Journal
JOURNAL OF ENERGY CHEMISTRY
Volume 71, Issue -, Pages 89-97Publisher
ELSEVIER
DOI: 10.1016/j.jechem.2022.02.042
Keywords
Formation mechanism; Hierarchical transition metal oxyhydroxides; Aqueous solution; Ambient temperature; Oxygen evolution reaction
Funding
- Deutsche Forschungsgemeinschaft DFG
- Sino-German Center for Research Promotion [GZ 1351, CO 194/19-1]
- Chinese Scholarship Council
- Particle Analysis Center at the University of Konstanz [SFB1214]
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This study presents a facile method for the preparation of hierarchical CoOOH, NiOOH, and MnOOH structures using a one-step coprecipitation route. The research reveals that K2S2O8 induces the oxidation state change of metal ion species, and the combination of NH3 diffusion and the presence of K2S2O8 enables the formation of hierarchical oxyhydroxide structures in aqueous solution at ambient temperature without heat energy or additional structure-directing agents. The hierarchical CoOOH structures exhibit excellent activity as electrocatalysts for the oxygen evolution reaction, outperforming many similar catalysts.
First-row (3d) transition metal oxyhydroxides have attracted increasing attention due to their various advantages. Although investigating the oxidation mechanism and processing such materials into hierarchical architectures are greatly desired for their further development, it remains unclear how the oxidation state change occurs, and efforts to produce hierarchical oxyhydroxides in compliance with high ecological and economic standards have progressed slowly. Here, we describe a facile one-step coprecipitation route for the preparation of hierarchical CoOOH, NiOOH and MnOOH, which involves the diffusion of NH3 originating from ammonium hydroxide solution into an aqueous solution containing metal ion salts and K2S2O8. Comprehensive characterizations by scanning electron microscope, transmission electron microscopy, X-ray diffraction analysis, X-ray photoelectron spectroscopy, ultraviolet-visible spectroscopy and in situ pH measurement demonstrated that K2S2O8 induces the oxidation state change of metal ion species after the start of hydrolysis. Meanwhile, it was found that, benefiting from the OH- concentration gradient created by the NH3 diffusion method and the suitable growth environment provided by the presence of K2S2O8 (high nucleation rate and secondary nucleation), the formation of hierarchical oxyhydroxide structures can be realized in aqueous solution at ambient temperature without the use of heat energy and additional structure-directing agents. The hierarchical CoOOH structures are performed as the electrocatalysts for the oxygen evolution reaction in alkaline media, which exhibit good activity with an overpotential of 320 mV at 10 mA cm-2 and a low Tafel slope of 59.6 mV dec-1, outperforming many congeneric electrocatalysts. Overall, our study not only provides important insights to understand the formation mechanism of hierarchical oxyhydroxides, but also opens up new opportunities for the preparation of hierarchical oxyhydroxides via a facile, green and low-cost method. (c) 2022 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.
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