Partitioning the interlayer space of covalent organic frameworks by embedding pseudorotaxanes in their backbones

Xing Li, Hai Sen Xu, Kai Leng, See Wee Chee, Xiaoxu Zhao, Noopur Jain, Hai Xu, Jingsi Qiao, Qiang Gao, In Hyeok Park, Su Ying Quek, Utkur Mirsaidov, Kian Ping Loh

Research output: Journal article publicationJournal articleAcademic researchpeer-review

88 Citations (Scopus)


Mono- or few-layer sheets of covalent organic frameworks (COFs) represent an attractive platform of two-dimensional materials that hold promise for tailor-made functionality and pores, through judicious design of the COF building blocks. But although a wide variety of layered COFs have been synthesized, cleaving their interlayer stacking to obtain COF sheets of uniform thickness has remained challenging. Here, we have partitioned the interlayer space in COFs by incorporating pseudorotaxane units into their backbones. Macrocyclic hosts based on crown ethers were embedded into either a ditopic or a tetratopic acylhydrazide building block. Reaction with a tritopic aldehyde linker led to the formation of acylhydrazone-based layered COFs in which one basal plane is composed of either one layer, in the case of the ditopic macrocyclic component, or two adjacent layers covalently held together by its tetratopic counterpart. When a viologen threading unit is introduced, the formation of a host–guest complex facilitates the self-exfoliation of the COFs into crystalline monolayers or bilayers, respectively. [Figure not available: see fulltext.]

Original languageEnglish
Pages (from-to)1115-1122
Number of pages8
JournalNature Chemistry
Issue number12
Publication statusPublished - Dec 2020
Externally publishedYes

ASJC Scopus subject areas

  • General Chemistry
  • General Chemical Engineering


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