Co-axial heterostructures integrating palladium/titanium dioxide with carbon nanotubes for efficient electrocatalytic hydrogen evolution

Giovanni Valenti, Alessandro Boni, Michele Melchionna, Matteo Cargnello, Lucia Nasi, Giovanni Bertoni, Raymond J. Gorte, Massimo Marcaccio, Stefania Rapino, Marcella Bonchio, Paolo Fornasiero (), Maurizio Prato () and Francesco Paolucci ()
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Giovanni Valenti: University of Bologna and INSTM
Alessandro Boni: University of Bologna and INSTM
Michele Melchionna: University of Trieste
Matteo Cargnello: Stanford University
Lucia Nasi: IMEM-CNR Institute, Parco area delle Scienze 37/A
Giovanni Bertoni: IMEM-CNR Institute, Parco area delle Scienze 37/A
Raymond J. Gorte: University of Pennsylvania
Massimo Marcaccio: University of Bologna and INSTM
Stefania Rapino: University of Bologna and INSTM
Marcella Bonchio: University of Padova
Paolo Fornasiero: University of Trieste
Maurizio Prato: University of Trieste
Francesco Paolucci: University of Bologna and INSTM

Nature Communications, 2016, vol. 7, issue 1, 1-8

Abstract: Abstract Considering the depletion of fossil-fuel reserves and their negative environmental impact, new energy schemes must point towards alternative ecological processes. Efficient hydrogen evolution from water is one promising route towards a renewable energy economy and sustainable development. Here we show a tridimensional electrocatalytic interface, featuring a hierarchical, co-axial arrangement of a palladium/titanium dioxide layer on functionalized multi-walled carbon nanotubes. The resulting morphology leads to a merging of the conductive nanocarbon core with the active inorganic phase. A mechanistic synergy is envisioned by a cascade of catalytic events promoting water dissociation, hydride formation and hydrogen evolution. The nanohybrid exhibits a performance exceeding that of state-of-the-art electrocatalysts (turnover frequency of 15000 H2 per hour at 50 mV overpotential). The Tafel slope of ∼130 mV per decade points to a rate-determining step comprised of water dissociation and formation of hydride. Comparative activities of the isolated components or their physical mixtures demonstrate that the good performance evolves from the synergistic hierarchical structure.

Date: 2016
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DOI: 10.1038/ncomms13549

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