吡嗪功能化的供体-受体共价有机框架，用于增强具有高质子传输的光催化 H2 演化,Small

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吡嗪功能化的供体-受体共价有机框架，用于增强具有高质子传输的光催化 H2 演化
Small ( IF 13.0 ) Pub Date : 2023-03-08 , DOI: 10.1002/smll.202207421
Feng-Dong Wang ₁ , Li-Juan Yang ₁ , Xin-Xin Wang ₁ , Yi Rong ₁ , Li-Bin Yang ₁ , Chen-Xi Zhang _{1,

2} , Fang-You Yan ₁ , Qing-Lun Wang ₃

Affiliation

共价有机框架（COFs）明确的2D或3D结构使其在光电转换和离子传导领域具有巨大的潜力。在此，一种新的供体-受体 (D-A) COF 材料，命名为 PyPz-COF，由电子供体 4,4',4″,4'″-(pyrene-1,3,6,8-tetrayl)tetraaniline 构成据报道，电子受体 4,4'-(pyrazine-2,5-diyl)dibenzaldehyde 具有有序且稳定的 π- 共轭结构。有趣的是，吡嗪环的引入赋予了PyPz-COF独特的光学、电化学、电荷转移特性，同时也带来了丰富的CN基团，通过氢键富集质子，提高了光催化性能。因此，PyPz-COF 表现出显着改善的光催化产氢性能，高达 7542 µmol g ⁻¹ h ⁻¹^{以 Pt 作为助催化剂，也与没有引入吡嗪的 PyTp-COF (1714 µmol g −1} h ⁻¹ )形成鲜明对比。此外，吡嗪环上丰富的氮位点和明确定义的一维纳米通道使所制备的 COF 能够通过氢键限制将 H ₃ PO ₄质子载体固定在 COF 中。所得材料在 353 K、98% RH 下具有高达 8.10 × 10 ⁻² S cm ^{−1的令人印象深刻的质子传导。}这项工作将激发未来具有高效光催化和质子传导性能的 COF 基材料的设计和合成。

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Pyrazine-Functionalized Donor–Acceptor Covalent Organic Frameworks for Enhanced Photocatalytic H2 Evolution with High Proton Transport

The well-defined 2D or 3D structure of covalent organic frameworks (COFs) makes it have great potential in photoelectric conversion and ions conduction fields. Herein, a new donor–accepter (D–A) COF material, named PyPz-COF, constructed from electron donor 4,4′,4″,4′″-(pyrene-1,3,6,8-tetrayl)tetraaniline and electron accepter 4,4′-(pyrazine-2,5-diyl)dibenzaldehyde with an ordered and stable π-conjugated structure is reported. Interestingly, the introduction of pyrazine ring endows the PyPz-COF a distinct optical, electrochemical, charge-transfer properties, and also brings plentiful CN groups that enrich the proton by hydrogen bonds to enhance the photocatalysis performance. Thus, PyPz-COF exhibits a significantly improved photocatalytic hydrogen generation performance up to 7542 µmol g⁻¹ h⁻¹ with Pt as cocatalyst, also in clear contrast to that of PyTp-COF without pyrazine introduction (1714 µmol g⁻¹ h⁻¹). Moreover, the abundant nitrogen sites of the pyrazine ring and the well-defined 1D nanochannels enable the as-prepared COFs to immobilize H₃PO₄ proton carriers in COFs through hydrogen bond confinement. The resulting material has an impressive proton conduction up to 8.10 × 10⁻² S cm⁻¹ at 353 K, 98% RH. This work will inspire the design and synthesis of COF-based materials with both efficient photocatalysis and proton conduction performance in the future.

更新日期：2023-03-08

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