Oxygen Reduction Performance of the Nitrogen-Doped Carbon Materials Pyrolyzed from Polyaniline/Carbon Nanocage Composites

doi:10.6023/A15050354

Acta Chim. Sinica ›› 2015, Vol. 73 ›› Issue (8): 793-798.DOI: 10.6023/A15050354 Previous Articles Next Articles

Communication

热解聚苯胺/碳纳米笼复合物制备氮掺杂碳材料及其氧还原性能研究

许智慧, 沈丽明, 吴强, 孙涛, 徐宇洋, 黎聃勤, 杜玲玉, 杨立军, 王喜章, 胡征

介观化学教育部重点实验室南京大学化学化工学院南京 210093

投稿日期:2015-05-24 发布日期:2015-07-07
通讯作者: 吴强 E-mail:wqchem@nju.edu.cn
基金资助:
项目受国家自然科学基金(Nos. 51232003, 21173115, 21203092, 21473089)和“973”项目(No. 2013CB932902)资助.

Oxygen Reduction Performance of the Nitrogen-Doped Carbon Materials Pyrolyzed from Polyaniline/Carbon Nanocage Composites

Xu Zhihui, Shen Liming, Wu Qiang, Sun Tao, Xu Yuyang, Li Danqin, Du Lingyu, Yang Lijun, Wang Xizhang, Hu Zheng

Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093

Received:2015-05-24 Published:2015-07-07
Supported by:
Project supported by the National Natural Science Foundation of China (Nos. 51232003, 21173115, 21203092, 21473089) and “973” program (No. 2013CB932902).

Fuel cells can efficiently convert chemical energy of fuels into electrical energy in a green manner, representing one of the most promising movable power sources. The main bottleneck for the wide application of fuel cells is the sluggish oxygen reduction reaction (ORR) which is usually catalyzed by expensive and unstable Pt catalysts. Hence, the exploration of cost-efficient and long-life ORR electrocatalysts is of great significance. Recently carbon-based metal-free ORR electrocatalysts have attracted much interest due to their superior activity and stability as well as the abundance and low cost. It is generally accepted that nitrogen doping of carbon materials boost the ORR activity by breaking the electroneutrality of carbon layer and activating π electrons. Considering that the embedded N doping sites are useless for ORR but significantly affect electron conduction, the carbon materials with N-enriched surface of high activity and pristine carbon bulk of high conductivity should present better ORR performance than the bulk N-doped counterpart. In this contribution, we report an efficient strategy for the synthesis of ORR electrocatalysts with surface enriched N doping and high conductive bulk by dispersing polyaniline (PANI) on the surface of 3D hierarchical carbon nanocages (CNC), followed by heat treatment in Ar. The N content and conductivity of the pyrolyzed products are regulated by changing the pyrolysis temperature and the weight ratio of PANI/CNC composite. The optimized electrocatalyst with the N content of 2.21 at% and the conductivity of 203 S·m^-1 exhibits excellent ORR catalytic performance with high onset potential of -46 mV vs Ag/AgCl, obvious superior to the bulk N-doped CNC (-105 mV). This catalyst also possesses high stability (96% activity retention after 10 h continuous tests) and dominated 2-electron pathway for ORR with transferred electron number of 2.8. This result suggests an efficient route to improve the ORR activity of carbon-based materials by increasing the N content enriched at the surface while keeping their high conductivity.

Key words: nitrogen doping, polyaniline pyrolysis, carbon nanocages, oxygen reduction, fuel cells

Cite this article

Xu Zhihui, Shen Liming, Wu Qiang, Sun Tao, Xu Yuyang, Li Danqin, Du Lingyu, Yang Lijun, Wang Xizhang, Hu Zheng. Oxygen Reduction Performance of the Nitrogen-Doped Carbon Materials Pyrolyzed from Polyaniline/Carbon Nanocage Composites[J]. Acta Chim. Sinica, 2015, 73(8): 793-798.

Export EndNote|Reference Manager|ProCite|BibTeX|RefWorks

share this article

References

[1] Chu, S.; Majumdar, A. Nature 2012, 488, 294.
[2] Wang, Z. H.; Shi, G. Y.; Xia, J. F.; Zhang, F. F.; Xia, Y. Z.; Li, Y. H.; Xia, L. H. Acta Chim. Sinica 2013, 71, 1225. (王宗花, 史国玉, 夏建飞, 张菲菲, 夏延致, 李延辉, 夏临华, 化学学报, 2013, 71, 1225.)
[3] Gasteiger, H. A.; Markovic, N. M. Science 2009, 324, 48.
[4] Gong, K. P.; Du, F.; Xia, Z. H.; Durstock, M.; Dai, L. M. Science 2009, 323, 760.
[5] Jiang, S. J.; Ma, Y. W.; Jian, G. Q.; Tao, H. S.; Wang, X. Z.; Fan, Y. N.; Lu, Y. N.; Hu, Z.; Chen, Y. Adv. Mater. 2009, 21, 4953.
[6] Wu, J. B.; Yang, H. Acc. Chem. Res. 2013, 46, 1848.
[7] Zhang, S.; Zhang, S.; Jiang, S. M.; Zhu, H. Y.; Guo, S. J.; Su, D.; Lu, G.; Sun, S. H. J. Am. Chem. Soc. 2014, 136, 7734.
[8] Chen, Z. W.; Higgins, D.; Yu, A. P.; Zhang, L.; Zhang, J. J. Energy Environ. Sci. 2011, 4, 3167.
[9] Liang, Y. Y.; Li, Y. G.; Wang, H. L.; Dai, H. J. J. Am. Chem. Soc. 2013, 135, 2013.
[10] Sun, T.; Wu, Q.; Che, R. C.; Bu, Y. F.; Jiang, Y. F.; Li, Y.; Yang, L. J.; Wang, X. Z.; Hu, Z. ACS Catal. 2015, 5, 1857.
[11] Qu, L.-T.; Liu, Y.; Baek, J. B.; Dai, L.-M. ACS Nano 2010, 4, 1321.
[12] Liu, R.-L.; Wu, D.-P.; Feng, X.-L.; Müllen, K. Angew. Chem., Int. Ed. 2010, 49, 1.
[13] Chen, S.; Bi, J. Y.; Zhao, Y.; Yang, L. J.; Zhang, C.; Ma, Y. W.; Wu, Q.; Wang, X. Z.; Hu, Z. Adv. Mater. 2012, 24, 5593.
[14] Yang, L. J.; Jiang, S. J.; Zhao, Y.; Zhu, L.; Chen, S.; Wang, X. Z.; Wu, Q.; Ma, J.; Ma, Y. W.; Hu, Z. Angew. Chem., Int. Ed. 2011, 50, 7132.
[15] Zhao, Y.; Yang, L. J.; Chen, S.; Wang, X. Z.; Ma, Y. W.; Wu, Q.; Jiang, Y. F.; Qian, W. J.; Hu, Z. J. Am. Chem. Soc. 2013, 135, 1201.
[16] Liang, J.; Jiao, Y.; Jaroniec, M.; Qiao, S.-Z. Angew. Chem., Int. Ed. 2012, 51, 11496.
[17] Yang, Z.; Yao, Z.; Li, G.-F.; Fang, G.-Y.; Nie, H.-G.; Liu, Z.; Zhou, X.-M.; Chen, X.; Huang, S.-M. ACS Nano 2012, 6, 205.
[18] Liu, Z. W.; Peng, F.; Wang, H. J.; Yu, H.; Zheng, W. X.; Yang, J. Angew. Chem., Int. Ed. 2011, 50, 3257.
[19] Wang, L. W.; Feng, R.; Xia, J. Z.; Chen, S.; Wu, Q.; Yang, L. J.; Wang, X. Z.; Hu, Z. Acta Chim. Sinica 2014, 72, 1070. (王立伟, 冯瑞, 夏婧竹, 陈盛, 吴强, 杨立军, 王喜章, 胡征, 化学学报, 2014, 72, 1070.)
[20] Dai, L. M.; Xue, Y. H.; Qu, L. T.; Choi, H. J.; Baek, J. B. Chem. Rev. 2015, 115, 4823.
[21] Tian, G. L.; Zhang, Q.; Zhang, B. S.; Jin, Y. G.; Huang, J. Q.; Su, D. S.; Wei, F. Adv. Funct. Mater. 2014, 24, 5956.
[22] Wang, X. Q.; Lee, J. S.; Zhu, Q.; Liu, J.; Wang, Y.; Dai, S. Chem. Mater. 2010, 22, 2178.
[23] Chen, L.; Du, R.; Zhu, J. H.; Mao, Y. Y.; Xue, C.; Zhang, N.; Hou, Y. L.; Zhang, J.; Yi, T. Small 2015, 11, 1423.
[24] Yazdi, A. Z.; Fei, H. L.; Ye, R. Q.; Wang, G.; Tour, J.; Sundararaj, U. ACS Appl. Mater. Interfaces 2015, 7, 7786.
[25] Zhang, L. J.; Su, Z. X.; Jiang, F. L.; Yang, L. L.; Qian, J. J.; Zhou, Y. F.; Li, W. M.; Hong, M. C. Nanoscale 2014, 6, 6590.
[26] Xie, K.; Qin, X. T.; Wang, X. Z.; Wang, Y. N.; Tao, H. S.; Wu, Q.; Yang, L. J.; Hu, Z. Adv. Mater. 2012, 24, 347.
[27] Lyu, Z. Y.; Xu, D.; Yang, L. J.; Che, R. C.; Feng, R.; Zhao, J.; Li, Y.; Wu, Q.; Wang, X. Z.; Hu, Z. Nano Energy 2015, 12, 657.
[28] Liang, Y.-Y.; Wang, H.-L.; Zhou, J.-G.; Li, Y.-G.; Wang, J.; Regier, T.; Dai, H.-J. J. Am. Chem. Soc. 2012, 134, 3517.

热解聚苯胺/碳纳米笼复合物制备氮掺杂碳材料及其氧还原性能研究

Oxygen Reduction Performance of the Nitrogen-Doped Carbon Materials Pyrolyzed from Polyaniline/Carbon Nanocage Composites

PDF

Knowledge

Cited

Abstract

Cite this article

share this article

References

Related Articles 15

Recommended Articles

Metrics

Comments

[1]	Ping Li, Qiyu Yang, Jing Zeng, Ran Zhang, Qiuyan Chen, Fei Yan. Effect of Fluorine Doping on the Performance of Reversible Solid Oxide Cells and Related Kinetic Studies [J]. Acta Chimica Sinica, 2024, 82(1): 36-45.
[2]	Jinjing Liu, Na Yang, Li Li, Zidong Wei. Theoretical Study on the Regulation of Oxygen Reduction Mechanism by Modulating the Spatial Structure of Active Sites on Platinum^★ [J]. Acta Chimica Sinica, 2023, 81(11): 1478-1485.
[3]	Qingxin Wang, Yong Cui, Yunqi Li, Shanfu Lu, Yan Xiang. Effect of Controllable Pyrolysis of Ionomers in Fe-N-C Cathode Catalytic Layer on Cell Performance and Stability of Membrane Electrode Assembly^★ [J]. Acta Chimica Sinica, 2023, 81(10): 1350-1356.
[4]	Shaobing Yan, Long Jiao, Chuanxin He, Hailong Jiang. Pyrolysis of ZIF-67/Graphene Composite to Co Nanoparticles Confined in N-Doped Carbon for Efficient Electrocatalytic Oxygen Reduction [J]. Acta Chimica Sinica, 2022, 80(8): 1084-1090.
[5]	Jiawei He, Liu Jiao, Xueyi Cheng, Guanghai Chen, Qiang Wu, Xizhang Wang, Lijun Yang, Zheng Hu. Structural Regulation of Metal Organic Framework-derived Hollow Carbon Nanocages and Their Lithium-Sulfur Battery Performance [J]. Acta Chimica Sinica, 2022, 80(7): 896-902.
[6]	Dan Wang, Bo Feng, Xiaoxin Zhang, Yanan Liu, Yan Pei, Minghua Qiao, Baoning Zong. Nitrogen-doped Carbon Pyrolyzed from ZIF-8 for Electrocatalytic Oxygen Reduction to Hydrogen Peroxide [J]. Acta Chimica Sinica, 2022, 80(6): 772-780.
[7]	Lu Xiaoqing, Cao Shoufu, Wei Xiaofei, Li Shaoren, Wei Shuxian. Investigation on Oxygen Reduction Reaction Mechanism on S Doped Fe-NC lsolated Single Atoms Catalyst [J]. Acta Chimica Sinica, 2020, 78(9): 1001-1006.
[8]	Sun Lian, Wang Honglei, Yu Jinshan, Zhou Xingui. Recent Progress on Proton-Conductive Metal-Organic Frameworks and Their Proton Exchange Membranes [J]. Acta Chimica Sinica, 2020, 78(9): 888-900.
[9]	Shui Ziyi, He Nana, Chen Li, Zhao Wei, Chen Xi. Porous Perovskite towards Oxygen Reduction Reaction in Flexible Aluminum-Air Battery [J]. Acta Chimica Sinica, 2020, 78(6): 557-564.
[10]	Zhang Jing, Tang Gong-ao, Zeng Yu, Wang Baoxing, Liu Liwei, Wu Qiang, Yang Lijun, Wang Xizhang, Hu Zheng. Hierarchical Carbon Nanocages as the High-performance Cathode for Li-O₂ Battery Promoted by Soluble Redox Mediator [J]. Acta Chimica Sinica, 2020, 78(6): 572-576.
[11]	Peng Zhengkang, Ding Huimin, Chen Rufan, Gao Chao, Wang Cheng. Research Progress in Covalent Organic Frameworks for Energy Storage and Conversion [J]. Acta Chim. Sinica, 2019, 77(8): 681-689.
[12]	Cui Lirui, Zhang Jin, Sun Yiyan, Lu Shanfu, Xiang Yan. Effect of Addition of Carbon Nanotubes on the Performance of a Low Pt Loading Membrane-Electrode-Assembly in Proton Exchange Membrane Fuel Cells [J]. Acta Chim. Sinica, 2019, 77(1): 47-53.
[13]	Zhang Zhiqi, Ge Chengxuan, Chen Yugang, Wu Qiang, Yang Lijun, Wang Xizhang, Hu Zheng. Construction of Cobalt/Nitrogen/Carbon Electrocatalysts with Highly Exposed Active Sites for Oxygen Reduction Reaction [J]. Acta Chim. Sinica, 2019, 77(1): 60-65.
[14]	Huang Wenjiao, Zhang Haoyu, Hu Shuozhen, Niu Dongfang, Zhang Xinsheng. Effect of Nitrogen-Containing Functional Groups of Cobalt Phthalocyanine Catalyst on the Oxygen Reduction Performance in Fuel Cells [J]. Acta Chim. Sinica, 2018, 76(9): 723-728.
[15]	Cai Yuejin, Liu Chenxia, Zhuo Ou, Wu Qiang, Yang Lijun, Chen Qiang, Wang Xizhang, Hu Zheng. Ruthenium Nanoparticles Supported on Hierarchical Nitrogen-Doped Carbon Nanocages for Selective Hydrogenation of Acetophenone in Mild Conditions [J]. Acta Chim. Sinica, 2017, 75(7): 686-691.