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Two biologically inspired tetranuclear nickel(II) catalysts: effect of the geometry of Ni4 core on electrocatalytic water oxidation

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Abstract

Two biologically inspired tetranuclear nickel complexes [Ni4(L–H)4(CH3COO)3]·Cl (1) and [Ni4(L–H)4(CH3COO)4]·2CH3OH (2) (L = di(pyridin-2-yl)methanediol) have been synthesized and investigated by a combination of X-ray crystallography, PXRD, electrochemistry, in-situ UV–Vis spectroelectrochemistry and DLS. Both of the two complexes feature a core composed of four Ni(II) ions with the same peripheral ligation provided by the anionic di(pyridin-2-yl)methanediol and MeCOO− ligands. Whereas, complex 1 possesses one distorted cubane-like [Ni4(µ3-O)4] core, while 2 has one extended butterfly-like [Ni4(µ3-O)2] core. The homogeneous electrocatalytic reactivity of the two water-soluble complexes for water oxidation have been thoroughly studied, which demonstrates that both of them can efficiently electrocatalyze water oxidation with high stability under alkaline conditions, at relatively low over-potentials (η) of 420–790 mV for 1 and 390–780 mV for 2, both in the pH range of 7.67–12.32, with the high TOF of about 139 s−1 (1) and 69 s−1 (2) at pH = 12.32, respectively. By a series of comparative experiments for complexes 1 and 2, we proposed that their crystal geometries play an important role in their electrocatalytic reactivity for water oxidation. We verified that biomimetic cubane geometry could promote OER catalysis with two very similar compounds for the first time.

Graphic abstract

Compared with 2, the biomimetic cubane topology of 1 could promote OER catalysis by facilitating efficient charge delocalization and electron-transfer.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (No. 21601171), Natural Science Foundation of Shandong Province (No. ZR2016BB08) and the Fundamental Research Funds for the Central Universities (Chinese Universities Scientific Fund, No. 201713028).

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  1. Key Laboratory of Marine Chemistry Theory and Technology, Ministry of Education, College of Chemistry and Chemical Engineering, Ocean University of China, Qingdao, 26610, Shandong, China

    Jinmiao Wang, Wangjing Xie, Xia Zhang, Yuhua Fan & Mei Wang

  2. Shandong Provincial Key Laboratory of Biochemical Engineering, College of Marine Science and Biological Engineering, Qingdao University of Science and Technology, Qingdao, 266042, Shandong, China

    Xiangmin Meng

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Wang, J., Meng, X., Xie, W. et al. Two biologically inspired tetranuclear nickel(II) catalysts: effect of the geometry of Ni4 core on electrocatalytic water oxidation. J Biol Inorg Chem 26, 205–216 (2021). https://doi.org/10.1007/s00775-020-01846-4

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