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题名: Understanding the High Activity of Fe-N-C Electrocatalysts in Oxygen Reduction: Fe/Fe3C Nanoparticles Boost the Activity of Fe-N-x
作者: Jiang, Wen-Jie1, 2; Gu, Lin3; Li, Li2; Zhang, Yun1, 2; Zhang, Xing1; Zhang, Lin-Juan4; Wang, Jian-Qiang4; Hu, Jin-Song1; Wei, Zidong2; Wan, Li-Jun1
刊名: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
发表日期: 2016-03-16
卷: 138, 期:10, 页:3570-3578
收录类别: SCI
英文摘要: 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.
语种: 英语
内容类型: 期刊论文
URI标识: http://ir.iccas.ac.cn/handle/121111/35937
Appears in Collections:分子纳米结构与纳米技术实验室_期刊论文

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作者单位: 1.Univ Chinese Acad Sci, Beijing Natl Lab Mol Sci, Key Lab Mol Nanostruct & Nanotechnol, Inst Chem, Beijing 100190, Peoples R China
2.Chongqing Univ, Coll Chem & Chem Engn, State Key Lab Power Transmiss Equipment & Syst Se, Chongqing 400044, Peoples R China
3.Chinese Acad Sci, Beijing Natl Lab Condensed Matter Phys, Inst Phys, Collaborat Innovat Ctr Quantum Matter, Beijing 100190, Peoples R China
4.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201800, Peoples R China
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