Directly anchoring Fe3C nanoclusters and FeNx sites in ordered mesoporous nitrogen-doped graphitic carbons to boost electrocatalytic oxygen reduction

Zhi Chen, Xingmin Gao, Xiangru Wei, Xinxia Wang, Yanguang Li, Tao Wu, Jun Guo, Qinfen Gu, Winston Duo Wu, Xiao Dong Chen, Zhangxiong Wu, Dongyuan Zhao

Research output: Contribution to journalArticleResearchpeer-review

Abstract

Porous carbon materials doped with nano-sized transition metal carbides and/or metal-nitrogen coordinative sites are promising oxygen reduction electrocatalysts. The doping of such functionalities in carbon materials with desirable concentration, ultra-small size and stable configuration is still a challenge. In this paper, by grinding and pyrolyzing solid mixtures of an amino acid, an iron salt, and a mesoporous silica template, we demonstrate a solvent-free assembly approach to directly anchor both Fe3C nanoclucters and FeNx sites into nitrogen-doped ordered mesoporous graphitic carbon materials. The carbonaceous electrocatalysts are imparted with several fascinating features, namely, highly dispersed ultra-small Fe3C nanoclusters of 1–3 nm, well-anchored FeNx sites, nitrogen-doped well-graphitized carbon frameworks, and ordered mesopores (∼5.4 nm) and high surface areas (>1000 m2/g), respectively. The combination of these features makes these electrocatalysts exceptional for oxygen reduction reaction under both alkaline and acidic electrolytes, i.e. superior catalytic activities (e.g. onset and half-wave potentials up to 1.00 and 0.89 V vs. the reversible hydrogen electrode in alkaline solution), outstanding stabilities and excellent methanol tolerance, respectively. An in-depth study has been conducted to identify and characterize the key active sites in these electrocatalysts and to elucidate several important influencing factors to optimize the catalytic performance.

Original languageEnglish
Pages (from-to)143-153
Number of pages11
JournalCarbon
Volume121
DOIs
Publication statusPublished - 1 Sep 2017

Cite this

Chen, Zhi ; Gao, Xingmin ; Wei, Xiangru ; Wang, Xinxia ; Li, Yanguang ; Wu, Tao ; Guo, Jun ; Gu, Qinfen ; Wu, Winston Duo ; Chen, Xiao Dong ; Wu, Zhangxiong ; Zhao, Dongyuan. / Directly anchoring Fe3C nanoclusters and FeNx sites in ordered mesoporous nitrogen-doped graphitic carbons to boost electrocatalytic oxygen reduction. In: Carbon. 2017 ; Vol. 121. pp. 143-153.
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title = "Directly anchoring Fe3C nanoclusters and FeNx sites in ordered mesoporous nitrogen-doped graphitic carbons to boost electrocatalytic oxygen reduction",
abstract = "Porous carbon materials doped with nano-sized transition metal carbides and/or metal-nitrogen coordinative sites are promising oxygen reduction electrocatalysts. The doping of such functionalities in carbon materials with desirable concentration, ultra-small size and stable configuration is still a challenge. In this paper, by grinding and pyrolyzing solid mixtures of an amino acid, an iron salt, and a mesoporous silica template, we demonstrate a solvent-free assembly approach to directly anchor both Fe3C nanoclucters and FeNx sites into nitrogen-doped ordered mesoporous graphitic carbon materials. The carbonaceous electrocatalysts are imparted with several fascinating features, namely, highly dispersed ultra-small Fe3C nanoclusters of 1–3 nm, well-anchored FeNx sites, nitrogen-doped well-graphitized carbon frameworks, and ordered mesopores (∼5.4 nm) and high surface areas (>1000 m2/g), respectively. The combination of these features makes these electrocatalysts exceptional for oxygen reduction reaction under both alkaline and acidic electrolytes, i.e. superior catalytic activities (e.g. onset and half-wave potentials up to 1.00 and 0.89 V vs. the reversible hydrogen electrode in alkaline solution), outstanding stabilities and excellent methanol tolerance, respectively. An in-depth study has been conducted to identify and characterize the key active sites in these electrocatalysts and to elucidate several important influencing factors to optimize the catalytic performance.",
author = "Zhi Chen and Xingmin Gao and Xiangru Wei and Xinxia Wang and Yanguang Li and Tao Wu and Jun Guo and Qinfen Gu and Wu, {Winston Duo} and Chen, {Xiao Dong} and Zhangxiong Wu and Dongyuan Zhao",
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language = "English",
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Directly anchoring Fe3C nanoclusters and FeNx sites in ordered mesoporous nitrogen-doped graphitic carbons to boost electrocatalytic oxygen reduction. / Chen, Zhi; Gao, Xingmin; Wei, Xiangru; Wang, Xinxia; Li, Yanguang; Wu, Tao; Guo, Jun; Gu, Qinfen; Wu, Winston Duo; Chen, Xiao Dong; Wu, Zhangxiong; Zhao, Dongyuan.

In: Carbon, Vol. 121, 01.09.2017, p. 143-153.

Research output: Contribution to journalArticleResearchpeer-review

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AU - Chen, Zhi

AU - Gao, Xingmin

AU - Wei, Xiangru

AU - Wang, Xinxia

AU - Li, Yanguang

AU - Wu, Tao

AU - Guo, Jun

AU - Gu, Qinfen

AU - Wu, Winston Duo

AU - Chen, Xiao Dong

AU - Wu, Zhangxiong

AU - Zhao, Dongyuan

PY - 2017/9/1

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AB - Porous carbon materials doped with nano-sized transition metal carbides and/or metal-nitrogen coordinative sites are promising oxygen reduction electrocatalysts. The doping of such functionalities in carbon materials with desirable concentration, ultra-small size and stable configuration is still a challenge. In this paper, by grinding and pyrolyzing solid mixtures of an amino acid, an iron salt, and a mesoporous silica template, we demonstrate a solvent-free assembly approach to directly anchor both Fe3C nanoclucters and FeNx sites into nitrogen-doped ordered mesoporous graphitic carbon materials. The carbonaceous electrocatalysts are imparted with several fascinating features, namely, highly dispersed ultra-small Fe3C nanoclusters of 1–3 nm, well-anchored FeNx sites, nitrogen-doped well-graphitized carbon frameworks, and ordered mesopores (∼5.4 nm) and high surface areas (>1000 m2/g), respectively. The combination of these features makes these electrocatalysts exceptional for oxygen reduction reaction under both alkaline and acidic electrolytes, i.e. superior catalytic activities (e.g. onset and half-wave potentials up to 1.00 and 0.89 V vs. the reversible hydrogen electrode in alkaline solution), outstanding stabilities and excellent methanol tolerance, respectively. An in-depth study has been conducted to identify and characterize the key active sites in these electrocatalysts and to elucidate several important influencing factors to optimize the catalytic performance.

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SN - 0008-6223

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