Ni(OH)2-based materials are widely studied in oxygen evolution reaction (OER), but no related synthesis, electrocatalytic application, or theoretical analysis of Sn4+-doped Ni(OH)2 has been reported. In this work, Sn–Ni(OH)2 with a homogeneously distributed nanosheet array was synthesized through a one-step hydrothermal process. It displays a hugely enhanced catalytic activity compared to undoped Ni(OH)2 throughout the OER and hydrogen evolution reaction (HER) processes. The overpotentials at 100 mA cm–2 of Sn–Ni(OH)2 are 312 mV (OER) and 298 mV (HER), which are lower than the corresponding 396 and 427 mV of Ni(OH)2, respectively. In addition, Sn–Ni(OH)2 can deliver stable large current densities (at ≈500 and ≈1000 mA cm–2) for the long-term (>100 h) chronoamperometry testing. Moreover, Sn–Ni(OH)2 illustrates catalytic activity comparable to that of a commercial Pt/C||RuO2 electrode pair during the overall water splitting course. Both experimental phenomena and relevant computed theoretical data confirm that the enhanced water splitting activity is mainly due to the introduced Sn4+ site, which acts as the active center activates the nearby Ni sites during the OER, while acting as the most active reaction site that participates in the HER. Although the doped Sn4+ has two different effects on OER and HER proceedings, water splitting performance of Sn–Ni(OH)2 has been conspicuously improved.
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