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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

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.

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.:
Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1347291
Report Number(s):
BNL-113588-2017-JA
Journal ID: ISSN 1613-6810; R&D Project: 16060; 16060; KC0403020
Grant/Contract Number:  
SC00112704; AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Small
Additional Journal Information:
Journal Volume: 13; Journal Issue: 15; Journal ID: ISSN 1613-6810
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Aerogels; transition metal–nitrogen–carbon structures; single-atom catalysts; nonprecious metal catalysts; oxygen reduction reaction

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. https://doi.org/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. https://doi.org/10.1002/smll.201603407. https://www.osti.gov/servlets/purl/1347291.
@article{osti_1347291,
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 = {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.},
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}
}

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Works referenced in this record:

Macroscopic-Scale Template Synthesis of Robust Carbonaceous Nanofiber Hydrogels and Aerogels and Their Applications
journal, April 2012

  • Liang, Hai-Wei; Guan, Qing-Fang; Chen, Li-Feng
  • Angewandte Chemie International Edition, Vol. 51, Issue 21
  • DOI: 10.1002/anie.201200710

Identification of catalytic sites for oxygen reduction in iron- and nitrogen-doped graphene materials
journal, August 2015

  • Zitolo, Andrea; Goellner, Vincent; Armel, Vanessa
  • Nature Materials, Vol. 14, Issue 9
  • DOI: 10.1038/nmat4367

Atomic cobalt on nitrogen-doped graphene for hydrogen generation
journal, October 2015

  • Fei, Huilong; Dong, Juncai; Arellano-Jiménez, M. Josefina
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9668

Self-Supporting Oxygen Reduction Electrocatalysts Made from a Nitrogen-Rich Network Polymer
journal, November 2012

  • Zhao, Yong; Watanabe, Kazuya; Hashimoto, Kazuhito
  • Journal of the American Chemical Society, Vol. 134, Issue 48
  • DOI: 10.1021/ja3085934

One-step synthesis of cobalt and nitrogen co-doped carbon nanotubes and their catalytic activity for the oxygen reduction reaction
journal, January 2015

  • Fu, Shaofang; Zhu, Chengzhou; Li, He
  • Journal of Materials Chemistry A, Vol. 3, Issue 24
  • DOI: 10.1039/C5TA01293G

Nitrogen-Doped Carbon Nanotube Arrays with High Electrocatalytic Activity for Oxygen Reduction
journal, February 2009


Structuring Porous Iron-Nitrogen-Doped Carbon in a Core/Shell Geometry for the Oxygen Reduction Reaction
journal, August 2014

  • Zhou, Ming; Yang, Chunzhen; Chan, Kwong-Yu
  • Advanced Energy Materials, Vol. 4, Issue 18
  • DOI: 10.1002/aenm.201400840

High-Rate Oxygen Electroreduction over Graphitic-N Species Exposed on 3D Hierarchically Porous Nitrogen-Doped Carbons
journal, July 2014

  • He, Wenhui; Jiang, Chunhuan; Wang, Jiabo
  • Angewandte Chemie International Edition, Vol. 53, Issue 36
  • DOI: 10.1002/anie.201404333

Hierarchically porous carbons with optimized nitrogen doping as highly active electrocatalysts for oxygen reduction
journal, September 2014

  • Liang, Hai-Wei; Zhuang, Xiaodong; Brüller, Sebastian
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms5973

Highly efficient nonprecious metal catalysts towards oxygen reduction reaction based on three-dimensional porous carbon nanostructures
journal, January 2016

  • Zhu, Chengzhou; Li, He; Fu, Shaofang
  • Chemical Society Reviews, Vol. 45, Issue 3
  • DOI: 10.1039/C5CS00670H

Mesoporous Metal–Nitrogen-Doped Carbon Electrocatalysts for Highly Efficient Oxygen Reduction Reaction
journal, October 2013

  • Liang, Hai-Wei; Wei, Wei; Wu, Zhong-Shuai
  • Journal of the American Chemical Society, Vol. 135, Issue 43
  • DOI: 10.1021/ja407552k

Accurate Control of Multishelled Co 3 O 4 Hollow Microspheres as High-Performance Anode Materials in Lithium-Ion Batteries
journal, May 2013

  • Wang, Jiangyan; Yang, Nailiang; Tang, Hongjie
  • Angewandte Chemie International Edition, Vol. 52, Issue 25
  • DOI: 10.1002/anie.201301622

Engineering Ordered and Nonordered Porous Noble Metal Nanostructures: Synthesis, Assembly, and Their Applications in Electrochemistry
journal, July 2015


Cobalt Imidazolate Framework as Precursor for Oxygen Reduction Reaction Electrocatalysts
journal, January 2011

  • Ma, Shengqian; Goenaga, Gabriel A.; Call, Ann V.
  • Chemistry - A European Journal, Vol. 17, Issue 7
  • DOI: 10.1002/chem.201003080

Nanostructured Nonprecious Metal Catalysts for Oxygen Reduction Reaction
journal, April 2013

  • Wu, Gang; Zelenay, Piotr
  • Accounts of Chemical Research, Vol. 46, Issue 8
  • DOI: 10.1021/ar400011z

Fe-N-C Oxygen Reduction Fuel Cell Catalyst Derived from Carbendazim: Synthesis, Structure, and Reactivity
journal, March 2014

  • Serov, Alexey; Artyushkova, Kateryna; Atanassov, Plamen
  • Advanced Energy Materials, Vol. 4, Issue 10
  • DOI: 10.1002/aenm.201301735

High-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt
journal, April 2011


Electrocatalyst approaches and challenges for automotive fuel cells
journal, June 2012


General Synthesis of Multi-Shelled Mixed Metal Oxide Hollow Spheres with Superior Lithium Storage Properties
journal, June 2014


Single-atom catalysis of CO oxidation using Pt1/FeOx
journal, July 2011

  • Qiao, Botao; Wang, Aiqin; Yang, Xiaofeng
  • Nature Chemistry, Vol. 3, Issue 8
  • DOI: 10.1038/nchem.1095

Bamboo-like Carbon Nanotube/Fe 3 C Nanoparticle Hybrids and Their Highly Efficient Catalysis for Oxygen Reduction
journal, January 2015

  • Yang, Wenxiu; Liu, Xiangjian; Yue, Xiaoyu
  • Journal of the American Chemical Society, Vol. 137, Issue 4
  • DOI: 10.1021/ja5129132

Photochemical route for synthesizing atomically dispersed palladium catalysts
journal, May 2016


Exploration of the active center structure of nitrogen-doped graphene-based catalysts for oxygen reduction reaction
journal, January 2012

  • Lai, Linfei; Potts, Jeffrey R.; Zhan, Da
  • Energy & Environmental Science, Vol. 5, Issue 7
  • DOI: 10.1039/c2ee21802j

Tuning Nanoparticle Catalysis for the Oxygen Reduction Reaction
journal, June 2013

  • Guo, Shaojun; Zhang, Sen; Sun, Shouheng
  • Angewandte Chemie International Edition, Vol. 52, Issue 33
  • DOI: 10.1002/anie.201207186

FePt Nanoparticles Assembled on Graphene as Enhanced Catalyst for Oxygen Reduction Reaction
journal, January 2012

  • Guo, Shaojun; Sun, Shouheng
  • Journal of the American Chemical Society, Vol. 134, Issue 5
  • DOI: 10.1021/ja2104334

Iron-Based Catalysts with Improved Oxygen Reduction Activity in Polymer Electrolyte Fuel Cells
journal, April 2009

  • Lefèvre, Michel; Proietti, Eric; Jaouen, Frédéric
  • Science, Vol. 324, Issue 5923, p. 71-74
  • DOI: 10.1126/science.1170051

A metal-free bifunctional electrocatalyst for oxygen reduction and oxygen evolution reactions
journal, April 2015

  • Zhang, Jintao; Zhao, Zhenghang; Xia, Zhenhai
  • Nature Nanotechnology, Vol. 10, Issue 5
  • DOI: 10.1038/nnano.2015.48

Efficient Oxygen Electroreduction: Hierarchical Porous Fe–N-doped Hollow Carbon Nanoshells
journal, May 2015


Metal-Free Catalysts for Oxygen Reduction Reaction
journal, May 2015

  • Dai, Liming; Xue, Yuhua; Qu, Liangti
  • Chemical Reviews, Vol. 115, Issue 11
  • DOI: 10.1021/cr5003563

Supportless Pt and PtPd Nanotubes as Electrocatalysts for Oxygen-Reduction Reactions
journal, May 2007

  • Chen, Zhongwei; Waje, Mahesh; Li, Wenzhen
  • Angewandte Chemie International Edition, Vol. 46, Issue 22
  • DOI: 10.1002/anie.200700894

Reducing Sugar: New Functional Molecules for the Green Synthesis of Graphene Nanosheets
journal, March 2010

  • Zhu, Chengzhou; Guo, Shaojun; Fang, Youxing
  • ACS Nano, Vol. 4, Issue 4
  • DOI: 10.1021/nn1002387

Experimental Observation of Redox-Induced Fe–N Switching Behavior as a Determinant Role for Oxygen Reduction Activity
journal, October 2015


A Generalized Synthesis of Metal Oxide Hollow Spheres Using a Hydrothermal Approach
journal, August 2006

  • Titirici, Maria-Magdalena; Antonietti, Markus; Thomas, Arne
  • Chemistry of Materials, Vol. 18, Issue 16
  • DOI: 10.1021/cm052768u

N-Doped Graphene Natively Grown on Hierarchical Ordered Porous Carbon for Enhanced Oxygen Reduction
journal, August 2013


Supportless Pt and PtPd Nanotubes as Electrocatalysts for Oxygen-Reduction Reactions
journal, May 2007


Macroscopic‐Scale Template Synthesis of Robust Carbonaceous Nanofiber Hydrogels and Aerogels and Their Applications
journal, April 2012

  • Liang, Hai‐Wei; Guan, Qing‐Fang; Chen, Li‐Feng
  • Angewandte Chemie, Vol. 124, Issue 21
  • DOI: 10.1002/ange.201200710

Accurate Control of Multishelled Co 3 O 4 Hollow Microspheres as High-Performance Anode Materials in Lithium-Ion Batteries
journal, May 2013

  • Wang, Jiangyan; Yang, Nailiang; Tang, Hongjie
  • Angewandte Chemie, Vol. 125, Issue 25
  • DOI: 10.1002/ange.201301622

High-Rate Oxygen Electroreduction over Graphitic-N Species Exposed on 3D Hierarchically Porous Nitrogen-Doped Carbons
journal, July 2014


General Synthesis of Multi-Shelled Mixed Metal Oxide Hollow Spheres with Superior Lithium Storage Properties
journal, June 2014

  • Zhang, Genqiang; Lou, Xiong Wen David
  • Angewandte Chemie International Edition, Vol. 53, Issue 34
  • DOI: 10.1002/anie.201404604

Works referencing / citing this record:

Metal‐Organic Frameworks Based Porous Carbons for Oxygen Reduction Reaction Electrocatalysts for Fuel Cell Applications
book, November 2019


Atomic Fe Dispersed on N-Doped Carbon Hollow Nanospheres for High-Efficiency Electrocatalytic Oxygen Reduction
journal, December 2018


Hierarchically Porous M-N-C (M = Co and Fe) Single-Atom Electrocatalysts with Robust MN x Active Moieties Enable Enhanced ORR Performance
journal, August 2018

  • Zhu, Chengzhou; Shi, Qiurong; Xu, Bo Z.
  • Advanced Energy Materials, Vol. 8, Issue 29
  • DOI: 10.1002/aenm.201801956

Oxygen Reduction Reactions on Single‐ or Few‐Atom Discrete Active Sites for Heterogeneous Catalysis
journal, September 2019

  • Sharifi, Tiva; Gracia‐Espino, Eduardo; Chen, Anran
  • Advanced Energy Materials, Vol. 10, Issue 11
  • DOI: 10.1002/aenm.201902084

Molecular Design of Single‐Atom Catalysts for Oxygen Reduction Reaction
journal, February 2020

  • Wan, Chengzhang; Duan, Xiangfeng; Huang, Yu
  • Advanced Energy Materials, Vol. 10, Issue 14
  • DOI: 10.1002/aenm.201903815

Synergistic Effects between Atomically Dispersed Fe−N−C and C−S−C for the Oxygen Reduction Reaction in Acidic Media
journal, September 2017

  • Shen, Hangjia; Gracia-Espino, Eduardo; Ma, Jingyuan
  • Angewandte Chemie, Vol. 129, Issue 44
  • DOI: 10.1002/ange.201706602

Single-Atom Electrocatalysts
journal, October 2017

  • Zhu, Chengzhou; Fu, Shaofang; Shi, Qiurong
  • Angewandte Chemie International Edition, Vol. 56, Issue 45
  • DOI: 10.1002/anie.201703864

Synergistic Effects between Atomically Dispersed Fe−N−C and C−S−C for the Oxygen Reduction Reaction in Acidic Media
journal, September 2017

  • Shen, Hangjia; Gracia-Espino, Eduardo; Ma, Jingyuan
  • Angewandte Chemie International Edition, Vol. 56, Issue 44
  • DOI: 10.1002/anie.201706602

Puffing Up Energetic Metal-Organic Frameworks to Large Carbon Networks with Hierarchical Porosity and Atomically Dispersed Metal Sites
journal, December 2018

  • Zhao, Ruo; Liang, Zibin; Gao, Song
  • Angewandte Chemie International Edition, Vol. 58, Issue 7
  • DOI: 10.1002/anie.201811126

Single Atom Catalysts on Carbon-Based Materials
journal, November 2018


Recent Progress of Carbon-Based Materials in Oxygen Reduction Reaction Catalysis
journal, January 2018


Impact of Textural Properties of Mesoporous Porphyrinic Carbon Electrocatalysts on Oxygen Reduction Reaction Activity
journal, April 2018


Synthesis and Active Site Identification of Fe−N−C Single-Atom Catalysts for the Oxygen Reduction Reaction
journal, November 2018


Nitrogen and Fluorine‐Codoped Carbon Nanowire Aerogels as Metal‐Free Electrocatalysts for Oxygen Reduction Reaction
journal, July 2017

  • Fu, Shaofang; Zhu, Chengzhou; Song, Junhua
  • Chemistry – A European Journal, Vol. 23, Issue 43
  • DOI: 10.1002/chem.201701969

Single-Atom Catalysts of Precious Metals for Electrochemical Reactions
journal, October 2017


Stable and Efficient Nitrogen-Containing Carbon-Based Electrocatalysts for Reactions in Energy-Conversion Systems
journal, June 2018


Heteroatom-Doped Carbon Nanotube and Graphene-Based Electrocatalysts for Oxygen Reduction Reaction
journal, September 2017


Oxidase‐Like Fe‐N‐C Single‐Atom Nanozymes for the Detection of Acetylcholinesterase Activity
journal, September 2019


Boosting the Loading of Metal Single Atoms via a Bioconcentration Strategy
journal, March 2020


Strategies for Stabilizing Atomically Dispersed Metal Catalysts
journal, December 2017


Single Atoms on Graphene for Energy Storage and Conversion
journal, April 2019


Atomic Cobalt on Defective Bimodal Mesoporous Carbon toward Efficient Oxygen Reduction for Zinc–Air Batteries
journal, January 2019


Insights into Single‐Atom Metal–Support Interactions in Electrocatalytic Water Splitting
journal, February 2019


Fabrication of Superior Single‐Atom Catalysts toward Diverse Electrochemical Reactions
journal, February 2019

  • Zhang, Bin‐Wei; Wang, Yun‐Xiao; Chou, Shu‐Lei
  • Small Methods, Vol. 3, Issue 9
  • DOI: 10.1002/smtd.201800497

Nitrogen Reduction to Ammonia on Atomic‐Scale Active Sites under Mild Conditions
journal, February 2019


Strategies for Enhancing the Electrocatalytic Activity of M–N/C Catalysts for the Oxygen Reduction Reaction
journal, May 2018


N-doped carbon nanocages: Bifunctional electrocatalysts for the oxygen reduction and evolution reactions
journal, March 2018


Highly dispersed γ-Fe 2 O 3 embedded in nitrogen doped carbon for the efficient oxygen reduction reaction
journal, January 2019

  • Xiao, Zhourong; Shen, Guoqiang; Hou, Fang
  • Catalysis Science & Technology, Vol. 9, Issue 17
  • DOI: 10.1039/c9cy01188a

Isolated Fe atoms dispersed on cellulose-derived nanocarbons as an efficient electrocatalyst for the oxygen reduction reaction
journal, January 2019

  • Li, Xiaofeng; Zhang, Yuhao; Zhang, Jinfang
  • Nanoscale, Vol. 11, Issue 48
  • DOI: 10.1039/c9nr07914a

Theoretical investigation of the ORR on boron–silicon nanotubes (B–SiNTs) as acceptable catalysts in fuel cells
journal, January 2019


A universal route to N-coordinated metals anchored on porous carbon nanosheets for highly efficient oxygen electrochemistry
journal, January 2019

  • Ren, Jin-Tao; Yuan, Zhong-Yong
  • Journal of Materials Chemistry A, Vol. 7, Issue 22
  • DOI: 10.1039/c9ta03300a

Oxygen-assisted stabilization of single-atom Au during photocatalytic hydrogen evolution
journal, January 2019

  • Zeng, Lei; Dai, Chunhui; Liu, Bin
  • Journal of Materials Chemistry A, Vol. 7, Issue 42
  • DOI: 10.1039/c9ta10290f

Nanoporous bimetallic Zn/Fe–N–C for efficient oxygen reduction in acidic and alkaline media
journal, January 2020

  • Xue, Jinling; Li, Yinshi; Hu, Jue
  • Journal of Materials Chemistry A, Vol. 8, Issue 15
  • DOI: 10.1039/c9ta13471a

Unveiling the high-activity origin of single-atom iron catalysts for oxygen reduction reaction
journal, June 2018

  • Yang, Liu; Cheng, Daojian; Xu, Haoxiang
  • Proceedings of the National Academy of Sciences, Vol. 115, Issue 26
  • DOI: 10.1073/pnas.1800771115

The effect of carbon support on the oxygen reduction activity and durability of single-atom iron catalysts
journal, August 2018

  • Li, Jin-Cheng; Tang, Dai-Ming; Hou, Peng-Xiang
  • MRS Communications, Vol. 8, Issue 03
  • DOI: 10.1557/mrc.2018.174

Puffing Up Energetic Metal-Organic Frameworks to Large Carbon Networks with Hierarchical Porosity and Atomically Dispersed Metal Sites
journal, December 2018


Theoretical study of single transition metal atom modified MoP as a nitrogen reduction electrocatalyst
journal, January 2019

  • Han, Miaomiao; Wang, Guozhong; Zhang, Haimin
  • Physical Chemistry Chemical Physics, Vol. 21, Issue 11
  • DOI: 10.1039/c9cp00621d

Enhanced Electrocatalytic Activity and Stability toward the Oxygen Reduction Reaction with Unprotected Pt Nanoclusters
journal, November 2018


Metal Catalysts for Heterogeneous Catalysis: From Single Atoms to Nanoclusters and Nanoparticles
journal, April 2018


Enhanced Electrocatalytic Activity and Stability toward the Oxygen Reduction Reaction with Unprotected Pt Nanoclusters
journal, November 2018