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Title: Tuning the Selectivity and Activity of Electrochemical Interfaces with Defective Graphene Oxide and Reduced Graphene Oxide

Abstract

Engineered solid-liquid interfaces will play an important role in the development of future energy storage and conversion (ESC) devices. In the present study, defective graphene oxide (GO) and reduced graphene oxide (rGO) structures were used as engineered interfaces to tune the selectivity and activity of Pt disk electrodes. GO was deposited on Pt electrodes via the Langmuir-Blodgett technique, which provided compact and uniform GO films, and these films were subsequently converted to rGO by thermal reduction. Electrochemical measurements revealed that both GO and rGO interfaces on Pt electrodes exhibit selectivity toward the oxygen reduction reaction (ORR), but they do not have an impact on the activity of the hydrogen oxidation reaction in acidic environments. Scanning transmission electron microscopy at atomic resolution, along with Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and scanning electron microscopy (SEM), revealed possible diffusion sites for H 2 and O 2 gas molecules and functional groups relevant to the selectivity and activity of these surfaces. Based on these insights, rGO interfaces are further demonstrated to exhibit enhanced activity for the ORR in nonaqueous environments and demonstrate the power of our ex situ engineering approach for the development of next-generation ESC devices.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3];  [4]; ORCiD logo [2];  [3];  [3]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division; Univ. of Ljubljana, Ljubljana (Slovenia). Faculty of Chemistry and Chemical Technology
  2. Sandia National Lab. (SNL-CA), Livermore, CA (United States). Nanoscale Sciences Dept.
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  4. National Inst. of Chemistry, Ljubljana (Slovenia)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States); Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; Slovenian Research Agency (ARRS); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1569847
Alternate Identifier(s):
OSTI ID: 1570266
Report Number(s):
SAND-2019-10400J
Journal ID: ISSN 1944-8244; 153933
Grant/Contract Number:  
AC02-06CH11357; AC04-94AL85000
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 11; Journal Issue: 37; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Graphene oxide; hydrogen oxidation reaction; interface, electrocatalysis; oxygen reduction reaction; reduced graphene oxide; selectivity

Citation Formats

Genorio, Bostjan, Harrison, Katharine L., Connell, Justin G., Dražić, Goran, Zavadil, Kevin R., Markovic, Nenad M., and Strmcnik, Dusan. Tuning the Selectivity and Activity of Electrochemical Interfaces with Defective Graphene Oxide and Reduced Graphene Oxide. United States: N. p., 2019. Web. doi:10.1021/acsami.9b13391.
Genorio, Bostjan, Harrison, Katharine L., Connell, Justin G., Dražić, Goran, Zavadil, Kevin R., Markovic, Nenad M., & Strmcnik, Dusan. Tuning the Selectivity and Activity of Electrochemical Interfaces with Defective Graphene Oxide and Reduced Graphene Oxide. United States. doi:10.1021/acsami.9b13391.
Genorio, Bostjan, Harrison, Katharine L., Connell, Justin G., Dražić, Goran, Zavadil, Kevin R., Markovic, Nenad M., and Strmcnik, Dusan. Tue . "Tuning the Selectivity and Activity of Electrochemical Interfaces with Defective Graphene Oxide and Reduced Graphene Oxide". United States. doi:10.1021/acsami.9b13391. https://www.osti.gov/servlets/purl/1569847.
@article{osti_1569847,
title = {Tuning the Selectivity and Activity of Electrochemical Interfaces with Defective Graphene Oxide and Reduced Graphene Oxide},
author = {Genorio, Bostjan and Harrison, Katharine L. and Connell, Justin G. and Dražić, Goran and Zavadil, Kevin R. and Markovic, Nenad M. and Strmcnik, Dusan},
abstractNote = {Engineered solid-liquid interfaces will play an important role in the development of future energy storage and conversion (ESC) devices. In the present study, defective graphene oxide (GO) and reduced graphene oxide (rGO) structures were used as engineered interfaces to tune the selectivity and activity of Pt disk electrodes. GO was deposited on Pt electrodes via the Langmuir-Blodgett technique, which provided compact and uniform GO films, and these films were subsequently converted to rGO by thermal reduction. Electrochemical measurements revealed that both GO and rGO interfaces on Pt electrodes exhibit selectivity toward the oxygen reduction reaction (ORR), but they do not have an impact on the activity of the hydrogen oxidation reaction in acidic environments. Scanning transmission electron microscopy at atomic resolution, along with Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and scanning electron microscopy (SEM), revealed possible diffusion sites for H2 and O2 gas molecules and functional groups relevant to the selectivity and activity of these surfaces. Based on these insights, rGO interfaces are further demonstrated to exhibit enhanced activity for the ORR in nonaqueous environments and demonstrate the power of our ex situ engineering approach for the development of next-generation ESC devices.},
doi = {10.1021/acsami.9b13391},
journal = {ACS Applied Materials and Interfaces},
issn = {1944-8244},
number = 37,
volume = 11,
place = {United States},
year = {2019},
month = {8}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Figures / Tables:

Figure 1 Figure 1: (a) Schematics of Langmuir−Blodgett trough depicting compression barriers and the holder for dipping the Pt disk electrodes. The holder is angled at 30° relative to the air−water interface, and the graphene oxide (GO) films were transferred in an upstroke direction. (b) A typical $Π$−Area isotherm for the GOmore » monolayer on the Langmuir trough measured with Wilhelmy plate positioned parallel to barriers. (c) Representative SEM depicting GO sheets on a Pt disk dipped at the surface pressure corresponding to the red dot in (b). (d) Representative SEM depicting GO sheets on a Pt disk dipped at the surface pressure corresponding to the blue dot in (b). The dark areas (flake boundary) consist of regions where GO sheets overlap, and arrows point to possible diffusion sites for gaseous reactants to access the underlying Pt.« less

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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.