For the utilization of CO2, formic acid (FA) or formate attracted as a promising target molecules because of their interconversion form of HCO3-, CO32-, HCOOH (FA) and HCOO- in basic media. Among these forms, FA is one of the liquid organic hydrogen carrier (LOHC) to store and transport of hydrogen. Recently we have developed a high-pressure hydrogen generation protocol without any compressing procedures through the dehydrogenation of FA using Ir containing homogeneous catalysts. The developed process has the advantage of simple and continuous H2/CO2 separation to produce purified H2 and CO2 from the resultant high-pressure gas mixture (H2 and CO2). After the successful attempts in homogeneous catalysts, we further explore the heterogeneous catalysts for the same reaction. In this work, we develop a PdAu bimetallic catalyst supported on phenylenediamine (PDA) alkalized reduced graphene oxide (PdAu/PDA-rGO) for the bicarbonate hydrogenation as well as FA/formate dehydrogenation. The Pd/Au heterogeneous catalyst, efficiently hydrogenate the potassium bicarbonate and a high yield of potassium formate (PF) was achieved. On the other hand, initial TOFs of 6981 h-1 were accomplished in the dehydrogenations of 8 mol/L FA. This work successfully demonstrates the highly efficient CO2 hydrogenation to FA which significantly enhanced the hydrogen capacity and is of great interest for practical applications.

Interconversion between CO2 and HCOOH catalyzed by PdAu reduced graphene oxide

256th National Meeting (2018)

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