CN109190311B - Method for predicting oxide film peeling of austenitic heat-resistant steel for ultra-supercritical thermal power generating unit - Google Patents
Method for predicting oxide film peeling of austenitic heat-resistant steel for ultra-supercritical thermal power generating unit Download PDFInfo
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- 239000010959 steel Substances 0.000 title claims abstract description 22
- 238000000034 method Methods 0.000 title claims abstract description 20
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- 239000000956 alloy Substances 0.000 claims abstract description 24
- 230000007547 defect Effects 0.000 claims abstract description 21
- 229910000604 Ferrochrome Inorganic materials 0.000 claims abstract description 7
- 230000008646 thermal stress Effects 0.000 claims abstract description 6
- 230000008859 change Effects 0.000 claims abstract description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 6
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 5
- 239000001301 oxygen Substances 0.000 claims description 5
- 229910052760 oxygen Inorganic materials 0.000 claims description 5
- 239000011159 matrix material Substances 0.000 claims description 4
- 239000000203 mixture Substances 0.000 claims description 3
- 230000008520 organization Effects 0.000 claims 1
- 239000000463 material Substances 0.000 abstract description 8
- 230000008569 process Effects 0.000 abstract description 6
- 238000009826 distribution Methods 0.000 abstract description 3
- 230000003647 oxidation Effects 0.000 description 12
- 238000007254 oxidation reaction Methods 0.000 description 12
- 238000005336 cracking Methods 0.000 description 6
- 230000006872 improvement Effects 0.000 description 5
- 238000012360 testing method Methods 0.000 description 4
- 238000001816 cooling Methods 0.000 description 3
- 238000005516 engineering process Methods 0.000 description 3
- 229910001566 austenite Inorganic materials 0.000 description 2
- 230000000977 initiatory effect Effects 0.000 description 2
- 238000012544 monitoring process Methods 0.000 description 2
- 238000009659 non-destructive testing Methods 0.000 description 2
- 238000004901 spalling Methods 0.000 description 2
- 239000000758 substrate Substances 0.000 description 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 1
- CDBYLPFSWZWCQE-UHFFFAOYSA-L Sodium Carbonate Chemical compound [Na+].[Na+].[O-]C([O-])=O CDBYLPFSWZWCQE-UHFFFAOYSA-L 0.000 description 1
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- 238000011161 development Methods 0.000 description 1
- 238000001983 electron spin resonance imaging Methods 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 230000003628 erosive effect Effects 0.000 description 1
- 239000003546 flue gas Substances 0.000 description 1
- 230000002401 inhibitory effect Effects 0.000 description 1
- 238000012423 maintenance Methods 0.000 description 1
- 230000007246 mechanism Effects 0.000 description 1
- 238000013021 overheating Methods 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 238000010248 power generation Methods 0.000 description 1
- 238000004626 scanning electron microscopy Methods 0.000 description 1
- 238000005480 shot peening Methods 0.000 description 1
- 238000005482 strain hardening Methods 0.000 description 1
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- 238000004627 transmission electron microscopy Methods 0.000 description 1
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Abstract
Description
技术领域technical field
本发明属于材料领域，具体涉及一种超超临界火电机组用奥氏体耐热钢氧化膜剥落预测方法。The invention belongs to the field of materials, and in particular relates to a method for predicting peeling off of an austenitic heat-resistant steel oxide film for an ultra-supercritical thermal power unit.
背景技术Background technique
超超临界火电机组(USC)具有高效率、低能耗、低排放等优点，目前已成为国内外火力发电行业发展的必然趋势。随着USC技术的推广，火电机组锅炉蒸汽参数明显提高，进而对锅炉关键部件材料的性能提出了极高的要求。其中，过热器/再热器是锅炉中工作环境最为恶劣的部件，运行过程中长期受到高温水蒸汽氧化、烟气腐蚀、蠕变等诸多因素的影响。因此，以TP91、TP92等为代表的铁素体耐热钢已逐渐无法满足过热器/再热器管道对材料性能的要求。目前，国内外600℃级以上的USC过热器/再热器已广泛采用了TP304H、TP347H等18-8系奥氏体耐热钢。与铁素体钢相比，奥氏体耐热钢具有更加优异的高温持久强度以及抗氧化性能。然而，由于奥氏体钢耐热钢的热膨胀系数与氧化膜相比明显较高，因此在冷却过程中氧化膜内部将产生较大的压应力，导致其在服役期间氧化皮剥落现象十分严重。其中，氧化皮剥落导致管道堵塞，进而造成管道超温运行甚至爆管现象已成为影响机组安全稳定运行的最主要原因之一，例如仅广东省2008-2012年600MW及以上超超临界火电机组由于氧化皮剥落堵塞而引起的爆管就高达23次，造成经济损失超过4.6亿元。此外，剥落氧化皮尺寸较小时将随蒸汽流动并导致汽水品质恶化，同时造成汽轮机叶片冲蚀磨损、主汽门卡涩等问题。可见，研究奥氏体耐热钢表面氧化皮的剥落行为并在此基础上改善其抗剥落性能具有重要的意义。Ultra-supercritical thermal power units (USC) have the advantages of high efficiency, low energy consumption, and low emissions, and have become an inevitable trend in the development of domestic and foreign thermal power generation industries. With the promotion of USC technology, the steam parameters of thermal power unit boilers have been significantly improved, which in turn puts forward extremely high requirements on the performance of key components of boilers. Among them, the superheater/reheater is the part with the worst working environment in the boiler. It is affected by many factors such as high-temperature water vapor oxidation, flue gas corrosion, and creep during operation for a long time. Therefore, ferritic heat-resistant steel represented by TP91, TP92, etc. has gradually been unable to meet the material performance requirements of superheater/reheater pipes. At present, 18-8 series austenitic heat-resistant steels such as TP304H and TP347H have been widely used in USC superheaters/reheaters above 600 °C at home and abroad. Compared with ferritic steel, austenitic heat-resistant steel has more excellent high-temperature durable strength and oxidation resistance. However, since the thermal expansion coefficient of austenitic heat-resistant steel is significantly higher than that of the oxide film, a large compressive stress will be generated inside the oxide film during the cooling process, resulting in serious scale peeling during service. Among them, pipeline clogging caused by scale peeling, which in turn causes pipeline overheating or even pipe bursting, has become one of the most important reasons affecting the safe and stable operation of units. There were as many as 23 pipe bursts caused by scale peeling and blockage, resulting in economic losses of more than 460 million yuan. In addition, when the size of the exfoliated oxide scale is small, it will flow with the steam and lead to deterioration of the quality of soda water. At the same time, it will cause problems such as erosion and wear of steam turbine blades and jamming of the main steam valve. It can be seen that it is of great significance to study the peeling behavior of the oxide scale on the surface of austenitic heat-resistant steel and improve its anti-flaking performance on this basis.
由于氧化膜与基体热膨胀系数不匹配，锅炉在服役期间的变负荷或启停等行为均会导致氧化膜内部产生较大的热应力，进而造成其开裂与剥落。EPRI在总结大量实验结果的基础上建立了氧化膜厚度与弹性应变的关系模型，结果发现随着氧化膜厚度的增加，诱发其开裂并剥落所需的最低弹性应变减小。由于这一模型可以为锅炉过热器/再热器等受热管材氧化皮剥落行为进行预测，因而已被广泛应用于电厂安全运行评估。根据该预测方法，氧化膜厚度越薄，则导致其开裂所需的弹性应变越高，氧化膜的抗剥落能力也越好。因此，为抑制氧化膜的剥落，目前国内外主要采用新型合金(TP347HFG、Super304H)以及表面处理(冷加工、喷丸)等方法，通过抑制氧化膜的生长速度进而提高其与基体的结合强度。然而，人们在随后的研究中发现过热器/再热器管材在服役达到一定时间后，其表面形成的氧化膜内存在大量孔洞缺陷。研究表明，氧化膜内部产生的缺陷对于其在热应力作用下的开裂方式具有显著影响，这是由于裂纹在萌生与扩展过程中需要克服产生新表面所需的表面能，而氧化膜内部或其与基体界面处缺陷的存在为裂纹的萌生与扩展提供了便捷途径。近年来，关于缺陷对氧化膜开裂与剥落行为的影响开始受到国外学者的关注。然而，目前关于含缺陷多层氧化膜的裂纹萌生与扩展机制方面的研究尚未见报道。对于600℃级超超临界机组过热器/再热器材料，现今应用最广泛的奥氏体耐热钢在服役期间氧化膜具有双层结构，并且缺陷具有在双层氧化膜内界面富集的特点，这对于其氧化膜开裂与剥落行为的有效预测提出了新的挑战。Due to the mismatch between the thermal expansion coefficient of the oxide film and the substrate, the behavior of changing load or starting and stopping of the boiler during service will cause large thermal stress inside the oxide film, which will cause cracking and peeling off. EPRI established a relationship model between oxide film thickness and elastic strain on the basis of summarizing a large number of experimental results. It was found that as the thickness of the oxide film increases, the minimum elastic strain required to induce cracking and peeling decreases. Because this model can predict the scale peeling behavior of heated pipes such as boiler superheaters/reheaters, it has been widely used in the assessment of power plant safety operation. According to this prediction method, the thinner the oxide film, the higher the elastic strain required to cause its cracking, and the better the peeling resistance of the oxide film. Therefore, in order to suppress the peeling of the oxide film, new alloys (TP347HFG, Super304H) and surface treatment (cold working, shot peening) are mainly used at home and abroad to increase the bonding strength with the substrate by inhibiting the growth rate of the oxide film. However, in subsequent studies, it was found that after the superheater/reheater pipes have been in service for a certain period of time, there are a large number of hole defects in the oxide film formed on the surface. Studies have shown that the defects generated inside the oxide film have a significant impact on its cracking mode under thermal stress. The existence of defects at the interface with the matrix provides a convenient way for crack initiation and propagation. In recent years, the influence of defects on the cracking and peeling behavior of oxide films has begun to attract the attention of foreign scholars. However, there are no reports on the mechanism of crack initiation and propagation in defect-containing multilayer oxide films. For superheater/reheater materials of 600°C ultra-supercritical units, the most widely used austenitic heat-resistant steel has a double-layer oxide film during service, and the defects are enriched at the inner interface of the double-layer oxide film. characteristics, which pose a new challenge for the effective prediction of the cracking and peeling behavior of its oxide film.
发明内容Contents of the invention
本发明的目的在于解决现有技术中的问题，提出一种超超临界火电机组用奥氏体耐热钢氧化膜剥落预测方法，该模型针对目前600℃级超超临界火电机组过热器/再热器常用材料(TP304H、TP347H、Super304H、TP347HFG)在服役过程中界面缺陷的尺寸及分布观察结果，能够对合金表面形成的双层氧化膜剥落行为进行预测。The purpose of the present invention is to solve the problems in the prior art, and propose a method for predicting the peeling off of the oxide film of austenitic heat-resistant steel for ultra-supercritical thermal power units. The observation results of the size and distribution of interface defects of commonly used materials for heaters (TP304H, TP347H, Super304H, TP347HFG) during service can predict the peeling behavior of the double-layer oxide film formed on the surface of the alloy.
为实现上述目的，本发明采用如下的技术方案：To achieve the above object, the present invention adopts the following technical solutions:
超超临界火电机组用奥氏体耐热钢氧化膜剥落预测方法，合金在服役过程中表面形成双层氧化膜，内层为FeCr2O4及外层为Fe3O4，并且双层氧化膜界面缺陷间距l与尺寸a之比满足如下条件：0.2≤l/a≤6，则通过临界温差随l/a的变化曲线预测氧化膜在不同热应力作用下的剥落行为。Prediction method for peeling off of austenitic heat-resistant steel oxide film for ultra-supercritical thermal power units. The alloy forms a double-layer oxide film on the surface during service. The inner layer is FeCr 2 O 4 and the outer layer is Fe 3 O 4 , and the double-layer oxidation The ratio of defect spacing l to size a at the film interface satisfies the following conditions: 0.2≤l/a≤6, then the peeling behavior of the oxide film under different thermal stresses can be predicted by the curve of critical temperature difference versus l/a.
本发明进一步的改进在于，合金的服役温度为600～650℃，水蒸汽流量不超过2500吨/小时，溶解氧含量不超过5ppm。The further improvement of the present invention lies in that the service temperature of the alloy is 600-650° C., the water vapor flow rate does not exceed 2500 tons/hour, and the dissolved oxygen content does not exceed 5 ppm.
本发明进一步的改进在于，合金成分满足Cr元素含量按质量百分比不超过20％，且合金基体为单一奥氏体组织。The further improvement of the present invention lies in that the composition of the alloy satisfies that the content of Cr element is not more than 20% by mass percentage, and the matrix of the alloy is a single austenite structure.
本发明进一步的改进在于，双层氧化膜的厚度均不低于5微米。The further improvement of the present invention lies in that the thickness of the double-layer oxide film is not less than 5 microns.
本发明进一步的改进在于，双层氧化膜界面缺陷尺寸不超过200nm。The further improvement of the present invention lies in that the size of the interface defects of the double-layer oxide film does not exceed 200nm.
本发明进一步的改进在于，临界温差随l/a的变化曲线通过ANSYS模拟软件计算得到。The further improvement of the present invention is that the variation curve of the critical temperature difference with l/a is calculated by ANSYS simulation software.
与现有技术相比，本发明具有的有益效果：Compared with the prior art, the present invention has the beneficial effects:
本发明的模型结合实际观测结果，主要考察了缺陷存在于双层氧化膜界面时对氧化皮剥落造成的影响。这一模型与合金实际氧化过程中氧化膜内部结构更加吻合，可以对氧化膜的剥落行为进行有效预测。本发明针对目前600℃级超超临界火电机组过热器/再热器常用材料(TP304H、TP347H、Super304H、TP347HFG)在服役过程中界面缺陷的尺寸及分布观察结果，能够对合金表面形成的双层氧化膜剥落行为进行预测，适用于超超临界火电机组过热器、再热器等关键部件用奥氏体耐热钢服役期间氧化膜剥落行为预测。The model of the present invention combines the actual observation results to mainly investigate the influence of defects on the peeling off of the oxide scale when the defects exist at the interface of the double-layer oxide film. This model is more consistent with the internal structure of the oxide film in the actual oxidation process of the alloy, and can effectively predict the peeling behavior of the oxide film. The present invention aims at the observation results of the size and distribution of interface defects of the commonly used materials (TP304H, TP347H, Super304H, TP347HFG) in the service process of the superheater/reheater of the current 600°C ultra-supercritical thermal power unit, and can analyze the double layer formed on the surface of the alloy. The prediction of oxide film spalling behavior is suitable for the prediction of oxide film spalling behavior of austenitic heat-resistant steel used in key components such as superheaters and reheaters of ultra-supercritical thermal power units during service.
附图说明Description of drawings
图1为多孔洞双层氧化膜模型临界温差VT随l/a的变化情况图。Figure 1 is a graph showing the variation of the critical temperature difference VT with l/a for the porous double-layer oxide film model.
图2为Super304H合金氧化后合金表面氧化膜形貌，其中，A为FeCr2O4，B为Fe3O4。Figure 2 shows the surface oxide film morphology of Super304H alloy after oxidation, where A is FeCr 2 O 4 and B is Fe 3 O 4 .
具体实施方式Detailed ways
本发明适用于长期在超超临界水蒸气条件下服役的奥氏体耐热钢，其表面在服役过程中形成双层氧化膜，且在双层氧化膜界面存在孔洞缺陷。The invention is applicable to the austenitic heat-resistant steel which has been in service under the ultra-supercritical water vapor condition for a long time. The surface of the austenitic heat-resistant steel forms a double-layer oxide film during the service process, and hole defects exist at the interface of the double-layer oxide film.
将服役温度为600～650℃，水蒸汽流量不超过2500吨/小时，溶解氧含量不超过5ppm的合金，合金在服役过程中表面形成双层氧化膜，内层为FeCr2O4及外层为Fe3O4，双层氧化膜的厚度均不低于5微米，双层氧化膜界面缺陷尺寸不超过200nm，缺陷间距l与尺寸a之比满足如下条件：0.2≤l/a≤6，则能够通过临界温差随l/a的变化曲线图预测氧化膜在不同热应力(温度降幅)作用下的剥落行为。其中，图1为临界温差随l/a的变化曲线，该变化曲线通过ANSYS模拟软件计算得到。The service temperature is 600-650 ℃, the water vapor flow rate is not more than 2500 tons/hour, and the dissolved oxygen content is not more than 5ppm. The alloy will form a double-layer oxide film on the surface during service. The inner layer is FeCr 2 O 4 and the outer layer It is Fe 3 O 4 , the thickness of the double-layer oxide film is not less than 5 microns, the size of the defect at the interface of the double-layer oxide film is not more than 200nm, and the ratio of defect spacing l to size a satisfies the following conditions: 0.2≤l/a≤6, Then the peeling behavior of the oxide film under different thermal stresses (temperature drop) can be predicted by the graph of the change of the critical temperature difference with l/a. Among them, Fig. 1 is the change curve of critical temperature difference with l/a, which is calculated by ANSYS simulation software.
合金成分满足Cr元素含量按质量百分比不超过20％，且合金基体为单一奥氏体组织。The composition of the alloy satisfies that the Cr element content does not exceed 20% by mass percentage, and the alloy matrix is a single austenite structure.
通过本发明能够掌握奥氏体耐热钢氧化皮剥落规律，优化火电机组维护检修周期。下面结合附图通过具体实施例进行详细说明。Through the invention, the peeling off rule of the austenitic heat-resistant steel oxide scale can be grasped, and the maintenance period of the thermal power unit can be optimized. The following describes in detail through specific embodiments in conjunction with the accompanying drawings.
实施例1Example 1
本实施例选用Super304H作为测试材料，蒸汽氧化实验条件为温度：620℃，溶解氧含量：5ppm，蒸汽流速：0mL/min，蒸汽氧化时间：600小时。In this embodiment, Super304H is selected as the test material, and the steam oxidation test conditions are temperature: 620°C, dissolved oxygen content: 5ppm, steam flow rate: 0mL/min, and steam oxidation time: 600 hours.
1)双层氧化膜厚度及界面缺陷观测：采用透射电子显微镜对氧化后合金表面氧化膜形貌进行观察，如图2所示。结果发现合金氧化后由内层FeCr2O4及外层Fe3O4构成，氧化膜厚度分别为12微米与15微米。界面孔洞尺寸约为150～180nm，而此时该合金l/a值均在3.5～4.5范围内，从图1中可以看出，在这一条件下氧化膜剥落所需的临界温度约为390～420℃。1) Observation of the thickness of the double-layer oxide film and interface defects: the morphology of the oxide film on the surface of the oxidized alloy was observed by a transmission electron microscope, as shown in Figure 2. It was found that the alloy is composed of inner layer FeCr 2 O 4 and outer layer Fe 3 O 4 after oxidation, and the oxide film thicknesses are 12 microns and 15 microns respectively. The interface hole size is about 150-180nm, and the l/a value of the alloy is in the range of 3.5-4.5 at this time. It can be seen from Figure 1 that the critical temperature required for the peeling off of the oxide film under this condition is about 390 ~420°C.
2)双层氧化膜剥落行为监测：采用声发射无损检测技术对氧化膜剥落行为进行测定，设置门槛值为30dB。结果发现在开始降温后2900秒后出现氧化膜剥落产生的声发射信号，对比炉膛温度下降速率，确定此时对应温度降幅为405℃，与本发明模型预测结果吻合。2) Monitoring of the peeling behavior of the double-layer oxide film: the peeling behavior of the oxide film is measured using the acoustic emission non-destructive testing technology, and the threshold value is set to 30dB. As a result, it was found that the acoustic emission signal generated by the peeling off of the oxide film appeared after 2900 seconds after the start of cooling. Comparing the furnace temperature drop rate, it was determined that the corresponding temperature drop at this time was 405°C, which was consistent with the prediction result of the model of the present invention.
实施例2Example 2
本实施例选用TP347HFG作为测试材料，蒸汽氧化实验条件为温度：650℃，溶解氧含量：5ppm，蒸汽流速：100mL/min，蒸汽氧化时间：400小时。In this example, TP347HFG was selected as the test material, and the steam oxidation test conditions were temperature: 650°C, dissolved oxygen content: 5ppm, steam flow rate: 100mL/min, and steam oxidation time: 400 hours.
1)双层氧化膜厚度及界面缺陷观测：采用扫描及透射电子显微镜对氧化后合金表面氧化膜形貌进行观察，发现合金氧化后由内层FeCr2O4及外层Fe3O4构成，氧化膜厚度分别为18微米与30微米。界面孔洞尺寸约为140～190nm，而此时四种合金l/a值均在4～5.5范围内。将其与ANSYS关于氧化膜剥落的模型相比较，表明在这一条件下氧化膜剥落所需的临界温度约为300～350℃。1) Observation of double-layer oxide film thickness and interface defects: Scanning and transmission electron microscopy were used to observe the oxide film morphology on the surface of the alloy after oxidation, and it was found that the alloy was composed of inner layer FeCr 2 O 4 and outer layer Fe 3 O 4 after oxidation, The oxide film thicknesses are 18 microns and 30 microns respectively. The interface pore size is about 140-190nm, and the l/a values of the four alloys are all in the range of 4-5.5. Comparing it with the ANSYS model about the peeling off of the oxide film shows that the critical temperature required for the peeling off of the oxide film under this condition is about 300-350°C.
2)双层氧化膜剥落行为监测：采用声发射无损检测技术对氧化膜剥落行为进行测定，设置门槛值为30dB。结果发现在开始降温后2000秒后出现氧化膜剥落产生的声发射信号，对比炉膛温度下降速率，确定此时对应温度降幅为360℃，与本发明的模型预测结果基本吻合。2) Monitoring of the peeling behavior of the double-layer oxide film: the peeling behavior of the oxide film is measured using the acoustic emission non-destructive testing technology, and the threshold value is set to 30dB. As a result, it was found that the acoustic emission signal generated by the peeling of the oxide film appeared after 2000 seconds after the start of cooling. Comparing the furnace temperature drop rate, it was determined that the corresponding temperature drop at this time was 360°C, which was basically consistent with the model prediction results of the present invention.
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| CN104372338A (en) * | 2014-11-04 | 2015-02-25 | 西安热工研究院有限公司 | Alloying method of austenitic stainless steel tube surface for boiler superheaters/reheaters |
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| CN104372338A (en) * | 2014-11-04 | 2015-02-25 | 西安热工研究院有限公司 | Alloying method of austenitic stainless steel tube surface for boiler superheaters/reheaters |
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