RESUMEN
High-quality MAPbX3(X= I, Br, Cl) single crystals with a desirable size were grown through an inverse temperature crystallization method. Systematically measurements of current-voltage (I-V) hysteresis show that the hysteresis is strongly dependent on the measuring protocol, including scan rate and light illumination condition, which reveals the competition of three main factors that influence the charge dynamics in different regimes, defect trap, MA+dipoles rotation, and ion migration. In the dark, defect trapping is the dominant charge transport dynamics at low bias in the MAPbI3, while the MA+dipole rotation is significant in MAPbBr3, and ion migration occurs in MAPbCl3. However, as bias increases, MA+dipole rotation plays a crucial role in the conductivity either in the dark or under light illumination. The time-dependent photoresponse exhibits different tendencies under various biases. The slow rising dynamics of photoresponse in MAPbX3is attributed to the slow rotation of MA+dipoles, while an immediate overshoot followed by a decay suggests significant ion migration contribution at high external bias. The results serve as comprehensive experimental support to understand the hysteresis behaviors and slow photoresponse in MAPbX3, particularly in MAPbCl3, and provide a guide for future work in MAPbX3based optoelectronic devices.
RESUMEN
Silver phosphate (Ag3PO4, APO) has attracted intense attention as a visible-light-driven photocatalyst, but its large-scale application is limited by severe charge recombination and inevitable photo-corrosion. Various rational APO-based heterostructures composed of APO nanoparticles (NPs) and band-matched semiconductor support are designed to address the above issues. Nevertheless, the size, density, stability, and dispersion of APO NPs are critical challenges for the photocatalytic performance of APO-based photocatalysts. Here, three-dimensional (3D) self-assembled TiO2 hierarchical spheres (THS) prepared by a simple one-step hydrothermal method are employed as innovative support, and ultrafine high-density APO NPs with an average size of about 3 nm are successfully deposited and uniformly dispersed throughout THS to form hierarchical THS/APO composites. The novel THS/APO microstructure provides abundant reactive sites for photocatalytic reactions and promotes the photogenerated charge separation and transfer due to the ultrafine size of APO NPs and the TiO2/APO Type-II heterojunction. As a result, the THS/APO composites show significant improvement in photocatalytic activity and stability in methylene blue (MB) degradation. The reaction constant of THS/APO composites far exceeds that of either THS or APO, roughly 16 and 7 times higher than that of THS and APO under full-spectrum light, and 41 and 4 times higher under visible light. Our results strongly suggest new insights into the low-cost, large-scale application of high-efficiency APO-based photocatalyst.
RESUMEN
The inorganic metal oxides (IMOs), including titanium dioxide (TiO2) and tin dioxide (SnO2), inevitably induce decomposition of perovskite under UV illumination owing to their photocatalytic activity, and the use of a UV filter will add extra cost and reduce the effective power output. Here, we first reveal that the weak Pb-I bond in I-based perovskite is prone to breakage under UV photocatalysis, leading to serious degradation of the SnO2/perovskite interface. We introduced a chlorine-rich mixed-halide perovskite interlayer (ClMPI), which possesses an excellent tolerance to photocatalysis owing to the strong Pb-Cl bond, between the SnO2 and I-based perovskite. The ClMPI-based device achieves an enhanced efficiency of up to 21.01% (certified 20.17%). Most importantly, the resultant devices can maintain >94% of their initial performance after 180 h under outdoor solar irradiation, >80% after 500 h under UV irradiation, and 500 h under continuous full spectrum illumination at their maximum power points.