Engineering Ru@Ir Core–Shell Nanoparticles on Titanium Oxynitride–Graphene Support for a Highly Active and Durable pH-Universal Hydrogen Evolution Reaction

Popović, A.; Marić, Ivan; Bele, M.; Rems, E.; Huš, M.; Pavko, L.; Ruiz-Zepeda, F.; Bijelić, L.; Grgur, B.; Hodnik, N.; Smiljanić, M. (2025) Engineering Ru@Ir Core–Shell Nanoparticles on Titanium Oxynitride–Graphene Support for a Highly Active and Durable pH-Universal Hydrogen Evolution Reaction. ACS Catalysis, 15 (15). pp. 13444-13457. ISSN 2155-5435

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Abstract

The rational design of electrocatalysts with high activity, durability, and low precious metal content is key to advancing hydrogen production via water electrolysis. Here, we present a multifunctional electrocatalyst based on Ru@Ir core-shell nanoparticles anchored on a conductive titanium oxynitride-graphene hybrid support (Ru@Ir/TiO x N y -C), achieving superior performance for the hydrogen evolution reaction (HER) in both acidic and alkaline media. The combination of the core-shell Ru@Ir architecture and the strong metal-support interaction (MSI) with TiO x N y optimizes hydrogen and hydroxide adsorption energies, as confirmed by X-ray photoelectron spectroscopy and density functional theory (DFT) calculations. In alkaline media, Ru@Ir/TiO x N y -C outperforms commercial Pt/C with a remarkably low overpotential of 13 mV at 10 mA cm-2 and high mass activity, while in acidic conditions, it rivals Pt/C and surpasses monometallic analogs. The long-term stability of the composite is attributed to the enhanced nanoparticle anchoring and structural integrity provided by the TiO x N y support. This work shows that combining core-shell nanostructures with engineered conductive supports can effectively replace platinum in HER applications. Such a nanocomposite strategy offers a versatile platform for the development of advanced electrocatalysts across a broad range of energy conversion reactions.

Item Type:	Article
Uncontrolled Keywords:	hydrogen evolution reaction; iridium; ruthenium; core−shell structures; TiOxNy; MSI; DFT
Subjects:	NATURAL SCIENCES > Chemistry
Divisions:	Division of Materials Chemistry
Depositing User:	Ema Buhin Šaler
Date Deposited:	10 Mar 2026 12:09
URI:	http://fulir.irb.hr/id/eprint/11344
DOI:	10.1021/acscatal.5c02831

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