Conductive MOFs based on Thiol-functionalized Linkers: Challenges, Opportunities, and Recent Advances

Deng, Xiangling; Zheng, Sai-Li; Zhong, Yuan-Hui; Hu, Jieying; Chung, Lai‐Hon

doi:10.1016/j.ccr.2021.214235

Cited by 67 publications

(37 citation statements)

References 249 publications

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“…From the structural perspective, the integration of bimetallic nodes inside OMCs could be an effective method to tailor the targeting structural topologies and introduce additional functionalities. However, the kinetic inertness and fast reaction rate of the metal–chalcogen bond formation reaction 13 make the direct synthesis impractical, since the reaction of ligands with different metal ions would inevitably suffer from the separate growth of OMCs in solution. Encouragingly, post-synthetic modification provides an alternative scheme for accessing materials when the direct synthesis route fails 14 , 15 .…”

Section: Introductionmentioning

confidence: 99%

Construction of conducting bimetallic organic metal chalcogenides via selective metal metathesis and oxidation transformation

Jin

Fang²,

Li³

et al. 2022

Nat Commun

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Conducting organic metal chalcogenides (OMCs) have attracted considerable interest for their superior electrical properties and fascinating functions. However, the electronic structural and functional regulation of OMCs are typically limited to the combination of monometallic nodes and graphene-like ligands. Here, we report a family of bimetallic OMCs ([CuAgx(C6S6)]n, x = 4 or 2) synthesized via selective metal metathesis and oxidation transformation. Both OMCs have alternatively stacked one-dimensional (1D) copper-dithiolene chains and 2D Ag-S networks, which can synergistically serve as charge transport pathways, rendering these bimetallic materials highly conductive. The incorporation of heterometallic nodes turned nonmagnetic [Ag5(C6S6)]n into paramagnetic metallic [CuAg4(C6S6)]n, which exhibited a coherence-incoherence crossover in magnetic susceptibility measurements and an unusually large Sommerfeld coefficient, reminiscent of the characteristics of Kondo lattice. This work opens up an avenue for tailoring the electronic structures of OMCs and provides a platform for studying the dichotomy between electronic localization and itinerancy.

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Section: Introductionmentioning

confidence: 99%

Construction of conducting bimetallic organic metal chalcogenides via selective metal metathesis and oxidation transformation

Jin

Fang²,

Li³

et al. 2022

Nat Commun

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“…The organic building blocks that are called linkers are available in different shapes and sizes and give MOFs a sundry of topological designs . Both metal nodes and organic linkers contribute to MOF structure-physical/chemical property relationships. ,, …”

Section: Introductionmentioning

confidence: 99%

“…29 Both metal nodes and organic linkers contribute to MOF structure-physical/chemical property relationships. 7,19,30 More than 90 000 unique MOFs have been synthesized. As a result of this enormous number of reported structures, it is difficult to identify MOFs with certain properties, for example, pore sizes with specific metal centers.…”

Section: Introductionmentioning

confidence: 99%

Demonstration of High-Throughput Building Block and Composition Analysis of Metal–Organic Frameworks

Hawley

Yao

et al. 2022

J. Chem. Inf. Model.

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Metal–organic frameworks (MOFs) are composed of inorganic metal-containing nodes and organic linker groups and are promising porous materials for a wide range of applications. More than 90 000 different MOFs have been synthesized with different inorganic nodes, organic linkers, and node-linker connectivity patterns. While databases have been created to catalog this enormous number of structures, they generally do not provide functionality to easily search, sort, and understand MOFs based on composition and building blocks. Because structure–property relationships are critical to identify, here we outline our new program MOFseek and demonstrate that it can perform high-throughput structure and composition analyses of MOF structures. This program enables the fast analysis of tens of thousands of MOFs in databases based on the local chemical environment. We demonstrate the unique capabilities of MOFseek by analyzing the CoRE MOF database of structures.

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“…These properties makes them useful in electronics, sensing, energy storage, sorption, and catalysis. 7 Scheme 1: Schematic representation of the versatility and applicability of the UiO-66-(SH)2 MOF.…”

Section: Introductionmentioning

confidence: 99%

“…4,5 Whereas, hard metal ions with carboxylate linkers carrying free standing thiols form another category. 6,7 Thiols are redox active functional groups that are generally prone to oxidation. When oxidized, they produce disulfides, sulfenic, sulfinic, and sulfonic acids.…”

Section: Introductionmentioning

confidence: 99%

Direct One-pot Synthesis of Highly Tunable Mixed-linker UiO-66-(SH)2 Metal-Organic Frameworks: Enroute Toward Robust Sulfonic Acid Tagged UiO-66 Architectures

Chowdhury

Sharma

Rathi

et al. 2022

Preprint

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Synthesis, storage, and characterization of thiol functionalized metal-organic frameworks (MOFs) is highly challenging. However, they continue to be of great interest due to their broad spectrum of applications. In this work, for the first time, a solid solution approach has been adopted to dilute the thiol content in UiO-66-(SH)2 [Universitetet i Oslo] MOF by terephthalic acid linker without influencing its topology. Detailed characterization of the mixed-linker UiO-66-(SH)2 MOF samples have been performed using powder X-ray diffraction (PXRD), N2 sorption, X-ray photoelectron spectroscopy (XPS) and electron microscopy. The solid dilution had an overall impact on the crystallinity, defects, porosity and particle size of the UiO-66-(SH)2 framework. This study has the potential to significantly influence the syntheses of nanoscale thiol functionalized MOF materials and their applications in photocatalysis, water purification and drug delivery. This work also incorporates post synthetic oxidation (PSO) to produce sulfonic acid tagged mixed-linker UiO-66 frameworks. The solid dilution has been found to be critical in preventing the frameworks from losing their crystallinity and porosity, upon activation. Thus, this work also paves the way for a general strategy to impart stability to sulfonic acid tagged UiO-66 framework having wide ranging applications.

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Conductive MOFs based on Thiol-functionalized Linkers: Challenges, Opportunities, and Recent Advances

Cited by 67 publications

References 249 publications

Construction of conducting bimetallic organic metal chalcogenides via selective metal metathesis and oxidation transformation

Construction of conducting bimetallic organic metal chalcogenides via selective metal metathesis and oxidation transformation

Demonstration of High-Throughput Building Block and Composition Analysis of Metal–Organic Frameworks

Direct One-pot Synthesis of Highly Tunable Mixed-linker UiO-66-(SH)2 Metal-Organic Frameworks: Enroute Toward Robust Sulfonic Acid Tagged UiO-66 Architectures

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