hatcher, P.G., D. L.VanderHart, and W.L. Earl. 1980. Use of solid-state 13C NMR in structural studies of humic acids and humin from Holocene sediments. Org. Geochem. 2: 87-92. Hayes, M.H.B., and R.S. Swift. 1978. The chemistry of soil organic colloids In: D. J. Greenland and M. H. B. Hayes, editors, The Chemistry of Soil Constituents. Wiley, Chichester. p. 179-320. Hayes, M.H.B. 2006. Solvent systems for the isolation of organic components from soils. Soil Sci. Soc. Am. J. 70: 986-994. Hayes, M.H.B. 1985. Extraction of humic substances from soil. In: G. R. Aiken, D. M. McKnight, R. L. Wershaw and P. MacCarthy, editors, Humic Substances in Soil, Sediment, and Water. John Wiley and Sons, New York. p. 329-362. Hayes, M.H.B., and C.E. Clapp. 2001. Humic substances: considerations of compositions, aspects of structure, and environmental influences. Soil Sci. 166: 723-737. Hayes, T.M., M.H.B. Hayes, J.O. Skjemstad, and R.S. Swift. 2008. Studies of compositional relationships between organic matter in a grassland soil and its drainage waters. Euro. J. Soil Sci. 59: 603-616. Hayes, T.M., M.H.B. Hayes, and R.S. Swift. 2012. Detailed investigation of organic matter components in extracts and drainage waters from a soil under long term cultivation. Org. Geochem. 52: 13-22. Hedges, J.I., and R.G. Keil. 1995. Sedimentary organic matter preservation: An assessment and speculative synthesis. Mar. Chem. 49: 81-115. Hedges, J.I. 1988. Polymerization of humic substances in natural environments. In: F. H. Frimmel and R. F. Christman, editors, Humic substances and their role in the environment. John Wiley and Sons, Chichester, UK. p. 45-58. Huang, P.M., and A.G. Hardie. 2009. Formation mechanisms of humic substances in the environment In: N. Senes, B. Xing and P.M. Huang, editors, Biophysico-chemical processes involving natural nonliving organic matter in environmental systems. John Wiley & Sons. p. 41-109. Huang, S.W., P.N. Chiang, J.C. Liu, J.T. Hung, W.H. Kuan, Y.M. Tzou, S.L. Wang, J.H. Huang, C. Chen, C. , M.K. Wang, and R.H. Loeppert. 2012. Chromate reduction on humic acid derived from a peat soil – Exploration of the activated sites on HAs for chromate removal. Chemosphere 87: 587-594. Huang, Y.Y., S.L. Wang, J.C. Liu, Y.M. Tzou, R.R. Chang, and J.H. Chen. 2008. Influences of preparative methods of humic acids on the sorption of 2,4,6-trichlorophenol. Chemosphere 70: 1218-1227. Hur, J., and M.A. Schlautman. 2003. Molecular weight fractionation of humic substances by adsorption onto minerals. J. Colloid Interface Sci. 264: 313-321. Hu, W.-G., J. Mao, B. Xing, and K. Schmidt-Rohr. 2000. Poly(methylene) crystallites in humic substances detected by nuclear magnetic resonance. Environ. Sci. Technol. 34: 530-534. Jokic, A., M.C. Wang, C. Liu, A.I. Frenkel, and P.M. Huang. 2004. Integration of the polyphenol and Maillard reactions into a unified abiotic pathway for humification in nature: the role of d-MnO2. Org. Geochem. 35: 747-762. Jones, D.L., and A.C. Edwards. 1998. Influence of sorption on the biological utilization of two simple carbon substrates. Soil Biol. Biochem. 30: 1895-1902. Julien, C., M. Massot, and C. Poinsignon. 2004. Lattice vibrations of manganese oxides - part 1 Periodic structures. Spectrochim Acta, Part A 60: 689-700. Kaiser, K. 2003. Sorption of natural organic matter fractions to goethite (a-FeOOH): effect of chemical composition as revealed by liquid-state 13C NMR and wet-chemical analysis. Org. Geochem. 34: 1569-1579. Kaiser, K., and G. Guggenberger. 2000. The role of DOM sorption to mineral surfaces in the preservation of organic matter in soils. Org. Geochem. 31: 711-725. Kaiser, K., R. Mikutta, and G. Guggenberger. 2007. Increased stability of organic matter sorbed to ferrihydrite and goethite on aging. Soil Sci. Soc. Am. J. 71: 711-719. Kaiser, K., and W. Zech. 1999. Release of natural organic matter sorbed to oxides and a subsoil. Soil Sci. Soc. Am. J. 63: 1157-1166. Kang, S., D. Amarasiriwardena, P. Veneman, and B. Xing. 2003. Characterization of ten sequentially extracted humic acids and a humin from a soil in western Massachusetts. Soil Sci. 168: 880-887. Kang, S., and B. Xing. 2005. Phenanthrene sorption to sequentially extracted soil humic acids and humins. Environ. Sci. Technol. 39: 134-140. Keil, R.G., D.B. Montlucon, F.G. Prahl, and J.I. Hedges. 1994. Sorptive preservation of labile organic matter in marine sediments. Nature 370: 549-552. Kleber, M., P. Sollins, and R. Sutton. 2007. A conceptual model of organo-mineral interactions in soils: self-assembly of organic molecular fragments into zonal structures on mineral surfaces. Biogeochemistry 85: 9-24. Kononova, M.M. 1966. Soil Organic Matter. Pergamon, Elmsford, NY., Pergamon, Elmsford, NY. Koyama, M. 1995. Adsorption of humic acid on Ca-montmorillonite. Soil Sci. Plant Nutr. 41: 215-223. Leinweber, P., O. BIumenstein, and H.-R. Schulten. 1996. Organic matter composition in sewage farm soils: Investigations by 13C-NMR and pyrolysis-field ionization mass spectrometry. Eur. J. Soil Sci. 47: 71-80. Liu, M.M., X.H. Cao, W.F. Tan, X.H. Feng, G.H. Qiu, X.H. Chen, and F. Liu. 2011.Structural controls on the catalytic polymerization of hydroquinone by birnessites. Clay Clay Miner. 59: 525-537. Liu, C., and P.M. Huang. 2002. Role of hydroxy aluminosilicate ions(proto-imogolite sol) in the formation of humic substances. Org. Geochem. 33: 295-305. Lu, X.Q., J.V. Hanna, and W.D. Johnson. 2000. Source indicators of humic substances: an elemental composition, solid state 13C CP/MAS NMR and Py-GC/MS study. Appl. Geochem.15: 1019-1033. Mayer, L.M. 1994. Relationships between mineral surfaces and organic carbon concentrations in soils and sedmiments. Chem. Geol. 114: 447-363. McKenzie, R.M. 1971. The synthesis of birnessite, cryptomelane, and some other oxides and hydroxides of manganese. Mineral Magazine 38: 493-502. Mehra, O.P., and M.L. Jackson. 1960. Iron oxides removal from soils and clays by a dithionite-citrate system buffered with sodium bicarbonate. Clay Clay Miner. 7: 317-327. Meier, M., K. Namjesnik-Dejanovic, P.A. Maurice, Y.-P. Chin, and G.R. Aiken.1999. Fractionation of aquatic natural organic matter upon sorption to goethite and kaolinite. Chem. Geol. 157: 275-284. Michalovic, M. 2009. Ancient soil chemists of the Amazon. ChemMatters: 7-9. Mikutta, R., C. Mikutta, K. Kalbitz, T. Scheel, K. Kaiser, and R. Jahn. 2007.Biodegradation of forest floor organic matter bound to minerals via different binding mechanisms. Geochim. Cosmochim. Acta 71: 2569-2590. McKeague, J.A. 1967. An evaluation of 0.1 M pyrophosphate and Pyrophosphate-Dithionite in comparison with oxalate as extractants of accumulation products in podzols and some other soils Can. J. Soil Sci. 47:95-99. McKeague, J.A., and J.H. Day. 1966. Dithionite and oxalate extractable Fe and Al as aids in differentiating various classes of soils. Can. J. Soil Sci. 46: 13-22. Moore, T.R., W.d. Souza, and J.F. Koprivnjak. 1992. Controls on the sorption of dissolved organic carbon by soils. Soil Sci. 154: 120-129. Oades, J.M. 1994. The retention of organic matter in soils. Biogeochemistry 5: 35-70. Olivella, M.A., J.C.d. Rio, J. Palacios, M.A. Vairavamurthy, and F.X.C.d.l. Heras.2002. Characterization of humic acid from leonardite coal: an integrated study of PY-GC-MS, XPS and XANES techniques. J. Anal. Appl. Pyrolysis 63: 59-68. Parfitt, R.L., A.R. Fraser, and V.C. Farmer. 1977. Adsorption on hydrous oxides. III. fulvic acid and humic acid on goethite, gibbsite and imogolite. Soil Sci. 28: 289-296. Piccolo, A. 2001. The supramolecular structure of humic substances. Soil Sci. 166: 810-832. Raich, J.W. 1992. The global carbon dioxide flux in soil respiration and its relationship to vegetation and climate. Tellus 44B: 81-99. Rasmussen, C., M.S. Torn, and R.J. Southard. 2005. Mineral assemblage and aggregates control carbon dynamics in a california conifer forest. Soil Sci. Soc. Am. J. 69: 1711-1721. Rice, J.A. 2001. Humin. Soil Sci. 166: 848-857. Rice, J.A., and P. MacCarthy. 1989. Isolation of humin by liquid-liquid partitioning. Sci. Total Environ. 81/82: 61-69. Rice, J.A., and P. MacCarthy. 1992. Disaggregation and characterization of humin. Sci. Total Environ. 117/118: 83-88. Risser, J.A., and G.W. Bailey. 1992. Spectroscopic study of surface redox reactions with manganese oxides. Soil Sci. Soc. Am. J. 56: 82-88. Schwertmann, U., and R.M. Cornell. 1991. Iron oxides in the laboratory: Preparation and characterizationVCH, Weinheim. Sherine, B., A.J.A. Nasser, and S. Rajendran. 2010. Inhibitive action of hydroquinone-Zn2+ system in controlling the corrosion of carbon steel in well water. Int. J. Eng. Sci. Tech. 2: 341-357. Shindo, H., and P.M. Huang. 1982. Role of Mn(VI) oxide in abiotic formation of humic substances in the environment. Nature 298: 363-365. Simpson, A., G. Song, E. Smith, B. Lam, E. Novotny, and M. Hayes. 2007 Unraveling the structural components of soil humin by use of solution-state nuclear magnetic resonance spectroscopy. Environ. Sci. Technol. 41: 876-883. Song, G., M.H.B. Hayes, E.H. Novotny, and A.J. Simpson. 2011. Isolation and fractionation of soil humin using alkaline urea and dimethylsulphoxide plus sulphuric acid. Naturwissenschaften 98: 7-13. Song, G., E.H. Novotny, A.J. Simpson, C.E. Clapp, and M.H.B. Hayes. 2008. Sequential exhaustive extraction of a Mollisol soil, and characterizations of humic components, including humin, by solid and solution state NMR. Eur. J. Soil Sci. 59: 505-516. Soil Survey Staff. 1999. Soil Taxonomy-A basic system of soil classification for making and interpreting soil surveys. USDA NRCS Agric. Handbook No. 436. US Govt. Print. Office, Washington, DC. Stevenson, F.J. 1994. Humus Chemistry-Genesis, Composition, Reactions, 2nd edn John Wiley and Sons, New York, NY. Stevenson, F.J., and M.S. Ardakani. 1972. Organic matter reactions involving micronutrients in soils. In: Morivedt, editor Micro-nutrients in Argriculture. Soil Sci. Soc. Am., Masison, USA. p. 79-114. Stumm, W. 1992. Chemistry of the solid-water interface John Wiley & Sons, New York. Swift, R.S. 1996. Organic matter characterization. In: D. L. S. e. al, editor Methods of soil analysis. Part 3. Chemical methods. Soil Science Society of America, American Society of Agronomy, Madison, WI. p. 1018-1020. Swift, R.S. 1985. Fractionation of soil substances. In: G. R. Aiken, editor Humic substances in soil, sediment and water. Wiley-Interscience, New York. p.387-408. Tipping, E. 1981. The adsorption of aquatic humic substances by iron oxides. Geochim. Cosmochim. Acta 45: 191-199. Torn, M.S., S.E. Trumbore, O.A. Chadwick, P.M. Vitousek, and D.M. Hendricks.1997. Mineral control of soil organic carbon storage and turnover. Nature 389:170-173. Tsai, C.C., Z.S. Chen, C.I. Kao, F. Ottner, S.J. Kao, and F. Zehetner. 2010. Pedogenic development of volcanic ash soils along a climosequence in northern Taiwan. Geoderma 156: 48-59. Tzou, Y.M., S.L. Wang, J.C. Liu, Y.Y. Huang, and J.H. Chen. 2008. Removal of 2,4,6-trichlorophenol from a solution by humic acids repeatedly extracted from a peat soil. J. Hazard. Mater.152: 812-819. Vermeer, A.W.P., and L.K. Koopal. 1998. Adsorption of humic acids to mineral particles. 2. polydispersity effects with polyelectrolyte adsorption. Langmuir 14: 4210-4216. Vermeer, A.W.P., W.H.v. Riemsdijk, and L.K. Koopal. 1998. Adsorption of humic acid to mineral particles. 1. Specific and electrostatic interactions. Langmuir 14: 2810-2819. Walkley, A., and I.A. Black. 1934. An examination of Degtjareff method for determining soil organic matter and a proposed modification of the chromic acid titration method. Soil Sci. 37: 29-37. Weng, L., W.H.V. Riemsdijk, L.K. Koopal, and T. Hiemstra. 2006. Adsorption of humic substances on goethite: Comparison between humic acids and fulvic acids. Environ. Sci. Technol. 40: 7494-7500. Williams, V.R. 1914. Soil sicence, Pochvovedenie 1. Wiseman, C.L.S., and W. Püttmann. 2006. Interactions between mineral phases in the preservation of soil organic matter. Geoderma 134: 109-118. Xing, B., and J.J. Pignatello. 1997. Dual-mode sorption of low-polarity compounds in glassy poly(vinyl chloride) and soil organic matter. Environ. Sci. Technol. 31: 792-799. Xing, B.S. 2001. Sorption of naphthalene and phenanthrene by soil humic acids. Environ. Pollut. 111: 303-309.zh_TW
dc.identifier.urihttp://hdl.handle.net/11455/90131-
dc.description.abstractMost studies of humic substances (HSs) been carried out on extracts of soils in dilute sodium hydroxide solutions, i.e., the isolation of the International Humic Substances Society (IHSS). However, humin, is insoluble in aqueous base. Recently, a sequential exhaustive extraction (SEE) process has been shown to be capable of isolating and separating the major components of the classically defined HSs from soils of the temperate and tropical regions. The SEE system was used to isolate the HA/FA and humin fractions from a subtropical volcanic Taiwanese soil. Increases in the aliphatic relative to aromatic carbon contents were observed for both the HA and FA fractions when the pH values of the extraction media were increased. HAs and FAs isolated using the SEE method have spectroscopic profiles similar to those from the IHSS isolate; however, the cumulative extraction efficiency (%) of the SEE method (65%) for the volcanic soil was much higher than for the traditional IHSS method (33%). When the residual volcanic soil, following extractions once, three, and eight times with 0.1 M NaOH were then extracted with dimethylsulphoxide (DMSO) plus concentrated sulphuric acid (the final solvent in the SEE sequence), it was seen that the content of crystalline polymethylene hydrocarbon (33 ppm 13 C NMR resonance in the humin (or DMSO-acid)) extract increased relative to the amorphous methylene (30 ppm). That highlights the difficulty in dissolving the more highly ordered hydrocarbon structures that would be expected to have closer associations with the mineral colloids.In addition,the interactions of HSs with clay minerals commonly occur in soil which may lead to the formations of soil aggregates, forming an organo-clay matrix. Quinones, naturally abiotic polyphenol polymerization reaction catalyzed by MnO2, have been considered as precursor of humification in soil. Clarifying the reactive mechanisms of quinones (HQs) and HSs with widely distributed Fe(oxy)hydroxides can provide insight into the effects of the inorganic minerals on the humification of organic components in soil and the important physico-chemical reactions of environmental processes. The organo-clay of HA and HQs adsorbed on Fe(oxy)hydroxides followed the order of HA > HQ-20 > HQ-7 > HQ-1. Adsorption results indicated that low pH was favorable for sorption of HA/FA on soil minerals, and OH-concentrations affected dramatically the sorption behaviors of the organic acids with a pH larger than the ZPC of the colloid adsorbents.Sorption of HA/FA on soil minerals followed generally the orderof ferrihydrite > goethite > kaolinite ≒ montmorillonite. The FTIR absorption band at 1720 cm-1 disappeared while the bands at 1609 and 1575 cm-1 broaden and increased in intensity, demonstrating that the formation of a strong complex through a ligand exchange of the carboxylic groups of HA and quinones with OH on the surfaces of Fe(oxy)hydroxides was the major reaction involved in the sorption process. The hollow-fiber filtration system could further fractionate efficiently HA into three categories of < 50, 50-100, and >100 kD HA, and high molecular weight (MWs) (i.e., > 100 kD HA) of HA exhibited a preferential sorption behavior on Fe(oxy)hydroxides. The preferential sorption of larger HA molecules may be attributed to the presence of higher contents of (1) aromatic carbon (helpful for increasing the hydrophobic interactions); (2) carboxylic group (the major reactive sites); and (3) carbon mass in their structures. Key Words: humin extraction; sequential exhaustive extraction; quinones; polyphenol polymerization; Fe(oxy)hydroxides; adsorptionen_US
dc.description.abstract腐植物質之研究大多數採用氫氧化鈉作為萃取溶液,也就是國際腐植質學會(IHSS)普遍選用的方法。然而,腐植素不溶於鹼液之特性難以用上述方法所萃取。近年來以連續消耗性抽出方法(SEE)進行腐植素的抽出已經被應用於與熱帶亞馬遜與溫帶愛爾蘭高緯度地區。實驗選用 SEE 萃取方法對台灣的火山土壤加以分離腐植酸、黃酸以及腐植素。結果顯示,各 pH 階段所萃取出的腐植酸及黃酸,隨著萃取 pH 值的升高,其所抽出的脂肪族碳含量相對性增加。而 SEE 所萃取出的腐植酸/黃酸與用 IHSS 方法有相似的結果,各萃取流程的組成份在效率和產量上雖有所不同,其累積萃取效率在 SEE(65%)方法較 IHSS(33%)為高,但不會改變各組分的化學結構。此外,將殘餘的土壤以鹼液連續性進行一次、三次以及八次的抽出後,再以 SEE 方法的最後一個步驟利用 DMSO 加以萃取腐植素,結果顯示隨著萃取次數的增加,其結晶性 polymethylene hydrocarbon 亦有增加之趨勢,說明晶性佳的烴結構與礦物膠體之鍵結將增加萃取的困難度。土壤中普遍存在的腐植物質與黏土礦物促成土壤團粒結構,即一種有機-黏土基質。醌類化合物是經由二氧化錳之非生物性催化作用氧化聚合多酚類化合物所形成,此多酚類的反應被認為是腐植化作用之前趨物之一。釐清醌類及腐植物質與廣泛分布於土壤環境中的鐵(氫)氧化物之反應機制有助於瞭解無機礦物在土壤中腐植化作用及其對環境中的物理及化學作用之影響。鐵(氫)氧化物吸附腐植酸及醌類化合物有 HA>HQ-20>HQ-7>HQ-1 之趨勢。在較低的 pH 值(pH 4),土壤礦物對腐植酸/黃酸有較高之吸附量;隨著 pH 值的增加,當礦物膠體的 ZPC 值大於溶液 pH, 將顯著地降低其吸附量。鐵(氫)氧化物與土壤礦物對於腐植酸/黃酸在吸附量上為水合鐵礦>針鐵礦>高嶺土≒蒙特石。經由傅立葉紅外光譜結果顯示,波數 1720的消失以及 1609、1575 的變寬及強度增加,顯示腐植酸/醌類化合物之羧基與鐵(氫)氧化物表面的氫氧基進行配位基交換,形成強的內圈錯合物。利用中空管柱過濾系統(hollow-fiber filtration)將腐植酸分為>100 kD、50-100 kD 以及<50 kD 三個不同分子量範圍的腐植酸分布。動力吸附結果顯示大分子腐植酸(> 100 KD)被固定在礦物表面比小分子腐植酸上有較高的偏好。而優先吸附的原因包含一、芳香性碳結構(增加疏水性交互作用),二、羧基官能基(主要的吸附位置),三、含碳量。 關鍵字: 腐植素萃取; 連續消耗性抽出方法; 醌; 氧化聚合; 鐵(氫)氧化物; 吸附zh_TW
dc.description.tableofcontents中文摘要.................................................. I ABSTRACT ............................................... III TABLE OF CONTENTS ........................................ V LIST OF TABLES......................................... VIII LIST OF FIGURES ......................................... IX CHAPTER 1 ................................................ 1 INTRODUCTION AND LITERATURE REVIEW ....................... 1 1.1. The Concepts and Importance of Humic Substances ... 1 1.2. Isolation and Fractionation of HSs................. 3 1.3. The Concepts of Humic Substances-like Materials ... 5 1.4. The Interactions of Humic Substances and Short-Ranged Ordered (SRO) Fe (oxy)hydroxide/mineral .................. 7 CHAPTER 2 ............................................... 12 A Comparison of the Compositional Differences Between Humic Fractions Isolated by the IHSS and Exhaustive Extraction Procedures............................................... 12 2.1. INTRODUCTION...................................... 12 2.2. MATERIALS AND METHODS ............................ 16 2.2.1. Sampling Site ............................... 16 2.2.2. Extraction of HAs and FAs ................... 17 2.2.3. Extraction of Humin .............................. 18 2.2.4. Sample Characterizations.......................... 22 2.2.4.1. UV-Vis Spectroscopy ......................... 22 2.2.4.2. Elemental Compositions ...................... 22 2.2.4.3. FT-IR Spectroscopy........................... 22 2.2.4.4. CPMAS 13C-NMR Spectroscopy................... 23 2.3. RESULTS AND DISCUSSION ............................. 23 2.3.1. Characteristics of HA and FA Extracted by IHSS Method .................................................. 23 2.3.2. Characteristics of HA and FA Fractions Extracted by SEE Method .............................................. 27 2.3.2.1. Isolation of Components with Base/Urea .... 33 2.3.3. Characteristics of Humins Isolated by IHSS and SEE Methods.................................................. 35 2.3.4. Cumulative Extraction Efficiency of SEE and IHSS Methods for the Volcanic Soil ........................... 39 2.3.5. Evaluation of the Suitability of the SEE Method for Isolations of Organic Matter from Soils in Different Climate Regions.................................................. 41 2.4. CONCLUSIONS ........................................ 44 CHAPTER 3................................................ 46 The Interactions of Humic Substances onto Clay and Fe-(oxy)hydroxide Colloid and Prolong the Quinones as Influenced by Chemical Structure and Molecular Size..................................................... 46 3.1. INTRODUCTION...................................... 46 3.2. MATERIALS AND METHODS ............................ 50 3.2.1. Sample Preparations.......................... 50 3.2.1.1. Clay Minerals ......................... 50 3.2.1.2. Syntheses of Fe(oxy)hydroxides .........51 3.2.2. Humic Substances ............................ 51 3.2.2.1. Extraction and Fractionation of HA and FA ......................................................... 51 3.2.3. Polymerization of Quinone ................... 52 3.2.4. Sorption of Humic Substances on Clay Minerals 53 3.2.4.1. Preparation of Stock Solution ......... 53 3.2.4.2. Sorption Kinetics ..................... 53 3.2.4.3. Sorption Kinetics of HA and FA on Goethite and Ferrihydrite at pH 4, 6 and 8 ....................... 54 3.2.4.4. Sorption Envelopes .................... 54 3.2.4.5. Sorption Isotherm...................... 54 3.2.5. Sample Characterization ..................... 55 3.2.5.1. Total Organic Carbon (TOC) ............ 55 3.2.5.2. Elemental Composition.................. 55 3.2.5.3. Fourier Transform Infrared Spectroscopy (FT-IR spectroscopy) .................................... 55 3.2.5.4. Carbon-13 Nuclear Magnetic Resonance (13C-NMR spectroscopy) ....................................... 56 3.2.5.5. High Performance Size Exclusion Chromatography (HPSEC) ................................................. 56 3.2.5.6. Gas Chromatography-Mass Spectrometry (GC-MS)...................................................... 56 3.2.6. Kinetic Models and Isotherm Models ............... 57 3.2.6.1. Kinetic Models .............................. 57 3.2.6.2. Isotherm Models ............................. 57 3.3. RESULTS AND DISCUSSION ............................. 58 3.3.1. Adsorption Kinetics of HA/FA on Goethite and Ferrihydrite ............................................ 58 3.3.2. Adsorption Envelopes of HA/FA on Goethite and Ferrihydrite............................................. 62 3.3.3. Adsorption Isotherm of HA/FA on Goethite and Ferrihydrite ............................................ 66 3.3.4. Prolonged Time to Oxidative Polymerization of Quinones in the Presence of Birnessite .................. 71 3.3.5. Comparisons of the Characteristics and Sorption of HA, FA and Quinones onto Goethite and Ferrihydrite and Discuss of Time-dependent Change in the MWs Distribution ......................................................... 81 3.3.6. The Possible Fates of Quinones into Soil Environment ......................................................... 95 3.4. CONCLUSIONS ........................................ 97 3.5. APPENDIX ........................................... 99 CHAPTER 4 .............................................. 102 CONCLUSIONS ............................................ 102 REFERENCE .............................................. 106 LIST OF TABLES Table 2.1. The physical/chemical properties of volcanic Yamgming Mountain soil .................................. 17 Table 2.2. Elemental compositions (on ash-free basis), H/C, O/C and E4/E6 ratios of humic substances isolated by the IHSS and SEE method ..................................... 28 Table 2.3. Comparison of extracts from the Taiwanese volcanic soil and selected soils from Brazil, the USA, and Ireland ................................................. 43 Table 3.1. Kinetic parameters for the sorption of HA/FA on goethite and ferrihydrite ............................... 61 Table 3.2. Parameters of Langmuir and Freundlich isotherm models of HA onto goethite and ferrihydrite at pH 4, 6 and 8, respectively ......................................... 70 Table 3.3. Elemental composition (%) of HQ samples and comparisons with HA...................................... 75 Table 3.4. GC-MS peaks of HQ samples and HA identified by NIST Library ............................................ 80 Table 3.5. Integration of 13C-NMR spectra of HA and FA .. 84 Table 3.6. First and second order regressions for adsorption kinetics ................................................ 90 LIST OF FIGURES Figure 2.1. Flow chart for organic matter extractions by (a) the IHSS and (b) sequential exhaustive extraction (SEE) procedures ............................................. 21 Figure 2.2. (a) Infrared and (b) 13C-NMR spectra of HAs and FAs isolated from extracts by the IHSS method ........... 26 Figure 2.3. Infrared spectra of (a) HAs, and of (b) FAs isolated by the exhaustive extraction (SEE) method (pH7,0.1 M NaOH + 6 M urea following the exhaustive extraction method. HA and FA samples isolated by the IHSS method are used for comparison. .................................... 30 Figure 2.4. 13C-NMR spectra of (a) HAs, and of (b) FAs isolated from the exhaustive extraction (SEE) method (pH7,M NaOH + 6 M urea following the exhaustive extractions. Spectra for the IHSS-HAs and FAs (isolated by the IHSS method) are used for comparison.......................... 32 Figure 2.5. Comparison of (a) Infrared and (b) 13C-NMR spectra of DMSO humin isolated from the residue of the SEE exhaustive extract, and of humin-1, humin-3,humin-8 isolated after 1, 3, and 8 extractions using the IHSS method and of the humin in the residual soil following the DMSO/H2SO4 extraction. ............................................. 38 Figure 2.6. A comparison of the organic carbon (OC) contents (%) isolated by the IHSS extraction method with the cumulative extraction percentage of the OC in the different extracts and in the residual materials following each stage of the SEE isolation. ................................... 40 Figure 3.1. Adsorption kinetics of HA on (a) goethite with initial of concentration (Ci) of 26 mg L-1 and solid solution ratio (SSR) of 0.51 g L-1 and (b) ferrihydrite with Ci of 105 mg L-1 and SSR of 0.46 g L-1 at pH 4, 6, and 8. ......................................................... 59 Figure 3.2. Adsorption kinetics of FA on goethite (SSR 0.52 g L-1) and ferrihydrite (SSR 0.24 g L-1) with initial of concentration of 18 and 35 mg L-1 at pH 4. .............. 60 Figure 3.3. Adsorption envelopes for (a) HA and (b) FA with clay and Fe(oxy)hydroxides (SSR approximately 0.5 g L-1 except ferrifydrite with FA)..............................65 Figure 3.4. Adsorption isotherm for HA adsorption onto goethite and ferrihydrite at pH 4, 6, and8 (initial of HA conc. 6-53 mg L-1 for goethite and initial HA conc.60-180 mg L-1 for ferrihydrite, SSR=0.5-0.55) (right Y axis represents adsorption normalize by surface area).................... 69 Figure 3.5. Effect of incubation time on absorbance (400-700 nm) of filtrates from reaction of hydroquinone (a) without and (b) with birnessite at pH 6. ........................ 71 Figure 3.6. (a) FT-IR spectra of HQ samples within 1, 7 and 20 days polymerization,denoted as HQ-1, HQ-7 and HQ-20, respectively. HA from Yangming volcanic mountain is provided for comparison. (b) Enlargement of 600-2000 cm-1 region.. 74 Figure 3.7. HPSEC spectra of HQ-1, HQ-7, HQ-20 and HA ... 76 Figure 3.8. Total ion chromatogram of GC-MS spectra of hydroquinone and HQ samples at 1 and 20 days, denoted as HQ-1 and HQ-20, respectively. HA is shown for comparison. .. 78 Figure 3.9. 3D profile of GC-MS spectra of hydroquinone and HQ samples at 1 and 20 days, denoted as HQ-1 and HQ-20, respectively. HA is shown for comparison. ............... 79 Figure 3.10. Comparison of adsorption isotherm for HA and FA onto goethite and ferrihydrite at pH 4 (initial of HA and FA conc. 6-53 mg L-1 for goethite and initial HA and FA conc. 60-180 mg L-1 for ferrihydrite, SSR=0.51-0.55). ........ 83 Figure 3.11. 13C-NMR spectra of HA and FA. .............. 84 Figure 3.12. Size distributions of fractionated humic acids analyzed by HPSEC. ...................................... 85 Figure 3.13. Sorption kinetics of HAs with different molecular weights onto ferrihydrite at pH 4 (with initial HA conc. of 8.7-9.94 mg L-1 and SSR of 0.05 g L-1). ........ 85 Figure 3.14. The HPSEC fractionation MWs of HA from the reaction solution (a) bulk (b) >100 kD (c) 50-100 kD and (d) <50 kD eliminated by ferrihydrite depending of time (0.05 g L-1, pH 4). ............................................. 86 Figure 3.15. Adsorption kinetics of HA, HQ-20, HQ-7, and HQ-1 on (a) ferrihydrite and (b) goethite at pH 4 and 25 oC with a suspension density of 0.25 and 0.62 g L-1, respectively ........................................... 89 Figure 3.16. Time-dependent changes for MW distribution of HQ-20 upon interaction with ferrihydrite. ............... 91 Figure 3.17. FTIR spectra of HA and FA. ................. 92 Figure 3.18. FTIR spectra of HA before and after interaction with (a) ferrihydrite and (b) goethite and spectra of HQ-20 before and after interaction with (c) ferrihydrite. ..... 94 Figure 3.19. The possible fate of hydroquinone into soil environment. ............................................ 96 Figure A3.1. XRD patterns of the solids residue separated from suspension by centrifugation after different reaction time between hydroquinone and birnessite................. 99 Figure A3.2. (a) FTIR spectra of the solids residue separated from suspension by centrifugation after different reaction time between hydroquinone and birnessite (b) comparison FTIR spectra of original birnessite and hydroquinone-birnessite system after 360 min. .......... 100 Fig. A3.3. Oxidative polymerization of hydroquinone with MnO2 by HPSEC. ......................................... 101zh_TW
dc.language.isoen_USzh_TW
dc.rights同意授權瀏覽/列印電子全文服務,2015-07-15起公開。zh_TW
dc.subjecthumin extractionen_US
dc.subjectsequential exhaustive extractionen_US
dc.subjectquinonesen_US
dc.subjectpolyphenol polymerizationen_US
dc.subjectFe(oxy)hydroxidesen_US
dc.subjectadsorptionen_US
dc.subject腐植素萃取zh_TW
dc.subject連續消耗性抽出方法zh_TW
dc.subjectzh_TW
dc.subject氧化聚合zh_TW
dc.subject鐵(氫)氧化物zh_TW
dc.subject吸附zh_TW
dc.titleInfluences of the chemical structures of humic substances (HS) extracted from a volcanic soil on the sorption of HS by selected clay minerals and Fe(oxy)hydroxidesen_US
dc.title火山灰土壤所萃取之腐植物質特性與其對吸附於黏土礦物及鐵(氫)氧化物的影響zh_TW
dc.typeThesis and Dissertationen_US
dc.date.paperformatopenaccess2015-07-15zh_TW
dc.date.openaccess2015-07-15-
item.openairecristypehttp://purl.org/coar/resource_type/c_18cf-
item.openairetypeThesis and Dissertation-
item.cerifentitytypePublications-
item.fulltextwith fulltext-
item.languageiso639-1en_US-
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