Photosensitizing metal covalent organic framework with fast charge transfer dynamics for efficient CO<sub>2</sub> photoreduction

Han, Wang-Kang; Li, Jiayu; Zhu, Ruo-Meng; Wei, Min; Xia, Shu-Kun; Fu, Jia-Xing; Zhang, Jinfang; Pang, Huan; Li, Ming-De; Gu, Zhi-Guo

doi:10.1039/d4sc01896f

Chem. Sci.

2024

DOI: 10.1039/d4sc01896f

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Photosensitizing metal covalent organic framework with fast charge transfer dynamics for efficient CO₂ photoreduction

Wang-Kang Han,

Jiayu Li,

Ruo-Meng Zhu

et al.

Abstract: Designing artificial photocatalysts for CO2 reduction is challenging, mainly due to the intrinsic difficulty for multiple functional units to cooperate efficiently. Here, three-dimensional metal covalent organic frameworks (3D MCOFs) were...

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Reticular Materials for Photocatalysis

Sun,

Qian,

et al. 2024

Advanced Materials

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Photocatalysis leverages solar energy to overcome the thermodynamic barrier, enabling efficient chemical reactions under mild conditions. It can greatly reduce reliance on traditional energy sources and has attracted significant research interest. Reticular materials, including metal‐organic frameworks (MOFs) and covalent organic frameworks (COFs), represent a class of crystalline materials constructed from molecular building blocks linked by coordination and covalent bonds, respectively. Reticular materials function as heterogeneous catalysts, combining well‐defined structures and high tailorability akin to homogeneous catalysts. In this review, the regulation of light absorption, charge separation, and surface reactions in the photocatalytic process through precise molecular‐level design based on the features of reticular materials is elaborated. Notably, for MOFsmicroenvironment modulation around catalytic sites affects photocatalytic performance is delved, with emphasis on their unique dynamic and flexible microenvironments. For COFs, the inherent excitonic effects due to their fully organic nature is discussed and highlight the strategies to regulate excitonic effects for charge‐ and/or energy‐transfer‐mediated photocatalysis. Finally, the current challenges and future directions in this field, aiming to provide a comprehensive understanding of how reticular materials can be optimized for enhanced photocatalysis is discussed.

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Reticular Materials for Photocatalysis

Sun,

Qian,

et al. 2024

Advanced Materials

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General Synthesis of Single‐Crystalline Ta₂O₅ Nanorods Towards Enhanced Photocatalytic H₂ Production Activity

Zhang,

Zhou,

Shi

et al. 2024

ChemPhysChem

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As a potential candidate for photocatalytic H2 production from water splitting, Ta2O5 catalyst presents suitable conduction and valence band positions, but suffers from poor charge transfer ability, which seriously limits its photocatalytic performance enhancement. Here, a facile and eco‐friendly hydrothermal method was developed for the fabrication of one‐dimensional (1D) Ta2O5 nanorods using the freshly precipitated tantalic acids as the precursors. An oriented attachment mechanism was proposed for the growth of Ta2O5 nanorods. Moreover, the present synthetic approach was further extended to direct synthesis of nine kinds of alkaline tantalates and alkaline‐earth tantalates nanostructures, suggesting its general applicability. A significant increase in activity in photocatalytic H2 production was revealed on 1D Ta2O5 nanorods. The improved photocatalytic H2 production activity of Ta2O5 nanorods was mainly attributed to its 1D nanorods structure with high crystallization and large specific surface areas as well as excellent charge transfer efficiency.

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The Structural Regulation of Photosensitive Unit and Conjugation in COFs for Efficient Photocatalytic H₂ Evolution

Zhang,

Ma,

Yang

et al. 2024

ChemSusChem

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The photosensitive unit and conjugation play a significant role in photocatalytic performance of covalent organic frameworks (COFs). In this work, a series of COFs that introduced the phenyl phenanthridine as photosensitive unit with different planarity of linkages were synthesized and the common regulation between them for photocatalysis hydrogen evolution reaction (HER) was also studied. The results indicate that DHTB‐PPD, with 2/3 planarity linkages (β‐ketoenamine/imine is 2/3) and the phenyl phenanthridine as building blocks, shows the narrowest bandgap and the strongest charge separation efficiency. Therefore, it shows the highest H2 production rate of 12.13 mmol g‐1 h‐1. The optimal photocatalytic efficiency of DTHB‐PPD can be attributed to the combined effect of the photosensitive unit and the long‐range ordering of the COF skeleton. According to The Density Functional Theory (DFT), the O site on β‐ketoamine is the most possible H2 generation site, but the photocatalytic efficiency of TP‐PPD, with the highest skeletal conjugation and the highest proportion of β‐ketoamine is not the most efficient photocatalyst, indicating that the long‐range ordering of COFs is important on photocatalytic performance. Thus, these findings provide valuable guidance for the structural design of COFs photocatalysts.

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Photosensitizing metal covalent organic framework with fast charge transfer dynamics for efficient CO₂ photoreduction

Abstract: Designing artificial photocatalysts for CO2 reduction is challenging, mainly due to the intrinsic difficulty for multiple functional units to cooperate efficiently. Here, three-dimensional metal covalent organic frameworks (3D MCOFs) were...

Cited by 3 publications

References 45 publications

Reticular Materials for Photocatalysis

Reticular Materials for Photocatalysis

General Synthesis of Single‐Crystalline Ta₂O₅ Nanorods Towards Enhanced Photocatalytic H₂ Production Activity

The Structural Regulation of Photosensitive Unit and Conjugation in COFs for Efficient Photocatalytic H₂ Evolution

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Photosensitizing metal covalent organic framework with fast charge transfer dynamics for efficient CO2 photoreduction

Abstract: Designing artificial photocatalysts for CO2 reduction is challenging, mainly due to the intrinsic difficulty for multiple functional units to cooperate efficiently. Here, three-dimensional metal covalent organic frameworks (3D MCOFs) were...

Cited by 3 publications

References 45 publications

Reticular Materials for Photocatalysis

Reticular Materials for Photocatalysis

General Synthesis of Single‐Crystalline Ta2O5 Nanorods Towards Enhanced Photocatalytic H2 Production Activity

The Structural Regulation of Photosensitive Unit and Conjugation in COFs for Efficient Photocatalytic H2 Evolution

Contact Info

Product

Resources

About

Photosensitizing metal covalent organic framework with fast charge transfer dynamics for efficient CO₂ photoreduction

General Synthesis of Single‐Crystalline Ta₂O₅ Nanorods Towards Enhanced Photocatalytic H₂ Production Activity

The Structural Regulation of Photosensitive Unit and Conjugation in COFs for Efficient Photocatalytic H₂ Evolution