氮掺杂石墨烯的制备及其对氧还原反应的电催化性能

doi:10.3866/PKU.WHXB201407112

Abstract

Abstract:

Nitrogen-doped graphene (NG) was prepared by chemical reduction of graphene oxide (GO) 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 GO sheets were effectively reduced by DMKO. NG samples with different nitrogen contents were obtained by adjusting the mass ratio of GO to DMKO; the nitrogen contents were in the range 4.40%-5.89% (atomic fraction). NG-1, obtained using a GO/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 good tolerance of methanol cross-over effects. It is therefore superior to commercial Pt/C catalysts.

Key words: Graphene, Nitrogen doping, Oxygen reduction reaction, Electrocatalysis

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

References

(1) Debe, M. K. Nature 2012, 486, 43. doi: 10.1038/nature11115
(2) Yang, R.; Leisch, J.; Strasser, P.; Toney, M. F. Chem. Mater. 2010, 22, 4712. doi: 10.1021/cm101090p
(3) Chen, A.; Holt-Hindle, P. Chem. Rev. 2010, 110, 3767. doi: 10.1021/cr9003902
(4) Zheng, Y.; Jiao, Y.; Jaroniec, M.; Jin, Y.; Qiao, S. Z. Small 2012, 8, 3550.
(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) Zhang, M.; Dai, L. Nano Energy, 2012, 1, 514. doi: 10.1016/j.nanoen.2012.02.008
(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) 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) 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) Park, S.; Ruoff, R. S. Nat. Nanotechnol. 2009, 4, 217. doi: 10.1038/nnano.2009.58
(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) 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) Avouris, P.; Chen, Z.; Perebeinos, V. Nat. Nanotechnol. 2007, 2, 605. doi: 10.1038/nnano.2007.300
(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) 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) 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) Qu, L.; Liu, Y.; Baek, J. B.; Dai, L. ACS Nano 2010, 4, 1321. doi: 10.1021/nn901850u
(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) 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) 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) Unni, S. M.; Devulapally, S.; Karjule, N.; Kurungot, S. J. Mater. Chem. 2012, 22, 23506. doi: 10.1039/c2jm35547g
(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) 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) 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) 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) Su, P.; Guo, H. L.; Tian, L.; Ning, S. K. Carbon 2012, 50, 5351. doi: 10.1016/j.carbon.2012.07.001
(27) Wang, Y.; Shao, Y.; Matson, D.W.; Li, J.; Lin, Y. ACS Nano 2010, 4, 1790. doi: 10.1021/nn100315s
(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) 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) Saidi,W. A. J. Phys. Chem. Lett. 2013, 4, 4160. doi: 10.1021/jz402090d
(31) Lai, L.; Potts, J. R.; Zhan, D.;Wang, L.; Poh, C. K.; Tang, C.; Gong, H.; Shen, Z.; Lin, J.; Ruoff, R. S. Energy Environ. Sci. 2012, 5, 7936. doi: 10.1039/c2ee21802j

[1]	Hanyu Xu, Xuedan Song, Qing Zhang, Chang Yu, Jieshan Qiu. Mechanistic Insights into Water-Mediated CO₂ Electrochemical Reduction Reactions on Cu@C₂N Catalysts: A Theoretical Study [J]. Acta Phys. -Chim. Sin., 2024, 40(1): 2303040-.
[2]	Xinxuan Duan, Marshet Getaye Sendeku, Daoming Zhang, Daojin Zhou, Lijun Xu, Xueqing Gao, Aibing Chen, Yun Kuang, Xiaoming Sun. Tungsten-Doped NiFe-Layered Double Hydroxides as Efficient Oxygen Evolution Catalysts [J]. Acta Phys. -Chim. Sin., 2024, 40(1): 2303055-.
[3]	Ning Wang, Yi Li, Qian Cui, Xiaoyue Sun, Yue Hu, Yunjun Luo, Ran Du. Metal Aerogels: Controlled Synthesis and Applications [J]. Acta Phys. -Chim. Sin., 2023, 39(9): 2212014-0.
[4]	Weifeng Xia, Chengyu Ji, Rui Wang, Shilun Qiu, Qianrong Fang. Metal-Free Tetrathiafulvalene Based Covalent Organic Framework for Efficient Oxygen Evolution Reaction [J]. Acta Phys. -Chim. Sin., 2023, 39(9): 2212057-0.
[5]	Yanhui Yu, Peng Rao, Suyang Feng, Min Chen, Peilin Deng, Jing Li, Zhengpei Miao, Zhenye Kang, Yijun Shen, Xinlong Tian. Atomic Co Clusters for Efficient Oxygen Reduction Reaction [J]. Acta Phys. -Chim. Sin., 2023, 39(8): 2210039-0.
[6]	Chang Lan, Yuyi Chu, Shuo Wang, Changpeng Liu, Junjie Ge, Wei Xing. Research Progress of Proton-Exchange Membrane Fuel Cell Cathode Nonnoble Metal M-N_x/C-Type Oxygen Reduction Catalysts [J]. Acta Phys. -Chim. Sin., 2023, 39(8): 2210036-0.
[7]	Shuai Yang, Yuxin Xu, Zikun Hao, Shengjian Qin, Runpeng Zhang, Yu Han, Liwei Du, Ziyi Zhu, Anning Du, Xin Chen, Hao Wu, Bingbing Qiao, Jian Li, Yi Wang, Bingchen Sun, Rongrong Yan, Jinjin Zhao. Recent Advances in High-Efficiency Perovskite for Medical Sensors [J]. Acta Phys. -Chim. Sin., 2023, 39(5): 2211025-0.
[8]	Yifei Xu, Hanwen Yang, Xiaoxia Chang, Bingjun Xu. Introduction to Electrocatalytic Kinetics [J]. Acta Phys. -Chim. Sin., 2023, 39(4): 2210025-0.
[9]	Aoqi Wang, Jun Chen, Pengfei Zhang, Shan Tang, Zhaochi Feng, Tingting Yao, Can Li. Relation between NiMo(O) Phase Structures and Hydrogen Evolution Activities of Water Electrolysis [J]. Acta Phys. -Chim. Sin., 2023, 39(4): 2301023-0.
[10]	Haoliang Lv, Xuejie Wang, Yu Yang, Tao Liu, Liuyang Zhang. RGO-Coated MOF-Derived In₂Se₃ as a High-Performance Anode for Sodium-Ion Batteries [J]. Acta Phys. -Chim. Sin., 2023, 39(3): 2210014-0.
[11]	Ruifang Wei, Dongfeng Li, Heng Yin, Xiuli Wang, Can Li. Operando Electrochemical UV-Vis Absorption Spectroscopy with Microsecond Time Resolution [J]. Acta Phys. -Chim. Sin., 2023, 39(2): 2207035-0.
[12]	Tianran Wei, Shusheng Zhang, Qian Liu, Yuan Qiu, Jun Luo, Xijun Liu. Oxygen Vacancy-Rich Amorphous Copper Oxide Enables Highly Selective Electroreduction of Carbon Dioxide to Ethylene [J]. Acta Phys. -Chim. Sin., 2023, 39(2): 2207026-0.
[13]	Jingxue Li, Yue Yu, Siran Xu, Wenfu Yan, Shichun Mu, Jia-Nan Zhang. Function of Electron Spin Effect in Electrocatalysts [J]. Acta Phys. -Chim. Sin., 2023, 39(12): 2302049-.
[14]	Zheng-Min Wang, Qing-Ling Hong, Xiao-Hui Wang, Hao Huang, Yu Chen, Shu-Ni Li. RuP Nanoparticles Anchored on N-doped Graphene Aerogels for Hydrazine Oxidation-Boosted Hydrogen Production [J]. Acta Phys. -Chim. Sin., 2023, 39(12): 2303028-.
[15]	Junhao Liao, Yixuan Zhao, Zhaoning Hu, Saiyu Bu, Qi Lu, Mingpeng Shang, Kaicheng Jia, Xiaohui Qiu, Qin Xie, Li Lin, Zhongfan Liu. Crack-Free Transfer of Graphene Wafers via Photoresist as Transfer Medium [J]. Acta Phys. -Chim. Sin., 2023, 39(10): 2306038-.

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

PDF

Like

Knowledge

Abstract

Cite this article

share this article

References

Related Articles 15

Metrics

Recommended 0