Interconversion between CO₂ and HCOOH under Basic Conditions Catalyzed by PdAu Nanoparticles Supported by Amine-Functionalized Reduced Graphene Oxide as a Dual Catalyst

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Abstract

Recently, the utilization of formic acid (FA) or formate as promising hydrogen carriers through the interconversion between CO2 and HCOOH or HCO3– and HCOO–, respectively, has attracted increasing research interest. In this work, a PdAu bimetallic catalyst supported on phenylenediamine-alkalized reduced graphene oxide (Pd0.50Au0.50/PDA-rGO) was developed for catalyzing bicarbonate hydrogenation under basic conditions as well as FA/formate dehydrogenation under acidic and basic conditions. Without any additives, a very high yield (94%) of potassium formate (PF) can be achieved from the hydrogenation of potassium bicarbonate at 50 °C for 16 h. On the other hand, initial TOFs of 1.63 × 103 and 6.98 × 103 h–1 were accomplished in the dehydrogenations of 6 mol/L PF and 8 mol/L FA, respectively, at 80 °C. This work successfully demonstrates highly efficient CO2 hydrogenation and is the first report of a Pd-based heterogeneous catalyst for the additive-free dehydrogenation of concentrated (>6 mol/L) PF or FA solution. It significantly enhanced the hydrogen capacity and is of great interest for practical applications. The good performance of this catalyst is probably attributed to (i) the nanosized (1.8 ± 0.5 nm) metal particles, (ii) the presence of an amine group on the support, which can act as a proton scavenger, and (iii) the additional Au component prohibiting CO formation and enhancing the durability of the catalyst even in high concentration FA/formate solutions.

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