Porous Aromatic Framework Nanosheets Anchored with Lewis Pairs for Efficient and Recyclable Heterogeneous Catalysis
Abstract 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 fram...
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doaj-6a6722fc36974ea5955d8239f1c77a9e2020-11-25T04:10:35ZengWileyAdvanced Science2198-38442020-11-01722n/an/a10.1002/advs.202000067Porous Aromatic Framework Nanosheets Anchored with Lewis Pairs for Efficient and Recyclable Heterogeneous CatalysisQinghao Meng0Yihan Huang1Dan Deng2Yajie Yang3Haoyan Sha4Xiaoqin Zou5Roland Faller6Ye Yuan7Guangshan Zhu8Key Laboratory of Polyoxometalate Science of Ministry of Education Northeast Normal University Renmin Avenue Changchun 130024 ChinaDepartment of Materials Science and Engineering University of California Davis Davis CA 95616 USAKey Laboratory of Polyoxometalate Science of Ministry of Education Northeast Normal University Renmin Avenue Changchun 130024 ChinaKey Laboratory of Polyoxometalate Science of Ministry of Education Northeast Normal University Renmin Avenue Changchun 130024 ChinaDepartment of Chemical Engineering University of California Davis Davis CA 95616 USAKey Laboratory of Polyoxometalate Science of Ministry of Education Northeast Normal University Renmin Avenue Changchun 130024 ChinaDepartment of Chemical Engineering University of California Davis Davis CA 95616 USAKey Laboratory of Polyoxometalate Science of Ministry of Education Northeast Normal University Renmin Avenue Changchun 130024 ChinaKey Laboratory of Polyoxometalate Science of Ministry of Education Northeast Normal University Renmin Avenue Changchun 130024 ChinaAbstract 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.https://doi.org/10.1002/advs.202000067heterogeneous catalysisLewis pairsnanosheetsporous aromatic frameworksporous organic frameworks |
collection |
DOAJ |
language |
English |
format |
Article |
sources |
DOAJ |
author |
Qinghao Meng Yihan Huang Dan Deng Yajie Yang Haoyan Sha Xiaoqin Zou Roland Faller Ye Yuan Guangshan Zhu |
spellingShingle |
Qinghao Meng Yihan Huang Dan Deng Yajie Yang Haoyan Sha Xiaoqin Zou Roland Faller Ye Yuan Guangshan Zhu Porous Aromatic Framework Nanosheets Anchored with Lewis Pairs for Efficient and Recyclable Heterogeneous Catalysis Advanced Science heterogeneous catalysis Lewis pairs nanosheets porous aromatic frameworks porous organic frameworks |
author_facet |
Qinghao Meng Yihan Huang Dan Deng Yajie Yang Haoyan Sha Xiaoqin Zou Roland Faller Ye Yuan Guangshan Zhu |
author_sort |
Qinghao Meng |
title |
Porous Aromatic Framework Nanosheets Anchored with Lewis Pairs for Efficient and Recyclable Heterogeneous Catalysis |
title_short |
Porous Aromatic Framework Nanosheets Anchored with Lewis Pairs for Efficient and Recyclable Heterogeneous Catalysis |
title_full |
Porous Aromatic Framework Nanosheets Anchored with Lewis Pairs for Efficient and Recyclable Heterogeneous Catalysis |
title_fullStr |
Porous Aromatic Framework Nanosheets Anchored with Lewis Pairs for Efficient and Recyclable Heterogeneous Catalysis |
title_full_unstemmed |
Porous Aromatic Framework Nanosheets Anchored with Lewis Pairs for Efficient and Recyclable Heterogeneous Catalysis |
title_sort |
porous aromatic framework nanosheets anchored with lewis pairs for efficient and recyclable heterogeneous catalysis |
publisher |
Wiley |
series |
Advanced Science |
issn |
2198-3844 |
publishDate |
2020-11-01 |
description |
Abstract 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. |
topic |
heterogeneous catalysis Lewis pairs nanosheets porous aromatic frameworks porous organic frameworks |
url |
https://doi.org/10.1002/advs.202000067 |
work_keys_str_mv |
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