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Title: A fluorescence-electrochemical study of carbon nanodots (CNDs) in bio- and photoelectronic applications and energy gap investigation

Abstract

Carbon nanodots (CNDs) have attracted significant attention due to their superior solubility, biocompatibility, tunable photoluminescence, and opto-electronic properties. Our work describes a new fluorescence-based spectroelectrochemistry approach to simultaneously study the photoluminescence and wavelength dependent photocurrent of microwave synthesized CNDs. The fluorescence of CNDs shows selective quenching upon a reversible redox couple, ferricyanide/ferrocyanide, reaction during cyclic voltammetry. The CND modified gold slide electrode demonstrates wavelength dependent photocurrent generation during the fluorescence-electrochemical study, suggesting the potential application of CNDs in photoelectronics. UV-Vis absorption and electrochemistry are used to quantify the energy gap of the CNDs, and then to calibrate a Hückel model for CNDs’ electronic energy levels. The Hückel (or tight binding) model treatment of an individual CND as a molecule combines the conjugated π states (C[double bond, length as m-dash]C) with the functional groups (C[double bond, length as m-dash]O, C–O, and COOH) associated with the surface electronic states. This experimental and theoretical investigation of CNDs provides a new perspective on the optoelectronic properties of CNDs and should aid in their development for practical use in biomedicine, chemical sensing, and photoelectric devices.

Authors:
 [1];  [1];  [1];  [2];  [1];  [1];  [1];  [1];  [1];  [2]; ORCiD logo [1]
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  1. Univ. of North Carolina at Greensboro, NC (United States)
  2. Univ. of Pittsburgh, PA (United States)
Publication Date:
Research Org.:
Univ. of Pittsburgh, PA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Southeastern Nanotechnology Infrastructure Corridor (SENIC); National Nanotechnology Coordinated Infrastructure (NNCI)
OSTI Identifier:
1604949
Grant/Contract Number:  
FG02-07ER46430; ECCS-1542174
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP
Additional Journal Information:
Journal Volume: 19; Journal Issue: 30; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY; Carbon nanodots; Fluorescence origin; Photocurrent; Electrochemicalfluorescence analysis; Microwave synthesis

Citation Formats

Zeng, Zheng, Zhang, Wendi, Arvapalli, Durga M., Bloom, Brian, Sheardy, Alex, Mabe, Taylor, Liu, Yiyang, Ji, Zuowei, Chevva, Harish, Waldeck, David H., and Wei, Jianjun. A fluorescence-electrochemical study of carbon nanodots (CNDs) in bio- and photoelectronic applications and energy gap investigation. United States: N. p., 2017. Web. doi:10.1039/C7CP02875J.
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Zeng, Zheng, Zhang, Wendi, Arvapalli, Durga M., Bloom, Brian, Sheardy, Alex, Mabe, Taylor, Liu, Yiyang, Ji, Zuowei, Chevva, Harish, Waldeck, David H., & Wei, Jianjun. A fluorescence-electrochemical study of carbon nanodots (CNDs) in bio- and photoelectronic applications and energy gap investigation. United States. https://doi.org/10.1039/C7CP02875J
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Zeng, Zheng, Zhang, Wendi, Arvapalli, Durga M., Bloom, Brian, Sheardy, Alex, Mabe, Taylor, Liu, Yiyang, Ji, Zuowei, Chevva, Harish, Waldeck, David H., and Wei, Jianjun. Mon . "A fluorescence-electrochemical study of carbon nanodots (CNDs) in bio- and photoelectronic applications and energy gap investigation". United States. https://doi.org/10.1039/C7CP02875J. https://www.osti.gov/servlets/purl/1604949.
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@article{osti_1604949,
title = {A fluorescence-electrochemical study of carbon nanodots (CNDs) in bio- and photoelectronic applications and energy gap investigation},
author = {Zeng, Zheng and Zhang, Wendi and Arvapalli, Durga M. and Bloom, Brian and Sheardy, Alex and Mabe, Taylor and Liu, Yiyang and Ji, Zuowei and Chevva, Harish and Waldeck, David H. and Wei, Jianjun},
abstractNote = {Carbon nanodots (CNDs) have attracted significant attention due to their superior solubility, biocompatibility, tunable photoluminescence, and opto-electronic properties. Our work describes a new fluorescence-based spectroelectrochemistry approach to simultaneously study the photoluminescence and wavelength dependent photocurrent of microwave synthesized CNDs. The fluorescence of CNDs shows selective quenching upon a reversible redox couple, ferricyanide/ferrocyanide, reaction during cyclic voltammetry. The CND modified gold slide electrode demonstrates wavelength dependent photocurrent generation during the fluorescence-electrochemical study, suggesting the potential application of CNDs in photoelectronics. UV-Vis absorption and electrochemistry are used to quantify the energy gap of the CNDs, and then to calibrate a Hückel model for CNDs’ electronic energy levels. The Hückel (or tight binding) model treatment of an individual CND as a molecule combines the conjugated π states (C[double bond, length as m-dash]C) with the functional groups (C[double bond, length as m-dash]O, C–O, and COOH) associated with the surface electronic states. This experimental and theoretical investigation of CNDs provides a new perspective on the optoelectronic properties of CNDs and should aid in their development for practical use in biomedicine, chemical sensing, and photoelectric devices.},
doi = {10.1039/C7CP02875J},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 30,
volume = 19,
place = {United States},
year = {Mon Jul 03 00:00:00 EDT 2017},
month = {Mon Jul 03 00:00:00 EDT 2017}
}
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