The crystalline linear polyimide with oriented photogenerated electron delivery powering CO2 reduction

Li, Huizhen; Chen, Y. B.; Niu, Qing; Wang, Xiaofeng; Liu, Zheyuan; Bi, Jinhong; Yu, Yan; Li, Liuyi

doi:10.1016/s1872-2067(23)64450-x

Cited by 7 publications

(4 citation statements)

References 37 publications

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“…25 Furthermore, Li et al synthesized a crystalline linear PI using pyromellitic dianhydride and 3,7-diaminodiphenylene sulfone, which can be used for efficient photocatalytic CO 2 reduction due to the directional intramolecular charge transfer driven by the dipole effects of adjacent building units in PI molecules. 26 More encouragingly, we note that crystalline PIs could form non-centrosymmetric crystal structures via rational structural design, and thus developing and constructing organic piezocatalysts with a strong polarized electric field is of great interest.…”

Section: Introductionmentioning

confidence: 85%

Organic piezocatalyst polyimide: molecular structure tailoring and robust built-in electric field

Zhang,

Liu,

et al. 2024

J. Mater. Chem. A

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Section: Introductionmentioning

confidence: 85%

Organic piezocatalyst polyimide: molecular structure tailoring and robust built-in electric field

Zhang,

Liu,

et al. 2024

J. Mater. Chem. A

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“…Currently, advancements have been made in the polyimide synthesis process to enhance the alignment of the polyimide chain and improve its crystallinity. These factors lead to anisotropic transport of photogenerated charges and an accelerated rate of combination of electron–hole pairs . Recent reports have conducted research on crystalline polyimide, focusing on the design and synthesis of polyimide with regular structure, oxygen vacancies (OVs), and the regulation of aggregated structure .…”

Section: Introductionmentioning

confidence: 99%

“…These factors lead to anisotropic transport of photogenerated charges and an accelerated rate of combination of electron−hole pairs. 27 Recent reports have conducted research on crystalline polyimide, focusing on the design and synthesis of polyimide with regular structure, oxygen vacancies (OVs), and the regulation of aggregated structure. 28 Therefore, self-assembly through dynamic chemical bonds has been applied to the synthesis of highly active polymeric photocatalytic materials to achieve the purpose of regulating the aggregate structure and π−π stacking, effectively solving the above problems.…”

Section: Introductionmentioning

confidence: 99%

Modulation of the Perylene Polyimide Crystalline Structure and Oxygen Vacancy Contents for Enhanced Photocatalytic Performance

Fan,

Liu,

et al. 2024

Ind. Eng. Chem. Res.

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Perylene polyimide networks are currently one of the most promising metal-free photocatalysts due to their excellent electrical and optical tunability. However, the disordered aggregation state structure in perylene polyimide resulting from the traditional imidization process is detrimental to the separation and migration of the photogenerated charges, which in turn greatly hampers its photocatalytic activity. Herein, we report a facile approach to construct highly crystalline (∼98%) perylene polyimide photocatalysts via cascade reactions involving the assembly of perylenetetracarboxylic acid-melamine monomer salt crystals (PTA-MA), followed by solid-state imidization of the PTA-MA monomer salt. Meanwhile, oxygen vacancies (OVs) were introduced during the polycondensation of the PTA-MA monomer salts. By adjusting the polycondensation temperature, perylene polyimide photocatalysts (PTA-MA-Tn) with varying crystallinity and contents of OVs were obtained. Benefiting from its highly ordered structure and optimized OVs content, the as-prepared perylene polyimide photocatalyst (PTA-MA-200) obtains a suitable crystal structure and excellent photon-to-electron conversion efficiency and exhibits exceptional photoactivity in the photocatalytic valorization of benzylamines into imines. An approximately 10fold increase in the rate of benzylamine photocatalytic conversion was observed in comparison to PTA. This study paves the way for the development of highly crystalline polyimide photocatalysts and has the potential to enhance the understanding of the structure− activity correlation in the context of applying perylene polyimide photocatalysts in practical scenarios.

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“…Two-dimensional covalent organic frameworks (COFs) − have attracted much attention for photocatalysis owing to their merits including well-customizable structures, periodic and permanent porosity, visible light harvesting capability, and π-conjugated backbone for charge carriers migration. − However, most reported COFs for water splitting suffer from the drawbacks of the strong exciton binding energy originating from the organic semiconductor nature, which could cause the rapid recombination of electrons and holes . They typically require sacrificed electron or hole reactants to maximize the half-reaction for H 2 or O 2 production. − A few successful implementations of COFs realized overall water splitting but were limited by the low charge separation efficiency. − The rational design of COF-based photocatalysts to integrate the two half-reactions of water splitting is an urgent issue …”

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confidence: 99%

Spatially Separated Photoredox in a Covalent Organic Frameworks Heterostructure Boosting Overall Water Splitting

Niu,

Chen,

Pan

et al. 2024

ACS Materials Lett.

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Covalent organic frameworks (COFs) with excellent structural tunability have emerged as fascinating photocatalysts to fulfill future energy demands. Here, we developed a COFs heterostructure by assembling two COFs for photocatalytic overall water splitting. The resulting heterostructure exhibited an effective spatial separation of photoredox sites originating from the efficient separation of photoinduced charge carriers through an orientated interfacial electron transfer pathway. Accordingly, the heterostructure of the COFs displays excellent activity for stoichiometric water splitting into H 2 and O 2 under 5 W white LED light irradiation. Our efficiencies of H 2 and O 2 evolution rates up to 120 and 58 μmol g −1 h −1 are significantly higher than those reported previously. The combination of experiments and theoretical calculations shows that water oxidation proceeds by a metal-free hydrationmediated pathway. This work sheds light on a rational design of the COF heterostructure with spatially separated photoredox for water splitting.

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The crystalline linear polyimide with oriented photogenerated electron delivery powering CO2 reduction

Cited by 7 publications

References 37 publications

Organic piezocatalyst polyimide: molecular structure tailoring and robust built-in electric field

Organic piezocatalyst polyimide: molecular structure tailoring and robust built-in electric field

Modulation of the Perylene Polyimide Crystalline Structure and Oxygen Vacancy Contents for Enhanced Photocatalytic Performance

Spatially Separated Photoredox in a Covalent Organic Frameworks Heterostructure Boosting Overall Water Splitting

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