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Amine-Functionalized Carbon Bowl-Supported Pd-La(OH)3 for Formic Acid Dehydrogenation
Xiongfei Sun1, Guiyuan Zhang1, Qilu Yao1
1National Engineering Research Center for Carbohydrate Synthesis, Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education, Key Laboratory of Energy Catalysis and Conversion of Nanchang, College of Chemistry and Chemical Engineering, Jiangxi Normal University, Nanchang 330022, China.
Abstract:
Formic acid (HCOOH, FA) is emerging as an appealing carrier for hydrogen storage owing to its renewability, a high volumetric capacity of 53 g H2/L, and convenient storage/transportation as a liquid. It is highly desired but still a challenge to search highly efficient catalysts to realize hydrogen evolution from FA. Here, monodispersed and ultrasmall Pd-La(OH)3 nanoparticles (NPs) anchored on amine-functionalized N-doped porous carbon bowl (N-PCB-NH2) substrates have been fabricated through a facile wet chemistry approach. As a result of the ultrafine size of Pd-La(OH)3 NPs (1.6 nm), the deprotonation ability of La(OH)3 and amine groups, and the strong metal-support interaction between Pd-La(OH)3 and N-PCB-NH2, the as-prepared Pd-La(OH)3/N-PCB-NH2 catalyst exhibits 100% H2 selectivity and exceptional catalytic property with a high turnover frequency value up to 9585 h-1 for FA dehydrogenation at 323 K, which is superior to most of the heterogeneous catalysts ever reported. Kinetic isotope effect measurements demonstrate that the C-H bond cleavage is a rate-determining step in the FA dehydrogenation reaction as compared to the O-H bond dissociation. This work presents a feasible approach to synthesize supported ultrafine metal NP catalysts with porous bowl structures for H2 generation from FA.
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