Please wait a minute...
金属学报  2017, Vol. 53 Issue (8): 1018-1024    DOI: 10.11900/0412.1961.2017.00053
  本期目录 | 过刊浏览 |
深过冷液态金属Cu的热物理性质和原子分布
朱姜蕾, 王庆, 王海鹏()
西北工业大学应用物理系 西安 710072
Thermophysical Properties and Atomic Distribution of Undercooled Liquid Cu
Jianglei ZHU, Qing WANG, Haipeng WANG()
Department of Applied Physics, Northwestern Polytechnical University, Xi'an 710072, China
全文: PDF(863 KB)   HTML
  
摘要: 

针对液态金属Cu在深过冷亚稳条件下的热物理性质和液态结构数据缺乏的问题,采用分子动力学方法结合修正嵌入原子势,研究了常规液态和亚稳液态金属Cu的热物理性质(熔点、密度、比热容和自扩散系数)和原子分布规律,体系温度范围为800~2400 K,最大过冷度达到556 K。通过构建晶体-液体-晶体结构,探索了金属Cu的熔化过程,获得最优的熔点计算温度为1341 K,与实验值误差1.11%。获得了宽广温度范围内液态金属Cu的密度随温度的变化规律,采用Mishin势函数计算的熔点处密度模拟值为7.86 g/cm3,与文献报道的实验结果的误差小于2%。液态金属Cu的焓在800~2400 K范围内随温度呈线性关系变化,即比热容几乎不随过冷度变化而变化,而自扩散系数则随温度呈指数关系变化。根据不同温度原子的位置变化,获得了相应的双体分布函数,发现液态体系始终处于短程有序、长程无序的状态,且原子短程有序度随温度升高而降低,短程有序结构仅保持在3~4个原子间距范围内,且随间距增大而展现出典型的无序特征。

关键词 深过冷液态金属热物理性质双体分布函数    
Abstract

Cu is commonly used in the field of electricity and electronics because of its high ductility, and electrical and thermal conductivity. The thermophysical properties and the atomic structure of liquid Cu, especially for undercooled state, are of practical significance in both application and fundamental researches. The major approaches to obtain thermophysical properties of undercooled metals are containerless techniques based on electrostatic levitation, electromagnetic levitation and ultrasonic levitation et al. However, the strong volatility of liquid Cu results in great difficulties to measure the thermophysical properties. Accordingly, computational prediction is becoming an expected method to obtain the thermophysical data of liquid Cu. The molecular dynamics (MD) simulation, in combination with a resonable potential model, has been extensively employed in studying the physical properties of several metals as a powerful approach. In this work, the atomic distribution and thermophysical properties including melting temperature, density, specific heat and self-diffusion coefficient of liquid Cu were studied by molecular dynamics simulation. Mishin's and Zhou's embedded-atom method potentials, and the modified embedded-atom method potential proposed by Baskes were used over the temperature range of 800~2400 K, reaching the maximum undercooling of 556 K. The simulated results are in good agreement with the reported experimental results. The crystal-liquid-crystal sandwich structure has been used to calculate the melting point. The melting point calculated by Baskes' potential model is 1341 K, just a difference of 1.11% from the experimental value. The density at the melting point calculated by Mishin's potential is 7.86 g/cm3, with a difference less than 2% compared with the reported data. It is found that the enthalpy of liquid Cu increases linearly with the increase of temperature. The specific heat is obtained to be 31.89 J/(molK) by Mishin's potential, which is constant in the corresponding temperature range. The self-diffusion coefficient is exponentially dependent on the temperature. The maximum error between the reported value and the present value of the self-diffusion coefficient calculated by Mishin's potential is only 4.93%. The pair distribution function was applied to investigate the atomic structure of liquid Cu, which suggests that the simulated system is still ordered in short range and disordered in long range for both normal liquid and undercooled state. It is found that the atomic ordered degree is weakened with the increase of temperature, and it is kept within 3~4 atom neighbor distance.

Key wordsundercooling    liquid metal    thermophysical property    pair distribution function
收稿日期: 2017-02-20     
ZTFLH:  O469  
基金资助:国家自然科学基金项目Nos.51474175和51522102及陕西省工业科技攻关项目No.2015GY138
作者简介:

作者简介 朱姜蕾,女,1992年生,硕士生

引用本文:

朱姜蕾, 王庆, 王海鹏. 深过冷液态金属Cu的热物理性质和原子分布[J]. 金属学报, 2017, 53(8): 1018-1024.
Jianglei ZHU, Qing WANG, Haipeng WANG. Thermophysical Properties and Atomic Distribution of Undercooled Liquid Cu. Acta Metall Sin, 2017, 53(8): 1018-1024.

链接本文:

https://www.ams.org.cn/CN/10.11900/0412.1961.2017.00053      或      https://www.ams.org.cn/CN/Y2017/V53/I8/1018

图1  晶体-液体-晶体结构法计算Cu内能随温度的变化
图2  不同设定温度时体系相变过程
图3  液态Cu密度随温度的变化
图4  液态Cu的焓随温度的变化
图5  液态Cu自扩散系数随温度的变化
图6  液态Cu在900~2300 K温度范围内双体分布函数
图7  液态Cu双体分布函数的第一近邻和第二近邻峰值随温度变化关系
[1] Iida T, Guthrie R I L, translated by Xian A P, Wang L W. The Physical Properties of Liquid Metals [M]. Beijing: Science Press, 2006: 97, 218(Iida T, Guthrie R I L著, 冼爱平, 王连文译. 液态金属的物理性能 [M]. 北京: 科学出版社, 2006: 97, 218)
[2] Yan E H, Sun L X, Xu F, et al.Prediction of the solidification path of Al-6.32Cu-25.13Mg alloy by a unified microsegregation model coupled with Thermo-Calc[J]. Acta Metall. Sin., 2016, 52: 632(闫二虎, 孙立贤, 徐芬等. 基于Thermo-Calc和微观偏析统一模型对Al-6.32Cu-25.13Mg合金凝固路径的预测[J]. 金属学报, 2016, 52: 632)
[3] Kim T H, Kelton K F.Structural study of supercooled liquid transition metals[J]. J. Chem. Phys., 2007, 126: 054513
[4] Wang H P, Yang S J, Hu L, et al.Molecular dynamics prediction and experimental evidence for density of normal and metastable liquid zirconium[J]. Chem. Phys. Lett., 2016, 653: 112
[5] Yan J H, Jian Z Y, Zhu M, et al.Solidification characteristics and microstructure of high undercooled Al-70%Si alloy[J]. Acta Metall. Sin., 2016, 52: 931(严军辉, 坚增运, 朱满等. 深过冷Al-70%Si合金的凝固特性与微观组织[J]. 金属学报, 2016, 52: 931)
[6] Lü P, Wang H P.Direct formation of peritectic phase but no primary phase appearance within Ni83.25Zr16.75peritectic alloy during free fall[J]. Sci. Rep., 2016, 6: 22641
[7] Demmel F, Hennet L, Brassamin S, et al.Nickel self-diffusion in a liquid and undercooled NiSi alloy[J]. Phys. Rev., 2016, 94B: 014206
[8] Hu L, Li L H, Yang S J, et al.Thermophysical properties and eutectic growth of electrostatically levitated and substantially undercooled liquid Zr91.2Si8.8 alloy[J]. Chem. Phys. Lett., 2015, 621: 91
[9] Perepezko J H, Imhoff S D.Crystallization control in highly undercooled liquids and glasses[J]. Int. J. Mater. Res., 2012, 103: 1083
[10] Johnson M L, Mauro N A, Vogt A J, et al.Structural evolution and thermophysical properties of ZrxNi100-x, metallic liquids and glasses[J]. J. Non-Cryst. Solids, 2014, 405: 211
[11] Ishikawa T, Okada J T, Paradis P F, et al.Thermophysical property measurements of liquid gadolinium by containerless methods[J]. Int. J. Thermophys., 2010, 31: 388
[12] Wunderlich R K, Fecht H J, Egry I, et al.Thermophysical properties of a Fe-Cr-Mo alloy in the solid and liquid phase[J]. Steel Res. Int., 2012, 83: 43
[13] Cho Y C, Kim B S, Yoo H, et al.Successful melting and density measurements of Cu and Ag single crystals with an electrostatic levitation (ESL) system[J]. CrystEngComm, 2014, 16: 7575
[14] Brillo J, Egry I.Density determination of liquid copper, nickel, and their alloys[J]. Int. J. Thermophys., 2003, 24: 1155
[15] Meyer A.Self-diffusion in liquid copper as seen by quasielastic neutron scattering[J]. Phys. Rev., 2010, 81B: 012102
[16] Yang H, Wang L, Yuan B, et al.Adhesion of an ultrasmall nanoparticle on a bilayer membrane is still size and shape dependent[J]. J. Mater. Sci. Technol., 2015, 31: 660
[17] Wu H N, Xu D S, Wang H, et al.Molecular dynamics simulation of tensile deformation and fracture of γ-TiAl with and without surface defects[J]. J. Mater. Sci. Technol., 2016, 32: 1033
[18] Chen F F, Zhang H F, Qin F X, et al.Molecular dynamics study of atomic transport properties in rapidly cooling liquid copper[J]. J. Chem. Phys., 2004, 120: 1826
[19] Wang H P, Wei B.Thermophysical properties of stable and metastable liquid copper and nickel by molecular dynamics simulation[J]. Appl. Phys., 2009, 95A: 661
[20] Han X J, Chen M, Guo Z Y.Thermophysical properties of undercooled liquid Au-Cu alloys from molecular dynamics simulations[J]. J. Phys.: Condens. Matter, 2004, 16: 705
[21] Lü Y J, Cheng H, Chen M.A molecular dynamics examination of the relationship between self-diffusion and viscosity in liquid metals[J]. J. Chem. Phys., 2012, 136: 214505
[22] Daw M S, Baskes M I.Embedded-atom method: derivation and application to impurities, surfaces, and other defects in metals[J]. Phys. Rev., 1984, 29B: 6443
[23] Stott M J, Zaremba E.Quasiatoms: An approach to atoms in nonuniform electronic systems[J]. Phys. Rev., 1980, 22B: 1564
[24] N?rskov J, Lang N D.Effective-medium theory of chemical binding: application to chemisorption[J]. Phys. Rev., 1980, 21B: 2131
[25] Baskes M I.Modified embedded-atom potentials for cubic materials and impurities[J]. Phys. Rev., 1992, 46B: 2727
[26] Baskes M I, Johnson R A.Modified embedded atom potentials for HCP metals[J]. Modell. Simul. Mater. Sci. Eng., 1994, 2: 147
[27] Baskes M I.Calculation of the behaviour of Si ad-dimers on Si(001)[J]. Modell. Simul. Mater. Sci. Eng., 1997, 5: 149
[28] Mishin Y, Mehl M J, Papaconstantopoulos D A, et al.Structural stability and lattice defects in copper: Ab initio, tight-binding, and embedded-atom calculations[J]. Phys. Rev., 2001, 63B: 224106
[29] Zhou X W, Johnson R A, Wadley H N G. Misfit-energy-increasing dislocations in vapor-deposited CoFe/NiFe multilayers[J]. Phys. Rev., 2004, 69B: 144113
[30] Plimpton S.Fast parallel algorithms for short-range molecular dynamics[J]. J. Comput. Phys., 1995, 117: 1
[31] Nasch P M, Steinemann S G.Density and thermal expansion of molten manganese, iron, nickel, copper, aluminum and tin by means of the gamma-ray attenuation technique[J]. Phys. Chem. Liq., 1995, 29: 43
[32] Assael M J, Kalyva A E, Antoniadis K D, et al.Reference data for the density and viscosity of liquid copper and liquid tin[J]. J. Phys. Chem. Ref. Data, 2010, 39: 033105
[1] 李金富, 周尧和. 液态金属深过冷快速凝固过程中初生固相的重熔[J]. 金属学报, 2018, 54(5): 627-636.
[2] 刘林, 孙德建, 黄太文, 张琰斌, 李亚峰, 张军, 傅恒志. 高梯度定向凝固技术及其在高温合金制备中的应用[J]. 金属学报, 2018, 54(5): 615-626.
[3] 翟斌, 周凯, 吕鹏, 王海鹏. 自由落体条件下Ti-6Al-4V合金微液滴的快速凝固研究[J]. 金属学报, 2018, 54(5): 824-830.
[4] 杨旭, 廖波, 刘坚, 严伟, 单以银, 肖福仁, 杨柯. 中国低活化马氏体钢在液态Pb-Bi中的脆化现象[J]. 金属学报, 2017, 53(5): 513-523.
[5] 严军辉,坚增运,朱满,常芳娥,许军锋. 深过冷Al-70%Si合金的凝固特性与微观组织*[J]. 金属学报, 2016, 52(8): 931-937.
[6] 杨柯, 严伟, 王志光, 单以银, 石全强, 史显波, 王威. 核用新型耐高温、抗辐照、耐液态金属腐蚀结构材料——SIMP钢的研究进展*[J]. 金属学报, 2016, 52(10): 1207-1221.
[7] 闫学伟,唐宁,刘孝福,税国彦,许庆彦,柳百成. 镍基高温合金铸件液态金属冷却定向凝固建模仿真及工艺规律研究[J]. 金属学报, 2015, 51(10): 1288-1296.
[8] 刘庆华,黄裕金,刘剑,胡侨丹,李建国. Ni-Fe-Ga-Co磁性形状记忆合金定向凝固稳定生长区的组织及择优取向[J]. 金属学报, 2013, 29(4): 391-398.
[9] 郭雄,林鑫,汪志太,曹永青,彭东剑,黄卫东. 深过冷Ni-30Sn合金凝固组织演化及反常共晶的形成机制[J]. 金属学报, 2013, 29(4): 475-482.
[10] 常芳娥 赵志伟 朱满 李娜 方雯 董广志 坚增运. 深过冷Ni-21.4%Si共晶合金的凝固特性研究[J]. 金属学报, 2012, 48(7): 875-881.
[11] 穆丹宁 杨长林 魏晓伟 刘峰. 深过冷铁钴基块体合金的细晶化研究[J]. 金属学报, 2012, 48(12): 1409-1414.
[12] 石倩颖 李相辉 郑运荣 谢光 张健 冯强. HRS和LMC工艺制备的两种镍基单晶高温合金铸态及固溶微孔的形成[J]. 金属学报, 2012, 48(10): 1237-1247.
[13] 周圣银 胡锐 蒋力 李金山 寇宏超 常辉 周廉. 深过冷凝固Co80Pd20合金中的枝晶生长[J]. 金属学报, 2011, 47(4): 391-396.
[14] 葛丙明 刘林 张胜霞 张军 李亚峰 傅恒志. 抽拉速率对定向凝固叶片状DZ125高温合金微观组织的影响[J]. 金属学报, 2011, 47(11): 1470-1476.
[15] 张健 申健 卢玉章 楼琅洪. 燃气轮机用大型定向结晶铸件制备及组织与性能研究[J]. 金属学报, 2010, 46(11): 1322-1326.