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

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

doi:10.1038/s41557-020-00562-5

Cited by 109 publications

(95 citation statements)

References 36 publications

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“…[31][32][33] F s is powered by ultrasonic generator or other power source, which can't be increased unlimited (around 5E-18 -5E-16 J for nm force area). F i is decided by the interaction energy between adjacent layers in unit area (3.2E-19 J per 1 nm 2 in graphene), weakening the interlaminar interaction is the key for the successful exfoliation of ultra-thin nanosheets, 34 the solvent or chemical intercalations are generally used at present to achieve To make the exfoliation possible, we need to decrease the value and increase the F s value, which requires rational design to substantially reduce the bonding energy and the number of bonding sites in unit area. Specifically, three key factors should be considered (Fig.…”

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confidence: 99%

Facile Exfoliation of Two-Dimensional Crystalline Monolayer Nanosheets from an Amorphous Metal–Organic Framework

et al. 2022

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The large-scale preparation of monolayer 2D material remains a great challenge, which hinders its real application. Herein, we report a novel layered MOF, IPM-1, which is synthesized from a cage-like organic linker with extremely weak interlaminar interaction.When subjected to external disturbance, IPM-1 degenerated into an intermediate state between the crystalline and amorphous phase, in which the layers retain the in-plane twodimension periodic structure but are misaligned in the third dimension, leading to the loss of apparent porosity and crystallinity. This amorphous IPM-1 is readily to be exfoliated into crystalline 2D nanosheets with a thickness of 1.15 nm at gram-scale, excellent thickness homogeneity, lateral size up to 10 μm, and restored microporosity. IPM-1 nanosheets exhibited high chemical stability and activity in the catalysis oxidation of alcohol, and combined the advantages of both homogeneous and heterogeneous catalyst. This work underlines that MOFs without apparent crystallinity can be idea precursors for the successful preparation of 2D crystalline monolayer nanosheets.

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confidence: 99%

Facile Exfoliation of Two-Dimensional Crystalline Monolayer Nanosheets from an Amorphous Metal–Organic Framework

et al. 2022

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“…6 In addition, some recent examples have revealed that few-and single-layered metal-organic frameworks (MOFs) 7,8 or covalent organic frameworks (COFs) [9][10][11] could be obtained through the exfoliation of their layered bulky parent materials. Very recently, Loh and co-workers 12 have developed a supramolecular approach to facilitate self-exfoliation of bulky 2D COFs into COF sheets with controllable thickness. In contrast to the top-down strategy, the other strategy is the more straightforward bottom-up construction of 2D materials via the direct polymerization of small organic building blocks at interfaces, 13,14 in solid state, 15,16 or even in solution.…”

Section: Introductionmentioning

confidence: 99%

Toward a Two-Dimensional Supramolecular Organic Framework with High Degree of Internal Order via Amphiphilic Modification

et al. 2022

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Solution-phase self-assembly of two-dimensional (2D) networks with a high degree of internal order and long-range periodicity is a great challenge. Herein, we report a rational design to improve 2D self-assembly in water through amphiphilic modification of the building block. An amphiphilic tritopic molecule ( 1) is designed and synthesized by introducing three hydrophilic oligo(ethylene glycol) moieties and three hydrophobic hexyl chains. The assembly of 1 and cucurbit [8]uril (CB[8]) leads to the formation of a Janus 2D supramolecular organic framework (SOF), which further creates unique bilayer supramolecular networks and exhibits an unprecedentedly high degree of internal order and long-range periodicity. In contrast, the assembly of a nonamphiphilic analog (2) with CB[8] only generates a 2D SOF with a lower degree of internal order, suggesting that the inherent amphiphilicity of 1 plays a crucial role in improving its 2D self-assembly in aqueous phase.

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“…Introduced by the pioneer work of Yaghi, [11] this type of COFs have attracted significant attention and shown great potentials in gas storage, [12] separation, [13,14] heterogeneous catalysis, [15][16][17][18][19] sensing, [5,[20][21][22] optoelectronics, [23] ion conduction, [24] and among others. [25][26][27][28][29][30] However, the low chemical stability for most of the acylhydrazone-linked COFs remains a major issue and prevents their wide applications. Although hydrophobic engineering and metal coordination interactions can protect the hydrazone from hydrolysis, thus improving the chemical stability of acylhydrazone-linked COFs, [9,14] fewer materials can survive in harsh chemical environments, such as strong acid, strong base, and redox conditions.…”

Section: Introductionmentioning

confidence: 99%

“…As a new type of robust linkages in the synthesis of COFs, the acylhydrazone‐linked COFs by condensation between hydrazides and aldehydes show high crystallinity and improved chemical stability. Introduced by the pioneer work of Yaghi, [11] this type of COFs have attracted significant attention and shown great potentials in gas storage, [12] separation, [13,14] heterogeneous catalysis, [15–19] sensing, [5,20–22] optoelectronics, [23] ion conduction, [24] and among others [25–30] . However, the low chemical stability for most of the acylhydrazone‐linked COFs remains a major issue and prevents their wide applications.…”

Section: Introductionmentioning

confidence: 99%

An Ultrastable Crystalline Acylhydrazone‐Linked Covalent Organic Framework for Efficient Removal of Organic Micropollutants from Water

Zhang

Zhao

et al. 2021

Chemistry A European J

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As an important member of crystalline porous polymers, acylhydrazone-linked covalent organic frameworks (COFs) have gained much attention in recent years. However, the low structural stability imparts a limit on their practical applications. To tackle this problem, we report a simple strategy to increase the chemical stability of acylhydrazonelinked COFs by incorporating azobenzene groups in the conjugated framework. Through reinforcing the π-π stacking interactions between the adjacent layers with increased πsurface, it is surprising to find that the resulting materials exhibit extreme stability in harsh environments, such as in strong acid, strong base, aqueous educing agent and boiling water, even exposed to air for one year. As a proof-ofconcept, such frameworks have been used to remove various organic micropollutants such as antibiotics, plastic components, endocrine disruptors, and carcinogens from water with high capacity, fast speed and excellent reusability over a wide pH range at environmentally relevant concentrations. The results provide a new avenue to significantly enhance the stability of COFs for practical applications.

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

Cited by 109 publications

References 36 publications

Facile Exfoliation of Two-Dimensional Crystalline Monolayer Nanosheets from an Amorphous Metal–Organic Framework

Facile Exfoliation of Two-Dimensional Crystalline Monolayer Nanosheets from an Amorphous Metal–Organic Framework

Toward a Two-Dimensional Supramolecular Organic Framework with High Degree of Internal Order via Amphiphilic Modification

An Ultrastable Crystalline Acylhydrazone‐Linked Covalent Organic Framework for Efficient Removal of Organic Micropollutants from Water

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