Design of Novel Graphene Materials as a Support for Palladium Nanoparticles: Highly Active Catalysts towards Ethanol Electrooxidation

Sadia Kabir, Alexey Serov, Kateryna Artyushkova, Plamen Atanassov

Research output: Contribution to journalArticlepeer-review

41 Scopus citations

Abstract

The electrooxidation of ethanol in alkaline media by palladium (Pd) nanoparticles supported on 3D-Graphene nanosheets with varying morphological and physicochemical properties was investigated using potentiodynamic and potentiostatic techniques. 30 wt.% Pd electrocatalysts were synthesized using a surfactant-free soft alcohol reduction method (SARM) and deposited on thermally (7 at.% H2, 800 °C) and chemically reduced (N2H4·xH2O, 80 °C) 3D-Graphene nanosheets. The morphology of the nanosheets was modified using silica (L90 and EH5) sacrificial templates. For the sake of comparison, Pd nanoparticles were also deposited on a commercial carbon support (Vulcan) using SARM and physically characterized using X-ray diffraction (XRD) and Transmission Electron Microscopy (TEM). The morphological and physicochemical properties of the 3D-Graphene supports were analyzed using Scanning Electron Microscopy (SEM), Nitrogen-sorption Brunauer-Emmett-Teller (BET), Energy-dispersive X-ray Spectroscopy (EDS) and Raman Spectroscopy. Our results show that thermally reduced 3D-Graphene nanosheets with a higher the degree of C-C sp2 hybridization improved the dispersion and reduced the average crystallite size of the Pd nanoparticles. Moreover, Pd nanoparticles supported on 3D-Graphene nanosheets modified with larger silica templates (L90) showed better tolerance towards poisoning species, possibly due to the larger pores etched into its matrix. Among the as-prepared catalysts, Pd nanoparticles of 6.3 nm supported on thermally reduced 3D-Graphene (BET surface area of 300 m2 g-1) exhibited the highest stability as well as peak current density of 1568 AgPdi-1, which was about 1.5, 2.5 and 3 times greater than Pd nanoparticles supported on chemically reduced 3D-Graphene, Vulcan and commercial Pt/C catalysts respectively.

Original languageEnglish
Pages (from-to)144-153
Number of pages10
JournalElectrochimica Acta
Volume203
DOIs
StatePublished - Jun 10 2016
Externally publishedYes

Funding

This material is based upon work supported in part by the U. S. Army Research Laboratory and the U. S. Army Research Office under contract/grant number W911NF1410092, “Nanomaterials Characterization Facility: Confocal Raman Microscope/Atomic Force Microscopy − WITec Alpha 300R”.

Keywords

  • 3D-Graphene
  • Ethanol electro-oxidation
  • alkaline media
  • electrocatalyst support
  • morphology

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