石墨烯在金属表面防腐中的应用

郭晓蒙; 青芳竹; 李雪松

doi:10.7498/aps.70.20210349

摘要

石墨烯作为一种新型材料, 因其出色的化学惰性和抗渗透性逐渐成为了防腐领域的研究热点. 本文结合最新的研究成果, 对包括石墨烯薄膜及石墨烯粉体在防腐领域的应用进行更加全面的讨论. 从石墨烯防腐作用机理(主要包括阻隔、屏蔽、缓蚀、加固、阴极保护和自修复)和其相应的涂层制备方法(化学气相沉积法制备的石墨烯薄膜及石墨烯粉体制备的复合涂料)开始, 进而探讨不同影响因素(缺陷、导电性、氧化程度、片层大小及含量等)对石墨烯防腐效果的影响, 最后对各种方法进行综合比较, 并对未来的发展进行展望. 本文通过对已有工作的回顾, 为今后制备防腐性能更加优良的石墨烯材料提供重要的参考.

关键词:

石墨烯 /
涂层 /
金属 /
防腐

Abstract

As an emerging material, graphene has become a research hotspot in the field of anti-corrosion because of its excellent chemical inertia and permeability resistance. In this paper, combined with the latest research results, the applications of graphene film and graphene powders in the field of anti-corrosion are discussed more comprehensively. First, the anti-corrosion mechanisms of graphene (mainly including barrier effect, shielding effect, corrosion inhibition synergy, enhancement of coating adhesion, cathodic protection, and self-healing effect) and its corresponding coating preparation methods (graphene film prepared by chemical vapor deposition method and composite coatings prepared with graphene powders) are introduced. Then, the influences of different factors such as defects, conductivity, oxidation degree, flake size, and content of graphene on the anti-corrosion performance are discussed. Finally, various methods are comprehensively compared with each other, and future development is prospected. This paper not only reviews the existing work, but also has a certain reference value for preparing graphene materials with better corrosion resistance in the future.

Keywords:

graphene /
coating /
metals /
anti-corrosion

作者及机构信息

1.
电子科技大学电子科学与工程学院, 电子薄膜与集成器件国家重点实验室, 成都　610054

2.
武汉工程大学化学与环境工程学院, 武汉　430074

通信作者: 青芳竹, qingfz@uestc.edu.cn ; 李雪松, lxs@uestc.edu.cn

作者简介:

青芳竹, 电子科技大学副教授, 四川大学材料学专业博士. 研究领域为石墨烯等二维材料的制备与应用, 已发表SCI论文20余篇. 现作为第一负责人主持国家自然科学基金、四川省应用基础研究项目两项

李雪松, 电子科技大学教授, 化学气相沉积甲烷在铜箔上合成大面积石墨烯薄膜方法的发明人. 清华大学机械工程专业学士、材料加工工程专业硕士, 美国伦斯勒理工材料工程专业博士. 研究领域为石墨烯等二维材料的制备与应用. 已发表包括Science等顶级期刊SCI文章70余篇, SCI统计引用次数27000多次. 2009年发表在Science的Large-area synthesis of high-quality and uniform graphene films on copper foils论文被Science选为2009年度重大突破之一, SCI引用8000余次. 该发明已在石墨烯薄膜制备研究与生产中得到了广泛的应用

基金项目: 国家自然科学基金(批准号: 51802036, 51772043)资助的课题

Authors and contacts

1.
State Key Laboratory of Electronic Thin Films and Integrated Devices, School of Electronic Science and Engineering, University of Electronic Science and Technology of China, Chengdu 610054, China

2.
School of Chemistry and Environmental Engineering, University of Wuhan Institute of Technology, Wuhan 430074, China

Corresponding author: Qing Fang-Zhu, qingfz@uestc.edu.cn ; Li Xue-Song, lxs@uestc.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 51802036, 51772043)

文章全文 : translate this paragraph

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施引文献

图 1 石墨烯防腐作用机理　(a) 阻隔作用^[13]; (b) 屏蔽作用^[17]; (c) 缓蚀作用^[18]; (d) 加固作用^[19]; (e) 阴极保护作用^[20]; (f) 自修复作用^[21]

Fig. 1. Anticorrosion mechanism of graphene: (a) Barrier effect^[13]; (b) shielding effect^[17]; (c) corrosion inhibition synergy^[18]; (d) enhancement of coating adhesion^[19]; (e) cathodic protection^[20]; (f) self-healing effect^[21].

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图 2 CVD石墨烯防腐性能^[24]　(a) 石墨烯作为化学惰性扩散阻挡层示意图; (b) 硬币经过H₂O₂浸泡(30%, 2 min)后的照片; (c) 带有和不带有石墨烯涂层的铜和铜镍合金在空气中退火(200 °C, 4 h)的照片

Fig. 2. Performance of CVD graphene as an anticorrosion layer^[24]: (a) Schematics of graphene as a chemically inert diffusion barrier; (b) photograph showing graphene coated (upper) and uncoated (lower) penny after H₂O₂ treatment (30%, 2 min); (c) photographs of Cu and Cu/Ni foils with and without graphene coating taken before and after annealing in air (200 °C, 4 h).

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图 3 不锈钢球包覆石墨烯涂层制备过程示意图^[31]

Fig. 3. Schematics of the preparation of graphene coated stainless steel balls^[31].

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图 4 溶液中FGO对碳钢表面的缓蚀机理示意图^[39]

Fig. 4. Schematics of inhibition mechanism on carbon steel surface for FGO in solution^[39].

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图 5 DETA, GO 和DETA-GO的HOMO和LUMO分布图^[40]　(a) HOMO图; (b) LUMO图

Fig. 5. HOMO and LUMO distribution maps of DETA, GO and DETA-GO^[40]: (a) LUMO; (b) HOMO.

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图 6 装有BTA的覆盆子状空心聚合物微球的制备示意图^[41]

Fig. 6. Schematics of the preparation of raspberry-like hollow polymeric microspheres loaded with BTA^[41].

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图 7 石墨烯基纳米容器的制备工艺^[42]

Fig. 7. Preparation process of graphene-based nanocontainer^[42].

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图 8 8-PG-BTA/EP涂层的防腐蚀机理^[42]　(a) 完整涂层; (b) 缺陷; (c) 腐蚀反应; (d) 自愈行为

Fig. 8. Corrosion protection mechanism of 8-PG-BTA/EP coating^[42]: (a) Intact coating; (b) defect; (c) corrosion reaction; (d) self-healing behavior.

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图 9 石墨烯薄膜的缺陷促进金属腐蚀^[14]

Fig. 9. Defects of graphene films promote the corrosion of metals^[14].

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图 10 在单层石墨烯(SLG)和多层石墨烯(FLG)中进行分子扩散的原子尺度模拟示意图^[52]　(a) 水分子在有缺陷的SLG中扩散需要的能量和示意图; (b) 氧气和水分子等物质易在SLG中扩散并使Cu表面氧化的情况示意图; (c) 水分子在有缺陷的双层石墨烯(BLG)中扩散需要的能量和示意图; (d) 示意图显示即使三层石墨烯包含多个晶界(GB)缺陷, 氧气和水分子也难以穿过多晶三层石墨烯并与下面的Cu表面接触

Fig. 10. Atomic-scale simulations of molecular diffusion through SLG and FLG^[52]: (a) Schematics and the calculated energy barrier for a water molecule to diffuse through a defective SLG; (b) schematic showing the easiness of reactive species such as oxygen and water molecules to diffuse through SLG and oxidize the Cu surface; (c) schematics and the calculated energy barrier for a water molecule to diffuse through a defective BLG; (d) schematic showing the difficulties for oxygen and water molecules to diffuse through polycrystalline trilayer graphene and contact with the underlying Cu surface, even when the trilayer graphene contains multiple GB defects.

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图 11 (a)−(c) 在含有0.1 mol/L KCl溶液的5 mmol/L K₃[Fe(CN)₆]溶液中通过循环伏安法修饰玻碳电极(GCE)上的GO样品(S-1至S-6); (d) 具有不同氧化水平的样品的I_pc^[56]

Fig. 11. (a)−(c) Cyclic voltammetry of GO samples (S-1 to S-6) modified on GCE in 5 mmol/L K₃[Fe(CN)₆] containing 0.1 mol/L KCl solution; (d) I_pcof the samples with different oxidation levels^[56].

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图 12 PU/GnP复合材料的横截面SEM图像(质量分数为1%的GnP, 其中(a)−(d)为低倍率; (e)−(f)为高倍率)　(a), (e) PU/H100; (b), (f) PU/M25; (c), (g) PU/M5; (d), (h) PU/C750^[59]

Fig. 12. Cross-sectional SEM images for the PU/GnP composites (GnP with weight fraction of 1%, (a)−(d) low magnification, (e)−(f) high magnification): (a), (e) PU/H100; (b), (f) PU/M25; (c), (g) PU/M5; (d), (h) PU/C750^[59].

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图 13 腐蚀介质在含有质量分数为1% GnP的PU复合材料层中的渗透示意图^[59]

Fig. 13. Schematic model for the permeation of the corrosive agent passing through the coating layer of the PU composite containing GnP with weight fraction of 1%^[59].

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