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Understanding Graphene Response to Neutral and Charged Lead Species: Theory and Experiment
Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering. NASU, Ukraine.
Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.
Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, Faculty of Science & Engineering.ORCID iD: 0000-0001-8478-4663
Linköping University, Department of Physics, Chemistry and Biology, Semiconductor Materials. Linköping University, Faculty of Science & Engineering.ORCID iD: 0000-0003-1000-0437
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2018 (English)In: Materials, ISSN 1996-1944, E-ISSN 1996-1944, Vol. 11, no 10, article id 2059Article in journal (Refereed) Published
Abstract [en]

Deep understanding of binding of toxic Lead (Pb) species on the surface of two-dimensional materials is a required prerequisite for the development of next-generation sensors that can provide fast and real-time detection of critically low concentrations. Here we report atomistic insights into the Lead behavior on epitaxial graphene (Gr) on silicon carbide substrates by thorough complementary study of voltammetry, electrical characterization, Raman spectroscopy, and Density Functional Theory (DFT). It is verified that the epitaxial graphene exhibits quasi-reversible anode reactions in aqueous solutions, providing a well-defined redox peak for Pb species and good linearity over a concentration range from 1 nM to 1 mu M. The conductometric approach offers another way to investigate Lead adsorption, which is based on the formations of stable charge-transfer complexes affecting the p-type conductivity of epitaxial graphene. Our results suggest the adsorption ability of the epitaxial graphene towards divalent Lead ions is concentration-dependent and tends to saturate at higher concentrations. To elucidate the mechanisms responsible for Pb adsorption, we performed DFT calculations and estimated the solvent-mediated interaction between Lead species in different oxidative forms and graphene. Our results provide central information regarding the energetics and structure of Pb-graphene interacting complexes that underlay the adsorption mechanisms of neutral and divalent Lead species. Such a holistic understanding favors design and synthesis of new sensitive materials for water quality monitoring.

Place, publisher, year, edition, pages
MDPI , 2018. Vol. 11, no 10, article id 2059
Keywords [en]
lead; electrochemical detection; conductometric detection; sensing mechanism; DFT; epitaxial graphene
National Category
Materials Chemistry
Identifiers
URN: urn:nbn:se:liu:diva-152827DOI: 10.3390/ma11102059ISI: 000448658400273PubMedID: 30360390OAI: oai:DiVA.org:liu-152827DiVA, id: diva2:1265153
Note

Funding Agencies|VR grants [VR 621-2014-5805, VR 2016-05362]; SSF [SSF GMT14-0077, SSF RMA15-0024]; Angpanneforeningens Forskningsstiftelse [16-541]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [2009-00971]

Available from: 2018-11-22 Created: 2018-11-22 Last updated: 2019-03-07

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