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1.
Chem Sci ; 11(42): 11498-11508, 2020 Sep 26.
Article in English | MEDLINE | ID: mdl-34094394

ABSTRACT

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 1H-13C HSQC NMR spectrum of the RCF oligomers. Specifically, ß-5 γ-OH, ß-5 ethyl, ß-1 γ-OH, ß-1 ethyl, ß-ß 2x γ-OH, ß-ß 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.

2.
Chem Soc Rev ; 45(12): 3564, 2016 06 21.
Article in English | MEDLINE | ID: mdl-26487280

ABSTRACT

Correction for 'Synthesis, characterisation, and catalytic evaluation of hierarchical faujasite zeolites: milestones, challenges, and future directions' by D. Verboekend et al., Chem. Soc. Rev., 2015, DOI: .

3.
Chem Soc Rev ; 45(12): 3331-52, 2016 Jun 13.
Article in English | MEDLINE | ID: mdl-26313001

ABSTRACT

Faujasite (X, Y, and USY) zeolites represent one of the most widely-applied and abundant catalysts and sorbents in the chemical industry. In the last 5 years substantial progress was made in the synthesis, characterisation, and catalytic exploitation of hierarchically-structured variants of these zeolites. Hererin, we provide an overview of these contributions, highlighting the main advancements regarding the evaluation of the nature and functionality of introduced secondary porosity. The novelty, efficiency, versatility, and sustainability of the reported bottom-up and (predominately) top-down strategies are discussed. The crucial role of the relative stability of faujasites in aqueous media is highlighted. The interplay between the physico-chemical properties of the hierarchical zeolites and their use in petrochemical and biomass-related catalytic processes is assessed.

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