TiO2-mediated visible-light-driven hydrogen evolution by ligand-capped Ru nanoparticles

Nuria Romero, Renan Barrach Guerra, Laia Gil, Samuel Drouet, Ivan Salmeron-Sànchez, Ona Illa, Karine Philippot, Mirco Natali, Jordi García-Antón*, Xavier Sala

*Corresponding author for this work

Research output: Contribution to journalArticleResearchpeer-review

1 Citation (Scopus)

Abstract

Ru nanomaterials have recently emerged as potential substitutes for classical Pt-based cathodes for the hydrogen evolution reaction (HER). In this regard, nanoparticle surface-functionalization through the so-called organometallic approach is a promising strategy towards synthesizing tailored highly active and durable HER (photo)electrocatalysts with limitless tunability. Herein, efficient (turnover numbers over 480 molH2 molRu-1 and a turnover frequency of 21.5 molH2 h-1 molRu-1; apparent quantum yield of 1.3%) and durable (>100 h) visible-light-driven hydrogen evolution has been achieved at neutral pH with a ternary hybrid nanomaterial combining 4-phenylpyridine-capped Ru nanoparticles (RuPP), TiO2 nanocrystals and [Ru(bpy)2(4,4′-(PO3H2)2(bpy))]Cl2 (RuP) using triethanolamine (TEOA) as a sacrificial electron-donor. Photophysical analysis by means of transient absorption spectroscopy has been performed in order to shed light on the kinetics of the electron transfer events and to identify the rate-determining step of the overall photocatalytic process. TiO2 is shown to have a key role as (1) the support aiding the dispersion of the photocatalyst and limiting its agglomeration under turnover conditions and (2) the electron-transfer mediator enabling efficient electron communication between the catalyst and the anchored molecular photoabsorber. Finally, the evolution and fate of the photocatalyst in long-term HER photocatalysis are thoroughly analyzed.

Original languageEnglish
Pages (from-to)4170-4178
Number of pages9
JournalSustainable Energy and Fuels
Volume4
Issue number8
DOIs
Publication statusPublished - Aug 2020

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