Abstract

With the wide application of supercapacitors, it has been recognized that the drop of energy storage capacity due to cold environmental temperatures limits their utilization efficiency. In this study, a binder-free Ni/Co-layered double hydroxide (LDH)-based high-performance energy storage device is constructed on Ni foam by in situ electrochemically triggered MOF hydrolysis, which exhibits a remarkably enhanced capacity under solar irradiation. Through electrochemically controlled hydrolysis, the ligands in MOFs are replaced by OH–, and the obtained NiCo-LDH retains the original hierarchical porous structure of the MOFs. Benefitting from the sufficient oxygen vacancies and large surface area, the NiCo-LDH electrode shows a high capacity of 5.4 C cm–2 at 1.25 mA cm–2, which is 64.3 times higher than that of the MOF template. Importantly, the excellent photothermal conversion ability (temperature increase of 52.9 °C within only 30 s) under solar irradiation increases the capacity to 226.0% even at sub-freezing temperature. Furthermore, the asymmetric supercapacitor fabricated using NiCo-LDH delivers an energy density increase of 329.2% in a low-temperature environment (−4 °C) after 15 min solar-light irradiation.

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