Miniaturized Electrochemiluminescence Platform With Laser-Induced Graphene-Based Single Electrode for Interference-Free Sensing of Dopamine, Xanthine, and Glucose

Electrochemiluminescence (ECL) plays a vital role in the development of point-of-care testing (POCT) devices. Conventional electrochemical and bipolar electrochemical-based ECL systems are time-consuming, expensive, and required more fabrication steps. To eliminate such challenges, in this work, for the first time, novel laser-induced graphene (LIG)-based single electrode (SE) system has been developed, and its application in enzymeless ECL detection of multiple analytes has been validated. SEs were fabricated over polyimide (PI) substrate by directing CO<sub>2</sub> laser leading to the creation of graphene over PI in a single step by optimizing the speed and power of the laser. Android smartphone was effectively used to provide dual functioning such as capturing the ECL image and driving the LIG-SE-ECL sensor. With optimized parameters, determination of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>), D-glucose (G), xanthine (X), and dopamine (D) was carried in the linear range from 0.1 to <inline-formula> <tex-math notation="LaTeX">$70~\mu \text{M}$ </tex-math></inline-formula>, 0.1 to <inline-formula> <tex-math notation="LaTeX">$70~\mu \text{M}$ </tex-math></inline-formula>, 0.1 to <inline-formula> <tex-math notation="LaTeX">$100~\mu \text{M}$ </tex-math></inline-formula>, and 0.1 to <inline-formula> <tex-math notation="LaTeX">$100~\mu \text{M}$ </tex-math></inline-formula>, with a limit of detection (LOD) 1.71, 3.76, 1.25, and <inline-formula> <tex-math notation="LaTeX">$3.40~\mu \text{M}$ </tex-math></inline-formula>, respectively. An interference study was performed and it was observed that LIG-SE-ECL device showed effective selectivity for different analytes with their respective voltages. The developed miniaturised, low-cost ECL platform can be suitably used in many diverse applications such as POCT, environmental monitoring, and multiple biomedical applications.

[1]  J. Tour,et al.  Laser-induced porous graphene films from commercial polymers , 2014, Nature Communications.

[2]  Moon-Sik Kang,et al.  Miniaturized ECL detection system for glucose biosensor , 2005, 2005 3rd IEEE/EMBS Special Topic Conference on Microtechnology in Medicine and Biology.

[3]  Chen-Zhong Li,et al.  Membraneless enzymatic biofuel cells based on graphene nanosheets. , 2010, Biosensors & bioelectronics.

[4]  Guobao Xu,et al.  A portable wireless single-electrode system for electrochemiluminescent analysis , 2019, Electrochimica Acta.

[5]  Y. Ying,et al.  Evaluation of trans-resveratrol level in grape wine using laser-induced porous graphene-based electrochemical sensor. , 2020, The Science of the total environment.

[6]  Chunsun Zhang,et al.  A low-cost, ultraflexible cloth-based microfluidic device for wireless electrochemiluminescence application. , 2016, Lab on a chip.

[7]  Dan Wang,et al.  A novel paperfluidic closed bipolar electrode-electrochemiluminescence sensing platform: Potential for multiplex detection at crossing-channel closed bipolar electrodes , 2018, Sensors and Actuators B: Chemical.

[8]  M. V. Gorbunova,et al.  A Monitor Calibrator as a Portable Tool for Determination of Luminescent Compounds , 2021, IEEE Transactions on Instrumentation and Measurement.

[9]  Chunsun Zhang,et al.  Battery-triggered open wireless electrochemiluminescence in a microfluidic cloth-based bipolar device , 2017 .

[10]  S. Garcia-Manyes,et al.  Steering chemical reactions with force , 2017 .

[11]  Guobao Xu,et al.  A single-electrode electrochemical system for multiplex electrochemiluminescence analysis based on a resistance induced potential difference† †Electronic supplementary information (ESI) available. See DOI: 10.1039/c8sc00410b , 2018, Chemical science.

[12]  Guonan Chen,et al.  An ECL biosensor for glucose based on carbon-nanotube/Nafion film modified glass carbon electrode , 2008 .

[13]  S. Goel,et al.  Miniaturized polymeric enzymatic biofuel cell with integrated microfluidic device and enhanced laser ablated bioelectrodes , 2020 .

[14]  Da Xing,et al.  Paper-based bipolar electrode-electrochemiluminescence (BPE-ECL) device with battery energy supply and smartphone read-out: A handheld ECL system for biochemical analysis at the point-of-care level , 2016 .

[15]  Zahra Abedi,et al.  A highly sensitive electrochemical sensor for simultaneous detection of uric acid, xanthine and hypoxanthine based on poly(l-methionine) modified glassy carbon electrode , 2013 .

[16]  Michael B. Ross,et al.  Efficient hydrogen peroxide generation using reduced graphene oxide-based oxygen reduction electrocatalysts , 2018, Nature Catalysis.

[17]  A. Mohamed,et al.  Effect of voltage applied for graphene oxide/latex nanocomposites produced via electrochemical exfoliation and its application as conductive electrodes , 2020 .

[18]  Vijay Srinivasan,et al.  Development of a digital microfluidic platform for point of care testing. , 2008, Lab on a chip.

[19]  S. Goel,et al.  Miniaturized Electrochemiluminescence Platform With Laser-Induced Graphene Electrodes for Multiple Biosensing , 2020, IEEE Transactions on NanoBioscience.

[20]  Min Liu,et al.  Open bipolar electrode-electrochemiluminescence imaging sensing using paper-based microfluidics , 2015 .

[21]  Guobao Xu,et al.  Applications and trends in electrochemiluminescence. , 2010, Chemical Society reviews.

[22]  A. Javed,et al.  Highly Selective Electrochemical Sensing of Dopamine, Xanthine, Ascorbic Acid and Uric Acid Using a Carbon Fiber Paper , 2020, IEEE Sensors Journal.

[23]  Sanket Goel,et al.  3-D Printed Integrated and Automated Electro-Microfluidic Viscometer for Biochemical Applications , 2019, IEEE Transactions on Instrumentation and Measurement.

[24]  Loïc J Blum,et al.  Electro-chemiluminescent biosensing , 2008, Analytical and bioanalytical chemistry.

[25]  Richard M Crooks,et al.  Bipolar electrochemistry. , 2013, Angewandte Chemie.

[26]  Sanket Goel,et al.  PDMS-Based Microfluidic Glucose Biofuel Cell Integrated With Optimized Laser-Induced Flexible Graphene Bioelectrodes , 2020, IEEE Transactions on Electron Devices.

[27]  S. Puneeth,et al.  Laser-Induced Flexible Electronics (LIFE) for Resistive, Capacitive and Electrochemical Sensing Applications , 2020, IEEE Sensors Journal.

[28]  Austin C. Faucett Voltage-induced reduction of graphene oxide , 2016 .

[29]  S. Goel,et al.  A Portable 3-D Printed Electrochemiluminescence Platform With Pencil Graphite Electrodes for Point-of-Care Multiplexed Analysis With Smartphone-Based Read Out , 2021, IEEE Transactions on Instrumentation and Measurement.

[30]  Lauro T. Kubota,et al.  Electrochemical Biosensors in Point‐of‐Care Devices: Recent Advances and Future Trends , 2017 .

[31]  Yi Xiao,et al.  Electrochemiluminescence bipolar electrode array for the multiplexed detection of glucose, lactate and choline based on a versatile enzymatic approach. , 2017, Talanta.