Bulut,A.Yurderi,M.Kaya,M.Aydemir,M.Baysal,A.Durap,F.Zahmakiran,M.Chemical Engineering2024-07-052024-07-052018251144-054610.1039/C8NJ03117G2-s2.0-85054025210https://doi.org/10.1039/C8NJ03117Ghttps://hdl.handle.net/20.500.14411/3892Formic 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 (H2) 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 (∼100% H2 selectivity), in the absence of any promoting additives (alkali formates, Brønsted bases, Lewis bases, etc.). PdAuNi/f-GNS nanocatalyst provides CO-free H2 generation with a turnover frequency of 1090 mol H2 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. © The Royal Society of Chemistry and the Centre National de la Recherche Scientifique.eninfo:eu-repo/semantics/closedAccess[No Keyword Available]ArticleQ2Q342191610316114