Catalytic Modification of Porous Two-Dimensional Ni-MOFs on Portable Electrochemical Paper-Based Sensors for Glucose and Hydrogen Peroxide Detection

Rapid and accurate detection of changes in glucose (Glu) and hydrogen peroxide (H2O2) concentrations is essential for the predictive diagnosis of diseases. Electrochemical biosensors exhibiting high sensitivity, reliable selectivity, and rapid response provide an advantageous and promising solution. A porous two-dimensional conductive metal–organic framework (cMOF), Ni-HHTP (HHTP = 2,3,6,7,10,11-hexahydroxytriphenylene), was prepared by using a one-pot method. Subsequently, it was employed to construct enzyme-free paper-based electrochemical sensors by applying mass-producing screen-printing and inkjet-printing techniques. These sensors effectively determined Glu and H2O2 concentrations, achieving low limits of detection of 1.30 μM and 2.13 μM, and high sensitivities of 5573.21 μA μM−1 cm−2 and 179.85 μA μM−1 cm−2, respectively. More importantly, the Ni-HHTP-based electrochemical sensors showed an ability to analyze real biological samples by successfully distinguishing human serum from artificial sweat samples. This work provides a new perspective for the use of cMOFs in the field of enzyme-free electrochemical sensing, highlighting their potential for future applications in the design and development of new multifunctional and high-performance flexible electronic sensors.

[1]  Jie Wu,et al.  Device integration of electrochemical biosensors , 2023, Nature Reviews Bioengineering.

[2]  Xiao He,et al.  Conductive Metal-Organic Framework Microelectrodes Regulated by Conjugated Molecular Wires for Monitoring of Dopamine in the Mouse Brain. , 2023, Journal of the American Chemical Society.

[3]  Shanli Liu,et al.  Minimally invasive electrochemical continuous glucose monitoring sensors: Recent progress and perspective. , 2023, Biosensors & bioelectronics.

[4]  Kuldeep Mahato,et al.  Wearable chemical sensors for biomarker discovery in the omics era , 2022, Nature Reviews Chemistry.

[5]  Ankur Gupta,et al.  A Chemometric-Assisted Colorimetric-Based Inexpensive Paper Biosensor for Glucose Detection , 2022, Biosensors.

[6]  Sanghyuk Yoon,et al.  A Nanoporous Carbon‐MXene Heterostructured Nanocomposite‐Based Epidermal Patch for Real‐Time Biopotentials and Sweat Glucose Monitoring , 2022, Advanced Functional Materials.

[7]  M. Ajmal,et al.  A Multicomponent Polymer-Metal-Enzyme System as Electrochemical Biosensor for H2O2 Detection , 2022, Frontiers in Chemistry.

[8]  Qin Xu,et al.  A highly flexible Ni-Co MOF nanosheet coated Au/PDMS film based wearable electrochemical sensor for continuous human sweat glucose monitoring. , 2022, The Analyst.

[9]  Chengyi Hou,et al.  A portable ascorbic acid in sweat analysis system based on highly crystalline conductive nickel-based metal-organic framework (Ni-MOF). , 2022, Journal of colloid and interface science.

[10]  Bor-Ran Li,et al.  Wearable hydrogel patch with noninvasive, electrochemical glucose sensor for natural sweat detection. , 2022, Talanta.

[11]  Huan-bao Fa,et al.  Bimetal-organic frameworks MnCo-MOF-74 derived Co/MnO@HC for the construction of a novel enzyme-free glucose sensor , 2021, Microchemical Journal.

[12]  Haidong Yu,et al.  Optical/electrochemical methods for detecting mitochondrial energy metabolism. , 2021, Chemical Society reviews.

[13]  Jinping Xiong,et al.  Fabrication of Co3O4/NiCo2O4 Nanocomposite for Detection of H2O2 and Dopamine , 2021, Biosensors.

[14]  F. Huo,et al.  Wearable Sweat Biosensors Refresh Personalized Health/Medical Diagnostics , 2021, Research.

[15]  Hossein Kazemian,et al.  A new nickel metal organic framework (Ni-MOF) porous nanostructure as a potential novel electrochemical sensor for detecting glucose , 2021, Journal of Porous Materials.

[16]  Siyuan Zhang,et al.  Cu-MOF/hemin: a bionic enzyme with excellent dispersity for the determination of hydrogen peroxide released from living cells. , 2021, The Analyst.

[17]  O. Chailapakul,et al.  A non-enzymatic disposable electrochemical sensor based on surface-modified screen-printed electrode CuO-IL/rGO nanocomposite for a single-step determination of glucose in human urine and electrolyte drinks. , 2021, Analytical methods : advancing methods and applications.

[18]  Xiaoya Liu,et al.  An Enzyme‐free Electrochemical H 2 O 2 Sensor Based on a Nickel Metal‐organic Framework Nanosheet Array , 2021, Electroanalysis.

[19]  J. Sempionatto,et al.  Touch‐Based Stressless Cortisol Sensing , 2021, Advanced materials.

[20]  Fei Xiao,et al.  Green and controllable synthesis of multi-heteroatoms co-doped graphene fiber as flexible and biocompatible microelectrode for in situ electrochemical detection of biological samples , 2021 .

[21]  Xueliang Li,et al.  Recent development and applications of electrical conductive MOFs. , 2021, Nanoscale.

[22]  Y. Luan,et al.  Cu-MOF chemodynamic nanoplatform via modulating glutathione and H2O2 in tumor microenvironment for amplified cancer therapy. , 2020, Journal of colloid and interface science.

[23]  Bin Qiu,et al.  In situ deposition of MOF-74(Cu) nanosheet arrays onto carbon cloth to fabricate a sensitive and selective electrocatalytic biosensor and its application for the determination of glucose in human serum , 2020, Microchimica Acta.

[24]  Chengyi Hou,et al.  A highly integrated sensing paper for wearable electrochemical sweat analysis. , 2020, Biosensors & bioelectronics.

[25]  Tingshuai Li,et al.  Electrochemical non-enzymatic glucose sensors: recent progress and perspectives. , 2020, Chemical communications.

[26]  Antara Vaidyanathan,et al.  Flexible and wearable electrochemical biosensors based on two-dimensional materials: Recent developments , 2020, Analytical and Bioanalytical Chemistry.

[27]  B. Smit,et al.  Charge Separation and Charge Carrier Mobility in Photocatalytic Metal‐Organic Frameworks , 2020, Advanced Functional Materials.

[28]  S. A. John,et al.  Tunable electrochemical synthesis of 3D nucleated microparticles like Cu-BTC MOF-carbon nanotubes composite: Enzyme free ultrasensitive determination of glucose in a complex biological fluid , 2020 .

[29]  T. Fujiwara,et al.  Glucose Fluctuation and Cardiovascular Diseases. , 2020, International heart journal.

[30]  Paloma Yáñez-Sedeño,et al.  Screen-Printed Electrodes: Promising Paper and Wearable Transducers for (Bio)Sensing , 2020, Biosensors.

[31]  Siyu Lu,et al.  High-performance non-enzymatic glucose detection: using a conductive Ni-MOF as an electrocatalyst. , 2020, Journal of materials chemistry. B.

[32]  K. Mirica,et al.  Employing Conductive Metal-Organic Frameworks for Voltammetric Detection of Neurochemicals. , 2020, Journal of the American Chemical Society.

[33]  Yucui Jiao,et al.  3D vertical-flow paper-based device for simultaneous detection of multiple cancer biomarkers by fluorescent immunoassay , 2020 .

[34]  Yichun Liu,et al.  Photothermal-enhanced tandem enzyme-like activity of Ag2-xCuxS nanoparticles for one-step colorimetric glucose detection in unprocessed human urine , 2020 .

[35]  E. Kavak,et al.  Synthesis of Ferrocene Based Naphthoquinones and its Application as Novel Non‐enzymatic Hydrogen Peroxide , 2020 .

[36]  Qihua Zhao,et al.  High-performance non-enzymatic glucose electrochemical sensor constructed by transition nickel modified Ni@Cu-MOF , 2020 .

[37]  B. Hemmateenejad,et al.  Dendrite gold nanostructures electrodeposited on paper fibers: Application to electrochemical non-enzymatic determination of glucose , 2020 .

[38]  Orawon Chailapakul,et al.  A copper oxide-ionic liquid/reduced graphene oxide composite sensor enabled by digital dispensing: Non-enzymatic paper-based microfluidic determination of creatinine in human blood serum. , 2019, Analytica chimica acta.

[39]  Tuomas Happonen,et al.  Regional and correlative sweat analysis using high-throughput microfluidic sensing patches toward decoding sweat , 2019, Science Advances.

[40]  Y. Xing,et al.  AuPt/MOF-Graphene: A Synergistic Catalyst with Surprisingly High Peroxidase-Like Activity and its Application for H2O2 Detection. , 2019, Analytical chemistry.

[41]  Haidong Yu,et al.  Two-component ratiometric sensor for Cu2+ detection on paper-based device , 2019, Analytical and Bioanalytical Chemistry.

[42]  C. Chen,et al.  Conductive MOF-Modified Separator for Mitigating the Shuttle Effect of Lithium-Sulfur Battery through a Filtration Method. , 2019, ACS applied materials & interfaces.

[43]  Run‐Wei Li,et al.  Intrinsically Stretchable Resistive Switching Memory Enabled by Combining a Liquid Metal–Based Soft Electrode and a Metal–Organic Framework Insulator , 2018, Advanced Electronic Materials.

[44]  B. Ye,et al.  An efficient electrochemical glucose sensor based on porous nickel-based metal organic framework/carbon nanotubes composite (Ni-MOF/CNTs) , 2018, Journal of Alloys and Compounds.

[45]  Jesús de Vicente,et al.  On the Determination of Uncertainty and Limit of Detection in Label-Free Biosensors , 2018, Sensors.

[46]  Hanjie Wang,et al.  Materials and Techniques for Implantable Nutrient Sensing Using Flexible Sensors Integrated with Metal–Organic Frameworks , 2018, Advanced materials.

[47]  Jian Tang,et al.  Layered assembly of NiMn-layered double hydroxide on graphene oxide for enhanced non-enzymatic sugars and hydrogen peroxide detection , 2018 .

[48]  Wei Chen,et al.  ZIF-67 derived porous Co3O4 hollow nanopolyhedron functionalized solution-gated graphene transistors for simultaneous detection of glucose and uric acid in tears. , 2018, Biosensors & bioelectronics.

[49]  Gang Xu,et al.  Layer-by-Layer Assembled Conductive Metal-Organic Framework Nanofilms for Room-Temperature Chemiresistive Sensing. , 2017, Angewandte Chemie.

[50]  Guangyu Zhao,et al.  Ni-Based metal–organic framework derived Ni@C nanosheets on a Ni foam substrate as a supersensitive non-enzymatic glucose sensor , 2017 .

[51]  Hui-yun Sun,et al.  Sugar-Breathing Glycopolymersomes for Regulating Glucose Level. , 2017, Journal of the American Chemical Society.

[52]  Guoan Zhang,et al.  Metal oxide intercalated layered double hydroxide nanosphere: With enhanced electrocatalyic activity towards H2O2 for biological applications , 2017 .

[53]  N. Wang,et al.  Amperometric cholesterol biosensor based on zinc oxide films on a silver nanowire–graphene oxide modified electrode , 2016 .

[54]  Hua Zhang Ultrathin Two-Dimensional Nanomaterials. , 2015, ACS nano.

[55]  Weisheng Liu,et al.  An electrochemical sensor for H2O2 based on a new Co-metal-organic framework modified electrode , 2015 .

[56]  Cailing Xu,et al.  Pt@UiO-66 heterostructures for highly selective detection of hydrogen peroxide with an extended linear range. , 2015, Analytical chemistry.

[57]  Nathan Efron,et al.  Biometry of eyes in type 1 diabetes. , 2015, Biomedical optics express.

[58]  Hua Li,et al.  A highly sensitive non-enzymatic glucose sensor based on bimetallic Cu-Ag superstructures. , 2015, Biosensors & bioelectronics.

[59]  Shuhua Zhu,et al.  Simultaneous separation and determination of fructose, sorbitol, glucose and sucrose in fruits by HPLC-ELSD. , 2014, Food chemistry.

[60]  Bruce Dunn,et al.  New Porous Crystals of Extended Metal-Catecholates , 2012 .

[61]  Hongcai Gao,et al.  Coating graphene paper with 2D-assembly of electrocatalytic nanoparticles: a modular approach toward high-performance flexible electrodes. , 2012, ACS nano.

[62]  Shoji Takeuchi,et al.  Injectable hydrogel microbeads for fluorescence-based in vivo continuous glucose monitoring , 2010, Proceedings of the National Academy of Sciences.

[63]  Probal Banerjee,et al.  Glucose-mediated assembly of phenylboronic acid modified CdTe/ZnTe/ZnS quantum dots for intracellular glucose probing. , 2010, Angewandte Chemie.

[64]  G. Whitesides,et al.  Simple telemedicine for developing regions: camera phones and paper-based microfluidic devices for real-time, off-site diagnosis. , 2008, Analytical chemistry.

[65]  G. Whitesides,et al.  Patterned paper as a platform for inexpensive, low-volume, portable bioassays. , 2007, Angewandte Chemie.

[66]  J. Stone,et al.  Hydrogen peroxide: a signaling messenger. , 2006, Antioxidants & redox signaling.

[67]  H. Elias,et al.  Reactive Peroxo Compounds Generated in Situ from Hydrogen Peroxide: Kinetics and Catalytic Application in Oxidation Processes , 2005 .

[68]  Ming Liu,et al.  Recent Progress in Metal-Organic Frameworks (MOFs) for Electrocatalysis , 2023, Industrial Chemistry & Materials.

[69]  Xuewen Shi,et al.  Paper-Based Sensors for Diagnostics, Human Activity Monitoring, Food Safety and Environmental Detection , 2022, Sensors & Diagnostics.

[70]  Fuxiang Chen,et al.  Engineering the modulation of active sites and pores of pristine metal-organic frameworks for high-performance sodium-ion storage , 2022, Inorganic Chemistry Frontiers.

[71]  Christopher,et al.  Diabetes and Cardiovascular Disease Outcomes in theMetabolically Healthy Obese Phenotype A cohort study , 2015 .

[72]  Weihua Tang,et al.  Bimetallic PdCu nanoparticle decorated three-dimensional graphene hydrogel for non-enzymatic amperometric glucose sensor , 2014 .

[73]  张中新 Dendritic Bimetallic Nanostructures Supported on Self-Assembled Titanate Films for Sensor Application , 2010 .