Synergistic Effects between Atomically Dispersed Fe-N-C and C-S-C for the Oxygen Reduction Reaction in Acidic Media

被引:475
作者
Shen, Hangjia [1 ,4 ]
Gracia-Espino, Eduardo [3 ]
Ma, Jingyuan [5 ]
Zang, Ketao [6 ]
Luo, Jun [6 ]
Wang, Le [1 ,4 ]
Gao, Sanshuang [1 ]
Mamat, Xamxikamar [1 ]
Hu, Guangzhi [1 ,3 ]
Wagberg, Thomas [3 ]
Guo, Shaojun [2 ]
机构
[1] Chinese Acad Sci, Xinjiang Tech Inst Phys & Chem, State Key Lab Basis Xinjiang Indigenous Med Plant, Key Lab Chem Plant Resources Arid Reg, Urumqi 830011, Peoples R China
[2] Peking Univ, Coll Engn, Dept Mat Sci & Engn, Beijing 100871, Peoples R China
[3] Umea Univ, Dept Phys, S-90187 Umea, Sweden
[4] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[5] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
[6] Tianjin Univ Technol, Ctr Electron Microscopy, Inst New Energy Mat & Low Carbon Technol, Tianjin Key Lab Adv Funct Porous Mat,Sch Mat, Tianjin 300384, Peoples R China
基金
中国国家自然科学基金;
关键词
doping; iron; oxygen reduction reaction; sulfur; synergistic effects; MESOPOROUS CARBON; DOPED GRAPHENE; FREE CATALYSTS; ELECTROCATALYSTS; IDENTIFICATION; NANOPARTICLES; PERFORMANCE; INSIGHTS; SBA-15; SITES;
D O I
10.1002/anie.201706602
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Various advanced catalysts based on sulfur-doped Fe/N/C materials have recently been designed for the oxygen reduction reaction (ORR); however, the enhanced activity is still controversial and usually attributed to differences in the surface area, improved conductivity, or uncertain synergistic effects. Herein, a sulfur-doped Fe/N/C catalyst (denoted as Fe/SNC) was obtained by a template-sacrificing method. The incorporated sulfur gives a thiophene-like structure (C-S-C), reduces the electron localization around the Fe centers, improves the interaction with oxygenated species, and therefore facilitates the complete 4e(-) ORR in acidic solution. Owing to these synergistic effects, the Fe/SNC catalyst exhibits much better ORR activity than the sulfur-free variant (Fe/NC) in 0.5m H2SO4.
引用
收藏
页码:13800 / 13804
页数:5
相关论文
共 42 条
[1]   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
[2]   Ordered mesoporous porphyrinic carbons with very high electrocatalytic activity for the oxygen reduction reaction [J].
Cheon, Jae Yeong ;
Kim, Taeyoung ;
Choi, YongMan ;
Jeong, Hu Young ;
Kim, Min Gyu ;
Sa, Young Jin ;
Kim, Jaesik ;
Lee, Zonghoon ;
Yang, Tae-Hyun ;
Kwon, Kyungjung ;
Terasaki, Osamu ;
Park, Gu-Gon ;
Adzic, Radoslav R. ;
Joo, Sang Hoon .
SCIENTIFIC REPORTS, 2013, 3
[3]   Metal-Free Catalysts for Oxygen Reduction Reaction [J].
Dai, Liming ;
Xue, Yuhua ;
Qu, Liangti ;
Choi, Hyun-Jung ;
Baek, Jong-Beom .
CHEMICAL REVIEWS, 2015, 115 (11) :4823-4892
[4]   DISTINCTION BETWEEN INTERMEDIATES PRODUCED IN MAIN AND SIDE ELECTRODIC REACTIONS [J].
DAMJANOVIC, A ;
GENSHAW, MA ;
BOCKRIS, JO .
JOURNAL OF CHEMICAL PHYSICS, 1966, 45 (11) :4057-+
[5]   A convenient route to synthesize SBA-15 rods with tunable pore length for lysozyme adsorption [J].
Ding, Yi ;
Yin, Guangfu ;
Liao, Xiaoming ;
Huang, Zhongbing ;
Chen, Xianchun ;
Yao, Yadong ;
Li, Jun .
MICROPOROUS AND MESOPOROUS MATERIALS, 2013, 170 :45-51
[6]   Behind the Synergistic Effect Observed on Phosphorus Nitrogen Codoped Graphene during the Oxygen Reduction Reaction [J].
Gracia-Espino, Eduardo .
JOURNAL OF PHYSICAL CHEMISTRY C, 2016, 120 (49) :27849-27857
[7]   Improved Oxygen Reduction Performance of Pt-Ni Nanoparticles by Adhesion on Nitrogen-Doped Graphene [J].
Gracia-Espino, Eduardo ;
Jia, Xueen ;
Wagberg, Thomas .
JOURNAL OF PHYSICAL CHEMISTRY C, 2014, 118 (05) :2804-2811
[8]   Unveiling N-Protonation and Anion-Binding Effects on Fe/N/C Catalysts for O2 Reduction in Proton-Exchange-Membrane Fuel Cells [J].
Herranz, Juan ;
Jaouen, Frederic ;
Lefevre, Michel ;
Kramm, Ulrike I. ;
Proietti, Eric ;
Dodelet, Jean-Pol ;
Bogdanoff, Peter ;
Fiechter, Sebastian ;
Abs-Wurmbach, Irmgard ;
Bertrand, Patrick ;
Arruda, Thomas M. ;
Mukerjee, Sanjeev .
JOURNAL OF PHYSICAL CHEMISTRY C, 2011, 115 (32) :16087-16097
[9]   Sulfur-Doped Fe/N/C Nanosheets as Highly Efficient Electrocatalysts for Oxygen Reduction Reaction [J].
Hu, Kui ;
Tao, Li ;
Liu, Dongdong ;
Huo, Jia ;
Wang, Shuangyin .
ACS APPLIED MATERIALS & INTERFACES, 2016, 8 (30) :19379-19385
[10]   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