Kaya, MuratBulut, AhmetYurderi, MehmetKaya, MuratAydemir, MuratBaysal, AkinDurap, FeyyazZahmakiran, MehmetChemical Engineering2024-07-052024-07-052018251144-05461369-926110.1039/c8nj03117ghttps://doi.org/10.1039/c8nj03117ghttps://hdl.handle.net/20.500.14411/2650Yurderi, Mehmet/0000-0002-0233-8940; Bulut, ahmet/0000-0002-1697-8623; Aydemir, Murat/0000-0002-4238-5012; Kaya, Murat/0000-0002-2458-8924Formic acid (HCOOH), a major by-product of biomass processing with high energy density, stability and non-toxicity, has a great potential as a safe and a convenient liquid hydrogen (H-2) storage material for combustion engines and fuel cell applications. However, high-purity hydrogen release from the catalytic decomposition of aqueous formic acid solution at desirable rates under mild conditions stands as a major challenge that needs to be solved for the practical use of formic acid in on-demand hydrogen generation systems. Described herein is a new nanocatalyst system comprised of 3-aminopropyltriethoxysilane-functionalized graphene nanosheet-supported PdAuNi alloy nanoparticles (PdAuNi/f-GNS), which can reproducibly be prepared by following double solvent method combined with liquid-phase chemical reduction, all at room temperature. PdAuNi/f-GNS selectively catalyzes the decomposition of aqueous formic acid through the dehydrogenation pathway (similar to 100% H-2 selectivity), in the absence of any promoting additives (alkali formates, Bronsted bases, Lewis bases, etc.). PdAuNi/f-GNS nanocatalyst provides CO-free H-2 generation with a turnover frequency of 1090 mol H-2 mol metal(-1) h(-1) in the additive-free dehydrogenation of formic acid at almost complete conversion (>= 92%) even at room temperature. The catalytic activity provided by PdAuNi/f-GNS nanocatalyst is higher than those obtained with the heterogeneous catalysts reported to date for the additive-free dehydrogenation of formic acid. Moreover, PdAuNi/f-GNS nanoparticles show high durability against sintering, clumping and leaching throughout the catalytic runs, so that the PdAuNi/f-GNS nanocatalyst retains almost its inherent catalytic activity and selectivity at the end of the 10th recycle.eninfo:eu-repo/semantics/closedAccess[No Keyword Available]ArticleQ2Q342191610316114WOS:000447971700068