Atomically FeN2 moieties dispersed on mesoporous carbon: A new atomic catalyst for efficient oxygen reduction catalysis
Shen, HJ; Gracia-Espino, E; Ma, JY; Tang, HD; Mamat, X; Wagberg, T; Hu, GZ; Guo, SJ
2017
发表期刊NANO ENERGY
ISSN2211-2855
卷号35页码:9-16
文章类型期刊论文
摘要Earth-abundant materials with Fe-N-C centers have been identified as promising catalysts for oxygen reduction reaction (ORR), but these alternatives for Pt catalysts are usually the porphyrin-like FeN4 configuration. The density functional theory (DFT) calculations reveal that FeN2 outperforms FeN4 due to its lower interaction with *O-2 and *OH intermediates and enhanced electron transport, however, achieving an optimum design of these earth-abundant materials with the enriched FeN2 catalytic centers is still a great challenge. Here, we report an intriguing template casting strategy to introduce a mass of atomically dispersed FeN2 moieties onto the surface of N-doped ordered mesoporous carbon for boosting ORR electrocatalysis. One of unique parts herein is to pre anchor Fe precursor on the surface of template (SBA-15) during catalyst synthesis, preventing Fe from penetrating into the carbon skeleton and facilitating the removal of excessive Fe-based particles during silica elimination by HF etching, resulting in a desirable model structure comprising only highly active atomically dispersed FeN2 sites, as confirmed by high-angle annular dark field-scanning transmission electron microscopy (HAADF-STEM), extended X-ray absorption fine structure (EXAFS) and Mossbauer spectroscopy analysis. The well-defined structure prompts us to understand the nature of the catalytic active sites, and to demonstrate that the catalyst activity is linearly proportional to the concentration of FeN2 sites. The obtained atomic electrocatalyst exhibits superior electrocatalytic performance for ORR with a more positive half-wave potential than that of Pt/C catalyst. We further establish a kinetic model to predict the ORR activity of these single-atom dispersed catalysts. The present work elaborates on a profound understanding for designing low-cost, highly efficient FeN2-based electrocatalyst for boosting ORR.
关键词Fen2 Atomic Dispersion Oxygen Reduction Reaction Kinetic Model Nitrogen-doped Carbon
DOI10.1016/j.nanoen.2017.03.027
收录类别SCI
语种英语
WOS记录号WOS:000400647900002
引用统计
被引频次:34[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.sinap.ac.cn/handle/331007/27261
专题中科院上海应用物理研究所2011-2018年
推荐引用方式
GB/T 7714
Shen, HJ,Gracia-Espino, E,Ma, JY,et al. Atomically FeN2 moieties dispersed on mesoporous carbon: A new atomic catalyst for efficient oxygen reduction catalysis[J]. NANO ENERGY,2017,35:9-16.
APA Shen, HJ.,Gracia-Espino, E.,Ma, JY.,Tang, HD.,Mamat, X.,...&Guo, SJ.(2017).Atomically FeN2 moieties dispersed on mesoporous carbon: A new atomic catalyst for efficient oxygen reduction catalysis.NANO ENERGY,35,9-16.
MLA Shen, HJ,et al."Atomically FeN2 moieties dispersed on mesoporous carbon: A new atomic catalyst for efficient oxygen reduction catalysis".NANO ENERGY 35(2017):9-16.
条目包含的文件 下载所有文件
文件名称/大小 文献类型 版本类型 开放类型 使用许可
Atomically FeN2 moie(1136KB)期刊论文作者接受稿开放获取CC BY-NC-SA浏览 下载
个性服务
推荐该条目
保存到收藏夹
查看访问统计
导出为Endnote文件
谷歌学术
谷歌学术中相似的文章
[Shen, HJ]的文章
[Gracia-Espino, E]的文章
[Ma, JY]的文章
百度学术
百度学术中相似的文章
[Shen, HJ]的文章
[Gracia-Espino, E]的文章
[Ma, JY]的文章
必应学术
必应学术中相似的文章
[Shen, HJ]的文章
[Gracia-Espino, E]的文章
[Ma, JY]的文章
相关权益政策
暂无数据
收藏/分享
文件名: Atomically FeN2 moieties dispersed on mesoporous carbon_ A new atomic catalyst for efficient oxygen reduction catalysis.pdf
格式: Adobe PDF
所有评论 (0)
暂无评论
 

除非特别说明,本系统中所有内容都受版权保护,并保留所有权利。