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Bromo- and iodo-bridged building units in metal-organic frameworks for enhanced carrier transport and CO2 photoreduction by water vapor
Nature Communications ( IF 14.7 ) Pub Date : 2022-08-06 , DOI: 10.1038/s41467-022-32367-0
Xinfeng Chen 1 , Chengdong Peng 1 , Wenyan Dan 1 , Long Yu 1 , Yinan Wu 2, 3 , Honghan Fei 1
Affiliation  

Organolead halide hybrids have many promising attributes for photocatalysis, e.g. tunable bandgaps and excellent carrier transport, but their instability constraints render them vulnerable to polar molecules and limit their photocatalysis in moisture. Herein, we report the construction of metal–organic frameworks based on [Pb2X]3+ (X = Br–/I–) chains as secondary building units and 2-amino-terephthalate as organic linkers, and extend their applications in photocatalytic CO2 reduction with water vapor as the reductant. Hall effect measurement and ultrafast transient absorption spectroscopy demonstrate the bromo/iodo-bridged frameworks have substantially enhanced photocarrier transport, which results in photocatalytic performances superior to conventional metal-oxo metal-organic frameworks. Moreover, in contrast to lead perovskites, the [Pb2X]3+-based frameworks have accessible porosity and high moisture stability for gas-phase photocatalytic reaction between CO2 and H2O. This work significantly advances the excellent carrier transport of lead perovskites into the field of metal-organic frameworks.



中文翻译:


金属有机框架中的溴桥和碘桥结构单元,用于增强载流子传输和水蒸气的二氧化碳光还原



有机铅卤化物杂化物具有许多有前景的光催化特性,例如。可调的带隙和出色的载流子传输,但它们的不稳定性限制使它们容易受到极性分子的影响,并限制了它们在潮湿环境中的光催化作用。在此,我们报道了基于[Pb 2 X] 3+ (X = Br–/I–)链作为二级结构单元和2-氨基对苯二甲酸酯作为有机连接体的金属有机框架的构建,并扩展了它们在光催化中的应用以水蒸气为还原剂进行CO 2还原。霍尔效应测量和超快瞬态吸收光谱表明,溴/碘桥联骨架显着增强了光载流子传输,从而导致光催化性能优于传统的金属-氧金属-有机骨架。此外,与铅钙钛矿相比,[Pb 2 X] 3+基框架具有良好的孔隙率和高湿度稳定性,适用于 CO 2和 H 2 O 之间的气相光催化反应。这项工作显着提高了铅的优异载流子传输性能钙钛矿进入金属有机框架领域。

更新日期:2022-08-06
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