Hydrogen production from additive-free formic acid over highly active metal organic frameworks-supported palladium-based catalysts

摘要

The metal organic frameworks (MOFs) supported Pd catalysts for H-2 generation from formic acid (FA) were synthesized in this work, via a facile excessive impregnation-low temperature reduction approach. Among the synthetic catalysts, 10% Pd/MOF-Cr (18) displayed a remarkable performance for catalyzing FA dehydrogenation in additive-free aqueous solution, and the corresponding TOFmid achieved 537.8 h(-1) at 323 K. Furthermore, the bimetallic Ni-Pd alloy catalysts were prepared by the introduction of Ni in the subsequent work. Fortunately, 10% Ni0.4Pd0.6/MOF-Cr was found to be a highly active and fairly durable catalyst, exhibiting a TOF mld as high as 737.9 h(-1) at 323 K with almost 100% X-FA (final) and S-H2, and remained 94% of its original activity in the third cyclic catalysis. Meanwhile, Ni was discovered to be indispensable in increasing the electron density of Pd, downsizing the immobilized metal particles and inhibiting the agglomeration of the loaded nanoparticles. (C) 2020 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.