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Wood Research and Technology

Holzforschung

Cellulose – Hemicelluloses – Lignin – Wood Extractives

Editor-in-Chief: Faix, Oskar / Salmén, Lennart

Editorial Board: Daniel, Geoffrey / Militz, Holger / Rosenau, Thomas / Sixta, Herbert / Vuorinen, Tapani / Argyropoulos, Dimitris S. / Balakshin, Yu / Barnett, J. R. / Burgert, Ingo / Rio, Jose C. / Evans, Robert / Evtuguin, Dmitry V. / Frazier, Charles E. / Fukushima, Kazuhiko / Gindl-Altmutter, Wolfgang / Glasser, W. G. / Holmbom, Bjarne / Isogai, Akira / Kadla, John F. / Koch, Gerald / Lachenal, Dominique / Laine, Christiane / Mansfield, Shawn D. / Morrell, J.J. / Niemz, Peter / Potthast, Antje / Ragauskas, Arthur J. / Ralph, John / Rice, Robert W. / Salin, Jarl-Gunnar / Schmitt, Uwe / Schultz, Tor P. / Sipilä, Jussi / Takano, Toshiyuki / Tamminen, Tarja / Theliander, Hans / Welling, Johannes / Willför, Stefan / Yoshihara, Hiroshi

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1437-434X
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Volume 65, Issue 4

Issues

Studies of the chemoenzymatic modification of cellulosic pulps by the laccase-TEMPO system

11th EWLP, Hamburg, Germany, August 16–19, 2010

Ilabahen Patel
  • Department of Chemistry, Division of Organic Chemistry, University of Natural Resources and Life Sciences (BOKU), Vienna, Austria
  • Department of Food Sciences and Technology, Division of Food Biotechnology, University of Natural Resources and Life Sciences, Vienna, Austria
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/ Roland Ludwig
  • Department of Food Sciences and Technology, Division of Food Biotechnology, University of Natural Resources and Life Sciences, Vienna, Austria
  • Research Center Applied Biocatalysis, Graz, Austria
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/ Dietmar Haltrich
  • Department of Food Sciences and Technology, Division of Food Biotechnology, University of Natural Resources and Life Sciences, Vienna, Austria
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/ Thomas Rosenau
  • Department of Chemistry, Division of Organic Chemistry, University of Natural Resources and Life Sciences (BOKU), Vienna, Austria
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/ Antje Potthast
  • Department of Chemistry, Division of Organic Chemistry, University of Natural Resources and Life Sciences (BOKU), Vienna, Austria
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Published Online: 2011-02-25 | DOI: https://doi.org/10.1515/hf.2011.035

Abstract

The chemoenzymatic modification of cellulosic pulps by the laccase-mediator system (LMS) consisting of laccase (EC 1.10.3.2) and the 2,2,6,6-tetramethylpiperidine-1-oxyl radical (TEMPO) has been investigated. The reaction proceeds under mild aqueous conditions (sodium citrate buffer pH 6, 30°C) and introduces primarily aldehyde groups into cellulose so that carboxyl groups amount to one-third to one-fifth of the carbonyl groups only. LMS treatment caused uniform oxidation of the material, also in the high-molecular weight area, which is a non-typical behavior compared to other chemical oxidations of cellulose. Treatment of the pulp only with TEMPO or only with laccase caused no changes whatsoever, whereas treatment with the TEMPO-derived oxoammonium ion (in the absence of laccase) introduced carbonyl groups into the pulp, but no carboxyls. This chemoenzymatic approach was compared to the well-known chemical approach by means of TEMPO and hypohalite. Both approaches yielded comparable distributions of functional groups at the low oxidation degrees studied, indicating a similar reaction mechanism with the TEMPO-derived oxoammonium ion being the actual oxidant. The laccase is able to generate this oxoammonium ion, which in turn oxidized the 6-hydroxymethyl group into the corresponding aldehyde.

Keywords: carbonyl content; carboxyl content; cellulose; gel permeation chromatography (GPC); laccase; laccase-mediator system (LMS); TEMPO oxidation

About the article

Corresponding author. Department of Chemistry, Division of Organic Chemistry, University of Natural Resources and Life Sciences (BOKU), Muthgasse 18, A-1190 Vienna, Austria


Received: 2010-09-24

Accepted: 2010-11-09

Published Online: 2011-02-25

Published Online: 2011-02-25

Published in Print: 2011-06-01


Citation Information: Holzforschung, Volume 65, Issue 4, Pages 475–481, ISSN (Online) 1437-434X, ISSN (Print) 0018-3830, DOI: https://doi.org/10.1515/hf.2011.035.

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