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Hydrogenation and hydrodeoxygenation of aromatic lignin monomers over Cu/C, Ni/C, Pd/C, Pt/C, Rh/C and Ru/C catalysts: Mechanisms, reaction micro-kinetic modelling and quantitative structure-activity relationships
Abstract
Abstract In this integrated in silico and experimental study, the activity, selectivity and mechanisms of commercially-available noble and transition metal heterogeneous catalysts, on neutral (carbon) support were investigated for hydrodeoxygenation (HDO) of eugenol. The latter was selected as a model compound of lignin building blocks. An influence of the process operating conditions (temperature, pressure and initial solid loading) on the reaction pathway and product distribution was studied as well. The previously-proposed reaction network for phenols HDO over Ru/C was found valid also for other platinum-group- (Pd, Pt and Rh) and non-noble (Cu or Ni) metallic clusters supported on C. Ru/C system exhibited the best HDO turnover performance, followed by the Rh/C, which especially demonstrated an excellent hydrogenation activity. Pt and Pd showed low deoxygenation and moderate hydrogenation activity. Kinetic parameters for all reactions on the surface were determined for all tested metals with a micro-kinetic model, by regression analysis on the foundation of 5760 experimentally-determined concentration values. Computation took into account resistances caused by transport phenomena, adsorption/desorption kinetics, and especially surface and bulk reaction kinetics. Ratio between adsorption and desorption rate constants for dissolved saturated, aromatic and hydrogen species were predicted, indicating a notable coverage effect on the catalyst reactivity. The saturation of functionalised benzene ring was approximately 3-, 11-, 32-, 10-, and 6-times faster than the C–O hydrogenolysis over ruthenium, platinum, palladium, rhodium and nickel, respectively. Methoxy group removal is easier from aromatics, compared to aliphatic species and also compared to the hydroxyl group removal. The heteroatom bond breaking for 2-methoxy-4-propylcyclohexanol proceed mostly via catechol-type diol formation, and subsequently, de-hydroxylation, particularly observable on Pt.
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Cites
Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell Cathode
Nørskov, J. K., Rossmeisl, J., Logadottir, A., Lindqvist, L., Kitchin, J. R., Bligaard, T., & Jónsson, H. (2004) · The Journal of Physical Chemistry B · doi:10.1021/jp047349j · Cited by 13,153
Cited by
Lignin as a potential source of high-added value compounds: A review
Zevallos Torres, L. A., Lorenci Woiciechowski, A., de Andrade Tanobe, V. O., Karp, S. G., Guimarães Lorenci, L. C., Faulds, C., & Soccol, C. R. (2020) · Journal of Cleaner Production · doi:10.1016/j.jclepro.2020.121499 · Cited by 389
Upgrading of biomass-derived bio-oil via catalytic hydrogenation with Rh and Pd catalysts
He, Y., Liu, R., Yellezuome, D., Peng, W., & Tabatabaei, M. (2022) · Renewable Energy · doi:10.1016/j.renene.2021.11.114 · Cited by 46
Lin, F., Ma, Y., Sun, Y., Song, Z., Men, X., Wu, Y., Zhu, Y., Gao, T., & Zhong, Y. (2022) · Renewable Energy · doi:10.1016/j.renene.2022.02.097 · Cited by 17
Metadata
- Authors
- Bjelić, A., Grilc, M., Huš, M., & Likozar, B.
- Venue
- Chemical Engineering Journal
- Publisher
- Elsevier BV
- Published
- 2019-03
- Volume
- 359
- Pages
- 305-320
- ISSN
- 1385-8947 (ISSN-L)
- OpenAlex
- W2901368818
- Cited by
- 242
- References
- 1
- FWCI
- 7.93
- Type
- journal article
- Language
- en
- Open access
- closed
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- CoChat. (2026). Citation check: Hydrogenation and hydrodeoxygenation of aromatic lignin monomers over Cu/C, Ni/C, Pd/C, Pt/C, Rh/C and Ru/C catalysts: Mechanisms, reaction micro-kinetic modelling and quantitative structure-activity relationships. https://app.cochat.ai/papers/10.1016/j.cej.2018.11.107
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- Bjelić, A., Grilc, M., Huš, M., & Likozar, B. (2019). Hydrogenation and hydrodeoxygenation of aromatic lignin monomers over Cu/C, Ni/C, Pd/C, Pt/C, Rh/C and Ru/C catalysts: Mechanisms, reaction micro-kinetic modelling and quantitative structure-activity relationships. Chemical Engineering Journal. https://doi.org/10.1016/j.cej.2018.11.107
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