Investigation of the chemocatalytic and biocatalytic valorization of a range of different lignin preparations: The importance of β-O-4 content

Lancefield, Christopher S.; Rashid, Goran M. M.; Bouxin, Florent; Wasak, Agata; Tu, Wei-Chien; Hallett, Jason; Zein, Sharif; Rodríguez, Jaime; Jackson, S. David; Westwood, Nicholas J.; Bugg, Timothy D. H.

Abstract

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 characterized 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 valorization 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 valorization methods were obtained from preparations that showed highest β-O-4 content, while variable yields were obtained with preparations containing intermediate β-O-4 content, and little or no product was obtained with preparations containing low β-O-4 content.

Citation

Lancefield, C. S., Rashid, G. M. M., Bouxin, F., Wasak, A., Tu, W.-C., Hallett, J., Zein, S., Rodríguez, J., Jackson, S. D., Westwood, N. J., & Bugg, T. D. H. (2016). Investigation of the chemocatalytic and biocatalytic valorization of a range of different lignin preparations: The importance of β-O-4 content. ACS Sustainable Chemistry and Engineering, 4(12), 6921-6930. https://doi.org/10.1021/acssuschemeng.6b01855

• Journal Article Type: Article
• Acceptance Date: Sep 29, 2016
• Online Publication Date: Oct 3, 2016
• Publication Date: Dec 5, 2016
• Deposit Date: Oct 6, 2016
• Publicly Available Date: Oct 6, 2016
• Journal: ACS sustainable chemistry & engineering
• Print ISSN: 2168-0485
• Publisher: American Chemical Society
• Peer Reviewed: Peer Reviewed
• Volume: 4
• Issue: 12
• Pages: 6921-6930
• DOI: https://doi.org/10.1021/acssuschemeng.6b01855
• Keywords: β-O-4
• Public URL: https://hull-repository.worktribe.com/output/443859
• Publisher URL: 10.1021/acssuschemeng.6b01855
• Additional Information: This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Sustainable Chemistry and Engineering, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://pubs.acs.org/doi/abs/10.1021/acssuschemeng.6b01855
• Contract Date: Oct 6, 2016