Revealing energy storage mechanism of CsPbBr₃ perovskite for ultra-stable symmetric supercapacitors

Abstract

Inorganic metal halide perovskites such as CsPbX₃ (X = I, Br) have been intensively studied in optoelectrical applications such as solar cells and light-emitting diodes due to better thermal and structural stability compared to the organic-inorganic hybrid perovskite counterparts. Limited studies have shown that inorganic perovskites could potentially be promising electrode materials in energy storage devices like supercapacitors. Nevertheless, there is some controversy regarding their electrochemical properties and energy storage mechanism. Furthermore, the stability of the inorganic perovskites in electrochemical energy storage systems is a big concern. In this work, we studied the electrochemical properties of CsPbBr₃ electrodes composed of pure CsPbBr₃ nanocrystals without any additives to reveal their intrinsic electrochemical characteristics. We carefully selected the electrolyte solution composed of tetrabutylammonium hexafluorophosphate in dichloromethane and the electrode substrate based on FTO glass to ensure they do not cause damage to the perovskite material or introduce side reactions during the charge-discharge process. The results showed that the CsPbBr₃ perovskite demonstrates electrical double-layer capacitive behaviour, and the specific capacitance of the electrode can reach 528 mF g^-1. A symmetrical supercapacitor based on this perovskite demonstrated exceptional cycling stability with a capacitance retention of 90% after 10,000 charge and discharge cycles at a discharge current density of 100 mA g^-1. The device also exhibited a constant power density of 25.0 mW kg^-1 with increasing energy density up to 33.3 mWh kg^-1. Further characterizations have revealed the important role of the large cations and anions of tetrabutylammonium hexafluorophosphate in the electrolyte in stabilizing the perovskite electrode material.

Keywords

CsPbBr₃ perovskite nanocrystals / energy storage mechanism / supercapacitors / stability / long cycling lifetime

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