First Principles Calculation of Al-Doped Mg/Mg2Sn Alloy Interface
WANG Furong1, ZHANG Yongmei1, BAI Guoning2, GUO Qingwei2, ZHAO Yuhong2,3()
1School of Semiconductors and Physics, North University of China, Taiyuan 030051, China 2School of Materials Science and Engineering, North University of China, Taiyuan 030051, China 3Beijing Advanced Innovation Center for Materials Genome Engineering, University of Science and Technology Beijing, Beijing 100083, China
Cite this article:
WANG Furong, ZHANG Yongmei, BAI Guoning, GUO Qingwei, ZHAO Yuhong. First Principles Calculation of Al-Doped Mg/Mg2Sn Alloy Interface. Acta Metall Sin, 2023, 59(6): 812-820.
Mg-Sn alloy is a high temperature-creep resistant magnesium alloy that has potential applications in lightweight automobiles. The addition of Sn to Mg can reduce the overall cost of the alloy as Sn is cheaper than rare earth elements. Sn and Mg form Mg2Sn phase on the grain boundary, and this Mg2Sn phase has an excellent precipitation hardening effect. However, coarsened Mg2Sn phase can reduce the age hardening effect of the alloy. Previous experimental studies have showed that the addition of Al element can considerably improve the age hardening effect of Mg-Sn alloy as it segregated at the interface between the Mg matrix and Mg2Sn phase. However, there is a lack of research on the different orientations of Al-doped Mg matrix and Mg2Sn phase and the distribution position of Al element at the interface. Therefore, in this study, the interface adhesion energy, interface energy, and interface doping energy of Al-doped Mg/Mg2Sn with different index surfaces were calculated based on density functional theory to determine more stable doping positions. The effects of Al doping on the electronic structure of Mg(0001)/Mg2Sn(022) interface were analyzed using the density of states and crystal orbital Hamilton population. The results demonstrate that only a part of the Al-doping positions is beneficial in strengthening the stability of Mg/Mg2Sn interface. After the addition of Al, the adhesion energy of Sn termination at Mg(0001)/Mg2Sn(001) interface is higher than that of Mg termination, but the adhesion energy of Sn termination at Mg(0001)/Mg2Sn(111) interface is lower than that of Mg termination. In addition, the interface energy of Mg(0001)/Mg2Sn(022) interface doped with Al decreased by 0.07 eV/nm compared to that of Mg(0001)/Mg2Sn(022) interface. The addition of Al element to Mg(0001)/Mg2Sn(022) facilitates the doping of a special position, which shows an obvious interaction between the s orbital of Al and the p orbital of Sn after Al doping. Moreover, the Al—Sn bonding is found to be dominant at the interface.
Fund: National Natural Science Foundation of China(52074246);National Natural Science Foundation of China(22008224);National Natural Science Foundation of China(52275390);National Natural Science Foundation of China(52205429);National Natural Science Foundation of China(52201146);National Defense Basic Scientific Research Program of China(JCKY20204-08B002);National Defense Basic Scientific Research Program of China(WDZC2022-12);Key Research and Development Program of Shanxi Province(202102050-201011);Guiding Local Science and Technology Development Projects by the Central Government(YDZJSX-2022A025);Guiding Local Science and Technology Development Projects by the Central Government(YDZJSX2021A027)
Corresponding Authors:
ZHAO Yuhong, professor, Tel:15035172958, E-mail: zhaoyuhong@nuc.edu.cn
Table 1 Interface spacing, interface energy, and lattice mismatch degree of Mg/Mg2Sn
Fig.1 Schematics of Mg/Mg2Sn interface model with different interface orientations doped with Al element (Roman numerals represent the different doping positions of Al at the interface) (a, b) Mg terminal (a) and Sn terminal (b) models of Mg(0001)/Mg2Sn(001) interface, respectively (c) Mg(0001)/Mg2Sn(022) interface model (d, e) Mg terminal (d) and Sn terminal (e) models of Mg(0001)/Mg2Sn(111) interface, respectively
Fig.2 Adhesion energies of Mg/Mg2Sn interface with doping Al element at different positions (Dotted lines represent the interface adhesion energies without Al element)
Position
Interface spacing / nm
Interface energy / (J·m-2)
Interface doping energy / (J·m-2)
Ⅰ
25.84
0.418
-5.031
Ⅱ
23.64
0.143
-5.070
Ⅲ
23.20
0.140
-5.076
Ⅳ
22.83
0.091
-5.079
Ⅴ
23.22
0.149
-5.075
Ⅵ
23.27
0.152
-5.075
Table 2 Interface spacing, interface energy, and doping energy of Al-doped Mg(0001)/Mg2Sn(022) interface
Fig.3 Interface energies of Mg(0001)/Mg2Sn(022) before (a) and after (b) doping Al element at position IV in Fig.1c (The intercept of the line in the figure represents the elastic strain energy, and the slope represents the interface energy. A—interface area, N—number of atoms in the interface, ΔGf—energy contained in a single atom in the interface)
Fig.4 Partial density of states (PDOS) curves of Mg(0001)/Mg2Sn(022) interface before (a) and after (b) doping Al element at position IV in Fig.1c (EF—Fermi level)
Fig.5 Side views (a1, b1) and top views (a2, b2) of differential charge density diagrams of the Mg(0001)/Mg2Sn(022) interface before (a1, a2) and after (b1, b2) doping Al element at position IV in Fig.1c (The red areas represent the accumulation of electric charge, and the blue areas represent the loss of electric charge)
Fig.6 Projected crystal orbital Hamilton population (pCOHP) curves of hcp Mg (a) and fcc Mg2Sn (b); Mg—Mg (c) and Mg—Sn (d) atoms at the Mg(0001)/Mg2Sn(022) interface; and Mg—Al (e) and Al—Sn (f) atoms at the Mg(0001)/Mg2Sn(022) interface after doping Al (ICOHP—integrated crystal orbital Hamilton population)
1
Xin T Z, Zhao Y H, Mahjoub R, et al. Ultrahigh specific strength in a magnesium alloy strengthened by spinodal decomposition [J]. Sci. Adv., 2021, 7: eabf3039
doi: 10.1126/sciadv.abf3039
2
Xin T Z, Tang S, Ji F, et al. Phase transformations in an ultralight BCC Mg alloy during anisothermal ageing [J]. Acta Mater., 2022, 239: 118248
doi: 10.1016/j.actamat.2022.118248
3
Zhang W Z, Sun Z P, Zhang J Y, et al. A near row matching approach to prediction of multiple precipitation crystallography of compound precipitates and its application to a Mg/Mg2Sn system [J]. J. Mater. Sci., 2017, 52: 4253
doi: 10.1007/s10853-016-0680-3
4
Jo S M, Kim S D, Kim T H, et al. Sequential precipitation behavior of Mg17Al12 and Mg2Sn in Mg-8Al-2Sn-1Zn alloys [J]. J. Alloys Compd., 2018, 749: 794
doi: 10.1016/j.jallcom.2018.03.380
5
Cheng W L, Park S S, You B S, et al. Microstructure and mechanical properties of binary Mg-Sn alloys subjected to indirect extrusion [J]. Mater. Sci. Eng., 2010, A527: 4650
6
Jung I C, Kim Y K, Cho T H, et al. Suppression of discontinuous precipitation in AZ91 by addition of Sn [J]. Met. Mater. Int., 2014, 20: 99
doi: 10.1007/s12540-013-6008-9
7
Huang S, Wang J F, Hou F, et al. Effect of Sn on the formation of the long period stacking ordered phase and mechanical properties of Mg-RE-Zn alloy [J]. Mater. Lett., 2014, 137: 143
doi: 10.1016/j.matlet.2014.08.145
8
Zhou D W, Xu S H, Zhang F Q, et al. First-principle study on structural stability of Sn alloying MgZn2 phase and Mg2Sn phase [J]. Chin. J. Nonferrous Met., 2010, 20: 914
Liu C Q, Chen H W, Wilson N C, et al. Zn segregation in interface between Mg17Al12 precipitate and Mg matrix in Mg-Al-Zn alloys [J]. Scr. Mater., 2019, 163: 91
doi: 10.1016/j.scriptamat.2019.01.001
10
Elsayed F R, Sasaki T T, Mendis C L, et al. Compositional optimization of Mg-Sn-Al alloys for higher age hardening response [J]. Mater. Sci. Eng., 2013, A566: 22
11
Sasaki T T, Oh-ishi K, Ohkubo T, et al. Enhanced age hardening response by the addition of Zn in Mg-Sn alloys [J]. Scr. Mater., 2006, 55: 251
doi: 10.1016/j.scriptamat.2006.04.005
12
Mendis C L, Bettles C J, Gibson M A, et al. Refinement of precipitate distributions in an age-hardenable Mg-Sn alloy through microalloying [J]. Philos. Mag. Lett., 2006, 86: 443
doi: 10.1080/09500830600871186
13
Pan H C, Qin G W, Xu M, et al. Enhancing mechanical properties of Mg-Sn alloys by combining addition of Ca and Zn [J]. Mater. Des., 2015, 83: 736
doi: 10.1016/j.matdes.2015.06.032
14
Tian S K, Guo X F. Microstructure and mechanical properties of as-cast Mg-Sn-Al-Zn alloy [J]. Hot Work. Technol., 2014, 43(4): 64
Kim S H, Park S H. Underlying mechanisms of drastic reduction in yield asymmetry of extruded Mg-Sn-Zn alloy by Al addition [J]. Mater. Sci. Eng., 2018, A733: 285
16
Luo Y X, Chen Y, Ran L, et al. Effects of Zn/Al mass ratio on microstructure evolution and mechanical properties of Mg-Sn based alloys [J]. Mater. Sci. Eng., 2021, A815: 141307
17
Xu X X. Microstructural characterization of aged Mg-Sn-Al alloy [D]. Chongqing: Chongqing University, 2019
徐孝新. 时效Mg-Sn-Al合金的微观结构研究 [D]. 重庆: 重庆大学, 2019
18
Bai G N, Tian J Z, Guo Q W, et al. First-principle study on Mg2X (X = Si, Ge, Sn) intermetallics by Bi micro-alloying [J]. Crystals, 2021, 11: 142
doi: 10.3390/cryst11020142
19
Wang S, Zhao Y H, Deng S J, et al. First-principle studies on the mechanical, thermodynamic and electronic properties of β″-Mg3Gdand β'-Mg7Gd alloys under pressure [J]. J. Phys. Chem. Solids, 2019, 125: 115
doi: 10.1016/j.jpcs.2018.10.020
20
Hou H, Pan Y, Bai G N, et al. High-throughput computing for hydrogen transport properties in ε-ZrH2 [J]. Adv. Compos. Hybrid Mater., 2022, 5: 1350
doi: 10.1007/s42114-022-00454-x
21
Chen L Q, Zhao Y H. From classical thermodynamics to phase-field method [J]. Prog. Mater. Sci., 2022, 124: 100868
doi: 10.1016/j.pmatsci.2021.100868
22
Liu B, Gu M, Liu X L, et al. First-principles study of fluorine-doped zinc oxide [J]. Appl. Phys. Lett., 2010, 97: 122101
doi: 10.1063/1.3492444
23
Li R W, Chen Q C, Ouyang L, et al. Insight into the strengthening mechanism of α-Al2O3/γ-Fe ceramic-metal interface doped with Cr, Ni, Mg, and Ti [J]. Ceram. Int., 2021, 47: 22810
doi: 10.1016/j.ceramint.2021.05.001
24
Li R W, Chen Q C, Ji M X, et al. Exploring failure mode and enhancement mechanism of doped rare-earth elements iron-based/alumina-ceramic interface [J]. Ceram. Int., 2022, 48: 7827
doi: 10.1016/j.ceramint.2021.11.330
25
Wang X H, Zhang C L, Hu X P, et al. First principle study on alloying effect of Al and Zn doping on Mg-Li phase interface [J]. Rare Met. Mater. Eng., 2014, 43: 1661
Liu P, Wang X Y, Chen D F, et al. Interface structure characterization and elements doping on interface bonding strength and tensile failure mechanism of NiCo coating/Cu matrix [J]. Results Phys., 2021, 30: 104883
doi: 10.1016/j.rinp.2021.104883
27
Zhang D L, Wang J, Kong Y, et al. First-principles investigation on stability and electronic structure of Sc-doped θ'/Al interface in Al-Cu alloys [J]. Trans. Nonferrous Met. Soc. China, 2021, 31: 3342
doi: 10.1016/S1003-6326(21)65733-3
28
Zhao Y H. Stability of phase boundary between L12-Ni3Al phases: A phase field study [J]. Intermetallics, 2022, 144: 107528
doi: 10.1016/j.intermet.2022.107528
29
Zhao Y H, Liu K X, Hou H, et al. Role of interfacial energy anisotropy in dendrite orientation in Al-Zn alloys: A phase field study [J]. Mater. Des., 2022, 216: 110555
doi: 10.1016/j.matdes.2022.110555
30
Tsuru T, Somekawa H, Chrzan D C. Interfacial segregation and fracture in Mg-based binary alloys: Experimental and first-principles perspective [J]. Acta Mater., 2018, 151: 78
doi: 10.1016/j.actamat.2018.03.061
31
Jin Y R, Feng Z Z, Ye L Y, et al. Mg2Sn: A potential mid-temperature thermoelectric material [J]. RSC Adv., 2016, 6: 48728
doi: 10.1039/C6RA04986A
32
Kresse G, Furthmüller J. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set [J]. Phys. Rev., 1996, 54B: 11169
33
Xiao J B, Yao J P. First-principle study on the influence of alloy elements on the stability of TiC/Mg interface [J]. Spec. Cast. Nonferrous Alloys, 2020, 40: 1152
Xie H N, Chen Y T, Zhang T B, et al. Adhesion, bonding and mechanical properties of Mo doped diamond/Al (Cu) interfaces: A first principles study [J]. Appl. Surf. Sci., 2020, 527: 146817
doi: 10.1016/j.apsusc.2020.146817
35
Wang S, Zhang C, Li X, et al. First-principle investigation on the interfacial structure evolution of the δ'/θ'/δ' composite precipitates in Al-Cu-Li alloys [J]. J. Mater. Sci. Technol., 2020, 58: 205
doi: 10.1016/j.jmst.2020.03.065
36
Wen Z Q, Zhao Y H, Hou H, et al. A first-principles study on interfacial properties of Ni(001)/Ni3Nb(001) [J]. Trans. Nonferrous Met. Soc. China, 2014, 24: 1500
doi: 10.1016/S1003-6326(14)63218-0
37
Wang C Q, Chen W G, Xie J P. Effects of transition element additions on the interfacial interaction and electronic structure of Al(111)/6H-SiC(0001) interface: A first-principles study [J]. Materials, 2021, 14: 630
doi: 10.3390/ma14030630
38
Deringer V L, Tchougréeff A L, Dronskowski R. Crystal orbital Hamilton population (COHP) analysis as projected from plane-wave basis sets [J]. J. Phys. Chem., 2011, 115A: 5461
