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Issue 19, 2018
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Amine-functionalized graphene nanosheet-supported PdAuNi alloy nanoparticles: efficient nanocatalyst for formic acid dehydrogenation

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Abstract

Formic 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.

Graphical abstract: Amine-functionalized graphene nanosheet-supported PdAuNi alloy nanoparticles: efficient nanocatalyst for formic acid dehydrogenation

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Publication details

The article was received on 22 Jun 2018, accepted on 27 Aug 2018 and first published on 29 Aug 2018


Article type: Paper
DOI: 10.1039/C8NJ03117G
Citation: New J. Chem., 2018,42, 16103-16114
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    Amine-functionalized graphene nanosheet-supported PdAuNi alloy nanoparticles: efficient nanocatalyst for formic acid dehydrogenation

    A. Bulut, M. Yurderi, M. Kaya, M. Aydemir, A. Baysal, F. Durap and M. Zahmakiran, New J. Chem., 2018, 42, 16103
    DOI: 10.1039/C8NJ03117G

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