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Remarkable stability of a molecular ruthenium complex in PEM water electrolysis

The dinuclear Ru diazadiene olefin complex, [Ru(2)(OTf)(μ-H)(Me(2)dad)(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, [Ru(2)(OTf)(μ-H)(Me(2)dad)(dbcot)(2)]@C evolves hydr...

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Detalles Bibliográficos
Autores principales: Bellini, Marco, Bösken, Jonas, Wörle, Michael, Thöny, Debora, Gamboa-Carballo, Juan José, Krumeich, Frank, Bàrtoli, Francesco, Miller, Hamish A., Poggini, Lorenzo, Oberhauser, Werner, Lavacchi, Alessandro, Grützmacher, Hansjörg, Vizza, Francesco
Formato: Online Artículo Texto
Lenguaje:English
Publicado: The Royal Society of Chemistry 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8966732/
https://www.ncbi.nlm.nih.gov/pubmed/35432912
http://dx.doi.org/10.1039/d1sc07234j
Descripción
Sumario:The dinuclear Ru diazadiene olefin complex, [Ru(2)(OTf)(μ-H)(Me(2)dad)(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, [Ru(2)(OTf)(μ-H)(Me(2)dad)(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(H(2)) 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 [Ru(2)(OTf)(μ-H)(Me(2)dad)(dbcot)(2)].