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Crystallinity and stability of covalent organic frameworks

Science China chemistry 2020年第10期63卷 1367-1390页

作者： Xin Huang Chao Sun Xiao Feng Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials Key Laboratory of Cluster ScienceMinistry of EducationSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China

Covalent organic frameworks(COFs)are a class of organic porous polymers with high crystallinity,and their structures can be precisely tailored via topology *** to the characteristics of permanent pores,periodic structures and rich building blocks,COFs have triggered tremendous attention in the past fifteen years and are extensively investigated in various *** and stability are two crucial features for practical *** general,these two features are contradictory for COFs formed via dynamic covalent chemistry(DCC).High thermodynamic reversibility is usually required to attain exceptional crystallinity of COFs,often resulting in limited *** first two reported COFs are based on the boroxine and boronate ester linkages,which are unstable in water and even in humid ***,many researchers doubt the stability of COFs for real ***,in these years,various novel linkages have been developed for the construction of COFs,and numerous newly synthesized COFs are robust towards strong acid/base and even some of them can resist the attack of strong oxidizing and reducing *** this review,we focus on the linkage chemistry of the COFs in terms of crystallinity and stability,further extending it to the investigation in the mechanisms of the crystal growth and the overall regulation of the contradiction between stability and *** strategies for improving the crystallinity,including selecting building units,introducing non-covalent interactions and slowing nucleation and growth rate,are described in the third section,while the methodologies for increasing the stability from the viewpoints of chemical modification and non-covalent interactions are summarized in the fourth ***,the challenges and perspectives are presented.

关键词： covalent organic frameworks crystallinity stability dynamic covalent chemistry linkage chemistry

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Converting Azine linkage into Highly Stable(Thio)Urea-Based Bicyclic-Fused-Ring Connections in Covalent Organic Frameworks via Criss-Cross[3+2]Cycloaddition

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CCS chemistry 2024年第9期6卷 2230-2240页

作者： Zhi-Bei Zhou Hui-Hui Sun Qiao-Yan Qi Xin Zhao Key Laboratory of Synthetic and Self-Assembly chemistry for Organic Functional Molecules Shanghai Institute of Organic ChemistryUniversity of Chinese Academy of SciencesChinese Academy of SciencesShanghai 200032

Exploring new linkage chemistry is of fundamental significance for covalent organic frameworks(COFs)to expand their structure and functional ***,we report a strategy for converting azine linkage into urea-and thiourea-based fused-ring connections in COFs by criss-cross[3+2]dipolar cycloaddition of azine with HNCO or *** as-prepared COFs with cyclized linkages exhibited enhanced chemical and thermal stability by locking the dynamic C=N linkages in the ***,functions could be introduced into the skeleton of COFs by this postsynthetic cyclization method,which enabled significant improvements in functionality,demonstrated by the studies on CO_(2)/N_(2) selective sorption,proton conduction,and Hg^(2+)*** use of this[3+2]cycloaddition strategy not only enriched the chemistry of linkage conversion for COFs but also offered a new way to fabricate fused-ring-linked COFs,thereby representing a high level of controllability on connectivity and functionality of COFs.

关键词： covalent organic frameworks linkage chemistry structural transformation [3+2]cycloaddition azine

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