Carbon Defect Characterization of Nitrogen-Doped Reduced Graphene Oxide Electrocatalysts for the Two-Electron Oxygen Reduction Reaction

Hyo Won Kim, Hun Park, Ji Soo Roh, Jae Eun Shin, Tae Hoon Lee, Liang Zhang, Young Hoon Cho, Hee Wook Yoon, Vanessa J. Bukas, Jinghua Guo, Ho Bum Park, Tae Hee Han, Bryan D. McCloskey

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Abstract

Numerous modified-carbon catalysts have been developed for the direct synthesis of hydrogen peroxide through electrochemical oxygen reduction. However, given the complex structure of most porous carbons and the poor oxygen reduction reaction (ORR) selectivity typically observed when they are used as catalysts, it is still unclear which carbon defects are responsible for the high two-electron ORR activity typically observed in these materials. Here, we study electrocatalytic peroxide formation activity of nitrogen-doped reduced graphene oxide (N-rGO) materials to relate carbon defects to electrocatalytic activity. To do so, we selected two N-rGO electrodes that selectively produce peroxide at all potentials studied (0.70-0.10 V vs RHE) under alkaline conditions. Oxygen reduction studies, combined with material characterization, especially solid-state 13carbon nuclear magnetic resonance coupled with magic angle spinning and cross-polarization, demonstrate that epoxy or ether groups in the N-rGO catalyst are likely associated with the active sites that form peroxide at the lowest overpotential in alkaline media.

Original languageEnglish
Pages (from-to)3967-3973
Number of pages7
JournalChemistry of Materials
Volume31
Issue number11
DOIs
StatePublished - 2019 Jun 11

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Graphite
Electrocatalysts
Oxides
Graphene
Peroxides
Nitrogen
Carbon
Oxygen
Defects
Electrons
Catalysts
Magic angle spinning
Catalyst selectivity
Hydrogen peroxide
Ether
Hydrogen Peroxide
Ethers
Nuclear magnetic resonance
Polarization
Electrodes

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Kim, Hyo Won ; Park, Hun ; Roh, Ji Soo ; Shin, Jae Eun ; Lee, Tae Hoon ; Zhang, Liang ; Cho, Young Hoon ; Yoon, Hee Wook ; Bukas, Vanessa J. ; Guo, Jinghua ; Park, Ho Bum ; Han, Tae Hee ; McCloskey, Bryan D. / Carbon Defect Characterization of Nitrogen-Doped Reduced Graphene Oxide Electrocatalysts for the Two-Electron Oxygen Reduction Reaction. In: Chemistry of Materials. 2019 ; Vol. 31, No. 11. pp. 3967-3973.
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abstract = "Numerous modified-carbon catalysts have been developed for the direct synthesis of hydrogen peroxide through electrochemical oxygen reduction. However, given the complex structure of most porous carbons and the poor oxygen reduction reaction (ORR) selectivity typically observed when they are used as catalysts, it is still unclear which carbon defects are responsible for the high two-electron ORR activity typically observed in these materials. Here, we study electrocatalytic peroxide formation activity of nitrogen-doped reduced graphene oxide (N-rGO) materials to relate carbon defects to electrocatalytic activity. To do so, we selected two N-rGO electrodes that selectively produce peroxide at all potentials studied (0.70-0.10 V vs RHE) under alkaline conditions. Oxygen reduction studies, combined with material characterization, especially solid-state 13carbon nuclear magnetic resonance coupled with magic angle spinning and cross-polarization, demonstrate that epoxy or ether groups in the N-rGO catalyst are likely associated with the active sites that form peroxide at the lowest overpotential in alkaline media.",
author = "Kim, {Hyo Won} and Hun Park and Roh, {Ji Soo} and Shin, {Jae Eun} and Lee, {Tae Hoon} and Liang Zhang and Cho, {Young Hoon} and Yoon, {Hee Wook} and Bukas, {Vanessa J.} and Jinghua Guo and Park, {Ho Bum} and Han, {Tae Hee} and McCloskey, {Bryan D.}",
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Kim, HW, Park, H, Roh, JS, Shin, JE, Lee, TH, Zhang, L, Cho, YH, Yoon, HW, Bukas, VJ, Guo, J, Park, HB, Han, TH & McCloskey, BD 2019, 'Carbon Defect Characterization of Nitrogen-Doped Reduced Graphene Oxide Electrocatalysts for the Two-Electron Oxygen Reduction Reaction', Chemistry of Materials, vol. 31, no. 11, pp. 3967-3973. https://doi.org/10.1021/acs.chemmater.9b00210

Carbon Defect Characterization of Nitrogen-Doped Reduced Graphene Oxide Electrocatalysts for the Two-Electron Oxygen Reduction Reaction. / Kim, Hyo Won; Park, Hun; Roh, Ji Soo; Shin, Jae Eun; Lee, Tae Hoon; Zhang, Liang; Cho, Young Hoon; Yoon, Hee Wook; Bukas, Vanessa J.; Guo, Jinghua; Park, Ho Bum; Han, Tae Hee; McCloskey, Bryan D.

In: Chemistry of Materials, Vol. 31, No. 11, 11.06.2019, p. 3967-3973.

Research output: Contribution to journalArticleResearchpeer-review

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T1 - Carbon Defect Characterization of Nitrogen-Doped Reduced Graphene Oxide Electrocatalysts for the Two-Electron Oxygen Reduction Reaction

AU - Kim, Hyo Won

AU - Park, Hun

AU - Roh, Ji Soo

AU - Shin, Jae Eun

AU - Lee, Tae Hoon

AU - Zhang, Liang

AU - Cho, Young Hoon

AU - Yoon, Hee Wook

AU - Bukas, Vanessa J.

AU - Guo, Jinghua

AU - Park, Ho Bum

AU - Han, Tae Hee

AU - McCloskey, Bryan D.

PY - 2019/6/11

Y1 - 2019/6/11

N2 - Numerous modified-carbon catalysts have been developed for the direct synthesis of hydrogen peroxide through electrochemical oxygen reduction. However, given the complex structure of most porous carbons and the poor oxygen reduction reaction (ORR) selectivity typically observed when they are used as catalysts, it is still unclear which carbon defects are responsible for the high two-electron ORR activity typically observed in these materials. Here, we study electrocatalytic peroxide formation activity of nitrogen-doped reduced graphene oxide (N-rGO) materials to relate carbon defects to electrocatalytic activity. To do so, we selected two N-rGO electrodes that selectively produce peroxide at all potentials studied (0.70-0.10 V vs RHE) under alkaline conditions. Oxygen reduction studies, combined with material characterization, especially solid-state 13carbon nuclear magnetic resonance coupled with magic angle spinning and cross-polarization, demonstrate that epoxy or ether groups in the N-rGO catalyst are likely associated with the active sites that form peroxide at the lowest overpotential in alkaline media.

AB - Numerous modified-carbon catalysts have been developed for the direct synthesis of hydrogen peroxide through electrochemical oxygen reduction. However, given the complex structure of most porous carbons and the poor oxygen reduction reaction (ORR) selectivity typically observed when they are used as catalysts, it is still unclear which carbon defects are responsible for the high two-electron ORR activity typically observed in these materials. Here, we study electrocatalytic peroxide formation activity of nitrogen-doped reduced graphene oxide (N-rGO) materials to relate carbon defects to electrocatalytic activity. To do so, we selected two N-rGO electrodes that selectively produce peroxide at all potentials studied (0.70-0.10 V vs RHE) under alkaline conditions. Oxygen reduction studies, combined with material characterization, especially solid-state 13carbon nuclear magnetic resonance coupled with magic angle spinning and cross-polarization, demonstrate that epoxy or ether groups in the N-rGO catalyst are likely associated with the active sites that form peroxide at the lowest overpotential in alkaline media.

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JO - Chemistry of Materials

JF - Chemistry of Materials

SN - 0897-4756

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