Hostname: page-component-78c5997874-8bhkd Total loading time: 0 Render date: 2024-10-31T23:36:34.178Z Has data issue: false hasContentIssue false

Effects of Pyrogallol on Al13 Tridecamer Formation And Humification

Published online by Cambridge University Press:  01 January 2024

G. S. R. Krishnamurti*
Affiliation:
Department of Soil Science, University of Saskatchewan, Saskatoon, SK, S7N 5A8, Canada
M. K. Wang*
Affiliation:
Department of Soil Science, University of Saskatchewan, Saskatoon, SK, S7N 5A8, Canada
P. M. Huang*
Affiliation:
Department of Soil Science, University of Saskatchewan, Saskatoon, SK, S7N 5A8, Canada
*
Present address: 313-855 West 16th Street, North Vancouver, B.C. V7P 1R2, Canada
Present address: Department of Agricultural Chemistry, National Taiwan University, Taipei, Taiwan 10764
*E-mail address of corresponding author: huangp@sask.usask.ca
Rights & Permissions [Opens in a new window]

Abstract

Core share and HTML view are not available for this content. However, as you have access to this content, a full PDF is available via the ‘Save PDF’ action button.

The Al13 polycation is the predominant hydroxy-Al species in partially neutralized solutions. However, the existence of the Al13 species and the factors governing its formation in terrestrial environments still remain obscure. The objective of this study was to investigate the influence of pyrogallol, a common polyphenol in soils, on the formation of Al13 tridecamer. Hydroxy-Al solutions with an OH/Al molar ratio of 2.2 (pH 4.53) at pyrogallol/Al molar ratios of 0, 0.01, 0.05, 0.1 and 0.5 were prepared and mixed with 0.5 M sodium sulfate to form aluminum sulfate precipitation products. The solid-state 27Al nuclear magnetic resonance (NMR) spectra of the precipitates show that the pyrogallol perturbed the formation of Al13 tridecamer species as indicated by the decrease in the intensity of resonance peak, observed at 62.5 ppm, with increase in the pyrogallol/Al molar ratio. The crystallization of the precipitated Al sulfates was also hampered by pyrogallol, resulting in the formation of X-ray non-crystalline products at a pyrogallol/Al molar ratio of 0.50. The absorbance at 465 and 650 nm of the hydroxy-Al-pyrogallol solutions, the C coprecipitated, the electron spin resonance and 13C CPMAS-NMR spectra of the precipitates indicate the concomitant enhanced abiotic humification of pyrogallol by the X-ray amorphous Al species.

Type
Research Article
Copyright
Copyright © 2004, The Clay Minerals Society

References

Akitt, J.W., (1989) Multinuclear studies of aluminum compounds Progress in NMR Spectroscopy 21 1139 10.1016/0079-6565(89)80001-9.CrossRefGoogle Scholar
Akitt, J.W. and Elders, J.M. (1988) Multinuclear magnetic resonance studies of the hydrolysis of aluminum (III). VIII. Base hydrolysis monitored at very high magnetic field. Journal of Chemical Society, Dalton Transactions, 13471356.Google Scholar
Akitt, J.W. and Farthing, A.J. (1981) Aluminum-27 nuclear magnetic resonance studies of the hydrolysis of aluminum (III). IV. Hydrolysis using sodium carbonate. Journal of Chemical Society, Dalton Transactions, 16171625.CrossRefGoogle Scholar
Akitt, J.W., Greenwood, N.N., Khandelwal, B.L. and Lester, G.D. (1972) 27Al nuclear magnetic resonance studies of the hydrolysis and polymerization of the hexa-aqua-aluminum (III) cation. Journal of Chemical Society, Dalton Transactions, 604610.CrossRefGoogle Scholar
Azaroff, L.V. and Buerger, M.J., (1958) The Powder Method in X-ray Crystallography New York McGraw Hill Inc. 342 pp.Google Scholar
Bassett, H. and Goodwin, T.H. (1949) The basic aluminum sulfates. Journal of Chemical Society (London), 22392279.CrossRefGoogle Scholar
Bersillon, J.L. Hsu, P.H. and Fiessinger, F., (1980) Characterization of hydroxy-aluminum solutions Soil Science Society of America Journal 44 630634 10.2136/sssaj1980.03615995004400030040x.CrossRefGoogle Scholar
Bertsch, P.M., (1987) Conditions for Al13 polymer formation in partially neutralized aluminum solutions Soil Science Society of America Journal 51 825828 10.2136/sssaj1987.03615995005100030046x.CrossRefGoogle Scholar
Bertsch, P.M., Adriano, D.C. and Salomons, W., (1989) Aluminum speciation: methodology and applications Advances in Environmental Sciences. Acidic Precipitation, Vol. 4: Soils, Aquatic Processes, and Lake Acidification New York Springer-Verlag 63105.Google Scholar
Bertsch, P.M. Parker, D.R. and Sposito, G., (1996) Aqueous polynuclear aluminum species The Environmental Chemistry of Aluminum Boca Raton, Florida CRC Press, Lewis Publishers 117168.Google Scholar
Bertsch, P.M. Layton, W.J. and Barnhisel, R.I., (1986) Speciation of hydroxyaluminum solutions by wet chemical and aluminum-27 NMR methods Soil Science Society of America Journal 50 14491454 10.2136/sssaj1986.03615995005000060014x.CrossRefGoogle Scholar
Bertsch, P.M. Thomas, G.W. and Barnhisel, R.L., (1986) Characterization of hydroxyaluminum solutions by aluminum-27 nuclear magnetic resonance spectroscopy Soil Science Society of America Journal 50 825828 10.2136/sssaj1986.03615995005000030051x.CrossRefGoogle Scholar
Bottero, J.Y. Cases, J.M. Fiessinger, F. and Peinier, J.E., (1980) Studies of hydrolyzed aluminum chloride solutions. I. Nature of aluminum species and composition of aqueous solutions Journal of Physical Chemistry 84 29332939 10.1021/j100459a021.CrossRefGoogle Scholar
Bottero, J.Y. Axelos, M. Tchoubar, D. Cases, J.M. Fripiat, J.J. and Fiessinger, F., (1987) Mechanism of formation of aluminum trihydroxide from Keggin Al13 polymers Journal of Colloid and Interface Science 117 4757 10.1016/0021-9797(87)90166-4.CrossRefGoogle Scholar
Flatten, T.P. and Garruto, R.M., (1992) Polynuclear ions in aluminum toxicity Journal of Theoretical Biology 156 129132 10.1016/S0022-5193(05)80660-5.CrossRefGoogle Scholar
Furrer, G. Phillips, B.L. Ulrich, K.-U. Pothie, R. and Casey, W.H., (2002) The origin of aluminum floes in polluted streams Science 297 22452247 10.1126/science.1076505.CrossRefGoogle Scholar
Hatcher, P.G. Schnitzer, M. Dennis, L.W. and Maciel, G.E., (1981) Aromaticity of humic substances in soils Soil Science Society of America Journal 45 10891094 10.2136/sssaj1981.03615995004500060016x.CrossRefGoogle Scholar
Hayes, M.H.B. Swift, R.S., Greenland, D.J. and Hayes, M.H.B., (1978) The chemistry of soil organic colloids The Chemistry of Soil Constituents New York John Wiley and Sons 179320.Google Scholar
Hiradate, S. Taniguchi, S. and Sakurai, K., (1998) Aluminum speciation in aluminum-silica solutions and potassium chloride extracts of acidic soils Soil Science Society of America Journal 62 630636 10.2136/sssaj1998.03615995006200030012x.CrossRefGoogle Scholar
Holland, T.J.B. and Redfern, S.A.T., (1997) Unit cell refinement from powder diffraction data: The use of regression diagnostics Mineralogical Magazine 61 6567 10.1180/minmag.1997.061.404.07.CrossRefGoogle Scholar
Huang, P.M., (1988) Ionic factors affecting aluminum transformations and the impact on soil and environmental sciences Advances in Soil Science 8 178 10.1007/978-1-4613-8771-8_1.CrossRefGoogle Scholar
Huang, P.M., Bollag, J.-M. and Stotzky, G., (1990) The role of soil minerals in influencing transformations of natural organics and xenobiotics in the environment Soil Biochemistry, Vol. 6 New York Marcel Dekker 29115.Google Scholar
Huang, P.M. Bollag, J.-M., Huang, P.M. Senesi, N. and Buffle, J., (1999) Minerals-organics-microorganisms interactions in the soil environment Structure and Surface Reactions of Soil Particles Chichester, UK John Wiley & Sons 339.Google Scholar
Huang, P.M. Wang, M.K. Kampf, N. Schulze, D.G., Dixon, J.B. and Schulze, D.G., (2002) Aluminum hydroxides Soil Mineralogy with Environmental Applications Madison, Wisconsin Soil Science Society of America 261289.Google Scholar
Hunter, D. and Ross, D.S., (1991) Evidence for a phytotoxic hydroxy-aluminum polymer in organic soil horizons Science 251 10561058 10.1126/science.251.4997.1056.CrossRefGoogle ScholarPubMed
Johansson, G., (1960) On the crystal structures of some basic aluminum sulfates Acta Chemica Scandinavica 14 771773 10.3891/acta.chem.scand.14-0771.CrossRefGoogle Scholar
Johansson, G. Lundgren, G. Sillen, L.G. and Soderquist, R., (1960) On the crystal structure of a basic aluminum sulfate and the corresponding selenate Acta Chemica Scandinavica 14 769771 10.3891/acta.chem.scand.14-0769.CrossRefGoogle Scholar
Kerven, G.L. Larsen, P.L. and Blarney, F.P.C., (1995) Detrimental sulfate effects on formation of Al13 tridecameric polycation in synthetic soil solutions Soil Science Society of America Journal 59 765771 10.2136/sssaj1995.03615995005900030019x.CrossRefGoogle Scholar
Krishnamurti, G.S.R. Wang, M.K. and Huang, P.M., (1999) Role of tartaric acid in the inhibition of the formation of Al13 tridecamer using sulfate precipitation Clays and Clay Minerals 47 658663 10.1346/CCMN.1999.0470512.CrossRefGoogle Scholar
Kunwar, A.C. Thompson, A.R. Gutowsky, H.S. and Oldfield, E., (1984) Solid state aluminum-27 NMR studies of tridecameric Al-oxo-hydroxy clusters in basic aluminum selenate, sulfate, and the mineral zunyite Journal of Magnetic Resonance 60 467474.Google Scholar
Larsen, P.L. Kerven, G.L. Edwards, D.G. et al. ,Date, R.A. (1995) et al. , Effects of silicic acid in the chemistry of monomeric and polymeric (Al13) aluminum species in solution Plant Soil Interactions at Low pH Dordrecht, The Netherlands Kluwer Academic Publishers 617621 10.1007/978-94-011-0221-6_97.CrossRefGoogle Scholar
Lothenbach, B. Furrer, G. and Schulin, R., (1997) Immobilization of heavy metals by polynuclear aluminum and montmorillonite compounds Environmental Science and Technology 31 14521462 10.1021/es960697h.CrossRefGoogle Scholar
Masion, A. Bottero, J.Y. Thomas, F. and Tchoubar, D., (1994) Chemistry and structure of Al(OH)/organic precipitates. A small-angle X-ray scattering study. 2. Speciation and structure of aggregates Langmuir 10 43494352 10.1021/la00023a068.CrossRefGoogle Scholar
Masion, A. Tchoubar, D. Bottero, J.Y. Thomas, F. and Villiéras, F., (1994) Chemistry and structure of Al(OH)/organic precipitates. A small angle X-ray scattering study. 1. Numerical procedure for speciation from scattering curves Langmuir 10 43444348 10.1021/la00023a067.CrossRefGoogle Scholar
Masion, A. Thomas, F. Tchoubar, D. Bottero, J.Y. and Tekely, P., (1994) Chemistry and structure of Al(OH)/organic precipitates. A small-angle X-ray scattering study. 3. Depolymerization of the Al13 polycation by organic ligands Langmuir 10 43534356 10.1021/la00023a069.CrossRefGoogle Scholar
McKeague, J.A. Cheshire, M.V. Andreaux, F. Berthelin, J., Huang, P.M. and Schnitzer, M., (1986) Organo-mineral complexes in relation to pedogenesis Interactions of Soil Minerals with Natural Organics and Microbes Madison, Wisconsin Soil Science Society of America 549592.Google Scholar
Mueller, D. Gessner, W. Schonherr, S. and Gorz, H., (1981) Basic aluminum salts and their solutions. X. NMR-investigations on the tridecameric aluminum-oxohydroxy cation Zeitschrift für Annorganische und Allgemeine Chemie 483 153160 10.1002/zaac.19814831219.Google Scholar
Parker, D.R. and Bertsch, P.M., (1992) Identification and quantification of the “Al13” tridecameric polycation using Ferron Environmental Science and Technology 26 908914 10.1021/es00029a006.CrossRefGoogle Scholar
Parker, D.R. and Bertsch, P.M., (1992) Formation of the “Al13” tridecameric polycation under diverse synthesis conditions Environmental Science and Technology 26 914921 10.1021/es00029a007.CrossRefGoogle Scholar
Parker, D.R. Kinraide, T.B. and Zelazny, L.W., (1989) On the phytotoxicity of polynuclear hydroxy-aluminum complexes Soil Science Society of America Journal 53 789796 10.2136/sssaj1989.03615995005300030027x.CrossRefGoogle Scholar
Poleo, A.B.S., (1995) Aluminum polymerization — a mechanism of acute toxicity of aqueous aluminum to fish Aquatic Toxicology 31 347352 10.1016/0166-445X(94)00083-3.CrossRefGoogle Scholar
Ross, D.S. Bartlett, R.J. and Zhang, H., (2001) Photochemically induced formation of the ‘Al13’ tridecameric polycation in the presence of Fe(III) and organic acids Chemosphere 44 827832 10.1016/S0045-6535(00)00341-6.CrossRefGoogle ScholarPubMed
Schnitzer, M., (1978) Recent findings on the characterization of humic substances extracted from soils from widely different climatic zones IAEA-SM-211/7, Soil Organic Matter Studies. Vol. II Vienna IAEA 117130.Google Scholar
Schnitzer, M. Barr, M. and Hortenstein, R., (1984) Kinetics and characteristics of humic acids produced from simple phenols Soil Biology and Biochemistry 16 371376 10.1016/0038-0717(84)90035-X.CrossRefGoogle Scholar
Shann, J.R. and Bertsch, P.M., (1993) Differential cultivar response to polynuclear hydroxy-aluminum complexes Soil Science Society of America Journal 57 116120 10.2136/sssaj1993.03615995005700010022x.CrossRefGoogle Scholar
Shindo, H. and Huang, P.M., (1982) Role of Mn(IV) oxide in abiotic formation of humic substances in the environment Nature 298 363365 10.1038/298363a0.CrossRefGoogle Scholar
Shindo, H. and Huang, P.M., (1984) Catalytic effects of manganese (IV), iron (III), aluminum and silicon oxides on the formation of phenolic polymers Soil Science Society of America Journal 48 927934 10.2136/sssaj1984.03615995004800040045x.CrossRefGoogle Scholar
Stevenson, F.J., (1994) Humus Chemistry 2nd New York John Wiley & Sons.Google Scholar
Thomas, F. Masion, A. Bottero, J.Y. Rouiller, J. Genevrier, F. and Boudot, D., (1991) Aluminum(III) speciation with acetate and oxalate. A Potentiometric and 27Al NMR study Environmental Science and Technology 25 15531559 10.1021/es00021a004.CrossRefGoogle Scholar
Thomas, F. Masion, A. Bottero, J.Y. Rouiller, J. Montigny, F. and Genevrier, F., (1993) Aluminum(III) speciation with hydroxy carboxylic acids. 27Al NMR study Environmental Science and Technology 27 25112516 10.1021/es00048a031.CrossRefGoogle Scholar
Thompson, A.R., Kunwar, A.C., Gutowsky, H.S. and Oldfield, E. (1987) Oxygen-17 and aluminum-27 nuclear magnetic resonance spectroscopic investigations of aluminum (III) hydrolysis products. Journal of Chemical Society, Dalton Transactions, 23172322.CrossRefGoogle Scholar
Tsai, P.P. and Hsu, P.H., (1984) Studies of aged OH-Al solutions using kinetics of Al-ferron reactions and sulfate precipitation Soil Science Society of America Journal 48 5965 10.2136/sssaj1984.03615995004800010011x.CrossRefGoogle Scholar
Vance, G.F. Stevenson, F.J. Sikora, F.J. and Sposito, G., (1996) Environmental chemistry of aluminum-organic complexes The Environmental Chemistry of Aluminum Boca Raton, Florida CRC Press, Lewis Publishers 169220.Google Scholar
Violante, A. Krishnamurti, G.S.R. Huang, P.M., Huang, P.M. Bollag, J.-M. and Senesi, N., (2002) Impact of organic substances on the formation and transformation of metal oxides in soil environments Interactions between Soil Particles and Microorganisms. Impact on the Terrestrial Ecosystem Chichester, UK John Wiley & Sons 133188.Google Scholar
Wang, D. and Anderson, D.W., (1998) Direct measurement of organic carbon content in soils by the Leco 12 carbon analyzer Communications in Soil Science and Plant Analysis 29 1521 10.1080/00103629809369925.CrossRefGoogle Scholar
Wang, M.C. and Huang, P.M., (2000) Characteristics of pyrogallol-derived polymers formed by catalysis of oxides Soil Science 165 737747 10.1097/00010694-200009000-00007.CrossRefGoogle Scholar
Wang, T.S.C. Huang, P.M. Chou, C.-H. Chen, J.-H., Huang, P.M. and Schnitzer, M., (1986) The role of soil minerals in the abiotic polymerization of phenolic compounds and formation of humic substances Interactions of Soil Minerals with Natural Organics and Microbes Madison, Wisconsin Soil Science Society of America 251285.Google Scholar
Wertz, J.E. and Bolton, J.R., (1972) Electron Spin Resonance — Elementary Theory and Practical Applications New York McGraw Hill Inc. 497 pp.Google Scholar
Wilson, M.A. and Goh, K.M., (1977) Proton-decoupled pulse Fourier-transform 13C NMR spectra of soil organic matter Journal of Soil Science 28 645652 10.1111/j.1365-2389.1977.tb02271.x.CrossRefGoogle Scholar
Yamaguchi, N.U. Hiradate, S. Mizoguchi, M. and Miyazaki, T., (2003) Formation and disappearance of Al tridecamer in the presence of low molecular weight organic ligands Soil Science and Plant Nutrition 49 551556 10.1080/00380768.2003.10410044.CrossRefGoogle Scholar