Interfacial engineering of Ni/SiO2 via moderate-temperature calcination: Steering metal-support interaction for poplar lignin hydroconversion
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更新:2026-10-30 14:31:28 浏览:10次
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摘要
Abstract: Cyclanes serve as critical platform molecules for the synthesis of sustainable jet fuels, fine chemicals, and polymers. Utilizing renewable biomass resources such as lignin to produce value-added chemicals and liquid fuels is essential for reducing fossil fuel dependence and advancing global carbon neutrality strategies. Nevertheless, the efficient cleavage of >C-O bonds and simultaneous deoxygenation of lignin macromolecules remain technical bottlenecks. Herein, a highly dispersed mesoporous Ni/SiO2-500 was prepared via a deposition-precipitation method, which exhibits exceptional performance in the catalytic hydroconversion of lignin and lignin related model compounds. A moderate calcination temperature of 500 oC was employed to induce a pronounced metal-support interaction (MSI) between the active nickel phase and the silica support. This MSI effect effectively suppressed the thermal sintering and aggregation of Ni nanoparticles during high-temperature reduction, resulting in uniformly dispersed Ni nanoparticles with an average diameter of 4.25 nm while preserving a well-developed mesoporous structure with pore sizes ranging from 3 to 5 nm. These favorable structural features endow the catalyst with a high specific surface area, maximized exposure of active metal sites, and remarkably reduced intraparticle diffusion resistance for bulky lignin-derived molecules. Under the optimized conditions (220 oC, 2 MPa initial H2 pressure, and 4 h), phenoxyethylbenzene, employed as a lignin model compound, was subjected to complete conversion over Ni/SiO2-500. Furthermore, a combined relative product proportion of 95.9% was obtained for cyclohexane and ethylcyclohexane, with a target-product carbon contribution of 48.1%, demonstrating its superior performance in >C-O bond cleavage and aromatic ring hydrogenation. In addition, the catalytic hydroconversion of lignin over Ni/SiO2-500 yielded 72% soluble portions, with cyclanes and alkanes as the major constituents. Collectively, this work provides a feasible strategy for modulating metal-support interfacial interactions to develop efficient and stable non-noble metal catalysts, offering both fundamental insights and practical pathways for the value-added utilization of lignin resources and the sustainable production of advanced liquid biofuels.
关键词
Lignin,Catalytic hydroconversion,Cyclanes
稿件作者
Shou-Cheng Jiao
Zaozhuang University
Li Lii
Zaozhuang University
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