Development, fabrication, and applications of laser-induced graphene-based biosensors in food and dairy sectors

Abstract

Laser-induced graphene (LIG) has emerged as a cutting-edge carbon material with a unique porous architecture and superior electrochemical properties. Owing to its promising potential to immobilize various biological analytes, LIG has gained intense interest in the development of next-generation biosensors. Direct laser scribing on natural or polymeric substrate materials produces LIG electrodes with tunable properties, offers controlled microstructures, ease surface modifications, and doping with suitable elements, making it promising for electroanalytical measurements. Furthermore, LIG technology stands out as being cost-effective and supports environmental sustainability and eco-conscious solutions. These diverse features open new frontiers, making it suitable for fundamental applications in diverse fields, particularly in the food and dairy industry, where rapid, on-site, and precise monitoring is vital. This review comprehensively discusses fabrications of LIG-based biosensors with a focus on various laser sources, substrate materials, and surface modifications. The core sensing mechanisms of LIG biosensors are thoroughly summarized which enable high sensitivity and selectivity. However, special attention is given to LIG biosensors' applications in the food and dairy industry for the monitoring of food pathogens, food ingredients, food spoilage, biogenic amines, food additives, antibiotics, chemical contaminants, and pesticides. Finally, this review discusses the current challenges of LIG-based biosensors, such as reproducibility, stability, and integration into commercial industries, while offering a future outlook for potential applications. By highlighting recent advances and summarizing knowledge gaps, this review provides new insights into LIG-based sensors and their applications in the food and dairy industry to ensure food quality and safety.

Keywords: Biosensor fabrication; Biosensors; Food and dairy; Laser-induced graphene; Sensing mechanism.

Fig. 1

A Schematic illustration of effective substrates used in LIG fabrication. B SEM images of laser-derived graphene (LDG) at (a) 20 μm, (b) 1 μm, (c) cross-sectional SEM image, and (d) Raman spectra of fabricated LDG. C Shows (a) Laser scribed graphene fabrication by laser scribing, (b) Raman spectra of designed carbon nanosphere-laser scribed graphene at different laser powers, and (c) ID/IG and IG/I2D peak ratio of LDG. D Depicts a 3D demonstration of laser derived graphene (LDG) development by laser scribing on lignin/PVA film deposited on polyimide sheet and gold coating of fabricated LDG. Reproduced with permission under copyright © 2020 Elsevier B.V. [48]

Fig. 2

a LIG development by laser irradiation on a polymeric substrate. b Nd:YAG crystal laser for LIG fabrication. c Schematic illustration of semiconductor laser diode construction. d Femtosecond Yb-fiber laser system based on photonic crystal fibers for LIG fabrication. Adapted with permission from OPTICA under copyright CC BY 4.0 [51].

Fig. 3

Schematic illustration of LIG fabrication. a Development of LIG on a polysulfone precursor material. b Image of LIG patterned on different polymer substrates. c Raman spectra of LIG developed using various polymeric materials. d PEEK components development via 3D printing. e Development of LIG on PEEK substrate. f SEM images of fabricated LIG on PEEK substrate. Reproduced with permission from American Chemical Society under copyright CC BY 4.0 [26]

Fig. 4

a LIG development on wood substrate. b SEM images of fabricated LIG. c Raman spectra of designed LIG. d Image of LIG printed electronic circuit on the leaf for developing flexible and wearable plant sensor devices. e Schematic illustration of LIG patterning mechanism. Reproduced with permission under copyright© 2019 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim [100]

Fig. 5

Sensing mechanisms of LIG biosensors

Fig. 6

Fabrication, functionalization, and sensing mechanism of LIG biosensor. a Development of LIG on polyimide sheet (PI). b LIG working electrode. c Passivation of LIG electrode with lacquer. d SEM image of fabricated LIG electrode. e Immobilization of Salmonella antibody on the surface of LIG electrode. f Attachment of salmonella to the modified LIG electrode and electrochemical sensing Nyquist plot. Reproduced with permission from American Chemical Society under copyright CC BY 4.0 [8]

Fig. 7

a Pictorial representation of Salmonella sensing by colorimetric and electrochemical method via LIG integrated immunoassay strip. Reproduced with permission from American Chemical Society under copyright CC BY 4.0 [73]. b Graphical explanation of E. coli sensing by laser-reduced graphene oxide modified electrode. Reproduced with permission from American Chemical Society under copyright CC BY 4.0 [74]. c Detection of Pseudomonas aeruginosa culture on LIG. c-i) SWV graph of PA14. c-ii) PA14_amp represents the peak after 22 h of testing. c-iii) Metabolic activity assay of E. coli on resazurin. SWV graph for live E.coli culture. c-iv) Normalized current graph for E.coli live and heat-killed. Error bars indicate the standard deviation. c-v) The OD600 value of E.coli culture having no resazurin, and error bars show standard deviation. Reproduced from Elsevier under copyright © 2023 Elsevier B.V. [75]

Fig. 8

A Schematic illustration of Cu/LIG fabrication through spin coating followed by laser induction on the substrate membrane. B Glucose oxidation mechanism during catalysis under heating. C Glucose oxidation in the electrochemical sensing system. Reproduced from Elsevier under copyright © 2024 Elsevier B.V. [76]

Fig. 9

Sensing of naringin and hesperidin in citrus fruit. A Linear sweep voltammetry (LSV) of LIG-based electrochemical chip in PBS buffer at different concentrations of naringin and hesperidin. B Current values against the concentration of naringin and hesperidin. C and D Show the association between the monitored and added load of bioflavonoids. Reproduced from Elsevier under copyright © 2023 Elsevier B.V. [148]

Fig. 10

a Schematic demonstration of the development of LIG/Ag modified electrode for the sensing of formaldehyde. Reproduced with permission from American Chemical Society under copyright CC BY 4.0 [149]. b Graphical explanation of (AuNPs)-polypyrrole-chitosan-LIG-based sensor development for the sensing of vitamin C. Reproduced from Elsevier under copyright © 2024 Elsevier B.V. [78]. c A smart wireless sensor based on nanoPd@LIG modified electrode for the sensing of formaldehyde. Reproduced from Elsevier under copyright © 2022 Elsevier B.V. [79]. d Development of LIG electrode functionalized with porphyrin/ZnO for non-enzymatic sensing of ascorbic acid. Reproduced with permission from American Chemical Society under copyright CC BY 4.0 [80]

Fig. 11

a Cyclic voltammetry (CV) response. b UV–visible spectra after 02 CV cycles. c Calibration curve for Cu-LIG/ITO modified electrode against different concentration of vanillin. d Absorbance values for vanillin in the presence of structural analog interfering molecules. e Selectivity of vanillin at different concentrations with interfering analytes. f Intraday and interday vanillin measurements. Reproduced from Elsevier under copyright © 2024 Elsevier B.V. [81]

Fig. 12

Schematic demonstration of LIPS fabrication. a Development of LIG on paper by laser induction. a-i) LIPS developed on the milk carton for food monitoring. a-ii) LIPS is designed on paper cups for the monitoring of food temperature. b Photograph of LIG fabricated on different materials. b-i) LIG fabricated on the milk carton. b-ii) LIG on paper cup substrate. b-iii) LIG on colored paper precursor. b-iv) A SEM image of LIG was fabricated on colored paper. Reproduced from Elsevier under copyright © 2022 Elsevier B.V. [7]

Fig. 13

Design of flexible sensing and heating system based on frostbite resistance in fruit cold storage. a Schematic presentation of flexible sensing and heating system on fruits. b Hardware layout of flexible sensing and heating system. c Diagrammatical illustration of flexible sensing and heating system. Reproduced with permission from American Chemical Society under copyright CC BY 4.0 [172]

Fig. 14

Spider web graph shows the monitoring of flavor variations of fresh-cut cucumber after 15 days with laser-induced microporous packaging (100 μm) and coating with chitosan carbon dot. Reproduced with permission from Springer Nature under Copyright @ 2021 [173]

Fig. 15

Schematic elaboration of a cost-effective disposable LSG biosensor for the sensing of biogenic amines in food samples by applying locally sourced materials and comparison was made with fabricated sensor of analytical grade materials. Reproduced with permission from MDPI under copyright CC BY 4.0 [150]

Fig. 16

a Graphical explanation of LIG ion-selective electrode development for the sensing of nitrite in food samples. Reproduced with permission from Springer Nature under Copyright @ 2022 [151]. b Diagrammatical illustration for the fabrication of Cu/LIG modified electrode for the sensing of vanillin in food samples. Reproduced from Elsevier under copyright © 2024 Elsevier B.V. [81]

Fig. 17

a Selectivity test of LIG electrode optimized by imprinted polymer-based biosensor for the sensing of tetracycline. a-i) The differential pulse voltammetry (DPV) curves against different concentrations of tetracycline. a-ii) Linear concentration range of the designed sensor. Reproduced with permission from MDPI under copyright CC BY 4.0 [2]. b Schematic demonstration for the development of LIG electrode modified by gold nanoparticles for the sensing of sulfonamide in shrimp food sample. Reproduced with permission from Springer Nature under Copyright @ 2022 [152]

Fig. 18

A DPV curves of AuNPs/LIG electrode against different concentrations of tigecycline. B Linear concentration curves of the designed sensor. C DPV curves of the fabricated sensor to detect the tigecycline in the milk sample. D DPV curves of the fabricated sensor to detect tigecycline in meat extract. Reproduced from Elsevier under copyright © 2024 Elsevier B.V. [153]

Fig. 19

a Graphical demonstration of portable and flexible biosensor based on LIG for the sensitive monitoring of sulfonamide. Reproduced from Elsevier under copyright © 2022 Elsevier B.V. [154]. b Schematic illustration of paper-based biosensor device based on LIG/PbS/CdS electrode modified with CoOOH nanosheets for the sensing of ampicillin. Reproduced from Elsevier under copyright © 2022 Elsevier B.V. [155]

Fig. 20

A Adsorptive stripping differential pulse voltammetry (AdsDPV) curves of fabricated LIG electrode-based biosensor against different concentrations of bisphenol A. B Correlation between peak current and bisphenol A concentration. C AdsDPV curves for real water sample analysis by using the standard addition method. D AdsDPV curves of the designed sensor against different concentrations of tartrazine. E Correlation between peak current and tartrazine concentration. F AdsDPV curves of the fabricated sensor for the monitoring of tartrazine in real isotonic drink sample by applying standard addition approach. Reproduced from Elsevier under copyright © 2024 Elsevier B.V. [198]

Fig. 21

Graphical demonstration of proposed sensing mechanism of designed LIG and MnO₂ linked DNA amplification-based sensor for the sensing of pesticides in food samples. Reproduced from Elsevier under copyright © 2021 Elsevier B.V. [157]

Fig. 22

A Demonstration of glyphosate LIG sensor development and sensing mechanism. a) LIG patterning on polyimide (PI) sheet by laser induction. b) Platinum deposition at potential −0.5 V against Ag/AgCl. c) SEM image of platinum-modified LIG electrode. d) Drop casting of glutaraldehyde, flavin adenine dinucleotide and glycine oxidase. e) Sensing mechanism of glyphosate via electrochemical oxidation at potential 0.6 V. Reproduced with permission from WILEY under copyright CC BY 4.0 [158]. B Schematic illustration of neonicotinoids sensing by using LIG sensor. Reproduced with permission under copyright CC BY 4.0 [199]. C LIG sensor for the electrochemical sensing of paraquat in water. Reproduced with permission under copyright CC BY 4.0 [200]. D Explanation of 3D porous LIG flexible plant sensor for pesticide monitoring. Reproduced from Elsevier under copyright © 2020 Elsevier B.V [201]

Fig. 23

a Schematic elaboration of LIG electrode fabrication by laser induction on polyimide sheet. b LIG surface modification by silver nanoparticles (AgNPs). c Immobilization of analyte and cell encapsulation on LIG electrode surface. d EC-SERS monitoring setup. “Silver nanoparticles–laser-induced graphene. Reproduced with permission from Royal Society of Chemistry under copyright CC BY-NC 3.0 [202]