Carbon-supported layered double hydroxide nanodots for efficient oxygen evolution: Active site identification and activity enhancement


In this study, we developed a novel confinement-synthesis approach to layered double hydroxide nanodots (LDH-NDs) anchored on carbon nanoparticles, which formed a three-dimensional (3D) interconnected network within a porous carbon support derived from pyrolysis of metal-organic frameworks (C-MOF). The resultant LDH-NDs@C-MOF nonprecious metal catalysts were demonstrated to exhibit super-high catalytic performance for oxygen evolution reaction (OER) with excellent operation stability and low overpotential (∼230 mV) at an exchange current density of 10 mAcm−2. The observed overpotential for the LDH-NDs@C-MOF is much lower than that of large-sized LDH nanosheets (321 mV), pure carbonized MOF (411 mV), and even commercial RuO2 (281 mV). X-ray absorption measurements and density functional theory (DFT) calculations revealed partial charge transfer from Fe3+ through an O bridge to Ni2+ at the edge of LDH-NDs supported by C-MOF to produce the optimal binding energies for OER intermediates. This, coupled with a large number of exposed active sides and efficient charge and electrolyte/reactant/product transports associated with the porous 3D C-MOF support, significantly boosted the OER performance of the LDH-ND catalyst with respect to its nanosheet counterpart. Apart from the fact that this is the first active side identification for LDH-ND OER catalysts, this work provides a general strategy to enhance activities of nanosheet catalysts by converting them into edge-rich nanodots to be supported by 3D porous carbon architectures.

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S. L. Z. and L. M. D. conceived and designed the project. S. L. Z., D. T. Z., S. J., Y. C. and J. C. D. performed the experiments. S. L. Z., H. J. L., J. C. D., and Z. R. X. analysed and discussed the experimental results. L. M. D. and S. L. Z. drafted the manuscript. D.-W. W., R. A., Z. H. X., and L. M. D. joined the discussion of data and gave useful suggestions. This work was supported by The ARC (Nos. DP190103881 and FL190100126).

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Correspondence to Liming Dai.

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Zhao, S., Zhang, D., Jiang, S. et al. Carbon-supported layered double hydroxide nanodots for efficient oxygen evolution: Active site identification and activity enhancement. Nano Res. (2021).

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  • carbon nanomaterials
  • layered double hydroxide (LDH) nanodots
  • metal-organic framework (MOF) derivatives
  • oxygen evolution reaction