Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 143, Issue 27, Pages 10243-10249Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c03739
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Funding
- Class D of Qianjiang Talent Program [ZD20011250001]
- Zhejiang University of Technology [2019125016829]
- Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang [2020R01002]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB20000000]
- Key Program of Frontier Science, CAS [QYZDJ-SSW-SLH033]
- Xiamen Science and Technology Program Project [3502Z20203085]
- Natural Science Foundation of Jiangsu Province [BK20200476]
- China Postdoctoral Science Foundation [2021M693178]
- National Natural Science Foundation of China (NSFC) [21771191]
- Shandong Natural Science Fund [ZR2020KB010]
- Fundamental Research Funds for the Central Universities [19CX05001A]
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Covalent organic frameworks (COFs) have shown significant success in the past decade, with recent research demonstrating the potential for sub-stoichiometric construction to create new structures and applications. This work highlights the possibility of partially connected frameworks in COFs, leading to new possibilities for enhanced functionality and controlled structures.
Covalent organic frameworks (COFs), a fast-growing field in crystalline porous materials, have achieved tremendous success in structure development and application exploration over the past decade. The vast majority of COFs reported to date are designed according to the basic concept of reticular chemistry, which is rooted in the idea that building blocks are fully connected within the frameworks. We demonstrate here that sub-stoichiometric construction of 2D/3D COFs can be accomplished by the condensation of a hexagonal linker with 4-connected building units. It is worth noting that the partially connected frameworks were successfully reticulated for 3D COFs for the first time, representing the highest BET surface area among imine-linked 3D COFs to data. The unreacted benzaldehydes in COF frameworks can enhance C2H2 and CO2 adsorption capacity and selectivities between C2H2/CH4 and C2H2/CO2 for sub-stoichiometric 2D COFs, while the reserved benzaldehydes control the interpenetrated architectures for the 3D case, achieving a rare non-interpenetrated pts topology for 3D COFs. This work not only paves a new avenue to build new COFs and endows residual function groups with further applications but also prompts redetermination of reticular frameworks in highly connected and symmetrical COFs.
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