非晶态Ni_(55)Nb_(35)Si_(10)合金的非等温纳米结晶动力学（英文）
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摘要
采用差示扫描量热法(DSC)研究机械合金化制备的Ni_(55)Nb_(35)Si_(10)非晶合金的非等温结晶动力学。结果表明,该非晶合金在加热过程中表现出单级结晶,导致非晶态基体中形成金属间化合物纳米晶体。由基辛格方程确定的合金结晶表观活化能较高(468 k J/mol),说明该非晶合金具有较高的热稳定性。采用等转换法对结晶过程中活化能的变化进行研究,活化能从结晶开始一直缓慢降低至结晶分数α=0.35,然后几乎保持不变直至结晶结束。通过测定Avrami指数,解释非晶合金非等温结晶的纳米结晶机理。透射电镜研究表明,在退火过程中通过纳米结晶可对非晶态合金进行微观结构调控。成核速率随时间的延长而减小,结晶机理主要受三维扩散控制生长支配。在Sestak-Berggren自催化模型的基础上,得到定量描述非等温结晶动力学的预测方程。
The non-isothermal crystallization kinetics of Ni_(55)Nb_(35)Si_(10) amorphous alloy, prepared by mechanical alloying, was studied using differential scanning calorimetry. The amorphous alloy showed one-stage crystallization on heating, which led to the formation of nano-intermetallic crystals in amorphous matrix. The apparent activation energy for the crystallization of the alloy, determined by the Kissinger equation, was relatively high(468 k J/mol), indicating that this amorphous alloy has high thermal stability. Changes in the activation energy during the crystallization process, were also evaluated by iso-conversional methods. The results showed that it decreases slowly from the beginning to crystallized fraction α=0.35 and it remains almost constant to the end of the process. The nano-crystallization mechanism for the non-isothermal crystallization of the amorphous alloy was explained by determining Avrami exponents. Transmission electron microscopy studies revealed the microstructural modification of amorphous alloy via nanocrystallization during annealing. The results suggest that the nucleation rate decreases with increasing time and the crystallization mechanism is governed dominantly by a three-dimensional diffusion-controlled growth. A predictive equation was obtained based on the Sestak-Berggren autocatalytic model to describe quantitatively the non-isothermal crystallization kinetics.
The non-isothermal crystallization kinetics of Ni_(55)Nb_(35)Si_(10) amorphous alloy, prepared by mechanical alloying, was studied using differential scanning calorimetry. The amorphous alloy showed one-stage crystallization on heating, which led to the formation of nano-intermetallic crystals in amorphous matrix. The apparent activation energy for the crystallization of the alloy, determined by the Kissinger equation, was relatively high(468 k J/mol), indicating that this amorphous alloy has high thermal stability. Changes in the activation energy during the crystallization process, were also evaluated by iso-conversional methods. The results showed that it decreases slowly from the beginning to crystallized fraction α=0.35 and it remains almost constant to the end of the process. The nano-crystallization mechanism for the non-isothermal crystallization of the amorphous alloy was explained by determining Avrami exponents. Transmission electron microscopy studies revealed the microstructural modification of amorphous alloy via nanocrystallization during annealing. The results suggest that the nucleation rate decreases with increasing time and the crystallization mechanism is governed dominantly by a three-dimensional diffusion-controlled growth. A predictive equation was obtained based on the Sestak-Berggren autocatalytic model to describe quantitatively the non-isothermal crystallization kinetics.
引文
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[29]SVOBODA R,MALEK J.Interpretation of crystallization kinetics results provided by DSC[J].Thermochim Acta,2011,526:237-251.
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[2]SHIRASAWA N,TAKIGAWA Y,UESUGI T,HIGASHI K.The evaluation parameters for glass-forming ability in Ti-Cu system metallic glasses[J].Materials Letters,2015,139:73-76.
[3]HAN Jia-jia,WANG Cui-ping,KOU Sheng-zhong,LIU Xing-jun.Thermal stability,crystallization behavior,Vickers hardness and magnetic properties of Fe-Co-Ni-Cr-Mo-C-B-Y bulk metallic glasses[J].Transactions of Nonferrous Metals Society of China,2013,23:148-155.
[4]ZHANG Jia-jia,LIU Wen-sheng,MA Yun-zhu,YE Xiao-shan,WUYa-yu,HUANG Bo-yun.Preparation and properties of Ni68.6W17.9B13.5 metallic glass[J].Transactions of Nonferrous Metals Society of China,2015,25:1575-1579.
[5]DéO L P,de OLIVEIRA M F.Accuracy of a selection criterion for glass forming ability in the Ni-Nb-Zr system[J].Journal of Alloys and Compounds,2014,615:s23-s28.
[6]MA Y,YE J H,PENG G J,WEN D H,ZHANG T H.Nanoindentation study of size effect on shear transformation zone size in a Ni-Nb metallic glass[J].Materials Science and Engineering A,2015,627:153-160.
[7]LESZ S,DERCZ G.Study on crystallization phenomenon and thermal stability of binary Ni-Nb amorphous alloy[J].Journal of Thermal Analysis and Calorimetry,2016,126:19-26.
[8]SURYANARAYANA C.Mechanical alloying and milling[J].Progress in Materials Science,2001,46:1-184.
[9]KOCH C C,CAVIN O B,MCKAMEY C G,SCARBROUGH J O.Preparation of amorphous Ni60Nb40 by mechanical alloying[J].Applied Physics Letters,1983,43:1017-1019.
[10]CHEN Gang,FERRY M.Crystallization of Mg-based bulk metallic glass[J].Transactions of Nonferrous Metals Society of China,2006,16:833-837.
[11]ZHANG J,TENG X,XU S,GE X,LENG J.Temperature dependence of resistivity and crystallization behaviors of amorphous melt-spun ribbon of Mg66Zn30Gd4 alloy[J].Materials Letters,2017,189:17-20.
[12]CZEPPE T.Mechanism and kinetics of nano-crystallization of the thermally stable NiNb(ZrTi)Al metallic glasses[J].Journal of Thermal Analysis and Calorimetry,2010,101:615-622.
[13]MINOUEI H,AKBARI G H,ENAYATI M H,HONG S I.Amorphization and nanocrystallization of Ni-Nb-Si alloys[J].Materials Science and Engineering A,2017,682:396-401.
[14]STARNIK M J.Analysis of aluminium based alloys by calorimetry:Quantitative analysis of reactions and reaction kinetics[J].International Materials Reviews,2004,49:191-226.
[15]BLAZQUEZ J S,CONDE C F,CONDE A.Non-isothermal approach to isokinetic crystallization processes:Application to the nanocrystallization of HITPERM alloys[J].Acta Materialia,2005,53:2305-2311.
[16]VYAZOVKIN S,BURNHAM A K,CRIADO J M,PéREZ-MAQUEDA L A,POPESCU C,SBIRRAZZUOLI N.ICTAC kinetics committee recommendations for performing kinetic computations on thermal analysis data[J].Thermochimica Acta,2011,520:1-19.
[17]KISSINGER H E.Reaction kinetics in differential thermal analysis[J].Analytical Chemistry,1957,29:1702-1706.
[18]AKAHIRA T,SUNOSE T.Method of determining activation deterioration constant of electrical insulating materials[J].Research Report Chiba Institute of Technology,1971,16:22-31.
[19]OZAWA T.A New method of analyzing thermogravimetric data[J].Bulletin of the Chemical Society of Japan,1965,38:1881-1886.
[20]FLYNN J H,WALL L A.Thermal analysis of polymer by thermogravimetric analysis[J].Journal of Research of the National Bureau of Standards Section A,1966,70:487-523.
[21]KIM S M,CHANDRA D,PAL N K,DOLAN M D,CHIEN W M,TALEKAR A,LAMB J,PAGLIERI S N,FLANAGAN T B.Hydrogen permeability and crystallization Kinetics in amorphous Ni-Nb-Zr alloys[J].International Journal of Hydrogen Energy,2012,37:3904-3913.
[22]TURNBULL D,FISHER J C.Rate of nucleation in condensed systems[J].Journal of Chemical Physics,1949,17:71-73.
[23]MATUSITA K,SAKKA S.Study on crystallization kinetics in glass by differential thermal analysis[J].Thermochimica Acta,1979,33:351-354.
[24]RANGANATHAN S,HEIMENDAHL M V.The three activation energies with isothermal transformations:applications to metallic glasses[J].Journal of Materials Science,1981,16:2401-2404.
[25]DOHERTY R D.Diffusive phase transformations in the solid state[C]//CAHN R W,HAASEN P.Physical metallurgy.Amsterdam,North-Holland:1996:1363-1506.
[26]SENUM G I,YANG R T.Rational approximations of the integral of the Arrhenius function[J].Journal of Thermal Analysis and Calorimetry,1977,11:445-447.
[27]MALEK J.The kinetic analysis of non-isothermal data[J].Thermochimica Acta,1992,200:257-269.
[28]MALEK J,CRIADO J M.The boundary conditions for kinetic models[J].Thermochimica Acta,1989,153:429-432.
[29]SVOBODA R,MALEK J.Interpretation of crystallization kinetics results provided by DSC[J].Thermochim Acta,2011,526:237-251.
[30]BROWN M E,DOLIMORE D,GALWEY A K.Reactions in the Solid State[M].Vol.22.Amsterdam:Elsevier,1980.