Meng Qinghao, Huang Yihan, Deng Dan, Yang Yajie, Sha Haoyan, Zou Xiaoqin, Faller Roland, Yuan Ye, Zhu Guangshan
Key Laboratory of Polyoxometalate Science of Ministry of Education Northeast Normal University Renmin Avenue Changchun 130024 China.
Department of Materials Science and Engineering University of California Davis Davis CA 95616 USA.
Adv Sci (Weinh). 2020 Oct 1;7(22):2000067. doi: 10.1002/advs.202000067. eCollection 2020 Nov.
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 (N and N), 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 N 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.
具有出色的非金属介导催化反应性能的路易斯对（LPs）具有很高的基础研究价值和显著的应用前景。然而，它们的溶解性特征导致在循环使用时不稳定并失活。在此，具有两种路易斯碱位点（N和N）的层状多孔芳香骨架（PAF-6）被剥离成少层纳米片，与路易斯酸形成LP实体。在与各种多孔网络进行比较并通过密度泛函理论（DFT）计算验证后，确定特定空间环境中的N原子优选以空间位阻模式与缺电子硼化合物配位。裸露LP的多孔产物对烯烃和亚胺化合物的氢化反应显示出高催化活性，并且在氢化反应中成功进行10次循环后仍显示出约100%的活性。考虑到多孔有机骨架构建LP基团的天然优势，为制备用于高效和可循环催化的其他非金属多相催化剂开辟了新的前景。
