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Ruthenium loaded moderate acidic SAPO-11 for hydrogenation of aromatic derivatives

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Abstract

Hydrotreating of lignin molecules by heterogeneous catalysts has been a significant area of research in recent eras. The current study describes the hydrotreatment of lignin-derived phenol, m-cresol, over ruthenium-incorporated SAPO-11. The developed catalyst hydrogenates m-cresol completely at 160 °C and 10 bar of hydrogen pressure, yielding 22% methyl cyclohexane, 22% methyl cyclohexanol, and 55% methyl cyclohexanone. Temperature-programmed reduction (TPR) studies using hydrogen as probe molecules show that metallic-ruthenium species exist on the SAPO-11. The desorption profile at 147–215 °C reveals the formation of dispersed metallic ruthenium on SAPO-11. The above observation is consistent with the in-situ formation of metallic ruthenium as an active species during the hydrotreating process at 160 °C in a hydrogen environment. The presence of ruthenium species increases the acidity of the ruthenium-incorporated SAPO-11 system, as demonstrated by the ammonia-temperature-programmed desorption profile. The increase in surface acidity and metallic ruthenium on the surface contribute to the hydrogenation of m-cresol via a hydrogen spillover process, as evidenced by hydrogen desorption in TPR using both fresh and reduced catalysts. The catalyst works for several cycles of m-cresol hydrotreating, and the system is easily regenerated, allowing it to maintain its original activity. The ruthenium incorporated SAPO-11 catalyst is a promising system as it can hydrogenate many other model systems, including guaiacol, toluene, anisole, and cumene.

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Acknowledgements

Dr. Soumya B. Narendranath acknowledges KSHEC, Govt. of Kerala for financial assistance (KSHEC-A3/344/Govt. Kerala-NKPDF/2022). Authors thank DST-SERB-CRG/2023/001107, for the financial support. Nimisha N P is grateful to DST INSPIRE (DST/INSPIRE/03/2019/000097) for the fellowship.

Funding

Funding was provided by Department of Science and Technology, Government of Kerala (Grant No. KSHEC-A3/344/Govt. Kerala-NKPDF/2022) and Department of Science and Technology, Ministry of Science and Technology, India (Grant Nos. DST/INSPIRE/03/2019/000097 and DST-SERB-CRG/2023/001107).

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SBN: Conceptualization-Lead, Formal analysis-Lead, Investigation-Lead, Methodology-Lead, Data curation-Equal, Software-Lead, Validation-Lead, Visualization-Lead, Writing—original draft-Lead, NPN: Conceptualization-Equal, Data curation-Equal, Formal analysis-Equal, Investigation-Equal, Methodology-Equal, Software-Equal, Writing—original draft-Equal. SN: Data curation-Equal, Investigation-Equal, Methodology-Equal, Software-Equal, Writing draft-Equal Formal analysis -Equal. KS: Data curation-Equal, Investigation-Equal, NJV: Data curation-Equal, Investigation-Equal, CPJ: Data curation-Equal, Investigation-Equal, AS: Project administration-Lead, Conceptualization-Lead, Conceptualization-Lead, Resources-Lead, Validation-Lead, Visualization-Lead, Supervision-Lead, Writing—review and editing-Lead.

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Correspondence to A. Sakthivel.

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Narendranath, S.B., Nimisha, N.P., Namitha, S. et al. Ruthenium loaded moderate acidic SAPO-11 for hydrogenation of aromatic derivatives. J Porous Mater 31, 1077–1086 (2024). https://doi.org/10.1007/s10934-024-01572-1

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