Formic acid (FA) is a promising hydrogen carrier due to its hydrogen content (4.3 wt.% or 53 g H2/L) and mild dehydrogenation reaction conditions (&lt; 80 °C). Previous studies revealed that the co-existence of formate during FA dehydrogenation increases the evolved gas quantity and reaction rate. Most of these studies considered formate a mere promoter, not considering that formate itself can be dehydrogenated by reacting with water by Pd nanoparticle catalyst. There has not enough study regarding the reaction path determinants during the dehydrogenation of mixtures of FA and formate. In this study, we demonstrate that the system proton concentration and FA concentration determines the hydrogen generation pathway. The system pH and composition of the accumulated gas were measured under operando conditions. By introducing the threshold point, the quantity and composition of the produced gas can be actively controlled and it can be determined when the dehydrogenation soucres can be changed. This can help discern whether the gas evolution suspension originates from chemical equilibrium or catalyst deactivation.

Determinants of the hydrogen generation soucres from a mixture of formic acid and formate

ACS Spring 2022

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