石墨烯纳米带的可控制备研究进展

doi:10.6023/A22120513

化学学报 ›› 2023, Vol. 81 ›› Issue (4): 406-419.DOI: 10.6023/A22120513 上一篇下一篇

综述

石墨烯纳米带的可控制备研究进展

宁聪聪^a, 杨倩^b^,^*(), 毛阿敏^a, 唐梓嘉^a, 金燕^a, 胡宝山^a^,^*()

a 重庆大学化学化工学院重庆 401331
b 重庆科技学院冶金与材料工程学院重庆 401331

投稿日期:2022-12-28 发布日期:2023-03-16

作者简介:

宁聪聪, 重庆大学2020级在读硕士生. 2020年毕业于江南大学, 获得学士学位. 主要从事石墨烯纳米带的生长及性质研究, 发表SCI论文1篇.

杨倩, 博士, 助理研究员, 硕士生导师. 2013年毕业于重庆大学获学士学位, 2018年毕业于重庆大学获博士学位. 2018年~2020年在北京大学化学与分子工程学院从事博士后研究, 2021年加入重庆科技学院工作. 研究方向为二维材料的制备及其应用. 主持国家自然科学基金1项, 发表SCI论文10余篇.

毛阿敏, 重庆大学2020级在读硕士生. 2020年毕业于重庆大学, 获得学士学位. 主要从事石墨烯的可控制备及性质应用研究.

唐梓嘉, 重庆大学2021级在读硕士生. 2021年毕业于武汉理工大学, 获得学士学位. 主要从事石墨烯条带的可控制备及其性质研究.

金燕, 重庆大学化学化工学院实验师, 主要从事石墨烯及其复合材料的控制制备及其应用研究, 发表SCI论文10余篇.

胡宝山, 重庆大学化学化工学院副院长, 副教授, 重庆市引进高层次人才. 主要研究方向为碳纳米材料控制制备、功能化及其应用. 主持多个国家级和省部级项目, 发表SCI论文50余篇.

基金资助:
重庆市教委科技攻关项目(KJZD-M202000102); 国家自然科学基金(22005040); 中央高校科研业务专项基金(2021CDJQY-005)

Research Progress in Controllable Preparation of Graphene Nanoribbons

Congcong Ning^a, Qian Yang^b^,^*(), Amin Mao^a, Zijia Tang^a, Yan Jin^a, Baoshan Hu^a^,^*()

a School of Chemistry and Chemical Engineering, Chongqing University, Chongqing 401331
b School of Metallurgy and Materials Engineering, Chongqing University of Science and Technology, Chongqing 401331

Received:2022-12-28 Published:2023-03-16
Contact: * E-mail: qianyang@cqust.edu.cn; hubaoshan@cqu.edu.cn
Supported by:
Science and Technology Research Project of Chongqing Education Commission(KJZD-M202000102); National Natural Science Foundation of China(22005040); Fundamental Research Funds for the Central Universities(2021CDJQY-005)

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摘要/Abstract

石墨烯纳米带是宽度为纳米尺度的石墨烯条带, 根据其边缘构型的不同可以分为锯齿型石墨烯纳米带和扶手型石墨烯纳米带. 纳米尺度导致的量子限域效应和边缘构型引起的边缘效应能够调节石墨烯纳米带的电子结构, 打开石墨烯的带隙. 而且, 石墨烯纳米带具有极大的长宽比和极高比例的边缘原子, 为通过结构裁剪实现功能定制提供了无限可能. 这些几何和电子结构特性使得石墨烯纳米带在电子器件等诸多领域比石墨烯具有更大的应用潜力, 因此, 石墨烯纳米带的相关研究一直是纳米材料领域的热点. 基于此, 本综述首先介绍了石墨烯纳米带的结构和性质, 全面介绍了石墨烯纳米带的制备方法, 相应的制备方法可以分为两部分: (1)自上而下法: 通过等离子体、离子束、扫描隧道显微镜和金属纳米颗粒对石墨烯和碳纳米管进行刻蚀和切割, 制备石墨烯纳米带. 该方法面临最大挑战在于如何提高刻蚀和切割精度. (2)自下而上法: 利用含碳前驱体, 如有机化合物、碳氢化合物气体以及碳化硅等, 制备石墨烯纳米带. 该方法利于实现原子精度的结构控制, 尤其是化学气相沉积法有望实现低成本、规模化制备. 最后展望石墨烯纳米带研究的挑战和前景. 我们相信, 随着材料和技术的创新发展, 石墨烯纳米带必将成为一种具有巨大应用潜力的新型功能材料.

关键词: 石墨烯纳米带, 制备, 结构, 性质, 功能化

Graphene nanoribbons (GNRs) are the ribbons of graphene with a width of nanoscale. According to the different edge configurations, the GNRs can be classified into Zigzag-edge graphene nanoribbons (ZGNRs) and Armchair-edge graphene nanoribbons (AGNRs), strongly affecting electronic structure and properties of GNRs. The triggered quantum confinement and edge effects by rationalizing the structural design can open the bandgap of GNRs. Besides, GNRs have huge length-to-width ratio and proportion of edge atoms, which provide infinite possibilities for realizing functional customization through structure tailoring. These geometric and electronic structural properties make graphene nanoribbons have more application potential than graphene in many fields such as electronic devices. Therefore, the related research of graphene nanoribbons has been a hot spot in the field of nanomaterials. This review introduces the structures and properties of graphene nanoribbons firstly, and then provides a comprehensive picture of the preparation approaches of GNRs, and the corresponding preparation methods can be divided into two parts: (1) Top-down categories: The GNRs are obtained by the etching and cutting of graphene, as well as carbon nanotubes (CNTs), with utilizing the plasma, ion beam, scanning tunneling microscope and metal nanoparticles. However, these methods are still in the stage of laboratory research, and fabrication of high quality GNRs is difficult because of lacking the processing accuracy. (2) Bottom-up categories: The GNRs can be synthesized using carbon containing precursors, e.g. organic compounds, hydrocarbon gas and SiC. The bottom-up method facilitates to prepare several nanometers-width GNRs with a certain degree of controllability, among which ultra-narrow GNRs can be fabricated using organic synthesis, and the chemical vapor deposition (CVD) method is expected to achieve the industrial production of high-quality GNRs with low-cost preparation. Finally, we discuss the challenges and prospects of the research of GNRs. We believe that GNRs will become a new structural and functional material with great application potential in numerous fields, as is catalyzed by innovative development of materials and techniques.

Key words: graphene nanoribbons, preparation, structure, property, functionalization

引用此文

宁聪聪, 杨倩, 毛阿敏, 唐梓嘉, 金燕, 胡宝山. 石墨烯纳米带的可控制备研究进展[J]. 化学学报, 2023, 81(4): 406-419.

Congcong Ning, Qian Yang, Amin Mao, Zijia Tang, Yan Jin, Baoshan Hu. Research Progress in Controllable Preparation of Graphene Nanoribbons[J]. Acta Chimica Sinica, 2023, 81(4): 406-419.

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图/表 8

图1. GNRs的构型图. (a)锯齿型石墨烯纳米带; (b)扶手椅型石墨烯纳米带; (c)边缘空位的石墨烯纳米带; (d) ZGNRs-AGNRs交替出现的GNRs

Figure 1. Structure illustration of graphene nanoribbons. (a) Zigzag-edge graphene nanoribbons; (b) Armchair-edge graphene nanoribbons; (c) GNRs with edge vacancy; (d) GNRs with ZGNRs-AGNRs alternate edge

图2. 掩模辅助切割石墨烯制备石墨烯纳米带. (a) HSQ保护下掩模刻蚀GNR的原子力显微镜(Atomic force microscopy, AFM)图像[21]; (b)不同宽度平行GNR的扫描电子显微镜(Scanning electron microscope, SEM)图像[21]; (c) GNRs器件的SEM图像[21]; (d, e)氧等离子体刻蚀前(d)、后(e) GNRs-FET的SEM图像[24]; (f)纳米线掩模等离子体刻蚀制备GNR的工艺原理图[27]; (g)纳米线掩模等离子体刻蚀制备GNR的工艺原理图[29]; (h~l)石墨烯褶皱自掩模制备GNRs阵列[30]

Figure 2. Preparation of graphene nanoribbons by cutting graphene with mask. (a) AFM image of GNRs covered by a protective HSQ etch mask[21]; (b) SEM of fabricated parallel GNRs with different widths[21]; (c) SEM image of a device containing GNR [21]; (d, e) SEM images and cross sections of FETs before (d) and after (e) oxygen plasma etched graphene[24]; (f) schematic fabrication process to obtain GNRs by oxygen plasma etch with a nanowire etch mask[27]; (g) Schematic illustration of the nanowire-masked O2 plasma etching process[29]; (h~l) wrinkle engineering for fabricating GNRs array[30]

图3. 无掩模切割石墨烯制备石墨烯纳米带. (a)氦离子束刻蚀制备GNRs示意图[35]; (b, c)纳米粒子刻蚀石墨烯形成两个120°角(b)和一个60°角(c)的示意图和AFM图[38]

Figure 3. Preparation of graphene nanoribbons by cutting graphene without mask. (a) Scheme of GNR arrays fabricated by helium ion beam lithography[35]; (b, c) drawing and AFM image of a nanoribbon created by a nanoparticle, forming two angles of 120o (b) and one angle of 60o (c) [38]

图4. 切割碳纳米管法制备石墨烯纳米带. (a)切割CNTs管壁制备GNRs的透射电子显微镜(Transmission electron microscope, TEM)[44]; (b, c) Ni纳米粒子切割MWCNTs的SEM图像[46]; (d) Ni或Co金属纳米粒子沿轴向切割MWCNTs制备GNRs的不同阶段示意图[46]; (e)等离子体刻蚀PMMA/MWCNTs复合体制备GNRs的示意图[47]; (f)裂解CNTs制备GNRs的分子动力学模拟图[48]

Figure 4. Preparation of graphene nanoribbons by cutting carbon nanotubes. (a) TEM images of the gradual unzipping of one wall of a carbon nanotube to form a nanoribbon[44]; (b, c) SEM images of MWCNTs cut with Ni nanoparticles[46]; (d) schematic diagram representing different stages of cutting MWCNTs along their axes with Ni or Co metal nanoparticles[46]; (e) making GNRs from MWCNTs which are partially embedded in PMMA[47]; (f) molecular dynamics simulation of making GNRs by unzipping CNTs [48]

图5. 有机合成法制备石墨烯纳米带. (a) Cai课题组[53]利用有机合成法制备GNRs的合成方案; (b)自下而上法制备纳米石墨烯和GNRs的示意图[58]; (c) RP-CVD反应装置示意图并阐明选用DBBA作单体制备GNRs的生长机理[59]; (d)常压Au(111)基底上由DBTT前驱体合成GNRs的示意图[60]; (e)非聚氨基(左)和十二聚氨基聚合物(右)的STM图[60]

Figure 5. Preparation of graphene nanoribbons by organic synthesis. (a) Reaction scheme for the formation of linear graphene nanoribbons as reported by Cai and co-workers[53]; (b) syntheses of NGs and nanoribbons by a bottom-up approach[58]; (c) experimental setup of RP-CVD with an illustration of the presumed GNRs growth mechanism when using DBBA as a monomer[59]; (d) schematic illustration of the synthesis for GNRs with DBTT precursors on Au(111) under atmospheric pressure[60]; (e) STM images of undecameric (left) and dodecameric (right) polymer [60]

图6. SiC外延生长法制备石墨烯纳米带. (a) SiC沟槽的AFM图像[66]; (b)图(a)中沟槽侧壁的STM图像[66]; (c)图(b)中侧壁阶梯的STM放大图[66]; (d) GNRs在SiC侧壁外延生长的示意图[66]; (e) SiC外延生长制备GNRs的示意图[68]

Figure 6. Preparation of graphene nanoribbons by SiC epitaxial growth method. (a) AFM image of the SiC sidewall[66]; (b) STM topography image of the ladder-pattern in part (a) [66]; (c) zoomed-in image of part (b) with the armchair edges superimposed[66]; (d) schematic illustration of graphene epitaxially grown on the SiC sidewall[66]; (e) schematic illustration of preparation GNRs by SiC epitaxial growth method [68]

图7. CVD法制备石墨烯纳米带. (a~d)石墨烯岛在Ge(001)表面作成核位点(a)和Ge(001)表面的GNRs阵列(b), 其中(a, b)为示意图, (c, d)为对应的SEM图像[82]; (e)液态Cu基底制备GNRs阵列示意图[85]; (f)模板辅助CVD生长GNRs的示意图[86]; (g) ZnS/G条带的SEM图像[86]; (h) Ni纳米棒直接生长制备GNRs的示意图[87]; (i) h-BN上沟槽的AFM图像, 沟槽的宽度和深度如图标记[89]; (j)嵌入沟槽GNR的AFM图像, 宽度如图标记[89]; (k)梯形槽内CVD生长GNRs阵列的示意图[90]; (l~n) G＋G (l), NG＋G (m)和NG＋NG (n)条带堆叠变温拉曼光谱图[90]

Figure 7. Preparation of graphene nanoribbons with the CVD method. (a~d) Graphene islands as growth seeds (a) and GNR arrays (b) on Ge(001) with schematic illustrations (a, b) and SEM images (c, d)[82]; (e) schematic illustration of growth of GNR array on liquid Cu[85]; (f) schematic diagram of the templated CVD growth of the GNRs[86]; (g) SEM images of the ZnS/G ribbons[86]; (h) schematic illustration of the direct conversion process of Ni nanobar to grow graphene nanoribbon[87]; (i) AFM image of zigzag trench on h-BN with width and depth as labelled[89]; (j) AFM image of a GNR embedded in trench with width as labelled[89]; (k) the schematic diagram for trapezoidal grooves and CVD growth of the GNR arrays[90]; (l~n) the variable temperature Raman spectra of stacked G＋G (l), NG＋G (m) and NG＋NG (n) samples [90]

制备方法		优点	缺点
切割石墨烯	掩模刻蚀法^{[24⇓⇓⇓⇓⇓-30]}	大面积、可控图案化制备	加工精度低、边缘结构不规则、掩模去除困难
切割石墨烯	无掩模刻蚀法^{[32⇓⇓⇓⇓⇓⇓⇓⇓⇓⇓-43]}	加工精度高、边缘结构可控、制备质量高	生产成本高、生产规模小
切割碳纳米管	氧化反应切割法^[44-45]	原料成本低	提纯工艺复杂
	纳米粒子切割法^[46]	条带缺陷少、边缘平直且洁净	切割方向难控制、边缘结构不规则
	等离子体切割法^[47]	条带宽度低至数十纳米	边缘结构不规则
有机合成法	真空表面合成法^{[53⇓⇓⇓⇓-58]}	条带宽度低至数纳米	条带较短、对设备要求高、成本高
	常压表面合成法^[59⇓-61]	效率高、条带宽度窄	生产规模小
	溶液合成法^{[62⇓⇓-65]}	反应条件温和、无需贵金属催化剂	提纯复杂、产率低、制备过程复杂
SiC外延生长法^{[66⇓⇓⇓-70]}	—	无需转移、条带质量高	生产规模小
CVD生长法	选区直接生长法^{[77⇓⇓⇓⇓⇓⇓⇓-85]}	条带质量高、大面积可控制备	条带长宽比较小
	模板生长法^[86⇓-88]	条带较长、质量高	条带长宽比较小
	限域生长法^[89-90]	条带较长、质量高、可控图案化制备	条带宽度控制困难

表1. 不同方法制备GNRs的优缺点

Table 1. Reported advantages and disadvantages for GNRs prepared with various processes

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石墨烯纳米带的可控制备研究进展

Research Progress in Controllable Preparation of Graphene Nanoribbons

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