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Volume 14
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10.3390/catal14120953
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Article

Hydrogenolysis of Benzyl Phenyl Ether Using Nickel–Molybdenum Clay Catalysts—A Model for Cleaving Ether Linkages in Lignin

by
Indri B. Adilina
1,2,*,
Muhammad A. Fitriady
1,
Ferensa Oemry
3,
Fauzan Aulia
1,
Nino Rinaldi
1,
Gagus K. Sunnardianto
3,
Ian P. Silverwood
4 and
Stewart F. Parker
4,*
1
Research Center for Chemistry, National Research and Innovation Agency, KST BJ Habibie, Tangerang Selatan 15314, Banten, Indonesia
2
Research Collaboration Center for Advanced Energy Materials, Jalan Ganesha 10, Bandung 40132, West Java, Indonesia
3
Research Center for Quantum Physics, National Research and Innovation Agency, KST BJ Habibie, Tangerang Selatan 15314, Banten, Indonesia
4
ISIS Neutron and Muon Source, STFC Rutherford Appleton Laboratory, Chilton, Didcot, Oxfordshire OX11 0QX, UK
*
Authors to whom correspondence should be addressed.
Catalysts 2024, 14(12), 953; https://doi.org/10.3390/catal14120953
Submission received: 25 November 2024 / Revised: 21 December 2024 / Accepted: 21 December 2024 / Published: 23 December 2024
(This article belongs to the Section Biomass Catalysis)
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Abstract

The solvent-free hydrogenolysis (HDL) of benzyl phenyl ether (BPE), a model for the C–O (α-O-4) linkage in lignin, was investigated using NiMo-pillared clay catalysts in their reduced (NiMoPR) and sulfided (NiMoPS) forms. NiMoPS show higher activity and selectivity to give an equimolar mixture of toluene and phenol, demonstrating selective cleavage of the Caliphatic–O of BPE, while non-equimolar amounts were found for NiMoPR. Strong acid sites are dominant in NiMoPS, giving a higher total acidity compared to NiMoPR, which explains the higher selectivity of the sulfided catalyst towards the HDL products and monomeric aromatics. To understand the interaction of BPE on the catalyst surface, we carried out a comprehensive investigation of the 2D potential energy surface (PES) of BPE and the vibrational spectra using neutron scattering and computational studies. The results suggest that BPE is weakly adsorbed on NiMoPS and the pillared clay support (PILC) via a van der Waals or H-bonding interaction, but they are strongly chemisorbed on the NiMoPR due to covalent bonding. Weakly adsorbed BPE allows higher mobility during diffusion to the catalytic site, which promotes the higher activity of NiMoPS for the HDL. This work demonstrates the potential use of clay-supported NiMo catalysts for lignin valorization and the future circular economy.
Keywords: hydrogenolysis; lignin; benzyl phenyl ether; NiMo catalyst; pillared clay hydrogenolysis; lignin; benzyl phenyl ether; NiMo catalyst; pillared clay

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MDPI and ACS Style

Adilina, I.B.; Fitriady, M.A.; Oemry, F.; Aulia, F.; Rinaldi, N.; Sunnardianto, G.K.; Silverwood, I.P.; Parker, S.F. Hydrogenolysis of Benzyl Phenyl Ether Using Nickel–Molybdenum Clay Catalysts—A Model for Cleaving Ether Linkages in Lignin. Catalysts 2024, 14, 953. https://doi.org/10.3390/catal14120953

AMA Style

Adilina IB, Fitriady MA, Oemry F, Aulia F, Rinaldi N, Sunnardianto GK, Silverwood IP, Parker SF. Hydrogenolysis of Benzyl Phenyl Ether Using Nickel–Molybdenum Clay Catalysts—A Model for Cleaving Ether Linkages in Lignin. Catalysts. 2024; 14(12):953. https://doi.org/10.3390/catal14120953

Chicago/Turabian Style

Adilina, Indri B., Muhammad A. Fitriady, Ferensa Oemry, Fauzan Aulia, Nino Rinaldi, Gagus K. Sunnardianto, Ian P. Silverwood, and Stewart F. Parker. 2024. "Hydrogenolysis of Benzyl Phenyl Ether Using Nickel–Molybdenum Clay Catalysts—A Model for Cleaving Ether Linkages in Lignin" Catalysts 14, no. 12: 953. https://doi.org/10.3390/catal14120953

APA Style

Adilina, I. B., Fitriady, M. A., Oemry, F., Aulia, F., Rinaldi, N., Sunnardianto, G. K., Silverwood, I. P., & Parker, S. F. (2024). Hydrogenolysis of Benzyl Phenyl Ether Using Nickel–Molybdenum Clay Catalysts—A Model for Cleaving Ether Linkages in Lignin. Catalysts, 14(12), 953. https://doi.org/10.3390/catal14120953

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