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Reversible chemiresistive sensing of ultra-low levels of elemental mercury vapor using thermally reduced graphene oxide

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Abstract

A chemiresistor sensor for ultra-low levels of elemental mercury (Hg0) vapor is described. The sensor was prepared through thermal reduction of graphene oxide (GO) deposited on an interdigitated electrode using only low temperature annealing typically at 230 °C. The sensor responds to the presence of Hg0 vapor within <1 min and spontaneously recovers its baseline through flushing with a Hg0-free carrier gas. The sensor has a linear response in the range of 0.5 to 12.2 ppbv of Hg0 vapor and a detection limit of 0.10 ppbv. The amount of GO and annealing temperature affect the sensor response and were optimized. The sensor can find use in monitoring exposure of persons to Hg0 vapors, for which a threshold value of 6.1 ppbv has been set by the World Health Organization.

Schematic of an interdigitated electrode modified with a layer of thermally reduced graphene oxide. It can be used as a chemiresistive sensor for Hg0 vapor. The sensor displays a rapid and reversible response and has an ultralow detection limit of 0.10 ppbv.

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References

  1. Pirrone N, Aas W, Cinnirella S, Ebinghaus R, Hedgecock IM, Pacyna J, Sprovieri F, Sunderland EM (2013) Toward the next generation of air quality monitoring: mercury. Atmos Environ 80:599–611. https://doi.org/10.1016/j.atmosenv.2013.06.053

    Article  CAS  Google Scholar 

  2. Pandey SK, Kim K-H, Brown RJC (2011) Measurement techniques for mercury species in ambient air. Trends Anal Chem 30:899–917. https://doi.org/10.1016/j.trac.2011.01.017

    Article  CAS  Google Scholar 

  3. Kabir KMM, Ippolito SJ, Kandjani AE, Sabri YM, Bhargava SK (2017) Nano-engineered surfaces for mercury vapor sensing: current state and future possibilities. TrAC Trends Anal Chem 88:77–99. https://doi.org/10.1016/j.trac.2016.12.009

    Article  CAS  Google Scholar 

  4. Griffin MJ, Kabir KMM, Coyle VE, Kandjani AE, Sabri YM, Ippolito SJ, Bhargava SK (2016) A Nanoengineered Conductometric device for accurate analysis of elemental mercury vapor. Environ Sci Technol 50:1384–1392. https://doi.org/10.1021/acs.est.5b05700

    Article  CAS  PubMed  Google Scholar 

  5. Wang D, Zhou K, Sun M, Fang Z, Liu X, Sun X (2013) Room temperature element mercury sensor using MoS2-PANI Nano- sheet-flowers composite. Anal Methods 5:6576–6578. https://doi.org/10.1039/b000000x

    Article  Google Scholar 

  6. Sarajlic M, Crossed D, Signuric Z, Jovic V, Petrovic S, Dordevic D (2013) Detection limit for an adsorption-based mercury sensor. Microelectron Eng 103:118–122. https://doi.org/10.1016/j.mee.2012.10.009

    Article  CAS  Google Scholar 

  7. Sabri YM, Kandjani AE, Ippolito SJ, Bhargava SK (2016) Ordered monolayer gold Nano-urchin structures and their size induced control for high gas sensing performance. Sci Rep 6:1–10. https://doi.org/10.1038/srep24625

    Article  CAS  Google Scholar 

  8. Kabir KMM, Sabri YM, Lay B, Ippolito SJ, Bhargava SK (2016) A silver electrode based surface acoustic wave (SAW) mercury vapor sensor: a physio-chemical and analytical investigation. RSC Adv 6:1–6. https://doi.org/10.1039/c6ra03148j

    Article  Google Scholar 

  9. Sabri YM, Kandjani AE, Ippolito SJ, Bhargava SK (2015) Nanosphere monolayer on a transducer for enhanced detection of gaseous heavy metal. ACS Appl Mater Interfaces 7:1491–1499. https://doi.org/10.1021/am507069z

    Article  CAS  PubMed  Google Scholar 

  10. James JZ, Lucas D, Koshland CP (2012) Gold nanoparticle films as sensitive and reusable elemental mercury sensors. Environ Sci Technol 46:9557–9562. https://doi.org/10.1021/es3005656

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  11. Varghese SS, Lonkar S, Singh KK, Swaminathan S, Abdala A (2015) Recent advances in graphene based gas sensors. Sensors Actuators B Chem 218:160–183. https://doi.org/10.1016/j.snb.2015.04.062

    Article  CAS  Google Scholar 

  12. Yuan W, Shi G (2013) Graphene-based gas sensors. J Mater Chem A 1:10078. https://doi.org/10.1039/c3ta11774j

    Article  CAS  Google Scholar 

  13. Deen MJ, Marsal LF, Moldovan O, Iñiguez B (2015) Graphene electronic sensors – review of recent developments and future challenges. IET Circuits Devices Syst 9:446–453. https://doi.org/10.1049/iet-cds.2015.0259

    Article  Google Scholar 

  14. Wang T, Huang D, Yang Z, Xu S, He G, Li X, Hu N, Yin G, He D, Zhang L (2016) A review on graphene-based gas/vapor sensors with unique properties and potential applications. Nano-Micro Lett 8:95–119. https://doi.org/10.1007/s40820-015-0073-1

    Article  CAS  Google Scholar 

  15. Tegou E, Pseiropoulos G, Filippidou MK, Chatzandroulis S (2016) Low-temperature thermal reduction of graphene oxide films in ambient atmosphere: infra-red spectroscopic studies and gas sensing applications. Microelectron Eng 159:146–150. https://doi.org/10.1016/j.mee.2016.03.030

    Article  CAS  Google Scholar 

  16. Dolbin AV, Khlistyuck MV, Esel’Son VB, Gavrilko VG, Vinnikov NA, Basnukaeva RM, Maluenda I, Maser WK, Benito AM (2016) The effect of the thermal reduction temperature on the structure and sorption capacity of reduced graphene oxide materials. Appl Surf Sci 361:213–220. https://doi.org/10.1016/j.apsusc.2015.11.167

    Article  CAS  Google Scholar 

  17. Zhang R, Alecrim V, Hummelgård M, Andres B, Forsberg S, Andersson M, Olin H (2015) Thermally reduced kaolin-graphene oxide nanocomposites for gas sensing. Sci Rep 5:1–6. https://doi.org/10.1038/srep07676

    Article  CAS  Google Scholar 

  18. Papamatthaiou S, Argyropoulos D-P, Farmakis F, Masurkar A, Alexandrou K, Kymissis I, Georgoulas N (2016) The effect of thermal reduction and film thickness on fast response transparent graphene oxide humidity sensors. Procedia Eng 168:301–304. https://doi.org/10.1016/j.proeng.2016.11.201

    Article  CAS  Google Scholar 

  19. Guo F, Silverberg G, Bowers S, Kim SP, Datta D, Shenoy V, Hurt RH (2012) Graphene-based environmental barriers. Environ Sci Technol 46:7717–7724. https://doi.org/10.1021/es301377y

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  20. Liu Y, Tian C, Yan B, Lu Q, Xie Y, Chen J, Gupta R, Xu Z, Kuznicki SM, Liu Q, Zeng H (2015) Nanocomposites of graphene oxide, ag nanoparticles, and magnetic ferrite nanoparticles for elemental mercury (Hg0) removal. RSC Adv 5:15634–15640. https://doi.org/10.1039/C4RA16016A

    Article  CAS  Google Scholar 

  21. Dumarey R, Brown RJC, Corns WT, Brown AS, Stockwell PB (2010) Elemental mercury vapour in air: the origins and validation of the “Dumarey equation” describing the mass concentration at saturation. Accred Qual Assur 15:409–414. https://doi.org/10.1007/s00769-010-0645-1

    Article  CAS  Google Scholar 

  22. Marcano DC, Kosynkin DV, Berlin JM, Sinitskii A, Sun Z, Slesarev A, Alemany LB, Lu W, Tour JM (2010) Improved synthesis of graphene oxide. ACS Nano 4:4806–4814. https://doi.org/10.1021/nn1006368

    Article  CAS  PubMed  Google Scholar 

  23. Zhou Y, Jiang Y, Xie T, Tai H, Xie G (2014) A novel sensing mechanism for resistive gas sensors based on layered reduced graphene oxide thin films at room temperature. Sensors Actuators B Chem 203:135–142. https://doi.org/10.1016/j.snb.2014.06.105

    Article  CAS  Google Scholar 

  24. Zhang P, Li JT, Meng JW, Jiang AQ, Zhuang J, Ning XJ (2017) Conductivity of graphene affected by metal adatoms. AIP Adv 7:35101. https://doi.org/10.1063/1.4977964

    Article  CAS  Google Scholar 

  25. Rahaman M, Aldalbahi A, Govindasami P, Khanam NP, Bhandari S, Feng P, Altalhi T (2017) A new insight in determining the percolation threshold of electrical conductivity for extrinsically conducting polymer composites through different sigmoidal models. Polymers (Basel) 9:1–17. https://doi.org/10.3390/polym9100527

    Article  CAS  Google Scholar 

  26. Latimer GW, AOAC International (2012) Appendix F : guidelines for standard method performance requirements. In: Off. Methods Anal. AOAC Int., 19th ed. Gaithersburg, Md. : AOAC International, p Appendix F, 1–17

  27. McNicholas TP, Zhao K, Yang C, Hernandez SC, Mulchandani A, Myung NV, Deshusses MA (2011) Sensitive detection of elemental mercury vapor by gold-nanoparticle- decorated carbon nanotube sensors. J Phys Chem C 115:13927–13931. https://doi.org/10.1021/jp203662w

    Article  CAS  Google Scholar 

  28. Safavi A, Maleki N, Doroodmand MM (2010) Fabrication of a selective mercury sensor based on the adsorption of cold vapor of mercury on carbon nanotubes: determination of mercury in industrial wastewater. J Hazard Mater 173:622–629. https://doi.org/10.1016/j.jhazmat.2009.08.130

    Article  CAS  PubMed  Google Scholar 

  29. Zhu Z (2017) An overview of carbon nanotubes and graphene for biosensing applications. Nano-Micro Lett 9:1–25. https://doi.org/10.1007/s40820-017-0128-6

    Article  CAS  Google Scholar 

  30. WHO (1980) Recommended health- based limits in occupational exposure to heavy metals. Report of WHO study group, World Health Organization, (WHO — Technical Report Series, No. 647), Geneva, Switzerland

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Acknowledgments

One of the authors (ARS) gratefully acknowledges the research support fund provided by the Accelerated Science and Technology Human Resource Development Program (ASTHRDP) of the Department of Science and Technology-Science Education Institute (DOST-SEI). We are grateful for the kind assistance of Dr. Stephen Lirio in the morphological characterization of GO and tRGO.

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Authors and Affiliations

  1. The Graduate School, University of Santo Tomas, España Boulevard, 1015, Manila, Philippines

    Alan Rodelle M. Salcedo

  2. College of Science, University of Santo Tomas, España Boulevard, 1015, Manila, Philippines

    Alan Rodelle M. Salcedo & Fortunato B. Sevilla III

  3. Research Center for the Natural and Applied Sciences, University of Santo Tomas, España Boulevard, 1015, Manila, Philippines

    Alan Rodelle M. Salcedo & Fortunato B. Sevilla III

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  1. Alan Rodelle M. Salcedo
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  2. Fortunato B. Sevilla III
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Correspondence to Alan Rodelle M. Salcedo.

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Salcedo, A.R.M., Sevilla, F.B. Reversible chemiresistive sensing of ultra-low levels of elemental mercury vapor using thermally reduced graphene oxide. Microchim Acta 185, 289 (2018). https://doi.org/10.1007/s00604-018-2831-5

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