Remarkable stability of a molecular ruthenium complex in PEM water electrolysis

Marco Bellini; Jonas Bösken; Michael Wörle; Debora Thöny; Juan José Gamboa-Carballo; Frank Krumeich; Francesco Bàrtoli; Hamish A. Miller; Lorenzo Poggini; Werner Oberhauser; Alessandro Lavacchi; Hansjörg Grützmacher; Francesco Vizza

doi:10.1039/D1SC07234J

Remarkable stability of a molecular ruthenium complex in PEM water electrolysis†

Marco Bellini,

‡^a Jonas Bösken,

‡^b Michael Wörle,

^b Debora Thöny,

^b Juan José Gamboa-Carballo,

^bd Frank Krumeich,

^b Francesco Bàrtoli,^ac Hamish A. Miller,^a Lorenzo Poggini,

^a Werner Oberhauser,^a Alessandro Lavacchi,^a Hansjörg Grützmacher

*^b and Francesco Vizza

*^a

Author affiliations

* Corresponding authors

^a Institute of Chemistry of Organometallic Compounds – National Research Council (ICCOM-CNR), Via Madonna del Piano 10, 50019 Sesto Fiorentino, Florence, Italy
E-mail: francesco.vizza@iccom.cnr.it

^b Department of Chemistry and Applied Biosciences, ETH Hönggerberg, CH-8093 Zürich, Switzerland
E-mail: hgruetzmacher@ethz.ch

^c Department of Biotechnology, Chemistry and Pharmacy, University of Siena, Via Aldo Moro 2, Siena, Italy

^d Higher Institute of Technologies and Applied Sciences (InSTEC), University of Havana, 10600 Havana, Cuba

Abstract

The dinuclear Ru diazadiene olefin complex, [Ru₂(OTf)(μ-H)(Me₂dad)(dbcot)₂], is an active catalyst for hydrogen evolution in a Polymer Exchange Membrane (PEM) water electrolyser. When supported on high surface area carbon black and at 80 °C, [Ru₂(OTf)(μ-H)(Me₂dad)(dbcot)₂]@C evolves hydrogen at the cathode of a PEM electrolysis cell (400 mA cm⁻², 1.9 V). A remarkable turn over frequency (TOF) of 7800 mol_H₂ mol_catalyst⁻¹ h⁻¹ is maintained over 7 days of operation. A series of model reactions in homogeneous media and in electrochemical half cells, combined with DFT calculations, are used to rationalize the hydrogen evolution mechanism promoted by [Ru₂(OTf)(μ-H)(Me₂dad)(dbcot)₂].

Chemical Science

Remarkable stability of a molecular ruthenium complex in PEM water electrolysis†

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