聚苯胺衍生Fe-N-C催化剂在碱性电解质中对氧还原反应的催化性能

doi:10.1016/S1872-2067(12)60714-1

催化学报 ›› 2013, Vol. 34 ›› Issue (11): 1992-1997.DOI: 10.1016/S1872-2067(12)60714-1

聚苯胺衍生Fe-N-C催化剂在碱性电解质中对氧还原反应的催化性能

严祥辉, 张贵荣, 徐柏庆

清华大学化学系, 有机光电子与分子工程教育部重点实验室, 北京100084

收稿日期:2013-07-20 修回日期:2013-09-16 出版日期:2013-10-18 发布日期:2013-10-18
通讯作者: Bo-Qing Xu
基金资助:
国家重点基础研究发展计划(973计划,2013CB933103).

Performance of polyaniline-derived Fe-N-C catalysts for oxygen reduction reaction in alkaline electrolyte

Xiang-Hui Yan, Gui-Rong Zhang, Bo-Qing Xu

Innovative Catalysis Program, Key Lab of Organic Optoelectronics & Molecular Engineering, Department of Chemistry, Tsinghua University, Beijing 100084, China

Received:2013-07-20 Revised:2013-09-16 Online:2013-10-18 Published:2013-10-18
Contact: Bo-Qing Xu
Supported by:
This work was supported by the National Basic Research Program of China (973 Program, 2013CB933103).

摘要/Abstract

摘要：

经过热解聚苯胺、碳和FeCl₃的混合物制备的Fe-N-C材料在酸性电解质中对氧还原反应表现出高的催化活性;由于材料中不存在任何贵金属, 因而被认为是一类新型非贵金属氧还原催化剂. 然而这类催化剂在碱性电解质中催化氧还原反应的性能如何尚不清楚. 本文使用旋转圆盘电极技术考察了制备的两个Fe-N-C催化剂在KOH水溶液中催化氧还原反应性能, 发现这两个催化剂表现出比无金属的N掺杂碳材料更高的活性. 与商业Pt/C催化剂相比, 它们催化氧还原反应的起始电势和半波电势分别仅低60和40 mV左右, 计时电流测试表明, 它们比Pt/C催化剂显示出更好的稳定性. 此外, 在这两个Fe-N-C催化剂上的氧还原反应主要遵循四电子途径. 本工作显示, Fe-N-C材料有望用于碱性燃料电池氧还原反应催化剂.

关键词: 铁-氮-碳, 氧还原反应, 阴极催化剂, 聚苯胺, 铁掺杂, 碱性电解质

Abstract:

Without the presence of any precious metal, Fe-N-C materials derived from pyrolysis of polyaniline (PANI)/carbon/FeCl₃ mixtures are recognized as new catalysts for cathodic oxygen reduction reaction (ORR) in acidic electrolyte. How these Fe-N-C catalysts would perform in an alkaline electrolyte remains yet unknown. Reported here are assessments of the ORR performance of two Fe-N-C catalysts (Fe content: 3.4% and 5.9%) in auqeous KOH by rotating disk electrode methods. Both Fe-N-C catalysts were found much more active than those metal-free N-doped carbon materials in literature. Moreover, the ORR onset and half-wave potentials over both Fe-N-C catalysts were respectively within 60 and 40 mV from those delivered by conventional Pt/C catalyst and both Fe-N-C catalysts even showed much superior catalytic stability in chronoamperometric measurement. ORR on the present Fe-N-C catalysts proceeded predominantly via a four-electron transfer mechanism. This work would shed a light on Fe-N-C materials for ORR catalysis in alkaline fuel cells.

Key words: Iron-nitrogen-carbon, Oxygen reduction reaction, Cathodic catalyst, Polyaniline, Iron-doping, Alkaline electrolyte

严祥辉, 张贵荣, 徐柏庆. 聚苯胺衍生Fe-N-C催化剂在碱性电解质中对氧还原反应的催化性能[J]. 催化学报, 2013, 34(11): 1992-1997.

Xiang-Hui Yan, Gui-Rong Zhang, Bo-Qing Xu. Performance of polyaniline-derived Fe-N-C catalysts for oxygen reduction reaction in alkaline electrolyte[J]. Chinese Journal of Catalysis, 2013, 34(11): 1992-1997.

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参考文献

[1] Jasinski R J. Nature, 1964, 201: 1212
[2] Deng X Y, Zhang D Y, Wang X, Yuan X X, Ma Z F. Chin J Catal (邓选英, 章冬云, 王昕, 原鲜霞, 马紫峰. 催化学报), 2008, 29: 519
[3] Liu R L, von Malotki C, Arnold L, Koshino N, Higashimura H, Baumgarten M, Müllen K. J Am Chem Soc, 2011, 133: 10372
[4] Meng H, Larouche N, Lefèvre M, Jaouen F, Stansfield B, Dodelet J P. Electrochim Acta, 2010, 55: 6450
[5] Meadowcroft D B. Nature, 1970, 226: 847
[6] Liang Y Y, Li Y G, Wang H L, Zhou J G, Wang J, Regier T, Dai H J. Nat Mater, 2011, 10: 780
[7] Byon H R, Suntivich J, Shao-Horn Y. Chem Mater, 2011, 23: 3421
[8] Lefèvre M, Proietti E, Jaouen F, Dodelet J P. Science, 2009, 324: 71
[9] Wu G, More K L, Johnston C M, Zelenay P. Science, 2011, 332: 443
[10] Wu G, Johnston C M, Mack N H, Artyushkova K, Ferrandon M, Nelson M, Lezama-Pacheco J S, Conradson S D, More K L, Myers D J, Zelenay P. J Mater Chem, 2011, 21: 11392
[11] Choi J Y, Hsu R S, Chen Z W. J Phys Chem C, 2010, 114: 8048
[12] Li X G, Liu G, Popov B N. J Power Sources, 2010, 195: 6373
[13] Yang S B, Feng X L, Wang X C, Müllen K. Angew Chem Int Ed, 2011, 50: 5339
[14] Zheng Y, Jiao Y, Chen J, Liu J, Liang J, Du A J, Zhang W M, Zhu Z H, Smith S C, Jaroniec M, Lu G Q, Qiao S Z. J Am Chem Soc, 2011, 133: 20116
[15] Liu Z W, Peng F, Wang H J, Yu H, Zheng W X, Yang J. Angew Chem Int Ed, 2011, 50: 3257
[16] Yang D S, Bhattacharjya D, Inamdar S, Park J, Yu J S. J Am Chem Soc, 2012, 134: 16127
[17] Yao Z, Nie H G, Yang Z, Zhou X M, Liu Z, Huang S M. Chem Commun, 2012, 48: 1027
[18] Sheng Z H, Gao H L, Bao W J, Wang F B, Xia X H. J Mater Chem, 2012, 22: 390
[19] Li Q Q, Zhang S, Dai L M, Li L S. J Am Chem Soc, 2012, 134: 18932
[20] Spendelow J S, Wieckowski A. Phys Chem Chem Phys, 2007, 9: 2654
[21] Lefèvre M, Dodelet J P, Bertrand P. J Phys Chem B, 2002, 106: 8705
[22] Jaouen F, Proietti E, Lefèvre M, Chenitz R, Dodelet J P, Wu G, Chung H T, Johnston C M, Zelenay P. Energy Environ Sci, 2011, 4: 114
[23] Chen Z W, Higgins D, Yu A P, Zhang L, Zhang J J. Energy Environ Sci, 2011, 4: 3167
[24] Parvez K, Yang S B, Hernandez Y, Winter A, Turchanin A, Feng X L, Müllen K. ACS Nano, 2012, 6: 9541
[25] Chokai M, Taniguchi M, Moriya S, Matsubayashi K, Shinoda T, Nabae Y, Kuroki S, Hayakawa T, Kakimoto M, Ozaki J, Miyata S. J Power Sources, 2010, 195: 5947
[26] Bard A J, Faulkner L R. Electrochemical Methods: Fundamentals and Applications. 2nd Ed. New York: Wiley, 2001
[27] Feng Y Y, Zhang G R, Ma J H, Liu G, Xu B Q. Phys Chem Chem Phys, 2011, 13: 3863
[28] Zhang G R, Xu B Q. Chin J Catal (张贵荣, 徐柏庆. 催化学报), 2013, 34: 942
[29] Markovic N M, Gasteiger H A, Ross P N Jr. J Phys Chem, 1996, 100: 6715
[30] Hyun S W, Shim I B, Kim C S. IEEE Trans Magn, 2008, 44: 2948

聚苯胺衍生Fe-N-C催化剂在碱性电解质中对氧还原反应的催化性能

Performance of polyaniline-derived Fe-N-C catalysts for oxygen reduction reaction in alkaline electrolyte

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