Metal-Modified Zr-MOFs with AIE Ligands for Boosting CO2 Adsorption and Photoreduction

Bolun Wang, Wen Li, Junmin Liu, Tao Gan, Shiqin Gao, Lin Li, Tianjun Zhang, Yida Zhou, Zhaohui Shi, Jiyang Li*, Yunling Liu*, Jihong Yu*

*此作品的通讯作者

科研成果: 期刊稿件文章同行评审

摘要

The design and synthesis of metal–organic frameworks (MOFs) with outstanding light-harvesting and photoexcitation for artificial photocatalytic CO2 reduction is an attractive but challenging task. In this work, a novel aggregation-induced emission (AIE)-active ligand, tetraphenylpyrazine (PTTBPC) is proposed and utilized for the first time to construct a Zr-MOF photocatalyst via coordination with stable Zr-oxo clusters. Zr-MOF is featured by a scu topology with a two-fold interpenetrated framework, wherein the PTTBPC ligands enable strong light-harvesting and photoexcitation, while the Zr-oxo clusters facilitate CO2 adsorption and activation, as well as offer potential sites for further metal modification. Consequently, the Zr-PTTBPC and its Co/Ni derivatives not only exhibit exceptional stability and high CO2 adsorption capability (73 cm3 g−1 at 273 K and 1 atm), but also demonstrate a CO production rate of up to 293.2 µmol g h−1 under 420 nm LED light that can be reused for at least three cycles. With insights from charge-carrier dynamics and theoretical calculations, the underlying mechanism is revealed, confirming that the single-phase multi-component synergy is the key for the outstanding photocatalytic CO2 reduction. This work showcases a brand-new type of MOF photocatalyst based on AIE ligands and their promising applications in photocatalytic C1 conversion.

源语言英语
期刊Advanced Materials
DOI
出版状态已接受/待刊 - 2025
已对外发布

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Wang, B., Li, W., Liu, J., Gan, T., Gao, S., Li, L., Zhang, T., Zhou, Y., Shi, Z., Li, J., Liu, Y., & Yu, J. (已接受/印刷中). Metal-Modified Zr-MOFs with AIE Ligands for Boosting CO2 Adsorption and Photoreduction. Advanced Materials. https://doi.org/10.1002/adma.202407154