等离子体对石墨烯的功能化改性

赵雯琪; 张岱; 崔明慧; 杜颖; 张树宇; 区琼荣

doi:10.7498/aps.70.20202078

摘要

等离子体态物质富含高反应活性粒子群, 包括电子、离子、自由基、光子等, 是催化或直接参与化学反应的重要因子, 在化学合成与材料改性领域有重要应用价值, 往往可以使热平衡条件下难以发生, 甚至不能发生的化学反应, 在等离子体催化下得以发生和加速. 常规条件下的石墨烯就是低反应活性物质, 往往需要在高温甚至高压和强酸强碱条件下才能发生化学反应, 对于新型石墨烯衍生材料的合成与改性是一个束缚. 而等离子体催化石墨烯反应, 可以在常温常压无腐蚀性条件下, 引发石墨烯的还原、氧化、缺陷修复、掺杂、接枝、外延生长和交联等一系列化学反应, 为石墨烯功能化改性及其新型复合材料合成提供了更多可能性, 值得深入探索. 过去十多年, 等离子体在石墨烯合成与改性方面的研究报道并不鲜见, 特色鲜明, 然而, 较多的报道停留在技术路线的尝试以及结果呈现层面, 化学反应动力学研究鲜有涉及, 本文对这些研究报道进行综合论述, 主要是对部分代表性研究结果的再报告和总结性讨论, 旨在促进相关领域的深入研究.

关键词:

石墨烯 /
等离子体 /
表面改性 /
掺杂 /
催化

Abstract

Plasma contains highly reactive species, including electrons, ions, radicals, photons, etc., which are critical for catalyzing or directly participating in chemical reactions. Plasma is a highly efficient tool in chemical synthesis and material modification, since it can make the chemical reactions that are difficult or even impossible to occur under thermal equilibrium conditions take place and accelerate through its catalysis. The chemical reactivity of graphene under conventional conditions is low, which means that the reaction of graphene requires high temperature, high pressure and/or strong acid or alkali, thereby restricting the synthesis and modification of novel graphene-derived materials. Plasma-assisted graphene reaction can trigger a series of chemical reactions, such as reduction, oxidation, defect repair, doping, grafting, epitaxial growth and cross-linking of graphene, under ambient temperature and pressure without any corrosive conditions. It provides great potentials for the functional modification of graphene and the synthesis of graphene composites, which deserve further exploration. Over the past decade, a number of studies of graphene synthesis and modification by using plasma with distinctive characteristics have been reported. However, most of reports focused on the presentation of technical routes and corresponding results, and the research on chemical reaction kinetics is still far from being fully addressed. In this review, we make a comprehensive discussion about these reports by mainly summarizing and discussing some of the representative results, in order to promote further research in the relevant fields.

Keywords:

graphene /
plasma /
surface modification /
doping /
catalysis

作者及机构信息

赵雯琪,
张岱,
崔明慧,
杜颖,
张树宇,
区琼荣

复旦大学电光源研究所, 工程与应用技术研究院超越照明研究所, 上海　200433

通信作者: 张树宇, zhangshuyu@fudan.edu.cn ; 区琼荣, qrou@fudan.edu.cn

基金项目: 国家自然科学基金 (批准号: 51677031, 11975081)资助的课题

Authors and contacts

Zhao Wen-Qi,
Zhang Dai,
Cui Ming-Hui,
Du Ying,
Zhang Shu-Yu,
Ou Qiong-Rong

Institute of Future Lighting, Academy for Engineering and Technology, Institute for Electric Light Sources, Fudan University, Shanghai 200433, China

Corresponding author: Zhang Shu-Yu, zhangshuyu@fudan.edu.cn ; Ou Qiong-Rong, qrou@fudan.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 51677031, 11975081)

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施引文献

图 1 等离子体技术改性石墨烯的主要物理过程示意图

Fig. 1. A schematic diagram of the main physical processes of graphene modification based on plasma technologies.

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图 2 (a) PECVD方法在Ni基板上生长石墨烯示意图^{[ 14]}; (b) PECVD方法在Si/SiO₂基板上生长单层石墨烯示意图^{[ 25]}; (c) PECVD方法在Cu催化与非催化条件下生长垂直石墨烯示意图^{[ 28]}

Fig. 2. A schematic diagram of (a) growing graphene on a Ni substrate by PECVD^{[ 14]}, (b) growing monolayer graphene on a Si/SiO₂ substrate by PECVD ^{[ 25]} and (c) growing vertical graphene by PECVD with and without Cu catalysis ^{[ 28]}.

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图 3 (a) DBD等离子体还原GO示意图^{[ 50]}; (b) CH₄/Ar等离子体同步还原与修复GO过程^{[ 54]}; (c) Ar等离子体一步还原HAuCl₄与GO示意图^{[ 57]}; (d)等离子体还原与热还原形核生长过程示意图^{[ 60]}

Fig. 3. A schematic diagram of (a) GO reduction using DBD plasma^{[ 50]}, (b) GO reduction and repair using CH₄/Ar plasma^{[ 54]}, (c) one-step reduction of HAuCl₄ and GO using Ar plasma^{[ 57]}, (d) nucleation and growth process using plasma reduction and thermal reduction, respectively^{[ 60]}.

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图 4 氧等离子体处理对石墨烯的功能化修饰　(a) SLG, BLG, FLG经氧等离子体处理后的光致发光行为及表面原子结构示意图^{[ 67]}; (b) GO与氧等离子体处理后的GO (P-GO)表面扫描电子显微镜(scanning electron microscope, SEM)图^{[ 78]}; (c) 碳化硅衬底(SiC)、高序热解石墨(highly oriented pyrolytic graphite, HOPG)以及SiC上的SLG和氧等离子体处理后的SLG上的水滴^{[ 86]}; (d) 单层纳米多孔石墨烯膜的制备与性能测试示意图^{[ 89]}

Fig. 4. Functional modification of graphene by oxygen plasma treatment: (a) Photoluminescence image of SLG, BLG and FLG after exposure to O₂ plasma and a schematic illustration of the atomic structure of graphene after O₂ plasma treatment^{[ 67]}; (b) SEM photos of pristine GO and P-GO surfaces^{[ 78]}; (c) water droplets on SiC, HOPG, SLG on SiC, and oxygen-plasma-etched graphene on SiC^{[ 86]}; (d) a schematic illustration of preparation and characterization of monolayer nanoporous graphene films^{[ 89]}.

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图 5 (a) 本征石墨烯的能带结构^{[ 92]}; (b) 石墨烯狄拉克点位置和费米能级随不同掺杂类型变化原理图^{[ 95]}; (c) 石墨烯氮掺杂的三种构型: 吡啶氮、吡咯氮和石墨氮^{[ 103]}; (d) 氮掺杂石墨烯催化H₂O₂电化学还原的循环伏安曲线^{[ 103]}; (e) 氮掺杂Co₉S₈/graphene的Co 2p轨道分峰谱(左)和N 1s轨道分峰谱(右)^{[ 108]}; (f) 硫掺杂石墨烯催化OER反应极化曲线^{[ 112]}

Fig. 5. (a) Band structure of pristine graphene^{[ 92]}; (b) the position of the Dirac point and the Fermi level as a function of doping type^{[ 95]}; (c) bonding configurations for nitrogen atoms in N-graphene^{[ 103]}; (d) cyclic voltammograms of H₂O₂ on N-graphene electrode^{[ 103]}; (e) Co 2p deconvolution spectra (left) and N 1s deconvolution spectra of N-Co₉S₈/graphene (right)^{[ 108]}; (f) linear sweep voltammograms for OER of S-graphene^{[ 112]}.

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