From Ru-bda to Ru-bds: a step forward to highly efficient molecular water oxidation electrocatalysts under acidic and neutral conditions

Jing Yang, Lei Wang, Shaoqi Zhan, Haiyuan Zou, Hong Chen, Mårten S. G. Ahlquist, Lele Duan () and Licheng Sun ()
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Jing Yang: Southern University of Science and Technology
Lei Wang: Biotechnology and Health, KTH Royal Institute of Technology
Shaoqi Zhan: Biotechnology and Health, KTH Royal Institute of Technology
Haiyuan Zou: Southern University of Science and Technology
Hong Chen: Southern University of Science and Technology
Mårten S. G. Ahlquist: Biotechnology and Health, KTH Royal Institute of Technology
Lele Duan: Southern University of Science and Technology
Licheng Sun: Biotechnology and Health, KTH Royal Institute of Technology

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract Significant advances during the past decades in the design and studies of Ru complexes with polypyridine ligands have led to the great development of molecular water oxidation catalysts and understanding on the O−O bond formation mechanisms. Here we report a Ru-based molecular water oxidation catalyst [Ru(bds)(pic)2] (Ru-bds; bds2− = 2,2′-bipyridine-6,6′-disulfonate) containing a tetradentate, dianionic sulfonate ligand at the equatorial position and two 4-picoline ligands at the axial positions. This Ru-bds catalyst electrochemically catalyzes water oxidation with turnover frequencies (TOF) of 160 and 12,900 s−1 under acidic and neutral conditions respectively, showing much better performance than the state-of-art Ru-bda catalyst. Density functional theory calculations reveal that (i) under acidic conditions, the high valent Ru intermediate RuV=O featuring the 7-coordination configuration is involved in the O−O bond formation step; (ii) under neutral conditions, the seven-coordinate RuIV=O triggers the O−O bond formation; (iii) in both cases, the I2M (interaction of two M−O units) pathway is dominant over the WNA (water nucleophilic attack) pathway.

Date: 2021
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DOI: 10.1038/s41467-020-20637-8

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