Chemically Activated Spruce Organosolv Lignin as a Carbocatalyst for Heterogeneous Oxidative Dehydrogenations in the Liquid Phase

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A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
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Date

2023-09-01

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Department of Bioproducts and Biosystems

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Language

en

Pages

14

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ACS Catalysis, Volume 13, issue 17, pp. 11362-11375

Abstract

Activated carbons obtained from organosolv lignin by chemical activation with KOH and oxidized with diluted HNO3 were studied as catalysts for aerobic oxidative dehydrogenation (ODH) reactions. The structure/activity relationship was investigated through multiple techniques revealing the crucial role of oxygen functionality distribution in promoting two mechanistically archetypical ODH probe reactions: (i) the tetrahydroquinoline (THQ) aromatization, which represents ODH triggered by hydride transfer, and (ii) the 2-phenyl indole homocoupling reaction, a model for single-electron transfer-promoted reactions. In particular, the catalytic activity, correlating with oxygen functionality distribution on the basis of X-ray photoelectron spectroscopy and temperature-programmed desorption analysis, was associated with the C═O surface functionalities, as confirmed by blocking experiments with 2,2,2-trifluoroethyl hydrazine. Kinetic profiling tools were employed to assess THQ ODH product inhibition effects on the overall yield of the process as well as the extent of stoichiometric activity of the carbocatalyst. The breadth of the developed catalysts’ applicability was explored through selected relevant ODH reactions.

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Funding Information: Financial support from the Academy of Finland [project no. 129062 (J.H.)] is acknowledged. The “Biocat” project funding from the Jane and Aatos Erkko Foundation is gratefully received (M.H. and J.H.). Publisher Copyright: © 2023 The Authors. Published by American Chemical Society.

Keywords

carbon materials, heterogeneous catalysis, lignin, organocatalysis, oxidative dehydrogenation

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DOI

10.1021/acscatal.3c02735

Citation

Lenarda, A, Melchionna, M, Aikonen, S, Montini, T, Fornasiero, P, Hu, T, Hummel, M & Helaja, J 2023, 'Chemically Activated Spruce Organosolv Lignin as a Carbocatalyst for Heterogeneous Oxidative Dehydrogenations in the Liquid Phase', ACS Catalysis, vol. 13, no. 17, pp. 11362-11375. https://doi.org/10.1021/acscatal.3c02735

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https://urn.fi/URN:NBN:fi:aalto-202309185918

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[article-cris] Kemian tekniikan korkeakoulu / CHEM