Two-dimensional sp2 carbon–conjugated covalent organic frameworks

Jin, Enquan; Asada, Mizue; Xu, Qing; Dalapati, Sasanka; Addicoat, Matthew A.; Brady, Michael A.; Xu, Hong; Nakamura, Toshikazu; Heine, Thomas; Chen, Qiuhong; Jiang, Donglin

doi:10.1126/science.aan0202

Title: Two-dimensional sp² carbon–conjugated covalent organic frameworks

Journal Article · Thu Aug 17 00:00:00 EDT 2017 · Science

DOI:https://doi.org/10.1126/science.aan0202· OSTI ID:1379913

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Japan Advanced Inst. of Science and Technology, Asahidai (Japan)
Inst. for Molecular Science, Nishigo-naka, Myodaiji (Japan)
Nottingham Trent Univ., Nottingham (United Kingdom)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS). Molecular Foundry
Japan Advanced Inst. of Science and Technology, Asahidai (Japan); Inst. for Molecular Science, Nishigo-naka, Myodaiji (Japan)
Leipzig Univ. (Germany). Wilhelm-Ostwald-Inst. for Physical and Theoretical Chemistry

In this work, we synthesized a two-dimensional (2D) crystalline covalent organic framework (sp²c-COF) that was designed to be fully π-conjugated and constructed from all sp² carbons by C=C condensation reactions of tetrakis(4-formylphenyl)pyrene and 1,4-phenylenediacetonitrile. The C=C linkages topologically connect pyrene knots at regular intervals into a 2D lattice with π conjugations extended along both x and y directions and develop an eclipsed layer framework rather than the more conventionally obtained disordered structures. The sp²c-COF is a semiconductor with a discrete band gap of 1.9 electron volts and can be chemically oxidized to enhance conductivity by 12 orders of magnitude. The generated radicals are confined on the pyrene knots, enabling the formation of a paramagnetic carbon structure with high spin density. The sp² carbon framework induces ferromagnetic phase transition to develop spin-spin coherence and align spins unidirectionally across the material.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); European Research Council (ERC); Ministry of Education, Culture, Sports, Science and Technology, Japan

Grant/Contract Number:: AC02-05CH11231; ERC-StG 256962C3ENV

OSTI ID:: 1379913

Journal Information:: Science, Vol. 357, Issue 6352; ISSN 0036-8075

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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PolyCOFs: A New Class of Freestanding Responsive Covalent Organic Framework Membranes with High Mechanical Performance Wang, Zhifang; Yu, Qi; Huang, Yubo ACS Central Science, Vol. 5, Issue 8 https://doi.org/10.1021/acscentsci.9b00212	journal	June 2019
Dual-template engineering of triple-layered nanoarray electrode of metal chalcogenides sandwiched with hydrogen-substituted graphdiyne Zhuo, Sifei; Shi, Yusuf; Liu, Lingmei Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-05474-0	journal	August 2018
Two-dimensional semiconducting covalent organic frameworks via condensation at arylmethyl carbon atoms Bi, Shuai; Yang, Can; Zhang, Wenbei Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-10504-6	journal	June 2019
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Regenerable and stable sp2 carbon-conjugated covalent organic frameworks for selective detection and extraction of uranium Cui, Wei-Rong; Zhang, Cheng-Rong; Jiang, Wei Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-14289-x	journal	January 2020
Covalent Organic Frameworks: From Materials Design to Biomedical Application Zhao, Fuli; Liu, Huiming; Mathe, Salva Nanomaterials, Vol. 8, Issue 1 https://doi.org/10.3390/nano8010015	journal	December 2017
Realization of Lieb Lattice in Covalent-organic Frameworks with Tunable Topology and Magnetism Cui, Bin; Zheng, Xingwen; Wang, Jianfeng arXiv https://doi.org/10.48550/arxiv.1904.12487	text	January 2019

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