On Laccase-Catalyzed Polymerization of Biorefinery Lignin Fractions and Alignment of Lignin Nanoparticles on the Nanocellulose SurfaceviaOne-Pot Water-Phase Synthesis

Luyao Wang; Liping Tan; Liqiu Hu; Xiaoju Wang; Rajesh Koppolu; Teija Tirri; Bas van Bochove; Petri Ihalainen; Liji Sobhana Seleenmary Sobhanadhas; Jukka V. Seppälä; Stefan Willför; Martti Toivakka; Chunlin Xu

doi:10.1021/acssuschemeng.1c01576

On Laccase-Catalyzed Polymerization of Biorefinery Lignin Fractions and Alignment of Lignin Nanoparticles on the Nanocellulose SurfaceviaOne-Pot Water-Phase Synthesis

Luyao Wang
, Liping Tan
, Liqiu Hu
, Xiaoju Wang
, Rajesh Koppolu
, Teija Tirri
, Bas van Bochove
, Petri Ihalainen
, Liji Sobhana Seleenmary Sobhanadhas
, Jukka V. Seppälä
, Stefan Willför
, Martti Toivakka
, Chunlin Xu

Research output: Contribution to journal › Article › Scientific › peer-review

57 Citations (Scopus)

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 situpolymerization 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.

Original language	English
Pages (from-to)	8770-8782
Number of pages	13
Journal	ACS Sustainable Chemistry and Engineering
Volume	9
Issue number	26
DOIs	https://doi.org/10.1021/acssuschemeng.1c01576
Publication status	Published - Jun 2021
MoE publication type	A1 Journal article-refereed

Funding

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.

Keywords

alkaliphilic laccase
biomass
green chemistry
lignin polymerization
lignocellulosic nanocomposites

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10.1021/acssuschemeng.1c01576

Cite this

Wang, L., Tan, L., Hu, L., Wang, X., Koppolu, R., Tirri, T., Bochove, B. V., Ihalainen, P., Sobhanadhas, L. S. S., 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 SurfaceviaOne-Pot Water-Phase Synthesis. ACS Sustainable Chemistry and Engineering, 9(26), 8770-8782. https://doi.org/10.1021/acssuschemeng.1c01576

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title = "On Laccase-Catalyzed Polymerization of Biorefinery Lignin Fractions and Alignment of Lignin Nanoparticles on the Nanocellulose SurfaceviaOne-Pot Water-Phase Synthesis",

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{\textquoteright} oxidation. Furthermore,in situpolymerization 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.",

keywords = "alkaliphilic laccase, biomass, green chemistry, lignin polymerization, lignocellulosic nanocomposites",

author = "Luyao Wang and Liping Tan and Liqiu Hu and Xiaoju Wang and Rajesh Koppolu and Teija Tirri and Bochove, \{Bas van\} and Petri Ihalainen and Sobhanadhas, \{Liji Sobhana Seleenmary\} and Sepp{\"a}l{\"a}, \{Jukka V.\} and Stefan Willf{\"o}r and Martti Toivakka and Chunlin Xu",

note = "Funding Information: 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 {\AA}bo Akademi University ({\AA}AU) 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 {\AA}AU, 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 {\AA}AU. This work also made use of Aalto University Bioeconomy Facilities. Publisher Copyright: {\textcopyright} 2021 The Authors. Published by American Chemical Society",

year = "2021",

month = jun,

doi = "10.1021/acssuschemeng.1c01576",

language = "English",

volume = "9",

pages = "8770--8782",

journal = "ACS Sustainable Chemistry and Engineering",

issn = "2168-0485",

publisher = "American chemical society",

number = "26",

}

Wang, L, Tan, L, Hu, L , Wang, X, Koppolu, R, Tirri, T, Bochove, BV, Ihalainen, P, Sobhanadhas, LSS, Seppälä, JV, Willför, S , Toivakka, M & Xu, C 2021, 'On Laccase-Catalyzed Polymerization of Biorefinery Lignin Fractions and Alignment of Lignin Nanoparticles on the Nanocellulose SurfaceviaOne-Pot Water-Phase Synthesis', ACS Sustainable Chemistry and Engineering, vol. 9, no. 26, pp. 8770-8782. https://doi.org/10.1021/acssuschemeng.1c01576

On Laccase-Catalyzed Polymerization of Biorefinery Lignin Fractions and Alignment of Lignin Nanoparticles on the Nanocellulose SurfaceviaOne-Pot Water-Phase Synthesis. / Wang, Luyao; Tan, Liping; Hu, Liqiu et al.
In: ACS Sustainable Chemistry and Engineering, Vol. 9, No. 26, 06.2021, p. 8770-8782.

Research output: Contribution to journal › Article › Scientific › peer-review

TY - JOUR

T1 - On Laccase-Catalyzed Polymerization of Biorefinery Lignin Fractions and Alignment of Lignin Nanoparticles on the Nanocellulose SurfaceviaOne-Pot Water-Phase Synthesis

AU - Wang, Luyao

AU - Tan, Liping

AU - Hu, Liqiu

AU - Wang, Xiaoju

AU - Koppolu, Rajesh

AU - Tirri, Teija

AU - Bochove, Bas van

AU - Ihalainen, Petri

AU - Sobhanadhas, Liji Sobhana Seleenmary

AU - Seppälä, Jukka V.

AU - Willför, Stefan

AU - Toivakka, Martti

AU - Xu, Chunlin

N1 - Funding Information: 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. Publisher Copyright: © 2021 The Authors. Published by American Chemical Society

PY - 2021/6

Y1 - 2021/6

N2 - 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 situpolymerization 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.

AB - 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 situpolymerization 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.

KW - alkaliphilic laccase

KW - biomass

KW - green chemistry

KW - lignin polymerization

KW - lignocellulosic nanocomposites

UR - https://www.scopus.com/pages/publications/85110273928

U2 - 10.1021/acssuschemeng.1c01576

DO - 10.1021/acssuschemeng.1c01576

M3 - Article

AN - SCOPUS:85110273928

SN - 2168-0485

VL - 9

SP - 8770

EP - 8782

JO - ACS Sustainable Chemistry and Engineering

JF - ACS Sustainable Chemistry and Engineering

IS - 26

ER -

On Laccase-Catalyzed Polymerization of Biorefinery Lignin Fractions and Alignment of Lignin Nanoparticles on the Nanocellulose SurfaceviaOne-Pot Water-Phase Synthesis

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