CN101037763A - Method for improving high temperature resistant sulfidation corrosion property of rare earth modified MCrAlY coating - Google Patents
Method for improving high temperature resistant sulfidation corrosion property of rare earth modified MCrAlY coating Download PDFInfo
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- CN101037763A CN101037763A CNA2007100721217A CN200710072121A CN101037763A CN 101037763 A CN101037763 A CN 101037763A CN A2007100721217 A CNA2007100721217 A CN A2007100721217A CN 200710072121 A CN200710072121 A CN 200710072121A CN 101037763 A CN101037763 A CN 101037763A
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Abstract
A method for improving sulfurized corrosion resistance under high temperature by rare-earth modified MCrAlY, relates to a material modified method. The invention solves the problem that the traditional MCrAlY generally may be corroded severely when it is used under high temperature in the sulfur partial pressure of more than 0.1 Pa and oxygen partial pressure of less than 10-5 Pa. The inventive method includes the steps of: at first thermal spraying feed is produced by rare-earth metal (RE), rare-earth oxide and MCrAlY, then RE-MCrAlY coating is produced by thermal spraying the feed on the based bady material, wherein M is Ni, Co or NiCo, rare-earth is 0.1-5% of weight of the feeding, the thickness of the coating is 300-400 Mum. The inventive method is easy, and can be widely usable for commercial process. The sulfurized corrosion resistance under high temperature of MCrAlY coating can be improved to twice by adding rare-earth.
Description
Technical field
The present invention relates to a kind of method of material modification, particularly a kind of MCrAlY of raising is the method for coating high temperature resistance sulphur corrosion performance.
Background technology
As the 4th generation protective coating representative, thermal barrier coating (TBC) is one of best surface protection coating of present high temperature protection performance the best, application prospect.The compound coating that traditional TBC generally is made up of ceramic topcoats and metal transfer bottom.Wherein, ceramic topcoats is generally by ceramic oxide such as Al
2O
3, ZrO
2Deng and stablizer constitute.And the metal transfer bottom is generally MCrAlY, because MCrAlY has better resistance to high temperature corrosion performance and bonding strength (wherein M is Fe, Co, Ni or NiCo, and Working environment is depended in its selection).The TBC key operation in high temperature atmosphere or have thermal etching quiet/dynamically in the atmosphere, work under bad environment, be subject to multiple infringements such as high temperature oxidation, thermal etching, thermal shocking, fluid erosion, coating itself exists bilayer or multilayer interface in addition, interface material at opposite sides physical and chemical performance difference, failure phenomenons such as the therefore coating stress field complexity of bearing under arms, coating be prone to cracking, peel off.
People are more complicated at continuous research structure, in the time of the more perfect thermal barrier coating of function, also with the MCrAlY coating as independent coatings applications on aircraft engine and gas-engine, directly as about 1000 ℃ high temperature resistant thermal boundary work coating with as the destructive high-temperature protection coatings such as high temperature oxidation, sulphur corrosion and erosion under 800-1100 ℃ of condition of opposing.This coating can prolong the work-ing life of superalloy parts.The MCrAlY coating also can be used for many occasions: air and flue gas air door as the coal-burning power plant are just benefited from thermospray MCrAlY coating.The stainless steel baffle plate of these parts is responsive especially with corrosion for the gouging abrasion of contained high-velocity particles in air and the flue gas; For another example, blast furnace wind, the cinder notch of Steel Plant just use the plasma spraying metal-ceramic coating, comprise the MCrAlY coating, to improve anti-molten metal etch, polishing machine, increase the service life.Also have many other high-temperature components surface just can use the heat barrier ceramic coating of plasma spraying resistance to high temperature oxidation or independent MCrAlY coating as thermal barrier coating.As power station suction, exhaust blower impeller, middle small plant turbine impeller.Have, rolling various steel such as plate, pipe, rod, foreplate (wheel) etc. was cast iron or general cast steel originally again, and the non-refractory corrosion is a base material if adopt 45#, and surface spraying or surfacing MCrAlY one type high temp alloy powder just can make the life-span improve greatly.
Ni-20Cr-10Al-Y coating studies show that to high speed oxygen flame (HVOF) spraying at circulation and isothermal oxidation under 1200 ℃ of conditions: fine and close Ni-20Cr-10Al-Y coating through 1200 ℃ of cyclic oxidations and isothermal oxidation the time, can generate densification, continuously, flawless, even and adhere to good protective oxide film.The compactness of coating has determined coating to form the needed time of protective membrane in the time of 1200 ℃.In the time of 1200 ℃, the existence of water vapor can be to coating, and particularly long-time oxidation exerts an influence.
From the present documents and materials of grasping, most study limitations consider the effect of water vapour on to MCrAlY resistance to high temperature oxidation and thermal etching simultaneously.And, also must consider the influence of fuel oil composition such as metallic element Na, K, vanadium etc. and sulphur to mechanized equipments such as ground combustion machines.In combustion gas, all change into SO as sulphur
2And SO
3, they and alkali metals such as sodium, potassium are in conjunction with forming alkali metal sulfates, and this is the one of the main reasons that the combustion machine passage of heat produces high temperature corrosion, and for the unit of the use device that has surplus heat, sulfur oxide causes the corrosion of low temperature heating surface easily.Have, in the course of processing of coal gasification and crude oil, high temperature steel is usually at sulphur content pressure＞0.1Pa, oxygen partial pressure＜10 again
-5The environment of Pa uses down.The temperature of these processes is no more than 700 ℃ usually, uses traditional high temperature steel can make high temperature steel be subjected to serious corrosion usually under such environment.Especially, resembling the used thermospray MCrAlY coating of the air of our above-mentioned coal-burning power plant of enumerating and flue gas air door, the blast furnace wind of Steel Plant, the MCrAlY coating that cinder notch uses etc. just often faces high-temperature sulfidation attack and destroys.Thereby, be necessary to research and develop the new coating or the novel process of new high temperature resistance sulphur corrosion.
Summary of the invention
The present invention is in order to solve traditional MCrAlY coating at high temperature, sulphur content pressure＞0.1Pa, oxygen partial pressure＜10
-5When the environment of Pa uses down, can be subjected to serious corrosive problem usually, provide a kind of rare earth modified MCrAlY coating to improve the method for its high temperature resistance sulphur corrosion performance.The method that rare earth modified MCrAlY coating of the present invention improves its high temperature resistance sulphur corrosion performance is as follows: earlier rare earth metal (abbreviating RE as) is prepared into the thermospray feeding with MCrAlY, then with the feeding thermospray on body material, obtain the RE-MCrAlY coating, wherein M is Ni, Co or NiCo, rare earth element accounts for 0.1～5% of feeding weight, and the thickness of coating is 300～400 μ m.
Also rare earth compound or lucium and MCrAlY can be prepared into the thermospray feeding in the method for the present invention.
Rare earth compound is CeO
2, La
2O
3Or Y
2O
3, lucium is RE
2O
3
The present invention is applied to rare-earth modification technology to prepare in the kinds of surface engineering that MCrAlY is a coating, is the high temperature resistance sulphur corrosion performance of coating to improve MCrAlY.The present invention particularly is applied to rare-earth modification technology industrial widely used hot-spraying techniques and prepares the process that MCrAlY is a coating, and promptly adopting hot-spraying techniques is coating with the MCrAlY that has high temperature resistance sulphur corrosion performance through rare earth modified hot spray powder material preparation.Common rare adding rare earth can improve the high temperature resistance sulfuration ability of MCrAlY coating more than one times.This manufacturing technology is simple, as other hot-spraying techniques, can be widely used in the suitability for industrialized production.
Description of drawings
Fig. 1 is the back scattering scanning electron photomicrograph that NiCrAlY is coated with layer cross section, and Fig. 2 is the back scattering scanning electron photomicrograph that RE-NiCrAlY is coated with layer cross section, and Fig. 3 is that matrix alloy HP steel and two kinds of coating samples descend the weightening finishes of exposure after 60 hours figure as a result at 700 ℃.
Embodiment:
Embodiment one: it is as follows that present embodiment middle-weight rare earths modified MCrAlY coating improves the method steps of its high temperature resistance sulphur corrosion performance: earlier rare earth metal (abbreviating RE as) is prepared into the thermospray feeding with MCrAlY, then with the feeding thermospray on body material, obtain the RE-MCrAlY coating, wherein M is Ni, Co or NiCo, rare earth metal accounts for 0.1～5% of feeding, and the thickness of coating is 300～400 μ m.
Embodiment two: what present embodiment and concrete mode one were different is that rare earth metal is the rare earth metal of nanostructure rare earth metal or nano-scale.Other is identical with embodiment one.
The coating that the present embodiment method obtains contains nanostructure or nano-scale.
Embodiment three: present embodiment and embodiment one are different is that rare earth compound or lucium and MCrAlY are prepared into the thermospray feeding.Other is identical with embodiment one.
Embodiment four: present embodiment and concrete mode three are different is that the structure of rare earth compound or lucium is nanostructure or nano-scale.Other is identical with embodiment three.
The coating that the present embodiment method obtains contains nanostructure or nano-scale.
Embodiment five: what present embodiment was different with embodiment three and four is that rare earth compound is CeO
2, La
2O
3Or Y
2O
3Other is identical with embodiment three and four.
Embodiment six: what present embodiment was different with embodiment three and four is that lucium is RE
2O
3Other is identical with embodiment three and four.
At occurring in nature, rare earth element is always symbiotic, with RE
2O
3Meter accounts for 0.016% of the earth's crust.
Embodiment seven: present embodiment and embodiment one to six are different be rare earth element account for feeding weight 1～4%.Other is identical with embodiment one to six.
Embodiment eight: present embodiment and embodiment one to six are different be rare earth element account for feeding weight 3%.Other is identical with embodiment one to six.
Embodiment nine: present embodiment and embodiment one to six are different be Cr or Al account for MCrAlY weight 0.1～40%.Other is identical with embodiment one to six.
Embodiment ten: present embodiment and embodiment one to six are different be Cr account for MCrAlY weight 5～30%.Other is identical with embodiment one to six.
Embodiment 11: present embodiment and embodiment one to six are different be Al account for MCrAlY weight 4～35%.Other is identical with embodiment one to six.
Embodiment 12: what present embodiment and embodiment one to six were different is that heat spraying method is supersonic flame (HVOF) spraying method, plasma spraying method, subsonic speed spraying method or detonation flame spraying method.Other is identical with embodiment one to six.
Embodiment 13: what present embodiment and embodiment one to six were different is that body material is iron and steel, non-ferrous metal or non-ferrous metal alloy, wherein iron and steel is carbon steel, stainless steel or steel alloy, non-ferrous metal titanium, aluminium or nickel, the alloy of titaniferous, aluminium or nickel.Other is identical with embodiment one to six.
Embodiment 14: present embodiment and embodiment one to six are different is that the thickness of RE-MCrAlY coating is 320～380 μ m.Other is identical with embodiment one to six.
Embodiment 15: present embodiment and embodiment one to six are different is that the thickness of RE-MCrAlY coating is 340～360 μ m.Other is identical with embodiment one to six.
Embodiment 16: present embodiment and embodiment one to six are different is that the thickness of RE-MCrAlY coating is 350 μ m.Other is identical with embodiment one to six.
By following representative example the present invention is described further again.This patent is not subjected to the restriction of following given example.
The rare earth oxide CeO of commercial NiCrAlY spray material 9.9kg of weighing and 0.1kg
2, mix powder with NiCrAlY and CeO by ball milling
2Two kinds of powders mix, but thereby prepare rare earth modified NiCrAlY thermospray feeding (Ce-NiCrAlY), on matrix alloy HP steel, obtain NiCrAlY coating and rare earth modified NiCrAlY coating (Ce-NiCrAlY coating) by the HVOF thermal spraying apparatus then.
Check to sample is that matrix alloy HP steel and two kinds of coatings (NiCrAlY and Ce-NiCrAlY) sample are placed on the vitrified pipe central authorities that are in controlled atmosphere tube furnace burner hearth, by tubular furnace the sample in the vitrified pipe is heated and vulcanizes test.The sulfuration test is carried out in 700 ℃ mixed gas, and this mixed gas comprises the H of 1.0% (volume fraction)
2S, the H of 0.1% (volume fraction)
2, add the O of 5ppm
2, remaining comes balance by argon gas.Mixture velocity should remain on 1000～2000mm
3S
-1, the corresponding equilibrium partial pressure of sulphur and oxygen is respectively 1 and 10
-19Pa.By precision is 10
-5The changes in weight of sample after the microbalance experiment with measuring of g.Fig. 2 shows matrix alloy HP steel and two kinds of coating sample weightening finish results after exposing 60 hours under 700 ℃.As seen from Figure 2: the high temperature resistance sulphur corrosion performance of NiCrAlY coating is 7.65 times of matrix alloy HP steel, add rare earth cerium oxide and can make the high temperature resistance sulphur corrosion performance of NiCrAlY coating improve 1.34 times in coating, the high temperature resistance sulphur corrosion performance that promptly contains the NiCrAlY coating of rare earth cerium oxide is 19.26 times of matrix alloy HP steel.
Sulfuration test shows, matrix alloy HP steel and have or not two kinds of rare earth modified MCrAlY be the coating sample under 700 ℃ of temperature, with interior corrosion kinetics curve and Fe-Al alloy phase seemingly the weightening finish variation was three different stages in time in 100 hours.Starting stage (beginning 20 hours): along with the prolongation of exposure duration, weightening finish slowly increases; Transitory stage (20～40 hours): the weightening finish meeting increases sharply with the prolongation of exposure duration; Steady-state process (after 40 hours): weightening finish is stablized increase with the prolongation of exposure duration, and with proportional variation of exposure duration, this stage has parabolical character.
Shown in Figure 1 is 700 ℃ of back scattering SEM photos that expose resulting two kinds of different coating sample sections after 60 hours.Table 1 (the EDX result of NiCrAlY coating) and table 2 (the EDX result of RE-NiCrAlY coating) have been listed the corrosion product that these two kinds of coatings record by EDS and the composition of coated substrate respectively.Can infer according to the result of EDX result and XRD and their calorifics stability and the main corrosion product that may exist.As shown in Figure 1, can form the multilayer corrosion product after exposing 60 hours under 700 ℃, the top layer dirt settling mainly is the sulfide of Ni, and the internal layer dirt settling mainly is that the sulfide of Cr is formed.XRD analysis shows that they are respectively NiS and Cr
2S
3Phase.Innermost layer corrosion product near coated substrate is (Ni, Cr, Al) sulfide.
Table 1
| Indicate | Ni | Al | S | Cr | Y |
| 1 | 36.29 | 46.72 | 16.60 | ||
| 2 | 7.19 | 8.02 | 53.03 | 31.76 | |
| 3 | 6.28 | 11.66 | 53.33 | 29.96 | |
| 4 | 62.62 | 12.63 | 24.13 | 0.62 |
Table 2
| Indicate | Ni | Al | S | Cr | Y |
| 1 | 33.77 | 51.26 | 14.66 | ||
| 2 | 9.71 | 7.52 | 52.96 | 29.80 | |
| 3 | 6.57 | 11.45 | 53.32 | 28.22 | |
| 4 | 65.49 | 22.61 | 4.28 | 7.62 | |
| 5 | 58.23 | 18.87 | 22.41 | 0.47 |
Draw through above-mentioned analysis: corrosion stage difference, corrosion mechanism is also different: the starting stage, the sulfuration of portion C r has suppressed the formation of other sulfide, thereby makes that weightening finish is less; Transitory stage because the decomposition of the sulfide of Cr and the deficiency of Cr concentration make the sulfide of Ni be able to quick formation, thereby causes the quick increase of weight; Steady-state process, positively charged ion and anionic solid-state diffusion are controlling mechanisms, kinetics is followed the para-curve proportionality principle.The adding of rare earth also fails to change the feature in different corrosion stages, but can reduce erosion rate, so significantly suppressed the increase of weight.Usually, the adding of rare earth can make weightening finish reduce more than one times.That is to say, add rare earth and can improve the high temperature resistance sulfuration ability of coating more than one times.
Claims (10)
1, a kind of rare earth modified MCrAlY coating improves the method for its high temperature resistance sulphur corrosion performance, the step that it is characterized in that this method is as follows: earlier rare earth metal and MCrAlY are prepared into the thermospray feeding, then with the feeding thermospray on body material, obtain the RE-MCrAlY coating, wherein M is Ni, Co or NiCo, rare earth element accounts for 0.1～5% of feeding weight, and the thickness of coating is 300～400 μ m.
2, rare earth modified MCrAlY coating according to claim 1 improves the method for its high temperature resistance sulphur corrosion performance, it is characterized in that rare earth metal is the rare earth metal of nanostructure rare earth metal or nano-scale.
3, rare earth modified MCrAlY coating according to claim 1 improves the method for its high temperature resistance sulphur corrosion performance, it is characterized in that rare earth compound or lucium and MCrAlY are prepared into the thermospray feeding, and wherein rare earth compound is CeO
2, La
2O
3Or Y
2O
3, lucium is RE
2O
3
4, rare earth modified MCrAlY coating according to claim 3 improves the method for its high temperature resistance sulphur corrosion performance, and the structure that it is characterized in that rare earth compound or lucium is nanostructure or nano-scale.
5, improve the method for its high temperature resistance sulphur corrosion performance according to claim 1 or 3 described rare earth modified MCrAlY coatings, it is characterized in that rare earth element accounts for 1～4% of feeding weight.
6, improve the method for its high temperature resistance sulphur corrosion performance according to claim 1 or 3 described rare earth modified MCrAlY coatings, it is characterized in that Cr or Al account for 0.1～40% of MCrAlY weight.
7, improve the method for its high temperature resistance sulphur corrosion performance according to claim 1 or 3 described rare earth modified MCrAlY coatings, it is characterized in that heat spraying method is supersonic flame spraying method, plasma spraying method, subsonic speed spraying method or detonation flame spraying method.
8, improve the method for its high temperature resistance sulphur corrosion performance according to claim 1 or 3 described rare earth modified MCrAlY coatings, it is characterized in that body material is iron and steel, non-ferrous metal or non-ferrous metal alloy, wherein iron and steel is carbon steel, stainless steel or steel alloy, non-ferrous metal is titanium, aluminium or nickel, and non-ferrous metal alloy is the alloy of titaniferous, aluminium or nickel.
9, improve the method for its high temperature resistance sulphur corrosion performance according to claim 1 or 3 described rare earth modified MCrAlY coatings, the thickness that it is characterized in that the RE-MCrAlY coating is 320～380 μ m.
10, improve the method for its high temperature resistance sulphur corrosion performance according to claim 1 or 3 described rare earth modified MCrAlY coatings, the thickness that it is characterized in that the RE-MCrAlY coating is 350 μ m.
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103196200A (en) * | 2013-04-02 | 2013-07-10 | 江苏瑞丰科技实业有限公司 | Integrated processing system for fire safety and air purification |
| CN103205607A (en) * | 2012-01-17 | 2013-07-17 | 中航商用航空发动机有限责任公司 | Anti-cavitation coating material, and high-speed fuel oil centrifugal pump with anti-cavitation coating |
| CN105861972A (en) * | 2016-04-15 | 2016-08-17 | 航天材料及工艺研究所 | Chromic oxide-titanium oxide based high-temperature and high-emissivity coating and preparation method thereof |
| CN108754386A (en) * | 2018-07-27 | 2018-11-06 | 北方工业大学 | Thermal shock resistant MCrAlY coating and preparation method thereof |
| CN110527942A (en) * | 2019-09-18 | 2019-12-03 | 西安交通大学 | A kind of high-temperature wearable damage oxidation susceptibility coating production |
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2007
- 2007-04-27 CN CN200710072121A patent/CN100577852C/en not_active Expired - Fee Related
Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103205607A (en) * | 2012-01-17 | 2013-07-17 | 中航商用航空发动机有限责任公司 | Anti-cavitation coating material, and high-speed fuel oil centrifugal pump with anti-cavitation coating |
| CN103205607B (en) * | 2012-01-17 | 2016-04-13 | 中航商用航空发动机有限责任公司 | Cavitation coating material and there is the high-speed fuel oil centrifugal pump of cavitation coating |
| CN103196200A (en) * | 2013-04-02 | 2013-07-10 | 江苏瑞丰科技实业有限公司 | Integrated processing system for fire safety and air purification |
| CN103196200B (en) * | 2013-04-02 | 2016-01-20 | 江苏瑞丰科技实业有限公司 | Security against fire and purification of air integral type treatment system |
| CN105861972A (en) * | 2016-04-15 | 2016-08-17 | 航天材料及工艺研究所 | Chromic oxide-titanium oxide based high-temperature and high-emissivity coating and preparation method thereof |
| CN108754386A (en) * | 2018-07-27 | 2018-11-06 | 北方工业大学 | Thermal shock resistant MCrAlY coating and preparation method thereof |
| CN110527942A (en) * | 2019-09-18 | 2019-12-03 | 西安交通大学 | A kind of high-temperature wearable damage oxidation susceptibility coating production |
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| CN100577852C (en) | 2010-01-06 |
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