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Title: Boron- and Nitrogen-Substituted Graphene Nanoribbons as Efficient Catalysts for Oxygen Reduction Reaction

Abstract

Here, we show that nanoribbons of boron- and nitrogen-substituted graphene can be used as efficient electrocatalysts for the oxygen reduction reaction (ORR). Optimally doped graphene nanoribbons made into three-dimensional porous constructs exhibit the highest onset and half-wave potentials among the reported metal-free catalysts for this reaction and show superior performance compared to commercial Pt/C catalyst. Moreover, this catalyst possesses high kinetic current density and four-electron transfer pathway with low hydrogen peroxide yield during the reaction. Finally, first-principles calculations suggest that such excellent electrocatalytic properties originate from the abundant edges of boron- and nitrogen-codoped graphene nanoribbons, which significantly reduce the energy barriers of the rate-determining steps of the ORR reaction.

Authors:
 [1];  [1];  [1];  [2];  [3];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Rice Univ., Houston, TX (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Rice Univ., Houston, TX (United States); Beihang Univ., Beijing (China)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1185918
Grant/Contract Number:  
AC05-00OR22725; DMR-0928297; W911NF-11-1-032; FA9550-09-1-0581; FA9550-12-1-0035; N000014-09-1-1066; OCI-0959097
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 27; Journal Issue: 4; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Gong, Yongji, Fei, Huilong, Zou, Xiaolong, Zhou, Wu, Yang, Shubin, Ye, Gonglan, Liu, Zheng, Peng, Zhiwei, Lou, Jun, Vajtai, Robert, Yakobson, Boris I., Tour, James M., and Ajayan, Pulickel M. Boron- and Nitrogen-Substituted Graphene Nanoribbons as Efficient Catalysts for Oxygen Reduction Reaction. United States: N. p., 2015. Web. doi:10.1021/cm5037502.
Gong, Yongji, Fei, Huilong, Zou, Xiaolong, Zhou, Wu, Yang, Shubin, Ye, Gonglan, Liu, Zheng, Peng, Zhiwei, Lou, Jun, Vajtai, Robert, Yakobson, Boris I., Tour, James M., & Ajayan, Pulickel M. Boron- and Nitrogen-Substituted Graphene Nanoribbons as Efficient Catalysts for Oxygen Reduction Reaction. United States. doi:10.1021/cm5037502.
Gong, Yongji, Fei, Huilong, Zou, Xiaolong, Zhou, Wu, Yang, Shubin, Ye, Gonglan, Liu, Zheng, Peng, Zhiwei, Lou, Jun, Vajtai, Robert, Yakobson, Boris I., Tour, James M., and Ajayan, Pulickel M. Mon . "Boron- and Nitrogen-Substituted Graphene Nanoribbons as Efficient Catalysts for Oxygen Reduction Reaction". United States. doi:10.1021/cm5037502. https://www.osti.gov/servlets/purl/1185918.
@article{osti_1185918,
title = {Boron- and Nitrogen-Substituted Graphene Nanoribbons as Efficient Catalysts for Oxygen Reduction Reaction},
author = {Gong, Yongji and Fei, Huilong and Zou, Xiaolong and Zhou, Wu and Yang, Shubin and Ye, Gonglan and Liu, Zheng and Peng, Zhiwei and Lou, Jun and Vajtai, Robert and Yakobson, Boris I. and Tour, James M. and Ajayan, Pulickel M.},
abstractNote = {Here, we show that nanoribbons of boron- and nitrogen-substituted graphene can be used as efficient electrocatalysts for the oxygen reduction reaction (ORR). Optimally doped graphene nanoribbons made into three-dimensional porous constructs exhibit the highest onset and half-wave potentials among the reported metal-free catalysts for this reaction and show superior performance compared to commercial Pt/C catalyst. Moreover, this catalyst possesses high kinetic current density and four-electron transfer pathway with low hydrogen peroxide yield during the reaction. Finally, first-principles calculations suggest that such excellent electrocatalytic properties originate from the abundant edges of boron- and nitrogen-codoped graphene nanoribbons, which significantly reduce the energy barriers of the rate-determining steps of the ORR reaction.},
doi = {10.1021/cm5037502},
journal = {Chemistry of Materials},
number = 4,
volume = 27,
place = {United States},
year = {2015},
month = {2}
}

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