非常规服役超临界锅炉的微纳尺度腐蚀动力学模型建立及应用

doi:10.11949/0438-1157.20230440

摘要/Abstract

摘要：

深度频繁调峰超（超）临界火电机组燃煤锅炉将服役于温度频繁、大幅度多变的非常规条件，然而，依赖于某一恒定温度下连续暴露时间的传统腐蚀动力学模型无法适用于非常规服役锅炉的腐蚀预测及安全评估。从锅炉高温受热面管内（处于超临界水环境）腐蚀的原子/分子尺度过程出发，提出了适用于超（超）临界锅炉非常服役条件的低密度超临界水环境合金腐蚀微纳尺度动力学模型构建方法，以及该模型在宏观腐蚀数据拟合及微尺度腐蚀过程解析方面的多尺度应用途径；获得了典型材料T92钢的微纳尺度腐蚀动力学模型，建立了以温度和膜厚为自变量的微纳尺度氧化膜生长速率模型，并开展超期服役（已知腐蚀程度）、频繁变负荷（非恒定温度）等非常规服役条件下锅炉的腐蚀预测，可为灵活调峰火电机组安全保障技术的开发奠定基础。

关键词: 超临界水, 非常规锅炉腐蚀, 动力学模型, 多尺度, 腐蚀预测, 生长速率模型

Abstract:

Deep and frequent peak shaving supercritical/ultra-supercritical coal-fired boilers of thermal power units will serve in non-conventional conditions with frequent temperature changes and large changes. However, the traditional corrosion kinetic model relies on continuous exposure time at a constant temperature, which is challenging to meet the corrosion prediction and safety assessment of boilers in non-conventional service. According to the fundamental atomic/molecular scale process of corrosion of boiler high-temperature heating tube (in supercritical water environments), this paper proposes a new micro-nano scale kinetic model construction method for the prediction of corrosion in non-conventional conditions and the multi-scale application of the model in macro-corrosion data fitting and micro-scale corrosion process analysis. On this basis, a mechanistic corrosion kinetic model with clear microscopic processes and physical meaning for T92 steel was obtained. And a micro-nano scale oxide film growth rate model with temperature and film thickness as independent variables was developed. Finally, these micro-nano scale kinetic models were employed for the corrosion prediction of boiler tubes with known corrosion levels or/and at frequent variable load (non-constant temperature). It is of tremendous importance for evaluating the safety of large coal-fired boilers in non-conventional service.

Key words: supercritical water, non-conventional boiler corrosion, kinetic model, multiscale, corrosion prediction, growth rate model

中图分类号:

TK 224.9

李艳辉, 丁邵明, 白周央, 张一楠, 于智红, 邢利梅, 高鹏飞, 王永贞. 非常规服役超临界锅炉的微纳尺度腐蚀动力学模型建立及应用[J]. 化工学报, 2023, 74(6): 2436-2446.

Yanhui LI, Shaoming DING, Zhouyang BAI, Yinan ZHANG, Zhihong YU, Limei XING, Pengfei GAO, Yongzhen WANG. Corrosion micro-nano scale kinetics model development and application in non-conventional supercritical boilers[J]. CIESC Journal, 2023, 74(6): 2436-2446.

图/表 13

图1 适用于超（超）临界火电机组的低密度超临界水体系金属腐蚀点缺陷模型vm — 基体原子空位;VMχ' — 阳离子空位;Miχ+ — 阳离子间隙;VÖ — 氧空位;OO —晶格氧;MM — 氧化膜晶格阳离子;MOχ/2/MOδ/2 — 膜阻挡层/外层氧化物;MOθ/2(d) — 膜外层氧化物溶解或者二次氧化产物

Fig.1 Point defect model of metal corrosion in supercritical water at low density for ultra-supercritical thermal power generationvm—vacancy in the metal substrate; VMχ'— cation vacancy; Miχ+—cation interstitial; VÖ —oxygen (anion) vacancy; OO—lattice oxygen within the oxides; MM—cation at the cation sublattice of oxides; MOχ/2/MOδ/2 —barrier / outer layer oxide; MOθ/2(d) — products by further oxidizing outer layer oxide

表1 9个原子/分子尺度界面反应速率常数的中间参数定义

Table 1 Definition of intermediate parameters for the rate constants of reactions at the 9 atomic/molecular scale interfaces

反应	$a i$ /V^-1	$b i$ /cm^-1	$c i$
R _i (i = 1, 2, 3)	$α i χ γ 1 - α$	$- α i χ γ ε$	$- α i χ γ β$
R _i (i = 4, 5, 6, 7, 8, 9)	0	0	0

表1 9个原子/分子尺度界面反应速率常数的中间参数定义

Table 1 Definition of intermediate parameters for the rate constants of reactions at the 9 atomic/molecular scale interfaces

反应	$a i$ /V^-1	$b i$ /cm^-1	$c i$
R _i (i = 1, 2, 3)	$α i χ γ 1 - α$	$- α i χ γ ε$	$- α i χ γ β$
R _i (i = 4, 5, 6, 7, 8, 9)	0	0	0

表2 基本界面反应的标准速率常数与基础速率常数表达式

Table 2 Expressions for the standard rate constants and base rate constants for basic interfacial reactions

反应	$k i 0$	$k i 00$
R _i (i = 1,2,3)	$k i 00 e x p - α i χ F φ 0 R T$	$k i 00' e x p - α i Δ G R, i 0 R 1 T - 1 T 0$
R _i (i = 4,5,6,7,8,9)	$k i 00$	$k i 00' e x p - α i Δ G R, i 0 R 1 T - 1 T 0$

表2 基本界面反应的标准速率常数与基础速率常数表达式

Table 2 Expressions for the standard rate constants and base rate constants for basic interfacial reactions

反应	$k i 0$	$k i 00$
R _i (i = 1,2,3)	$k i 00 e x p - α i χ F φ 0 R T$	$k i 00' e x p - α i Δ G R, i 0 R 1 T - 1 T 0$
R _i (i = 4,5,6,7,8,9)	$k i 00$	$k i 00' e x p - α i Δ G R, i 0 R 1 T - 1 T 0$

表3 600℃下T92钢氧化增重动力学模型优化所得基本参数

Table 3 Basic parameters obtained from the optimization of the kinetic model in mass gain for T92 steel at 600℃

符号	参数	数值
T/℃	温度	600
DO/(mg/L)	溶解氧量	0.01
pH	pH	11
$α$	阻挡层/外层界面极化率	0.70
$α 3$	传递系数	0.10
$k 300$ /(mol/(cm²∙s)）	基本速率常数	8.26×10^-11
$k 800$ /(mol/(cm²∙s)）	基本速率常数	9.97×10^-9
$k 900$ /(mol/(cm²∙s)）	基本速率常数	8.55×10^-9
$β$	阻挡层/环境界面处电势降对pH的依赖性	-0.005
V/V	等效腐蚀电位	0.76
ε/(V/cm)	膜内电场强度	128.20
$ρ b l$ /(g/cm³)	阻挡层平均密度	4.97
$ρ o l$ /(g/cm³)	外层平均密度	5.04
PBR	平均Pilling-Bedworth比率	2.08
n、m、q、r	界面反应对氧浓度的动力学级数	0.50

表3 600℃下T92钢氧化增重动力学模型优化所得基本参数

Table 3 Basic parameters obtained from the optimization of the kinetic model in mass gain for T92 steel at 600℃

符号	参数	数值
T/℃	温度	600
DO/(mg/L)	溶解氧量	0.01
pH	pH	11
$α$	阻挡层/外层界面极化率	0.70
$α 3$	传递系数	0.10
$k 300$ /(mol/(cm²∙s)）	基本速率常数	8.26×10^-11
$k 800$ /(mol/(cm²∙s)）	基本速率常数	9.97×10^-9
$k 900$ /(mol/(cm²∙s)）	基本速率常数	8.55×10^-9
$β$	阻挡层/环境界面处电势降对pH的依赖性	-0.005
V/V	等效腐蚀电位	0.76
ε/(V/cm)	膜内电场强度	128.20
$ρ b l$ /(g/cm³)	阻挡层平均密度	4.97
$ρ o l$ /(g/cm³)	外层平均密度	5.04
PBR	平均Pilling-Bedworth比率	2.08
n、m、q、r	界面反应对氧浓度的动力学级数	0.50

表4 500~700℃下T92钢氧化增重动力学模型中宏观参数取值

Table 4 Macroscopic parameter values of kinetic model in mass gain for T92 at 500—700℃

参数	工况
	500℃^①	600℃		650℃^①	700℃^①
	500℃^①	宏观拟合值^①	微观计算值^②	650℃^①	700℃^①
P₁/(mg/cm²)	0.130	0.130	0.104	0.130	0.130
P₂/(mg/cm²)	-0.98	-2.60	-2.70	-4.30	-5.20
P₃/(mg/(cm²∙s))	4.98×10^-7	6.92×10^-6	6.81×10^-6	2.06×10^-5	3.97×10^-5
P₄/(mg/(cm²∙s))	3.46×10^-8	3.68×10^-8	3.74×10^-8	3.75×10^-8	3.85×10^-8
P₅/(mg/(cm²∙s))	5.41×10^-7	7.22×10^-6	7.38×10^-6	2.23×10^-5	4.31×10^-5
P₆/(mg/(cm²∙s))	3.83×10^-8	4.07×10^-8	4.05×10^-8	4.12×10^-8	4.17×10^-8
P₇/(mg/cm²)	-22.9	-51.0	-55.5	-82.7	-96.2

图2 P3~P6与温度的拟合曲线

Fig.2 Fitting curves of P3—P6vs temperature

表5 直接拟合所得增重动力学模型中宏观参数对温度的依赖性

Table 5 The dependence of macroscopic parameters on temperature in the mass gain kinetic model obtained by direct fitting

参数	关系式
P₁	1.30×10^-4
P₂	$- 0.0011 e x p T 409.95 + 0.0060$
P₃	$1.43 e x p - 16785.74 T$
P₄	$5.80 × 10 - 11 e x p - 395.80 T$
P₅	$1.54 e x p - 16787.19 T$
P₆	$5.86 × 10 - 11 e x p - 324.99 T$
P₇	$- P 5 P 2 P 3 l n P 3 e P 1 P 2 - P 4 + P 1$

表5 直接拟合所得增重动力学模型中宏观参数对温度的依赖性

Table 5 The dependence of macroscopic parameters on temperature in the mass gain kinetic model obtained by direct fitting

参数	关系式
P₁	1.30×10^-4
P₂	$- 0.0011 e x p T 409.95 + 0.0060$
P₃	$1.43 e x p - 16785.74 T$
P₄	$5.80 × 10 - 11 e x p - 395.80 T$
P₅	$1.54 e x p - 16787.19 T$
P₆	$5.86 × 10 - 11 e x p - 324.99 T$
P₇	$- P 5 P 2 P 3 l n P 3 e P 1 P 2 - P 4 + P 1$

图3 基于表5的500~700℃超临界水下T92钢腐蚀增重预测

Fig.3 Prediction of T92 corrosion mass gain in 500—700℃ supercritical water based on Table 5

图4 T92钢部分腐蚀微观反应基础速率常数与温度的拟合关系

Fig.4 Fitted rate constants vs temperature for the microscopic reaction basis of partial corrosion of steel T92

表6 部分原子尺度反应速率常数及增重动力学模型中间参数P1~P7与温度的函数关系

Table 6 Atomic-scale reaction rate constants and intermediate parameters P1—P7 of the mass gain kinetic model as a function of temperature

参数	关系式	常数
$k 30$	$0.071 e x p - 17841.47 T$	—
$k 8$	$1.21 × 10 - 8 e x p - 165.63 T$	—
$k 9$	$1.23 × 10 - 8 e x p - 316.02 T$	—
ε	$2.48 × 106 e x p - T 83.99 + 48.41$	—
P₁	1.04×10^-4	—
P₂	$C 1 T ε$	$C 1 = - 4.00 × 10 - 4$
P₃	$C 2 k 30 e x p 993.16 T$	$C 2 = 21.21$
P₄	$C 3 k 8$	$C 3 = 37.50 × 10 - 4$
P₅	$C 4 k 30 e x p 993.16 T$	$C 4 = 23.00$
P₆	$C 5 k 8 + C 6 k 9$	$C 5 = 40.65 × 10 - 4$ $C 6 = 37.64 × 10 - 4$
P₇	$- P 5 P 2 P 3 l n P 3 e P 1 P 2 - P 4 + P 1$	—

表6 部分原子尺度反应速率常数及增重动力学模型中间参数P1~P7与温度的函数关系

Table 6 Atomic-scale reaction rate constants and intermediate parameters P1—P7 of the mass gain kinetic model as a function of temperature

参数	关系式	常数
$k 30$	$0.071 e x p - 17841.47 T$	—
$k 8$	$1.21 × 10 - 8 e x p - 165.63 T$	—
$k 9$	$1.23 × 10 - 8 e x p - 316.02 T$	—
ε	$2.48 × 106 e x p - T 83.99 + 48.41$	—
P₁	1.04×10^-4	—
P₂	$C 1 T ε$	$C 1 = - 4.00 × 10 - 4$
P₃	$C 2 k 30 e x p 993.16 T$	$C 2 = 21.21$
P₄	$C 3 k 8$	$C 3 = 37.50 × 10 - 4$
P₅	$C 4 k 30 e x p 993.16 T$	$C 4 = 23.00$
P₆	$C 5 k 8 + C 6 k 9$	$C 5 = 40.65 × 10 - 4$ $C 6 = 37.64 × 10 - 4$
P₇	$- P 5 P 2 P 3 l n P 3 e P 1 P 2 - P 4 + P 1$	—

图5 基于腐蚀微纳尺度反应动力学的T92钢微纳尺度氧化增重模型的验证

Fig.5 Verification of the micro-nano scale oxidation mass gain model of steel T92 based on the kinetics of the micro-nano corrosion reactions

图6 面向具有一定腐蚀程度的在役或拟超期服役锅炉的腐蚀预测应用

Fig.6 Application of oxide film growth rate model for corrosion prediction for in-service or intended to be extended service boilers with certain degree of corrosion

图7 T92钢在550和600℃的循环交变温度下腐蚀增重预测

Fig.7 Prediction of corrosion mass gain for cyclic oxidation of T92 at 550 and 600℃

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