Ru(III)-Based Metal–Organic Gels: Intrinsic Horseradish and NADH Peroxidase-Mimicking Nanozyme

He, Limin; Li, Yang; Wu, Qingping; Wang, Dong Mei; Li, Chun Mei; Huang, Cheng; Li, Yuan Fang

doi:10.1021/acsami.9b09283

Cited by 60 publications

(29 citation statements)

References 61 publications

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“…Metal–organic gels (MOGs) have emerged as a new type of metal–organic hybrid material, and they can be rapidly built up by straightforward self-assembling from metal ions and organic ligands through metal–ligand interactions and intermolecular forces. − In particular, MOGs can be obtained by a facile and mild strategy (e.g., neutral condition, relatively low reaction temperature, routine solvents, and short reaction time). Due to the well-defined metal–ligand catalytically active sites, high thermal stability, large surface areas, and unique porous structures, MOGs have been widely applied in the fields of adsorption, catalysis, , drug delivery, sensing, − white-light-emitting diodes, and environmental pollution abatement. , Recently, Li’s group employed the silver-based MOG as the solid coreactants to enhance the ECL of Ru(bpy) 3 2+ for DNA assay, with the MOG being used for the loading of Ru(bpy) 3 2+ molecules . In addition, Li’s group synthesized terbium metal–organic gels (TOGs) and employed the cathode ECL emission of TOGs for the detection of tetracycline, with TOGs being used as the luminophor .…”

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confidence: 85%

“…39−41 In particular, MOGs can be obtained by a facile and mild strategy (e.g., neutral condition, relatively low reaction temperature, routine solvents, and short reaction time). Due to the well-defined metal−ligand catalytically active sites, high thermal stability, large surface areas, and unique porous structures, 42 MOGs have been widely applied in the fields of adsorption, 39 catalysis, 43,44 drug delivery, 45 sensing, 46−50 white-light-emitting diodes, 51 and environmental pollution abatement. 52,53 Recently, Li's group employed the silver-based MOG as the solid coreactants to enhance the ECL of Ru(bpy) 3 2+ for DNA assay, with the MOG being used for the loading of Ru(bpy) 3 2+ molecules.…”

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confidence: 99%

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A Host–Guest Interaction-Based and Metal–Organic Gel-Based Biosensor with Aggregation-Induced Electrochemiluminescence Enhancement for Methyltransferase Assay

Cui

Zhao

et al. 2021

Anal. Chem.

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Metal−organic gels (MOGs) are new soft materials with the characteristics of high colloidal stability, superb luminescence properties, and facile synthesis. Herein, we develop for the first time a host−guest interaction-based and MOG-based biosensor with aggregation-induced electrochemiluminescence (ECL) enhancement for M.SssI methyltransferase (M.SssI MTase) assay. This biosensor employs a MOG as the luminophor and potassium persulfate as the coreactant, and the formation of the Ag-MOG from the aggregation of silver nanoclusters can induce significant ECL enhancement. Two complementary single-stranded DNAs (ssDNAs, i.e., biotinylated DNA-1 and Fc-labeled DNA-2) that contain specific recognition sequence 5′-CCGG-3′ can form a double-stranded DNA (dsDNA) probe. In the absence of M.SssI MTase, the dsDNA probe will be digested by restriction endonuclease HpaII, leading to the release of Fc from magnetic beads (MBs). The β-CD can specifically recognize the released Fc through guest−host interaction, resulting in the quenching of an ECL signal. In contrast, the presence of M.SssI MTase enables the formation of fully methylated dsDNA, which cannot be cleaved by HpaII, making Fc remain on the MB surface and consequently generating an improved ECL signal. This biosensor can specifically detect M.SssI MTase with a linear range of 0.05−100 U mL −1 and a limit of detection of 3.5 × 10 −3 U mL −1 , and it enables accurate detection of M.SssI MTase in human serum. In addition, it can be used for inhibitor screening, with wide applications in drug discovery and disease diagnosis.

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confidence: 85%

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confidence: 99%

A Host–Guest Interaction-Based and Metal–Organic Gel-Based Biosensor with Aggregation-Induced Electrochemiluminescence Enhancement for Methyltransferase Assay

Cui

Zhao

et al. 2021

Anal. Chem.

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“…55 In addition to transition metal nodes, noble metal ones can also be used to construct metal−organic structures with catalytic or enzyme-mimicking abilities. 56 For instance, Wang et al successfully synthesized a series of coordinated single-atom (Co, Cu, and Au) metal sites with zirconium porphyrinic hollow MOF nanotubes as the supporting matrix. 57 During the synthesis process, the porphyrin molecule not only serves as the bridging linker but also provides a central coordination environment for anchoring and regulating the electronic properties of single metal atoms.…”

Section: Mof-based Metal Doping Strategymentioning

confidence: 99%

“…In a study reported by Hwang and co-workers, they demonstrated that the binding of aliphatic diamines to unsaturated Fe metal nodes in MIL-100(Fe) can significantly enhance the POD-mimicking catalytic activity of the functionalized MOFs, since the surface with enhanced negative potential could show higher affinity for positively charged TMB . In addition to transition metal nodes, noble metal ones can also be used to construct metal–organic structures with catalytic or enzyme-mimicking abilities . For instance, Wang et al successfully synthesized a series of coordinated single-atom (Co, Cu, and Au) metal sites with zirconium porphyrinic hollow MOF nanotubes as the supporting matrix .…”

Section: Mof-based Metal Doping Strategymentioning

confidence: 99%

Metal–Organic Framework Derived Nanozymes in Biomedicine

2020

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Nanozymes that integrate the advantages of both nanomaterials and natural enzymes have accumulated enormous research interest over the past decades because of the opportunity it provides to appreciate and further cultivate artificial enzymes with comparable property. By mimicking the coordination environments of the catalytic sites in natural enzymes, nanozymes with confined nanostructures can serve as substitutes for many catalytic processes with comparable activity and robust stability even in harsh conditions. Since the pioneered report about peroxidase-mimicking ferromagnetic nanoparticles in 2007, the nanozymes are specialized for nanomaterials with intrinsic enzyme-mimicking property. With the rapid development in nanoscience and nanotechnology, nanomaterials with superior advantages such as large-scale production, desired activity, and robust stability can bridge the natural enzymes with nanozymes.Metal-organic frameworks (MOFs) and their derivatives hold a great promise to serve as direct surrogates of conventional enzymes for enzymatic reactions. According to the chemical nature, MOF-based nanozymes can be divided into three main categories: pristine MOFs, enzyme-encapsulated MOF composites, and MOF-based derivatives. Due to the versatility of metallic nodes and bridging linkers together with the feasibility of post-synthetic engineering and modification, MOFs and their derivatives are envisioned as one of the most appropriate surrogates for this purpose. Using MOFs as precursors or sacrificial templates, multiple MOF-based derivatives including carbon-based nanomaterials (e.g., heteroatom-doped carbon or carbon with M-N-C moiety), metal oxide/carbon nanoparticles, and metal/carbon nanomaterials can be rationally synthesized through one-step direct carbonization/oxidation or indirect post-treatments of MOFs (e.g., bridging linker-exchange and metallic node-doping). Compared with the existing nanozymes, MOF-based derivatives open up a new avenue for constructing mesoporous nanozymes. In this way, the intrinsic mesoporous property of MOFs can still be maintained, while the stability and activity can be largely improved. In this Account, we highlight some important research advances in MOF-based derivatives (including M-N-C moiety (M = single metal atom), metal oxide/carbon, metal/carbon, and MOF derivatives obtained through post-synthetic linker exchange and metal doping strategies) with enzyme-mimicking activity. We also portray that, through integrating physicochemical properties of mesoporous nanomaterials and enzymatic activities of natural enzymes, MOF-derived nanozymes can provide multifunctional platforms in biomedical community such as anti-bacteria, biosensor, imaging, cancer therapy, and environmental protection. Finally, we propose future design principles and possible research approaches for deeper understanding of mechanisms, thus pointing out future research directions to offer more opportunities for conventional enzyme-engineering industry.

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“…Metal-organic gels combine the advantages of stimuli-response of physical gels (weak non-covalent interactions) and stability of chemical gels (strong chemical bonds). [1][2][3][4] Metal-organic gels have found applications in various elds such as sensing, [5][6][7][8][9][10] catalysis, [11][12][13][14] environmental remediation, 15,16 renewable energy conversion, [17][18][19] and templates for nanomaterials. 20 Metalorganic framework (MOF)-based gels are particularly interesting because they incorporate MOF nanoparticles with well-dened microporosity in their gel matrix.…”

Section: Introductionmentioning

confidence: 99%