Quasi-Homogeneous Photocatalysis in Ultrastiff Microporous Polymer Aerogels,Journal of the American Chemical Society

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Quasi-Homogeneous Photocatalysis in Ultrastiff Microporous Polymer Aerogels
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2024-05-23 , DOI: 10.1021/jacs.4c03862
Yan Su ₁ , Bo Li _{2,

3} , Zaoming Wang ₄ , Alexandre Legrand _{4,

5} , Takuma Aoyama ₆ , Shuai Fu ₇ , Yishi Wu ₈ , Ken-Ichi Otake ₄ , Mischa Bonn ₇ , Hai I Wang _{7,

9} , Qing Liao ₈ , Kenji Urayama ₁₀ , Susumu Kitagawa ₄ , Liangbin Huang ₃ , Shuhei Furukawa ₄ , Cheng Gu _{1,

2}

Affiliation

State Key Laboratory of Luminescent Materials and Devices, Institute of Polymer Optoelectronic Materials and Devices, South China University of Technology, No. 381 Wushan Road, Tianhe District, Guangzhou 510640, PR China.
College of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering, Sichuan University, Chengdu 610065, PR China.
Key Laboratory of Functional Molecular Engineering of Guangdong Province, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510641, PR China.
Institute for Integrated Cell-Material Sciences, Kyoto University, Yoshida, Sakyo-ku, Kyoto 606-8501, Japan.
Unité de Catalyse et Chimie du Solide (UCCS), CNRS, Centrale Lille, Université de Lille, Université d'Artois, UMR 8181, Lille F-59000, France.
Department of Macromolecular Science and Engineering, Kyoto Institute of Technology, Matsugasaki, Sakyo-ku, Kyoto 606-8585, Japan.
Max Planck Institute for Polymer Research, Ackermannweg 10, Mainz 55122, Germany.
Beijing Key Laboratory for Optical Materials and Photonic Devices, Department of Chemistry, Capital Normal University, Beijing 100048, PR China.
Nanophotonics, Debye Institute for Nanomaterials Science, Utrecht University, Princetonplein 1, Utrecht 3584 CC, The Netherlands.
Department of Material Chemistry, Kyoto University, Katsura, Nishikyo-ku, Kyoto 615-8510, Japan.

The development of efficient and low-cost catalysts is essential for photocatalysis; however, the intrinsically low photocatalytic efficiency as well as the difficulty in using and recycling photocatalysts in powder morphology greatly limit their practical performance. Herein, we describe quasi-homogeneous photocatalysis to overcome these two limitations by constructing ultrastiff, hierarchically porous, and photoactive aerogels of conjugated microporous polymers (CMPs). The CMP aerogels exhibit low density but high stiffness beyond 10⁵ m² s^–2, outperforming most low-density materials. Extraordinary stiffness ensures their use as robust scaffolds for scaled photocatalysis and recycling without damage at the macroscopic level. A challenging but desirable reaction for direct deaminative borylation is demonstrated using CMP aerogel-based quasi-homogeneous photocatalysis with gram-scale productivity and record-high efficiency under ambient conditions. Combined terahertz and transient absorption spectroscopic studies unveil the generation of high-mobility free carriers and long-lived excitonic species in the CMP aerogels, underlying the observed superior catalytic performance.

中文翻译：

超硬微孔聚合物气凝胶中的准均相光催化

开发高效、低成本的催化剂对于光催化至关重要；然而，本质上较低的光催化效率以及粉末形态光催化剂的使用和回收困难极大地限制了其实际性能。在此，我们描述了准均质光催化，通过构建共轭微孔聚合物（CMP）的超硬、分层多孔和光活性气凝胶来克服这两个限制。 CMP 气凝胶具有低密度和超过 10 ⁵ m ² s ^–2的高刚度，优于大多数低密度材料。非凡的刚度确保它们用作大规模光催化和回收的坚固支架，而不会在宏观水平上造成损坏。使用基于 CMP 气凝胶的准均相光催化，证明了一种具有挑战性但理想的直接脱氨基硼化反应，在环境条件下具有克级生产率和创纪录的高效率。太赫兹和瞬态吸收光谱相结合的研究揭示了 CMP 气凝胶中高迁移率自由载流子和长寿命激子物种的生成，这是观察到的优异催化性能的基础。

更新日期：2024-05-23

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