Coating a DNA self-assembled monolayer with a metal organic framework-based exoskeleton for improved sensing performance

Ma, Jianhua; Chai, Wenxin; Lu, Jui‐Han; Tian, Tian; Yang, Yucai; Yang, Jie; Li, Chao; Li, Genxi

doi:10.1039/c9an00084d

Cited by 6 publications

(4 citation statements)

References 40 publications

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“…To date, four mechanisms have been proposed to underly the degradation of EAB sensors in complex biological fluids: (1) desorption of the alkane-thiolate SAM from the surface of the gold electrode; − (2) irreversible redox reactions degrading the redox reporter; (3) enzymatic degradation of the DNA; , and (4) fouling from interferents, such as blood cells and proteins, adsorbing to the sensor surface. − The relative contributions of each of these mechanisms to EAB sensor degradation and drift, however, have not yet been defined, rendering it difficult to develop rational approaches to their remediation. To address this, here we have characterized the relative contributions of each of these mechanisms to the degradation of a simple, EAB-like proxy when exposed in vitro to undiluted whole blood at 37 °C as a straightforward and easily reproducible mimic of in vivo conditions.…”

Section: Resultsmentioning

confidence: 99%

Elucidating the Mechanisms Underlying the Signal Drift of Electrochemical Aptamer-Based Sensors in Whole Blood

et al. 2021

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The ability to monitor drugs, metabolites, hormones, and other biomarkers in situ in the body would greatly advance both clinical practice and biomedical research. To this end, we are developing electrochemical aptamer-based (EAB) sensors, a platform technology able to perform real-time, in vivo monitoring of specific molecules irrespective of their chemical or enzymatic reactivity. An important obstacle to the deployment of EAB sensors in the challenging environments found in the living body is signal drift, whereby the sensor signal decreases over time. To date, we have demonstrated a number of approaches by which this drift can be corrected sufficiently well to achieve good measurement precision over multihour in vivo deployments. To achieve a much longer in vivo measurement duration, however, will likely require that we understand and address the sources of this effect. In response, here, we have systematically examined the mechanisms underlying the drift seen when EAB sensors and simpler, EAB-like devices are challenged in vitro at 37 °C in whole blood as a proxy for in vivo conditions. Our results demonstrate that electrochemically driven desorption of a self-assembled monolayer and fouling by blood components are the two primary sources of signal loss under these conditions, suggesting targeted approaches to remediating this degradation and thus improving the stability of EAB sensors and other, similar electrochemical biosensor technologies when deployed in the body.

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Section: Resultsmentioning

confidence: 99%

Elucidating the Mechanisms Underlying the Signal Drift of Electrochemical Aptamer-Based Sensors in Whole Blood

et al. 2021

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“…The interaction between Au and thiolated molecules allows DNA probes to grow on the Au electrode surface, forming DNA self-assembled monolayers (SAMs) that are sensitive but show low stability as a sensing element. To compensate for the stability deficiency, zeolitic imidazolate framework-8 (ZIF-8) was grown on an electrode surface modified with DNA SAMs, forming a favorable barrier outside the nanoprobe ( Ma et al, 2019 ). Such MOF–biomolecule integration strategies reduce the activity loss of sensing materials during assembly, storage, transportation, and inspection operations, which have advanced their dissemination.…”

Section: Synthesis and Modification Of Mofs For Electroactive Materialsmentioning

confidence: 99%

Recent Advances in Metal-Organic Framework-Based Electrochemical Biosensing Applications

Li¹,

Zhang²,

Boakye³

et al. 2021

Front. Bioeng. Biotechnol.

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In the face of complex environments, considerable effort has been made to accomplish sensitive, accurate and highly-effective detection of target analytes. Given the versatility of metal clusters and ligands, high porosity and large specific surface area, metal–organic framework (MOF) provides researchers with prospective solutions for the construction of biosensing platforms. Combined with the benefits of electrochemistry method such as fast response, low cost and simple operation, the untapped applications of MOF for biosensors are worthy to be exploited. Therefore, this review briefly summarizes the preparation methods of electroactive MOF, including synthesize with electroactive ligands/metal ions, functionalization of MOF with biomolecules and modification for MOF composites. Moreover, recent biosensing applications are highlighted in terms of small biomolecules, biomacromolecules, and pathogenic cells. We conclude with a discussion of future challenges and prospects in the field. It aims to offer researchers inspiration to address the issues appropriately in further investigations.

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“…Then, the electrodes are incubated in the zeolitic imidazolate framework (ZIF-8) precursors (i.e., ZnAc and 2-methylimidazolate (2-mIm)) to stimulate the in situ self-growth of MOF nanostructures. The DNA molecules on the electrode are encapsulated in the ZIF-8 nanoparticles, and consequently, methylene blue (MB)-labeled DNA molecules cannot collide with the underlying electrode, thus diminishing the electrochemical signal . Meanwhile, the resulting electrodes can collect exosomes in the biofluids directly via the strong electrostatic and coordination interactions between ZIF-8 nanoparticles and exosomes.…”

Section: Resultsmentioning

confidence: 99%

“…The DNA molecules on the electrode are encapsulated in the ZIF-8 nanoparticles, and consequently, methylene blue (MB)-labeled DNA molecules cannot collide with the underlying electrode, thus diminishing the electrochemical signal. 17 Meanwhile, the resulting electrodes can collect exosomes in the biofluids directly via the strong electrostatic and coordination interactions between ZIF-8 nanoparticles and exosomes.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Precise Molecular Profiling of Circulating Exosomes Using a Metal–Organic Framework-Based Sensing Interface and an Enzyme-Based Electrochemical Logic Platform

Wang

Gui

et al. 2022

Anal. Chem.

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Exosomes have emerged as a promising circulating tumor biomarker; however, it is a big challenge for convenient, multiparametric, and accurate profiling of tumorous exosomes due to their unique structure and heterogeneity. To address these problems, we develop a highly integrated electrochemical platform for molecular profiling of tumor exosomes. A metal–organic framework-functionalized sensing interface is fabricated through a simple self-growth process, which collects exosomes from biofluids without additional separation steps. Meanwhile, a sensing strategy is designed to analyze both exosomal protein and RNA markers on a single chip based on the unique sensor architecture, allowing detection of low-abundance targets (∼250 vesicles in a 10 μL sample) using an integrated microfluidic electrochemical device. Furthermore, a multiple-input, protein enzyme-based logic gate is introduced into the system to accurately identify breast cancer patients with 100% sensitivity and specificity, thus revealing the advantageous role of logical profiling of exosomes in early diagnostics of tumor.

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Coating a DNA self-assembled monolayer with a metal organic framework-based exoskeleton for improved sensing performance

Abstract: The relatively poor stability of DNA self-assembled monolayers (SAMs) greatly limits their use in real applications. A new strategy is reported to protect the DNA SAMs by using a metal organic framework (MOF)-based exoskeleton.

Cited by 6 publications

References 40 publications

Elucidating the Mechanisms Underlying the Signal Drift of Electrochemical Aptamer-Based Sensors in Whole Blood

Elucidating the Mechanisms Underlying the Signal Drift of Electrochemical Aptamer-Based Sensors in Whole Blood

Recent Advances in Metal-Organic Framework-Based Electrochemical Biosensing Applications

Precise Molecular Profiling of Circulating Exosomes Using a Metal–Organic Framework-Based Sensing Interface and an Enzyme-Based Electrochemical Logic Platform

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