TY - JOUR
T1 - Investigation of the chemocatalytic and biocatalytic valorization of a range of different lignin preparations
T2 - the importance of β-O-4 content
AU - Lancefield, Christopher S.
AU - Rashid, Goran M. M.
AU - Bouxin, Florent
AU - Wasak, Agata
AU - Tu, Wei-Chien
AU - Hallett, Jason P.
AU - Zein, Sharif
AU - Rodríguez, Jaime
AU - Jackson, S. David
AU - Westwood, Nicholas J.
AU - Bugg, Timothy D. H.
N1 - This project was supported by a grant from the Lignocellulosic Biorefinery Network, a BBSRC-funded network in Biotechnology and Bioenergy.
PY - 2016/12/5
Y1 - 2016/12/5
N2 - A set of seven different lignin preparations was generated from a range of organosolv (acidic, alkaline, ammonia-treated and dioxane-based), ionic liquid, autohydrolysis and Kraft pretreatments of lignocelluloses. Each lignin was characterised by 2D HSQC NMR spectroscopy, showing significant variability in the β-O-4 content of the different lignin samples. Each lignin was then valorised using three biocatalytic methods (microbial biotransformation with Rhodococcus jostii RHA045, treatment with Pseudomonas fluorescens Dyp1B or Sphingobacterium sp. T2 manganese superoxide dismutase) and two chemocatalytic methods (catalytic hydrogenation using Pt/alumina catalyst, DDQ benzylic oxidation/Zn reduction). Highest product yields for DDQ/Zn valorisation were observed from poplar ammonia percolation-organosolv lignin, which had the highest β-O-4 content of the investigated lignins and also gave the highest yield of syringaldehyde (243 mg L-1) when using R. jostii RHA045, and the most enzymatic products using P. fluorescens Dyp1B. The highest product yield from the Pt/alumina hydrogenation was observed using oak dioxasolv lignin, which also had a high β-O-4 content. In general, highest product yields for both chemocatalytic and biocatalytic valorisation methods were obtained from preparations that showed highest β-O-4 content, while variable yields were obtained with preparations containing intermediate β-O-4content, and little or no product was obtained with preparations containing low β-O-4 content.
AB - A set of seven different lignin preparations was generated from a range of organosolv (acidic, alkaline, ammonia-treated and dioxane-based), ionic liquid, autohydrolysis and Kraft pretreatments of lignocelluloses. Each lignin was characterised by 2D HSQC NMR spectroscopy, showing significant variability in the β-O-4 content of the different lignin samples. Each lignin was then valorised using three biocatalytic methods (microbial biotransformation with Rhodococcus jostii RHA045, treatment with Pseudomonas fluorescens Dyp1B or Sphingobacterium sp. T2 manganese superoxide dismutase) and two chemocatalytic methods (catalytic hydrogenation using Pt/alumina catalyst, DDQ benzylic oxidation/Zn reduction). Highest product yields for DDQ/Zn valorisation were observed from poplar ammonia percolation-organosolv lignin, which had the highest β-O-4 content of the investigated lignins and also gave the highest yield of syringaldehyde (243 mg L-1) when using R. jostii RHA045, and the most enzymatic products using P. fluorescens Dyp1B. The highest product yield from the Pt/alumina hydrogenation was observed using oak dioxasolv lignin, which also had a high β-O-4 content. In general, highest product yields for both chemocatalytic and biocatalytic valorisation methods were obtained from preparations that showed highest β-O-4 content, while variable yields were obtained with preparations containing intermediate β-O-4content, and little or no product was obtained with preparations containing low β-O-4 content.
KW - Catalytic hydrogenation
KW - Dyp peroxidase
KW - Lignin valorization
KW - Microbial biotransformation
KW - Rhodococcus jostii RHA1
KW - Superoxide dismutase
U2 - 10.1021/acssuschemeng.6b01855
DO - 10.1021/acssuschemeng.6b01855
M3 - Article
SN - 2168-0485
VL - 4
SP - 6921
EP - 6930
JO - ACS Sustainable Chemistry & Engineering
JF - ACS Sustainable Chemistry & Engineering
IS - 12
ER -