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Title: Highly Active and Stable Graphene Tubes Decorated with FeCoNi Alloy Nanoparticles via a Template-Free Graphitization for Bifunctional Oxygen Reduction and Evolution

Abstract

Development of highly active and stable bifunctional oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) catalysts from earth–abundant elements remains a grand challenge for highly demanded reversible fuel cells and metal–air batteries. Carbon catalysts have many advantages over others due to their low cost, excellent electrical conductivity, high surface area, and easy functionalization. However, they typically cannot withstand the highly oxidative OER environment. Here, a new class of bifunctional electrocatalyst is reported, consisting of ultralarge sized nitrogen doped graphene tubes (N–GTs) (>500 nm) decorated with FeCoNi alloy particles. These tubes are prepared from an inexpensive precursor, dicyandiamide, via a template–free graphitization process. The ORR/OER activity and the stability of these graphene tube catalysts depend strongly on the transition metal precursors. The best performing FeCoNi–derived N–GT catalyst exhibits excellent ORR and OER activity along with adequate electrochemical durability over a wide potential window (0–1.9 V) in alkaline media. Here, the measured OER current is solely due to desirable O2 evolution, rather than carbon oxidation. Extensive electrochemical and physical characterization indicated that high graphitization degree, thicker tube walls, proper nitrogen doping, and presence of FeCoNi alloy particles are vital for high bifunctional activity and electrochemical durability of tubular carbon catalysts.

Authors:
 [1];  [1];  [2];  [2];  [3];  [1];  [1];  [1];  [1]
  1. University at Buffalo, State University of New York, Buffalo, NY (United States)
  2. Giner Inc, Newton, MA (United States)
  3. University of South Carolina, Columbia, SC (United States)
Publication Date:
Research Org.:
Giner, Inc., Newton, MA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Fuel Cell Technologies Office
OSTI Identifier:
1533063
Alternate Identifier(s):
OSTI ID: 1464414
Grant/Contract Number:  
EE0006960
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 6; Journal Issue: 22; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Chemistry; Energy & Fuels; Materials Science; Physics; Electrocatalysis; Graphene tubes; Oxygen evolution; Oxygen reduction; Reversible energy storage and conversion

Citation Formats

Gupta, Shiva, Qiao, Liang, Zhao, Shuai, Xu, Hui, Lin, Ye, Devaguptapu, Surya V., Wang, Xianliang, Swihart, Mark T., and Wu, Gang. Highly Active and Stable Graphene Tubes Decorated with FeCoNi Alloy Nanoparticles via a Template-Free Graphitization for Bifunctional Oxygen Reduction and Evolution. United States: N. p., 2016. Web. https://doi.org/10.1002/aenm.201601198.
Gupta, Shiva, Qiao, Liang, Zhao, Shuai, Xu, Hui, Lin, Ye, Devaguptapu, Surya V., Wang, Xianliang, Swihart, Mark T., & Wu, Gang. Highly Active and Stable Graphene Tubes Decorated with FeCoNi Alloy Nanoparticles via a Template-Free Graphitization for Bifunctional Oxygen Reduction and Evolution. United States. https://doi.org/10.1002/aenm.201601198
Gupta, Shiva, Qiao, Liang, Zhao, Shuai, Xu, Hui, Lin, Ye, Devaguptapu, Surya V., Wang, Xianliang, Swihart, Mark T., and Wu, Gang. Tue . "Highly Active and Stable Graphene Tubes Decorated with FeCoNi Alloy Nanoparticles via a Template-Free Graphitization for Bifunctional Oxygen Reduction and Evolution". United States. https://doi.org/10.1002/aenm.201601198. https://www.osti.gov/servlets/purl/1533063.
@article{osti_1533063,
title = {Highly Active and Stable Graphene Tubes Decorated with FeCoNi Alloy Nanoparticles via a Template-Free Graphitization for Bifunctional Oxygen Reduction and Evolution},
author = {Gupta, Shiva and Qiao, Liang and Zhao, Shuai and Xu, Hui and Lin, Ye and Devaguptapu, Surya V. and Wang, Xianliang and Swihart, Mark T. and Wu, Gang},
abstractNote = {Development of highly active and stable bifunctional oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) catalysts from earth–abundant elements remains a grand challenge for highly demanded reversible fuel cells and metal–air batteries. Carbon catalysts have many advantages over others due to their low cost, excellent electrical conductivity, high surface area, and easy functionalization. However, they typically cannot withstand the highly oxidative OER environment. Here, a new class of bifunctional electrocatalyst is reported, consisting of ultralarge sized nitrogen doped graphene tubes (N–GTs) (>500 nm) decorated with FeCoNi alloy particles. These tubes are prepared from an inexpensive precursor, dicyandiamide, via a template–free graphitization process. The ORR/OER activity and the stability of these graphene tube catalysts depend strongly on the transition metal precursors. The best performing FeCoNi–derived N–GT catalyst exhibits excellent ORR and OER activity along with adequate electrochemical durability over a wide potential window (0–1.9 V) in alkaline media. Here, the measured OER current is solely due to desirable O2 evolution, rather than carbon oxidation. Extensive electrochemical and physical characterization indicated that high graphitization degree, thicker tube walls, proper nitrogen doping, and presence of FeCoNi alloy particles are vital for high bifunctional activity and electrochemical durability of tubular carbon catalysts.},
doi = {10.1002/aenm.201601198},
journal = {Advanced Energy Materials},
number = 22,
volume = 6,
place = {United States},
year = {2016},
month = {8}
}

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