Fe-N-Doped Carbon Capsules with Outstanding Electrochemical Performance and Stability for the Oxygen Reduction Reaction in Both Acid and Alkaline Conditions

被引:416
作者
Ferrero, Guillermo A. [1 ]
Preuss, Kathrin [2 ]
Marinovic, Adam [2 ]
Jorge, Ana Belen [3 ,4 ]
Mansor, Noramalina [5 ]
Brett, Dan J. L. [5 ]
Fuertes, Antonio B. [1 ]
Sevilla, Marta [1 ]
Titirici, Maria-Magdalena [2 ]
机构
[1] CSIC, Inst Nacl Carbon, POB 73, E-33080 Oviedo, Spain
[2] Queen Mary Univ London, Sch Engn & Mat Sci, Mile End Rd, London E1 4NS, England
[3] Queen Mary Univ London, Sch Engn & Mat Sci, Mat Res Inst, Mile End Rd, London E1 4NS, England
[4] UCL, Dept Chem, London WC1H 0AJ, England
[5] UCL, Dept Chem Engn, London WC1E 7JE, England
关键词
carbon nanomaterial; nitrogen-doping; oxygen reduction reaction; non-noble metal catalysts; capsule; HIGH ELECTROCATALYTIC ACTIVITY; METAL-FREE ELECTROCATALYSTS; POROUS CARBON; EFFICIENT ELECTROCATALYSTS; NITROGEN ADSORPTION; HOLLOW SPHERES; GLASSY-CARBON; FREE CATALYST; IRON; GRAPHENE;
D O I
10.1021/acsnano.6b01247
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
High surface area N-doped mesoporous carbon capsules with iron traces exhibit outstanding electrocatalytic activity for the oxygen reduction reaction in both alkaline and acidic media. In alkaline conditions, they exhibit more positive onset (0.94 V vs RHE) and half-wave potentials (0.83 V vs RHE,) than commercial Pt/C, while in acidic media the onset potential is comparable to that of commercial Pt/C with a peroxide yield lower than 10%. The Fe N-doped carbon catalyst combines high catalytic activity with remarkable performance stability (3500 cycles between 0.6 and 1.0 V vs RHE), which stems from the fact that iron is coordinated to nitrogen. Additionally, the newly developed electrocatalyst is unaffected by the methanol crossover effect in both acid and basic media, contrary to commercial Pt/C. The excellent catalytic behavior of the Fe N-doped carbon, even in the more relevant acid medium, is attributable to the combination of chemical functions (N-pyridinic, N-quaternary, and Fe-N coordination sites) and structural properties (large surface area, open mesoporous structure, and short diffusion paths), which guarantees a large number of highly active and fully accessible catalytic sites and rapid mass-transfer kinetics. Thus, this catalyst represents an important step forward toward replacing Pt catalysts with cheaper alternatives. In this regard, an alkaline anion exchange membrane fuel cell was assembled with Fe-N-doped mesoporous carbon capsules as the cathode catalyst to provide current and power densities matching those of a commercial Pt/C, which indicates the practical applicability of the Fe N-carbon catalyst.
引用
收藏
页码:5922 / 5932
页数:11
相关论文
共 82 条
[21]   Designing nitrogen-enriched echinus-like carbon capsules for highly efficient oxygen reduction reaction and lithium ion storage [J].
Hu, Chuangang ;
Wang, Lixia ;
Zhao, Yang ;
Ye, Minhui ;
Chen, Qing ;
Feng, Zhihai ;
Qu, Liangti .
NANOSCALE, 2014, 6 (14) :8002-8009
[22]   Hollow Spheres of Iron Carbide Nanoparticles Encased in Graphitic Layers as Oxygen Reduction Catalysts [J].
Hu, Yang ;
Jensen, Jens Oluf ;
Zhang, Wei ;
Cleemann, Lars N. ;
Xing, Wei ;
Bjerrum, Niels J. ;
Li, Qingfeng .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2014, 53 (14) :3675-3679
[23]   Recent advances in non-precious metal catalysis for oxygen-reduction reaction in polymer electrolyte fuel cells [J].
Jaouen, Frederic ;
Proietti, Eric ;
Lefevre, Michel ;
Chenitz, Regis ;
Dodelet, Jean-Pol ;
Wu, Gang ;
Chung, Hoon Taek ;
Johnston, Christina Marie ;
Zelenay, Piotr .
ENERGY & ENVIRONMENTAL SCIENCE, 2011, 4 (01) :114-130
[24]  
Jia Z, 2014, ROTATING ELECTRODE METHODS AND OXYGEN REDUCTION ELECTROCATALYSTS, P199, DOI 10.1016/B978-0-444-63278-4.00006-9
[25]   Residual metals present in "metal-free" N-doped carbons [J].
Jin, Xiuyan ;
Zhang, Guoxin ;
Hao, Yongchao ;
Chang, Zheng ;
Sun, Xiaoming .
CHEMICAL COMMUNICATIONS, 2015, 51 (85) :15585-15587
[26]   Application of large pore MCM-41 molecular sieves to improve pore size analysis using nitrogen adsorption measurements [J].
Kruk, M ;
Jaroniec, M ;
Sayari, A .
LANGMUIR, 1997, 13 (23) :6267-6273
[27]   Nitrogen adsorption studies of novel synthetic active carbons [J].
Kruk, M ;
Jaroniec, M ;
Gadkaree, KP .
JOURNAL OF COLLOID AND INTERFACE SCIENCE, 1997, 192 (01) :250-256
[28]   Nitrogen-doped ordered mesoporous carbon sphere with short channel as an efficient metal-free catalyst for oxygen reduction reaction [J].
Li, Jinlei ;
Li, Zelong ;
Tong, Jinhui ;
Xia, Chungu ;
Li, Fuwei .
RSC ADVANCES, 2015, 5 (86) :70010-70016
[29]  
Li YG, 2012, NAT NANOTECHNOL, V7, P394, DOI [10.1038/NNANO.2012.72, 10.1038/nnano.2012.72]
[30]   Hierarchically porous carbons with optimized nitrogen doping as highly active electrocatalysts for oxygen reduction [J].
Liang, Hai-Wei ;
Zhuang, Xiaodong ;
Bruller, Sebastian ;
Feng, Xinliang ;
Mullen, Klaus .
NATURE COMMUNICATIONS, 2014, 5