Influence of chloride and sulfate on steel corrosion in simulated concrete pore solutions
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摘要: 通过电化学测试、XRD测试和DFT计算，本研究探讨了在不同pH值(12.4、12.9和13.5)的模拟混凝土孔隙溶液中Cl−和\text{SO}_{\text{4}}^{{2-}}单独及共同作用对钢筋锈蚀行为的影响及其机制。结果表明，在pH值较低的CH溶液中，当Cl−浓度仅达到0.02mol/L时，开路电位(OCP)即由−375mV急剧下降至−575 mV，表明Cl−在低浓度情况下就会显著加速腐蚀；而在pH值较高的ST溶液中，随着腐蚀离子浓度从0.01 mol/L逐步增加至0.4 mol/L，钢筋的极化电阻(Rp)从约100 kΩ·cm2稳定下降至5 kΩ·cm2，但整体耐腐蚀性明显优于其他pH值的情况，显示了高pH值对腐蚀的有效抑制作用。此外，当Cl−和$\text{SO}_{\text{4}}^{{2-}} $共存时，由于竞争吸附机制的作用，整体腐蚀速率介于两者单独存在时之间，$\text{SO}_{\text{4}}^{{2-}} $的存在一定程度上减缓了Cl−引发的腐蚀。本研究基于上述结果提出了一个竞争吸附-催化腐蚀的两阶段反应模型，详细揭示了二者共同作用下的腐蚀行为，Cl−通过破坏钝化膜加速腐蚀进程，$\text{SO}_{\text{4}}^{{2-}} $则通过影响腐蚀产物的稳定性和分布参与腐蚀过程。Abstract: Through electrochemical tests, XRD analysis, and DFT calculations, this study investigated the individual and combined effects of Cl− and $\text{SO}_{\text{4}}^{{2-}} $ ions on the corrosion behavior of steel reinforcement in simulated concrete pore solutions at different pH values (12.4, 12.9 and 13.5). The results reveal that in the lower pH CH solution, even at a Cl− concentration of only 0.02 mol/L, the open circuit potential (OCP) drops sharply from −375 mV to −575 mV, indicating significant acceleration of corrosion by Cl− at low concentrations. Conversely, in the higher pH ST solution, as the concentration of corrosion ions increases gradually from 0.01 mol/L to 0.4 mol/L, the steel’s polarization resistance (Rp) stabilizes and decreases from approximately 100 kΩ·cm2 to 5 kΩ·cm2, demonstrating superior overall corrosion resistance compared to lower pH conditions, highlighting the effective inhibition of corrosion at higher pH value. Furthermore, in the presence of both Cl− and $\text{SO}_{\text{4}}^{{2-}} $ ions, the overall corrosion rate lies between the rates observed when each ion is present individually, due to the competitive adsorption mechanism. The presence of $\text{SO}_{\text{4}}^{{2-}} $ mitigates to some extent the corrosion initiated by Cl−. Based on these findings, the study proposes a two-stage competitive adsorption-catalytic corrosion reaction model, elucidating in detail the corrosion behavior under their combined influence: Cl− accelerates corrosion by disrupting the passive film, while $\text{SO}_{\text{4}}^{{2-}} $ participates in the corrosion process by influencing the stability and distribution of corrosion products.
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图 1 不同模拟液中腐蚀阶段钢试样的腐蚀电位($ {E}_{\mathrm{c}\mathrm{o}\mathrm{r}\mathrm{r}} $)曲线：(a)第一种模拟液(CH)中；(b)第二种模拟液(LC)中；(c)第三种模拟液(ST)中
Figure 1. Corrosion potential ($ {E}_{\mathrm{c}\mathrm{o}\mathrm{r}\mathrm{r}} $) curves of steel specimens in corrosion stage of SCPSs: (a) in the first simulated solution (CH); (b) in the second simulated solution (LC); (c) in the third simulated solution (ST)
图 2 不同模拟液中腐蚀阶段钢试样的极化电阻($ {R}_{\mathrm{p}} $)曲线：(a)第一种模拟液(CH)中；(b)第二种模拟液(LC)中；(c)第三种模拟液(ST)中
Figure 2. Polarization resistance ($ {R}_{\mathrm{p}} $) curves of steel specimens in corrosion stage of SCPSs: (a) in the first simulated solution (CH); (b) in the second simulated solution (LC); (c) in the third simulated solution (ST)
图 3 不同模拟液中腐蚀阶段钢试样的腐蚀电流密度($ {I}_{\mathrm{c}\mathrm{o}\mathrm{r}\mathrm{r}} $)曲线：(a)第一种模拟液(CH)中；(b)第二种模拟液(LC)中；(c)第三种模拟液(ST)中
Figure 3. Corrosion current density ($ {I}_{\mathrm{c}\mathrm{o}\mathrm{r}\mathrm{r}} $) curves of steel specimens in corrosion stage of SCPSs: (a) in the first simulated solution (CH); (b) in the second simulated solution (LC); (c) in the third simulated solution (ST)
图 4 第一种模拟液(CH)中不同腐蚀离子对普通低碳钢试样腐蚀过程的电化学阻抗谱(EIS)结果及等效电路拟合结果：(a) Nyquist图；(b) Bode和Phase图
Figure 4. Electrochemical impedance spectroscopy (EIS) results and equivalent electrical circuit fitting results for the corrosion process of low-carbon steel specimens by different corrosive ions in the first simulated solution (CH): (a) Nyquist diagram; (b) Bode and Phase diagram
图 5 第二种模拟液(LC)中不同腐蚀离子对普通低碳钢试样腐蚀过程的电化学阻抗谱(EIS)结果及等效电路拟合结果：(a)Nyquist图；(b)Bode和Phase图
Figure 5. Electrochemical impedance spectroscopy (EIS) results and equivalent electrical circuit fitting results for the corrosion process of low-carbon steel specimens by different corrosive ions in the second simulated solution (LC): (a) Nyquist diagram; (b) Bode and Phase diagram
图 6 第三种模拟液(ST)中不同腐蚀离子对普通低碳钢试样腐蚀过程的电化学阻抗谱(EIS)结果及等效电路拟合结果：(a)Nyquist图；(b)Bode和Phase图
Figure 6. Electrochemical impedance spectroscopy (EIS) results and fitting results for the corrosion process of low-carbon steel specimens by different corrosive ions in the third simulated solution (ST): (a) Nyquist diagram; (b) Bode and Phase diagram
图 8 腐蚀离子作用下钢筋腐蚀产物的XRD图谱
Figure 8. XRD patterns of corrosion products of steel reinforcement under the action of corrosive ions
图 9 Cl−和$\text{SO}_{\text{4}}^{{2-}} $在Fe(100)表面不同吸附位点的示意图
Figure 9. Schematic diagram of different adsorption sites of Cl− and $\text{SO}_{\text{4}}^{{2-}} $ on Fe(100) surface
图 10 Cl−和$\text{SO}_{\text{4}}^{{2-}} $的竞争吸附及腐蚀过程的示意图
Figure 10. Schematic diagram of competitive adsorption of Cl− and $\text{SO}_{\text{4}}^{{2-}} $ and corrosion process: (a) Initial state; (b) Competitive adsorption;(c) Catalytic corrosion
表 1 不同模拟液中腐蚀电化学阻抗谱(EIS)数据的等效电路拟合结果
Table 1. Equivalent electrical circuit fitting results of electrochemical impedance spectroscopy (EIS) data in different simulated solutions
Content/
(mol·L−1)$ {R}_{\mathrm{S}} $/
(Ω·cm2)CPE1, Q/
(S·sn·cm−2)CPE1,$ a $
[0<$ a $<1]$ {R}_{1} $ /(Ω·cm2) CPE2, Q/
(S·sn·cm−2)CPE2,$ a $
[0<$ a $<1]$ {R}_{\mathrm{c}\mathrm{t}} $/
(Ω·cm2)Chi-squared CH-Cl− 0.01 65.42 0.0000917 0.8863 4164 0.0000714 0.4761 41280 5.62×10−4 0.02 40.35 0.0001129 0.8703 2597 0.0002508 0.4036 6510 1.85×10−3 0.03 42.19 0.0001079 0.8758 2195 0.0002016 0.3551 9236 7.96×10−4 0.05 33.03 0.0001247 0.8633 802.3 0.0004566 0.2367 19660 7.51×10−4 0.07 28 0.0001379 0.8521 752.2 0.0010090 0.3267 13790 6.27×10−4 0.1 23.6 0.0001617 0.83 298.7 0.0015650 0.3055 1665 6.81×10−4 CH-$\text{SO}_{\text{4}}^{{2-}} $ 0.01 41.22 0.0001062 0.8848 4059 0.0000951 0.6181 16650 1.05×10−3 0.02 35.17 0.0001150 0.8848 1883 0.0002298 0.5316 6555 6.93×10−4 0.03 30.32 0.0001140 0.8887 1317 0.0002200 0.5174 5769 2.09×10−3 0.05 24.24 0.0001285 0.8705 1027 0.0003002 0.5019 6891 8.19×10−4 0.07 18.98 0.0001310 0.8709 605.9 0.0004202 0.4764 7953 3.39×10−3 0.1 16.46 0.0001365 0.8598 335.3 0.0005371 0.4666 8298 6.53×10−3 CH
Cl−+$\text{SO}_{\text{4}}^{{2-}} $0.01 26.53 0.0001563 0.8879 4824 0.0000884 0.8907 26730 1.29×10−3 0.02 20.73 0.0001161 0.8732 1628 0.0001767 0.4851 5558 3.03×10−3 0.03 15.74 0.0001152 0.8735 1646 0.0002093 0.4884 6707 1.83×10−3 0.05 12.29 0.0001198 0.8693 1362 0.0002904 0.4951 7037 8.45×10−4 0.07 13.03 0.0001175 0.8771 565.2 0.0003434 0.4542 7912 1.83×10−3 0.1 11.07 0.0001478 0.8374 235 0.0005624 0.453 9741 4.18×10−3 LC-Cl− 0.01 32.04 0.0001148 0.8847 8330 0.0000563 0.6299 73860 3.93×10−4 0.02 25.3 0.0001290 0.8744 2978 0.0001182 0.6136 20830 5.60×10−4 0.03 24.19 0.0001079 0.8758 2195 0.0002016 0.3551 9236 7.96×10−4 0.05 23.1 0.0001176 0.8458 719.1 0.0002957 0.4679 12410 3.83×10−3 0.07 20.43 0.0001043 0.8391 379.3 0.0004010 0.4495 27850 3.01×10−3 0.1 18.96 0.0001411 0.7874 338.4 0.0004679 0.3499 9680 3.23×10−3 LC-$\text{SO}_{\text{4}}^{{2-}} $ 0.01 30.1 0.0001085 0.8736 12400 0.0001089 0.4981 89150 6.82×10−4 0.02 25.22 0.0001202 0.8592 1608 0.0001916 0.4244 13390 9.59×10−4 0.03 23.07 0.0001673 0.8145 1621 0.0000909 0.4929 12360 2.51×10−3 0.05 20.76 0.0001310 0.8047 1110 0.0002258 0.4652 20660 8.88×10−4 0.07 19.5 0.0002658 0.7727 2373 0.0004917 0.4257 40920 1.52×10−3 0.1 14.82 0.0001614 0.7415 7872 0.0005338 0.3576 18148 1.16×10−3 LC
Cl−+$\text{SO}_{\text{4}}^{{2-}} $0.01 23.06 0.0001348 0.8229 6727 0.0000550 0.5558 60790 4.27×10−3 0.02 22.16 0.0001216 0.8733 7205 0.0001543 0.5928 12610 2.06×10−3 0.03 18.79 0.0001121 0.8835 841 0.0001819 0.5644 11890 4.18×10−3 0.05 12.29 0.0001198 0.8693 1362 0.0002904 0.4951 7037 8.45×10−4 0.07 11.43 0.0001043 0.8391 379.3 0.0004010 0.4495 27850 3.01×10−3 0.1 10.37 0.0001018 0.8181 2699 0.0006246 0.4161 11730 4.13×10−3 ST-Cl− 0.01 5.391 0.0000566 0.9609 18140 0.0001331 0.6403 323900 5.83×10−3 0.04 5.112 0.0000465 0.9876 19410 0.0001591 0.6505 216900 7.50×10−3 0.07 4.982 0.0000389 0.982 9934 0.0001715 0.6763 141800 5.65×10−3 0.10 4.486 0.0001388 0.9657 1653 0.0002079 0.6374 193900 7.77×10−3 0.19 4.112 0.0001461 0.9329 1604 0.0001977 0.6628 173000 2.59×10−2 0.22 4.658 0.0001180 0.9443 2733 0.0004016 0.5089 16170 2.00×10−2 0.31 3.681 0.0001627 0.9025 2393 0.0004476 0.444 29290 2.54×10−2 0.40 4.152 0.0001806 0.9225 1345 0.0007194 0.5227 8297 2.98×10−2 ST-$\text{SO}_{\text{4}}^{{2-}} $ 0.01 5.761 0.0000489 0.9533 45472 0.0002232 0.6262 898000 3.12×10−2 0.04 4.793 0.0000472 0.9437 32150 0.0002417 0.6331 840400 2.02×10−2 0.07 3.71 0.0000440 0.9333 12270 0.0002724 0.6245 314900 1.92×10−2 0.10 4.133 0.0000433 0.9126 11170 0.0002714 0.6367 339800 1.72×10−2 0.19 3.825 0.0002788 0.9491 1614 0.0000467 0.5169 445500 8.33×10−3 0.22 5.145 0.0002587 0.8349 2539 0.0005471 0.5214 17930 2.91×10−3 0.31 3.417 0.0000819 0.9798 836 0.0006337 0.5135 32580 1.98×10−2 0.40 3.221 0.0000762 0.9458 1027 0.0009938 0.4746 12670 3.14×10−2 ST
Cl+$\text{SO}_{\text{4}}^{{2-}} $0.01 5.634 0.0000442 0.9522 89602 0.0000362 0.6685 262700 1.72×10−2 0.04 4.987 0.0000429 0.9726 16280 0.0002398 0.6297 267200 1.04×10−2 0.07 5.009 0.0000435 0.9695 13440 0.0002551 0.6265 15990 4.26×10−3 0.10 4.637 0.0000544 0.9868 1703 0.0003090 0.6111 26560 7.15×10−3 0.19 4.223 0.0001823 0.8697 3961 0.0003349 0.551 21510 2.00×10−3 0.22 3.682 0.0006716 0.9053 1201 0.0009439 0.514 34670 1.32×10−2 0.31 3.418 0.0007192 0.9147 913 0.0011370 0.5202 16320 1.36×10−2 0.40 3.547 0.0009536 0.9461 906 0.0010946 0.5018 8690 2.43×10−2 Notes: $ {R}_{s} $ is the electrolyte resistance; $ {R}_{1} $ is the passivation film resistance; $ {R}_{\mathrm{c}\mathrm{t}} $ is the charge transfer resistance; $ Q $ and $ a $ are parameters in the constant phase angle elements CPE1 and CPE2; Chi-squared is the chi-squared test result. 
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表 2 Cl−和$\text{SO}_{\text{4}}^{{2-}} $在Fe(100)表面的吸附能
Table 2. Adsorption energy of chloride and $\text{SO}_{\text{4}}^{{2-}} $ adsorption on Fe (100) surface
Adsorption energy on Fe(100) /(kJ·mol−1) Top Bridge Hollow Chloride −449.896 −458.134 −363.154 $\text{SO}_{\text{4}}^{{2-}} $ −674.245 −691.32 −739.124
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