Abstract
In this work, hierarchically porous carbon spheres co-doped by iron and nitrogen were synthesized via in situ dehalogenation. The rich porous structure and relatively high specific surface area (210 m2/g) facilitate the formation of an ultra-fine Fe2N active phase and FeN4 active centers within the carbon matrix. Transmission electron microscopy and X-ray photoelectron spectroscopy analysis further reveal the presence of a dominant Fe2N phase and minor FeN4 bonds in the as-prepared Fe-N-C-pd-800 samples. Because of this, the oxygen reduction reaction (ORR) process can more readily take place on Fe2N than on FeN4, and the Fe2N phase enriched Fe-N-C-pd-800 carbon spheres exhibit a promising onset potential (Eonset=1.02 V) and half-wave potential (E1/2=0.86 V) in alkaline media. In addition, Fe-N-C-pd-800 also shows excellent methanol resistance and long-cycling stability.
Similar content being viewed by others
References
M. Sun, D. Davenport, H. Liu, Qu. Jiuhui, M. Elimelech, and J. Li, J. Mater. Chem. A 6, 2527 (2018).
J.K. Seok, M. Javeed, K. Changmin, H. Gaofeng, W.K. Seong, J. Sunmin, Z. Guomin, J.J. De Yoreo, K. Guntae, and B.B. Jong, J. Am. Chem. Soc. 140, 1737 (2018).
A.M. Rasol, A.F. Azam, and B. Maliheh, J. Electron. Mater. 48, 2971 (2019).
Y. Li, F. Li, Y. Zhao, S. Li, J. Zeng, H. Yao, and Yu. Chen, J. Mater. Chem. A 7, 20658 (2019).
Y. Li, F. Li, X. Meng, Wu. Xinru, S. Li, and Yu. Chen, Nano Energy 54, 238 (2018).
L. Ma, S. Chen, Z. Pei, Y. Huang, G. Liang, F. Mo, Q. Yang, J. Su, Y. Gao, J.A. Zapien, and C. Zhi, ACS Nano 12, 1949 (2018).
R.A. Mirzaie, A.A. Firooz, and N.M. Khori, J. Electron. Mater. 47, 6995 (2018).
H. Tan, Y. Li, X. Jiang, J. Tang, Z. Wang, H. Qian, P. Mei, V. Malgras, Y. Bando, and Y. Yamauchi, Nano Energy 36, 286 (2017).
L. Cao, Z. Lin, J. Huang, Yu. Xiang, Wu. Xiaoxian, B. Zhang, Y. Zhan, F. Xie, W. Zhang, J. Chen, W. Xie, W. Mai, and H. Meng, Int. J. Hydrogen Energy. 42, 876 (2017).
Y.J. Sa, D.J. Seo, J. Woo, J.T. Lim, J.Y. Cheon, S.Y. Yang, J.M. Lee, D. Kang, T.J. Shin, H.S. Shin, H.Y. Jeong, C.S. Kim, M.G. Kim, T.Y. Kim, and S.H. Joo, J. Am. Chem. Soc. 138, 15046 (2016).
F. Meng, Z. Wang, H. Zhong, J. Wang, J. Yan, and X. Zhang, Adv. Mater. 28, 7948 (2016).
X. Cui, S. Yang, X. Yan, J. Leng, S. Shuang, P.M. Ajayan, and Z. Zhang, Adv. Funct. Mater. 26, 5708 (2016).
W. Jiang, Gu. Lin, Li. Li, Y. Zhang, X. Zhang, L. Zhang, J. Wang, Hu. Jinsong, Z. Wei, and L. Wan, J. Am. Chem. Soc. 138, 3570 (2016).
J. Wang, Wu. Haihua, D. Gao, S. Miao, G. Wang, and X. Bao, Nano Energy 13, 387 (2015).
D. Zhou, L. Yang, L. Yu, J. Kong, X. Yao, W. Liu, Z. Xu, and X. Lu, Nanoscale 7, 1501 (2015).
Ji. Liang, R. Zhou, and X. Chen, Adv. Mater. 26, 6074 (2014).
L. Lin, Q. Zhu, and X. Anwu, J. Am. Chem. Soc. 136, 11027 (2014).
U. Tylus, Q. Jia, K. Strickland, N. Ramaswamy, A. Serov, P. Atanassov, and S. Mukerjee, J. Phys. Chem. C. 118, 8999 (2014).
Y. Chen, Z. Li, Y. Zhu, D. Sun, X. Liu, Xu. Lin, and Y. Tan, Adv. Mater. 31, e1806312 (2019).
J. Li, S. Li, Y. Tang, M. Han, Z. Dai, J. Bao, and Y. Lan, Chem. Commun. 51, 2710 (2015).
Z. Zhang, J. Sun, F. Wang, and L. Dai, Angew. Chem. Int. Ed. 57, 9038 (2018).
W. Yan, W. Cheong, R. Shen, Fu. Ninghua, Gu. Lin, Z. Zhuang, C. Chen, D. Wang, Q. Peng, J. Li, and Y. Li, Adv. Mater. 30, e1800588 (2018).
W.J. Jiang, H. Weili, Q. Zhang, T. Zhao, H. Luo, X. Zhang, Gu. Lin, Hu. Jinsong, and L. Wan, Chem. Commu. 54, 1307 (2018).
Y. Qiao, P. Yuan, Hu. Yongfeng, J. Zhang, Mu. Shichun, J. Zhou, H. Li, H. Xia, J. He, and Xu. Qun, Adv. Mater. 30, e1804504 (2018).
Z. Guan, X. Zhang, W. Chen, J. Pei, Di. Liu, Y. Xue, W. Zhu, and Z. Zhuang, Chem. Commun. 54, 12073 (2018).
R. Jiang, Li. Li, T. Sheng, Hu. Gaofei, Y. Chen, and L. Wang, J. Am. Chem. Soc. 140, 11594 (2018).
J. Wei, Y. Liang, Y. Hu, B. Kong, G.P. Simon, J. Zhang, S.P. Jiang, and H. Wang, Angew. Chem. Int. Ed. 55, 1355 (2016).
Wu. Zhenyu, Xu. Xingxing, Hu. Bicheng, H. Liang, Y. Lin, L. Chen, and Yu. ShuHong, Angew. Chem. Int. Ed. 54, 8179 (2015).
G. Yang, W. Choi, X. Pub, and Yu. Choongho, Energy Environ. Sci. 8, 1799 (2015).
Y. Wang, N. Guo, L. Zhu, Y. Pan, R. Wang, Z. Zhang, and S. Qiu, Chem. Commun. 54, 12974 (2018).
C. Cheng, S. Li, Yi. Xia, L. Ma, C. Nie, C. Roth, A. Thomas, and R. Haag, Adv. Mater. 30, 1802669 (2018).
Hu. Bicheng, Wu. Zhenyu, S. Chu, H. Zhu, H. Liang, J. Zhang, and Yu. Shuhong, Energy Environ. Sci. 11, 2208 (2018).
J. Han, H. Bao, J. Wang, L. Zheng, S. Sune, Z.L. Wang, and C. Sun, Appl. Catal. B 280, 119411 (2021).
L. Jiang, J. Duan, J. Zhu, S. Chen, and M. Antonietti, ACS Nano 14, 2436 (2020).
D. Lei, G. Zhang, X. Liu, A. Hassanpour, M. Dubois, A. Tavares, and S. Sun, Carbon Energy 2, 561 (2020).
X. Yan, Yi. Jia, K. Wang, Z. Jin, C. Dong, Y. Huang, J. Chen, and X. Yao, Carbon Energy 2, 452 (2020).
R. Paul, Q. Dai, Hu. Chuangang, and L. Dai, Carbon Energy 1, 19 (2019).
Y. Lou, J. Liu, M. Liu, and F. Wang, ACS Catal. 10, 2443 (2020).
H. Jin, X. Feng, J. Li, M. Li, Y. Xia, Y. Yuan, C. Yang, B. Dai, Z. Lin, J. Wang, Lu. Jun, and S. Wang, Angew. Chem. Int. Ed. 58, 2397 (2019).
C. Cui, Y. Gao, J. Li, C. Yang, M. Liu, H. Jin, Z. Xia, L. Dai, Y. Lei, J. Wang, and S. Wang, Angew. Chem. Int. Ed. 59, 7928 (2020).
C. Yang, H. Jin, C. Cui, J. Li, J. Wang, K. Amine, Lu. Jun, and S. Wang, Nano Energy 54, 192 (2018).
Lu. Huihang, C. Yang, J. Chen, J. Li, H. Jin, J. Wang, S. Wang, and T.H.P. Nitrogen-, Small 16, 1906584 (2020).
Acknowledgments
This work was supported by the National Natural Science Foundation of China (51872209, 51772219), the Zhejiang Provincial Natural Science Foundation of China (LZ17E020002, LZ21E020001) and Natural Sciences and Engineering Research Council of Canada (NSERC).
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interest
The authors declare that they have no conflict of interest.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary Information
Below is the link to the Supplementary Information.
Rights and permissions
About this article
Cite this article
Wu, W., Wang, M., Huang, H. et al. Porous Carbon Spheres with Ultra-fine Fe2N Active Phase for Efficient Electrocatalytic Oxygen Reduction. J. Electron. Mater. 50, 3078–3083 (2021). https://doi.org/10.1007/s11664-021-08824-9
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11664-021-08824-9