Abstract
To understand the underlying mechanism of the interfacial charge transfer and local chemical state variation in the nonprecious-based hydrogen evolution reaction (HER) electrocatalysts, a model system of the NiO/CeO2 heterostructure was chosen for investigation using a combination of the advanced electron microscopic characterization and first-principles calculations. The results directly proved that interfacial charge transfer occurs from Ni to Ce, leading to reduction in the valence state of Ce and increased formation of VO. This would optimize ΔGH* and facilitate the hydrogen evolution process, resulting in outstanding HER performance in 1 M KOH with a low overpotential of 99 mV at the current density of 10 mA•cm−2 and a modest Tafel slope of 78.4 mV•dec−1 for the NiO/CeO2 heterostructure sample. Therefore, the improved HER performance could be attributed to the synergistic coupling interactions and electron redistribution at the interface of NiO and CeO2. These results concretely demonstrate the direct determination of the interfacial structure of the heterostructure and provide atomistic insights to unravel the underlying mechanism of interfacial charge transfer induced HER performance improvement.
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