期刊
CHEMICAL SCIENCE
卷 11, 期 42, 页码 11498-11508出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0sc04182c
关键词
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资金
- EoS project BIOFACT
- FWO-SBO project BioWood
- Catalisti-SBO project NIBCON
- KU Leuven Internal Funds (PDM)
- Flanders Innovation & Entrepreneurship (innovation mandate - posdoc), through the Catalisti-SBO project NIBCON
- Bio Based Industries Joint Undertaking under the European Union's Horizon 2020 research and innovation programme [837890]
- KU Leuven (IDN project - FFASSD) EoS project BIOFACT
- Internal Funds of KU Leuven (C3 project - BIOCON)
- H2020 Societal Challenges Programme [837890] Funding Source: H2020 Societal Challenges Programme
In-depth structural analysis of biorefined lignin is imperative to understand its physicochemical properties, essential for its efficient valorization to renewable materials and chemicals. Up to now, research on Reductive Catalytic Fractionation (RCF) of lignocellulose biomass, an emerging biorefinery technology, has strongly focused on the formation, separation and quantitative analysis of the abundant lignin-derived phenolic monomers. However, detailed structural information on the linkages in RCF lignin oligomers, constituting up to 50 wt% of RCF lignin, and their quantification, is currently lacking. This study discloses new detailed insights into the pine wood RCF lignin oil's molecular structure through the combination of fractionation and systematic analysis, resulting in the first assignment of the major RCF-derived structural units in the H-1-C-13 HSQC NMR spectrum of the RCF oligomers. Specifically, beta-5 gamma-OH, beta-5 ethyl, beta-1 gamma-OH, beta-1 ethyl, beta-beta 2x gamma-OH, beta-beta THF, and 5-5 inter-unit linkages were assigned unambiguously, resulting in the quantification of over 80% of the lignin inter-unit linkages and end-units. Detailed inspection of the native lignin inter-unit linkages and their conversion reveals the occurring hydrogenolysis chemistry and the unambiguous proof of absence of lignin fragment condensation during proper RCF processing. Overall, the study offers an advanced analytical toolbox for future RCF lignin conversion and lignin structural analysis research, and valuable insights for lignin oil valorization purposes.
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