Abstract

Alcohols are attractive portable chemical carriers of hydrogen thanks to their reversible dehydrogenation, but the hydrogen release reaction is thermodynamically unfavorable. Coupling the alcohol dehydrogenation to acetal formation can shift the reaction thermodynamics for hydrogen production. Here, we stabilized Ir3+ and Sc3+ in a metal-organic framework (MOF) for tandem catalysis. The Ir3+ center bearing an α-hydroxybipyridine ligand catalyzes alcohol dehydrogenation, and the Sc3+ Lewis acid site catalyzes acetal formation that allows further dehydrogenation to form esters. The bifunctional UiO-bpyOH-IrCp-Sc catalyst effectively converts ethylene glycol to ester and H2 without producing CO.

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