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

doi:10.1021/acs.jpcc.8b01893

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

Full Record
Other Related Research

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 »« less

Authors:

Grewal, Simranjit ^[1]; Macedo Andrade, Angela ^[1]; Nelson, Art J. ^[2]; Thai, Kevin ^[3]; Karimaghaloo, Alireza ^[1];

^[3];

^[1]

Univ. of California, Merced, CA (United States)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Univ. of Alabama, Huntsville, AL (United States)

Publication Date:: 2018-04-23

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.

Copy to clipboard


                    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.

Copy to clipboard


                    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.

Copy to clipboard


                    
@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}

}

Copy to clipboard

Journal Article:

Free Publicly Available Full Text

Accepted Manuscript (DOE)

Publisher's Version of Record

DOI: 10.1021/acs.jpcc.8b01893

Other availability

Search WorldCat to find libraries that may hold this journal

Citation Metrics:

Cited by: 2 works

Citation information provided by
Web of Science

Save / Share:

Export Metadata

Save to My Library

Similar Records in DOE PAGES and OSTI.GOV collections:

Probing the nature of electron transfer in metalloproteins on graphene-family materials as nanobiocatalytic scaffold using electrochemistry

Journal Article Gupta, Sanju ; Biotechnology Center, Western Kentucky University, 1906 College Heights Blvd. Bowling Green, KY 42101-3576 ; Irihamye, Aline - AIP Advances

Graphene-based nanomaterials have shown great promise not only in nanoelectronics due to ultrahigh electron mobility but also as biocatalytic scaffolds owing to irreversible protein surface adsorption and facilitating direct electron transfer. In this work, we synthesized stable dispersions of graphene using liquid-phase exfoliation approach based on non-covalent interactions between graphene and 1-pyrenesulfonic acid sodium salt (Py–1SO{sub 3}), 1-pyrenemethylamine salt (Py − Me-NH{sub 2}) and Pluronic{sup ®} P-123 surfactant using only water as solvent compatible with biomolecules. The resulting graphene nanoplatelets (Gr-LPE) are characterized by a combination of analytical (microscopy and spectroscopy) techniques revealing mono- to few-layer graphene displaying that themore »« less
DOI: 10.1063/1.4914186
Synergistic enhancement of nitrogen and sulfur co-doped graphene with carbon nanospheres insertion for electrocatalytic oxygen reduction reaction

Journal Article Wu, Min ; Xin, Huolin L. ; Wang, Jie ; ... - Journal of Materials Chemistry. A

A nitrogen and sulfur co-doped graphene/carbon black (NSGCB) nanocomposite for the oxygen reduction reaction (ORR) was synthesized through a one-pot annealing of a precursor mixture containing graphene oxide, thiourea, and acidized carbon black (CB). The NSGCB showed excellent performance for the ORR with the onset and half-way potentials at 0.96 V and 0.81 V (vs. RHE), respectively. It is significantly improved over that of the catalysts derived from only graphene (0.90 V and 0.76 V) or carbon nanosphere (0.82 V and 0.74 V). The enhanced catalytic activity on the NSGCB electrode could be attributed to the synergistic effect of N/Smore »« less
Cited by 23
DOI: 10.1039/C4TA06323F

Full Text Available
Mechanisms of Two-Electron and Four-Electron Electrochemical Oxygen Reduction Reactions at Nitrogen-Doped Reduced Graphene Oxide

Journal Article Kim, Hyo Won ; Bukas, Vanessa J. ; Park, Hun ; ... - ACS Catalysis

Doped carbon-based systems have been extensively studied over the past decade as active electrocatalysts for both the two-electron (2e–) and four-electron (4e–) oxygen reduction reactions (ORRs). However, the mechanisms for ORR are generally poorly understood. Here, we report an extensive experimental and first-principles theoretical study of the ORR at nitrogen-doped reduced graphene oxide (NrGO). We synthesize three distinct NrGO catalysts and investigate their chemical and structural properties in detail via X-ray photoelectron spectroscopy, infrared and Raman spectroscopies, high-resolution transmission electron microscopy, and thin-film electrical conductivity. ORR experiments include the pH dependences of 2e– versus 4e– ORR selectivity, ORR onset potentials,more »« less
DOI: 10.1021/acscatal.9b04106
Highly regenerable carbon-Fe{sub 3}O{sub 4} core–satellite nanospheres as oxygen reduction electrocatalyst and magnetic adsorbent

Journal Article Zhou, Wenqiang ; School of Materials Science and Engineering, Jiangsu University of Science and Technology, Zhenjiang 212003 ; Liu, Minmin ; ... - Journal of Solid State Chemistry

We present the synthesis and multifunctional utilization of core-satellite carbon-Fe{sub 3}O{sub 4} nanoparticles to serve as the enabling platform for a range of applications including oxygen reduction reaction (ORR) and magnetic adsorbent. Starting from polydopamine (PDA) nanoparticles and Fe(NO{sub 3}){sub 3}, carbon-Fe{sub 3}O{sub 4} core–satellite nanospheres are synthesized through successive steps of impregnation, ammoniation and carbonization. The synergistic combination of Fe{sub 3}O{sub 4} and N-doped carbon endows the nanocomposite with high electrochemical activity in ORR and mainly four electrons transferred in reaction process. Furthermore, carbon-Fe{sub 3}O{sub 4} nanoparticles used as magnetic adsorbent exhibit the efficient removal of Rhodamine B frommore »« less
DOI: 10.1016/J.JSSC.2016.12.014
Development of Novel Non-Pt Group Metal Electrocatalysts for PEM Fuel Cell Applications

Technical Report Mukerjee, Sanjeev ; Atanassov, Plamen ; Barton, Scott ; ...

The objective of this multi-institutional effort was to comprehensively pursue the goal of eliminating noble metal (Pt group metals, PGM) from the cathodic oxygen reduction reaction (ORR) electrode thereby providing a quantum leap in lowering the overall PGM loading in a polymer electrolyte fuel cell (PEMFC). The overall project scope encompassed (a) comprehensive materials discovery effort, (b) a concomitant effort to scale up these materials with very high ( ±5%) reproducibility, both intra and inter, (c) understanding mass transport in porous medium both in gas diffusion and micro-porous layers for enhanced areal activity, (d) understanding mechanistic aspects of active sitemore »« less
DOI: 10.2172/1332697

Full Text Available

Similar Records