Electrochimica Acta, volume 508, pages 145221

Flexible electrodes based on laser-induced graphene as an analytical platform to monitor amoxicillin

Cassiano Cunha De Souza
Mayane Sousa Carvalho
Wallace Burger veríssimo De Oliveira
Thalles Pedrosa Lisboa
Raylla Santos Oliveira
Osmando F Lopes
Rodrigo Alejandro Abarza Muñoz
Maria Auxiliadora Costa Matos
Maria A C Matos
Renato Camargo Matos
Show full list: 11 authors
Publication typeJournal Article
Publication date2024-12-01
scimago Q1
wos Q1
SJR1.159
CiteScore11.3
Impact factor5.5
ISSN00134686, 18733859
Adiraju A., Jalasutram A., Wang J., Tegenkamp C., Kanoun O.
Advanced Materials Interfaces scimago Q1 wos Q2 Open Access
2024-04-09 citations by CoLab: 7 PDF Abstract  
AbstractLaser‐induced graphene (LIG) is a promising technology enabling cost‐effective, scalable, and high surface area 3D‐porous graphene electrodes for electrochemical applications. Nitrate in water bodies is a harmful contaminant to humans and the ecosystems. Its detection by electrochemical sensors is challenging due to the interference from nitrite. Herein, for the first time, a LIG‐based electrochemical sensor modified with electrodeposited silver dendrites (EdAg/LIG) without using surfactants is proposed for the detection of nitrate with tunable selectivity and sensitivity. The modified electrode surface is extensively characterized by spectroscopic and electrochemical methods and the underlying mechanism for the formation of dendrites is substantiated. The developed EdAg dendrites/LIG electrode shows excellent sensing properties for the detection of nitrate at pH 2. The interference with nitrite in acidic media is eliminated by implementing a novel strategy to shift the working pH of the electrode to 7. The achieved sensor properties at both pH values surpass other LIG‐based sensors with limit of detection of 0.46 at pH 2 and 5.53 µm at pH 7. The developed sensor also shows good recovery characteristics in mineral, tap, and groundwater across a wide range of concentrations and also demonstrates good stability under temperature fluctuations and deformations.
Blasques R.V., Camargo J.R., Veloso W.B., Meloni G.N., Fernandes F.A., Germinare B.F., Guterres e Silva L.R., de Siervo A., Paixão T.R., Janegitz B.C.
2024-02-13 citations by CoLab: 3
Farissi S., Zakkariya S., Akhilghosh K.A., Prasanthi T., Muthukumar A., Muthuchamy M.
Chemosphere scimago Q1 wos Q1
2023-12-01 citations by CoLab: 5 Abstract  
Contaminants of emerging concern (CECs) such as antibiotics have become a matter of worry in aquatic environments worldwide. Their presence in the environment has been increasing due to the inability of conventional wastewater and water treatments to annihilate them. Hence, attempts have been made to remove CECs using electrochemical oxidation (EO). Present study employed the low cost, active carbon based graphite sheet electrodes as anode and cathode to oxidize and degrade Amoxicillin (AMOX)- a β-lactum thiazolidine antibiotic. Optimization studies found pH 9, 45 mA cm-2, 81 cm2 electrode surface area, 6 mM electrolyte concentration and 60 min treatment time to be optimal for AMOX removal. Studies with varying concentrations of AMOX (20 mg L-1, 30 mg L-1 and 40 mg L-1) found that increase in concentrations of AMOX require higher current densities and treatment time for better TOC removal. High performance liquid chromatography photo diode array (HPLC-PDA) studies found 94% removal for 40 mg L-1 of AMOX at optimal conditions with 90% COD and 46% TOC removal. High resolution mass spectrometry (HRMS) studies using Ultra performance liquid chromatography-quadrupole time of flight-mass spectrometry (UPLC-Q-ToF-MS) identified major degradation mechanisms to be hydroxylation, β-lactum ring cleavage, breakage of thiazolidine ring chain from the aromatic ring and piperazinyl ring formation. The final byproducts of AMOX oxidation were carboxylic acids.
Lisboa T.P., de Faria L.V., de Oliveira W.B., Oliveira R.S., de Souza C.C., Matos M.A., Dornellas R.M., Matos R.C.
2023-11-04 citations by CoLab: 4 Abstract  
In this work, we are pleased to present for the first time a 3D-printed electrochemical device using a lab-made conductive filament based on graphite (Gr) and polylactic acid (PLA) polymer matrix for the simultaneous detection of amoxicillin (AMX) and paracetamol (PAR). The sensor was properly characterized by scanning electron microscopy (SEM), electrochemical impedance spectroscopy (EIS), and cyclic voltammetry (CV). Compared to the commercial glassy carbon electrode (GCE), the superior performance of the 3D-Gr/PLA electrode was verified with a 3.8-fold more favored charge transfer. A differential pulse voltammetry (DPV) method was proposed providing a linear working range of 4 to 12 μmol L-1 for both analytes and a limit of detection (LOD) of 0.80 and 0.51 μmol L-1 for AMX and PAR, respectively. Additionally, repeatability studies (n = 5, RSD < 5.7%) indicated excellent precision, and recovery percentages ranging from 89 to 109% when applied to synthetic human urine, saliva, and plasma samples, attested to the accuracy of the method. The studies also indicate that the sensor does not suffer significant interference from common substances (antibiotics and biomarkers) present in the biological fluids, which makes it a promising analytical tool considering its low-cost, ease of manufacturing, robustness, and electrochemical performance.
Fiodorov V., Trusovas R., Mockus Z., Ratautas K., Račiukaitis G.
Polymers scimago Q1 wos Q1 Open Access
2023-10-26 citations by CoLab: 6 PDF Abstract  
Our study presents laser-assisted methods to produce conductive graphene layers on the polymer surface. Specimens were treated using two different lasers at ambient and nitrogen atmospheres. A solid-state picosecond laser generating 355 nm, 532 nm, or 1064 nm wavelengths and a CO2 laser generating mid-infrared 10.6 µm wavelength radiation operating in a pulsed regime were used in experiments. Sheet resistance measurements and microscopic analysis of treated sample surfaces were made. The chemical structure of laser-treated surfaces was investigated using Raman spectroscopy, and it showed the formation of high-quality few-layer graphene structures on the PI surface. The intensity ratios I(2D)/I(G) and I(D)/I(G) of samples treated with 1064 nm wavelength in nitrogen atmosphere were 0.81 and 0.46, respectively. After laser treatment, a conductive laser-induced graphene layer with a sheet resistance as low as 5 Ω was formed. Further, copper layers with a thickness of 3–10 µm were deposited on laser-formed graphene using a galvanic plating. The techniques of forming a conductive graphene layer on a polymer surface have a great perspective in many fields, especially in advanced electronic applications to fabricate copper tracks on 3D materials.
Zhang Z., Zhu H., Zhang W., Zhang Z., Lu J., Xu K., Liu Y., Saetang V.
Carbon scimago Q1 wos Q1
2023-10-01 citations by CoLab: 67 Abstract  
Porous graphene, as an emerging carbon nanomaterial, possesses a range of distinctive physical and chemical properties, such as its lightweight nature and high specific surface area. These properties hold great promise for numerous applications in the fields of physics, chemistry, materials science, energy, and information science, among others. Consequently, research and exploration in this area have gained global attention. Nevertheless, the conventional methods for fabricating porous graphene and two-dimensional planar graphene are complex, and obtaining specific patterns with precise graphene areas presents a challenge. In recent years, laser-induced graphene (LIG) has emerged as a promising technology that offers efficient fabrication of graphene and precise control over patterned structures. This technology significantly reduces production costs compared to traditional processing methods. Consequently, scholars have become increasingly interested in LIG and have made numerous efforts to explore its applications in various fields, including energy, information, and environmental sciences. This review systematically compares different synthesis methods of LIG, summarizes and analyzes the effects of laser processing parameters, laser types, precursor materials, process atmospheres, and other factors on the performance of LIG. In addition, the formation mechanism of LIG is discussed over experimental observation and theoretical simulation, and the structure evolution both in micro- and atomic levels are also explored. Furthermore, this review comprehensively covers recent applications of LIG across a wide range of fields, encompassing various sensors, energy devices, environmental protection techniques, and terahertz modulation equipment. Finally, insights are provided into the future directions and trends of this research technology.
Fu L., Zheng Y., Li X., Liu X., Lin C., Karimi-Maleh H.
Molecules scimago Q1 wos Q2 Open Access
2023-09-20 citations by CoLab: 23 PDF Abstract  
Graphene is an emerging nanomaterial increasingly being used in electrochemical biosensing applications owing to its high surface area, excellent conductivity, ease of functionalization, and superior electrocatalytic properties compared to other carbon-based electrodes and nanomaterials, enabling faster electron transfer kinetics and higher sensitivity. Graphene electrochemical biosensors may have the potential to enable the rapid, sensitive, and low-cost detection of cancer biomarkers. This paper reviews early-stage research and proof-of-concept studies on the development of graphene electrochemical biosensors for potential future cancer diagnostic applications. Various graphene synthesis methods are outlined along with common functionalization approaches using polymers, biomolecules, nanomaterials, and synthetic chemistry to facilitate the immobilization of recognition elements and improve performance. Major sensor configurations including graphene field-effect transistors, graphene modified electrodes and nanocomposites, and 3D graphene networks are highlighted along with their principles of operation, advantages, and biosensing capabilities. Strategies for the immobilization of biorecognition elements like antibodies, aptamers, peptides, and DNA/RNA probes onto graphene platforms to impart target specificity are summarized. The use of nanomaterial labels, hybrid nanocomposites with graphene, and chemical modification for signal enhancement are also discussed. Examples are provided to illustrate applications for the sensitive electrochemical detection of a broad range of cancer biomarkers including proteins, circulating tumor cells, DNA mutations, non-coding RNAs like miRNA, metabolites, and glycoproteins. Current challenges and future opportunities are elucidated to guide ongoing efforts towards transitioning graphene biosensors from promising research lab tools into mainstream clinical practice. Continued research addressing issues with reproducibility, stability, selectivity, integration, clinical validation, and regulatory approval could enable wider adoption. Overall, graphene electrochemical biosensors present powerful and versatile platforms for cancer diagnosis at the point of care.
Souza L.K., Silva-Neto H.A., Rocha D.S., de Abreu F.C., Silva A.C., Dantas N.O., Coltro W.K., Garcia P.T.
2023-08-01 citations by CoLab: 7 Abstract  
In this study, we propose the combination of stencil-printed carbon electrodes (SPCE) and a new nanocomposite based on titanium dioxide-cobalt (1.0 w/w %) (TiO2-1%Co) for the analysis of Amoxicillin (AMX) in pharmaceutical samples. The modification process by drop casting approach of the SPCE was performed with TiO2-1%Co and provided an increase in analytical sensitivity. Detailed morphological, structural, and electrochemical characterizations of the electrodes surface were investigated. The results obtained from characterization showed that the TiO2-1%Co nanocrystals were distributed on the surface of the carbon electrode. The detection of AMX (pH 7.0) was performed with square wave voltammetry using optimized conditions and resulted in a satisfactory linear response (R2 = 0.99) in the range of 20 to 150 μmol L−1, and the estimated limits of detection and quantification were 5.8 μmol L−1 and 19.5 μmol L−1, respectively. Repeatability studies (intra-day and inter-day) of modified electrodes revealed relative standard deviation values ranging from 5.8 to 8.1%. The selectivity of the proposed sensor indicated an acceptable interference (lower than 5%). Additionally, the results obtained with TiO2-1%Co/SPCE for real pharmaceutical samples were compared with UV–Vis Spectroscopy, and was possible to infer that the analytical responses were adequate concerning the labeled values, there are no statistical differences between the reference analysis and the proposed electrochemical method with a confidence level of 95%. The modified electrode offered some advantages such as a disposable sensor, low cost, low sample volume, high repeatability, and reproducibility. The proposed combination of SPCE modified with novel TiO2-1%Co nanocrystals is an attractive strategy for AMX analysis.
Matias T.A., Ramos D.L., Faria L.V., de Siervo A., Richter E.M., Muñoz R.A.
Microchimica Acta scimago Q1 wos Q1
2023-07-18 citations by CoLab: 10 Abstract  
A new electrochemical device fabricated by the combination of 3D printing manufacturing and laser-generated graphene sensors is presented. Cell and electrodes were 3D printed by the fused deposition modeling (FDM) technique employing acrylonitrile butadiene styrene filament (insulating material that composes the cell) and conductive filament (lab-made filament based on graphite dispersed into polylactic acid matrix) to obtain reference and auxiliary electrodes. Infrared-laser engraved graphene, also reported as laser-induced graphene (LIG), was produced by laser conversion of a polyimide substrate, which was assembled in the 3D-printed electrochemical cell that enables the analysis of low volumes (50–2000 μL). XPS analysis revealed the formation of nitrogen-doped graphene multilayers that resulted in excellent electrochemical sensing properties toward the detection of atropine (ATR), a substance that was found in beverages to facilitate sexual assault and other criminal acts. Linear range between 5 and 35 μmol L−1, detection limit of 1 μmol L−1, and adequate precision (RSD = 4.7%, n = 10) were achieved using differential-pulse voltammetry. The method was successfully applied to beverage samples with recovery values ranging from 80 to 105%. Interference studies in the presence of species commonly found in beverages confirmed satisfactory selectivity for ATR sensing. The devices proposed are useful portable analytical tools for on-site applications in the forensic scenario.
Karimi-Maleh H., Darabi R., Baghayeri M., Karimi F., Fu L., Rouhi J., Niculina D.E., Gündüz E.S., Dragoi E.N.
2023-07-15 citations by CoLab: 70 Abstract  
Methyl parathion (MP), an organophosphorus insecticide, is commonly used in agricultural products for food preservation and pest control. Due to the severe threat it poses to food safety and the environment, monitoring MP residues has attracted much attention. Traditional spectroscopic and chromatographic methods have been used successfully to analyze MP in a wide range of samples; however, these approaches have several drawbacks, such as requiring specialized equipment, trained technicians, and extensive sample preparation time. Due to these restrictions, there is a growing demand for analysis methods that can reliably and quickly detect MP at trace quantities while also being quick, sensitive, and selective. Electrochemical sensors have emerged over the past few decades as a viable alternative to more time-consuming and laborious analysis methods for detecting MP. However, the performance of electrochemical sensors has been dramatically improved thanks to recent breakthroughs in nanoscience. This study offers an overview of the creation and operation of carbon nanomaterial-based electrochemical sensors (including carbon nanotubes (CNTs), graphene (Gr), and other carbon nanomaterials) to identify MP residues in waters, fruits, and vegetables. A brief discussion of the potential benefits, drawbacks, and future research prospects of MP electrochemical sensors based on carbon nanomaterials is also offered.
Wang L., Li M., Li B., Wang M., Zhao H., Zhao F.
Foods scimago Q1 wos Q1 Open Access
2023-06-06 citations by CoLab: 13 PDF Abstract  
Carbendazim (CBZ) abuse can lead to pesticide residues, which may threaten the environment and human health. In this paper, a portable three-electrode sensor based on laser-induced graphene (LIG) was proposed for the electrochemical detection of CBZ. Compared with the traditional preparation method of graphene, LIG is prepared by exposing the polyimide film to a laser, which is easily produced and patterned. To enhance the sensitivity, platinum nanoparticles (PtNPs) were electrodeposited on the surface of LIG. Under optimal conditions, our prepared sensor (LIG/Pt) has a good linear relationship with CBZ concentration in the range of 1–40 μM, with a low detection limit of 0.67 μM. Further, the sensor shows good recovery rates for the detection of CBZ in wastewater, which provides a fast and reliable method for real-time analysis of CBZ residues in water samples.
Koukouviti E., Soulis D., Economou A., Kokkinos C.
Analytical Chemistry scimago Q1 wos Q1
2023-04-20 citations by CoLab: 10
de Souza C.C., Lisboa T.P., de Oliveira W.B., Abarza Muñoz R.A., Costa Matos M.A., Matos R.C.
Talanta scimago Q1 wos Q1
2023-02-01 citations by CoLab: 14 Abstract  
In this work, it is presented a simple and affordable method for the paper-based electrodes (PBE) manufacturing using a filter paper and conductive ink based on graphite and nail polish. Additionally, the disposable sensors were applied to the best of knowledge, in the first time for the electrochemical monitoring of amoxicillin (AMX) in complex samples as milk, pharmaceutical formulations, and synthetic urine by differential pulse voltammetry (DPV). Under optimized conductive ink composition, the AMX showed excellent electrochemical behavior on PBE surface with oxidation peak potential at +0.69 V (vs Ag|AgCl|KCl (sat.) ) in phosphate buffer solution. Moreover, the proposed method presented a wide linear working range from 29.8 to 126.7 μmol L −1 and adequate detectability (detection limit of 8 μmol L −1 ). The electroanalytical measurements presented excellent precision with relative standard deviation less than 3% and good accuracy for the spiked samples ranging from 90 to 103%. In addition, the sensor did not undergo significant interference toward other commonly evaluated drugs, which demonstrates the potential of these electrodes for implementation in routine analysis and quality control. • Amoxicillin monitoring using paper-based electrode. • An accessible device for amoxicillin determination in milk samples. • Conductive ink based on graphite and nail polish. • Filter paper, an economical platform for sensors manufacturing. • First report of amoxicillin determination on a paper-based electrode.
Ferreira L.M., Silva P.S., Augusto K.K., Gomes-Júnior P.C., Farra S.O., Silva T.A., Fatibello-Filho O., Vicentini F.C.
2022-11-01 citations by CoLab: 26 Abstract  
The outstanding electronic properties of carbon black (CB) and its economic advantages have fueled its application as nanostructured electrode material for the development of new electrochemical sensors and biosensors. CB-based electrochemical sensing devices have been found to exhibit high surface area, fast charge transfer kinetics, and excellent functionalization. In the present work, we set forth a comprehensive review of the recent advances made in the development and application of CB-based electrochemical devices for pharmaceutical and biomedical analyses - from quantitative monitoring of drug formulations to clinical diagnoses - and the underlying challenges and constraints that need to be overcome. We also present a thorough discussion about the strategies and techniques employed in the development of new electrochemical sensing platforms and in the enhancement of their analytical properties and biocompatibility for anchoring active biomolecules, as well as the combination of these sensing devices with other materials aiming at boosting the performance and efficiency of the sensors.
Yarkaeva Y., Maistrenko V., Dymova D., Zagitova L., Nazyrov M.
Electrochimica Acta scimago Q1 wos Q1
2022-11-01 citations by CoLab: 16 Abstract  
• To AMX determination, sensors based on molecular imprinted PANI and PMOA were developed. • PANI and PMOA were obtained through electrochemical polymerization. • The interaction energy of AMX-PMOA complex is greater than AMX-PANI complex. • PMOA based MIP-sensor has a higher sensitivity, selectivity, and lower detection limit. • Proposed MIP-sensors determine AMX in urine and blood plasma with high accuracy. In this work, sensors based on molecular imprinted polyaniline (MIPANI) and poly-2-methoxyaniline (MIPMOA) for amoxicillin (AMX) determination were developed and compared with each other. MIPANI and MIPMOA were deposited on the surface of modified by graphene oxide (GO) glassy carbon electrode (GCE) through electrochemical polymerization using cyclic voltammetry, which was carried out in a 1 M sulfuric acid solution containing the corresponding monomer and amoxicillin as a template, followed by removal of the template. Using a scanning electron microscopy and electrochemical impedance spectroscopy, the morphology and electrochemical properties of the modified surface of GCE were studied. The applying PANI and PMOA on the GCE/GO surface leads to a decrease in [Fe(CN) 6 ] 3-/4− currents. The electron transfer resistance on PMOA sensor (62 ± 4 Ω) is lower than on PANI sensor (71 ± 5 Ω). The areas of the electroactive surface of GCE/GO/PANI and GCE/GO/PMOA are 6.64 ± 0.12 mm 2 and 7.75 ± 0.14 mm 2 , respectively. After the removal of the AMX, the electron transfer rate increases due to the formation of pores in the polymers through which [Fe(CN) 6 ] 3-/4− ions penetrate. Using FTIR spectroscopy, it was shown that amoxicillin is incorporated into both polymer films. In this case, the binding of AMX to PMOA is stronger, which is confirmed by quantum chemical modeling. The optimal conditions for analysis were selected: the number of polymerization cycles was 7, the template concentration was 1 mM, and the pH of the analyzed solution was 7.00. Square wave voltammograms MIPANI and MIPMOA sensors show a pronounced electrooxidation peak, which are linear over the AMX concentration range of 1.0 × 10 −5 – 5.0 × 10 −3 and 5.0 × 10 −6 – 5.0 × 10 −3 M with detection limits of 2.6 × 10 −6 and 6.1 × 10 −7 M, respectively. It is shown that the MIPMOA sensor exhibits higher sensitivity and selectivity to AMX than MIPANI sensor, as well as high accuracy in determining AMX in urine and blood plasma.

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