J55钢在模拟CO2 注入井环空环境中的关键性腐蚀因素

doi:10.11901/1005.3093.2023.288

材料研究学报

2024, Vol. 38

Issue (4): 308-320 DOI: 10.11901/1005.3093.2023.288

研究论文

本期目录 | 过刊浏览

J55钢在模拟CO₂ 注入井环空环境中的关键性腐蚀因素

崔怀云¹, 刘智勇¹^,²(

), 卢琳¹^,³(

)

^1.北京科技大学新材料技术研究院北京 100083
^2.国家市场监管重点实验室(钢制管子及管件安全评价) 石家庄 050000
^3.海洋装备用金属材料及其应用国家重点实验室鞍山 114000

Critical Corrosion Factors for J55 Tubing Steel in a Simulated Annulus Environment of CO₂ Injection Well

CUI Huaiyun¹, LIU Zhiyong¹^,²(

), LU Lin¹^,³(

)

^1.Institute for Advanced Materials and Technology, University of Science and Technology Beijing, Beijing 100083, China
^2.Key Laboratory of Safety Evaluation of Steel Pipes and Fittings for State Market Regulation, Shijiazhuang 050000, China
^3.State Key Laboratory of Metal Material for Marine Equipment and Application, Anshan 114000, China

引用本文:

崔怀云, 刘智勇, 卢琳. J55钢在模拟CO₂ 注入井环空环境中的关键性腐蚀因素[J]. 材料研究学报, 2024, 38(4): 308-320.
Huaiyun CUI, Zhiyong LIU, Lin LU. Critical Corrosion Factors for J55 Tubing Steel in a Simulated Annulus Environment of CO₂ Injection Well[J]. Chinese Journal of Materials Research, 2024, 38(4): 308-320.

全文: PDF(7742 KB) HTML

摘要:

基于实际CO₂驱注井环空环境计算环空参数、测试电化学和进行相关性分析，研究了环境总压、CO₂分压、pH值以及温度对J55钢腐蚀电化学行为的影响。结果表明，CO₂分压和温度是影响J55钢腐蚀速度的关键因素。CO₂分压与电荷转移电阻(R_ct)显著相关，Spearman相关系数为-0.623；CO₂分压的升高使溶液的pH值降低从而促进析氢反应，使腐蚀速率提高。温度与R_ct的相关行显著，Spearman相关系数为-0.692；温度的降低抑制材料的电化学反应活性且阻碍腐蚀产物膜的形成，减缓了J55钢的腐蚀。溶液初始pH值的降低能促进J55钢的腐蚀，但是温度和CO₂分压的影响可将其覆盖。

关键词 ：材料失效与保护, CO₂腐蚀, 电化学, J55钢, 环空环境

Abstract：

CO₂-enchanced oil recovery technology has been widely used to enhance the profitability of oil fields. The leakage of CO₂ into the annulus environment results in the formation of strong corrosive annulus fluid there, which is ineluctable. Due to the fluctuations of annulus environmental parameters in the practice, therefore, to simulate the annulus environment in the laboratory may be very difficult. Based on the parameters of the real annulus environment, the impact of total pressure, partial pressure of CO₂ ( $P C O 2$ ), pH value and temperature (T) etc., on the corrosion behavior of J55 steel are investigated by means of numerical simulation in terms of the parameters, electrochemical test and correlation analysis. Results shows that the $P C O 2$ and T are the critical factors influencing corrosion behavior. The Spearman correlation coefficient (r) between $P C O 2$ and charge transfer resistance (R_ct) is -0.623, where the significant level is 0.013 (2-tailed), which means that the R_ct is significantly correlated with the $P C O 2$ . The increasing $P C O 2$ can decrease the pH value of the simulated annulus environment and accelerate the corrosion of J55 steel. The r between T and R_ct is -0.692, where the significant level is 0.004 (2-tailed), which means that the R_ct is significantly correlated with the T. The decreasing temperature can reduce the reaction activity of J55 steel, mitigate the corrosion and restrict the formation of FeCO₃ scale. The initial pH of the simulated solution has a little promoting effect on the corrosion of J55 steel, which may be covered by the effect of T and $P C O 2$ .

Key words： materials failure and protection CO₂ corrosion electrochemical J55 steel annulus environment

收稿日期: 2023-06-09

ZTFLH:

TG172

基金资助:国家市场监督管理总局科技计划(2021MK020)

通讯作者: 刘智勇，研究员，liuzhiyong7804@126.com，研究方向为金属材料腐蚀与防护;

Corresponding author: LIU Zhiyong, Tel: (010)62333931, E-mail: liuzhiyong7804@126.com;

作者简介: 崔怀云，男，1995年生，博士生

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表1 实验用J55级油管钢的化学成分

图1 J55油管钢的金相组织

Composition	Value
Sulfate / mg·L^-1	3000~15000
NaHCO₃ / mg·L^-1	150~1000
KCl / mg·L^-1	12000~15000
NaCl / mg·L^-1	12000~15000
Inhibitor / mg·L^-1	50~200
$P C O 2$ / MPa	4.00

表2 油田水介质的成分

Parameters	$K H' *$ / 10¹ mol·L^-1·MPa^-1	$K 1' *$ / mol·L^-1	$K 2 *$ / mol·L^-1	$K w *$ /(mol·L^-1)²	ρ_w / g·cm^-3
a₁	2.0302	-7.8294	-15.707	-4.098	1.8105 × 10^-3
a₂	-2.3508 × 10^-2	8.2473 × 10^-3	3.0972 × 10^-2	-3245.2	138.08
a₃	2.6144 × 10^-5	-1.0530 × 10^-5	-4.3124 × 10^-5	2.2362 × 10⁴	-
a₄	-	4.4527 × 10^-4	3.8058 × 10^-4	-3.9840 × 10⁷	-
a₅	-	0.4772	1.166	13.957	-
a₆	-	-0.118	-0.3466	-1262.3	-
a₇	-	-	-	8.5641 × 10⁵	-

表3 修正后的平衡常数计算参数[23]

图2 模拟环空环境中pH值的计算结果

图3 在25℃环空pH值与CO2分压的关系

图4 电化学试样的示意图

图5 J55钢在不同总压下的Nyquist和Bode图，Nyquist图中的插图为对应的等效电路

图6 J55钢在不同温度下EIS谱拟合的等效电路

表4 J55钢在不同总压下的电化学阻抗谱拟合数据

图7 J55油管钢在不同总压下的动电位极化曲线和拟合结果

图8 J55油管钢在不同PCO2下的Nyquist和Bode图，Nyquist图中的插图为对应的等效电路

$P C O 2$ / MPa	R_s / Ω·cm²	Q_dl × 10^-4 /Ω^-1·cm^-2·s^-n	n_dl	R_ct / Ω·cm²	R_L / Ω·cm²	L / H·cm^-2	C_f / F·cm^-2	R_pore / Ω·cm²
4	7.10	6.23	0.812	56.67	217.9	112.3	1.349	12.77
3	8.36	5.12	0.820	95.87	314.4	233	1.801	12.23
2	7.80	5.12	0.817	115.1	449.2	451.7	1.386	10.84
1	7.871	3.94	0.823	197.8	620.1	640	1.284	22.69
0.1	6.163	2.84	0.847	268.7	933.2	1330	0.3175	25.57

表5 J55钢在不同PCO2下的阻抗谱拟合数据

图9 J55钢在不同PCO2下的动电位极化曲线和拟合结果

图10 在不同pH值下J55钢的Nyquist和Bode图

表6 J55钢在不同pH下的阻抗谱拟合数据

图11 J55钢在不同pH值下的动电位极化曲线和拟合结果

图12 J55钢在不同温度下的Nyquist和Bode图

表7 J55钢在不同温度下电化学阻抗谱的拟合数据

图13 J55钢在不同温度下的极化曲线和拟合结果

Number	P_total / MPa	$P C O 2$ / MPa	pH	T / ^oC	R_ct / Ω·cm²	I_corr / μA·cm^-2
PP1	9	4	4	25	56.67	428.00
PP2	9	3	4	25	95.87	201.00
PP3	9	2	4	25	115.1	116.00
PP4	9	1	4	25	197.8	88.00
PP5	9	0.1	4	25	268.7	32.00
pH1	9	4	4	25	56.67	428.00
pH2	9	4	5	25	62.8	386.00
pH3	9	4	6	25	81.5	312.00
T1	9	4	4	5	242.8	95.10
T2	9	4	4	15	116.8	189.80
T3	9	4	4	25	56.67	428.00
T4	9	4	4	40	26.84	1101.30
T5	9	4	4	50	18.3	1422.90
PT1	15	4	4	25	75.18	236.21
PT2	12	4	4	25	70.08	313.92
PT3	9	4	4	25	56.67	428.00
PT4	6	4	4	25	59.40	418.17
PT5	4	4	4	25	67.92	395.23

表8 相关性计算的原始数据表

	Shapiro-Wilk
	Statistic	Sig. (P value)
P_total / MPa	0.741	0.001
$P C O 2$ / MPa	0.599	0.000
pH	0.421	0.000
T / ^oC	0.736	0.001
R_ct / Ω·cm²	0.837	0.011
I_corr / μA·cm^-2	0.742	0.001

表9 表7中数据的正态性检验

图14 环境因素与J55钢腐蚀动力学参数的频率直方图

		P_total	$P C O 2$	pH	T	R_ct	I_corr
P_total	r	1.000	0.000	0.000	0.000	0.147	-0.211
P_total	P	-	1.000	1.000	1.000	0.602	0.451
$P C O 2$	r	0.000	1.000	0.232	0.000	-0.623^*	0.692^**
$P C O 2$	P	1.000	-	0.405	1.000	0.013	0.004
pH	r	0.000	0.232	1.000	0.000	-0.078	0.085
pH	P	1.000	0.405	-	1.000	0.781	0.765
T	r	0.000	0.000	0.000	1.000	-0.692^**	0.633^*
T	P	1.000	1.000	1.000	-	0.004	0.011
R_ct	r	0.147	-0.623^*	-0.078	-0.692^**	1.000	-0.986^**
R_ct	P	0.602	0.013	0.781	0.004	-	0.000
I_corr	r	-0.211	0.692^**	0.085	0.633^*	-0.986^**	1.000
I_corr	P	0.451	0.004	0.765	0.011	0.000	-

表10 Spearman等级相关分析结果

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