Citation: PENG San, GUO Hui-Lin, KANG Xiao-Feng. Preparation of Nitrogen-Doped Graphene and Its Electrocatalytic Activity for Oxygen Reduction Reaction[J]. Acta Physico-Chimica Sinica, ;2014, 30(9): 1778-1786. doi: 10.3866/PKU.WHXB201407112 shu

Preparation of Nitrogen-Doped Graphene and Its Electrocatalytic Activity for Oxygen Reduction Reaction

1.
Key Laboratory of Synthetic and Natural Functional Molecule Chemistry Ministry of Education, College of Chemistry and Materials Science, Northwest University, Xi'an 710069, P. R. China

Received Date: 15 May 2014
Available Online: 11 July 2014
Fund Project:

Nitrogen-doped graphene (NG) was prepared by chemical reduction of graphene oxide ( ) using dimethyl ketoxime (DMKO) as reducing and doping agents. The morphologies, structures, compositions, and electrocatalytic activities of the as-prepared materials were investigated using field-emission transmission electron microscopy (FETEM), ultraviolet- visible (UV-Vis) spectroscopy, Fourier-transform infrared (FTIR) spectroscopy, X-ray photoelectron spectroscopy (XPS), zeta potential and nanoparticle analyses, cyclic voltammetry (CV), and the rotating disk electrode (RDE) method. The results showed that sheets were effectively reduced by DMKO. NG samples with different nitrogen contents were obtained by adjusting the mass ratio of to DMKO; the nitrogen contents were in the range 4.40%-5.89% (atomic fraction). NG-1, obtained using a /DMKO mass ratio of 1:0.7, showed excellent electrocatalytic activity in the oxygen reduction reaction (ORR) in an O₂-saturated 0.1 mol·L^-1 KOH solution. The peak current was 0.93 mA·cm^-2, and the number of electrons transferred per O₂ was 3.6; this was attributed to the increase in the number of ORR active sites in the presence of pyridinic-N. In addition, the electrocatalytic activity of NG was found to be dependent on the graphitic-N content, which determined the limiting current density, because of its higher electronic conductivity. The pyridinic-N content improved the onset potential, because of its lower overpotential for the ORR. NG therefore exhibited a high selectivity in the ORR, with od tolerance of methanol cross-over effects. It is therefore superior to commercial Pt/C catalysts.
- Graphene,
- Nitrogen doping,
- Oxygen reduction reaction,
- Electrocatalysis
1. [1]
  
  (1) Debe, M. K. Nature 2012, 486, 43. doi: 10.1038/nature11115
2. [2]
  (2) Yang, R.; Leisch, J.; Strasser, P.; Toney, M. F. Chem. Mater. 2010, 22, 4712. doi: 10.1021/cm101090p
3. [3]
  (3) Chen, A.; Holt-Hindle, P. Chem. Rev. 2010, 110, 3767. doi: 10.1021/cr9003902
4. [4]
  (4) Zheng, Y.; Jiao, Y.; Jaroniec, M.; Jin, Y.; Qiao, S. Z. Small 2012, 8, 3550.
5. [5]
  (5) Zhang, L.; Zhang, J.;Wilkinson, D. P.;Wang, H. J. Power Sources 2006, 156, 171. doi: 10.1016/j.jpowsour.2005.05.069
6. [6]
  (6) Zhang, M.; Dai, L. Nano Energy, 2012, 1, 514. doi: 10.1016/j.nanoen.2012.02.008
7. [7]
  (7) Nallathambi, V.; Lee, J.W.; Kumaraguru, S. P.;Wu, G.; Popov, B. N. J. Power Sources 2008, 183, 34. doi: 10.1016/j.jpowsour.2008.05.020
8. [8]
  (8) Hu, Y. J.; Jin, J.; Zhang, H.;Wu, P.; Cai, C. X. Acta Phys. -Chim. Sin. 2010, 26, 2073. [胡耀娟, 金娟, 张卉, 吴萍, 蔡称心. 物理化学学报, 2010, 26, 2073.] doi: 10.3866/PKU.WHXB20100812
9. [9]
  (9) Bunch, J. S.; Verbridge, S. S.; Alden, J. S.; van der Zande, A. M.; Parpia, J. M.; Craighead, H. G.; McEuen, P. L. Nano Lett. 2008, 8, 2458. doi: 10.1021/nl801457b
10. [10]
  (10) Park, S.; Ruoff, R. S. Nat. Nanotechnol. 2009, 4, 217. doi: 10.1038/nnano.2009.58
11. [11]
  (11) Novoselov, K. S.; Jiang, Z.; Zhang, Y.; Morozov, S. V.; Stormer, H. L.; Zeitler, U.; Maan, J. C.; Boebinger, G. S.; Kim, P.; Geim, A. K. Science 2007, 315, 1379. doi: 10.1126/science.1137201
12. [12]
  (12) Balandin, A. A.; Ghosh, S.; Bao,W.; Calizo, I.; Teweldebrhan, D.; Miao, F.; Lau, C. N. Nano Lett. 2008, 8, 902. doi: 10.1021/nl0731872 doi: 10.1021/nl0731872
13. [13]
  (13) Avouris, P.; Chen, Z.; Perebeinos, V. Nat. Nanotechnol. 2007, 2, 605. doi: 10.1038/nnano.2007.300
14. [14]
  (14) Wang, X.; Li, X.; Zhang, L.; Yoon, Y.;Weber, P. K.;Wang, H.; Guo, J.; Dai, H. Science 2009, 324, 768. doi: 10.1126/science.1170335
15. [15]
  (15) Jeon, I. Y.; Choi, H. J.; Choi, M.; Seo, J. M.; Jung, S. M.; Kim, M. J.; Zhang, S.; Zhang, L.; Xia, Z.; Dai, L.; Park, N.; Baek, J. B. Scientific Reports 2013, 3, 1810.
16. [16]
  (16) Geng, D.; Chen, Y.; Chen, Y.; Li, Y.; Li, R.; Sun, X.; Ye, S.; Knights, S. Energy Environ. Sci. 2011, 4, 760. doi: 10.1039/c0ee00326c
17. [17]
  (17) Qu, L.; Liu, Y.; Baek, J. B.; Dai, L. ACS Nano 2010, 4, 1321. doi: 10.1021/nn901850u
18. [18]
  (18) Shao, Y.; Zhang, S.; Engelhard, M. H.; Li, G.; Shao, G.;Wang, Y.; Liu, J.; Aksay, I. A.; Lin, Y. J. Mater. Chem. 2010, 20, 7491. doi: 10.1039/c0jm00782j
19. [19]
  (19) Sheng, Z. H.; Shao, L.; Chen, J. J.; Bao,W. J.;Wang, F. B.; Xia, X. H. ACS Nano 2011, 5, 4350. doi: 10.1021/nn103584t
20. [20]
  (20) Ma, G. X.; Zhao, J. H.; Zheng, J. F.; Zhu, Z. P. New Carbon Mater. 2012, 27, 258. [马贵香, 赵江红, 郑剑锋, 朱珍平. 新型炭材料, 2012, 27, 258.]
21. [21]
  (21) Unni, S. M.; Devulapally, S.; Karjule, N.; Kurun t, S. J. Mater. Chem. 2012, 22, 23506. doi: 10.1039/c2jm35547g
22. [22]
  (22) Yang, S.; Zhi, L.; Tang, K.; Feng, X.; Maier, J.; Müllen, K. Adv. Funct. Mater. 2012, 22, 3634. doi: 10.1002/adfm.v22.17
23. [23]
  (23) Li, N.;Wang, Z.; Zhao, K.; Shi, Z.; Gu, Z.; Xu, S. Carbon 2010, 48, 255. doi: 10.1016/j.carbon.2009.09.013
24. [24]
  (24) Su, P.; Guo, H. L.; Peng, S.; Ning, S. K. Acta Phys. -Chim. Sin. 2012, 28, 2745. [苏鹏, 郭慧林, 彭三, 宁生科. 物理化学学报, 2012, 28, 2745.] doi: 10.3866/PKU.WHXB201208221
25. [25]
  (25) Li, X.;Wang, H.; Robinson, J. T.; Sanchez, H.; Diankov, G.; Dai, H. J. Am. Chem. Soc. 2009, 131, 15939. doi: 10.1021/ja907098f
26. [26]
  (26) Su, P.; Guo, H. L.; Tian, L.; Ning, S. K. Carbon 2012, 50, 5351. doi: 10.1016/j.carbon.2012.07.001
27. [27]
  (27) Wang, Y.; Shao, Y.; Matson, D.W.; Li, J.; Lin, Y. ACS Nano 2010, 4, 1790. doi: 10.1021/nn100315s
28. [28]
  (28) Lin, Z.;Waller, G. H.; Liu, Y.; Liu, M.;Wong, C. P. Carbon 2013, 53, 130. doi: 10.1016/j.carbon.2012.10.039
29. [29]
  (29) Subramanian, N. P.; Li, X.; Nallathambi, V.; Kumaraguru, S. P.; Colon-Mercado, H.;Wu, G.; Lee, JW.; Popov, B. N. J. Power Sources 2009, 188, 38. doi: 10.1016/j.jpowsour.2008.11.087
30. [30]
  (30) Saidi,W. A. J. Phys. Chem. Lett. 2013, 4, 4160. doi: 10.1021/jz402090d
31. [31]
  (31) Lai, L.; Potts, J. R.; Zhan, D.;Wang, L.; Poh, C. K.; Tang, C.; ng, H.; Shen, Z.; Lin, J.; Ruoff, R. S. Energy Environ. Sci. 2012, 5, 7936. doi: 10.1039/c2ee21802j
1. [1]
  Hailang JIA , Hongcheng LI , Pengcheng JI , Yang TENG , Mingyun GUAN . Preparation and performance of N-doped carbon nanotubes composite Co₃O₄ as oxygen reduction reaction electrocatalysts. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 693-700. doi: 10.11862/CJIC.20230402
2. [2]
  Jinyi Sun , Lin Ma , Yanjie Xi , Jing Wang . Preparation and Electrocatalytic Nitrogen Reduction Performance Study of Vanadium Nitride@Nitrogen-Doped Carbon Composite Nanomaterials: A Recommended Comprehensive Chemistry Experiment. University Chemistry, 2024, 39(4): 184-191. doi: 10.3866/PKU.DXHX202310094
3. [3]
  Zhaomei LIU , Wenshi ZHONG , Jiaxin LI , Gengshen HU . Preparation of nitrogen-doped porous carbons with ultra-high surface areas for high-performance supercapacitors. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 677-685. doi: 10.11862/CJIC.20230404
4. [4]
  Zhihuan XU , Qing KANG , Yuzhen LONG , Qian YUAN , Cidong LIU , Xin LI , Genghuai TANG , Yuqing LIAO . Effect of graphene oxide concentration on the electrochemical properties of reduced graphene oxide/ZnS. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1329-1336. doi: 10.11862/CJIC.20230447
5. [5]
  Xiaofeng Zhu , Bingbing Xiao , Jiaxin Su , Shuai Wang , Qingran Zhang , Jun Wang . Transition Metal Oxides/Chalcogenides for Electrochemical Oxygen Reduction into Hydrogen Peroxides. Acta Physico-Chimica Sinica, 2024, 40(12): 2407005-. doi: 10.3866/PKU.WHXB202407005
6. [6]
  Tongtong Zhao , Yan Wang , Shiyue Qin , Liang Xu , Zhenhua Li . New Experiment Development: Upgrading and Regeneration of Discarded PET Plastic through Electrocatalysis. University Chemistry, 2024, 39(3): 308-315. doi: 10.3866/PKU.DXHX202309003
7. [7]
  Zhuo WANG , Junshan ZHANG , Shaoyan YANG , Lingyan ZHOU , Yedi LI , Yuanpei LAN . Preparation and photocatalytic performance of CeO₂-reduced graphene oxide by thermal decomposition. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1708-1718. doi: 10.11862/CJIC.20240067
8. [8]
  Kai CHEN , Fengshun WU , Shun XIAO , Jinbao ZHANG , Lihua ZHU . PtRu/nitrogen-doped carbon for electrocatalytic methanol oxidation and hydrogen evolution by water electrolysis. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1357-1367. doi: 10.11862/CJIC.20230350
9. [9]
  Yunting Shang , Yue Dai , Jianxin Zhang , Nan Zhu , Yan Su . Something about RGO (Reduced Graphene Oxide). University Chemistry, 2024, 39(9): 273-278. doi: 10.3866/PKU.DXHX202306050
10. [10]
  Jie XIE , Hongnan XU , Jianfeng LIAO , Ruoyu CHEN , Lin SUN , Zhong JIN . Nitrogen-doped 3D graphene-carbon nanotube network for efficient lithium storage. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1840-1849. doi: 10.11862/CJIC.20240216
11. [11]
  Kaihui Huang , Dejun Chen , Xin Zhang , Rongchen Shen , Peng Zhang , Difa Xu , Xin Li . Constructing Covalent Triazine Frameworks/N-Doped Carbon-Coated Cu₂O S-Scheme Heterojunctions for Boosting Photocatalytic Hydrogen Production. Acta Physico-Chimica Sinica, 2024, 40(12): 2407020-. doi: 10.3866/PKU.WHXB202407020
12. [12]
  Jiapei Zou , Junyang Zhang , Xuming Wu , Cong Wei , Simin Fang , Yuxi Wang . A Comprehensive Experiment Based on Electrocatalytic Nitrate Reduction into Ammonia: Synthesis, Characterization, Performance Exploration, and Applicable Design of Copper-based Catalysts. University Chemistry, 2024, 39(6): 373-382. doi: 10.3866/PKU.DXHX202312081
13. [13]
  Xiaoxia WANG , Ya'nan GUO , Feng SU , Chun HAN , Long SUN . Synthesis, structure, and electrocatalytic oxygen reduction reaction properties of metal antimony-based chalcogenide clusters. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1201-1208. doi: 10.11862/CJIC.20230478
14. [14]
  Xi Xu , Chaokai Zhu , Leiqing Cao , Zhuozhao Wu , Cao Guan . Experiential Education and 3D-Printed Alloys: Innovative Exploration and Student Development. University Chemistry, 2024, 39(2): 347-357. doi: 10.3866/PKU.DXHX202308039
15. [15]
  Rui PAN , Yuting MENG , Ruigang XIE , Daixiang CHEN , Jiefa SHEN , Shenghu YAN , Jianwu LIU , Yue ZHANG . Selective electrocatalytic reduction of Sn(Ⅳ) by carbon nitrogen materials prepared with different precursors. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 1015-1024. doi: 10.11862/CJIC.20230433
16. [16]
  Zhenlin Zhou , Siyuan Chen , Yi Liu , Chengguo Hu , Faqiong Zhao . A New Program of Voltammetry Experiment Teaching Based on Laser-Scribed Graphene Electrode. University Chemistry, 2024, 39(2): 358-370. doi: 10.3866/PKU.DXHX202308049
17. [17]
  Zeyu XU , Anlei DANG , Bihua DENG , Xiaoxin ZUO , Yu LU , Ping YANG , Wenzhu YIN . Evaluation of the efficacy of graphene oxide quantum dots as an ovalbumin delivery platform and adjuvant for immune enhancement. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1065-1078. doi: 10.11862/CJIC.20240099
18. [18]
  Hao BAI , Weizhi JI , Jinyan CHEN , Hongji LI , Mingji LI . Preparation of Cu₂O/Cu-vertical graphene microelectrode and detection of uric acid/electroencephalogram. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1309-1319. doi: 10.11862/CJIC.20240001
19. [19]
  Yan LIU , Jiaxin GUO , Song YANG , Shixian XU , Yanyan YANG , Zhongliang YU , Xiaogang HAO . Exclusionary recovery of phosphate anions with low concentration from wastewater using a CoNi-layered double hydroxide/graphene electronically controlled separation film. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1775-1783. doi: 10.11862/CJIC.20240043
20. [20]
  Zhiwen HU , Weixia DONG , Qifu BAO , Ping LI . Low-temperature synthesis of tetragonal BaTiO₃ for piezocatalysis. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 857-866. doi: 10.11862/CJIC.20230462

Get Citation

PDF

XML

Metrics

PDF Downloads(901)
Abstract views(939)
HTML views(29)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142