Influence of Fe on electrocatalytic activity of iron-nitrogen-doped carbon materials toward oxygen reduction reaction

doi:10.1007/s11708-020-0669-0

Front. Energy

2022, Vol. 16

Issue (5) : 812-821 https://doi.org/10.1007/s11708-020-0669-0

RESEARCH ARTICLE

Influence of Fe on electrocatalytic activity of iron-nitrogen-doped carbon materials toward oxygen reduction reaction

Lin LI¹, Cehuang FU¹, Shuiyun SHEN¹, Fangling JIANG¹, Guanghua WEI², Junliang ZHANG¹(

)

¹. Institute of Fuel Cells, School of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai 200240, China
². SJTU-ParisTech Elite Institute of Technology, Shanghai Jiao Tong University, Shanghai 200240, China

Download: PDF(1812 KB) HTML
Export: BibTeX | EndNote | Reference Manager | ProCite | RefWorks

Abstract

The development of highly active nitrogen-doped carbon-based transition metal (M-N-C) compounds for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs) greatly helps reduce fuel cell cost, thus rapidly promoting their commercial applications. Among different M-N-C electrocatalysts, the series of Fe-N-C materials are highly favored because of their high ORR activity. However, there remains a debate on the effect of Fe, and rare investigations focus on the influence of Fe addition in the second heat treatment usually performed after acid leaching in the catalyst synthesis. It is thus very critical to explore the influences of Fe on the ORR electrocatalytic activity, which will, in turn, guide the design of Fe-N-C materials with enhanced performance. Herein, a series of Fe-N-C electrocatalysts are synthesize and the influence of Fe on the ORR activity are speculated both experimentally and theoretically. It is deduced that the active site lies in the structure of Fe-N₄, accompanied with the addition of appropriate Fe, and the number of active sites increases without the occurrence of agglomeration particles. Moreover, it is speculated that Fe plays an important role in stabilizing N as well as constituting active sites in the second pyrolyzing process.

Keywords oxygen reduction reaction Fe-N-C active sites Fe addition second heat treatment

Corresponding Author(s): Junliang ZHANG

Online First Date: 11 June 2020 Issue Date: 28 November 2022

Cite this article:

Lin LI,Cehuang FU,Shuiyun SHEN, et al. Influence of Fe on electrocatalytic activity of iron-nitrogen-doped carbon materials toward oxygen reduction reaction[J]. Front. Energy, 2022, 16(5): 812-821.

URL:

https://academic.hep.com.cn/fie/EN/10.1007/s11708-020-0669-0
https://academic.hep.com.cn/fie/EN/Y2022/V16/I5/812

Fig.1 Characterization of the Fe-N-C-X electrocatalysts.

Fig.2 XAFS of Fe-N-C-20 and Fe foil.

Fig.3 ORR activity and XPS analysis of the Fe-N-C-X electrocatalysts.

Tab.1 Adsorption information and free energy of different catalyst models

Fig.4 Free energy change diagram for the ORR.

Fig.5 ORR activity and XPS analysis of the Fe-N-C-X-II-Y electrocatalysts.

1	J K Nørskov, J Rossmeisl, A Logadottir, L Lindqvist, J R Kitchin, T Bligaard, H Jonsson. Origin of the overpotential for oxygen reduction at a fuel-cell cathode. Journal of Physical Chemistry B, 2004, 108(46): 17886–17892 https://doi.org/10.1021/jp047349j
2	J Zhang, K Sasaki, E Sutter, R Adzic. Stabilization of platinum oxygen-reduction electrocatalysts using gold clusters. Science, 2007, 315(5809): 220–222 https://doi.org/10.1126/science.1134569
3	L Luo, F Zhu, R Tian, L Li, S Shen, X Yan, J Zhang. Composition-graded PdxNi1–x nanospheres with Pt monolayer shells as high-performance electrocatalysts for oxygen reduction reaction. ACS Catalysis, 2017, 7(8): 5420–5430 https://doi.org/10.1021/acscatal.7b01775
4	B Cai, R Hübner, K Sasaki, Y Zhang, D Su, C Ziegler, M B Vukmirovic, B Rellinghaus, R R Adzic, A Eychmüller. Core-shell structuring of pure metallic aerogels towards highly efficient platinum utilization for the oxygen reduction reaction. Angewandte Chemie International Edition, 2018, 57(11): 2963–2966 https://doi.org/10.1002/anie.201710997
5	Y Guo, J Tang, J Henzie, B Jiang, H Qian, Z Wang, H Tan, Y Bando, Y Yamauchi. Assembly of hollow mesoporous nanoarchitectures composed of ultrafine Mo2C nanoparticles on N-doped carbon nanosheets for efficient electrocatalytic reduction of oxygen. Materials Horizons, 2017, 4(6): 1171–1177 https://doi.org/10.1039/C7MH00586E
6	M Lefèvre, E Proietti, F Jaouen, J P Dodelet. Iron-based catalysts with improved oxygen reduction activity in polymer electrolyte fuel cells. Science, 2009, 324(5923): 71–74 https://doi.org/10.1126/science.1170051
7	J Wang, Z Huang, W Liu, C Chang, H Tang, Z Li, W Chen, C Jia, T Yao, S Wei, Y Wu, Y Li. Design of N-coordinated dual-metal sites: a stable and active Pt-free catalyst for acidic oxygen reduction reaction. Journal of the American Chemical Society, 2017, 139(48): 17281–17284 https://doi.org/10.1021/jacs.7b10385
8	D Papageorgopoulos. Fuel cells R&D overview. 2018, available at the website of hydrogen.energy.gov
9	P C Vesborg, T F Jaramillo. Addressing the terawatt challenge: scalability in the supply of chemical elements for renewable energy. RSC Advances, 2012, 2(21): 7933–7947 https://doi.org/10.1039/c2ra20839c
10	H Zhang, S Hwang, M Wang, Z Feng, S Karakalos, L Luo, Z Qiao, X Xie, C Wang, D Su, Y Shao, G Wu. Single atomic iron catalysts for oxygen reduction in acidic media: particle size control and thermal activation. Journal of the American Chemical Society, 2017, 139(40): 14143–14149 https://doi.org/10.1021/jacs.7b06514
11	J S Lee, G S Park, S T Kim, M Liu, J Cho. A highly efficient electrocatalyst for the oxygen reduction reaction: N-doped ketjenblack incorporated into Fe/Fe3C–functionalized melamine foam. Angewandte Chemie International Edition, 2013, 125(3): 1060–1064 https://doi.org/10.1002/ange.201207193
12	Y Hu, J O Jensen, W Zhang, L N Cleemann, W Xing, N J Bjerrum, Q Li. Hollow spheres of iron carbide nanoparticles encased in graphitic layers as oxygen reduction catalysts. Angewandte Chemie International Edition, 2014, 53(14): 3675–3679 https://doi.org/10.1002/anie.201400358
13	H Xu, Y Li, R Wang. Pore-rich iron-nitrogen-doped carbon nanofoam as an efficient catalyst towards the oxygen reduction reaction. International Journal of Hydrogen Energy, 2019, 44(48): 26285–26295 https://doi.org/10.1016/j.ijhydene.2019.08.104
14	W Li, J Wu, D C Higgins, J Y Choi, Z Chen. Determination of iron active sites in pyrolyzed iron-based catalysts for the oxygen reduction reaction. ACS Catalysis, 2012, 2(12): 2761–2768 https://doi.org/10.1021/cs300579b
15	W Jiang, L Gu, L Li, Y Zhang, X Zhang, L Zhang, J Wang, J Hu, Z Wei, L Wan. Understanding the high activity of Fe-N-C electrocatalysts in oxygen reduction: Fe/Fe3C nanoparticles boost the activity of Fe-Nx. Journal of the American Chemical Society, 2016, 138(10): 3570–3578 https://doi.org/10.1021/jacs.6b00757
16	S Kattel, G Wang. Reaction pathway for oxygen reduction on FeN4 embedded graphene. Journal of Physical Chemistry Letters, 2014, 5(3): 452–456 https://doi.org/10.1021/jz402717r
17	P H Matter, E Wang, J M M Millet, U S Ozkan. Characterization of the iron phase in CNx-based oxygen reduction reaction catalysts. Journal of Physical Chemistry C, 2007, 111(3): 1444–1450 https://doi.org/10.1021/jp0651236
18	V Nallathambi, J W Lee, S P Kumaraguru, G Wu, B N Popov. Development of high performance carbon composite catalyst for oxygen reduction reaction in PEM Proton Exchange Membrane fuel cells. Journal of Power Sources, 2008, 183(1): 34–42 https://doi.org/10.1016/j.jpowsour.2008.05.020
19	P H Matter, E Wang, M Arias, E J Biddinger, U S Ozkan. Oxygen reduction reaction catalysts prepared from acetonitrile pyrolysis over alumina-supported metal particles. Journal of Physical Chemistry B, 2006, 110(37): 18374–18384 https://doi.org/10.1021/jp062206d
20	P H Matter, L Zhang, U S Ozkan. The role of nanostructure in nitrogen-containing carbon catalysts for the oxygen reduction reaction. Journal of Catalysis, 2006, 239(1): 83–96 https://doi.org/10.1016/j.jcat.2006.01.022
21	S Hofmann, R Blume, C T Wirth, M Cantoro, R Sharma, C Ducati, M Hävecker, S Zafeiratos, P Schnoerch, A Oestereich, D Teschner, M Albrecht, A Knop-Gericke, R Schlögl, J Robertson. State of transition metal catalysts during carbon nanotube growth. Journal of Physical Chemistry C, 2009, 113(5): 1648–1656 https://doi.org/10.1021/jp808560p
22	G Liu, X Li, P Ganesan, B N Popov. Studies of oxygen reduction reaction active sites and stability of nitrogen-modified carbon composite catalysts for PEM fuel cells. Electrochimica Acta, 2010, 55(8): 2853–2858 https://doi.org/10.1016/j.electacta.2009.12.055
23	G Liu, X Li, P Ganesan, B N Popov. Development of non-precious metal oxygen-reduction catalysts for PEM fuel cells based on N-doped ordered porous carbon. Applied Catalysis B: Environmental, 2009, 93(1–2): 156–165 https://doi.org/10.1016/j.apcatb.2009.09.025
24	L Lai, J R Potts, D Zhan, L Wang, C K Poh, C Tang, H Gong, Z Shen, J Lin, R S Ruoff. Exploration of the active center structure of nitrogen-doped graphene-based catalysts for oxygen reduction reaction. Energy & Environmental Science, 2012, 5(7): 7936–7942 https://doi.org/10.1039/c2ee21802j
25	D Guo, R Shibuya, C Akiba, S Saji, T Kondo, J Nakamura. Active sites of nitrogen-doped carbon materials for oxygen reduction reaction clarified using model catalysts. Science, 2016, 351(6271): 361–365 https://doi.org/10.1126/science.aad0832
26	K Gong, F Du, Z Xia, M Durstock, L Dai. Nitrogen-doped carbon nanotube arrays with high electrocatalytic activity for oxygen reduction. Science, 2009, 323(5915): 760–764 https://doi.org/10.1126/science.1168049
27	S Kundu, T C Nagaiah, W Xia, Y Wang, S V Dommele, J H Bitter, M Santa, G Grundmeier, M Bron, W Schuhmann, M Muhler. Electrocatalytic activity and stability of nitrogen-containing carbon nanotubes in the oxygen reduction reaction. Journal of Physical Chemistry C, 2009, 113(32): 14302–14310 https://doi.org/10.1021/jp811320d
28	B Delley. From molecules to solids with the DMol3 approach. Journal of Chemical Physics, 2000, 113(18): 7756–7764 https://doi.org/10.1063/1.1316015
29	J P Perdew, K Burke, M Ernzerhof. Generalized gradient approximation made simple. Physical Review Letters, 1996, 77(18): 3865–3868 https://doi.org/10.1103/PhysRevLett.77.3865
30	S Grimme. Semiempirical GGA-type density functional constructed with a long-range dispersion correction. Journal of Computational Chemistry, 2006, 27(15): 1787–1799 https://doi.org/10.1002/jcc.20495
31	C J Cramer. Essentials of Computational Chemistry: Theories and Models. Wiley, 2004
32	Q Liu, X Liu, L Zheng, J Shui. The solid-phase synthesis of an Fe-N-C electrocatalyst for high-power proton-exchange membrane fuel cells. Angewandte Chemie International Edition, 2018, 57(5): 1204–1208 https://doi.org/10.1002/anie.201709597
33	M Wu, Q Tang, F Dong, Z Bai, L Zhang, J Qiao. Fe/N/S-composited hierarchically porous carbons with optimized surface functionality, composition and nanoarchitecture as electrocatalysts for oxygen reduction reaction. Journal of Catalysis, 2017, 352: 208–217 https://doi.org/10.1016/j.jcat.2017.05.011
34	W Xia, J Tang, J Li, S Zhang, K Wu, J He, Y Yamauchi. Defect-rich graphene nanomech produced by thermal exfoliation of metal-organic frameworks for the oxygen reduction reaction. Angewandte Chemie International Edition, 2019, 58(38): 13354–13359 https://doi.org/10.1002/anie.201906870
35	Y Jiang, L Yang, X Wang, Q Wu, J Ma, Z Hu. Doping sp2 carbon to boost the activity for oxygen reduction in an acidic medium: a theoretical exploration. RSC Advances, 2016, 6(54): 48498–48503 https://doi.org/10.1039/C6RA06473F
36	B Hammer, J K Nørskov. Theoretical surface science and catalysis-calculations and concepts. Advances in Catalysis, 2000, 45: 71–129 https://doi.org/10.1016/S0360-0564(02)45013-4
37	H Tan, Y Li, J Kim, T Takei, Z Wang, X Xu, J Wang, Y Bando, Y Kang, J Tang, Y Yamauchi. Sub-50 nm iron-nitrogen-doped hollow carbon sphere encapsulated iron carbide nanoparticles as efficient oxygen reduction catalysts. Advancement of Science, 2018, 5(7): 1800120 https://doi.org/10.1002/advs.201800120
38	P Chen, T Zhou, L Xing, K Xu, Y Tong, H Xie, L Zhang, W Yan, W Chu, C Wu, Y Xie. Atomically dispersed iron-nitrogen species as electrocatalysts for bifunctional oxygen evolution and reduction reactions. Angewandte Chemie International Edition, 2017, 56(2): 610–614 https://doi.org/10.1002/anie.201610119
39	H Tan, J Tang, J Henzie, Y Li, X Xu, T Chen, Z Wang, J Wang, Y Ide, Y Bando, Y Yamauchi. Assembly of hollow carbon nanospheres on graphene nanosheets and creation of iron-nitrogen-doped porous carbon for oxygen reduction. ACS Nano, 2018, 12(6): 5674–5683 https://doi.org/10.1021/acsnano.8b01502

[1]

FEP-20014-OF-LL_suppl_1

Download

[1]	Yanyan GAO, Ming HOU, Manman QI, Liang HE, Haiping CHEN, Wenzhe LUO, Zhigang SHAO. New insight into effect of potential on degradation of Fe-N-C catalyst for ORR[J]. Front. Energy, 2021, 15(2): 421-430.
[2]	Xiashuang LUO, Yangge GUO, Hongru ZHOU, Huan REN, Shuiyun SHEN, Guanghua WEI, Junliang ZHANG. Thermal annealing synthesis of double-shell truncated octahedral Pt-Ni alloys for oxygen reduction reaction of polymer electrolyte membrane fuel cells[J]. Front. Energy, 2020, 14(4): 767-777.
[3]	Changlin ZHANG, Xiaochen SHEN, Yanbo PAN, Zhenmeng PENG. A review of Pt-based electrocatalysts for oxygen reduction reaction[J]. Front. Energy, 2017, 11(3): 268-285.
[4]	Qiaowan CHANG, Yuan XU, Shangqian ZHU, Fei XIAO, Minhua SHAO. Pt-Ni nanourchins as electrocatalysts for oxygen reduction reaction[J]. Front. Energy, 2017, 11(3): 254-259.
[5]	Hongjie ZHANG, Yachao ZENG, Longsheng CAO, Limeng YANG, Dahui FANG, Baolian YI, Zhigang SHAO. Enhanced electrocatalytic performance of ultrathin PtNi alloy nanowires for oxygen reduction reaction[J]. Front. Energy, 2017, 11(3): 260-267.
[6]	Junliang ZHANG. Recent advances in cathode electrocatalysts for PEM fuel cells[J]. Front Energ, 2011, 5(2): 137-148.
[7]	T.S. Zhao, Y.S. Li, S.Y. Shen. Anion-exchange membrane direct ethanol fuel cells: Status and perspective[J]. Front Energ Power Eng Chin, 2010, 4(4): 443-458.

Viewed

Full text

Abstract

Cited

Shared

Discussed