High throughput synthesis enabled exploration of CoCrFeNi-based high entropy alloys

doi:10.1016/j.jmst.2021.09.031

Abstract

Abstract:

To accelerate the exploration, screening, and discovery of structural high-entropy alloys with targeted properties, the newly developed High-Throughput Hot-Isostatic-Pressing based Micro-Synthesis Approach (HT-HIP-MSA) is employed to efficiently synthesize and characterize 85 combinatorial alloys in a 13-principal element alloying space. These CoCrFeNi-based high entropy alloys span 1 quaternary, 9 quinary, and 36 senary alloy systems, and their composition-structure-property relationships are characterized and analyzed experimentally and computationally. From the single-phase FCC CoCrFeNi alloy base, with Mn, Cu, Ti, Nb, Ta, Mo, W, Al, and Si as principal element alloying additions, we find (1) the extended Mn solubility in the single-phase FCC CoCrFeNi-Mn_x alloys, (2) the destabilizing behavior for most of the quinary and senary alloys, and (3) the distinctive solid-solution-strengthening effects in the alloys. In combining the computational methods, the HT-HIP-MSA can be systematic and economic to explore and refine the compositions, structures, and properties of structural high-entropy alloys.

Key words: High-entropy alloys, High-throughput, Composition-structure-property

L. Zhao, L. Jiang, L.X. Yang, H. Wang, W.Y. Zhang, G.Y. Ji, X. Zhou, W.A. Curtin, X.B. Chen, P.K. Liaw, S.Y. Chen, H.Z. Wang. High throughput synthesis enabled exploration of CoCrFeNi-based high entropy alloys[J]. J. Mater. Sci. Technol., 2022, 110: 269-282.

Figures/Tables 9

References 71

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Cell No.	Designed atomic percentage	Experimental Phases	Literature's Phases	Calculated phases	Experimental Hardness (HV)
1	Fe₁Cr₁Co₁Ni₁	FCC	FCC [1]	FCC
2	FeCrCoNiMo_0.5	FCC+μ	FCC+σ [48]	FCC+σ	403
3	FeCrCoNiMo_1.0	FCC+μ	FCC+σ+μ [49] FCC+BCC+Laves [50]	FCC+σ	619
4	FeCrCoNiMo_1.5	FCC+μ	-	FCC+σ	783
5	FeCrCoNiMo_2.0	FCC+BCC (Mo) +μ	-	FCC+σ	845
6	FeCrCoNiMo_2.5	FCC+BCC (Mo) +μ	-	FCC+σ1+σ2	857
7	FeCrCoNiMn_0.5	FCC	-	FCC	268
8	FeCrCoNiMn_1.0	FCC	FCC [51]	FCC	266
9	FeCrCoNiMn_1.5	FCC	-	FCC	266
10	FeCrCoNiMn_2.0	FCC	-	FCC	254
11	FeCrCoNiMn_2.5	FCC	-	FCC	248
12	FeCrCoNiMn_3.0	FCC	-	FCC	251
13	FeCrCoNiW_0.5	FCC+BCC (W) +μ	FCC+μ [37]	FCC+σ+μ	410
14	FeCrCoNiW_1.0	FCC+BCC (W) +μ	-	FCC+σ+μ	550
15	FeCrCoNiW_1.5	FCC+BCC (W) +μ	-	-	539
16	FeCrCoNiW_2.0	FCC+BCC (W) +μ	-	σ+μ	693
17	FeCrCoNiW_2.5	FCC+BCC (W) +μ	-	BCC+σ+μ	648
18	FeCrCoNiSi_0.5	FCC+IM	Si_0.2 FCC+Unknown [52]	FCC+Cr₃Si	728
19	FeCrCoNiSi_1.0	BCC+IM	-	FCC+Co₂Si+Cr₃Si	748
20	FeCrCoNiSi_1.5	IM	-	BCC+Co₂Si+Cr₃Si	911
21	FeCrCoNiSi_2.0	IM	-	Co₂Si+Cr₃Si+MSi	727
22	FeCrCoNiSi_2.5	IM	-	Co₂Si+MSi+Cr₃Si	850
23	FeCrCoNiSi_3.0	IM	-	MSi+Co₂Si+Cr₃Si	912
24	FeCrCoNiNb_0.5	FCC+Laves	FCC+Laves [27]	FCC+Laves	441
25	FeCrCoNiNb_1.0	FCC+Laves	FCC+Laves [53]	FCC+Laves	588
26	FeCrCoNiNb_1.5	FCC+Laves	-	FCC+Laves	658
27	FeCrCoNiNb_2.0	BCC (Nb) +Laves	-	Laves	650
28	FeCrCoNiNb_2.5	BCC (Nb) +Laves	-	Laves+μ	627
29	FeCrCoNiTi_0.5	FCC+HCP	FCC+Laves+R+σ [29]	FCC+BCC+Ni3Ti	416
30	FeCrCoNiTi_1.0	FCC+BCC+IMs	FCC [54]	FCC+BCC+σ	627
31	FeCrCoNiTi_1.5	BCC+ IMs	-	BCC1+BCC2	652
32	FeCrCoNiTi_2.0	BCC+ IMs	-	BCC1+BCC2+Laves	690
33	FeCrCoNiTi_2.5	BCC+ IMs	-	BCC1+BCC2+Laves	665
34	FeCrCoNiTa_0.5	FCC+Laves	FCC+Laves [27]	FCC+Laves	458
35	FeCrCoNiTa_1.0	FCC+Laves	FCC+Laves [27]	FCC+σ+Laves	643
36	FeCrCoNiTa_1.5	FCC+Laves	-	BCC+Laves	740
37	FeCrCoNiTa_2.0	BCC+Laves	-	Laves	730
38	FeCrCoNiTa_2.5	BCC+Laves	-	Laves+μ	706
39	FeCrCoNiCu_0.5	FCC1+FCC2	FCC [55]	FCC1+FCC2	218
40	FeCrCoNiCu_1.0	FCC1+FCC2	FCC1+FCC2 [35]	FCC1+FCC2	196
41	FeCrCoNiCu_1.5	FCC1+FCC2	-	FCC1+FCC2	184
42	FeCrCoNiCu_2.0	FCC1+FCC2	FCC1+FCC2 [56]	FCC1+FCC2	170
43	FeCrCoNiCu_2.5	FCC1+FCC2	Cu₄ FCC1+FCC2 [57]	FCC1+FCC2	160
44	FeCrCoNiAl_0.5	FCC	FCC [58] FCC+BCC [59]	FCC+BCC	332
45	FeCrCoNiAl_1.0	FCC+BCC+Order BCC	FCC+BCC [60]	BCC1+BCC2+σ	432
46	FeCrCoNiAl_1.5	BCC+Order BCC	BCC+OrderBCC [61]	BCC1+BCC2	463
47	FeCrCoNiAl_2.0	BCC+Order BCC	BCC+orderBCC [62]	BCC1+BCC2	481
48	FeCrCoNiAl_2.5	BCC+Order BCC	BCC [24]	BCC1+BCC3	478
49	FeCrCoNiAl_3.0	BCC+Order BCC	BCC [24]	BCC1+BCC3	535
50	FeCrCoNiMoMn	FCC+Oxide	FCC+BCC [63]	FCC+σ	479
51	FeCrCoNiMoW	FCC+BCC+Unknown	FCC+BCC [63]	BCC+FCC+σ	669
52	FeCrCoNiMoSi	FCC+HCP (Ni) +IM+Unknown	-	Cr₃Si+Co₂Si+σ	722
53	FeCrCoNiMoNb	Unknown	-	σ+Laves+Ni₃Nb	726
54	FeCrCoNiMoTi	FCC+BCC+HCP (Cr)	FCC+BCC [63]	BCC+Ni3Ti+σ	757
55	FeCrCoNiMoCu	FCC+Unknown	-	FCC1+FCC2+σ	391
56	FeCrCoNiMoTa	BCC(Mo)+FCC+HCP+Unknown	-	Laves+σ+μ+Ni3Ta	791
57	FeCrCoNiMoAl	BCC+σ	Mo_0.5Al BCC+σ [64]	BCC+σ	626
58	FeCrCoNiMnW	BCC (W) +FCC+HCP (Cr)	FCC+BCC [63]	FCC+BCC	453
59	FeCrCoNiMnSi	BCC+IM	-	FCC+Cr₃Si+MnNiSi	560
60	FeCrCoNiMnNb	FCC+HCP (Cr) +Unknown	-	FCC+Laves	549
61	FeCrCoNiMnTi	FCC+HCP (Mn) +IM	FCC [63]	FCC+BCC1+BCC2+σ	521
62	FeCrCoNiMnTa	FCC+BCC+HCP(Cr)+Unknown	-	FCC+σ+Laves	672
63	FeCrCoNiMnCu	FCC1(Cu)+FCC2	-	FCC1+FCC2	261
64	FeCrCoNiMnAl	FCC+BCC+Oxide	FCC+BCC [65]	BCC1+BCC2+σ	471
65	FeCrCoNiWSi	FCC+BCC+IM	-	FCC+Laves+Ni5Si2	737
66	FeCrCoNiWNb	BCC(W)+Unknown	-	FCC+Laves+μ	680
67	FeCrCoNiWTi	BCC(W)+HCP(Cr)	FCC+BCC [63]	BCC1+BCC2+Laves+Ni3Ti	735
68	FeCrCoNiWTa	BCC+Unknown	-	FCC+μ+σ+Laves	715
69	FeCrCoNiWCu	BCC+FCC+Unknown	-	FCC+μ+σ+CuB_A13	392
70	FeCrCoNiWAl	BCC(W)+BCC(Fe,Cr)+Unknown	-	BCC+R+μ+σ	566
71	FeCrCoNiSiNb	FCC +BCC+IM	-	Liquid+Laves+M11Si₈+Cr₃Si	794
72	FeCrCoNiSiTi	BCC(Fe,Cr)+FCC(Ti)+Oxide	-	Liquid+Laves+Cr₃Si+G	749
73	FeCrCoNiSiTa	BCC+IM+Unknown	-	Liquid+Laves+Cr₃Si	881
74	FeCrCoNiSiCu	FCC+IM	FCC1+FCC2+σ [66]	FCC1+FCC2+Co₂Si+Cr₃Si	574
75	FeCrCoNiSiAl	BCC+IM	BCC+σ [67]	BCC3+BCC2+Cr3Si+Co2Si	779
76	FeCrCoNiNbTi	BCC+IM	-	BCC+Laves+Ni3Ti	573
77	FeCrCoNiNbTa	BCC+IM+Unknown	-	Laves+σ+μ	650
78	FeCrCoNiNbCu	FCC+Laves+Unknown	- FCC+Laves [66]	FCC1+FCC2+Laves	438
79	FeCrCoNiNbAl	BCC+Unknown	BCC+Laves+B2 [68]	BCC1+BCC2+Laves	555
80	FeCrCoNiTiCu	FCC+Unknown	FCC+Laves [69]	BCC+FCC1+FCC2+σ+T6CuNiTi	488
81	FeCrCoNiTiAl	BCC	BCC1+BCC2 [70] BCC1+BCC2+Laves [54]	BCC1+BCC3	584
82	FeCrCoNiTiTa	FCC+BCC+HCP+Unknown	-	BCC+Laves+Liquid	680
83	FeCrCoNiTaCu	FCC+BCC+IM+Unknown	-	FCC1+FCC2+Laves+σ	485
84	FeCrCoNiTaAl	BCC +Oxide	-	BCC1+BCC3+Laves	614
85	FeCrCoNiAlCu	FCC1(Cu)+FCC2+BCC+IM	FCC+BCC [71]	FCC+BCC+σ+Liquid	385

Cell No.	Designed atomic percentage	Experimental Phases	Literature's Phases	Calculated phases	Experimental Hardness (HV)
1	Fe₁Cr₁Co₁Ni₁	FCC	FCC [1]	FCC
2	FeCrCoNiMo_0.5	FCC+μ	FCC+σ [48]	FCC+σ	403
3	FeCrCoNiMo_1.0	FCC+μ	FCC+σ+μ [49] FCC+BCC+Laves [50]	FCC+σ	619
4	FeCrCoNiMo_1.5	FCC+μ	-	FCC+σ	783
5	FeCrCoNiMo_2.0	FCC+BCC (Mo) +μ	-	FCC+σ	845
6	FeCrCoNiMo_2.5	FCC+BCC (Mo) +μ	-	FCC+σ1+σ2	857
7	FeCrCoNiMn_0.5	FCC	-	FCC	268
8	FeCrCoNiMn_1.0	FCC	FCC [51]	FCC	266
9	FeCrCoNiMn_1.5	FCC	-	FCC	266
10	FeCrCoNiMn_2.0	FCC	-	FCC	254
11	FeCrCoNiMn_2.5	FCC	-	FCC	248
12	FeCrCoNiMn_3.0	FCC	-	FCC	251
13	FeCrCoNiW_0.5	FCC+BCC (W) +μ	FCC+μ [37]	FCC+σ+μ	410
14	FeCrCoNiW_1.0	FCC+BCC (W) +μ	-	FCC+σ+μ	550
15	FeCrCoNiW_1.5	FCC+BCC (W) +μ	-	-	539
16	FeCrCoNiW_2.0	FCC+BCC (W) +μ	-	σ+μ	693
17	FeCrCoNiW_2.5	FCC+BCC (W) +μ	-	BCC+σ+μ	648
18	FeCrCoNiSi_0.5	FCC+IM	Si_0.2 FCC+Unknown [52]	FCC+Cr₃Si	728
19	FeCrCoNiSi_1.0	BCC+IM	-	FCC+Co₂Si+Cr₃Si	748
20	FeCrCoNiSi_1.5	IM	-	BCC+Co₂Si+Cr₃Si	911
21	FeCrCoNiSi_2.0	IM	-	Co₂Si+Cr₃Si+MSi	727
22	FeCrCoNiSi_2.5	IM	-	Co₂Si+MSi+Cr₃Si	850
23	FeCrCoNiSi_3.0	IM	-	MSi+Co₂Si+Cr₃Si	912
24	FeCrCoNiNb_0.5	FCC+Laves	FCC+Laves [27]	FCC+Laves	441
25	FeCrCoNiNb_1.0	FCC+Laves	FCC+Laves [53]	FCC+Laves	588
26	FeCrCoNiNb_1.5	FCC+Laves	-	FCC+Laves	658
27	FeCrCoNiNb_2.0	BCC (Nb) +Laves	-	Laves	650
28	FeCrCoNiNb_2.5	BCC (Nb) +Laves	-	Laves+μ	627
29	FeCrCoNiTi_0.5	FCC+HCP	FCC+Laves+R+σ [29]	FCC+BCC+Ni3Ti	416
30	FeCrCoNiTi_1.0	FCC+BCC+IMs	FCC [54]	FCC+BCC+σ	627
31	FeCrCoNiTi_1.5	BCC+ IMs	-	BCC1+BCC2	652
32	FeCrCoNiTi_2.0	BCC+ IMs	-	BCC1+BCC2+Laves	690
33	FeCrCoNiTi_2.5	BCC+ IMs	-	BCC1+BCC2+Laves	665
34	FeCrCoNiTa_0.5	FCC+Laves	FCC+Laves [27]	FCC+Laves	458
35	FeCrCoNiTa_1.0	FCC+Laves	FCC+Laves [27]	FCC+σ+Laves	643
36	FeCrCoNiTa_1.5	FCC+Laves	-	BCC+Laves	740
37	FeCrCoNiTa_2.0	BCC+Laves	-	Laves	730
38	FeCrCoNiTa_2.5	BCC+Laves	-	Laves+μ	706
39	FeCrCoNiCu_0.5	FCC1+FCC2	FCC [55]	FCC1+FCC2	218
40	FeCrCoNiCu_1.0	FCC1+FCC2	FCC1+FCC2 [35]	FCC1+FCC2	196
41	FeCrCoNiCu_1.5	FCC1+FCC2	-	FCC1+FCC2	184
42	FeCrCoNiCu_2.0	FCC1+FCC2	FCC1+FCC2 [56]	FCC1+FCC2	170
43	FeCrCoNiCu_2.5	FCC1+FCC2	Cu₄ FCC1+FCC2 [57]	FCC1+FCC2	160
44	FeCrCoNiAl_0.5	FCC	FCC [58] FCC+BCC [59]	FCC+BCC	332
45	FeCrCoNiAl_1.0	FCC+BCC+Order BCC	FCC+BCC [60]	BCC1+BCC2+σ	432
46	FeCrCoNiAl_1.5	BCC+Order BCC	BCC+OrderBCC [61]	BCC1+BCC2	463
47	FeCrCoNiAl_2.0	BCC+Order BCC	BCC+orderBCC [62]	BCC1+BCC2	481
48	FeCrCoNiAl_2.5	BCC+Order BCC	BCC [24]	BCC1+BCC3	478
49	FeCrCoNiAl_3.0	BCC+Order BCC	BCC [24]	BCC1+BCC3	535
50	FeCrCoNiMoMn	FCC+Oxide	FCC+BCC [63]	FCC+σ	479
51	FeCrCoNiMoW	FCC+BCC+Unknown	FCC+BCC [63]	BCC+FCC+σ	669
52	FeCrCoNiMoSi	FCC+HCP (Ni) +IM+Unknown	-	Cr₃Si+Co₂Si+σ	722
53	FeCrCoNiMoNb	Unknown	-	σ+Laves+Ni₃Nb	726
54	FeCrCoNiMoTi	FCC+BCC+HCP (Cr)	FCC+BCC [63]	BCC+Ni3Ti+σ	757
55	FeCrCoNiMoCu	FCC+Unknown	-	FCC1+FCC2+σ	391
56	FeCrCoNiMoTa	BCC(Mo)+FCC+HCP+Unknown	-	Laves+σ+μ+Ni3Ta	791
57	FeCrCoNiMoAl	BCC+σ	Mo_0.5Al BCC+σ [64]	BCC+σ	626
58	FeCrCoNiMnW	BCC (W) +FCC+HCP (Cr)	FCC+BCC [63]	FCC+BCC	453
59	FeCrCoNiMnSi	BCC+IM	-	FCC+Cr₃Si+MnNiSi	560
60	FeCrCoNiMnNb	FCC+HCP (Cr) +Unknown	-	FCC+Laves	549
61	FeCrCoNiMnTi	FCC+HCP (Mn) +IM	FCC [63]	FCC+BCC1+BCC2+σ	521
62	FeCrCoNiMnTa	FCC+BCC+HCP(Cr)+Unknown	-	FCC+σ+Laves	672
63	FeCrCoNiMnCu	FCC1(Cu)+FCC2	-	FCC1+FCC2	261
64	FeCrCoNiMnAl	FCC+BCC+Oxide	FCC+BCC [65]	BCC1+BCC2+σ	471
65	FeCrCoNiWSi	FCC+BCC+IM	-	FCC+Laves+Ni5Si2	737
66	FeCrCoNiWNb	BCC(W)+Unknown	-	FCC+Laves+μ	680
67	FeCrCoNiWTi	BCC(W)+HCP(Cr)	FCC+BCC [63]	BCC1+BCC2+Laves+Ni3Ti	735
68	FeCrCoNiWTa	BCC+Unknown	-	FCC+μ+σ+Laves	715
69	FeCrCoNiWCu	BCC+FCC+Unknown	-	FCC+μ+σ+CuB_A13	392
70	FeCrCoNiWAl	BCC(W)+BCC(Fe,Cr)+Unknown	-	BCC+R+μ+σ	566
71	FeCrCoNiSiNb	FCC +BCC+IM	-	Liquid+Laves+M11Si₈+Cr₃Si	794
72	FeCrCoNiSiTi	BCC(Fe,Cr)+FCC(Ti)+Oxide	-	Liquid+Laves+Cr₃Si+G	749
73	FeCrCoNiSiTa	BCC+IM+Unknown	-	Liquid+Laves+Cr₃Si	881
74	FeCrCoNiSiCu	FCC+IM	FCC1+FCC2+σ [66]	FCC1+FCC2+Co₂Si+Cr₃Si	574
75	FeCrCoNiSiAl	BCC+IM	BCC+σ [67]	BCC3+BCC2+Cr3Si+Co2Si	779
76	FeCrCoNiNbTi	BCC+IM	-	BCC+Laves+Ni3Ti	573
77	FeCrCoNiNbTa	BCC+IM+Unknown	-	Laves+σ+μ	650
78	FeCrCoNiNbCu	FCC+Laves+Unknown	- FCC+Laves [66]	FCC1+FCC2+Laves	438
79	FeCrCoNiNbAl	BCC+Unknown	BCC+Laves+B2 [68]	BCC1+BCC2+Laves	555
80	FeCrCoNiTiCu	FCC+Unknown	FCC+Laves [69]	BCC+FCC1+FCC2+σ+T6CuNiTi	488
81	FeCrCoNiTiAl	BCC	BCC1+BCC2 [70] BCC1+BCC2+Laves [54]	BCC1+BCC3	584
82	FeCrCoNiTiTa	FCC+BCC+HCP+Unknown	-	BCC+Laves+Liquid	680
83	FeCrCoNiTaCu	FCC+BCC+IM+Unknown	-	FCC1+FCC2+Laves+σ	485
84	FeCrCoNiTaAl	BCC +Oxide	-	BCC1+BCC3+Laves	614
85	FeCrCoNiAlCu	FCC1(Cu)+FCC2+BCC+IM	FCC+BCC [71]	FCC+BCC+σ+Liquid	385

Element n	Apparent volume Ån(Å3)
Ni	10.94 [45]
Co	11.12 [45]
Fe	12.09 [45]
Cr	12.27 [45]
Mn	12.60 [45]
Al	14.10*
Cu	12.80*(11.80 [43])
Mo	15.91*
Ti	16.02*

Element n	Apparent volume Ån(Å3)
Ni	10.94 [45]
Co	11.12 [45]
Fe	12.09 [45]
Cr	12.27 [45]
Mn	12.60 [45]
Al	14.10*
Cu	12.80*(11.80 [43])
Mo	15.91*
Ti	16.02*