Shao Changxiang, Guo Bingpeng, Lu Bing, Yu Jiahui, Kong Huijun, Wang Baolei, Ding Meichun, Li Chenwei
School of Chemistry & Pharmaceutical Engineering, Medical Science and Technology Innovation Center, Shandong First Medical University & Shandong Academy of Medical Sciences, Jinan, 250117, China.
School of Chemistry and Chemical Engineering, Qilu University of Technology Shandong Academy of Sciences, Jinan, 250103, China.
Small. 2023 Dec;19(52):e2305856. doi: 10.1002/smll.202305856. Epub 2023 Aug 27.
Organic small molecules with processing feasibility, structural diversity, and fine-tuned properties have the potential applications in solar vapor generation. However, the common defects of narrow solar absorption, low photothermal conversion efficiency, and photobleaching result in limited materials available and unsatisfactory evaporation performance. Herein, the perylene diimide (PDI) derivatives are exploited as stable sunlight absorbers for solar vapor generation. Particularly, the N,N'-bis(3,4,5-trimethoxyphenyl)-3,4,9,10-perylenetetracarboxylic diimide (PDI-DTMA) is well-designed with donor-acceptor-donor configuration based on plane rigid PDI core. The efficient photothermal conversion is enabled through strong intermolecular π-π stacking and intramolecular charge transfer, as revealed by experimental demonstration and theoretical calculation. The PDI-DTMA with a narrow band gap of 1.17 eV exhibits expanded absorption spectrum and enhanced nonradiative transition capability. The 3D hybrid hydrogels (PPHs) combining PDI-DTMA and polyvinyl alcohol are constructed. With the synergistic effect of solar-to-heat conversion, thermal localization management, water activation, and unobstructed water transmission of PPHs, the high water evaporation rates can reach 3.61-10.07 kg m h under one sun. The hydrogels also possess great potential in seawater desalination and sewage treatment. Overall, this work provides valuable insights into the design of photothermal organic small molecules and demonstrates their potentials in solar water evaporation.
具有可加工性、结构多样性和可精细调控性质的有机小分子在太阳能蒸汽产生方面具有潜在应用。然而，常见的窄太阳能吸收、低光热转换效率和光漂白等缺陷导致可用材料有限且蒸发性能不尽人意。在此，苝二酰亚胺（PDI）衍生物被开发用作太阳能蒸汽产生的稳定阳光吸收剂。特别地，基于平面刚性苝二酰亚胺核心，以给体-受体-给体构型精心设计了N，N'-双（3,4,5-三甲氧基苯基）-3,4,9,10-苝四羧酸二酰亚胺（PDI-DTMA）。实验证明和理论计算表明，通过强分子间π-π堆积和分子内电荷转移实现了高效光热转换。具有1.17 eV窄带隙的PDI-DTMA展现出扩展的吸收光谱和增强的非辐射跃迁能力。构建了结合PDI-DTMA和聚乙烯醇的三维杂化水凝胶（PPHs）。凭借PPHs的太阳能到热能转换、热局域管理、水活化和畅通的水传输的协同效应，在一个太阳光照下高水蒸发速率可达3.61 - 10.07 kg m² h⁻¹。这些水凝胶在海水淡化和污水处理方面也具有巨大潜力。总体而言，这项工作为光热有机小分子的设计提供了有价值的见解，并展示了它们在太阳能水蒸发中的潜力。
