Abstract
Three of the major ligninolytic enzymes, lignin peroxidase (LiP), manganese peroxidase (MnP), and laccase (LA), as well as the secretome of a white-rot fungi, Grammothele fuligo, are tested on three industrial lignins (organosolv, alkali, and Kraft), to investigate and study the differences in biodegradation reactions and mechanism of these three lignins. Strategies involving additives in laccase mediated systems were also considered to produce small phenolic compounds. Three new or underreported additives including 2,4,6-tri-tert-butylphenol (TTBP), 4-tert-butyl-2,6-dimethylphenol (TBDMP), and 3-hydroxyanthranilic acid (HAA) are compared to three classic laccase mediators violuric acid (VA), 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) (ABTS), and 1-hydroxybenzotriazole (1-HBT). Decrease of molecular weight by up to 73% could be obtained on organosolv lignin with LA-VA systems, and by 49%, 43%, and 39% when LA was used with ABTS, TBDMP, and 1-HBT, respectively. In-depth analysis of the degradation products by quantitative 2D HMQC NMR indicated that the oxidation is mediator-dependent and provides new insights on the enzymatic mechanism.
| Original language | English |
|---|---|
| Pages (from-to) | 10097-10107 |
| Number of pages | 11 |
| Journal | ACS Sustainable Chemistry and Engineering |
| Volume | 6 |
| Issue number | 8 |
| DOIs | |
| Publication status | Published - 6 Aug 2018 |
Keywords
- Biodegradation
- Biomass
- Degradation
- Depolymerization
- Enzymes
- Laccase
- Lignin
- Lignin peroxidase
- Manganese peroxidase
- Mediator
Cite this
}
Importance of mediators for lignin degradation by fungal laccase. / Longe, Lionel F.; Couvreur, Julien; Leriche Grandchamp, Mathilde; Garnier, Gil; Allais, Florent; Saito, Kei.
In: ACS Sustainable Chemistry and Engineering, Vol. 6, No. 8, 06.08.2018, p. 10097-10107.Research output: Contribution to journal › Article › Research › peer-review
TY - JOUR
T1 - Importance of mediators for lignin degradation by fungal laccase
AU - Longe, Lionel F.
AU - Couvreur, Julien
AU - Leriche Grandchamp, Mathilde
AU - Garnier, Gil
AU - Allais, Florent
AU - Saito, Kei
PY - 2018/8/6
Y1 - 2018/8/6
N2 - Three of the major ligninolytic enzymes, lignin peroxidase (LiP), manganese peroxidase (MnP), and laccase (LA), as well as the secretome of a white-rot fungi, Grammothele fuligo, are tested on three industrial lignins (organosolv, alkali, and Kraft), to investigate and study the differences in biodegradation reactions and mechanism of these three lignins. Strategies involving additives in laccase mediated systems were also considered to produce small phenolic compounds. Three new or underreported additives including 2,4,6-tri-tert-butylphenol (TTBP), 4-tert-butyl-2,6-dimethylphenol (TBDMP), and 3-hydroxyanthranilic acid (HAA) are compared to three classic laccase mediators violuric acid (VA), 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) (ABTS), and 1-hydroxybenzotriazole (1-HBT). Decrease of molecular weight by up to 73% could be obtained on organosolv lignin with LA-VA systems, and by 49%, 43%, and 39% when LA was used with ABTS, TBDMP, and 1-HBT, respectively. In-depth analysis of the degradation products by quantitative 2D HMQC NMR indicated that the oxidation is mediator-dependent and provides new insights on the enzymatic mechanism.
AB - Three of the major ligninolytic enzymes, lignin peroxidase (LiP), manganese peroxidase (MnP), and laccase (LA), as well as the secretome of a white-rot fungi, Grammothele fuligo, are tested on three industrial lignins (organosolv, alkali, and Kraft), to investigate and study the differences in biodegradation reactions and mechanism of these three lignins. Strategies involving additives in laccase mediated systems were also considered to produce small phenolic compounds. Three new or underreported additives including 2,4,6-tri-tert-butylphenol (TTBP), 4-tert-butyl-2,6-dimethylphenol (TBDMP), and 3-hydroxyanthranilic acid (HAA) are compared to three classic laccase mediators violuric acid (VA), 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) (ABTS), and 1-hydroxybenzotriazole (1-HBT). Decrease of molecular weight by up to 73% could be obtained on organosolv lignin with LA-VA systems, and by 49%, 43%, and 39% when LA was used with ABTS, TBDMP, and 1-HBT, respectively. In-depth analysis of the degradation products by quantitative 2D HMQC NMR indicated that the oxidation is mediator-dependent and provides new insights on the enzymatic mechanism.
KW - Biodegradation
KW - Biomass
KW - Degradation
KW - Depolymerization
KW - Enzymes
KW - Laccase
KW - Lignin
KW - Lignin peroxidase
KW - Manganese peroxidase
KW - Mediator
UR - http://www.scopus.com/inward/record.url?scp=85049171065&partnerID=8YFLogxK
U2 - 10.1021/acssuschemeng.8b01426
DO - 10.1021/acssuschemeng.8b01426
M3 - Article
VL - 6
SP - 10097
EP - 10107
JO - ACS Sustainable Chemistry & Engineering
JF - ACS Sustainable Chemistry & Engineering
SN - 2168-0485
IS - 8
ER -