TiO2-mediated visible-light-driven hydrogen evolution by ligand-capped Ru nanoparticles
Romero Fernández, Nuria (Universitat Autònoma de Barcelona. Departament de Química)
Barrach Guerra, Renan (UNICAMP - Instituto de Química)
Gil Jiménez, Laia (Universitat Autònoma de Barcelona. Departament de Química)
Drouet, Samuel (Centre National de la Recherche Scientifique. Université de Toulouse. Paul Sabatier University)
Salmeron-Sànchez, Ivan (Universitat Autònoma de Barcelona. Departament de Química)
Illa, Ona (Universitat Autònoma de Barcelona. Departament de Química)
Philippot, Karine (Centre National de la Recherche Scientifique. Université de Toulouse. Paul Sabatier University)
Natali, Mirco (Università degli Studi di Ferrara. Dipartimento di Scienze Chimiche e Farmaceutiche)
García-Antón, Jordi (Universitat Autònoma de Barcelona. Departament de Química)
Sala Román, Xavier (Universitat Autònoma de Barcelona. Departament de Química)

Data:	2020
Resum:	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-determiningstep 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.
Ajuts:	Ministerio de Economía y Competitividad CTQ2015-64261-R
Drets:	Tots els drets reservats.
Llengua:	Anglès
Document:	Article ; recerca ; Versió acceptada per publicar
Matèria:	SDG 7 - Affordable and Clean Energy
Publicat a:	Sustainable energy & fuels, Vol. 4, Issue 8 (August 2020) , p. 4170-4178, ISSN 2398-4902

DOI: 10.1039/d0se00446d

Postprint 11 p, 832.5 KB

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