Tailoring the Nanoporosity and Photoactivity of Metal-Organic Frameworks With Rigid Dye Modulators for Toluene Purification.

Facile synthesis of hierarchically porous metal-organic frameworks (MOFs) with adjustable porosity and high crystallinity attracts great attention yet remains challenging. Herein, a micromolar amount of dye-based modulator (Rhodamine B (RhB)) is employed to easily and controllably tailor the pore size of a Ti-based metal-organic framework (MIL-125-NH2 ). The RhB used in this method is easily removed by washing or photodegradation, avoiding secondary posttreatment. It is demonstrated that the carboxyl functional group and the steric effects of RhB are indispensable for enlarging the pore size of the MIL-125-NH2 . The resulting hierarchically porous MIL-125-NH2 (RH-MIL-125-NH2 ) exhibits optimized adsorption and photocatalytic activity because the newly formed mesopore with defects concurrently facilitates mass transport of guest molecules (toluene) and photogenerated charge separation. This work offers a meaningful basis for the construction of hierarchically porous MOFs and demonstrates the superiority of the hierarchical pore structure for adsorption and heterogeneous catalysis.

High-Valent Iodoplumbate-Rich Perovskite Precursor Solution via Solar Illumination for Reproducible Power Conversion Efficiency.

The power conversion efficiency (PCE) of solution-processed organic-inorganic hybrid perovskite solar cells has been drastically improved. Despite this considerable progress, systematic research on precursor solution chemistry and its effects on photovoltaic parameters has been limited thus far. Herein, we report on the tracking of changes in chemical species in a precursor solution under solar illumination and investigate the correlation between the equilibrium change and the corresponding perovskite film formation. The illuminated perovskite precursors display a higher density of high-valent iodoplumbate, where the resulting perovskite film exhibits reduced defect density with uniform film formation. Conclusively, the perovskite solar cells prepared by the photoaged precursor solution demonstrate not only improved average PCE but also enhanced reproducibility with a narrow PCE distribution. This discovery shows robust control of perovskite precursor solutions from a simple treatment and suggests that the resulting uniform film may be applicable to various halide perovskite-based devices.

Band Alignment Engineering between Planar SnO2 and Halide Perovskites via Two-Step Annealing.

Managing defects in SnO2 is critical for improving the power conversion efficiency (PCE) of halide perovskite-based solar cells. However, typically reported SnO2-based perovskite solar cells have inherent defects in the SnO2 layer, which lead to a lower PCE and hysteresis. Here, we report that a dual-coating approach for SnO2 with different annealing temperatures can simultaneously form a SnO2 layer with high crystallinity and uniform surface coverage. Along with these enhanced physical properties, the dual-coated SnO2 layer shows favorable band alignment with a mixed halide perovskite. After careful optimization of the dual-coating method, the average PCE of the perovskite solar cell based on the dual-coated SnO2 layer increases from 18.07 to 19.23% with a best-performing cell of 20.03%. Note that a facile two-step coating and annealing method can open new avenues to develop SnO2-based perovskite solar cells with stabilized and improved photovoltaic performances.