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Title: Nitrogen and Fluorine-Codoped Carbon Nanowire Aerogels as Metal-Free Electrocatalysts for Oxygen Reduction Reaction

Abstract

The development of active, durable, and low-cost catalysts to replace noble metal-based materials is highly desirable to promote the sluggish oxygen reduction reaction in fuel cells. Herein, nitrogen and fluorine-codoped three-dimensional carbon nanowire aerogels, composed of interconnected carbon nanowires, were synthesized for the first time by a hydrothermal carbonization process. Owing to their porous nanostructures and heteroatom-doping, the as-prepared carbon nanowire aerogels, with optimized composition, present excellent electrocatalytic activity that is comparable to commercial Pt/C. Remarkably, the aerogels also exhibit superior stability and methanol tolerance. This synthesis procedure paves a new way to design novel heteroatomdoped catalysts.

Authors:
 [1]; ORCiD logo [1];  [1];  [2];  [3];  [1]; ORCiD logo [1]
  1. School of Mechanical and Materials Engineering, Washington State University, Pullman, WA 99164 USA
  2. Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, Richland WA 99352 USA
  3. Energy and Environmental Directory, Pacific Northwest National Laboratory, Richland WA 99352 USA
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1378010
Report Number(s):
PNNL-SA-128735
Journal ID: ISSN 0947-6539; 48877; KP1704020
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Chemistry - A European Journal; Journal Volume: 23; Journal Issue: 43
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; Environmental Molecular Sciences Laboratory

Citation Formats

Fu, Shaofang, Zhu, Chengzhou, Song, Junhua, Engelhard, Mark H., Xiao, Biwei, Du, Dan, and Lin, Yuehe. Nitrogen and Fluorine-Codoped Carbon Nanowire Aerogels as Metal-Free Electrocatalysts for Oxygen Reduction Reaction. United States: N. p., 2017. Web. doi:10.1002/chem.201701969.
Fu, Shaofang, Zhu, Chengzhou, Song, Junhua, Engelhard, Mark H., Xiao, Biwei, Du, Dan, & Lin, Yuehe. Nitrogen and Fluorine-Codoped Carbon Nanowire Aerogels as Metal-Free Electrocatalysts for Oxygen Reduction Reaction. United States. doi:10.1002/chem.201701969.
Fu, Shaofang, Zhu, Chengzhou, Song, Junhua, Engelhard, Mark H., Xiao, Biwei, Du, Dan, and Lin, Yuehe. Tue . "Nitrogen and Fluorine-Codoped Carbon Nanowire Aerogels as Metal-Free Electrocatalysts for Oxygen Reduction Reaction". United States. doi:10.1002/chem.201701969.
@article{osti_1378010,
title = {Nitrogen and Fluorine-Codoped Carbon Nanowire Aerogels as Metal-Free Electrocatalysts for Oxygen Reduction Reaction},
author = {Fu, Shaofang and Zhu, Chengzhou and Song, Junhua and Engelhard, Mark H. and Xiao, Biwei and Du, Dan and Lin, Yuehe},
abstractNote = {The development of active, durable, and low-cost catalysts to replace noble metal-based materials is highly desirable to promote the sluggish oxygen reduction reaction in fuel cells. Herein, nitrogen and fluorine-codoped three-dimensional carbon nanowire aerogels, composed of interconnected carbon nanowires, were synthesized for the first time by a hydrothermal carbonization process. Owing to their porous nanostructures and heteroatom-doping, the as-prepared carbon nanowire aerogels, with optimized composition, present excellent electrocatalytic activity that is comparable to commercial Pt/C. Remarkably, the aerogels also exhibit superior stability and methanol tolerance. This synthesis procedure paves a new way to design novel heteroatomdoped catalysts.},
doi = {10.1002/chem.201701969},
journal = {Chemistry - A European Journal},
number = 43,
volume = 23,
place = {United States},
year = {Tue Jul 11 00:00:00 EDT 2017},
month = {Tue Jul 11 00:00:00 EDT 2017}
}
  • Te nanowires were used as template to synthesize N,S-codoped carbon nanowires. Enhanced electrocatalytic performance on oxygen reduction was demonstrated.
  • As one of the alternatives to replace precious metal catalysts, transition metal-nitrogen-carbon (M-N-C) electrocatalysts have attracted great research interest due to their low cost and good catalytic activities. Despite nanostructured M-N-C catalysts can achieve good electrochemical performances, they are vulnerable to aggregation and insufficient catalytic sites upon continuous catalytic reaction. Thus, M-N-C’s stability and selectivity have not been comparable to their noble metal counterparts. In this work, metal-organic frameworks (MOFs)-derived porous single-atom electrocatalysts (SAEs) were successfully prepared by simple pyrolysis procedure without any further post-treatment. Combining the X-ray absorption near-edge spectroscopy (XANES) and electrochemical measurements, the SAEs have been identifiedmore » with superior ORR activity and stability compared with Pt/C catalysts in alkaline condition. More impressively, the SAEs also show excellent ORR electrocatalytic performance in both acid and neutral media. Furthermore, this study of nonprecious catalysts provides new insights on nano-engineering catalytically active sites and porous structures for nonprecious metal ORR catalysis in a wide range of pH.« less
  • As one of the alternatives to replace precious metal catalysts, transition-metal–nitrogen–carbon (M–N–C) electrocatalysts have attracted great research interest due to their low cost and good catalytic activities. Despite nanostructured M–N–C catalysts can achieve good electrochemical perfor-mances, they are vulnerable to aggregation and insufficient catalytic sites upon continuous catalytic reaction. In this work, metal–organic frameworks derived porous single-atom electrocatalysts (SAEs) were successfully prepared by simple pyrolysis procedure without any further posttreatment. Combining the X-ray absorption near-edge spectroscopy and electrochemical measure-ments, the SAEs have been identified with superior oxygen reduction reaction (ORR) activity and stability compared with Pt/C catalysts in alkaline condition.more » More impressively, the SAEs also show excellent ORR electrocatalytic perfor-mance in both acid and neutral media. This study of nonprecious catalysts provides new insights on nanoengineering catalytically active sites and porous structures for nonprecious metal ORR catalysis in a wide range of pH.« less
  • Finely controlled synthesis of high active and robust non-precious metal catalysts with excellent electrocatalytic efficiency towards oxygen reduction reaction is extremely vital for successful implementation of fuel cells and metal batteries. Unprecedented oxygen reduction reaction electrocatalytic performances and the diversified synthetic procedure in term of favorable structure/morphology characteristics make transition metals-derived M–N–C (M=Fe, Co) structures the most promising nanocatalysts. Herein, using the nitrogen-containing small molecular and inorganic salt as precursors and ultrathin tellurium nanowires as templates, we successfully synthesized a series of well-defined M-N-doped hollow carbon nanowire aerogels through one step hydrothermal route and subsequent facile annealing treatment. Taking advantagemore » of the porous nanostructures, one-dimensional building block as well as homogeneity of active sites, the resultant Fe-N-doped carbon hollow nanowire aerogels exhibited excellent ORR electrocatalytic performance even better than commercial Pt/C in alkaline solution, holding great potential in fuel cell applications.« less