含磷石墨烯的制备及复合涂层的耐蚀性能

doi:10.11901/1005.3093.2021.556

材料研究学报

2022, Vol. 36

Issue (12): 933-944 DOI: 10.11901/1005.3093.2021.556

研究论文

本期目录 | 过刊浏览

含磷石墨烯的制备及复合涂层的耐蚀性能

李玉峰¹^,²(

), 张念飞¹, 刘丽爽¹, 赵甜甜¹, 高文博¹, 高晓辉¹

^1.齐齐哈尔大学化学与化学工程学院齐齐哈尔 161006
^2.齐齐哈尔大学轻工与纺织学院齐齐哈尔 161006

Preparation of Phosphorus-containing Graphene and Corrosion Resistance of Composite Coating

LI Yufeng¹^,²(

), ZHANG Nianfei¹, LIU Lishuang¹, ZHAO Tiantian¹, GAO Wenbo¹, GAO Xiaohui¹

^1.College of Chemistry and Chemical Engineering, Qiqihar University, Qiqihar 161006, China
^2.College of Light Industry and Textile, Qiqihar University, Qiqihar 161006, China

引用本文:

李玉峰, 张念飞, 刘丽爽, 赵甜甜, 高文博, 高晓辉. 含磷石墨烯的制备及复合涂层的耐蚀性能[J]. 材料研究学报, 2022, 36(12): 933-944.
Yufeng LI, Nianfei ZHANG, Lishuang LIU, Tiantian ZHAO, Wenbo GAO, Xiaohui GAO. Preparation of Phosphorus-containing Graphene and Corrosion Resistance of Composite Coating[J]. Chinese Journal of Materials Research, 2022, 36(12): 933-944.

全文: PDF(31236 KB) HTML

摘要:

以植酸(PhA)为原料，采用热解法制备含磷石墨烯(PhA-G)，并以硅树脂(SiR)为成膜物制备含磷石墨烯/硅树脂(PhA-G/SiR)复合防腐蚀涂层。通过拉曼光谱和XPS分析含磷石墨烯的结构，通过SEM、TEM和AFM观察含磷石墨烯的形貌，通过接触角、吸水率、电化学阻抗谱、极化曲线和盐雾实验等研究复合涂层的耐蚀性能。结果表明：相比于纯SiR涂层和氧化石墨烯/硅树脂(GO/SiR)复合涂层，PhA-G/SiR复合涂层对金属的保护作用更好；当含磷石墨烯添加量为3%(质量分数)时，PhA-G/SiR复合涂层表现出较好的疏水性和优异的防腐蚀性能，其接触角为103.5°，吸水率为3.72%；腐蚀电流密度为3.53×10^-10 A/cm²，电化学阻抗值达到3.82×10⁷ Ω·cm²，耐盐雾达到960 h。

关键词 ：材料失效与保护, 耐蚀性能, 含磷石墨烯, 硅树脂, 复合涂层

Abstract：

The phosphorus-containing graphene (PhA-G) was prepared by pyrolysis method with phytic acid (PhA) as raw material, and next the PhA-G/SiR composite anticorrosion coating was prepared with silicone resin (SiR) as film forming material. The structure and morphology of phosphorus-containing graphene was characterized by means of Raman spectroscope, X-ray photoelectron spectroscope (XPS), scanning electron microscope (SEM), transmission electron microscope (TEM) and atomic force microscope (AFM). The prepared coatings with the different additive amount of PhA-G (1%~4% in mass fraction), were comparatively examined by means of measurements of contact angle, water absorption, potentiodynamic polarization curves, electrochemical impedance spectroscopy (EIS), as well as salt spray test. The results show that the protectiveness of PhA-G/SiR composite coatings for metal substrate is greater than that of the plain SiR coating, and graphene oxide/silicone resin (GO/SiR) coating. The PhA-G/SiR composite coating exhibits good hydrophobicity and excellent corrosion resistance when the mass fraction of PhA-G is 3%. Correspondingly, which exhibits hydrophobic contact angle of 103.5° and water absorption rate of 3.72%, while corrosion current density of 3.53×10^-10 A/cm²and electrochemical impedance as high as 3.82×10⁷ Ω·cm² in 3.5%(mass fraction) NaCl solution. Furthermore, the PhA-G/SiR composite coating presents excellent resistance to salt spray testing, up to above 960 h.

Key words： materials failure and protection corrosion resistance phosphorus-containing graphene silicone resin composite coating

收稿日期: 2021-09-26

ZTFLH:

TB304

基金资助:黑龙江省省属高等学校基本科研业务费科研项目(135509128)

作者简介: 李玉峰，男，1970年生，教授

	服务

	把本文推荐给朋友
	加入引用管理器
	E-mail Alert
	RSS
	作者相关文章
	李玉峰
	张念飞
	刘丽爽
	赵甜甜
	高文博
	高晓辉
44.8K

链接本文:

https://www.cjmr.org/CN/10.11901/1005.3093.2021.556 或 https://www.cjmr.org/CN/Y2022/V36/I12/933

图1 GO和PhA-G的拉曼光谱图

图2 GO和PhA-G的XPS谱图

图3 GO和PhA-G的SEM图

图4 GO和PhA-G的TEM图像

图5 PhA-G样品的AFM图像及厚度分析

图6 不同PhA-G含量的PhA-G/SiR复合涂层的表面形貌照片

图7 PhA-G含量对复合涂层接触角和吸水率的影响

图8 SiR涂层、GO/SiR涂层和4种PhA-G/SiR复合涂层在3.5% NaCl溶液中浸泡不同时间的Nyquist和Bode图

图9 裸钢、SiR涂层、GO/SiR涂层和4种PhA-G/SiR复合涂层的极化曲线

表1 极化曲线拟合数据

图10 不同涂层经不同时间的盐雾实验后以及去掉涂层后钢片表面的宏观形貌照片

图11 盐雾实验960 h后去掉涂层后钢基体表面的显微形貌照片

图12 PhA-G/SiR复合涂层防腐蚀机理示意图

1	BERRY V. Impermeability of graphene and its applications [J]. Carbon, 2013, 62: 1 doi: 10.1016/j.carbon.2013.05.052
2	Qi K, Sun Y M, Duan H W, et al. A corrosion-protective coating based on a solution-processable polymer-grafted graphene oxide nanocomposite [J]. Corros. Sci., 2015, 98: 500 doi: 10.1016/j.corsci.2015.05.056
3	Wang N, Chen J S, Wang S W, et al. Application of aminated grap-hite oxide for waterborne anti-corrosion and fireproof coatings [J]. Chin. J. Mater. Res., 2018, 32(10): 721
3	王娜, 陈俊声, 王树伟等. 氨基化氧化石墨烯在水性防腐防火一体化涂料中的应用 [J]. 材料研究学报, 2018, 32(10): 721
4	Palaniappan N, Cole I, Kuznetsov A E. Experimental and computational studies of graphene oxide covalently functionalized by octylamine: electrochemical stability, hydrogen evolution, and corrosion inhibition of the AZ13 Mg alloy in 3.5%NaCl [J]. RSC Adv., 2020, 10(19): 11426 doi: 10.1039/c9ra10702a pmid: 35495345
5	Wen S, Ma J. Synergistic effect of polyvinylpyrrolidone noncovalently modified graphene and epoxy resin in anticorrosion application [J]. High. Perform. Polym., 2020, 33(2): 146 doi: 10.1177/0954008320942293
6	Ning L, Wang D D, Wang L, et al. Interesting corrosion inhibition performance and mechanism of two silanes containing multiple phosphate group [J]. Silicon-Neth., 2019, 12(6): 1455
7	Hermas A A, Wahdan M H, Ahmed E M. Phosphate-doped polyaniline/Al₂O₃ nanocomposite coating for protection of stainless steel [J]. Anti-Corros. Method. M, 2020, 64(5): 491
8	Zhu K, Li J Y, Fei G Q. Anticorrosive performance of phosphorylated graphene oxide applied at waterborne epoxy coating [J]. China Adhes., 2018, 27(9): 501
8	朱科, 李菁熠, 费贵强. 磷酸化氧化石墨烯对水性环氧涂料防腐增强作用研究 [J]. 中国胶粘剂, 2018, 27(9): 501
9	Huang H, Tian Y, Xie Y, et al. Modification of graphene oxide with acrylate phosphorus monomer via thiol-Michael addition click reaction to enhance the anti-corrosive performance of waterborne epoxy coating [J]. Prog. Org. Coat., 2020, 146: 105724
10	Ding J, Rahman O U, Peng W, et al. A novel hydroxyl epoxy phosp hate monomer enhancing the anticorrosive performance of waterborne Graphene/Epoxy coatings [J]. Appl. Surf. Sci., 2018, 427: 981 doi: 10.1016/j.apsusc.2017.08.224
11	Albero J, Vidal A, Migani A, et al. Phosphorus-doped graphene as a metal-free material for thermochemical water reforming at unusually mild conditions [J]. Acs. Sustain. Chem. Eng., 2019, 7(1): 838 doi: 10.1021/acssuschemeng.8b04462
12	Suleiman R, Estaitie M, Mizanurahman M. Hybrid organosiloxane coatings containing epoxide precursors for protecting mild steel against corrosion in a saline medium [J]. J. Appl. Polym. Sci., 2016, 133(38): 1
13	Zhang L, Shi Z, Hu W H, et al. Curing mechanism, heat resistance, and anticorrosion properties of a furan/methyl phenyl silicone coating [J]. Polym. Advan. Technol., 2018, 29(7): 1913 doi: 10.1002/pat.4300
14	Wu J X, Xu H, Zhang J. Raman spectroscopy of graphene [J]. Atca. Chim. Sin. 2014, 72(3): 301
14	吴娟霞, 徐华, 张锦. 拉曼光谱在石墨烯结构表征中的应用 [J]. 化学学报, 2014, 72(3): 301 doi: 10.6023/A13090936
15	Wang C, Jia Y J, Liu Z C, et al. Preparation and characterization of phosphorus-doped graphene [J]. Ind. Catal., 2014, 22(7): 510
15	王灿, 贾银娟, 刘志成等. 磷掺杂石墨烯的制备与表征 [J]. 工业催化, 2014, 22(7): 510
16	Yuan B H, Xing W Y, Hu Y X, et al. Boron/phosphorus doping for retarding the oxidation of reduced graphene oxide [J]. Carbon., 2016, 101: 152 doi: 10.1016/j.carbon.2016.01.080
17	Shen X Y, Li X D, Zhao F H, et al. Preparation and structure study of phosphorus-doped porous graphdiyne and its efficient lithium storage application [J]. 2D Mater., 2019, 6(3): 035020
18	Balaji S S, Ganesh P A, Moorthy M, et al. Efficient electrocatalytic activity for oxygen reduction reaction by phosphorus-doped graphene using supercritical fluid processing [J]. B. Mater. Sci., 2020, 43: 151 doi: 10.1007/s12034-020-02142-2
19	Yu Y, Zhang Q, Wu L, et al. Reaction mechanism of N-(4-hydroxyphenyl)ethanamide electrodegradation via phosphorus-graphene prepared from triphenylphosphine: Generation and destruction of the reactive species [J]. Chem. Eng. J., 2021, 403: 126322 doi: 10.1016/j.cej.2020.126322
20	Kong S, Hu W J, Li J S. Tribological properties of graphene in PAO base oil [J]. China Surf. Eng., 2019, 32(3): 162
20	孔尚, 胡文敬, 李久盛. 石墨烯在PAO基础油中的摩擦学性能 [J]. 中国表面工程, 2019, 32(3): 162
21	Li Y, Xu Y, Wang S, et al. Preparation of graphene/polyaniline nanocomposite by in situ intercalation polymerization and their application in anti-corrosion coatings [J]. High Perform. Polym., 2019, 31(9-10): 1226 doi: 10.1177/0954008319839442
22	Pourhashem S, Vaezi M R, Rashidi A, et al. Distinctive roles of silane coupling agents on the corrosion inhibition performance of graphene oxide in epoxy coatings [J]. Prog. Org. Coat., 2017, 111: 47
23	Li Y F, Li J Y, Gao X H, et al. Synthesis of stabilized dispersion covalently-jointed SiO₂@polyaniline with core-shell structure and anticorrosion performance of its hydrophobic coating for Mg-Li alloy [J]. Appl. Surf. Sci., 2018, 462(1): 362 doi: 10.1016/j.apsusc.2018.08.118

[1]	高巍, 刘江南, 魏敬鹏, 要玉宏, 杨巍. TC4钛合金表面氧化亚铜掺杂微弧氧化层的结构和性能[J]. 材料研究学报, 2022, 36(6): 409-415.
[2]	杨留洋, 谭卓伟, 李同跃, 张大磊, 邢少华, 鞠虹. 利用WBE及EIS测试技术对管道缺陷区动态冲刷腐蚀行为的研究[J]. 材料研究学报, 2022, 36(5): 381-391.
[3]	陈铮, 杨芳, 王成, 杜瑶, 卢壹梁, 朱圣龙, 王福会. 惰性无机填料比例和颗粒尺寸对纳米Al/Al₂O₃ 改性有机硅涂料抗高温氧化行为的影响[J]. 材料研究学报, 2022, 36(4): 271-277.
[4]	李蕊, 王浩, 张天刚, 牛伟. Ti811合金表面激光熔覆Ti₂Ni+TiC+Al₂O₃+Cr_xS_y复合涂层的组织和性能[J]. 材料研究学报, 2022, 36(1): 62-72.
[5]	陈艺文, 王成, 娄霞, 李定骏, 周科, 陈明辉, 王群昌, 朱圣龙, 王福会. 无机复合涂层对CB2铁素体耐热钢在650℃水蒸气中的防护[J]. 材料研究学报, 2021, 35(9): 675-681.
[6]	唐荣茂, 刘光明, 刘永强, 师超, 张帮彦, 田继红, 甘鸿禹. 用电化学噪声技术研究Q235钢在含氯盐模拟混凝土孔隙液中的腐蚀行为[J]. 材料研究学报, 2021, 35(7): 526-534.
[7]	郝欣欣, 席通, 张宏镇, 杨春光, 杨柯. 淬火温度对含铜5Cr15MoV马氏体不锈钢性能的影响[J]. 材料研究学报, 2021, 35(12): 933-941.
[8]	张大磊, 魏恩泽, 荆赫, 杨留洋, 豆肖辉, 李同跃. 超级铁素体不锈钢表面超疏水结构的制备及其耐腐蚀性能[J]. 材料研究学报, 2021, 35(1): 7-16.
[9]	王冠一, 车欣, 张浩宇, 陈立佳. Al-5.4Zn-2.6Mg-1.4Cu合金板材的低周疲劳行为[J]. 材料研究学报, 2020, 34(9): 697-704.
[10]	黄安然, 张伟, 王学林, 尚成嘉, 范佳杰. 铁素体不锈钢在高温尿素环境中的腐蚀行为研究[J]. 材料研究学报, 2020, 34(9): 712-720.
[11]	公维炜, 杨丙坤, 陈云, 郝文魁, 王晓芳, 陈浩. 扫描电化学显微镜原位观察碳钢涂层缺陷处的交流腐蚀行为[J]. 材料研究学报, 2020, 34(7): 545-553.
[12]	郭铁明, 徐秀杰, 张延文, 宋志涛, 董志林, 金玉花. Q345q桥梁钢和Q345qNH耐候钢在模拟工业大气+除冰盐混合介质中的腐蚀行为[J]. 材料研究学报, 2020, 34(6): 434-442.
[13]	朱金阳, 谭成通, 暴飞虎, 许立宁. 一种新型含Al低Cr合金钢在模拟油田采出液环境下的CO₂腐蚀行为[J]. 材料研究学报, 2020, 34(6): 443-451.
[14]	梁新磊, 刘茜, 王刚, 王震宇, 韩恩厚, 王帅, 易祖耀, 李娜. 氧化石墨烯改性环氧隔热涂层的耐蚀和隔热性能研究[J]. 材料研究学报, 2020, 34(5): 345-352.
[15]	王志虎,张菊梅,白力静,张国君. 水热处理对AZ31镁合金微弧氧化陶瓷层组织结构及耐蚀性的影响[J]. 材料研究学报, 2020, 34(3): 183-190.

Viewed

Full text

Abstract

Cited

Shared

Discussed