分子钌配合物在质子交换膜水电解中的显著稳定性。
Remarkable stability of a molecular ruthenium complex in PEM water electrolysis.
作者信息
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
机构信息
Institute of Chemistry of Organometallic Compounds - National Research Council (ICCOM-CNR) Via Madonna del Piano 10, 50019 Sesto Fiorentino Florence Italy
Department of Chemistry and Applied Biosciences, ETH Hönggerberg CH-8093 Zürich Switzerland
出版信息
Chem Sci. 2022 Mar 3;13(13):3748-3760. doi: 10.1039/d1sc07234j. eCollection 2022 Mar 30.
The dinuclear Ru diazadiene olefin complex, [Ru(OTf)(μ-H)(Medad)(dbcot)], 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(OTf)(μ-H)(Medad)(dbcot)]@C evolves hydrogen at the cathode of a PEM electrolysis cell (400 mA cm, 1.9 V). A remarkable turn over frequency (TOF) of 7800 mol mol h 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(OTf)(μ-H)(Medad)(dbcot)].
双核钌二氮杂二烯烯烃配合物[Ru(OTf)(μ-H)(Medad)(dbcot)]是聚合物电解质膜（PEM）水电解槽中析氢的活性催化剂。当负载在高比表面积炭黑上且温度为80°C时，[Ru(OTf)(μ-H)(Medad)(dbcot)]@C在PEM电解槽的阴极析氢（400 mA cm，1.9 V）。在运行7天的过程中，保持了7800 mol mol⁻¹ h⁻¹的显著周转频率（TOF）。通过一系列在均相介质和电化学半电池中的模型反应，结合密度泛函理论（DFT）计算，来阐明[Ru(OTf)(μ-H)(Medad)(dbcot)]促进析氢的机理。
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