Highly Accessible Atomically Dispersed Fe-Nx Sites Electrocatalyst for Proton-Exchange Membrane Fuel Cell

被引:95
作者
Guo, Jianing [1 ,2 ]
Li, Bingjie [3 ]
Zhang, Qiyu [1 ]
Liu, Qingtao [4 ]
Wang, Zelin [5 ]
Zhao, Yufei [5 ]
Shui, Jianglan [4 ]
Xiang, Zhonghua [1 ]
机构
[1] Beijing Univ Chem Technol, State Key Lab Organ Inorgan Composites, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, Beijing 100029, Peoples R China
[2] Hebei Normal Univ, Coll Chem & Mat Sci, Hebei Key Lab Inorgan Nanomat, Shijiazhuang 050024, Hebei, Peoples R China
[3] Zhengzhou Univ, Affiliated Hosp 1, Dept Oncol, 1 Jianshe St, Zhengzhou 450052, Henan, Peoples R China
[4] Beihang Univ, Sch Mat Sci & Engn, Beijing, Peoples R China
[5] Beijing Univ Chem Technol, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China
基金
北京市自然科学基金;
关键词
acidic media; covalent organic polymer; oxygen reduction reaction; proton exchange membrane fuel cells; single-atom catalysts; OXYGEN REDUCTION REACTION; ACTIVE-SITES; CARBON; IRON; ARCHITECTURES;
D O I
10.1002/advs.202002249
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Atomically dispersed transition metal-N-x sites have emerged as a frontier for electrocatalysis because of the maximized atom utilization. However, there is still the problem that the reactant is difficult to reach active sites inside the catalytic layer in the practical proton exchange membrane fuel cell (PEMFC) testing, resulting in the ineffective utilization of the deeply hided active sites. In the device manner, the favorite structure of electrocatalysts for good mass transfer is vital for PEMFC. Herein, a facile one-step approach to synthesize atomically dispersed Fe-N-x species on hierarchically porous carbon nanostructures as a high-efficient and stable atomically dispersed catalyst for oxygen reduction in acidic media is reported, which is achieved by a predesigned hierarchical covalent organic polymer (COP) with iron anchored. COP materials with well-defined building blocks can stabilize the dopants and provide efficient mass transport. The appropriate hierarchical pore structure is proved to facilitate the mass transport of reactants to the active sites, ensuring the utilization of active sites in devices. Particularly, the structurally optimized HSAC/Fe-3 displays a maximum power density of up to 824 mW cm(-2), higher than other samples with fewer mesopores. Accordingly, this work will offer inspirations for designing efficient atomically dispersed electrocatalyst in PEMFC device.
引用
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页数:7
相关论文
共 27 条
[1]  
Cao D.P., 2016, ADV FUNCT MATER, V28, P21
[2]   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
[3]   A specific demetalation of Fe-N4 catalytic sites in the micropores of NC_Ar + NH3 is at the origin of the initial activity loss of the highly active Fe/N/C catalyst used for the reduction of oxygen in PEM fuel cells [J].
Chenitz, Regis ;
Kramm, Ulrike I. ;
Lefevre, Michel ;
Glibin, Vassili ;
Zhang, Gaixia ;
Sun, Shuhui ;
Dodelet, Jean-Pol .
ENERGY & ENVIRONMENTAL SCIENCE, 2018, 11 (02) :365-382
[4]   Is the rapid initial performance loss of Fe/N/C non precious metal catalysts due to micropore flooding? [J].
Choi, Ja-Yeon ;
Yang, Lijun ;
Kishimoto, Takeaki ;
Fu, Xiaogang ;
Ye, Siyu ;
Chen, Zhongwei ;
Banham, Dustin .
ENERGY & ENVIRONMENTAL SCIENCE, 2017, 10 (01) :296-305
[5]   Highly Accessible Atomically Dispersed Fe-Nx Sites Electrocatalyst for Proton-Exchange Membrane Fuel Cell [J].
Guo, Jianing ;
Li, Bingjie ;
Zhang, Qiyu ;
Liu, Qingtao ;
Wang, Zelin ;
Zhao, Yufei ;
Shui, Jianglan ;
Xiang, Zhonghua .
ADVANCED SCIENCE, 2021, 8 (05)
[6]   A Pyrolysis-Free Covalent Organic Polymer for Oxygen Reduction [J].
Guo, Jianing ;
Lin, Chun-Yu ;
Xia, Zhenhai ;
Xiang, Zhonghua .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2018, 57 (38) :12567-12572
[7]   Novel Route to Fe-Based Cathode as an Efficient Bifunctional Catalysts for Rechargeable Zn-Air Battery [J].
Han, Sancan ;
Hu, Xiaoyi ;
Wang, Jiacheng ;
Fang, Xiaosheng ;
Zhu, Yufang .
ADVANCED ENERGY MATERIALS, 2018, 8 (22)
[8]   Spectroscopic insights into the nature of active sites in iron-nitrogen-carbon electrocatalysts for oxygen reduction in acid [J].
Jia, Qingying ;
Ramaswamy, Nagappan ;
Tylus, Urszula ;
Strickland, Kara ;
Li, Jingkun ;
Serov, Alexey ;
Artyushkova, Kateryna ;
Atanassov, Plamen ;
Anibal, Jacob ;
Gumeci, Cenk ;
Barton, Scott Calabrese ;
Sougrati, Moulay-Tahar ;
Jaouen, Frederic ;
Halevi, Barr ;
Mukerjee, Sanjeev .
NANO ENERGY, 2016, 29 :65-82
[9]   Understanding the High Activity of Fe-N-C Electrocatalysts in Oxygen Reduction: Fe/Fe3C Nanoparticles Boost the Activity of Fe-Nx [J].
Jiang, Wen-Jie ;
Gu, Lin ;
Li, Li ;
Zhang, Yun ;
Zhang, Xing ;
Zhang, Lin-Juan ;
Wang, Jian-Qiang ;
Hu, Jin-Song ;
Wei, Zidong ;
Wan, Li-Jun .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2016, 138 (10) :3570-3578
[10]   The role of pre-defined microporosity in catalytic site formation for the oxygen reduction reaction in iron- and nitrogen-doped carbon materials [J].
Kim, Minhyoung ;
Kim, Hee Soo ;
Yoo, Sung Jong ;
Yoo, Won Cheol ;
Sung, Yung-Eun .
JOURNAL OF MATERIALS CHEMISTRY A, 2017, 5 (08) :4199-4206