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Methylammonium‐mediated phase‐evolution behavior of FA1−xMAxPbI3 mixed‐organic‐cation perovskite (MOCP) is studied. It is found that by simply enriching the MOCP precursor solutions with excess methylammonium cations, the MOCPs form via a dynamic composition‐tuning process that is key to obtaining MOCP thin films with superior properties. This simple chemical approach addresses several key challenges, such as control over phase purity, uniformity, grain size, composition, etc., associated with the solution‐growth of MOCP thin films with targeted compositions.  相似文献   

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Tin‐based halide perovskite materials have been successfully employed in lead‐free perovskite solar cells, but the overall power conversion efficiencies (PCEs) have been limited by the high carrier concentration from the facile oxidation of Sn2+ to Sn4+. Now a chemical route is developed for fabrication of high‐quality methylammonium tin iodide perovskite (MASnI3) films: hydrazinium tin iodide (HASnI3) perovskite film is first solution‐deposited using presursors hydrazinium iodide (HAI) and tin iodide (SnI2), and then transformed into MASnI3 via a cation displacement approach. With the two‐step process, a dense and uniform MASnI3 film is obtained with large grain sizes and high crystallization. Detrimental oxidation is suppressed by the hydrazine released from the film during the transformation. With the MASnI3 as light harvester, mesoporous perovskite solar cells were prepared, and a maximum power conversion efficiency (PCE) of 7.13 % is delivered with good reproducibility.  相似文献   

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Conjugated microporous polymers are a unique class of polymers that combine extended π‐conjugation with inherent porosity. However, these polymers are synthesized through solution‐phase reactions to yield insoluble and unprocessable solids, which preclude not only the evaluation of their conducting properties but also the fabrication of thin films for device implementation. Here, we report a strategy for the synthesis of thin films of π‐conjugated microporous polymers by designing thiophene‐based electropolymerization at the solution–electrode interface. High‐quality films are prepared on a large area of various electrodes, the film thickness is controllable, and the films are used for device fabrication. These films are outstanding hole conductors and, upon incorporation of fullerenes into the pores, function as highly efficient photoactive layers for energy conversions. Our film strategy may boost the applications in photocatalysis, energy storage, and optoelectronics.  相似文献   

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The tunable growth of metal–organic materials has implications for engineering particles and surfaces for diverse applications. Specifically, controlling the self‐assembly of metal–phenolic networks (MPNs), an emerging class of metal–organic materials, is challenging, as previous studies suggest that growth often terminates through kinetic trapping. Herein, kinetic strategies were used to temporally and spatially control MPN growth by promoting self‐correction of the coordinating building blocks through oxidation‐mediated MPN assembly. The formation and growth mechanisms were investigated and used to engineer films with microporous structures and continuous gradients. Moreover, reactive oxygen species generated by ultrasonication expedite oxidation and result in faster (ca. 30 times) film growth than that achieved by other MPN assembly methods. This study expands our understanding of metal–phenolic chemistry towards engineering metal–phenolic materials for various applications.  相似文献   

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