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Porous Aromatic Framework Nanosheets Anchored with Lewis Pairs for Efficient and Recyclable Heterogeneous Catalysis
Advanced Science ( IF 14.3 ) Pub Date : 2020-10-01 , DOI: 10.1002/advs.202000067 Qinghao Meng 1 , Yihan Huang 2 , Dan Deng 1 , Yajie Yang 1 , Haoyan Sha 3 , Xiaoqin Zou 1 , Roland Faller 3 , Ye Yuan 1 , Guangshan Zhu 1
Advanced Science ( IF 14.3 ) Pub Date : 2020-10-01 , DOI: 10.1002/advs.202000067 Qinghao Meng 1 , Yihan Huang 2 , Dan Deng 1 , Yajie Yang 1 , Haoyan Sha 3 , Xiaoqin Zou 1 , Roland Faller 3 , Ye Yuan 1 , Guangshan Zhu 1
Affiliation
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Lewis pairs (LPs) with outstanding performance for nonmetal‐mediated catalysis reactions have high fundamental interest and remarkable application prospects. However, their solubility characteristics lead to instability and deactivation upon recycling. Here, the layered porous aromatic framework (PAF‐6), featuring two kinds of Lewis base sites (NPiperazine and NTriazine), is exfoliated into few‐layer nanosheets to form the LP entity with the Lewis acid. After comparison with various porous networks and verification by density functional theory (DFT) calculations, the NTriazine atom in the specific spatial environment is determined to preferably coordinate with the electron‐deficient boron compound in a sterically hindered pattern. LP‐bare porous product displays high catalytic activity for the hydrogenation of both olefin and imine compounds, and demonstrates ≈100% activity after 10 successful cycles in hydrogenation reactions. Considering the natural advantage of porous organic frameworks to construct LP groups opens up novel prospects for preparing other nonmetallic heterogeneous catalysts for efficient and recyclable catalysis.
中文翻译：
路易斯对锚定的多孔芳香骨架纳米片用于高效且可回收的多相催化
路易斯对（LPs）在非金属介导的催化反应中具有出色的性能，具有很高的基础兴趣和显着的应用前景。然而，它们的溶解度特性导致回收时不稳定和失活。在这里，具有两种路易斯碱位点（N哌嗪和N三嗪）的层状多孔芳香骨架（PAF-6）被剥离成几层纳米片，与路易斯酸形成LP实体。通过与各种多孔网络的比较以及密度泛函理论（DFT）计算的验证，确定特定空间环境中的N-三嗪原子优选以位阻模式与缺电子硼化合物配位。LP裸多孔产物对烯烃和亚胺化合物的加氢表现出高催化活性，并且在加氢反应10次成功循环后表现出约100%的活性。考虑到多孔有机骨架构建LP基团的天然优势，为制备其他非金属多相催化剂以实现高效和可回收的催化开辟了新的前景。
更新日期：2020-11-19
中文翻译：
路易斯对锚定的多孔芳香骨架纳米片用于高效且可回收的多相催化
路易斯对（LPs）在非金属介导的催化反应中具有出色的性能，具有很高的基础兴趣和显着的应用前景。然而，它们的溶解度特性导致回收时不稳定和失活。在这里，具有两种路易斯碱位点（N哌嗪和N三嗪）的层状多孔芳香骨架（PAF-6）被剥离成几层纳米片，与路易斯酸形成LP实体。通过与各种多孔网络的比较以及密度泛函理论（DFT）计算的验证，确定特定空间环境中的N-三嗪原子优选以位阻模式与缺电子硼化合物配位。LP裸多孔产物对烯烃和亚胺化合物的加氢表现出高催化活性，并且在加氢反应10次成功循环后表现出约100%的活性。考虑到多孔有机骨架构建LP基团的天然优势，为制备其他非金属多相催化剂以实现高效和可回收的催化开辟了新的前景。
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