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Efficient Quasi-Homogenous Photocatalysis Enabled by Molecular Nanophotocatalysts with Donor-Acceptor Motif
Advanced Materials ( IF 27.4 ) Pub Date : 2024-12-02 , DOI: 10.1002/adma.202413440
Xueyan Liu, Miaojie Yu, Kai Huang, Haiyang Huang, Hongxu Gu, Changhao Tian, Jing Qi, Zhiqian Guo, Cheng Lian, Yongzhen Wu, Weiwei Zhang, Wei-Hong Zhu

Polymer semiconductors have attracted much attention for photocatalytic hydrogen evolution, but they typically exhibit micrometer-sized particles in water-suspension, causing severe loss in light absorption and exciton recombination. Here a molecular nanophotocatalyst featuring a donor-acceptor motif is presented that solution is processed via a facile stirring nanoprecipitation method assisted by hydrophilic surfactants, enabling an efficient quasi-homogenous hydrogen evolution. In contrast to the original bulk powder (heterogeneous system), these quasi-homogenous nanophotocatalysts exhibit significantly improved light-harvesting, water-wettability, and exciton dissociation, resulting in distinctly enhanced (by four-order-of-magnitude) photocatalytic hydrogen evolution rate. The optimized nanophotocatalysts (4CzPN/DDBAB/SDBS) generate an outstanding hydrogen evolution rate of 116.42 mmol g−1 h−1 and apparent quantum yield of 30.2% at 365 nm, which are among the highest reported for single-junction organic photocatalysts. The scalability of the quasi-homogenous photocatalysts is further demonstrated using a flow-based flash nanoprecipitation (FNP) processing.

中文翻译:


具有供体-受体基序的分子纳米光催化剂实现高效的准均相光催化



聚合物半导体在光催化析氢方面备受关注,但它们通常在水悬浮液中表现出微米级的颗粒,导致光吸收和激子复合的严重损失。这里提出了一种具有供体-受体基序的分子纳米光催化剂,在亲水性表面活性剂的辅助下,通过简单的搅拌纳米沉淀方法处理溶液,从而实现高效的准均相析氢。与原始的块状粉末(异质系统)相比,这些准均质纳米光催化剂表现出显着改善的光捕获、水润湿性和激子解离,从而明显提高了光催化析氢速率(四个数量级)。优化的纳米光催化剂 (4CzPN/DDBAB/SDBS) 在 365 nm 处产生 116.42 mmol g-1 h-1 的出色析氢速率和 30.2% 的表观量子产率,这是单结有机光催化剂中报道的最高值之一。使用基于流动的闪光纳米沉淀 (FNP) 工艺进一步证明了准均质光催化剂的可扩展性。
更新日期:2024-12-03
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