Skip to main content
Log in

Reduced Graphene Oxide-Modified Screen-Printed Carbon (rGO-SPCE)-Based Disposable Electrochemical Sensor for Sensitive and Selective Determination of Ethyl Carbamate

  • Published:
Food Analytical Methods Aims and scope Submit manuscript

Abstract

Ethyl carbamate (EC), a multi-site genotoxic carcinogen, exists in fermented food and beverages. However, the existing analytical methods need precise instrument, complex sample pretreatment, time-consuming, and high cost. Therefore, a disposable electrochemical biomimetic sensor was developed for fast and selective detection of EC based on reduced graphene oxide/screen-printed carbon composite electrode (rGO/SPCE). Firstly, the SPCE is modified with rGO by electrodeposition process that increased current signal and decreased the impedance of contact interface. Secondly, the OAP/rGO/SPCE biomimetic sensor was synthesized through electropolymerization by cyclic voltammograms in mixed solution of template of EC and monomer of O-aminophenol (OAP). The sensor specifically bound to EC quickly without sample pretreatment. A linear range was from 100 to 1300 nM, and a detection limit of 37 nM was achieved. The detection time is less than 5 min. The sensor possesses advantages include good chemical and mechanical stability, simplicity, low cost of preparation, and sensitive and label-free determination.

Schematic diagram of preparation of rGO-SPCE based sensor

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8

Similar content being viewed by others

References

  • Alberts P, Stander M, Villiers A (2011) Development of a novel solid-phase extraction, LC-MS/MS method for the analysis of ethyl carbamate in alcoholic beverages: application to South African wine and spirits. Food Additives and Contaminants Part A-Chemistry Analysis Control Exposure & Risk Assessment 28:826–839

    CAS  Google Scholar 

  • Allen M, Tung V, Kaner R (2010) Honeycomb carbon: a review of graphene. Chem Rev 110:132–145

    Article  CAS  Google Scholar 

  • Borisova B, Sánchez A, Jiménez-Falcao S, Martín M, Salazar P, Parrado C, Pingarrón J, Villalonga R (2016) Reduced graphene oxide-carboxymethylcellulose layered with platinum nanoparticles/PAMAM dendrimer/magnetic nanoparticles hybrids. Application to the preparation of enzyme electrochemical biosensors. Sensors Actuators B Chem 232:84–90

    Article  CAS  Google Scholar 

  • Chen D, Ren Y, Zhong Q, Shao Y, Zhao Y, Wu Y (2017) Ethyl carbamate in alcoholic beverages from China: levels, dietary intake, and risk assessment. Food Control 10:283–288

    Article  Google Scholar 

  • Deák E, Gyepes A, Stefanovits-Bányai É, Dernovics M (2010) Determination of ethyl carbamate in palinka spirits by liquid chromatography-electrospray tandem mass spectrometry after derivatization. Food Res Int 43:2452–2455

    Article  Google Scholar 

  • Ebarvia B, Cabanilla S, Sevilla F (2005) Biomimetic properties and surface studies of a piezoelectric caffeine sensor based on electrosynthesized polypyrrole. Talanta 66:145–152

    Article  CAS  Google Scholar 

  • Fu M, Liu J, Chen Q, Liu X, He G, Chen J (2010) Determination of ethyl carbamate in Chinese yellow rice wine using high-performance liquid chromatography with fluorescence detection. Int J Food Sci Technol 45:1297–1302

    Article  CAS  Google Scholar 

  • Fu Z, Yang L, Ma L, Liu X, Li J (2016) Occurrence of ethyl carbamate in three types of Chinese wines and its possible reasons. Food Sci Biotechnol 4:949–953

    Article  Google Scholar 

  • Gustavo González A, Ángeles Herrador M (2007) A practical guide to analytical method validation, including measurement uncertainty and accuracy profiles. Trac-Trends in Analytical Chemistry 26:227–238

    Article  Google Scholar 

  • Hai H, An X, Li Y (2015) Molecularly imprinted electrochemical sensor selective determination of oxidized glutathione. Anal Methods 7:2210–2214

    Article  CAS  Google Scholar 

  • Hernández-Ibáñez N, García-Cruz L, Montiel V, Foster C, Banks C, Inirsta J (2016) Electrochemical lactate biosensor based upon chitosan/carbon nanotubes modified screen-printed graphite electrodes for the determination of lactate in embryonic cell cultures. Biosens Bioelectron 77:1168–1174

    Article  Google Scholar 

  • Lachenmeier D, Frank W, Kuballa T (2005) Application of tandem mass spectrometry combined with gas chromatography to the routine analysis of ethyl carbamate in stone-fruit spirits. Rapid Commun Mass Spectrom 19:108–112

    Article  CAS  Google Scholar 

  • Lee P, Compton R (2015) Selective thiol detection in authentic biological samples with the use of screen-printed electrodes. Anal Sci 31:685–691

    Article  CAS  Google Scholar 

  • Li T, Aoki K, Chen J, Nishiumi T (2011) Voltammetric electrodes modified with swollen polyacrylic latex particles. J Electroanal Chem 656:279–284

    Article  CAS  Google Scholar 

  • Li T, Xu J, Zhou L, Wang L, Sun Y, Cheng J, Yuan M, Wang L, Yue Y, Wang J (2013) Voltammetric determination of the adsorption kinetics of acetic acid on activated carbon. Journal of Electrochemical Society 160:H568–H572

    Article  CAS  Google Scholar 

  • Li T, Xu J, Zhou L, Shen S, Zhao L, Yuan M, Wang J (2014a) Voltammetric behavior of carboxyl hydrogel particles on a cavity electrode surface. Electrochem Commun 38:75–78

    Article  Google Scholar 

  • Li B, Qiu Z, Wan Q, Liu Y, Yang N (2014b) β-Cyclodextrin functionalized graphene nano platelets for electrochemical determination of triclosan. Phys Status Solidi B/Physica Status Solidi B-Basic Solid State Physics 12:2773–2777

    Google Scholar 

  • Li G, Zhong Q, Wang D, Zhang X, Gao H (2015) Determination and formation of ethyl carbamate in Chinese spirits. Food Control 56:169–176

    Article  CAS  Google Scholar 

  • Liu J, Xu Y, Zhao G (2012) Rapid determination of ethyl carbamate in Chinese rice using headspace solid-phase microextraction and gas chromatography-mass spectrometry. J Inst Brew 118:217–222

    Article  CAS  Google Scholar 

  • Liu Y, Dong B, Qin Z, Yang N, Liu Y, Yang L, Chang F, Wu Y (2014) Ethyl carbamate levels in wine and spirits from markets in Hebei Province, China. Food Additives & Contaminants Part b-Surveillance 4:1–5

    Article  Google Scholar 

  • Liu Y, Qiu Z, Wan Q, Wang Z, Wu K, Yang N (2016) High-performance hydrazine sensor based on graphene nano platelets supported metal nanoparticles. Electroanalysis 28:126–132

    Article  CAS  Google Scholar 

  • Masson J, Gardoso M, Zacaroni L, dos Anjos J, Santiago W, Machado A, Saczk A, Nelson D (2014) GC-MS analysis of ethyl carbamate in distilled sugar cane spirits from the northern and southern regions of Minas Gerais. J Inst Brew 120:516–520

    CAS  Google Scholar 

  • Nóbrega I, Pereira G, Silva M, Pereira E, Medeiros M, Telles D, Albuquerque E, Oliveira J, Lachenmeier D (2015) Improved sample preparation for GC-MS-SIM analysis of ethyl carbamate in wine. Food Chem 177:23–28

    Article  Google Scholar 

  • Pearce N, Blair A, Vineis P, Ahrens W, Andersen A, Anto J, Armstrong B, Baccarelli A, Beland F, Berrington A (2015) IARC monographs: 40 years of evaluating carcinogenic hazards to humans. Environ Health Perspect 123:507–514

    Google Scholar 

  • Ping J, Wang Y, Fan K, Wu J, Ying Y (2011) Direct electrochemical reduction of graphene oxide on ionic liquid doped screen-printed electrode and its electrochemical biosensing application. Biosens Bioelectron 28:204–209

    Article  CAS  Google Scholar 

  • Qiu Z, Yu J, Peng Y, Wang Z, Wan Q, Yang N (2016) Electrochemical grafting of graphene nano platelets with aryl diazonium salts. ACS Applied Materials and Interface 8(42):28291–28298

    Article  CAS  Google Scholar 

  • Rella S, Giuri A, Corcione C, Acocella M, Colella S, Guerra G, Listorti A, Rizzo A, Malitesta C (2015) X-ray photoelectron spectroscopy of reduced graphene oxide prepared by a novel green method. Vacuum 119:159–162

    Article  CAS  Google Scholar 

  • Shi H, Yang E (2012) Simultaneous determination of methylcarbanmate and ethylcarbamate in fermented foods and beverages by derivatization and GC-MS analysis. Chemistry Central Journal 6:1–8

    Google Scholar 

  • Shojaei S, Nasirizadeh N, Entezam M, Koosha M, Azimzadeh M (2016) An electrochemical nanosensor based on molecularly imprinted polymer (MIP) for detection of gallic acid in fruit juices. Food Anal Methods 9:2721–2731

    Article  Google Scholar 

  • Silva M, Dias A, Cordeiro M, Marques E, Goulart M, Dutra R (2014) A thiophene-modified screen printed electrode for detection of dengue virus NS1 protein. Talanta 128:505–510

    Article  CAS  Google Scholar 

  • Su D, Zhang Y, Wang Z, Wan Q, Yang N (2017) Decoration of graphene nano platelets with gold nanoparticles for voltammetry of 4-nonylphenol. Carbon. doi:10.1016/j.carbon.2017.02.103

    Google Scholar 

  • Torrente-Rodríguez R, Montiel V, Campuzano S, Farchado-Dinia M, Barderas R, Segundo-Acosta P, Montoya J, Pingarron J (2016) Fast electrochemical miRNAs determination in cancer cells and tumor tissues with antibody-functionalized magnetic microcarriers. ACS Sensors 1:896–903

    Article  Google Scholar 

  • Wan Q, Wang X, Yu F, Wang X, Yang N (2009) Effects of capacitance and resistance of MWNT-film coated electrodes on voltammetric detection of acetaminophen. J Appl Electrochem 39:1145–1151

    Article  CAS  Google Scholar 

  • Wang Z, Luo X, Wan Q, Wu K, Yang N (2014) Versatile matrix for constructing enzyme-based biosensors. ACS Appl Mater Interfaces 6:17296–17305

    Article  CAS  Google Scholar 

  • Wu S, Tan W, Xu H (2010) Protein molecularly imprinted polyacrylamide membrane: for hemoglobin sensing. Analyst 135:2523–2527

    Article  CAS  Google Scholar 

  • Wu P, Cai C, Shen X, Wang L, Zhang J, Tan Y, Jiang W, Pan X (2014) Formation of ethyl carbamate and changes during fermentation and storage of yellow rice wine. Food Chem 152:108–112

    Article  CAS  Google Scholar 

  • Yáñez-Sedeño P, Campuzano S, Pingarrón J (2016) Magnetic particles coupled to disposable screen printed transducers for electrochemical biosensing. Sensors 16:1–32

    Article  Google Scholar 

  • Yang N, Waldvogel S, Jiang X (2016) Electrochemistry of carbon dioxide on carbon electrodes. ACS Appl Mater Interfaces 42:28357–28371

    Article  Google Scholar 

  • Zhao X, Zhang W, Chen H, Chen Y, Huang G (2014) Disposable electrochemical ascorbic acid sensor based on molecularly imprinted poly (o-phenylenediamine)-modified dual channel screen-printed electrode for orange juice analysis. Food Anal Methods 7:1557–1563

    Article  Google Scholar 

Download references

Author information

Authors and Affiliations

Authors

Corresponding authors

Correspondence to Xiaoyu Zhao or Juankun Zhang.

Ethics declarations

Funding

This study was funded by the Tianjin Municipal Science and Technology Commission of China (no. 16YFXTSY00210), the National Natural Science Foundation of China (NSFC Grant no. 21503146), and the Tianjin Front Tec. LTD.

Conflict of Interest

Xiaoyu Zhao declares that he has no conflict of interest. Juanjuan Zuo declares that she has no conflict of interest. Shue Qiu declares that she has no conflict of interest. Wenshuai Hu declares that he has no conflict of interest. Yanfei Wang declares that he has no conflict of interest. Juankun Zhang declares that she has no conflict of interest.

Ethical Approval

This article does not contain any studies with human participants or animals performed by any of the authors.

Informed Consent

Not applicable.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Zhao, X., Zuo, J., Qiu, S. et al. Reduced Graphene Oxide-Modified Screen-Printed Carbon (rGO-SPCE)-Based Disposable Electrochemical Sensor for Sensitive and Selective Determination of Ethyl Carbamate. Food Anal. Methods 10, 3329–3337 (2017). https://doi.org/10.1007/s12161-017-0886-2

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s12161-017-0886-2

Keywords

Navigation