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

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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
    Dalian University of Technology (DUT))

  • Licheng Sun

    (Biotechnology and Health, KTH Royal Institute of Technology
    Dalian University of Technology (DUT)
    Westlake University)

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.

Suggested Citation

  • Jing Yang & Lei Wang & Shaoqi Zhan & Haiyuan Zou & Hong Chen & Mårten S. G. Ahlquist & Lele Duan & Licheng Sun, 2021. "From Ru-bda to Ru-bds: a step forward to highly efficient molecular water oxidation electrocatalysts under acidic and neutral conditions," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-020-20637-8
    DOI: 10.1038/s41467-020-20637-8
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