The mixed caesium and formamidinium lead triiodide perovskite system (Cs1-xFAxPbI3) in the form of quantum dots (QDs) offers a new pathway towards stable perovskite-based photovoltaics and optoelectronics. However, it remains challenging to synthesize such multinary QDs with desirable properties for high-performance QD solar cells (QDSCs). Here we report an effective ligand-assisted cation exchange strategy that enables controllable synthesis of Cs1-xFAxPbI3 QDs across the whole composition range (x: 0-1), which is inaccessible in large-grain polycrystalline thin films. The surface ligands play a key role in driving the cross-exchange of cations for the rapid formation of Cs1-xFAxPbI3 QDs with suppressed defect density. The hero Cs0.5FA0.5PbI3 QDSC achieves a certified record power conversion efficiency (PCE) of 16.6% with negligible hysteresis. We further demonstrate that QD devices exhibit substantially enhanced photostability compared to their thin film counterparts because of the suppressed phase segregation, retaining 94% of the original PCE under continuous 1-sun illumination for 600 hours.
The
limitations of the Haber–Bosch reaction, particularly
high-temperature operation, have ignited new interests in low-temperature
ammonia-synthesis scenarios. Ambient N2 electroreduction
is a compelling alternative but is impeded by a low ammonia production
rate (mostly <10 mmol gcat
–1 h–1), a small partial current density (<1 mA cm–2), and a high-selectivity hydrogen-evolving side reaction.
Herein, we report that room-temperature nitrate electroreduction catalyzed
by strained ruthenium nanoclusters generates ammonia at a higher rate
(5.56 mol gcat
–1 h–1) than the Haber–Bosch process. The primary contributor to
such performance is hydrogen radicals, which are generated by suppressing
hydrogen–hydrogen dimerization during water splitting enabled
by the tensile lattice strains. The radicals expedite nitrate-to-ammonia
conversion by hydrogenating intermediates of the rate-limiting steps
at lower kinetic barriers. The strained nanostructures can maintain
nearly 100% ammonia-evolving selectivity at >120 mA cm–2 current densities for 100 h due to the robust subsurface Ru–O
coordination. These findings highlight the potential of nitrate electroreduction
in real-world, low-temperature ammonia synthesis.
Low cost, high efficiency, and stability are straightforward research challenges in the development of organic-inorganic perovskite solar cells. Organolead halide is unstable at high temperatures or in some solvents. The direct preparation of a carbon layer on top becomes difficult. In this study, we successfully prepared full solution-processed low-cost TiO2/CH3NH3PbI3 heterojunction (HJ) solar cells based on a low-temperature carbon electrode. Power conversion efficiency of mesoporous (M-)TiO2/CH3NH3PbI3/C HJ solar cells based on a low-temperature-processed carbon electrode achieved 9%. The devices of M-TiO2/CH3NH3PbI3/C HJ solar cells without encapsulation exhibited advantageous stability (over 2000 h) in air in the dark. The ability to process low-cost carbon electrodes at low temperature on top of the CH3NH3PbI3 layer without destroying its structure reduces the cost and simplifies the fabrication process of perovskite HJ solar cells. This ability also provides higher flexibility to choose and optimize the device, as well as investigate the underlying active layers.
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