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High-Performance Hydrogen Evolution Electrocatalysis Using Proton-Intercalated TiO2 Nanotube Arrays as Interactive Supports for Ir Nanoparticles

Abstract

Developing ultraefficient electrocatalytic materials for the hydrogen evolution reaction (HER) with low content of expensive platinum group metals (PGMs) via low-energy-input procedures is the key to the successful commercialization of green water electrolysis technologies for sustainable production of high-purity hydrogen. In this study, we report a facile room-temperature synthesis of ultrafine metallic Ir nanoparticles on conductive, proton-intercalated TiO2 nanotube (H-TNT) arrays via galvanic displacement. A series of experiments demonstrate that a controlled transformation of the H-TNT surface microstructure from neat open-top tubes to disordered nanostripe bundles (“nanograss”) is highly beneficial for providing an abundance of exposed Ir active sites. Consequently, for nanograss-engineered composites, outstanding HER activity metrics are achieved already at very low Ir(III) precursor concentrations. An optimum Ir@TNT cathode loaded with 5.7 μgIr cm–2 exhibits an overpotential of –63 mV at –100 mA cm–2 and a mass activity of 34 A mg–1Ir at –80 mV in acidic conditions, along with excellent catalytic durability and structural integrity. Density functional theory (DFT) simulations disclose that the hydrogen-rich TiO2 surface not only stabilizes the deposited Ir and weakens its H binding strength to moderate intensity, but also actively takes part in the HER mechanism by refreshing the Ir catalytic sites near the Ir|H-TiO2 interface, thus substantially promoting H2 generation. The comprehensive characterization combined with theory provides an in-depth understanding of the electrocatalytic behavior of H-TNT supported PGM nanoparticles and demonstrates their high potential as competitive electrocatalyst systems for the HER.

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Supplementary files

Article information


Submitted
31 Jul 2020
Accepted
07 Oct 2020
First published
08 Oct 2020

J. Mater. Chem. A, 2020, Accepted Manuscript
Article type
Paper

High-Performance Hydrogen Evolution Electrocatalysis Using Proton-Intercalated TiO2 Nanotube Arrays as Interactive Supports for Ir Nanoparticles

U. C. Lacnjevac, R. Vasilic, A. Dobrota, S. Djurdjic, O. Tomanec, R. Zboril, S. Mohajernia, N. T. Nguyen, N. V. Skorodumova, D. Manojlovic, N. R. Elezovic, I. A. Pasti and P. Schmuki, J. Mater. Chem. A, 2020, Accepted Manuscript , DOI: 10.1039/D0TA07492F

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