On Laccase-Catalyzed Polymerization of Biorefinery Lignin Fractions and Alignment of Lignin Nanoparticles on the Nanocellulose Surface via One-Pot Water-Phase Synthesis
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A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
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Date
2021-07-05
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Language
en
Pages
13
8770-8782
8770-8782
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ACS Sustainable Chemistry and Engineering, Volume 9, issue 26
Abstract
Two series of well-defined lignin fractions derived from birch and spruce alkaline lignin (AL) by sequential solvent fractionation (i-PrOH-EtOH-MeOH) were engaged in a structure–property-application relationship study. The bacterial-derived alkaliphilic laccase (MetZyme) extensively catalyzed the oxidation and polymerization of AL fractions in an aqueous alkaline solution (pH 10). Lignin fractions with low molar mass reached a higher polymerization degree due to more phenolic-OH groups serving as reactive sites of oxidation and better lignin-laccase accessibility arose from a lower lignin condensation degree than the high molar mass ones. In comparison, AL fractions from spruce were found to be less reactive toward the laccase-catalyzed polymerization than those from birch, which was attributed to the much pronounced aryl-vinyl moieties’ oxidation. Furthermore, in situ polymerization of birch AL fractions using microfibrillated cellulose as a structural template was conducted in an aqueous medium and a dispersion of nanocellulose with its fiber network evenly coated by aligned lignin nanoparticles was obtained. The present study not only provides fundamental insights on the laccase-assisted oxidation and polymerization of lignin but also presents a new perspective for valorizing lignin in biobased fiber products through green processing of solvent fractionation and enzymatic treatment.Description
Business Finland Project (43674/31/2020) is acknowledged for the research funding to the current work. L.T. would like to thank the financial support to conduct research mobility at Åbo Akademi University (ÅAU) provided by Johan Gadolin Scholar mobility funding programme. Both L.W. and L.H. would like to acknowledge the financial support from the China Scholarship Council (Student ID 201804910639 for L.W. and Student ID 201908120107 for L.H.) to their doctoral study at ÅAU, Finland. Jarl Hemming and Dr. Annika Smeds are greatly acknowledged on their help with GPC and Py/GC–MS analysis. Qingbo Wang is thanked for his work with DMA measurements. Dr. Andrey Pranovich is thanked for discussing while initializing the project. CH-Bioforce Oy (Espoo, Finland) is thanked for providing birch and spruce ALs. This work is also part of activities within the Johan Gadolin Process Chemistry Centre (PCC) at ÅAU. This work also made use of Aalto University Bioeconomy Facilities.
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Wang, L, Tan, L, Hu, L, Wang, X, Koppolu, R, Tirri, T, van Bochove, B, Ihalainen, P, Sobhana Seleenmary Sobhanadhas, L, Seppälä, J V, Willför, S, Toivakka, M & Xu, C 2021, ' On Laccase-Catalyzed Polymerization of Biorefinery Lignin Fractions and Alignment of Lignin Nanoparticles on the Nanocellulose Surface via One-Pot Water-Phase Synthesis ', ACS Sustainable Chemistry and Engineering, vol. 9, no. 26, pp. 8770-8782 . https://doi.org/10.1021/acssuschemeng.1c01576
