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 language | English |
|---|---|
| Pages (from-to) | 143-153 |
| Number of pages | 11 |
| Journal | Carbon |
| Volume | 121 |
| DOIs | |
| Publication status | Published - 1 Sep 2017 |
Cite this
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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 journal › Article › Research › peer-review
TY - JOUR
T1 - Directly anchoring Fe3C nanoclusters and FeNx sites in ordered mesoporous nitrogen-doped graphitic carbons to boost electrocatalytic oxygen reduction
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
Y1 - 2017/9/1
N2 - 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.
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.
UR - http://www.scopus.com/inward/record.url?scp=85019772953&partnerID=8YFLogxK
U2 - 10.1016/j.carbon.2017.05.078
DO - 10.1016/j.carbon.2017.05.078
M3 - Article
VL - 121
SP - 143
EP - 153
JO - Carbon
JF - Carbon
SN - 0008-6223
ER -