Constructing new metal–organic frameworks with complicated ligands from “One-Pot” <i>in situ</i> reactions

Kong, Xiang‐Jing; He, Tao; Zhang, Yongzheng; Wu, Xue‐Qian; Wang, Si-Nan; Xu, Mingming; Si, Guang-Rui; Li, Jian‐Rong

doi:10.1039/c9sc00178f

“…16,17,18 In addition to the interpenetrated Zr-based MOF investigated in this study, other interpenetrated Zr-based MOFs have been reported. [19][20][21][22] Among these, the UiO-66 type interpenetrated MOFs have been well known. [23][24][25][26][27][28][29] Other systems which exhibit interpenetration were found during isoreticular expansion of the linkers and have either ditopic [30][31][32][33][34] or tetratopic linkers, [35][36][37][38] which makes the relatively short tritopic linker used in this study a unique case.…”

Section: Introductionmentioning

confidence: 99%

Transient Catenation in a Zirconium-Based Metal–Organic Framework and Its Effect on Mechanical Stability and Sorption Properties

Robison

¹

,

Gong

²

,

Evans

³

et al. 2021

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Interpenetration of two or more sublattices is common among many metal-organic frameworks (MOFs). However, interpenetration in zirconium cluster-based MOFs is rarely observed. Herein, we study the evolution of one zirconium cluster-based, 3,8-connected MOF from its noninterpenetrated (NU-1200) to interpenetrated (STA-26) isomer. We observe this transient catenation process indirectly using ensemble methods, such as nitrogen porosimetry and X-ray diffraction, and directly, using high-resolution transmission electron microscopy. The approach detailed here will serve as a template for other researchers to monitor the interpenetration of their MOF samples at the bulk and single-particle limits. We investigate the mechanical stability of both lattices experimentally by pressurized in situ X-ray diffraction and nanoindentation as well as computationally with density functional theory (DFT) calculations. Both lines of study reveal that STA-26 is considerably more mechanically stable than NU-1200. We conclude this study by demonstrating the potential of these MOFs and their mixed phases for the capture of gaseous nhexane, used as a structural mimic for the chemical warfare agent, sulfur mustard gas.

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“…While the stabilities of Zr-MOFs constructed with low connection-number (5, and 4) nodes are still under debate 15,16,17,18 , 6-connection is likely the limit to keep the material stability at an acceptable level toward certain applications 19,20,21 . In a sharp contrast to the large number of Zr-MOFs based on high connection-number (above till 12) building units, only six compounds are constructed from 6connected Zr6-oxo clusters, including PCN-224 22 , PCN-777 23 (PCN, Porous Coordination Network), UMCM-309 24 (UMCM, University of Michigan Crystalline Material), the interpenetrated Zr-BTB 25 , MOF-808 19 and BUT-108 (BUT, Beijing University of Technology) 26 .…”

Section: Resultsmentioning

confidence: 99%

A Zirconium Metal-Organic Framework with SOC Topological Net for Catalytic Peptide Bond Hydrolysis

Wang¹,

Ly

²

,

Wahiduzzaman

³

et al. 2021

Preprint

0

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The discovery of nanozymes for selective fragmentation of proteins would boost the emerging areas of modern proteomics, however, the development of efficient and reusable artificial catalysts for peptide bond hydrolysis is challenging. Here we report the detailed catalytic properties of a microporous zirconium carboxylate metal-organic framework, MIP-201, in promoting peptide bond hydrolysis in a simple dipeptide, as well as in horse-heart myoglobin (Mb) protein that consists of 153 amino acids. We demonstrate that MIP-201 features an excellent catalytic activity and selectivity, a good tolerance toward reaction conditions covering a wide range of different pH values, and importantly, an exceptional recycling ability associated with easy regeneration process. Taking into account the excellent catalytic performance of MIP-201 and its other advantages such as 6-connected Zr6 cluster active sites, the green, scalable and cost-effective synthesis, and an outstanding chemical and architectural stability, our finding suggests that MIP-201 may be a promising and practical alternative to the current commercially available catalysts for peptide bond hydrolysis.

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“…While the stabilities of Zr-MOFs constructed with low connection-number (5, and 4) nodes are still under debate 15,16,17,18 , 6-connection is likely the limit to keep the material stability at an acceptable level toward certain applications 19,20,21 . In a sharp contrast to the large number of Zr-MOFs based on high connection-number (above 8 till 12) building units, only six compounds are constructed from 6connected Zr6-oxo clusters, including PCN-224 22 , PCN-777 23 (PCN, Porous Coordination Network), UMCM-309 24 (UMCM, University of Michigan Crystalline Material), the interpenetrated Zr-BTB 25 , MOF-808 19 and BUT-108 (BUT, Beijing University of Technology) 26 .…”

Section: Resultsmentioning

confidence: 99%

A Zirconium Metal-Organic Framework with SOC Topological Net for Catalytic Peptide Bond Hydrolysis

Wang¹,

Hgt

²

,

Wahiduzzaman

³

et al. 2021

Preprint

0

View full text Add to dashboard Cite

The discovery of nanozymes for selective fragmentation of proteins would boost the emerging areas of modern proteomics, however, the development of efficient and reusable artificial catalysts for peptide bond hydrolysis is challenging. Here we report the detailed catalytic properties of a microporous zirconium carboxylate metal-organic framework, MIP-201, in promoting peptide bond hydrolysis in a simple dipeptide, as well as in horse-heart myoglobin (Mb) protein that consists of 153 amino acids. We demonstrate that MIP-201 features an excellent catalytic activity and selectivity, a good tolerance toward reaction conditions covering a wide range of different pH values, and importantly, an exceptional recycling ability associated with easy regeneration process. Taking into account the excellent catalytic performance of MIP-201 and its other advantages such as 6-connected Zr6 cluster active sites, the green, scalable and cost-effective synthesis, and an outstanding chemical and architectural stability, our finding suggests that MIP-201 may be a promising and practical alternative to the current commercially available catalysts for peptide bond hydrolysis.

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Constructing new metal–organic frameworks with complicated ligands from “One-Pot” in situ reactions

Abstract: A “One-Pot” strategy has been developed to construct new metal–organic frameworks with complicated ligands from simple precursors by integrating organic and coordination chemistry.

Cited by 65 publications

References 57 publications

Transient Catenation in a Zirconium-Based Metal–Organic Framework and Its Effect on Mechanical Stability and Sorption Properties

Transient Catenation in a Zirconium-Based Metal–Organic Framework and Its Effect on Mechanical Stability and Sorption Properties

A Zirconium Metal-Organic Framework with SOC Topological Net for Catalytic Peptide Bond Hydrolysis

A Zirconium Metal-Organic Framework with SOC Topological Net for Catalytic Peptide Bond Hydrolysis

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