电弧复合磁控溅射结合热退火制备Ti_2AlC涂层
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摘要
利用电弧复合磁控溅射技术制备不同Ti/Al比的Ti-Al-C涂层,结合后续的退火处理制备Ti_2AlC相涂层。利用SEM、EDS、XRD、Raman光谱仪和TEM等研究了Ti/Al比及退火温度对退火后Ti-Al-C涂层的相和微观结构的影响。结果表明,Ti-Al-C沉积态涂层为富Al层和TiCx层交替堆垛的多层结构,涂层表面大颗粒较少且结构致密。Ti/Al比对退火后涂层中的相结构有重要的影响:当Ti/Al比为2.04时,退火后涂层中Ti_2AlC的纯度和结晶度最高;Ti/Al比过高(3.06)时,退火后涂层中形成TiC和Ti_3AlC杂质相,而低Ti/Al比(0.54)则大幅度降低Ti_2AlC相的纯度和结晶度。同时,退火温度很大程度影响Ti_2AlC相的形成,当沉积态涂层中Ti/Al比为2.38时,Ti_2AlC相涂层形成的最佳退火温度为750℃,偏低的退火温度(600℃)下,原子不能充分扩散,难以形成211结构的Ti_2AlC相,而退火温度过高时(900℃)涂层中存在较多的TiC、TiAlx等杂质相。
Nuclear power generation provides a reliable and economic supply of electricity, due to low carbon emissions and relatively few waste. However, the reaction between zirconium and steam at high temperature is accompanied by the release of large amounts of hydrogen gas, which will bring serious consequences. After the Fukushima nuclear accident, the concept of accident-tolerant fuels(ATF)has been proposed and widely investigated. In terms of nuclear claddings, one key requirement is reduced oxidation kinetics with high-temperature steam and hence significantly reduced heat and hydrogen generation. An economical and simple method could be the preparation of protective coatings on the surface of zirconium alloys to improve the oxidation resistance. The MAX phase has been considered to be one of the most promising coating materials for nuclear cladding coatings. In this work, Ti-Al-C coatings with different Ti/Al ratios have been deposited on Zirlo alloy using a hybrid arc/magnetron sputtering method, and the Ti_2AlC coatings were obtained by post-annealing. The effects of Ti/Al ratios and annealing temperatures on the phase and microstructure of Ti-Al-C coatings after annealing were studied by SEM,EDS, XRD, Raman spectrometer and TEM. It is found that Ti-Al-C coatings with different Ti/Al ratios deposited by the hybrid cathode arc/magnetron sputtering are a multi-layer structure of an alternative Al-rich layer and TiCxlayer. The as-deposited coatings are compact with a small amount of large particles. The Ti/Al ratio has an important influence on the phase structure of the annealed coating. When the Ti/Al ratio is 2.04, the highest purity and crystallinity of Ti_2AlC are obtained. TiC and Ti3 AlC impurities will form within the coating at a higher Ti/Al ratio(3.06), while the purity and crystallinity of Ti_2AlC will decrease at a lower Ti/Al ratio(0.54). In addition, the annealing temperature affects the formation of Ti_2AlC to a great extent.When the Ti/Al ratio is 2.38, the optimum temperature for Ti-Al-C coatings to Ti_2AlC coatings is at 750 ℃.The atom cannot diffuse fully at a lower annealing temperature(600 ℃), which is difficult to form the Ti_2AlC phase, while a higher annealing temperature(900 ℃) will enable the formation of Ti_2AlC coatings with more TiC, TiAlxand other impurities.
Nuclear power generation provides a reliable and economic supply of electricity, due to low carbon emissions and relatively few waste. However, the reaction between zirconium and steam at high temperature is accompanied by the release of large amounts of hydrogen gas, which will bring serious consequences. After the Fukushima nuclear accident, the concept of accident-tolerant fuels(ATF)has been proposed and widely investigated. In terms of nuclear claddings, one key requirement is reduced oxidation kinetics with high-temperature steam and hence significantly reduced heat and hydrogen generation. An economical and simple method could be the preparation of protective coatings on the surface of zirconium alloys to improve the oxidation resistance. The MAX phase has been considered to be one of the most promising coating materials for nuclear cladding coatings. In this work, Ti-Al-C coatings with different Ti/Al ratios have been deposited on Zirlo alloy using a hybrid arc/magnetron sputtering method, and the Ti_2AlC coatings were obtained by post-annealing. The effects of Ti/Al ratios and annealing temperatures on the phase and microstructure of Ti-Al-C coatings after annealing were studied by SEM,EDS, XRD, Raman spectrometer and TEM. It is found that Ti-Al-C coatings with different Ti/Al ratios deposited by the hybrid cathode arc/magnetron sputtering are a multi-layer structure of an alternative Al-rich layer and TiCxlayer. The as-deposited coatings are compact with a small amount of large particles. The Ti/Al ratio has an important influence on the phase structure of the annealed coating. When the Ti/Al ratio is 2.04, the highest purity and crystallinity of Ti_2AlC are obtained. TiC and Ti3 AlC impurities will form within the coating at a higher Ti/Al ratio(3.06), while the purity and crystallinity of Ti_2AlC will decrease at a lower Ti/Al ratio(0.54). In addition, the annealing temperature affects the formation of Ti_2AlC to a great extent.When the Ti/Al ratio is 2.38, the optimum temperature for Ti-Al-C coatings to Ti_2AlC coatings is at 750 ℃.The atom cannot diffuse fully at a lower annealing temperature(600 ℃), which is difficult to form the Ti_2AlC phase, while a higher annealing temperature(900 ℃) will enable the formation of Ti_2AlC coatings with more TiC, TiAlxand other impurities.
引文
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[2]Eklund P,Beckers M,Jansson U,et al.The Mn+1AXnphases:Materials science and thin-film processing[J].Thin Solid Films,2010,518:1851
[3]Yang H Y,Zhang R Q,Peng X M,et al.Research progress regarding surface coating of zirconium alloy cladding[J].Surf.Technol.,2017,46(1):69(杨红艳,张瑞谦,彭小明等.锆合金包壳表面涂层研究进展[J].表面技术,2017,46(1):69)
[4]Yueh K,Terrani K A.Silicon carbide composite for light water reactor fuel assembly applications[J].J.Nucl.Mater.,2014,448:380
[5]Terrani K A,Zinkle S J,Snead L L.Advanced oxidation-resistant iron-based alloys for LWR fuel cladding[J].J.Nucl.Mater.,2014,448:420
[6]Luo K,Zha X H,Huang Q,et al.Theoretical investigations on helium trapping in the Zr/Ti2AlC interface[J].Surf.Coat.Technol.,2017,322:19
[7]Basu S,Obando N,Gowdy A,et al.Long-term oxidation of Ti2AlC in air and water vapor at 1000-1300℃temperature range[J].J.Electrochem.Soc.,2012,159:C90
[8]Li S B,Song G M,Kwakernaak K,et al.Multiple crack healing of a Ti2AlC ceramic[J].J.Eur.Ceram.Soc.,2012,32:1813
[9]Maier B R,Garcia-Diaz B L,Hauch B,et al.Cold spray deposition of Ti2AlC coatings for improved nuclear fuel cladding[J].J.Nucl.Mater.,2015,466:712
[10]Frodelius J,Eklund P,Beckers M,et al.Sputter deposition from a Ti2AlC target:Process characterization and conditions for growth of Ti2AlC[J].Thin Solid Films,2010,518:1621
[11]Feng Z J,Ke P L,Wang A Y.Preparation of Ti2AlC MAX phase coating by DC magnetron sputtering deposition and vacuum heat treatment[J].J.Mater.Sci.Technol.,2015,31:1193
[12]Feng Z J,Ke P L,Huang Q,et al.The scaling behavior and mechanism of Ti2AlC MAX phase coatings in air and pure water vapor[J].Surf.Coat.Technol.,2015,272:380
[13]Fu J J,Zhang T F,Xia Q X,et al.Oxidation and corrosion behavior of nanolaminated MAX-phase Ti2AlC film synthesized by highpower impulse magnetron sputtering and annealing[J].J.Nanomater.,2015,2015:213128
[14]Yeom H,Hauch B,Cao G P,et al.Laser surface annealing and characterization of Ti2AlC plasma vapor deposition coating on zirconium-alloy substrate[J].Thin Solid Films,2016,615:202
[15]Tang C,Klimenkov M,Jaentsch U,et al.Synthesis and characterization of Ti2AlC coatings by magnetron sputtering from three elemental targets and ex-situ annealing[J].Surf.Coat.Technol.,2017,309:445
[16]Guenette M C,Tucker M D,Ionescu M,et al.Cathodic arc codeposition of highly oriented hexagonal Ti and Ti2AlC MAX phase thin film[J].Thin Solid Films,2010,519:766
[17]Rosén J,Ryves L,PerssonP O?,et al.Deposition of epitaxial Ti2AlC thin films by pulsed cathodic arc[J].J.Appl.Phys.,2007,101:056101
[18]Shu R,Ge F F,Meng F P,et al.One-step synthesis of polycrystalline V2AlC thin films on amorphous substrates by magnetron cosputtering[J].Vacuum,2017,146:106
[19]Wang J Y,Zhou Y C,Liao T,et al.A first-principles investigation of the phase stability of Ti2AlC with Al vacancies[J].Scr.Mater.,2008,58:227
[20]Li J J,Hu L F,Li F Z,et al.Variation of microstructure and composition of the Cr2AlC coating prepared by sputtering at 370℃and500℃[J].Surf.Coat.Technol.,2010,204:3838
[21]Su R R,Zhang H L,O'Connor D J,et al.Deposition and characterization of Ti2AlC MAX phase and Ti3AlC thin films by magnetron sputtering[J].Mater.Lett.,2016,179:194
[22]Liu J Z,Zuo X,Wang Z Y,et al.Fabrication and mechanical properties of high purity of Cr2Al Ccoatings by adjustable Al contents[J].J.Alloys Compd.,2018,753:11
[23]Li Y M,Zhao G R,Qian Y H,et al.Deposition and characterization of phase-pure Ti2AlC and Ti3AlC2coatings by DC magnetron sputtering with cost-effective targets[J].Vacuum,2018,153:62
[24]Wang Z Y,Liu J Z,Wang L,et al.Dense and high-stability Ti2AlNMAX phase coatings prepared by the combined cathodic arc/sputter technique[J].Appl.Surf.Sci.,2017,396:1435
[25]Low I M,Pang W K,Kennedy S J,et al.High-temperature thermal stability of Ti2AlN and Ti4AlN3:A comparative diffraction study[J].J.Eur.Ceram.Soc.,2011,31:159
[26]Wilhelmsson O,Palmquist J P,Nyberg T,et al.Deposition of Ti2AlC and Ti3AlC2epitaxial films by magnetron sputtering[J].Appl.Phys.Lett.,2004,85:1066
[27]Li J J,Qian Y H,Niu D,et al.Phase formation and microstructure evolution of arc ion deposited Cr2AlC coating after heat treatment[J].Appl.Surf.Sci.,2012,263:457
[28]Miernik K,Walkowicz J.Spatial distribution of microdroplets generated in the cathode spots of vacuum arcs[J].Surf.Coat.Technol.,2000,125:161
[29]Bandyopadhyay D,Sharma R C,Chakraborti N.The Ti-Al-C system(titanium-aluminum-carbon)[J].J.Phase Equilib.,2000,21:195
[30]Presser V,Naguib M,Chaput L,et al.First-order Raman scattering of the MAX phases:Ti2AlN,Ti2AlC0.5N0.5,Ti2AlC,(Ti0.5V0.5)2AlC,V2AlC,Ti3AlC2,and Ti3GeC2[J].J.Raman Spectro.,2012,43:168
[31]Hakamada M,Nakamoto Y,Matsumoto H,et al.Relationship between hardness and grain size in electrodeposited copper films[J].Mater.Sci.Eng.,2007,A457:120
[32]Tang C C,Steinbrueck M,Stueber M,et al.Deposition,characterization and high-temperature steam oxidation behavior of singlephase Ti2AlC-coated Zircaloy-4[J].Corros.Sci.,2018,135:87
[33]Wang J M,Wang J Y,Zhou Y C.Stable M2AlC(0001)surfaces(M=Ti,V and Cr)by first-principles investigation[J].J.Phys.:Condens Matter,2008,20:225006