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486 results on '"Liu, Tian‐Fu"'

17. A solution processible single-crystal porous organic polymer

Author

Liu, Bai-Tong, primary, Gong, Sheng-Hao, additional, Jiang, Xiao-Tian, additional, Zhang, Yuan, additional, Wang, Rui, additional, Chen, Zhijie, additional, Zhang, Shuo, additional, Kirlikovali, Kent O., additional, Liu, Tian-Fu, additional, Farha, Omar K., additional, and Cao, Rong, additional

Published
2023
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18. Efficient CO2 photoreduction enabled by the energy transfer pathway in metal‐organic framework.

Author

Liu, Hai‐Xiong, Si, Duan‐Hui, Smith, Mallory F., Li, Ren‐Fu, Li, Xi‐Ya, Li, Lan, Huang, Hai‐Bo, Fang, Zhi‐Bin, Zhou, Hong‐Cai, and Liu, Tian‐Fu

Subjects
FLUORESCENCE resonance energy transfer, ENERGY transfer, PHOTOCATALYSTS, METAL-organic frameworks, ELECTRON paramagnetic resonance, DOPING agents (Chemistry), REFLECTANCE spectroscopy
Abstract

Many studies in metal‐organic frameworks (MOFs) aiming for high photocatalytic activity resort to self‐assembling both energy donor and acceptor building units in skeleton to achieve effective energy transfer, which, however, usually needs tedious synthetic procedure and design of a new MOF. In this work, we demonstrated that building a Förster resonance energy transfer (FRET) pathway can be realized through suitable molecular doping in a given MOF structure without altering the original porous structure, presenting an alternative strategy to design efficient photocatalysts for CO2 reduction. In situ electron spin resonance, ultrafast transient absorption spectroscopy, and computational studies reveal that the FRET‐induced excitation has dramatically altered the exciton transfer pathway in structure and facilitated electron‐hole separation. As a result, the molecular doped MOFs synthesized through one‐pot reaction show outstanding selectivity (96%) and activity (1314 μmol·g−1·h−1) for CO production versus almost no activity for the pristine MOFs, and this result stands out from existing competitors. Furthermore, the reaction mechanism was proposed and the intermediate signals were detected by in situ diffuse reflectance infrared Fourier transform spectroscopies. This study presents a clear picture of building FRET process in MOFs through molecular doping and provides a new design strategy for MOF‐based photocatalysts. [ABSTRACT FROM AUTHOR]

Published
2023
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41. Tandem Photocatalysis of CO2to C2H4via a Synergistic Rhenium-(I) Bipyridine/Copper-Porphyrinic Triazine Framework

Author

Xu, Rui, Si, Duan-Hui, Zhao, Shao-Shuai, Wu, Qiu-Jin, Wang, Xu-Sheng, Liu, Tian-Fu, Zhao, Hui, Cao, Rong, and Huang, Yuan-Biao

Abstract

The photocatalytic conversion of CO2into C2+products such as ethylene is a promising path toward the carbon neutral goal but remains a big challenge due to the high activation barrier for CO2and similar reduction potentials of many possible multi-electron-transfer products. Herein, an effective tandem photocatalysis strategy has been developed to support conversion of CO2to ethylene by construction of the synergistic dual sites in rhenium-(I) bipyridine fac-[ReI(bpy)(CO)3Cl] (Re-bpy) and copper-porphyrinic triazine framework [PTF(Cu)]. With these two catalysts, a large amount of ethylene can be produced at a rate of 73.2 μmol g–1h–1under visible light irradiation. However, ethylene cannot be obtained from CO2by use of either component of the Re-bpy or PTF(Cu) catalysts alone; with a single catalyst, only monocarbon product CO is produced under similar conditions. In the tandem photocatalytic system, the CO generated at the Re-bpy sites is adsorbed by the nearby Cu single sites in PTF(Cu), and this is followed by a synergistic C–C coupling process which ultimately produces ethylene. Density functional theory calculations demonstrate that the coupling process between PTF(Cu)–*CO and Re-bpy-*CO to form the key intermediate Re-bpy-*CO–*CO-PTF(Cu) is vital to the C2H4production. This work provides a new pathway for the design of efficient photocatalysts for photoconversion of CO2to C2products via a tandem process driven by visible light under mild conditions.

Published
2023
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47. Partial Metalation of Porphyrin Moieties in Hydrogen‐Bonded Organic Frameworks Provides Enhanced CO2 Photoreduction Activity.

Author

Zhang, An‐An, Si, Duanhui, Huang, Haibo, Xie, Lei, Fang, Zhi‐Bin, Liu, Tian‐Fu, and Cao, Rong

Subjects
METALATION, PORPHYRINS, MOIETIES (Chemistry), PHOTOREDUCTION, CATALYTIC activity, HETEROGENEOUS catalysts
Abstract

In natural photosynthesis, the architecture of multiproteins integrates more chromophores than redox centers and simultaneously creates a well‐controlled environment around the active site. Herein, we demonstrate that these features can be emulated in a prototype hydrogen‐bonded organic framework (HOF) through simply varying the proportion of metalated porphyrin in the structure. Further studies demonstrate that changing the metalloporphyrin content not only realizes a fine tuning of the photosensitizer/catalyst ratio, but also alters the microenvironment surrounding the active site and the charge separation efficiency. As a result, the obtained material achieves the challenging overall CO2 reduction with a high HCOOH production rate (29.8 μmol g−1 h−1, scavenger free), standing out from existing competitors. This work unveils that the degree of metalation is vital to the catalytic activity of the porphryinic framework, presenting as a new strategy to optimize the performance of heterogeneous catalysts. [ABSTRACT FROM AUTHOR]

Published
2022
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