PdAu-MnOx nanoparticles supported on amine-functionalized SiO2 for the room temperature dehydrogenation of formic acid in the absence of additives
| Autor: | Orhan Alal, Mehmet Zahmakiran, Murat Kaya, Mehmet Gülcan, Metin Celebi, Ahmet Bulut, Yaşar Karataş, Ilknur Efecan Ertas, Hilal Kivrak, Mehmet Yurderi |
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| Jazyk: | angličtina |
| Rok vydání: | 2016 |
| Předmět: |
Hydrogen
Formic acid Process Chemistry and Technology Inorganic chemistry Nanoparticle chemistry.chemical_element 02 engineering and technology 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences Catalysis 0104 chemical sciences chemistry.chemical_compound Hydrogen carrier chemistry Dehydrogenation 0210 nano-technology General Environmental Science Palladium Hydrogen production |
| Popis: | Formic acid (HCOOH) has recently been suggested as a promising hydrogen carrier for fuel cell applications. However efficient hydrogen production through the decomposition of formic acid in the absence of additives under mild thermodynamic conditions constitutes a major challenge because of the ease poisoning of active metals with CO formed as intermediate during formic acid decomposition. Recently, we have reported (App. Catal. B: Env. 164 (2015) 324) our discovery that the separately nucleated MnOx nanoparticles act as CO-sponge around catalytically active Pd nanoparticles exist on the same support and enhances both the activity and CO-resistivity of Pd nanoparticles. Using this important finding, herein, we present a new catalyst system consists of the physical mixture of PdAu alloy and MnOx nanoparticles supported on amine-grafted silica (PdAu-MnOx/N-SiO2) for the room temperature dehydrogenation of formic acid in the absence of any additives. PdAu-MnOx/N-SiO2 catalyst was simply prepared by deposition-reduction technique in water at room temperature with high reproducibility and characterized by the combination of various spectroscopic tools including ICP-OES, P-XRD, DR/UV-vis, XPS, BFTEM, STEM-EDX, STEM-line analysis and CO-stripping voltammetry techniques. The sum of their results shows that the formation of physical mixture of PdAu alloy and MnOx (dmean=2.2 nm) nanoparticles on the surface of support material. This new catalytic material facilitates the hydrogen liberation through the additive-free formic acid dehydrogenation at room temperature with previously unprecedented activity (TOF=785 mol H-2 mol catalyst(-1) h(-1)), converging to that of the existing state of the art homogenous catalysts. This new superior catalytic system enables facile catalyst recovery and very high stability against agglomeration, leaching and CO poisoning, which make it highly reusable catalyst (retains >92% activity and 85% conversion at the 5th catalytic reuse) in the additive-free formic acid dehydrogenation at room temperature. (C) 2015 Elsevier B.V. All rights reserved. |
| Databáze: | OpenAIRE |
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