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Title: Critical Impact of Graphene Functionalization for Transition Metal Oxide/Graphene Hybrids on Oxygen Reduction Reaction

Abstract

Transition metal oxides (TMOs) anchored on a carbon nanostructure have been widely pursued for oxygen reduction reaction (ORR) catalysis. The high ORR activity of TMO/graphene has been often attributed to the synergistic nature between TMO and carbon but with little relevant mechanistic study. In this report, the focus is made on how the type of majority oxygen-containing functional group of graphene affects the ORR performance of the resulting TMO/graphene nanocomposites. Our TiO 2/carboxylated graphene and ZrO 2/hydroxylated graphene rendered an ORR activity very close to that of Pt/C with an equal mass loading, via a four-electron transfer dominant process unlike other TMO/graphene variants of study. It is revealed that a stable anchoring of nanoparticles (NPs) on the graphene surface, which is essential to prevent the restacking of graphene layers, is established only through a specific type of functional groups on the graphene. In addition, the interplay among TMOs, graphene, and functional groups is found to be deterministic in the activity and electron transfer pathway of ORR, which is supported by density function theory (DFT) calculations. Finally, the calculations indicate that the electron transfer pathway is dependent upon the structure of NPs interfacing with functional groups of the graphene as itmore » affects the preferred sites for oxygen dissociation.« less

Authors:
 [1];  [1];  [2];  [3];  [1]; ORCiD logo [3]; ORCiD logo [1]
  1. Univ. of California, Merced, CA (United States)
  2. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  3. Univ. of Alabama, Huntsville, AL (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1543645
Grant/Contract Number:  
[AC02-05CH11231]
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
[ Journal Volume: 122; Journal Issue: 18]; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; chemistry; science & technology - other topics; materials science

Citation Formats

Grewal, Simranjit, Macedo Andrade, Angela, Nelson, Art J., Thai, Kevin, Karimaghaloo, Alireza, Lee, Eunseok, and Lee, Min Hwan. Critical Impact of Graphene Functionalization for Transition Metal Oxide/Graphene Hybrids on Oxygen Reduction Reaction. United States: N. p., 2018. Web. doi:10.1021/acs.jpcc.8b01893.
Grewal, Simranjit, Macedo Andrade, Angela, Nelson, Art J., Thai, Kevin, Karimaghaloo, Alireza, Lee, Eunseok, & Lee, Min Hwan. Critical Impact of Graphene Functionalization for Transition Metal Oxide/Graphene Hybrids on Oxygen Reduction Reaction. United States. doi:10.1021/acs.jpcc.8b01893.
Grewal, Simranjit, Macedo Andrade, Angela, Nelson, Art J., Thai, Kevin, Karimaghaloo, Alireza, Lee, Eunseok, and Lee, Min Hwan. Mon . "Critical Impact of Graphene Functionalization for Transition Metal Oxide/Graphene Hybrids on Oxygen Reduction Reaction". United States. doi:10.1021/acs.jpcc.8b01893. https://www.osti.gov/servlets/purl/1543645.
@article{osti_1543645,
title = {Critical Impact of Graphene Functionalization for Transition Metal Oxide/Graphene Hybrids on Oxygen Reduction Reaction},
author = {Grewal, Simranjit and Macedo Andrade, Angela and Nelson, Art J. and Thai, Kevin and Karimaghaloo, Alireza and Lee, Eunseok and Lee, Min Hwan},
abstractNote = {Transition metal oxides (TMOs) anchored on a carbon nanostructure have been widely pursued for oxygen reduction reaction (ORR) catalysis. The high ORR activity of TMO/graphene has been often attributed to the synergistic nature between TMO and carbon but with little relevant mechanistic study. In this report, the focus is made on how the type of majority oxygen-containing functional group of graphene affects the ORR performance of the resulting TMO/graphene nanocomposites. Our TiO2/carboxylated graphene and ZrO2/hydroxylated graphene rendered an ORR activity very close to that of Pt/C with an equal mass loading, via a four-electron transfer dominant process unlike other TMO/graphene variants of study. It is revealed that a stable anchoring of nanoparticles (NPs) on the graphene surface, which is essential to prevent the restacking of graphene layers, is established only through a specific type of functional groups on the graphene. In addition, the interplay among TMOs, graphene, and functional groups is found to be deterministic in the activity and electron transfer pathway of ORR, which is supported by density function theory (DFT) calculations. Finally, the calculations indicate that the electron transfer pathway is dependent upon the structure of NPs interfacing with functional groups of the graphene as it affects the preferred sites for oxygen dissociation.},
doi = {10.1021/acs.jpcc.8b01893},
journal = {Journal of Physical Chemistry. C},
number = [18],
volume = [122],
place = {United States},
year = {2018},
month = {4}
}

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