Graphene modification based on plasma technologies

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

doi:10.7498/aps.70.20202078

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:

Authors and contacts

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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Cited By

图 1 等离子体技术改性石墨烯的主要物理过程示意图

Figure 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]

Figure 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]

Figure 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]

Figure 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]

Figure 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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