Synthesis of Nitrogen-doped Graphene and Its Electrocatalytic Performance Toward Oxygen Reduction Reaction

doi:10.7503/cjcu20120658

Abstract

Abstract:

A series nGs with different electrocatalytic abilities toward oxygen reduction reaction(ORR) was prepared via a two-steps pyrolysis method by controlling the reaction temperature on the physical mixture of graphene oxideand urea. Transmission electron microscopy and scanning electron microscopy display nG with highly wrinkled and overlapping structures. X-ray photoelectron spectroscopy shows that nitrogen is successfu-lly doped in graphene with the formation of pyridinic N, pyrrolic N and graphitic N, and the maximum nitrogen content is 6.6%(molar fraction). Cyclic voltammogram and rotating disk electrode measurement show that nGs exhibit high electrocatalytic activity with an onset potential of 0.1 V in an acid electrolyte. Moreover, the nGs catalyzed oxygen reduction revealed a favorable formation of water via a four-electron pathway and excellent stability over Pt/C catalyst. Furthermore, the nG obtained at 200 ℃ in the first pyrolysis step displays the best catalytic perfor-mance.

Key words: Nitrogen-doped graphene, Urea, Pyrolysis, Oxygen reduction reaction, Electrocatalyst

CLC Number:

O613
O646

TrendMD:

LI Jing, WANG Xian-Bao, YANG Jia, YANG Xu-Yu, WAN Li. Synthesis of Nitrogen-doped Graphene and Its Electrocatalytic Performance Toward Oxygen Reduction Reaction[J]. Chem. J. Chinese Universities, 2013, 34(4): 800.

References

[1] Novoselov K. S., Geim A. K., Morozov S. V., Jiang D., Zhang Y., Dubonos S. V., Grigorieva I. V., Firsov A. A., Science, 2004, 306(5696), 666—669
[2] Lee C. G., Wei X. D., Kysar J. W., Hone J., Science, 2008, 321(5887), 385—388
[3] Balandin A. A., Ghosh S., Bao W. Z., Calizo I., Teweldebrhan D., Miao F., Lau C. N., Nano Lett., 2008, 8(3), 902—907
[4] Service R. F., Science, 2009, 324(5929), 875—877
[5] Stoller M. D., Park S., Zhu Y. W., An J. H., Ruoff R. S., Nano Lett., 2008, 8(10), 3498—3502
[6] Xu D., Zhou N. L., Shen J., Chem. J. Chinese Universities, 2010, 31(12), 2354—2359(徐东, 周宁琳, 沈健. 高等学校化学学报, 2010, 31(12), 2354—2359)
[7] Zhu L. X., Li Y. Z., Zhao X., Zhang Q. H., Chem. J. Chinese Universities, 2012, 33(8), 1804—1808(朱龙秀, 李英芝, 赵昕, 张清华. 高等学校化学学报, 2012, 33(8), 1804—1808)
[8] Ao Z. M., Peeters F. M., J. Phys. Chem. C, 2010, 114(34), 14503—14509
[9] Wehling T. O., Novoselov K. S., Morozov S. V., Vdovin E. E., Katsnelson M. I., Geim A. K., Lichtenstein A. I., Nano Lett., 2008, 8(1), 173—177
[10] Shao Y. Y., Zhang S., Engelhard M. H., Li G. S., Shao G. C., Wang Y., Liu J., Aksay I. A., Lin Y. H., J. Mater. Chem., 2010, 20, 7491—7496
[11] Schedin F., Geim A. K., Morozov S.V., Hill E.W., Blake P., Katsnelson M. I., Novoselov K. S., Nat. Mater., 2007, 6, 652—655
[12] Shi Y. M., Kim K. K., Reina A., Hofmann M., Li L. J., Kong J., ACS Nano, 2010, 4(5), 2689—2694
[13] Jeong H. M., Lee J. W., Shin W. H., Choi Y. J., Shin H. J., Kang J. K., Choi J. W., Nano Lett., 2011, 11(6), 2472—2477
[14] Nistor R. A., Newns D. M., Martyna G. J., ACS Nano, 2011, 5(4), 3096—3103
[15] Jung N., Kim N., Jockusch S., Turro N. J., Kim P., Brus L., Nano Lett., 2009, 9(12), 4133—4137
[16] Attaccalite C., Rubio A., Phys. Status Solidi B, 2009, 246(11), 2523—2526
[17] Jorio A., Dresselhaus G., Dresselhaus M. S., Carbon Nanotubes: Advanced Topics in the Synthesis, Structure, Properties and Applications, Springer, Berlin, 2008, 531—566
[18] Yu S. S., Zheng W. T., Wang C., Jiang Q., ACS Nano, 2010, 4(12), 7619—7629
[19] Panchakarla L. S., Subrahmanyam K. S., Saha S. K., Govindaraj A., Krishnamurthy H. R., Waghmare U. V., Rao C. N. R., Adv. Mater., 2009, 21(46), 4726—4730
[20] Zhang L. P., Xia Z. H., J. Phys. Chem. C, 2011, 115(22), 11170—11176
[21] Lherbier A., Blase X., Niquet Y. M., Triozon F., Roche S., Phys. Rev. Lett., 2008, 101, 036808-1—036808-4
[22] Wu M., Cao C., Jiang J. Z., Nanotechnology, 2010, 21, 505202-1—505202-6
[23] Deifallah M., McMillan P. F., Corà F., J. Phys. Chem. C, 2008, 112(14), 5447—5453
[24] Wei D. C., Liu Y. Q., Wang Y., Zhang H. L., Huang L. P., Yu G., Nano Lett., 2009, 9(5), 1752—1758
[25] Wang X. R., Li X. L., Zhang L., Yoon Y., Weber P. K., Wang H. L., Guo J., Dai H. J., Science, 2009, 324(5928), 768—771
[26] Reddy A. L. M., Srivastava A., Gowda S. R., Gullapalli H., Dubey M., Ajayan P. M., ACS Nano, 2010, 4(11), 6337—6342
[27] Wang H. B., Zhang C. J., Liu Z. H., Wang L., Han P. X., Xu H. X., Zhang K. J., Dong S. M., Yao J. H., Cui G. L., J. Mater. Chem., 2011, 21(14), 5430—5434
[28] Wang Y., Shao Y. Y., Matson D. W., Li J. H., Lin Y. H., ACS Nano, 2010, 4(4), 1790—1798
[29] Lin Z. Y., Liu Y., Yao Y. G., Hildreth O. J., Li Z., Moon K., Wong C. P., J. Phys. Chem. C, 2011, 115(14), 7120—7125
[30] Guan L., Cui L., Lin K., Wang Y. Y., Wang X. T., Jin F. M., He F., Chen X. P., Cui S., Appl. Phys. A, 2011, 102(2), 289—294
[31] Deng D. H., Pan X. L., Yu L., Cui Y., Jiang Y. P., Qi J., Li W. X., Fu Q., Ma X. C., Xue Q. K., Sun G. Q., Bao X. H., Chem. Mater., 2011, 23(5), 1188—1193
[32] Long D. H., Li W., Ling L. C., Miyawaki J., Mochida I., Yoon S. H., Langmuir, 2010, 26(20), 16096—16102
[33] Geng D. H., Chen Y., Chen Y. G., Li Y. L., Li R. Y., Sun X. L., Ye S. Y., Knights S., Energy Environ. Sci., 2011, 4(3), 760—764
[34] Li X. L., Wang H. L., Robinson J. T., Sanchez H., Diankov G., Dai H. J., J. Am. Chem. Soc., 2009, 131(43), 15939—15944
[35] Sheng Z. H., Shao L., Chen J. J., Bao W. J., Wang F. B., Xia X. H., ACS Nano, 2011, 5(6), 4350—4358
[36] Mou Z. G., Chen X. Y., Du Y. K., Wang X. M., Yang P., Wang S. D., Appl. Surf. Sci., 2011, 258(5), 1704—1710
[37] Wang X. B., You H. J., Liu F. M., Li M. J., Li S. Q., Li Q., Xu Y., Tian R., Yu Z. Y., Xiang D., Cheng J., Chem. Vapor Depos., 2009, 15(1), 53—56
[38] Wang J. C., Wang X. B., Wan L., Yang Y. K., Wang S. M., Chin. J. Chem., 2010, 28(10), 1935—1940
[39] Shen Y., Zhou P., Sun Q. Q., Wan L., Li J., Chen L. Y., Zhang D. W., Wang X. B., Appl. Phys. Lett., 2011, 99(14), 141911-1—141911-3
[40] Yang X. Y., Wang X. B., Li J., Yang J., Wan L., Wang J. C., Chem. J. Chinese Universities, 2012, 33(9), 1902—1907(杨旭宇, 王贤保, 李静, 杨佳, 万丽, 王敬超. 高等学校化学学报, 2012, 33(9), 1902—1907)
[41] Xu C. H., Wang X. B., Wang J. C., Hu H. T., Wan L., Chem. Phys. Lett., 2010, 498(1), 162—167
[42] Hu H. T., Wang X. B., Wang J. C., Wan L., Liu F. M., Zheng H., Chen R., Xu C. H., Chem. Phys. Lett., 2010, 484(4), 247—253
[43] Wang J. C., Wang X. B., Xu C. H., Zhang M., Shang X. P., Polym. Int., 2011, 60(5), 816—822
[44] Xu C. H., Wang J. C., Wan L., Lin J. J., Wang X. B., J. Mater. Chem., 2011, 21(28), 10463—10471
[45] Xu C. H., Li J., Wang X. B., Wang J. C., Wan L., Li Y. Y., Zhang M., Shang X. P., Yang Y. K., Mater. Chem. Phys., 2012, 132(2), 858—864
[46] Lv H. F., Mu S. C., Cheng N. C., Pan M., Appl. Catal. B, 2010, 100(1), 190—196
[47] Bard A. J., Faulkner L. R., Electrochemical Methods: Fundamentals and Aplications, Wiley, New York, 2001, 341—342