Detailed Characterization of an Annealed Reduced Graphene Oxide Catalyst for Selective Peroxide Formation Activity
Abstract
Recently, electrochemical hydrogen peroxide (H2O2) generation from oxygen molecules has been extensively studied. Thus far, the best peroxide activity under alkaline conditions has been reported at the surface of a mild reduced graphene oxide annealed at 600 °C (mrGO-600). However, the detailed material information, such as chemical functionality and structural morphology, is unknown, which results in ambiguous debates on its catalytic active sites. Therefore, to solve this problem, we intensively characterize the structure of mrGO-600 to clarify the origin of its catalytic activity. Various characterizations, including X-ray photoelectron spectroscopy, Raman spectroscopy, infrared spectroscopy, near-edge X-ray absorption fine spectroscopy, and high-resolution transmittance electron microscopy coupled with in situ infrared spectroelecrochemistry, reveal that the annealing process generates not only various hole edge defects that are related to the ring ether group but also numerous point defects that result in a small-sized disconnected graphitic carbon region. These defects are believed to form a unique atomic level configuration in mrGO-600, which enables it to facilitate high peroxide-generated activity from oxygen molecules in an alkaline electrolyte.
- Authors:
-
[3];
[5];
[1];
[2];
[6]
- Hanyang Univ., Seoul (South Korea)
- Sookmyung Women’s Univ., Seoul (South Korea)
- Soochow Univ., Suzhou (China). Inst. of Functional Nano & Soft Materials (FUNSOM), Joint International Research Lab. of Carbon-Based Functional Materials and Devices; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
- Kangwon National Univ., Samcheok (South Korea)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Univ. of California, Santa Cruz, CA (United States)
- Kangwon National Univ., Samcheok (South Korea); Univ. of California, Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Research Foundation of Korea (NRF)
- OSTI Identifier:
- 1838622
- Grant/Contract Number:
- AC02-05CH11231; 2019M2EA1064109
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Materials and Interfaces
- Additional Journal Information:
- Journal Volume: 12; Journal Issue: 41; 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; electrocatalyst; oxygen reduction reaction; reduced graphene oxide; carbon characterization; spectroelectrochemistry; redox reactions; oxides; infrared spectroscopy; carbon; oxygen
Citation Formats
Lee, Tae Hoon, Park, Sojung, Choi, Tae Hwan, Zhang, Liang, Kim, Juyoung, Guo, Jinghua, Park, Ho Bum, Kim, Wooyul, and Kim, Hyo Won. Detailed Characterization of an Annealed Reduced Graphene Oxide Catalyst for Selective Peroxide Formation Activity. United States: N. p., 2020.
Web. doi:10.1021/acsami.0c11359.
Lee, Tae Hoon, Park, Sojung, Choi, Tae Hwan, Zhang, Liang, Kim, Juyoung, Guo, Jinghua, Park, Ho Bum, Kim, Wooyul, & Kim, Hyo Won. Detailed Characterization of an Annealed Reduced Graphene Oxide Catalyst for Selective Peroxide Formation Activity. United States. https://doi.org/10.1021/acsami.0c11359
Lee, Tae Hoon, Park, Sojung, Choi, Tae Hwan, Zhang, Liang, Kim, Juyoung, Guo, Jinghua, Park, Ho Bum, Kim, Wooyul, and Kim, Hyo Won. Fri .
"Detailed Characterization of an Annealed Reduced Graphene Oxide Catalyst for Selective Peroxide Formation Activity". United States. https://doi.org/10.1021/acsami.0c11359. https://www.osti.gov/servlets/purl/1838622.
@article{osti_1838622,
title = {Detailed Characterization of an Annealed Reduced Graphene Oxide Catalyst for Selective Peroxide Formation Activity},
author = {Lee, Tae Hoon and Park, Sojung and Choi, Tae Hwan and Zhang, Liang and Kim, Juyoung and Guo, Jinghua and Park, Ho Bum and Kim, Wooyul and Kim, Hyo Won},
abstractNote = {Recently, electrochemical hydrogen peroxide (H2O2) generation from oxygen molecules has been extensively studied. Thus far, the best peroxide activity under alkaline conditions has been reported at the surface of a mild reduced graphene oxide annealed at 600 °C (mrGO-600). However, the detailed material information, such as chemical functionality and structural morphology, is unknown, which results in ambiguous debates on its catalytic active sites. Therefore, to solve this problem, we intensively characterize the structure of mrGO-600 to clarify the origin of its catalytic activity. Various characterizations, including X-ray photoelectron spectroscopy, Raman spectroscopy, infrared spectroscopy, near-edge X-ray absorption fine spectroscopy, and high-resolution transmittance electron microscopy coupled with in situ infrared spectroelecrochemistry, reveal that the annealing process generates not only various hole edge defects that are related to the ring ether group but also numerous point defects that result in a small-sized disconnected graphitic carbon region. These defects are believed to form a unique atomic level configuration in mrGO-600, which enables it to facilitate high peroxide-generated activity from oxygen molecules in an alkaline electrolyte.},
doi = {10.1021/acsami.0c11359},
journal = {ACS Applied Materials and Interfaces},
number = 41,
volume = 12,
place = {United States},
year = {Fri Oct 02 00:00:00 EDT 2020},
month = {Fri Oct 02 00:00:00 EDT 2020}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Mechanisms of Two-Electron and Four-Electron Electrochemical Oxygen Reduction Reactions at Nitrogen-Doped Reduced Graphene Oxide
journal, November 2019
- Kim, Hyo Won; Bukas, Vanessa J.; Park, Hun
- ACS Catalysis, Vol. 10, Issue 1
Raman spectroscopy of graphene and graphite: Disorder, electron–phonon coupling, doping and nonadiabatic effects
journal, July 2007
- Ferrari, Andrea C.
- Solid State Communications, Vol. 143, Issue 1-2, p. 47-57
Atomic Structure of Reduced Graphene Oxide
journal, April 2010
- Gómez-Navarro, Cristina; Meyer, Jannik C.; Sundaram, Ravi S.
- Nano Letters, Vol. 10, Issue 4
Determination of the Local Chemical Structure of Graphene Oxide and Reduced Graphene Oxide
journal, August 2010
- Erickson, Kris; Erni, Rolf; Lee, Zonghoon
- Advanced Materials, Vol. 22, Issue 40, p. 4467-4472
Tailoring the electrocatalytic oxygen reduction reaction pathway by tuning the electronic states of single-walled carbon nanotubes
journal, June 2019
- Hu, Rongtao; Wu, Chuxin; Hou, Kun
- Carbon, Vol. 147
Carbon Defect Characterization of Nitrogen-Doped Reduced Graphene Oxide Electrocatalysts for the Two-Electron Oxygen Reduction Reaction
journal, May 2019
- Kim, Hyo Won; Park, Hun; Roh, Ji Soo
- Chemistry of Materials, Vol. 31, Issue 11
Epitaxial Growth of Au-Pt-Ni Nanorods for Direct High Selectivity H 2 O 2 Production
journal, October 2016
- Zheng, Zhaoke; Ng, Yun Hau; Wang, Da-Wei
- Advanced Materials, Vol. 28, Issue 45
Electrocatalysts for O2 reduction
journal, November 1984
- Yeager, E.
- Electrochimica Acta, Vol. 29, Issue 11
Nitrogen doped carbon nanotubes synthesized from aliphatic diamines for oxygen reduction reaction
journal, January 2011
- Higgins, Drew; Chen, Zhu; Chen, Zhongwei
- Electrochimica Acta, Vol. 56, Issue 3
Soft X-ray Absorption Spectroscopy Studies of the Electronic Structure Recovery of Graphene Oxide upon Chemical Defunctionalization
journal, September 2012
- Lee, Vincent; Dennis, Robert V.; Schultz, Brian J.
- The Journal of Physical Chemistry C, Vol. 116, Issue 38
KOH-treated reduced graphene oxide: 100% selectivity for H2O2 electroproduction
journal, November 2019
- Zhu, Jingyi; Xiao, Xue; Zheng, Kai
- Carbon, Vol. 153
Defective Carbon-Based Materials for the Electrochemical Synthesis of Hydrogen Peroxide
journal, November 2017
- Chen, Shucheng; Chen, Zhihua; Siahrostami, Samira
- ACS Sustainable Chemistry & Engineering, Vol. 6, Issue 1
Electroless deposition of gold thin films on silicon for surface-enhanced infrared spectroelectrochemistry
journal, December 2002
- Miyake, Hiroto; Ye, Shen; Osawa, Masatoshi
- Electrochemistry Communications, Vol. 4, Issue 12
High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials
journal, January 2018
- Lu, Zhiyi; Chen, Guangxu; Siahrostami, Samira
- Nature Catalysis, Vol. 1, Issue 2
Nitrogen-Doped Graphene and Its Iron-Based Composite As Efficient Electrocatalysts for Oxygen Reduction Reaction
journal, October 2012
- Parvez, Khaled; Yang, Shubin; Hernandez, Yenny
- ACS Nano, Vol. 6, Issue 11
Understanding the high activity of mildly reduced graphene oxide electrocatalysts in oxygen reduction to hydrogen peroxide
journal, January 2019
- Tan, Xin; Tahini, Hassan A.; Smith, Sean C.
- Materials Horizons, Vol. 6, Issue 7
Restoration of graphene from graphene oxide by defect repair
journal, June 2012
- Cheng, Meng; Yang, Rong; Zhang, Lianchang
- Carbon, Vol. 50, Issue 7
Molecular-level origin of the carboxylate head group response to divalent metal ion complexation at the air–water interface
journal, July 2019
- Denton, Joanna K.; Kelleher, Patrick J.; Johnson, Mark A.
- Proceedings of the National Academy of Sciences, Vol. 116, Issue 30
Atomic and Electronic Structure of Graphene-Oxide
journal, March 2009
- Mkhoyan, K. Andre; Contryman, Alexander W.; Silcox, John
- Nano Letters, Vol. 9, Issue 3
In situ near-edge x-ray absorption fine structure spectroscopy investigation of the thermal defunctionalization of graphene oxide
journal, November 2012
- Lee, Vincent; Dennis, Robert V.; Jaye, Cherno
- Journal of Vacuum Science & Technology B, Nanotechnology and Microelectronics: Materials, Processing, Measurement, and Phenomena, Vol. 30, Issue 6
IR Spectroscopic Study of H 2 O 2 , HDO 2 , and D 2 O 2 Isolated in Ar, Kr, and Xe Matrices
journal, February 1997
- Pettersson, Mika; Tuominen, Susanna; Räsänen, Markku
- The Journal of Physical Chemistry A, Vol. 101, Issue 6
Efficient hydrogen peroxide generation using reduced graphene oxide-based oxygen reduction electrocatalysts
journal, March 2018
- Kim, Hyo Won; Ross, Michael B.; Kornienko, Nikolay
- Nature Catalysis, Vol. 1, Issue 4
Electronic structure and chemical bonding of a graphene oxide–sulfur nanocomposite for use in superior performance lithium–sulfur cells
journal, January 2012
- Zhang, Liang; Ji, Liwen; Glans, Per-Anders
- Physical Chemistry Chemical Physics, Vol. 14, Issue 39
Selective Electrochemical H 2 O 2 Production through Two-Electron Oxygen Electrochemistry
journal, September 2018
- Jiang, Yuanyuan; Ni, Pengjuan; Chen, Chuanxia
- Advanced Energy Materials, Vol. 8, Issue 31
Chemical Vapor Deposition Repair of Graphene Oxide: A Route to Highly-Conductive Graphene Monolayers
journal, August 2009
- López, Vicente; Sundaram, Ravi S.; Gómez-Navarro, Cristina
- Advanced Materials, Vol. 21, Issue 46
Electrocatalytic Production of Hydrogen Peroxide with Poly(3,4-ethylenedioxythiophene) Electrodes
journal, October 2018
- Mitraka, Evangelia; Gryszel, Maciej; Vagin, Mikhail
- Advanced Sustainable Systems, Vol. 3, Issue 2
Active Edge‐Site‐Rich Carbon Nanocatalysts with Enhanced Electron Transfer for Efficient Electrochemical Hydrogen Peroxide Production
journal, January 2019
- Sa, Young Jin; Kim, Jae Hyung; Joo, Sang Hoon
- Angewandte Chemie International Edition, Vol. 58, Issue 4
Unusual infrared-absorption mechanism in thermally reduced graphene oxide
journal, September 2010
- Acik, M.; Lee, G.; Mattevi, C.
- Nature Materials, Vol. 9, Issue 10
Exploration of the active center structure of nitrogen-doped graphene-based catalysts for oxygen reduction reaction
journal, January 2012
- Lai, Linfei; Potts, Jeffrey R.; Zhan, Da
- Energy & Environmental Science, Vol. 5, Issue 7
The Role of Oxygen during Thermal Reduction of Graphene Oxide Studied by Infrared Absorption Spectroscopy
journal, September 2011
- Acik, Muge; Lee, Geunsik; Mattevi, Cecilia
- The Journal of Physical Chemistry C, Vol. 115, Issue 40
Elucidation of the Mechanism of Dioxygen Reduction on Metal-Free Carbon Electrodes
journal, January 2000
- Yang, Hsueh-Hui; McCreery, Richard L.
- Journal of The Electrochemical Society, Vol. 147, Issue 9
Mussel-Inspired Surface Chemistry for Multifunctional Coatings
journal, October 2007
- Lee, H.; Dellatore, S. M.; Miller, W. M.
- Science, Vol. 318, Issue 5849
Combining theory and experiment in electrocatalysis: Insights into materials design
journal, January 2017
- Seh, Zhi Wei; Kibsgaard, Jakob; Dickens, Colin F.
- Science, Vol. 355, Issue 6321
Nitrogen-Doped Colloidal Graphene Quantum Dots and Their Size-Dependent Electrocatalytic Activity for the Oxygen Reduction Reaction
journal, November 2012
- Li, Qiqi; Zhang, Sheng; Dai, Liming
- Journal of the American Chemical Society, Vol. 134, Issue 46
Hydrogen Peroxide Synthesis: An Outlook beyond the Anthraquinone Process
journal, October 2006
- Campos-Martin, Jose M.; Blanco-Brieva, Gema; Fierro, Jose L. G.
- Angewandte Chemie International Edition, Vol. 45, Issue 42
Applications of Transition-Metal Catalysts to Textile and Wood-Pulp Bleaching
journal, January 2006
- Hage, Ronald; Lienke, Achim
- Angewandte Chemie International Edition, Vol. 45, Issue 2
Enhancing the production of hydrogen peroxide from electrocatalytic oxygen reduction reaction by tailoring the electronic states of single-walled carbon nanotubes: a synergistic effect from interior filling and exterior oxidation
journal, January 2019
- Hu, Rongtao; Yao, Fenfa; Wu, Chuxin
- Sustainable Energy & Fuels, Vol. 3, Issue 8
Combining Experiment and Theory To Unravel the Mechanism of Two-Electron Oxygen Reduction at a Selective and Active Co-catalyst
journal, October 2018
- Bukas, Vanessa J.; Kim, Hyo Won; Sengpiel, Robert
- ACS Catalysis, Vol. 8, Issue 12