Publication date: 11th March 2026
Wide-bandgap perovskite solar cells (PSCs) based on Br-rich and Br/Cl compositions enable the high photovoltages required for tandem photovoltaics, unassisted solar-driven water splitting, and emerging applications such as indoor photovoltaics (IPV) and building-integrated photovoltaics (BIPV). Full-bromide FAPbBr3 represents a benchmark system, combining a large bandgap of 2.28 eV with compositional simplicity and intrinsic halide stability. Extending this class to mixed Br/Cl perovskites allows further bandgap widening but introduces challenges related to crystallization kinetics, optoelectronic losses, and halide redistribution. Across both systems, suppressing nonradiative recombination and interfacial energy losses is essential for high-performance devices.
We first report on full-bromide FAPbBr3 PSCs developed for unassisted photovoltaic-electrochemical (PV-EC) water splitting. To meet the high voltage requirements imposed by thermodynamic and kinetic overpotentials, nonradiative recombination is minimized through dual passivation: formamidinium thiocyanate (FASCN) for bulk passivation and 1,3-propane diammonium iodide (PDAI2) for surface passivation. This promotes larger grain growth, reduces interfacial recombination, and improves charge extraction. Further optimization of the electron-transport layer using a ternary fullerene blend (PCBM:CMC:ICBA) improves energetic alignment and suppresses interfacial losses, increasing open-circuit voltage (VOC) from 1.41 to 1.60 V and yielding a power conversion efficiency of 9.4% in small-area devices. Scaled to a 1.0 cm2 active area and integrated into a PV-EC system with Pt and RuO2 catalysts, the device achieves continuous solar-driven water splitting with a solar-to-hydrogen (STH) efficiency of 6.5%, the highest reported for a single-absorber system.[1]
Starting from full-bromide FAPbBr3, we investigate mixed Br/Cl perovskites with chloride incorporation up to 80%. Structural and optical measurements confirm full chloride incorporation, resulting in lattice contraction and bandgap widening up to 2.85 eV, along with shifts in the valence and conduction band edges and altered film morphology. In situ UV-vis spectroscopy shows that higher chloride content retards crystallization, consistent with stronger Pb–Cl bonding. Mixed Br/Cl perovskites exhibit light-induced halide segregation, with remixing after dark storage. Time-resolved and absolute photoluminescence measurements indicate similar carrier lifetimes, but higher bandgaps yield increased quasi-Fermi level splitting alongside larger nonradiative voltage losses. Focusing on a 20% chloride composition, targeted bulk and surface engineering with small cesium incorporation and F-PEACl passivation effectively suppresses nonradiative recombination, hysteresis, and halide segregation, improving performance and stability. This approach is extended to 40% and 60% chloride devices.
