Journal
APPLIED CATALYSIS A-GENERAL
Volume 603, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcata.2020.117770
Keywords
Sorbitol; Selective hydrogenolysis; PdZn alloy; Propylene glycol; Ethylene glycol; Reaction mechanism
Categories
Funding
- National Key Research and Development Program of China [2016YFB0701100]
- Natural Science Foundation of China [21690081, 21832001, 21821004, 21805309]
- Beijing National Laboratory for Molecular Sciences [BNLMS-CXXM-201905]
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Sorbitol hydrogenolysis to industrially important propylene glycol and ethylene glycol receives increasing attention, recently. Here, we developed an efficient and stable PdZn alloy catalyst, in-situ formed from a physical mixture of Pd/ZrO2 and ZnO, for the sorbitol hydrogenolysis with Mg3AlOx as a solid base, and obtained a 54.6% yield of the two target glycols (493 K and 5.0 MPa H-2). The amounts of ZnO and Mg3AlOx strongly influenced the activity and selectivity, due to their effects on the formation of the PdZn alloys and the competitive metal-catalyzed dehydrogenation/hydrogenation and base-catalyzed retro-aldol condensation steps. The kinetic isotope effects, combined with the inhibiting effects of H-2 pressure on the activity in a broad range (3.0-8.0 MPa), confirm that the sorbitol dehydrogenation to hexose intermediates is the kinetically-relevant step in the sorbitol hydrogenolysis. This study provides insights into the catalytic functions and reaction parameters for the hydrogenolysis of polyols to the target glycols.
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