Understanding the catalysis mechanism of the sluggish oxygen evolution reaction (OER) involved in water splitting is of vital importance for the development of clean hydrogen energy. Earthabundant transition-metal (oxy)hydroxide with low cost and high performance is one of the most promising OER catalysts. These catalysts often dynamically and heterogeneously transform from inactive precatalysts into active phases under operation conditions, and thus, the operando/in situ method is needed for the direct observation. Herein, using in situ Raman spectroscopy and density functional theory simulation, we correlate the OER activity with the dynamic crystal-and electronic-structure reconstruction of nano-sheet cobalt hydroxide. A complicated dual-transformation path is observed as the applied voltage is gradually increased; the pristine single-phase α-Co(OH) 2 catalyst transforms into the hydrous Co(OH) 2 phase through hydroxide intercalation, then to mixed β/γ-CoOOH phases through dehydration and dehydrogenation, and finally to OER-active γ-CoOOH x and β-CoOOH y . Moreover, the observed spectral and Tafel behaviors at different scan rates manifest the rate-dependent formation of the dual-active-phase, demonstrating the correlation between the OER ability and thermodynamics of structural reconstruction, which is critical in the fabrication of high-activity catalysts.
HIGHLIGHTS • A facile strategy for fabricating Ni x Co 1−x Se hollow nanocages was developed, and the formation mechanism was well explained. • Ni 0.2 Co 0.8 Se outperformed a Pt/C + RuO 2 catalyst in rechargeable and all-solid-state Zn-air battery tests, as well as in overall water splitting. • The hydrogen adsorption onto Ni x Co 1−x Se was simulated, and Gibbs free energies were calculated.
A facile strategy is developed to create a MIL-88A/Ni(OH)2 heterostructure, where the interfacial charge transfer significantly boosted the OER performance.
One of the most successful approaches for balancing the high stability and activity of water oxidation in alkaline solutions is to use amorphous and crystalline heterostructures. However, due to the...
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