Exploiting quasi-one-dimensional confinement for proficient hydrogen production from formic acid at room temperature

摘要

We describe herein that the quasi-one-dimensional confinement effect of functionalized nanoporous supports is particularly advantageous for boosting formic acid(FA)dehydrogenation efficiency over palladium nanoparticles(NPs).Benefiting from their unique structural merits that lead to significant lowering of the entropic barrier for FA activation,the Pd NPs interiorly located on the amino-modified MCM-41 offer the promise of more than an order of magnitude speedup of the initial activity in H2 production from FA over their exterior analogs.Under mild and additive-free conditions,ultrafine Pd NPs confined in aminomodified MCM-41 channels exhibit an initial turnover frequency as high as 46,677 h-1 and a turnover number up to 1,060,000 at 60℃.In conjunction with the enhancement and robust performance for efficient regeneration of FA via CO2 hydrogenation,the presented approach greatly contributes to the development of FA-based hydrogen storage and related technologies as viable means of enabling sustainable future energy prospects.