The polyphenol pathway and Maillard reaction (polycondensation of sugars and amino acids) are regarded as important pathways in natural humification. The significance of linking the Maillard reaction and polyphenol pathways into an integrated humification pathway has been addressed. However, the ability of mineral colloids commonly occurring in tropical and temperate environments to promote the Maillard reaction and integrated polyphenol-Maillard humification pathways remained to be uncovered. Furthermore, the effect of the nature and relative abundance of biomolecules on humification and associated reaction products remained to be studied.<p>The results of this study show that the structure of polyphenols and the relative molar ratio of polyphenol, glucose and glycine, significantly affected humification processes and the associated carbonate formation in the integrated polyphenol-Maillard reaction catalyzed by birnessite. Increasing the molar ratio of ortho-polyphenols (catechol and pyrogallol) to Maillard reagents in the polyphenol-Maillard pathway catalyzed by birnessite enhanced humification while suppressing the formation of rhodochrosite (MnCO3). The opposite trend of MnCO3 formation was observed in the meta-polyphenol (resorcinol)-Maillard reaction system. Increasing the amount of glucose in the integrated catechol-Maillard system under the catalysis of birnessite promoted the formation of Maillard reaction-type humic acid in the supernatant and MnCO3 in the solid phase.<p>The catalytic abilities of commonly occurring mineral colloids from temperate and tropical regions greatly differed in influencing humification processes and products in the Maillard reaction and integrated polyphenol-Maillard pathways. Compared with layer silicate colloids, the poorly ordered Fe and Mn oxides were by far the strongest catalysts of humification reactions in the Maillard and catechol-Maillard pathways. This accounted for the significant difference in reactivity between the sesquioxide-rich Oxisol clay from the high rainfall region of South Africa and the Mollisol clay from the Canadian Prairies. Furthermore, the nature of the mineral colloids also affected the extent of organic C accumulation in the solid phase upon humification, and related mineral surface alteration. The metal oxide- and Oxisol clay-catalyzed Maillard and catechol-Maillard reaction systems had the highest accumulation of organic C in the solid phase, indicating their significance in contributing to C sequestration in the environment.<p>The findings obtained in this study are of fundamental significance in understanding the influence of the atomic bonding, structural configuration and related surface properties of mineral colloids, and the nature and abundance of biomolecules on the abiotic humification pathways and related reaction products in natural environments.
| Identifer | oai:union.ndltd.org:LACETR/oai:collectionscanada.gc.ca:SSU.etd-08192008-094240 |
| Date | 21 August 2008 |
| Creators | Hardie, Ailsa Ghillaine |
| Contributors | Ward, D.E., Laird, D.A,, Kozak, L.M., Peak, D, Anderson, D.W., Huang, P.M. |
| Publisher | University of Saskatchewan |
| Source Sets | Library and Archives Canada ETDs Repository / Centre d'archives des thèses électroniques de Bibliothèque et Archives Canada |
| Language | English |
| Detected Language | English |
| Type | text |
| Format | application/pdf |
| Source | http://library.usask.ca/theses/available/etd-08192008-094240/ |
| Rights | unrestricted, I hereby certify that, if appropriate, I have obtained and attached hereto a written permission statement from the owner(s) of each third party copyrighted matter to be included in my thesis, dissertation, or project report, allowing distribution as specified below. I certify that the version I submitted is the same as that approved by my advisory committee. I hereby grant to University of Saskatchewan or its agents the non-exclusive license to archive and make accessible, under the conditions specified below, my thesis, dissertation, or project report in whole or in part in all forms of media, now or hereafter known. I retain all other ownership rights to the copyright of the thesis, dissertation or project report. I also retain the right to use in future works (such as articles or books) all or part of this thesis, dissertation, or project report. |
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