Controllable synthesis of Fe-N4 species for acidic oxygen reduction

被引:48
作者
Yan, Xuecheng [1 ]
Jia, Yi [1 ]
Wang, Kang [1 ,2 ]
Jin, Zhao [3 ]
Dong, Chung-Li [4 ]
Huang, Yu-Cheng [4 ]
Chen, Jun [5 ]
Yao, Xiangdong [1 ]
机构
[1] Griffith Univ, Queensland Micro & Nanotechnol Ctr, Nathan Campus, Nathan, Qld 4111, Australia
[2] Univ Sci & Technol, Dept Chem, Beijing, Peoples R China
[3] Chinese Acad Sci, Lab Adv Power Sources, Changchun Inst Appl Chem, Changchun, Peoples R China
[4] Tamkang Univ, Dept Phys, New Taipei, Taiwan
[5] Univ Wollongong, Intelligent Polymer Res Inst, ARC Ctr Excellence Electromat Sci, AIIM Facil, Innovat Campus, Wollongong, NSW, Australia
基金
澳大利亚研究理事会;
关键词
atomic Fe-N-4 site; controllable synthesis; fuel cells; oxygen reduction reaction; SINGLE-ATOM CATALYSTS; GRAPHITE OXIDE; CO OXIDATION; ACTIVE-SITES; ELECTROCATALYST; IDENTIFICATION; CHALLENGES; GRAPHENE; CARBON;
D O I
10.1002/cey2.47
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Controllable design and synthesis of catalysts with the target active sites are extremely important for their applications such as for the oxygen reduction reaction (ORR) in fuel cells. However, the controllably synthesizing electrocatalysts with a single type of active site still remains a grand challenge. In this study, we developed a facile and scalable method for fabricating highly efficient ORR electrocatalysts with sole atomic Fe-N-4 species as the active site. Herein, the use of cost-effective highly porous carbon as the support not only could avoid the aggregation of the atomic Fe species but also a feasible approach to reduce the catalyst cost. The obtained atomic Fe-N-4 in activated carbon (aFe@AC) shows excellent ORR activity. Its half-wave potential is 59mV more negative but 47mV more positive than that of the commercial Pt/C in acidic and alkaline electrolytes, respectively. The full cell performance test results show that the aFe@AC sample is a promising candidate for direct methanol fuel cells. This study provides a general method to prepare catalysts with a certain type of active site and definite numbers.
引用
收藏
页码:452 / 460
页数:9
相关论文
共 32 条
[1]   Integrating PGM-Free Catalysts into Catalyst Layers and Proton Exchange Membrane Fuel Cell Devices [J].
Bonham, Dustin ;
Choi, Ja-Yeon ;
Kishimoto, Takeaki ;
Ye, Siyu .
ADVANCED MATERIALS, 2019, 31 (31)
[2]   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
[3]   Isolated Single Iron Atoms Anchored on N-Doped Porous Carbon as an Efficient Electrocatalyst for the Oxygen Reduction Reaction [J].
Chen, Yuanjun ;
Ji, Shufang ;
Wang, Yanggang ;
Dong, Juncai ;
Chen, Wenxing ;
Li, Zhi ;
Shen, Rongan ;
Zheng, Lirong ;
Zhuang, Zhongbin ;
Wang, Dingsheng ;
Li, Yadong .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2017, 56 (24) :6937-6941
[4]   Ultralow-loading platinum-cobalt fuel cell catalysts derived from imidazolate frameworks [J].
Chong, Lina ;
Wen, Jianguo ;
Kubal, Joseph ;
Sen, Fatih G. ;
Zou, Jianxin ;
Greeley, Jeffery ;
Chan, Maria ;
Barkholtz, Heather ;
Ding, Wenjiang ;
Liu, Di-Jia .
SCIENCE, 2018, 362 (6420) :1276-+
[5]   RAMAN MICROPROBE STUDIES ON CARBON MATERIALS [J].
CUESTA, A ;
DHAMELINCOURT, P ;
LAUREYNS, J ;
MARTINEZALONSO, A ;
TASCON, JMD .
CARBON, 1994, 32 (08) :1523-1532
[6]   Electrocatalyst approaches and challenges for automotive fuel cells [J].
Debe, Mark K. .
NATURE, 2012, 486 (7401) :43-51
[7]   Identification of active sites in CO oxidation and water-gas shift over supported Pt catalysts [J].
Ding, Kunlun ;
Gulec, Ahmet ;
Johnson, Alexis M. ;
Schweitzer, Neil M. ;
Stucky, Galen D. ;
Marks, Laurence D. ;
Stair, Peter C. .
SCIENCE, 2015, 350 (6257) :189-192
[8]   General synthesis and definitive structural identification of MN4C4 single-atom catalysts with tunable electrocatalytic activities [J].
Fei, Huilong ;
Dong, Juncai ;
Feng, Yexin ;
Allen, Christopher S. ;
Wan, Chengzhang ;
Volosskiy, Boris ;
Li, Mufan ;
Zhao, Zipeng ;
Wang, Yiliu ;
Sun, Hongtao ;
An, Pengfei ;
Chen, Wenxing ;
Guo, Zhiying ;
Lee, Chain ;
Chen, Dongliang ;
Shakir, Imran ;
Liu, Mingjie ;
Hu, Tiandou ;
Li, Yadong ;
Kirkland, Angus I. ;
Duan, Xiangfeng ;
Huang, Yu .
NATURE CATALYSIS, 2018, 1 (01) :63-72
[9]   Preparation of high active Pt/C cathode electrocatalyst for direct methanol fuel cell by citrate-stabilized method [J].
Jiang Qing-lai ;
Peng Zhong-dong ;
Xie Xiao-feng ;
Du Ke ;
Hu Guo-rong ;
Liu Ye-xiang .
TRANSACTIONS OF NONFERROUS METALS SOCIETY OF CHINA, 2011, 21 (01) :127-132
[10]   Raman spectra of graphite oxide and functionalized graphene sheets [J].
Kudin, Konstantin N. ;
Ozbas, Bulent ;
Schniepp, Hannes C. ;
Prud'homme, Robert K. ;
Aksay, Ilhan A. ;
Car, Roberto .
NANO LETTERS, 2008, 8 (01) :36-41