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Title: Electron Transfer Kinetics at Graphene Quantum Dot Assembly Electrodes

Abstract

Electrochemical performance of nanostructured carbon electrodes was evaluated using cyclic voltammetry and a simple simulation model. The electrodes were prepared from soluble precursors by anodic electrodeposition of two sizes of graphene quantum dot assemblies (hexabenzocoronene (HBC) and carbon quantum dot (CQD)) onto a conductive support. Experimental and simulated voltammograms enabled the extraction of the following electrode parameters: conductivity of the electrodes (a combination of ionic and electronic contributions), density of available electrode states at different potentials, and tunneling rate constant (Marcus Gerischer model) for interfacial charge transfer to ferrocene/ferrocenium (Fc/Fc +) couple. The parameters indicate that HBC and CQD have significant density of electronic states at potentials more positive than -0.5 V versus Ag/Ag + Enabled by these large densities, the electron transfer rates at the Fc/Fc + thermodynamic potential are several orders of magnitude slower than those commonly observed on other carbon electrodes. This study is expected to accelerate the discovery of improved synthetic carbon electrodes by providing fast screening methodology of their electrochemical behavior.

Authors:
 [1];  [1];  [2];  [3];  [4];  [5];  [1]
  1. Univ. of Illinois, Chicago, IL (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Georgia Inst. of Technology, Atlanta, GA (United States)
  3. Univ. of Illinois, Chicago, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
  4. Middle Georgia State Univ., Macon, GA (United States)
  5. Univ. of Illinois, Chicago, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Science Foundation (NSF); USDOE
OSTI Identifier:
1582581
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 11; Journal Issue: 49; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; cyclic voltammetry; electrode; electron transfer; graphene quantum dots; interface; kinetics

Citation Formats

Zoric, Marija R., Singh, Varun, Warren, Sean, Plunkett, Samuel, Khatmullin, Renat R., Chaplin, Brian P., and Glusac, Ksenija D. Electron Transfer Kinetics at Graphene Quantum Dot Assembly Electrodes. United States: N. p., 2019. Web. doi:10.1021/acsami.9b14161.
Zoric, Marija R., Singh, Varun, Warren, Sean, Plunkett, Samuel, Khatmullin, Renat R., Chaplin, Brian P., & Glusac, Ksenija D. Electron Transfer Kinetics at Graphene Quantum Dot Assembly Electrodes. United States. doi:10.1021/acsami.9b14161.
Zoric, Marija R., Singh, Varun, Warren, Sean, Plunkett, Samuel, Khatmullin, Renat R., Chaplin, Brian P., and Glusac, Ksenija D. Fri . "Electron Transfer Kinetics at Graphene Quantum Dot Assembly Electrodes". United States. doi:10.1021/acsami.9b14161.
@article{osti_1582581,
title = {Electron Transfer Kinetics at Graphene Quantum Dot Assembly Electrodes},
author = {Zoric, Marija R. and Singh, Varun and Warren, Sean and Plunkett, Samuel and Khatmullin, Renat R. and Chaplin, Brian P. and Glusac, Ksenija D.},
abstractNote = {Electrochemical performance of nanostructured carbon electrodes was evaluated using cyclic voltammetry and a simple simulation model. The electrodes were prepared from soluble precursors by anodic electrodeposition of two sizes of graphene quantum dot assemblies (hexabenzocoronene (HBC) and carbon quantum dot (CQD)) onto a conductive support. Experimental and simulated voltammograms enabled the extraction of the following electrode parameters: conductivity of the electrodes (a combination of ionic and electronic contributions), density of available electrode states at different potentials, and tunneling rate constant (Marcus Gerischer model) for interfacial charge transfer to ferrocene/ferrocenium (Fc/Fc+) couple. The parameters indicate that HBC and CQD have significant density of electronic states at potentials more positive than -0.5 V versus Ag/Ag+ Enabled by these large densities, the electron transfer rates at the Fc/Fc+ thermodynamic potential are several orders of magnitude slower than those commonly observed on other carbon electrodes. This study is expected to accelerate the discovery of improved synthetic carbon electrodes by providing fast screening methodology of their electrochemical behavior.},
doi = {10.1021/acsami.9b14161},
journal = {ACS Applied Materials and Interfaces},
number = 49,
volume = 11,
place = {United States},
year = {2019},
month = {11}
}

Journal Article:
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This content will become publicly available on November 15, 2020
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