Han-xian Meng, Hao-ze Chen, Bin Hu, Ji Liu, Yang-wen Wu, Kai Li, Yao-bing Huang, Qiang Lu
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引用次数: 0
Abstract
Hydrogenation of biomass-derived levoglucosenone (LGO) into versatile dihydroleveglucosenone (Cyrene) is one of the most attractive biomass transformations due to its widespread application in chemical synthesis. LGO hydrogenation is commonly catalyzed by Pd/Pt catalysts, with the reaction being influenced by their crystal facets and reaction environment. Regrettably, the current understanding of the hydrogenation mechanism of LGO to Cyrene over these catalysts is limited. Herein, the catalytic hydrogenation mechanism of LGO to Cyrene on Pd/Pt catalysts was systematically studied based on the first principle calculations. Particularly, the roles of exposed crystal facets and the aqueous solution have been discussed. The hydrogenation of LGO begins with the absorption of its C═C bond, and the optimal pathways over Pd/Pt catalysts vary depending on different crystal facets. In addition, Pd(101) exhibits superior catalytic activity for LGO hydrogenation than that of Pt(111) when comparing the optimal facets of Pb and Pt catalysts (19.50 versus 185.05 kJ mol⁻¹). H2O chiefly affects the hydrogenation reactions by forming a hydrated derivative with LGO, altering the hydrogenation pathway for Cyrene production. This work can provide a theoretical basis for developing high-performance catalysts and exploring new ways to realize the efficient hydrogenation of LGO to Cyrene.
期刊介绍:
With an impact factor of 4.495 (2018), ChemCatChem is one of the premier journals in the field of catalysis. The journal provides primary research papers and critical secondary information on heterogeneous, homogeneous and bio- and nanocatalysis. The journal is well placed to strengthen cross-communication within between these communities. Its authors and readers come from academia, the chemical industry, and government laboratories across the world. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies, and is supported by the German Catalysis Society.