Visualizing the degradation of nerve agent simulants using functionalized Zr-based MOFs: from solution to hydrogels

Su, Hongyan; Huang, Pengcheng; Wu, Fang

doi:10.1039/d1cc05199g

Cited by 11 publications

(6 citation statements)

References 38 publications

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“…The fabrication of phosphotriesterase-inspired MOFs is also critical for practical application under working conditions. Therefore, many efforts have been made to fabricate the MOFs into mixed-matrix membranes, nanofiber kebabs, hydrogels, or integrate the MOFs onto activated carbon, fibers, and polymer sponge. − In 2015, Barea and Navarro took advantage of lithium alkoxide doped UiO-66 to develop self-detoxifying adsorbents of CWA containing hydrolyzable P–F, P–O, and C–Cl bonds . This work demonstrated a novel strategy to combine air-permeation properties of the textiles with the self-detoxifying properties of MOFs, paving the way to integrate MOFs into self-detoxifying protective fabrics (Figure ).…”

Section: Mofs With Enzyme Active Sitesmentioning

confidence: 99%

Bioinspired Framework Catalysts: From Enzyme Immobilization to Biomimetic Catalysis

et al. 2023

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Enzymatic catalysis has fueled considerable interest from chemists due to its high efficiency and selectivity. However, the structural complexity and vulnerability hamper the application potentials of enzymes. Driven by the practical demand for chemical conversion, there is a long-sought quest for bioinspired catalysts reproducing and even surpassing the functions of natural enzymes. As nanoporous materials with high surface areas and crystallinity, metal−organic frameworks (MOFs) represent an exquisite case of how natural enzymes and their active sites are integrated into porous solids, affording bioinspired heterogeneous catalysts with superior stability and customizable structures. In this review, we comprehensively summarize the advances of bioinspired MOFs for catalysis, discuss the design principle of various MOF-based catalysts, such as MOF−enzyme composites and MOFs embedded with active sites, and explore the utility of these catalysts in different reactions. The advantages of MOFs as enzyme mimetics are also highlighted, including confinement, templating effects, and functionality, in comparison with homogeneous supramolecular catalysts. A perspective is provided to discuss potential solutions addressing current challenges in MOF catalysis.

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Section: Mofs With Enzyme Active Sitesmentioning

confidence: 99%

Bioinspired Framework Catalysts: From Enzyme Immobilization to Biomimetic Catalysis

et al. 2023

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“…S15). Generally, in the degradation of nerve agent and simulants by Zr-MOFs, the hydrolysis products would bind to the Zr 6 node through two adjacent Zr-oxo bonds, which in turn leads to a distinct change in the chemical environment around Zr [25,48,49]. Based on the obtained results above, we thus infer that in this study Zr may be not involved in the catalytic degradation of POX.…”

Section: Resultsmentioning

confidence: 64%

“…Among them, zirconium-based MOFs (Zr-MOFs) have been demonstrated to be highly effective due to the Zr 6 -based nodes analogous to the active sites in phosphotriesterase [11][12][13]. Generally, there are two main approaches to improve the catalytic activity of Zr-MOFs: engineering more defective sites on the Zr 6 node [14-18], and functionalizing the organic linkers of MOFs [19][20][21][22][23][24][25]. Although great success has been achieved by these two approaches, they usually encountered the complexity in design and synthesis, especially when polyaromatic compounds were utilized as the multitopic ligands [20,21,26].…”

Section: Introductionmentioning

confidence: 99%

Single copper sites dispersed on metal-organic frameworks boost the degradation of nerve agent simulants

Cai

Chen

et al. 2023

Sci. China Mater.

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The detoxification of nerve agents, a class of extremely toxic chemical warfare agents, is urgently needed because they have remained a threat to humanity. To date, zirconium-based metal-organic frameworks (Zr-MOFs) are the most popular catalysts in this realm. However, it is still essential to develop new and efficient catalysts based on Zr-MOFs to achieve more rapid hydrolysis. Herein, we report that the single-atom catalyst (SAC) with Cu single atoms on a UiO-66-NH 2 support (Cu@UiO-66-NH 2 ) could significantly boost the degradation of the nerve agent simulant. Compared with the pristine UiO-66-NH 2 , this SAC exhibited remarkable catalytic activity with a half-life for hydrolysis of ~2 min and better reusability in cyclic experiments. Both experimental and theoretical studies suggest that the atomically dispersed Cu species anchored to the amino groups rather than to the Zr 6 node of UiO-66-NH 2 acted as the catalytic active sites, leading to favorable binding geometries with the substrate and the product. A catalytic mechanism on the SAC different from that generally considered on the pristine Zr-MOFs was thus presented to elucidate the enhanced catalytic efficiency.

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“…Diethyl chlorophosphate (DCP) is a less toxic sarin (GB) simulant that shows similar reactivity and is used as a model compound belonging to organophosphates (OPs) . There were various available methods explored for the detection of CWAs such as fluorescence-based probes, − hydrogels, carbon nanoparticles, gas chromatography–mass spectrometry (GC–MS), molecular imprinting coupled with lanthanide luminescence, Raman spectrometers, metal organic framework (MOF), − paper-strip based detection, chemoresistors, colorimetric, , polymer based detection, , and optical waveguide sensor . However, a number of drawbacks are associated with each of these techniques, such as restrictions in terms of applicability, nonportability, operational difficulties, and nonspecificity.…”

Section: Introductionmentioning

confidence: 99%

Calix Decorated ZnO Nanohybrid Material Based Smart Portable Electrochemical Device for On-Site Analysis of Diethylchlorophosphate

Kaur,

Bhardwaj,

Singh

et al. 2024

ACS Appl. Nano Mater.

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Chemical warfare agents (CWAs) pose a severe threat to both civilians and military personnel due to their extreme toxicity. The urgent necessity of creating a portable device for rapid on-site quantification of CWAs is evident. This article presents the design and synthesis of a specialized material, calix[4]pyrrole R2 modified zinc oxide nanohybrid material (R2-ZnO), and its utilization in crafting a smart portable electrochemical device (SPED). The detection capability of the R2-ZnO nanohybrid material was evaluated using various electrochemical techniques, specifically targeting the identification of CWAs' mimic compound, diethyl chlorophosphate (DCP). Upon interaction with the R2-ZnO nanohybrid material, DCP gets entrapped within the pyrrolic cavity of the R2-ZnO nanohybrid material and transforms into hydrolyzed, nontoxic compounds, resulting in a significant increase in current intensity. The interaction of DCP with the R2-ZnO nanohybrid material generates a quick response by enhancing the remarkable current density of the material. Surprisingly, when the R2-ZnO nanohybrid material was exposed to other organophosphates, there was no observable change in the current. Additionally, the developed SPED was tailored for the quantification of DCP, demonstrating fast response times within seconds of exposure. This pioneering research offers a promising pathway to develop a cost-effective, portable device for the rapid on-site quantification of hazardous CWAs.

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Visualizing the degradation of nerve agent simulants using functionalized Zr-based MOFs: from solution to hydrogels

Abstract: Visual monitoring of degradation of nerve agent simulants based on switchable fluorescence of UiO-66-NH2 was developed. In the hydrolysis, the decomposition products perturbed the linker-to-cluster charge transfer and stimulated the...

Cited by 11 publications

References 38 publications

Bioinspired Framework Catalysts: From Enzyme Immobilization to Biomimetic Catalysis

Bioinspired Framework Catalysts: From Enzyme Immobilization to Biomimetic Catalysis

Single copper sites dispersed on metal-organic frameworks boost the degradation of nerve agent simulants

Calix Decorated ZnO Nanohybrid Material Based Smart Portable Electrochemical Device for On-Site Analysis of Diethylchlorophosphate

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