Understanding the High Activity of Fe-N-C Electrocatalysts in Oxygen Reduction: Fe/Fe3C Nanoparticles Boost the Activity of Fe-N-x
Jiang, WJ; Gu, L; Li, L; Zhang, Y; Zhang, X; Zhang, LJ; Wang, JQ; Hu, JS; Wei, ZD; Wan, LJ; Wan, LJ (reprint author), Univ Chinese Acad Sci, Beijing Natl Lab Mol Sci, Key Lab Mol Nanostruct & Nanotechnol, Inst Chem, Beijing 100190, Peoples R China.; Wei, ZD (reprint author), Chongqing Univ, Coll Chem & Chem Engn, State Key Lab Power Transmiss Equipment & Syst Se, Chongqing 400044, Peoples R China.
2016
发表期刊JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
ISSN0002-7863
卷号138期号:10页码:3570—3578
文章类型期刊文献
摘要Understanding the origin of high activity of Fe-N-C electrocatalysts in oxygen reduction reaction (ORR) is critical but still challenging for developing efficient sustainable nonprecious metal catalysts in fuel. cells and metal air batteries. Herein, we developed a new highly active Fe-N-C ORR catalyst containing Fe-N-x coordination sites and Fe/Fe3C nanocrystals (Fe@C-FeNC), and revealed the origin of its activity by intensively investigating the composition and the structure of the catalyst and their correlations with the electrochemical performance. The detailed analyses unambiguously confirmed the coexistence of Fe/Fe3C nanocrystals and Fe-N-x in the best catalyst. A series of designed experiments disclosed that (1) N-doped carbon substrate, Fe/Fe3C nanocrystals or Fe-N-x themselves did not deliver the high activity; (2) the catalysts with both Fe/Fe3C nanocrystals and Fe-N-x exhibited the high activity; (3) the higher content of Fe-N-x gave the higher activity; (4) the removal of Fe/Fe3C nanocrystals severely degraded the activity; (5) the blocking of Fe-N-x downgraded the activity and the recovery of the blocked Fe-N-x recovered the activity. These facts supported that the high ORR activity of the Fe@C-FeNC electrocatalysts should be ascribed to that Fe/Fe3C nanocrystals boost the activity of Fe-N-x. The coexistence of high content of Fe-N-x and sufficient metallic iron nanoparticles is essential for the high ORR activity. DFT calculation corroborated this conclusion by indicating that the interaction between metallic iron and Fe-N-4 coordination structure favored the adsorption of oxygen molecule. These new findings open an avenue for the rational design and bottom-up synthesis of low-cost highly active ORR electrocatalysts.
关键词Membrane Fuel-cells High-performance Electrocatalysts Iron Carbide Nanoparticles Nitrogen-doped Carbon Metal-air Batteries Efficient Electrocatalysts Electrochemical Reactions Cathode Catalyst Porous Carbon Ion Batteries
DOI10.1021/jacs.6b00757
收录类别SCI
语种英语
WOS记录号WOS:000372477700044
引用统计
被引频次:329[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/331007/25883
专题中科院上海应用物理研究所2011-2018年
通讯作者Hu, JS; Wan, LJ (reprint author), Univ Chinese Acad Sci, Beijing Natl Lab Mol Sci, Key Lab Mol Nanostruct & Nanotechnol, Inst Chem, Beijing 100190, Peoples R China.; Wei, ZD (reprint author), Chongqing Univ, Coll Chem & Chem Engn, State Key Lab Power Transmiss Equipment & Syst Se, Chongqing 400044, Peoples R China.
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Jiang, WJ,Gu, L,Li, L,et al. Understanding the High Activity of Fe-N-C Electrocatalysts in Oxygen Reduction: Fe/Fe3C Nanoparticles Boost the Activity of Fe-N-x[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2016,138(10):3570—3578.
APA Jiang, WJ.,Gu, L.,Li, L.,Zhang, Y.,Zhang, X.,...&Wei, ZD .(2016).Understanding the High Activity of Fe-N-C Electrocatalysts in Oxygen Reduction: Fe/Fe3C Nanoparticles Boost the Activity of Fe-N-x.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,138(10),3570—3578.
MLA Jiang, WJ,et al."Understanding the High Activity of Fe-N-C Electrocatalysts in Oxygen Reduction: Fe/Fe3C Nanoparticles Boost the Activity of Fe-N-x".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 138.10(2016):3570—3578.
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