Isolated Single Iron Atoms Anchored on N-Doped Porous Carbon as an Efficient Electrocatalyst for the Oxygen Reduction Reaction

被引:1830
作者
Chen, Yuanjun [1 ]
Ji, Shufang [1 ]
Wang, Yanggang [1 ]
Dong, Juncai [2 ]
Chen, Wenxing [1 ]
Li, Zhi [1 ]
Shen, Rongan [1 ]
Zheng, Lirong [2 ]
Zhuang, Zhongbin [3 ,4 ]
Wang, Dingsheng [1 ]
Li, Yadong [1 ]
机构
[1] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
[2] Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing, Peoples R China
[3] Beijing Univ Chem Technol, State Key Lab Organ Inorgan Composites, Beijing 100029, Peoples R China
[4] Beijing Univ Chem Technol, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, Beijing 100029, Peoples R China
基金
中国国家自然科学基金;
关键词
electrocatalysts; iron; oxygen reduction reaction; porous carbons; single-atom catalysts; PERFORMANCE; CATALYSTS; GRAPHENE; COORDINATION; STABILITY; COBALT;
D O I
10.1002/anie.201702473
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The development of low-cost, efficient, and stable electrocatalysts for the oxygen reduction reaction (ORR) is desirable but remains a great challenge. Herein, we made a highly reactive and stable isolated single-atom Fe/N-doped porous carbon (ISA Fe/CN) catalyst with Fe loading up to 2.16 wt%. The catalyst showed excellent ORR performance with a half-wave potential (E-1/2) of 0.900 V, which outperformed commercial Pt/C and most non-precious-metal catalysts reported to date. Besides exceptionally high kinetic current density (J(k)) of 37.83 mVcm(-2) at 0.85 V, it also had a good methanol tolerance and outstanding stability. Experiments demonstrated that maintaining the Fe as isolated atoms and incorporating nitrogen was essential to deliver the high performance. First principle calculations further attributed the high reactivity to the high efficiency of the single Fe atoms in transporting electrons to the adsorbed OH species.
引用
收藏
页码:6937 / 6941
页数:5
相关论文
共 34 条
[1]  
[Anonymous], 2016, ANGEW CHEM
[2]  
[Anonymous], 2017, Angew. Chem, DOI DOI 10.1002/ANGE.201610119
[3]   Highly Crystalline Multimetallic Nanoframes with Three-Dimensional Electrocatalytic Surfaces [J].
Chen, Chen ;
Kang, Yijin ;
Huo, Ziyang ;
Zhu, Zhongwei ;
Huang, Wenyu ;
Xin, Huolin L. ;
Snyder, Joshua D. ;
Li, Dongguo ;
Herron, Jeffrey A. ;
Mavrikakis, Manos ;
Chi, Miaofang ;
More, Karren L. ;
Li, Yadong ;
Markovic, Nenad M. ;
Somorjai, Gabor A. ;
Yang, Peidong ;
Stamenkovic, Vojislav R. .
SCIENCE, 2014, 343 (6177) :1339-1343
[4]   Atomically Dispersed Iron-Nitrogen Species as Electrocatalysts for Bifunctional Oxygen Evolution and Reduction Reactions [J].
Chen, Pengzuo ;
Zhou, Tianpei ;
Xing, Lili ;
Xu, Kun ;
Tong, Yun ;
Xie, Hui ;
Zhang, Lidong ;
Yan, Wensheng ;
Chu, Wangsheng ;
Wu, Changzheng ;
Xie, Yi .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2017, 56 (02) :610-614
[5]   A review on non-precious metal electrocatalysts for PEM fuel cells [J].
Chen, Zhongwei ;
Higgins, Drew ;
Yu, Aiping ;
Zhang, Lei ;
Zhang, Jiujun .
ENERGY & ENVIRONMENTAL SCIENCE, 2011, 4 (09) :3167-3192
[6]   Atomic cobalt on nitrogen-doped graphene for hydrogen generation [J].
Fei, Huilong ;
Dong, Juncai ;
Arellano-Jimenez, M. Josefina ;
Ye, Gonglan ;
Kim, Nam Dong ;
Samuel, Errol L. G. ;
Peng, Zhiwei ;
Zhu, Zhuan ;
Qin, Fan ;
Bao, Jiming ;
Yacaman, Miguel Jose ;
Ajayan, Pulickel M. ;
Chen, Dongliang ;
Tour, James M. .
NATURE COMMUNICATIONS, 2015, 6
[7]   Fe-N-Doped Carbon Capsules with Outstanding Electrochemical Performance and Stability for the Oxygen Reduction Reaction in Both Acid and Alkaline Conditions [J].
Ferrero, Guillermo A. ;
Preuss, Kathrin ;
Marinovic, Adam ;
Jorge, Ana Belen ;
Mansor, Noramalina ;
Brett, Dan J. L. ;
Fuertes, Antonio B. ;
Sevilla, Marta ;
Titirici, Maria-Magdalena .
ACS NANO, 2016, 10 (06) :5922-5932
[8]   Atomically Dispersed Supported Metal Catalysts [J].
Flytzani-Stephanopoulos, Maria ;
Gates, Bruce C. .
ANNUAL REVIEW OF CHEMICAL AND BIOMOLECULAR ENGINEERING, VOL 3, 2012, 3 :545-574
[9]  
HAN J, 2015, ANGEW CHEM, V127, P12813
[10]   Coordination Chemistry of [Co(acac)2] with N-Doped Graphene: Implications for Oxygen Reduction Reaction Reactivity of Organo-metallic Co-O4-N Species [J].
Han, Jongwoo ;
Sa, Young Jin ;
Shim, Yeonjun ;
Choi, Min ;
Park, Noejung ;
Joo, Sang Hoon ;
Park, Sungjin .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2015, 54 (43) :12622-12626