Experimental and molecular simulation of corrosion of steel in [BMIM]HSO4 ionic liquid

doi:10.11949/j.issn.0438-1157.20170232

Abstract

Abstract:

The corrosion behaviors of steel in[BMIM]HSO₄ ionic liquid (IL) were investigated by immersion tests and molecular simulation. The corrosion rates of stainless steel 304 in IL were determined by mass loss measurement. The result indicates that the presence of H₂O greatly enhances the corrosivity of IL. The distribution of HOMO and LUMO, Fukui indices and quantum chemical parameters on IL molecule were calculated. The results show that the imidazolium ring and hydrogen sulfate play the most important role in the interaction between IL and metal surface. The quantum chemical parameters of IL in aqueous solution significantly change. The chemical adsorption ability of IL becomes weak. The adsorption process and adsorption energy of IL on steel surface in water-free and aqueous environments were investigated by molecular dynamics simulation. The molecular simulation results are consistent well with corrosion results, which can provide a better understanding of the interaction between ionic liquid and metal surface at the molecular level.

Key words: ionic liquids, corrosion, mass loss measurement, molecular simulation, quantum chemical calculation, molecular dynamic simulation

摘要：

基于失重法和分子模拟方法，研究了1-丁基-3-甲基咪唑硫酸氢盐（[BMIM]HSO₄）的腐蚀性和离子液体分子与金属表面的相互作用。实验结果表明[BMIM]HSO₄对304不锈钢具有腐蚀性，且在水溶液中腐蚀性显著增强。基于量子化学方法计算了[BMIM]HSO₄分子的HOMO和LUMO分布、Fukui指数及分子内部特征参数，计算结果表明[BMIM]HSO₄在Fe金属表面吸附的位置主要集中在阴离子硫酸氢根和阳离子咪唑环上，可分别形成配位键和反馈键，在水溶液中[BMIM]HSO₄分子与金属表面的相互作用变弱。分子动力学模拟揭示了在不同的环境中[BMIM]HSO₄分子在Fe金属表面的吸附过程和吸附能。量子化学计算和分子动力学模拟结果一致，从理论上解释了在水溶液中[BMIM]HSO₄腐蚀性增强的原因。

关键词: 离子液体, 腐蚀, 失重法, 分子模拟, 量子化学计算, 分子动力学模拟

CLC Number:

TG174

ZHANG Jinwei, CHENG Hongye, CHEN Lifang, QI Zhiwen. Experimental and molecular simulation of corrosion of steel in [BMIM]HSO₄ ionic liquid[J]. CIESC Journal, 2018, 69(2): 808-814.

张晋玮, 成洪业, 陈立芳, 漆志文. [BMIM]HSO₄离子液体腐蚀性的实验与分子模拟[J]. 化工学报, 2018, 69(2): 808-814.

References

[1] WISHART J F. Energy applications of ionic liquids[J]. Energy & Environmental Science, 2009, 2(9):956-961.
[2] MEINDERSMA G W, PODT A J, DE HAAN A B. Selection of ionic liquids for the extraction of aromatic hydrocarbons from aromatic/aliphatic mixtures[J]. Fuel Processing Technology, 2005, 87(1):59-70.
[3] KULKARNI P S, AFONSO C A. Deep desulfurization of diesel fuel using ionic liquids:current status and future challenges[J]. Green Chemistry, 2010, 12(7):1139-1149.
[4] ZHAO D S, WANG J L, ZHOU E P. Oxidative desulfurization of diesel fuel using a Brønsted acid room temperature ionic liquid in the presence of H₂O₂[J]. Green Chemistry, 2007, 9(11):1219-1222.
[5] ZHANG W, XU K, ZHANG Q, et al. Oxidative desulfurization of dibenzothiophene catalyzed by ionic liquid[BMIm]HSO₄[J]. Industrial & Engineering Chemistry Research, 2010, 49(22):11760-11763.
[6] SONG Z, ZHOU T, ZHANG J N, et al. Screening of ionic liquids for solvent-sensitive extraction-with deep desulfurization as an example[J]. Chemical Engineering Science, 2015, 129:69-77.
[7] SONG Z, ZHANG J J, ZENG Q, et al. Effect of cation alkyl chain length on liquid-liquid equilibria of {ionic liquids+thiophene+ heptane}:COSMO-RS prediction and experimental verification[J]. Fluid Phase Equilibria, 2016, 425:244-251.
[8] GREAVES T L, DRUMMOND C J. Protic ionic liquids:properties and applications[J]. Chemical Reviews, 2008, 108(1):206-237.
[9] UERDINGEN M, TREBER C, BALSER M, et al. Corrosion behaviour of ionic liquids[J]. Green Chem., 2005, 7(5):321-325.
[10] MASHUGA M, OLASUNKANMI L, ADEKUNLE A, et al. Adsorption, thermodynamic and quantum chemical studies of 1-hexyl-3-methylimidazolium based ionic liquids as corrosion inhibitors for mild steel in HCl[J]. Materials, 2015, 8(6):3607-36032.
[11] SHERIF E S, ABDO H, ABEDIN S. Corrosion inhibition of cast iron in arabian gulf seawater by two different ionic liquids[J]. Materials, 2015, 8(7):3883-3895.
[12] QIANG Y J, GUO L, ZHANG S T, et al. Synergistic effect of tartaric acid with 2, 6-diaminopyridine on the corrosion inhibition of mild steel in 0. 5 mol·L-1 HCl[J]. Scientific Reports, 2016, 6:33305.
[13] TANAK H, KÖ YSAL Y, ÜNVER Y, et al. Experimental and DFT studies of ethyl N'-3-(1H-imidazol-1-yl) propylcarbamoyl benzohydrazonate monohydrate[J]. Structural Chemistry, 2009, 20(3):409-416.
[14] ULLAH S, BUSTAM M A, SHARIFF A M, et al. Experimental and quantum study of corrosion of A36 mild steel towards 1-butyl-3-methylimidazolium tetrachloroferrate ionic liquid[J]. Applied Surface Science, 2016, 365:76-83.
[15] CAO J S, REN Q, CHEN F W, et al. Comparative study on the methods for predicting the reactive site of nucleophilic reaction[J]. Science China Chemistry, 2015, 58(12):1-8.
[16] 胡松青, 胡建春, 高元军, 等. 月桂基咪唑啉对Q235钢的缓蚀吸附作用[J]. 化工学报, 2011, 62(1):147-155. HU S Q, HU J C, GAO Y J, et al. Corrosion inhibition and adsorption of lauryl-imidazolines for Q235 steel[J]. CIESC Journal, 2011, 62(1):147-155.
[17] 钱建华, 潘晓娜, 张强, 等. 2, 5-二芳基-1, 3, 4-噻二唑衍生物的合成及缓蚀性能[J]. 化工学报, 2015, 66(7):2737-2748. QIAN J H, PAN X N, ZHANG Q, et al. Synthesis of 2, 5-diaryl-1, 3, 4-thiadiazole corrosion inhibitors and their performance[J]. CIESC Journal, 2015, 66(7):2737-2748.
[18] FAN C H, HUANG X M, HAN L H, et al. Novel colorimetric and fluorescent off-on enantiomers with high selectivity for Fe³⁺ imaging in living cells[J]. Sensors & Actuators B Chemical, 2015, 224:592-599.
[19] FAUVET P, BALBAUD F, ROBIN R. Corrosion mechanisms of austenitic stainless steels in nitric media used in reprocessing plants[J]. Journal of Nuclear Materials, 2008, 375(1):52-64.
[20] SCHUTT T C, HEGDE G A, BHARADWAJ V S, et al. Impact of water-dilution on the biomass solvation properties of the ionic liquid 1-methyltriethoxy-3-ethylimidazolium acetate[J]. The Journal of Physical Chemistry B, 2017, 121(4):843-853.
[21] KANNAN P, KARTHIKEYAN J, MURUGAN P, et al. Corrosion inhibition effect of novel methyl benzimidazolium ionic liquid for carbon steel in HCl medium[J]. Journal of Molecular Liquids, 2016, 221:368-380.
[22] OLASUNKANMI L, OBOT I B, KABANDA M M, et al. Some quinoxalin-6-yl derivatives as corrosion inhibitors for mild steel in hydrochloric acid:experimental and theoretical studies[J]. Journal of Physical Chemistry C, 2015, 119(28):16004-16019.
[23] ZHENG X W, ZHANG S T, LI W P, et al. Experimental and theoretical studies of two imidazolium-based ionic liquids as inhibitors for mild steel in sulfuric acid solution[J]. Corrosion Science, 2015, 95:168-179.
[24] ASEGBELOYIN J, EJIKEME P, OLASUNKANMI L, et al. A novel schiff base of 3-acetyl-4-hydroxy-6-methyl-(2H)pyran-2-one and 2, 2'-(ethylenedioxy)diethylamine as potential corrosion inhibitor for mild steel in acidic medium[J]. Materials, 2015, 8(6):2918-2934.
[25] ONA O B, DE CLERCQ O, ALCOBA D R, et al. Atom and bond Fukui functions and matrices:a Hirshfeld-I atoms-in-molecule approach[J]. Chemphyschem A European Journal of Chemical Physics & Physical Chemistry, 2016, 17(18):2881-2889.
[26] UDHAYAKALA P, JAYANTHI A, RAJENDIRAN T V, et al. Quantum chemical studies on some thiadiazolines as corrosion inhibitors for mild steel in acidic medium[J]. Research on Chemical Intermediates, 2012, 39(39):895-906.
[27] SULAIMAN K O, ONAWOLE A T. Quantum chemical evaluation of the corrosion inhibition of novel aromatic hydrazide derivatives on mild steel in hydrochloric acid[J]. Computational & Theoretical Chemistry, 2016, 1093:73-80.
[28] YILMAZ N, FITOZ A, ERGUN Ü, et al. A combined electrochemical and theoretical study into the effect of 2-((thiazole-2-ylimino)methyl)phenol as a corrosion inhibitor for mild steel in a highly acidic environment[J]. Corrosion Science, 2016, 111:110-120.
[29] DENG S D, LI X H, XIE X G. Hydroxymethyl urea and 1, 3-bis(hydroxymethyl) urea as corrosion inhibitors for steel in HCl solution[J]. Corrosion Science, 2014, 80(3):276-289.
[30] LIU X Q, XUE Y, TIAN Z Y, et al. Adsorption of CH₄ on nitrogen-and boron-containing carbon models of coal predicted by density-functional theory[J]. Applied Surface Science, 2013, 285(19):190-197.
[31] 王小露, 万辉, 管国锋.[EPy]Cl和[EPy]Br离子对的气相和液相结构及阴阳离子间的相互作用[J]. 物理化学学报, 2008, 24(11):2077-2082. WANG X L, WAN H, GUAN G F. Structure and interaction of ion-pairs of[EPy]Cl and[EPy]Br in gas and liquid phases[J]. Acta Phys. -Chim. Sin., 2008, 24(11):2077-2082.

Experimental and molecular simulation of corrosion of steel in [BMIM]HSO₄ ionic liquid

[BMIM]HSO₄离子液体腐蚀性的实验与分子模拟

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