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Title: Self-Assembled Fe-N-Doped Carbon Nanotube Aerogels with Single-Atom Catalyst Feature as High-Efficiency Oxygen Reduction Electrocatalysts

Abstract

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 advantage 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.

Authors:
 [1];  [1];  [1];  [1];  [2];  [3];  [4];  [3];  [3];  [4];  [1];  [5]
  1. School of Mechanical and Materials Engineering, Washington State University, Pullman WA 99164 USA
  2. Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton NY 11973 USA
  3. Environmental Molecular Science Laboratory, Pacific Northwest National Laboratory, Richland WA 99354 USA
  4. Energy and Environmental Directory, Pacific Northwest National Laboratory, Richland WA 99354 USA
  5. School of Mechanical and Materials Engineering, Washington State University, Pullman WA 99164 USA; Environmental Molecular Science Laboratory, Pacific Northwest National Laboratory, Richland WA 99354 USA
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1355090
Report Number(s):
PNNL-SA-119038
Journal ID: ISSN 1613-6810; 48877; KC0203020
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Small; Journal Volume: 13; Journal Issue: 15
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

Citation Formats

Zhu, Chengzhou, Fu, Shaofang, Song, Junhua, Shi, Qiurong, Su, Dong, Engelhard, Mark H., Li, Xiaolin, Xiao, Dongdong, Li, Dongsheng, Estevez, Luis, Du, Dan, and Lin, Yuehe. Self-Assembled Fe-N-Doped Carbon Nanotube Aerogels with Single-Atom Catalyst Feature as High-Efficiency Oxygen Reduction Electrocatalysts. United States: N. p., 2017. Web. doi:10.1002/smll.201603407.
Zhu, Chengzhou, Fu, Shaofang, Song, Junhua, Shi, Qiurong, Su, Dong, Engelhard, Mark H., Li, Xiaolin, Xiao, Dongdong, Li, Dongsheng, Estevez, Luis, Du, Dan, & Lin, Yuehe. Self-Assembled Fe-N-Doped Carbon Nanotube Aerogels with Single-Atom Catalyst Feature as High-Efficiency Oxygen Reduction Electrocatalysts. United States. doi:10.1002/smll.201603407.
Zhu, Chengzhou, Fu, Shaofang, Song, Junhua, Shi, Qiurong, Su, Dong, Engelhard, Mark H., Li, Xiaolin, Xiao, Dongdong, Li, Dongsheng, Estevez, Luis, Du, Dan, and Lin, Yuehe. Mon . "Self-Assembled Fe-N-Doped Carbon Nanotube Aerogels with Single-Atom Catalyst Feature as High-Efficiency Oxygen Reduction Electrocatalysts". United States. doi:10.1002/smll.201603407.
@article{osti_1355090,
title = {Self-Assembled Fe-N-Doped Carbon Nanotube Aerogels with Single-Atom Catalyst Feature as High-Efficiency Oxygen Reduction Electrocatalysts},
author = {Zhu, Chengzhou and Fu, Shaofang and Song, Junhua and Shi, Qiurong and Su, Dong and Engelhard, Mark H. and Li, Xiaolin and Xiao, Dongdong and Li, Dongsheng and Estevez, Luis and Du, Dan and Lin, Yuehe},
abstractNote = {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 advantage 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.},
doi = {10.1002/smll.201603407},
journal = {Small},
number = 15,
volume = 13,
place = {United States},
year = {Mon Feb 06 00:00:00 EST 2017},
month = {Mon Feb 06 00:00:00 EST 2017}
}
  • In this study, self-assembled M–N-doped carbon nanotube aerogels with single-atom catalyst feature are for the first time reported through one-step hydrothermal route and subsequent facile annealing treatment. By taking advantage of the porous nanostructures, 1D nanotubes as well as single-atom catalyst feature, the resultant Fe–N-doped carbon nanotube aerogels exhibit excellent oxygen reduction reaction electrocatalytic performance even better than commercial Pt/C in alkaline solution.
  • 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.
  • A simple and easily processible photovoltaic device has been developed based on borondoped single-walled carbon nanotubes (B-SWNTs) and n-type silicon (n-Si) heterojunctions. The single-walled carbon nanotubes (SWNTs) were substitutionally doped with boron atoms by thermal annealing, in the presence of B 2O 3. The samples used for these studies were characterized by Raman spectroscopy, thermal gravimetric analysis (TGA), transmission electron microscopy (TEM), and x-ray photoelectron spectroscopy (XPS). The fully functional solar cell devices were fabricated by airbrush deposition that generated uniform B-SWNT films on top of the n-Si substrates. The carbon nanotube films acted as exciton-generation sites, charge collection andmore » transportation, while the heterojunctions formed between B-SWNTs and n-Si acted as charge dissociation centers. The current-voltage characteristics in the absence of light and under illumination, as well as optical transmittance spectrum are reported here. It should be noted that the device fabrication process can be made amenable to scalability by depositing direct and uniform films using airbrushing, inkjet printing, or spin-coating techniques.« less