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Cucurbit[8]uril as a supramolecular lock for designing a dual-chain conjugated polymer photocatalyst for enhanced H2O2 production
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2024-08-22 , DOI: 10.1039/d4ta04302b Jie Yin 1 , Si-zhe Li 1 , Hao Zhang 1 , Yao Lu 1 , Yan Zhao 1 , K. A. I. Zhang 1
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2024-08-22 , DOI: 10.1039/d4ta04302b Jie Yin 1 , Si-zhe Li 1 , Hao Zhang 1 , Yao Lu 1 , Yan Zhao 1 , K. A. I. Zhang 1
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Conjugated polymers (CPs) have garnered attention for their tailorable structural properties, particularly in the context of efficient photosynthetic hydrogen peroxide (H2O2) production. However, the challenge lies in the precise molecular engineering of CPs to facilitate different reaction pathways, thereby enhancing the H2O2 photogeneration efficiency. In this study, we developed dual-chain CPs (DC-CPs) with a distinctive architecture, employing the supramolecular host cucurbit[8]uril as a “molecular lock” to conjoin two polymer chains. The dual-chain configuration is designed to harbour a central reaction centre conducive to oxygen reduction, providing dual conduction pathways for reactant molecules. The existence of this central reaction center was confirmed through in situ diffuse reflectance infrared Fourier transform (DRIFT) spectroscopy measurements and density functional theory (DFT) calculations. In addition, femtosecond transient absorption spectroscopy (fs-TAS), variable temperature fluorescence spectroscopy and time-resolved photoluminescence (TRPL) measurements reveal double-stranded structures favourable for carrier transport and reactive site activation between dual polymer chains. Ultimately, DC-CPs demonstrate up to a threefold increase in H2O2 production compared to their respective single-chain CPs (SC-CPs). This work contributes significantly to the application of CPs for efficient H2O2 photogeneration through a molecular engineering strategy.
中文翻译:
葫芦[8]脲作为超分子锁,用于设计双链共轭聚合物光催化剂,以增强 H2O2 的产量
共轭聚合物(CP)因其可定制的结构特性而受到关注,特别是在高效光合过氧化氢(H 2 O 2 )生产的背景下。然而,挑战在于对CP进行精确的分子工程以促进不同的反应途径,从而提高H 2 O 2光生效率。在这项研究中,我们开发了具有独特结构的双链CP(DC-CP),采用超分子主体葫芦[8]脲作为“分子锁”来连接两个聚合物链。双链构型旨在容纳有利于氧还原的中央反应中心,为反应物分子提供双传导途径。通过原位漫反射红外傅里叶变换(DRIFT)光谱测量和密度泛函理论(DFT)计算证实了该中心反应中心的存在。此外,飞秒瞬态吸收光谱(fs-TAS)、变温荧光光谱和时间分辨光致发光(TRPL)测量揭示了有利于载流子传输和双聚合物链之间的反应位点激活的双链结构。最终,与各自的单链 CP (SC-CP) 相比,DC-CP 的 H 2 O 2产量增加了三倍。 这项工作对通过分子工程策略将CP应用于高效H 2 O 2光生成做出了重大贡献。
更新日期:2024-08-22
中文翻译:
![](https://scdn.x-mol.com/jcss/images/paperTranslation.png)
葫芦[8]脲作为超分子锁,用于设计双链共轭聚合物光催化剂,以增强 H2O2 的产量
共轭聚合物(CP)因其可定制的结构特性而受到关注,特别是在高效光合过氧化氢(H 2 O 2 )生产的背景下。然而,挑战在于对CP进行精确的分子工程以促进不同的反应途径,从而提高H 2 O 2光生效率。在这项研究中,我们开发了具有独特结构的双链CP(DC-CP),采用超分子主体葫芦[8]脲作为“分子锁”来连接两个聚合物链。双链构型旨在容纳有利于氧还原的中央反应中心,为反应物分子提供双传导途径。通过原位漫反射红外傅里叶变换(DRIFT)光谱测量和密度泛函理论(DFT)计算证实了该中心反应中心的存在。此外,飞秒瞬态吸收光谱(fs-TAS)、变温荧光光谱和时间分辨光致发光(TRPL)测量揭示了有利于载流子传输和双聚合物链之间的反应位点激活的双链结构。最终,与各自的单链 CP (SC-CP) 相比,DC-CP 的 H 2 O 2产量增加了三倍。 这项工作对通过分子工程策略将CP应用于高效H 2 O 2光生成做出了重大贡献。