Al和Mo对难熔高熵合金高温氧化行为的影响（英文）
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摘要
难熔高熵合金在高温下具有优异的力学性能,其高温氧化行为非常重要。本文作者研究Ti NbT a_(0.5)Zr、Ti NbT a_(0.5)ZrA l及Ti Nb Ta_(0.5)ZrA l Mo_(0.5)3种合金的高温氧化行为,并讨论合金元素的影响。研究结果表明,Ti NbT a_(0.5)Zr及Ti NbT a_(0.5)ZrA l合金的氧化速率受扩散控制,符合指数型氧化规律。但Ti Nb Ta_(0.5)ZrA l Mo_(0.5)合金的氧化速率受界面反应控制,符合直线型氧化规律。添加Al可形成氧化保护膜从而提高合金的抗氧化性能;然而,添加Mo会破坏富Al保护膜。Ti NbT a_(0.5)ZrA l Mo_(0.5)合金的氧化膜中出现大量的孔洞和裂纹,导致其抗氧化性能明显下降。
Refractory high entropy alloys have superior mechanical properties at high temperatures, and the oxidation behavior of these alloys is very important. The present work investigated the high temperature oxidation behavior of three alloys with compositions of Ti Nb Ta_(0.5)Zr, Ti Nb Ta_(0.5)Zr Al and Ti Nb Ta_(0.5)Zr Al Mo0.5, and the effects of alloying elements were discussed. Results indicated that the oxidation rates of the Ti Nb Ta_(0.5)Zr and Ti Nb Ta_(0.5)Zr Al alloys are controlled by diffusion, and obey the exponential rule. However, the oxidation rate of the Ti Nb Ta_(0.5)Zr Al Mo_(0.5)alloy is controlled by interface reaction, and obeys the linear rule. The addition of Al leads to a better oxidation resistance by forming a protective oxide scale. However, the protection of Al-rich scale is weakened by the addition of Mo. Extensive pores and cracks occur in the oxide scale of the Ti Nb Ta_(0.5)Zr Al Mo_(0.5)alloy, resulting in a significant decrease in oxidation resistance.
Refractory high entropy alloys have superior mechanical properties at high temperatures, and the oxidation behavior of these alloys is very important. The present work investigated the high temperature oxidation behavior of three alloys with compositions of Ti Nb Ta_(0.5)Zr, Ti Nb Ta_(0.5)Zr Al and Ti Nb Ta_(0.5)Zr Al Mo0.5, and the effects of alloying elements were discussed. Results indicated that the oxidation rates of the Ti Nb Ta_(0.5)Zr and Ti Nb Ta_(0.5)Zr Al alloys are controlled by diffusion, and obey the exponential rule. However, the oxidation rate of the Ti Nb Ta_(0.5)Zr Al Mo_(0.5)alloy is controlled by interface reaction, and obeys the linear rule. The addition of Al leads to a better oxidation resistance by forming a protective oxide scale. However, the protection of Al-rich scale is weakened by the addition of Mo. Extensive pores and cracks occur in the oxide scale of the Ti Nb Ta_(0.5)Zr Al Mo_(0.5)alloy, resulting in a significant decrease in oxidation resistance.
引文
[1] SENKOV O N, WILKS G B, MIRACLE D B, CHUANG C P, LIAW P K. Refractory high-entropy alloys[J]. Intermetallics, 2010, 18:1758-1765.
[2] SENKOV O N, SCOTT J M, SENKOVA S V, MIRACLE D B,WOODWARD C F. Microstructure and room temperature properties of a high-entropy Ta Nb Hf Zr Ti alloy[J]. Journal of Alloys and Compounds, 2011, 509:6043-6048.
[3] MICHAEL C G, YEH J W, LIAW P K, ZHANG Y. High-entropy alloys:Fundamentals and applications[M]. Heidlburg:Springer,2016.
[4] TODA C I, RIVERA D P. Modelling solid solution hardening in high entropy alloys[J]. Acta Materialia, 2015, 85:14-23.
[5] GORSSE S, MIRACLE D B, SENKOV O N. Mapping the world of complex concentrated alloys[J]. Acta Materialia, 2017, 135:177-187.
[6] LIN C M, JUAN C C, CHANG C H, TSAI C W, YEH J W. Effect of Al addition on mechanical properties and microstructure of refractory Alx Hf Nb Ta Ti Zr alloys[J]. Journal of Alloys and Compounds, 2015,624:100-107.
[7] HAN Z D, CHEN N, ZHAO S F, FAN L W, YANG G N, SHAO Y,YAO K F. Effect of Ti additions on mechanical properties of Nb Mo Ta W and VNb Mo Ta W refractory high entropy alloys[J].Intermetallics, 2017, 84:153-157.
[8] FAZAKASé, ZADOROZHNYY V, VARGA L K, INOUE A,LOUZGUINE L D, TIAN F, VITOS L. Experimental and theoretical study of Ti20Zr20Hf20Nb20X20(X=V or Cr)refractory high-entropy alloys[J]. International Journal of Refractory Metals and Hard Materials, 2014, 47:131-138.
[9] SENKOV O N, WILKS G B, SCOTT J M, MIRACLE D B.Mechanical properties of Nb25Mo25Ta25W25 and V20Nb20Mo20Ta20-W20 refractory high entropy alloys[J]. Intermetallics, 2011, 19:698-706.
[10] FENG Rui, MICHAEL C G, CHANHO L, MICHAEL M, ZUO Ting-ting, CHEN Shu-ying, HAWK J, ZHANG Yong, LIAW P.Design of light-weight high-entropy alloys[J]. Entropy, 2016, 18:1-21.
[11] SENKOV O N, SENKOVA S V, WOODWARD C. Effect of aluminum on the microstructure and properties of two refractory high-entropy alloys[J]. Acta Materialia, 2014, 68:214-228.
[12] SENKOV O N, SENKOVA S V, DIMIDUK D M, WOODWARD C,MIRACLE D B. Oxidation behavior of a refractory Nb Cr Mo0.5Ta0.5-Ti Zr alloy[J]. Journal of Materials Science, 2012, 47:6522-6534.
[13] KOFSTAD P. High-temperature oxidation of titanium[J]. Journal of the Less-Common Metals, 1967, 12:449-464.
[14] JIANG H W, MA W, FENG X, DONG Z, ZHANG L, LIU Y. Effects of Nb and Si on high temperature oxidation of Ti Al[J]. Transactions of Nonferrous Metals Society of China, 2008, 18:512-517.
[15] YU H, UKAI S, HAYASHI S, OONO N. Effect of Al content on the high-temperature oxidation of Co-20Cr-(5,10)Al oxide dispersion strengthened superalloys[J]. Corrosion Science, 2017, 118:49-59.
[16] HAN Bao-hong, MA Yue, PENG Hui, ZHENG Lei, GUO Hong-bo.Effect of Mo, Ta, and Re on high-temperature oxidation behavior of minor Hf dopedβ-Ni Al alloy[J]. Corrosion Science, 2016, 102:222-232.
[17] KARAHAN T, OUYANG Gao-yuan, RAY P K, KRAMER M J,AKINC M. Oxidation mechanism of W substituted Mo-Si-B alloys[J]. Intermetallics, 2017, 87:38-44.
[18] BUTLER T M, CHAPUT K J, DIETRICH J R, SENKOV O N. High temperature oxidation behaviors of equimolar Nb Ti Zr V and Nb Ti Zr Cr refractory complex concentrated alloys(RCCAs)[J].Journal of Alloys and Compounds, 2017, 729:1004-1019.
[19] CHEN H, KAUFFMANN A, GORR B, SCHLIEPHAKE D,SEEMüLLER C, WAGNER J N, CHRIST S J, HEILMAIER M.Microstructure and mechanical properties at elevated temperatures of a new Al-containing refractory high-entropy alloy Nb-Mo-CrTi-Al[J]. Journal of Alloys and Compounds, 2016, 661:206-215.
[20] DIRRAS G, COUQUE H, LILENSTEN L, HECZEL A, TINGAUD D, COUZINIéJ P, PERRIèRE L, GUBICZA J, GUILLOT I.Mechanical behavior and microstructure of Ti20Hf20Zr20Ta20Nb20high-entropy alloy loaded under quasi-static and dynamic compression conditions[J]. Materials Characterization, 2016, 111:106-113.
[21] OSTROVSKAYA O, BADINI C, BAUDANA G, PADOVANO E,BIAMINO S. Thermogravimetric investigation on oxidation kinetics of complex Ti-Al alloys[J]. Intermetallics, 2018, 93:244-250.
[22] GORR B, MULLER F, AZIM M, CHRIST H J, MULLER T, CHEN H, KAUFFMANN A, HEILMAIER M. High-temperature oxidation behavior of refractory high-entropy alloys:Effect of alloy composition[J]. Oxidation of Metals, 2017, 88:339-349.
[23] PROFF C, ABOLHASSANI S, LEMAIGNAN C. Oxidation behaviour of zirconium alloys and their precipitates—A mechanistic study[J]. Journal of Nuclear Materials, 2013, 432:222-238.
[24] LI Ya-li, MORRAL J E. A local equilibrium model for internal oxidation[J]. Acta Materialia, 2002, 50:3683-3691.
[25] REDDY A, HOVIS D B, HEUER A H, PAULIKAS A P, VEAL B W.In situ study of oxidation-induced growth strains in a model Ni Cr Al Y bond-coat alloy[J]. Oxidation of Metals, 2007, 67:153-177.
[26] XU J L, LIU F, WANG F P, YU D Z, ZHAO L C. The corrosion resistance behavior of Al2O3 coating prepared on Ni Ti alloy by micro-arc oxidation[J]. Journal of Alloys and Compounds, 2009, 472:276-280.
[27] SUSHKO M L, ALEXANDROV V, SCHREIBER D K, ROSSO K M, BRUEMMER S M. Multiscale model of metal alloy oxidation at grain boundaries[J]. Journal of Chemical Physics, 2015, 142:1-8.
[28] GORR B, MUELLER F, CHRIST H J, MUELLER T, CHEN H,KAUFFMANN A, HEILMAIER M. High temperature oxidation behavior of an equimolar refractory metal-based alloy 20Nb-20Mo-20Cr-20Ti-20Al with and without Si addition[J]. Journal of Alloys and Compounds, 2016, 688:468-477.
[29] SUPATARAWANICH V, JOHNSON D R, LIU C T. Effects of microstructure on the oxidation behavior of multiphase Mo-Si-B alloys[J]. Materials Science and Engineering A, 2003, 344:328-339.
[30] GENG J, TSAKIROPOULOS P. A study of the microstructures and oxidation of Nb-Si-Cr-Al-Mo in situ composites alloyed with Ti,Hf and Sn[J]. Intermetallics, 2007, 15:382-395.
[2] SENKOV O N, SCOTT J M, SENKOVA S V, MIRACLE D B,WOODWARD C F. Microstructure and room temperature properties of a high-entropy Ta Nb Hf Zr Ti alloy[J]. Journal of Alloys and Compounds, 2011, 509:6043-6048.
[3] MICHAEL C G, YEH J W, LIAW P K, ZHANG Y. High-entropy alloys:Fundamentals and applications[M]. Heidlburg:Springer,2016.
[4] TODA C I, RIVERA D P. Modelling solid solution hardening in high entropy alloys[J]. Acta Materialia, 2015, 85:14-23.
[5] GORSSE S, MIRACLE D B, SENKOV O N. Mapping the world of complex concentrated alloys[J]. Acta Materialia, 2017, 135:177-187.
[6] LIN C M, JUAN C C, CHANG C H, TSAI C W, YEH J W. Effect of Al addition on mechanical properties and microstructure of refractory Alx Hf Nb Ta Ti Zr alloys[J]. Journal of Alloys and Compounds, 2015,624:100-107.
[7] HAN Z D, CHEN N, ZHAO S F, FAN L W, YANG G N, SHAO Y,YAO K F. Effect of Ti additions on mechanical properties of Nb Mo Ta W and VNb Mo Ta W refractory high entropy alloys[J].Intermetallics, 2017, 84:153-157.
[8] FAZAKASé, ZADOROZHNYY V, VARGA L K, INOUE A,LOUZGUINE L D, TIAN F, VITOS L. Experimental and theoretical study of Ti20Zr20Hf20Nb20X20(X=V or Cr)refractory high-entropy alloys[J]. International Journal of Refractory Metals and Hard Materials, 2014, 47:131-138.
[9] SENKOV O N, WILKS G B, SCOTT J M, MIRACLE D B.Mechanical properties of Nb25Mo25Ta25W25 and V20Nb20Mo20Ta20-W20 refractory high entropy alloys[J]. Intermetallics, 2011, 19:698-706.
[10] FENG Rui, MICHAEL C G, CHANHO L, MICHAEL M, ZUO Ting-ting, CHEN Shu-ying, HAWK J, ZHANG Yong, LIAW P.Design of light-weight high-entropy alloys[J]. Entropy, 2016, 18:1-21.
[11] SENKOV O N, SENKOVA S V, WOODWARD C. Effect of aluminum on the microstructure and properties of two refractory high-entropy alloys[J]. Acta Materialia, 2014, 68:214-228.
[12] SENKOV O N, SENKOVA S V, DIMIDUK D M, WOODWARD C,MIRACLE D B. Oxidation behavior of a refractory Nb Cr Mo0.5Ta0.5-Ti Zr alloy[J]. Journal of Materials Science, 2012, 47:6522-6534.
[13] KOFSTAD P. High-temperature oxidation of titanium[J]. Journal of the Less-Common Metals, 1967, 12:449-464.
[14] JIANG H W, MA W, FENG X, DONG Z, ZHANG L, LIU Y. Effects of Nb and Si on high temperature oxidation of Ti Al[J]. Transactions of Nonferrous Metals Society of China, 2008, 18:512-517.
[15] YU H, UKAI S, HAYASHI S, OONO N. Effect of Al content on the high-temperature oxidation of Co-20Cr-(5,10)Al oxide dispersion strengthened superalloys[J]. Corrosion Science, 2017, 118:49-59.
[16] HAN Bao-hong, MA Yue, PENG Hui, ZHENG Lei, GUO Hong-bo.Effect of Mo, Ta, and Re on high-temperature oxidation behavior of minor Hf dopedβ-Ni Al alloy[J]. Corrosion Science, 2016, 102:222-232.
[17] KARAHAN T, OUYANG Gao-yuan, RAY P K, KRAMER M J,AKINC M. Oxidation mechanism of W substituted Mo-Si-B alloys[J]. Intermetallics, 2017, 87:38-44.
[18] BUTLER T M, CHAPUT K J, DIETRICH J R, SENKOV O N. High temperature oxidation behaviors of equimolar Nb Ti Zr V and Nb Ti Zr Cr refractory complex concentrated alloys(RCCAs)[J].Journal of Alloys and Compounds, 2017, 729:1004-1019.
[19] CHEN H, KAUFFMANN A, GORR B, SCHLIEPHAKE D,SEEMüLLER C, WAGNER J N, CHRIST S J, HEILMAIER M.Microstructure and mechanical properties at elevated temperatures of a new Al-containing refractory high-entropy alloy Nb-Mo-CrTi-Al[J]. Journal of Alloys and Compounds, 2016, 661:206-215.
[20] DIRRAS G, COUQUE H, LILENSTEN L, HECZEL A, TINGAUD D, COUZINIéJ P, PERRIèRE L, GUBICZA J, GUILLOT I.Mechanical behavior and microstructure of Ti20Hf20Zr20Ta20Nb20high-entropy alloy loaded under quasi-static and dynamic compression conditions[J]. Materials Characterization, 2016, 111:106-113.
[21] OSTROVSKAYA O, BADINI C, BAUDANA G, PADOVANO E,BIAMINO S. Thermogravimetric investigation on oxidation kinetics of complex Ti-Al alloys[J]. Intermetallics, 2018, 93:244-250.
[22] GORR B, MULLER F, AZIM M, CHRIST H J, MULLER T, CHEN H, KAUFFMANN A, HEILMAIER M. High-temperature oxidation behavior of refractory high-entropy alloys:Effect of alloy composition[J]. Oxidation of Metals, 2017, 88:339-349.
[23] PROFF C, ABOLHASSANI S, LEMAIGNAN C. Oxidation behaviour of zirconium alloys and their precipitates—A mechanistic study[J]. Journal of Nuclear Materials, 2013, 432:222-238.
[24] LI Ya-li, MORRAL J E. A local equilibrium model for internal oxidation[J]. Acta Materialia, 2002, 50:3683-3691.
[25] REDDY A, HOVIS D B, HEUER A H, PAULIKAS A P, VEAL B W.In situ study of oxidation-induced growth strains in a model Ni Cr Al Y bond-coat alloy[J]. Oxidation of Metals, 2007, 67:153-177.
[26] XU J L, LIU F, WANG F P, YU D Z, ZHAO L C. The corrosion resistance behavior of Al2O3 coating prepared on Ni Ti alloy by micro-arc oxidation[J]. Journal of Alloys and Compounds, 2009, 472:276-280.
[27] SUSHKO M L, ALEXANDROV V, SCHREIBER D K, ROSSO K M, BRUEMMER S M. Multiscale model of metal alloy oxidation at grain boundaries[J]. Journal of Chemical Physics, 2015, 142:1-8.
[28] GORR B, MUELLER F, CHRIST H J, MUELLER T, CHEN H,KAUFFMANN A, HEILMAIER M. High temperature oxidation behavior of an equimolar refractory metal-based alloy 20Nb-20Mo-20Cr-20Ti-20Al with and without Si addition[J]. Journal of Alloys and Compounds, 2016, 688:468-477.
[29] SUPATARAWANICH V, JOHNSON D R, LIU C T. Effects of microstructure on the oxidation behavior of multiphase Mo-Si-B alloys[J]. Materials Science and Engineering A, 2003, 344:328-339.
[30] GENG J, TSAKIROPOULOS P. A study of the microstructures and oxidation of Nb-Si-Cr-Al-Mo in situ composites alloyed with Ti,Hf and Sn[J]. Intermetallics, 2007, 15:382-395.