Abstract
In this work, pyrolysis–molecular beam mass spectrometry analysis coupled with principal components analysis and 13C-labeled tetramethylammonium hydroxide thermochemolysis were used to study lignin oxidation, depolymerization, and demethylation of spruce wood treated by biomimetic oxidative systems. Neat Fenton and chelator-mediated Fenton reaction (CMFR) systems as well as cellulosic enzyme treatments were used to mimic the nonenzymatic process involved in wood brown-rot biodegradation. The results suggest that compared with enzymatic processes, Fenton-based treatment more readily opens the structure of the lignocellulosic matrix, freeing cellulose fibrils from the matrix. The results demonstrate that, under the current treatment conditions, Fenton and CMFR treatment cause limited demethoxylation of lignin in the insoluble wood residue. However, analysis of a water-extractable fraction revealed considerable soluble lignin residue structures that had undergone side chain oxidation as well as demethoxylation upon CMFR treatment. This research has implications for our understanding of nonenzymatic degradation of wood and the diffusion of CMFR agents in the wood cell wall during fungal degradation processes.
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Acknowledgments
We appreciate the support of the Department of Earth and Atmospheric Sciences at Purdue University for the 13C-TMAH thermochemolysis work, the Wood Utilization Research Center at the University of Maine for the financial support for the collaborative research conducted at Purdue University, and support from the National Renewable Energy Laboratory in Golden, Colorado, for their MBMS facilities and support staff. V.A. is also grateful to the Coordination for the Improvement of Higher Level Personnel (CAPES-Brazil) Grant No. 5192/06-4 for the financial support for his stay at the Wood Science and Technology Laboratories at the University of Maine, Orono, Maine, USA. This is paper 3058 of the Maine Agricultural and Forest Experiment Station.
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Arantes, V., Qian, Y., Kelley, S.S. et al. Biomimetic oxidative treatment of spruce wood studied by pyrolysis–molecular beam mass spectrometry coupled with multivariate analysis and 13C-labeled tetramethylammonium hydroxide thermochemolysis: implications for fungal degradation of wood. J Biol Inorg Chem 14, 1253–1263 (2009). https://doi.org/10.1007/s00775-009-0569-6
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DOI: https://doi.org/10.1007/s00775-009-0569-6