Structural Stability of Mixed-Halide Perovskite Nanocrystals in Energy Storage: The Role of Iodine Expulsion

Abstract

In the pursuit of efficient optoelectronics devices, hybrid lead halide perovskite quantum dots (PQDs) have emerged as highly promising semiconductor materials due to their intriguing properties. While these materials have been used in many applications, the fundamental understanding of their behavior remains relatively unexplored, especially for the mixed halide perovskite samples. To facilitate the advancement of PQD technologies for commercial applications, it is essential to gain insights into the role of ion migration. This study delves into the fundamental aspects of ion migration in halide perovskite nanocrystals. Porous electrodes for supercapacitor application were fabricated using CsPbBr_3–xI_x (x=0,1,2) nanocrystals prepared via the ligand-assisted re-precipitation (LARP) method. Three-electrode electrochemical measurements and several other characterizations were conducted under dark conditions to evaluate device performance and elucidate the impact of mixed halides on device kinetics and stability. X-ray photoelectron spectroscopy before and after the electrochemical measurement reveals intriguing findings. Notably, the analysis uncovered the phase segregation in the metal halide perovskite nanocrystals with particular emphasis on CsPbBr₂I due to its distinctive mixed-halide behavior. The specific capacitance increases with the increasing cycles. Interestingly, as the iodide content increases, there is no selective halide expulsion as the structure collapses rapidly.