Engineering the electronic structure of Pt for selective hydrogenation of vanillin to vanillyl alcohol and p-cresol

[Display omitted] •The electronic structure of Pt was elaborately designed via regulating the SMSI.•Pt nanoparticles with 68.1 % Pt2+ facilitate the selective hydrogenation of vanillin to VA.•Pt nanoparticles with 64.7 % Pt4+ promote the hydrodeoxygenation of vanillin into p-cresol.•Pt2+ facilitates...

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Veröffentlicht in:Chemical engineering science 2024-12, Vol.300, p.120616, Article 120616
Hauptverfasser: Zhao, Zijiang, Huang, Songtao, Dong, Guanglu, Chen, Yi, Wang, Mingxuan, Xia, Molin, Song, Xin, Li, Xiaonian, Wei, Zhongzhe, Wang, Jianguo
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Sprache:eng
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Zusammenfassung:[Display omitted] •The electronic structure of Pt was elaborately designed via regulating the SMSI.•Pt nanoparticles with 68.1 % Pt2+ facilitate the selective hydrogenation of vanillin to VA.•Pt nanoparticles with 64.7 % Pt4+ promote the hydrodeoxygenation of vanillin into p-cresol.•Pt2+ facilitates the desorption of VA whilst Pt4+ showcases strong adsorption for VA.•H2 reduction strategy facilitates the electron transfer from Mo2TiC2 to Pt. The hydrogenation of vanillin stands as a pivotal platform reaction within biomass conversion processes, presenting a significant challenge in achieving controlled synthesis of different products. Here, we proffer different methodology for elaborately designing the electronic structure of Pt via regulating the strong metal-support interactions (SMSI) between Pt and Mo2TiC2, thereby facilitating the targeted synthesis of vanillyl alcohol (VA) and 2-methoxy-4-methylphenol (MMP) from vanillin. Appropriate H2 reduction can enhance the SMSI between Pt and Mo2TiC2, promoting the electron transfer from Mo2TiC2 to Pt, resulting in 200-Pt/Mo2TiC2 with 68.1 of Pt2+. However, the SR-Pt/Mo2TiC2 obtained through the galvanic replacement strategy possesses 64.7 % of Pt4+, which is attributed to the weaker spontaneous SMSI between Pt and Mo2TiC2. XPS adsorption experiments highlight the pivotal role of Pt2+ in facilitating the desorption of VA, resulting in the 200-Pt/Mo2TiC2 catalyst demonstrating exceptional selectivity towards VA (96 %). Meanwhile, SR-Pt/Mo2TiC2 showcases a predilection for the direct hydrogenation and deoxygenation of vanillin into MMP. This research not only marks the application of the MXene system to biomass conversion but also illuminates the relationship between the electronic structure of Pt and its selectivity towards VA and MMP.
ISSN:0009-2509
DOI:10.1016/j.ces.2024.120616