Novel A–D–A Type Naphthalenediimide Supramolecule for H2O2 Photosynthesis with Solar-to-Chemical Conversion 1.03%,Advanced Energy Materials

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Novel A–D–A Type Naphthalenediimide Supramolecule for H2O2 Photosynthesis with Solar-to-Chemical Conversion 1.03%
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2024-05-17 , DOI: 10.1002/aenm.202401437
Rong Ji ₁ , Yuming Dong ₁ , Xinyu Sun ₁ , Pengken Li ₁ , Renbao Zhang ₁ , Chengsi Pan ₁ , Hui Zhao ₁ , Yongfa Zhu ₂

Affiliation

Organic supermolecules have shown great promise for photocatalytic hydrogen peroxide (H₂O₂) production. However, the limitation of intramolecular charge separation efficiency is still a crucial scientific problem. In this study, a novel acceptor–donor–acceptor (A–D–A) type naphthalenediimide supramolecule (SA-NDI) is successfully designed for overcoming fundamental issues in organic supermolecule. Composed of one electron-rich core (naphthalenediimide) and two electron-poor units (aminopyridine), the supramolecule possesses strong intramolecular charge transfer ability. Meanwhile, the SA-NDI has an obviously stronger internal electric field, which is 2.83 times higher than that of D–A type supramolecule. The A–D–A type SA-NDI efficiently accelerates charge separation, so that the intramolecular electron quickly migrates to the acceptor for a two-electron oxygen reduction reaction. The SA-NDI supramolecule shows excellent H₂O₂ accumulation ability (13.7 mm) and stable cyclic time above 120 h. Meanwhile, the catalyst exhibits a superior solar-to-chemical conversion efficiency of 1.03% under simulated solar irradiation. This work provides an entirely new idea to design an organic supramolecule with an efficient intramolecular charge transfer monomer.

中文翻译：

新型 A–D–A 型萘二亚胺超分子用于 H2O2 光合作用，太阳能转化为化学物质的转化率为 1.03%

有机超分子在光催化过氧化氢（H ₂ O ₂ ）生产方面显示出巨大的前景。然而，分子内电荷分离效率的限制仍然是一个至关重要的科学问题。在这项研究中，成功设计了一种新型受体-供体-受体（A-D-A）型萘二亚胺超分子（SA-NDI），用于克服有机超分子的基本问题。该超分子由一个富电子核（萘二亚胺）和两个缺电子单元（氨基吡啶）组成，具有很强的分子内电荷转移能力。同时，SA-NDI具有明显更强的内电场，是D-A型超分子的2.83倍。 A-D-A型SA-NDI有效加速电荷分离，使分子内电子快速迁移到受体进行双电子氧还原反应。 SA-NDI超分子表现出优异的H ₂ O ₂积累能力(13.7 m m )和稳定的循环时间超过120 h。同时，该催化剂在模拟太阳辐照下表现出优异的太阳能化学转化效率，达到1.03%。这项工作为设计具有高效分子内电荷转移单体的有机超分子提供了全新的思路。

更新日期：2024-05-17

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