微波辐照气相法合成氮掺杂石墨烯

doi:10.3724/SP.J.1077.2012.00146

无机材料学报 ›› 2012, Vol. 27 ›› Issue (2): 146-150.DOI: 10.3724/SP.J.1077.2012.00146 CSTR: 32189.14.SP.J.1077.2012.00146

微波辐照气相法合成氮掺杂石墨烯

王灿¹, 王艳莉¹, 詹亮¹, 何星², 杨俊和², 乔文明¹, 凌立成¹

(1. 华东理工大学化学工程联合国家重点实验室, 上海 200237; 2. 上海理工大学材料科学与工程学院, 上海200093)

收稿日期:2011-06-04 修回日期:2011-07-26 出版日期:2012-02-10 网络出版日期:2012-01-05
作者简介:王灿(1983-), 男, 博士研究生.
基金资助:
国家自然科学基金(20806024, 50672025, 5073003, 51002051);中央高校基本科研业务费专项基金(WA1014016);国家863重点项目(2008AA062302)

Synthesis of Nitrogen Doped Graphene through Microwave Irradiation

WANG Can¹, WANG Yan-Li¹, ZHAN Liang¹, HE Xing², YANG Jun-He², QIAO Wen-Ming¹, LING Li-Cheng¹

(1. State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China; 2. School of Material Science and Technology, University of Shanghai for Science and Technology, Shanghai 200093, China)

Received:2011-06-04 Revised:2011-07-26 Published:2012-02-10 Online:2012-01-05
About author:WANG Can
Supported by:
National Natural Science Foundation of China (20806024, 50672025, 5073003, 51002051);The Central University Scientific Tesearch (WA1014016);863 Program (2008AA062302)

摘要/Abstract

摘要：

以天然鳞片石墨为原料, 采用Staudenmaier法先制备出石墨氧化物, 再经饱和碳酸铵溶液浸渍后生成NH₄⁺插层石墨氧化物. 在微波照射下, NH₄⁺分解生成的NH₃与剥离的石墨烯氧化物反应原位合成出氮掺杂石墨烯. 通过SEM、TEM、EDS、XRD、XPS和Raman测试手段对氮掺杂石墨烯进行了表征. 结果表明, 所合成的氮掺杂石墨烯呈透明绢丝状结构, 每个石墨烯片含有2~5层石墨层; 氮元素含量为1.56wt%, 其中N元素是以pyridinc N、 pyrrolic N和graphitic N形式掺入石墨层网格中.

关键词: 石墨烯, 氮掺杂, 微波辐照气相法

Abstract:

Graphite oxide was synthesized with Staudenmaier method using natural flake graphite as carbon source. After graphite oxide was impregnated into ammonium carbonate saturated solution, NH₄⁺intercalated graphite oxide was given. Rapid thermal exfoliation and reduction of NH₄⁺intercalated graphite oxide to graphene was achieved as well as the nitrogen-doping of graphene under the condition of microwave irradiation. SEM, TEM, EDS, XRD, XPS and Raman were performed to characterize the synthesized nitrogen-doping of graphene. The synthesized nitrogen-doped graphene was transparent and wrinkled with 2-5 graphite layers. The nitrogen content of as-prepared nitrogen-doped graphene was 1.56wt%, corresponding to pyridinc N, pyrrolic N and graphitic N incorporated into the graphitic network.

Key words: graphene, nitrogen-doped, microwave irradiation

中图分类号:

TQ383

王灿, 王艳莉, 詹亮, 何星, 杨俊和, 乔文明, 凌立成. 微波辐照气相法合成氮掺杂石墨烯[J]. 无机材料学报, 2012, 27(2): 146-150.

WANG Can, WANG Yan-Li, ZHAN Liang, HE Xing, YANG Jun-He, QIAO Wen-Ming, LING Li-Cheng. Synthesis of Nitrogen Doped Graphene through Microwave Irradiation[J]. Journal of Inorganic Materials, 2012, 27(2): 146-150.

图/表 6

图1 石墨、石墨插层化合物和氮掺杂石墨烯的XRD图谱

Fig. 1 XRD patterns of natural graphite, NH4+ intercalated graphite oxide and nitrogen doped graphene

图2 NH4+插层石墨氧化物在微波辐照前(a)后(b)的对比图, NH4+插层石墨氧化物(c)和氮掺杂石墨烯(d,e)的SEM照片

Fig. 2 Optical photos of NH4+ intercalated graphite oxide before (a) and after (b) microwave treatment. SEM images of NH4+ intercalated graphite oxide (c) and nitrogen doped graphene (d,e)

图3 氮掺杂石墨烯的TEM照片(a,b), HRTEM图片(c)和EDS分析(d)

Fig. 3 (a,b) TEM, (c) HRTEM images of nitrogen doped graphene and (d) EDS analysis of nitrogen doped grapheme

图4 氮掺杂石墨烯的XPS图谱(a)XPS全谱; (b)C1s谱; (c)N1s谱; (d)示意图

Fig. 4 (a) Full-range XPS spectra of graphene and nitrogen doped graphene; (b) C1s and (c) N1s spectra of nitrogen doped graphene; (d) Schematic representation of the nitrogen doped graphene

图5 微波辐照气相法合成的石墨烯和氮掺杂石墨烯的Raman光谱

Fig. 5 Raman spectra of graphene and nitrogen doped graphene

图6 微波辐照气相法合成氮掺杂石墨烯的机理

Fig. 6 Schematic illustration of simultaneous doping and exfoliation of graphite oxide

参考文献 16

[1]	Novoselov K S, Geim A K, Morozov S V, et al. Electric field effect in atomically thin carbon films. Science, 2004, 306(5696): 666-669.
[2]	Lee C G, Wei X D, Kysar J W, et al. Measurement of the elastic properties and intrinsic strength of monolayer graphene. Science, 2008, 321(5887): 385-388.
[3]	Balandin A A, Ghosh S, Bao W Z, et al. Superior thermal conductivity of single-layer graphene. Nano Letters, 2008, 8(10): 902-907.
[4]	Stankovich S, Dikin D A, Dommett G H B, et al. Graphene-based composite materials. Nature, 2006, 442(7100): 282-286.
[5]	Chen J H, Jang C, Xiao S D, et al. Intrinsic and extrinsic performance limits of graphene devices on SiO2. Nature Nanotechnol., 2008, 3(4): 206-209.
[6]	Wang X R, Li X L, Zhang L, et al. N-doping of graphene through electrothermal reactions with ammonia. Science, 2009, 324(5928): 768-771.
[7]	Wang Y, Shao Y Y, Matson D W, et al. Nitrogen-doped graphene and its application in electrochemical biosensing. ACS Nano, 2010, 4(4): 1790-1798.
[8]	Shao Y Y, Zhang S, Engelhard M H, et al. Nitrogen-doped graphene and its electrochemical applications. Journal of Chemical materials, 2010, 20(35): 7491-7496.
[9]	Guo B D, Liu Q, Chen E, et al. Controllable N-doping of graphene. Nano Letters, 2010, 10(12): 4975-4980.
[10]	Li N, Wang Z Y, Zhao K K, et al. Large scale synthesis of N-doped multi-layered graphene sheets by simple arc-discharge method. Carbon, 2010, 48(1): 255-259.
[11]	Li X L, Wang H L, Robinson J T, et al. Simultaneous nitrogen doping and reduction of graphene oxide. Journal of the American Chemical Society, 2009, 131(43):15939-15944.
[12]	Qu LT, Liu Y, Baek J B, et al. Nitrogen-doped graphene as efficient metal-free electrocatalyst for oxygen reduction in fuel cells. ACS Nano, 2010, 4(3): 1321-1326.
[13]	Reddy A L M, Srivastava A, Gowda S R, et al. Synthesis of nitrogen- doped graphene films for lithium battery application. ACS Nano, 2010, 4(11): 6337-6342.
[14]	Bujans F B, Cerveny S, Verdejo R, et al. Permanent adsorption of organic solvents in graphite oxide and its effect on the thermal exfoliation. Carbon, 2010, 48(4): 1079-1087.
[15]	Matsuo Y, Higashika S, Kimura K, et al. Synthesis of polyaniline- intercalated layered materials via exchange reaction. Journal of Materials Chemistry, 2002, 12(5):1592-1596.
[16]	Seredych M, Bandosz T J. Removal of ammonia by graphite oxide via its intercalation and reactive adsorption. Carbon, 2007, 45(10): 2126-2139.

微波辐照气相法合成氮掺杂石墨烯

Synthesis of Nitrogen Doped Graphene through Microwave Irradiation

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