非晶态U60Fe27.5Al12.5 合金的晶化动力学行为

doi:10.11900/0412.1961.2021.00077

金属学报

2022, Vol. 58

Issue (10): 1316-1324 DOI: 10.11900/0412.1961.2021.00077

研究论文

本期目录 | 过刊浏览

非晶态U₆₀Fe_27.5Al_12.5 合金的晶化动力学行为

韩录会¹, 柯海波²(

), 张培¹, 桑革¹, 黄火根¹(

)

^1.中国工程物理研究院材料研究所江油 621907
^2.松山湖材料实验室东莞 523808

Kinetic Crystallization Behavior of Amorphous U₆₀Fe_27.5Al_12.5 Alloy

HAN Luhui¹, KE Haibo²(

), ZHANG Pei¹, SANG Ge¹, HUANG Huogen¹(

)

^1.Institute of Materials, China Academy of Engineering Physics, Jiangyou 621907, China
^2.Songshan Lake Materials Laboratory, Dongguan 523808, China

引用本文:

韩录会, 柯海波, 张培, 桑革, 黄火根. 非晶态U₆₀Fe_27.5Al_12.5 合金的晶化动力学行为[J]. 金属学报, 2022, 58(10): 1316-1324.
Luhui HAN, Haibo KE, Pei ZHANG, Ge SANG, Huogen HUANG. Kinetic Crystallization Behavior of Amorphous U₆₀Fe_27.5Al_12.5 Alloy[J]. Acta Metall Sin, 2022, 58(10): 1316-1324.

全文: PDF(1667 KB) HTML

摘要:

针对典型的U₆₀Fe_27.5Al_12.5非晶合金,利用差示扫描量热仪进行了非等温晶化与等温晶化过程的动力学研究,并采用不同的理论方法进行了数据分析。发现该合金的玻璃化转变激活能略高于270 kJ/mol,熔体脆度接近22,证实了其属于强金属玻璃体系材料。基于第一放热晶化峰,由非等温晶化方法得到其晶化激活能位于205~275 kJ/mol范围,而由等温晶化方法得到的结果位于280~390 kJ/mol区间,前者明显低于后者,与一般的非晶合金表现一致,其原因是前一种方法的测试过程中温度不断升高,更易于激发晶化反应。前一种方法获得的动力学因子大都位于3~4之间,略高于后一种方法得到的动力学因子主体区间2.5~3,这既证明该非晶的晶化以形核为主,也说明升温过程更易于促使形核发生。

关键词 ：铀合金, 非晶合金, 晶化机制, 热分析

Abstract：

Due to their high strength and excellent anticorrosive properties, U-based amorphous alloys are quite promising for applications in nuclear-related fields. However, they face the challenge of crystallization due to high temperatures during some applications. Currently, focus on the crystallization mechanism of such materials is limited; thus, further investigation is required. Herein, using differential scanning calorimetry, both nonisothermal and isothermal crystallization kinetics of typical amorphous U₆₀Fe_27.5Al_12.5 alloy were investigated. This alloy was further analyzed using different theoretical methods. The alloy exhibited the glass transition activation energy of slightly more than 270 kJ/mol and the melt fragility value of about 22, indicating that it is a strong metallic glass material. Based on the first exothermal crystallization peak, this glassy alloy is believed to possess the crystallization activation energy of 205-275 kJ/mol within nonisothermal method and 280-390 kJ/mol within the other method. The former value is much lower than the latter, which is consistent with the results of the conventional amorphous alloys. This general trend is mainly because crystallization can be activated more easily by a continuous increase in temperature. The kinetic factor of the alloy was in the ranges of 3-4 and 2.5-3 under the nonisothermal and isothermal conditions, respectively, demonstrating that the devitrification of the noncrystalline U-Fe-Al alloy greatly depends on the nucleation process, which is prone to occur during a rise in temperature.

Key words： uranium alloy amorphous alloy crystallization mechanism thermal analysis

收稿日期: 2021-02-25

ZTFLH:

TG139

基金资助:国家自然科学基金联合基金项目(U2030208);国家自然科学基金项目(51731002);基础加强计划项目(JCJQ-20190415);表面物理与化学重点实验室预研基金项目(6142A02200205)

作者简介: 韩录会,男,1982年生,博士生

	服务

	把本文推荐给朋友
	加入引用管理器
	E-mail Alert
	RSS
	作者相关文章
	韩录会
	柯海波
	张培
	桑革
	黄火根
44.8K

链接本文:

https://www.ams.org.cn/CN/10.11900/0412.1961.2021.00077 或 https://www.ams.org.cn/CN/Y2022/V58/I10/1316

图1 不同升温速率下U60Fe27.5Al12.5非晶合金的DSC曲线,不同特征温度的Kissinger图和Ozawa图,及不同升温速率下玻璃转变温度Tg、晶化温度Tx1和Tx2外延获得的Kauzmann温度

表1 U60Fe27.5Al12.5非晶合金的热力学温度

表2 U60Fe27.5Al12.5非晶合金的激活能与脆度参数

图2 不同升温速率下U60Fe27.5Al12.5非晶合金的DSC晶化曲线与晶化体积分数(x)随温度的变化曲线

图3 U60Fe27.5Al12.5非晶合金的-lnθ~1000 / T关系图及其晶化激活能Ec(x)随晶化体积分数的演化图

图4 U60Fe27.5Al12.5非晶合金的ln[-ln(1 - x)]与1000 / T的关系,及局域动力学因子n(x)随x的演化

图5 U60Fe27.5Al12.5非晶合金在不同温度退火后的DSC晶化曲线及晶化体积分数随温度的变化曲线

图6 U60Fe27.5Al12.5非晶合金在不同温度退火下,晶化时间与退火温度的变化关系及晶化激活能与晶化体积分数的关系

图7 U60Fe27.5Al12.5非晶合金的ln[-ln(1 - x)] vs ln(t - τ)的关系及局域动力学因子随1 - x的演化

表3 部分非晶合金的特征温度与晶化动力学参数[19,20,23~32]

1	Ortega L H, Blamer B, Stern K M, et al. Thermal conductivity of uranium metal and uranium-zirconium alloys fabricated via powder metallurgy [J]. J. Nucl. Mater., 2020, 531: 151982 doi: 10.1016/j.jnucmat.2019.151982
2	Li H B, Ding Q, Gu Y J, et al. The initial oxidation behavior of uranium and uranium-titanium alloys in standing storage [J]. Corros. Sci., 2020, 176: 108879 doi: 10.1016/j.corsci.2020.108879
3	Zubelewicz A, Addessio F L, Cady C M. A constitutive model for a uranium-niobium alloy [J]. J. Appl. Phys., 2006, 100: 013523
4	Dash S, Ghoshal K, Kutty T R G. Thermodynamic investigations of uranium-rich binary and ternary alloys [J]. J. Therm. Anal. Calorim., 2013, 112: 179 doi: 10.1007/s10973-012-2801-9
5	Maslennikov A, Bessonov A, Peretroukhine V, et al. Uranium and U-Zr and U-Ru alloy corrosion rates in the transpassive state [J]. J. Alloys Compd., 2007, 444-445: 345 doi: 10.1016/j.jallcom.2007.06.078
6	Banos A, Harker N J, Scott T B. A review of uranium corrosion by hydrogen and the formation of uranium hydride [J]. Corros. Sci., 2018, 136: 129 doi: 10.1016/j.corsci.2018.03.002
7	Long Z, Liu K Z, Bai B, et al. Corrosion resistance of modified layer on uranium formed by plasma immersion ion implantation [J]. J. Alloys Compd., 2010, 491: 252 doi: 10.1016/j.jallcom.2009.09.164
8	Wang W H, Luo P. The dynamic behavior hidden in the long time scale of metallic glasses and its effect on the properties [J]. Acta. Metall. Sin., 2018, 54: 1479 doi: 10.11900/0412.1961.2018.00247
8	汪卫华, 罗鹏. 金属玻璃中隐藏在长时间尺度下的动力学行为及其对性能的影响 [J]. 金属学报, 2018, 54: 1479 doi: 10.11900/0412.1961.2018.00247
9	Huang H G, Zhang P G, Zhang P, et al. Comparison of glass forming ability between U-Co and U-Fe base systems [J]. Acta. Metall. Sin., 2020, 56: 849 doi: 10.11900/0412.1961.2019.00349
9	黄火根, 张鹏国, 张培等. U-Co与U-Fe基础体系非晶形成能力的比较 [J]. 金属学报, 2020, 56: 849 doi: 10.11900/0412.1961.2019.00349
10	Xu H Y, Ke H B, Huang H G, et al. U-based metallic glasses with superior glass forming ability [J]. J. Nucl. Mater., 2018, 499: 372 doi: 10.1016/j.jnucmat.2017.11.043
11	Huang H G, Wang Y M, Chen L, et al. Study on formation and corrosion resistance of amorphous alloy in U-Co system [J]. Acta. Metall. Sin., 2015, 51: 623
11	黄火根, 王英敏, 陈亮等. U-Co系非晶合金的形成与耐蚀性研究 [J]. 金属学报, 2015, 51: 623
12	Zhang P, Pu Z, Zhang P G, et al. U-Fe-Al metallic glasses with superior glass forming ability and corrosion resistance [J]. J. Mater. Res. Technol., 2020, 9: 6209 doi: 10.1016/j.jmrt.2020.03.039
13	Wang W H. The nature and properties of amorphous matter [J]. Prog. Phys., 2013, 33: 177
13	汪卫华. 非晶态物质的本质和特性 [J]. 物理学进展, 2013, 33: 177
14	Kissinger H E. Reaction kinetics in differential thermal analysis [J]. Anal. Chem., 1957, 29: 1702 doi: 10.1021/ac60131a045
15	Ozawa T. A new method of analyzing thermogravimetric data [J]. Bull. Chem. Soc. Japan, 1965, 38(11): 1881 doi: 10.1246/bcsj.38.1881
16	Böhmer R, Ngai K L, Angell C A, et al. Nonexponential relaxations in strong and fragile glass formers [J]. J. Chem. Phys., 1999, 99: 4201 doi: 10.1063/1.466117
17	Wang T, Yang Y Q, Li J B, et al. Thermodynamics and structural relaxation in Ce-based bulk metallic glass-forming liquids [J]. J. Alloys Compd., 2011, 509: 4569 doi: 10.1016/j.jallcom.2011.01.106
18	Huang H G, Ke H B, Zhang P, et al. U-based binary strong glass forming system [J]. J. Non-Cryst. Solids, 2019, 511: 68 doi: 10.1016/j.jnoncrysol.2018.12.041
19	Liu L, Wu Z F, Zhang J. Crystallization kinetics of Zr₅₅Cu₃₀Al₁₀Ni₅ bulk amorphous alloy [J]. J. Alloys Compd., 2002, 339: 90 doi: 10.1016/S0925-8388(01)01977-6
20	Qiao J C, Pelletier J M. Crystallization kinetics in Cu₄₆Zr₄₅Al₇Y₂ bulk metallic glass by differential scanning calorimetry (DSC) [J]. J. Non-Cryst. Solids, 2011, 357: 2590 doi: 10.1016/j.jnoncrysol.2010.12.071
21	Málek J. The applicability of Johnson-Mehl-Avrami model in the thermal analysis of the crystallization kinetics of glasses [J]. Thermochim. Acta, 1995, 267: 61 doi: 10.1016/0040-6031(95)02466-2
22	Lu W, Yan B, Huang W H. Complex primary crystallization kinetics of amorphous Finemet alloy [J]. J. Non-Cryst. Solids, 2005, 351: 3320 doi: 10.1016/j.jnoncrysol.2005.08.018
23	Zhuang Y X, Wang W H, Zhang Y, et al. Crystallization kinetics and glass transition of Zr₄₁Ti₁₄Cu_12.5Ni_{10 -} _x Fe _x Be_22.5 bulk metallic glasses [J]. Appl. Phys. Lett., 1999, 75: 2392 doi: 10.1063/1.125024
24	Venkataraman S, Rozhkova E, Eckert J, et al. Thermal stability and crystallization kinetics of Cu-reinforced Cu₄₇Ti₃₃Zr₁₁Ni₈Si₁ metallic glass composite powders synthesized by ball milling: The effect of particulate reinforcement [J]. Intermetallics, 2005, 13: 833 doi: 10.1016/j.intermet.2005.01.010
25	Yuan Z Z, Chen X D, Wang B X, et al. Kinetics study on non-isothermal crystallization of the metallic Co₄₃Fe₂₀Ta_5.5B_31.5 glass [J]. J. Alloys Compd., 2006, 407: 163 doi: 10.1016/j.jallcom.2005.06.022
26	Kozmidis-Petrović A F, Lukić S R, Štrbac G R. Calculation of non-isothermal crystallization parameters for the Cu₁₅(As₂Se₃)₈₅ metal-chalcogenide glass [J]. J. Non-Cryst. Solids, 2010, 356: 2151 doi: 10.1016/j.jnoncrysol.2010.08.026
27	Zhuang Y X, Duan T F, Shi H Y. Calorimetric study of non-isothermal crystallization kinetics of Zr₆₀Cu₂₀Al₁₀Ni₁₀ bulk metallic glass [J]. J. Alloys Compd., 2011, 509: 9019 doi: 10.1016/j.jallcom.2011.06.112
28	Hu L, Ye F. Crystallization kinetics of Ca₆₅Mg₁₅Zn₂₀ bulk metallic glass [J]. J. Alloys Compd., 2013, 557: 160 doi: 10.1016/j.jallcom.2012.12.158
29	Wu J L, Pan Y, Huang J D, et al. Non-isothermal crystallization kinetics and glass-forming ability of Cu-Zr-Ti-In bulk metallic glasses [J]. Thermochim. Acta, 2013, 552: 15 doi: 10.1016/j.tca.2012.11.012
30	Cui J, Li J S, Wang J, et al. Crystallization kinetics of Cu₃₈Zr₄₆Ag₈Al₈ bulk metallic glass in different heating conditions [J]. J. Non-Cryst. Solids, 2014, 404: 7 doi: 10.1016/j.jnoncrysol.2014.07.029
31	Gong P, Yao K F, Ding H Y. Crystallization kinetics of TiZrHfCuNiBe high entropy bulk metallic glass [J]. Mater. Lett., 2015, 156: 146 doi: 10.1016/j.matlet.2015.05.018
32	Ke H B, Xu H Y, Huang H G, et al. Non-isothermal crystallization behavior of U-based amorphous alloy [J]. J. Alloys Compd., 2017, 691: 436 doi: 10.1016/j.jallcom.2016.08.252

[1]	刘帅帅, 侯超楠, 王恩刚, 贾鹏. Zr₆₁Cu₂₅Al₁₂Ti₂ 和Zr_52.5Cu_17.9Ni_14.6Al₁₀Ti₅ 块体非晶合金过冷液相区的塑性流变行为[J]. 金属学报, 2022, 58(6): 807-815.
[2]	李金富, 李伟. 铝基非晶合金的结构与非晶形成能力[J]. 金属学报, 2022, 58(4): 457-472.
[3]	张雷, 施韬, 黄火根, 张培, 张鹏国, 吴敏, 法涛. 铀基非晶复合材料的相分离与凝固序列研究[J]. 金属学报, 2022, 58(2): 225-230.
[4]	张金勇, 赵聪聪, 吴宜谨, 陈长玖, 陈正, 沈宝龙. (Fe_0.33Co_0.33Ni_0.33)₈₄_-_x Cr₈Mn₈B _x 高熵非晶合金薄带的结构特征及其晶化行为[J]. 金属学报, 2022, 58(2): 215-224.
[5]	刘日平, 马明臻, 张新宇. 块体非晶合金铸造成形的研究新进展[J]. 金属学报, 2021, 57(4): 515-528.
[6]	毕甲紫, 刘晓斌, 李然, 张涛. 非晶合金粉末作为润滑油添加剂的摩擦学性能[J]. 金属学报, 2021, 57(4): 559-566.
[7]	李宁, 黄信. 块体非晶合金的3D打印成形研究进展[J]. 金属学报, 2021, 57(4): 529-541.
[8]	潘杰, 段峰辉. 非晶合金的回春行为[J]. 金属学报, 2021, 57(4): 439-452.
[9]	胡祥, 葛嘉城, 刘思楠, 伏澍, 吴桢舵, 冯涛, 刘冬, 王循理, 兰司. 具有异常放热现象的Fe-Nb-B-Y非晶合金燃烧机理[J]. 金属学报, 2021, 57(4): 542-552.
[10]	朱敏, 欧阳柳章. 镁基储氢合金动力学调控及电化学性能[J]. 金属学报, 2021, 57(11): 1416-1428.
[11]	黄火根, 张鹏国, 张培, 王勤国. U-Co与U-Fe基础体系非晶形成能力的比较[J]. 金属学报, 2020, 56(6): 849-854.
[12]	耿遥祥, 王英敏. 铁基非晶合金局域结构与性能关联：基于微合金化机理研究[J]. 金属学报, 2020, 56(11): 1558-1568.
[13]	徐秀月, 李艳辉, 张伟. Fe(Pt, Ru)B非晶带材脱合金制备纳米多孔PtRuFe及其甲醇电催化性能[J]. 金属学报, 2020, 56(10): 1393-1400.
[14]	金辰日, 杨素媛, 邓学元, 王扬卫, 程兴旺. 纳米晶化对锆基非晶合金动态压缩性能的影响[J]. 金属学报, 2019, 55(12): 1561-1568.
[15]	杨高林, 林鑫, 卢献钢. 激光多次熔凝Zr₅₅Cu₃₀Al₁₀Ni₅非晶合金的晶化形态与演化机理[J]. 金属学报, 2019, 55(12): 1544-1550.

Viewed

Full text

Abstract

Cited

Shared

Discussed