Structures and room-temperature magnetic properties of entropy-modulated  Gd<sub>2</sub>Co<sub>17</sub> based intermetallic compounds

Dong Xiao-Peng; Zhao Xing; Yin Lin-Han; Peng Si-Qi; Wang Jing-Nan; Guo Yong-Quan

doi:10.7498/aps.72.20221995

Abstract

The entropy-modulated material has been a hot topic due to its unique design concept and excellent properties. However, previous studies of entropy-modulated materials mainly focused on the alloys with simple face-centered cubic, or body-centered cubic, or hexagonal close-packed structures. In this work, the design concept of entropy-modulation is introduced into Gd₂Co₁₇ based intermetallic compound, and the effect of high configuration entropy on the structural stabilization and room-temperature magnetic properties of Gd₂Co₁₇ based intermetallic compound are studied systematically.The samples are prepared by vacuum Arc melting technology in an ultrahigh-purity Ar atmosphere and followed by annealing at 1000 ℃ for 8 days and finally by quenching in cool water. The fine powders are prepared by grinding the ingots in an agate mortar. The powder XRD and SEM-EDS are used to check the crystal structures and chemical compositions. To study the magnetic properties, the column-like samples are prepared by mixing the fine powder and epoxy with a weight ratio of 1∶1, and then aligned under an applied field of 1 T at room temperature.The high configuration entropy is found to play an important role in the structural stabilization and magnetic properties of Gd₂Co₁₇ based medium- and high-entropy intermetallic compounds. The XRD patterns and Rietveld structural refinement results confirm that all the samples are single-phase. The structure depends on the effective atomic radius R_A, the structure of entropized Gd₂Co₁₇ based intermetallics can be stabilized into rhombohedral Th₂Zn₁₇-type with R_A> 1.416 or hexagonal Th₂Ni₁₇-type with R_A< 1.4105. According to thermodynamic calculations of entropized Gd₂Co₁₇ intermeatllics, the atomic radius difference Δr ranges from 0.55% to 1.81%, and the mixing enthalpy $ \Delta {{\boldsymbol{H}}}_{{\rm{m}}{\rm{i}}{\rm{x}}} $ is corresponding to 0 for the rare earth site, –4 to –1 kJ/mol for the transition metal site, and –8.54 to –5.13 kJ/mol between rare earth and transition metal sites. It is suggested that all the thermodynamic parameters meet the criteria for the formation of single-phase medium- and high-entropy intermetallic compounds. The configuration entropy changes from 0.69R to 1.39R. The room temperature magnetic properties are significantly improved by the modulation of entropized design at rare earth and transition metal sublattices. The entropization enhances the saturation moments of all samples, which can be explained with a modified magnetic valence model. The value of ${N}_{{\rm{sp}}}^{\uparrow }$ (the number of the electrons in the unpolarized sp conduction bands) increases from 0.3 to 0.4 after entropization, the indirect interaction between rare earth and transition metal sublattice is increased, the spin moment of s conducting electron as a medium of two sublattices is enhanced, and the magnetic moment is increased. The entropization also induces magnetic anisotropy to transform from basal plane to easy axis for the entropized design at transition metal sublattice and the coercivity of rare earth to increase.

Keywords:

Authors and contacts

School of Energy Power and Mechanical Engineering, North China Electric Power University, Beijing 102206, China

Corresponding author: Guo Yong-Quan, yqguo@ncepu.edu.cn

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图 1 熵调控Gd₂Co₁₇系列样品XRD图谱　(a) Gd₂Co₁₇; (b) Gd₂(Co_1/2Fe_1/2)₁₇; (c) Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇; (d) Gd₂(Co_1/4Fe_1/4Ni_1/4Mn_1/4)₁₇; (e) (Gd_1/2Tb_1/2)₂Co₁₇; (f) (Gd_1/3Tb_1/3Dy_1/3)₂Co₁₇; (g) (Gd_1/4Tb_1/4Dy_1/4Ho_1/4)₂Co₁₇

Figure 1. The XRD patterns of the entropized Gd₂Co₁₇ intermetallic compounds: (a) Gd₂Co₁₇; (b) Gd₂(Co_1/2Fe_1/2)₁₇; (c) Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇; (d) Gd₂(Co_1/4Fe_1/4Ni_1/4Mn_1/4)₁₇; (e) (Gd_1/2Tb_1/2)₂Co₁₇; (f) (Gd_1/3Tb_1/3Dy_1/3)₂Co₁₇; (g) (Gd_1/4Tb_1/4Dy_1/4Ho_1/4)₂Co₁₇.

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图 2 代表性样品的精修XRD图谱　(a) Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇; (b) Gd₂(Co_1/4Fe_1/4Ni_1/4Mn_1/4)₁₇

Figure 2. Refined XRD pattern of typical samples: (a) Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇; (b) Gd₂(Co_1/4Fe_1/4Ni_1/4Mn_1/4)₁₇.

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图 3 代表性样品的SEM图像、EDS图谱　(a) Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇; (b) Gd₂(Co_1/4Fe_1/4Ni_1/4Mn_1/4)₁₇

Figure 3. SEM image and EDS pattern of typical samples: (a) Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇; (b) Gd₂(Co_1/4Fe_1/4Ni_1/4 Mn_1/4)₁₇.

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图 4 Gd₂(T₁, T₂, ···, T_n)₁₇系列取向样品XRD图谱　(a) Gd₂Co₁₇; (b) Gd₂(Co_1/2Fe_1/2)₁₇; (c) Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇; (d) Gd₂(Co_1/4Fe_1/4Ni_1/4Mn_1/4)₁₇

Figure 4. XRD patterns of aligned Gd₂(T₁, T₂, ···, T_n)₁₇ intermetallic compounds: (a) Gd₂Co₁₇; (b) Gd₂(Co_1/2Fe_1/2)₁₇; (c) Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇; (d) Gd₂(Co_1/4Fe_1/4Ni_1/4Mn_1/4)₁₇.

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图 5 (R₁, R₂, ···, R_n)₂Co₁₇系列取向样品XRD图谱　(a) (Gd_1/2Tb_1/2)₂Co₁₇; (b) (Gd_1/3Tb_1/3Dy_1/3)₂Co₁₇; (c) (Gd_1/4Tb_1/4Dy_1/4Ho_1/4)₂Co₁₇

Figure 5. XRD patterns of aligned (R₁, R₂, ···, R_n)₂Co₁₇ intermetallic compounds: (a) (Gd_1/2Tb_1/2)₂Co₁₇; (b) (Gd_1/3Tb_1/3Dy_1/3)₂Co₁₇;(c) (Gd_1/4Tb_1/4Dy_1/4Ho_1/4)₂Co₁₇.

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图 6 熵调控Gd₂Co₁₇系列取向样品平行和垂直于外加磁场方向的磁滞回线　(a)Gd₂(Co_1/2Fe_1/2)₁₇; (b) Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇; (c) Gd₂(Co_1/4Fe_1/4Ni_1/4Mn_1/4)₁₇; (d) (Gd_1/2Tb_1/2)₂Co₁₇; (e) (Gd_1/3Tb_1/3Dy_1/3)₂Co₁₇; (f) (Gd_1/4Tb_1/4Dy_1/4Ho_1/4)₂Co₁₇

Figure 6. Hysteresis loops of entropized Gd₂Co₁₇ samples with magnetic aligned direction parallel and perpendicular to the direction of applied magnetic field: (a) Gd₂(Co_1/2Fe_1/2)₁₇; (b) Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇; (c) Gd₂(Co_1/4Fe_1/4Ni_1/4Mn_1/4)₁₇; (d) (Gd_1/2Tb_1/2)₂Co₁₇; (e) (Gd_1/3Tb_1/3Dy_1/3)₂Co₁₇; (f) (Gd_1/4Tb_1/4Dy_1/4Ho_1/4)₂Co₁₇.

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图 7 Gd₂(T₁, T₂, ···, T_n)₁₇系列取向样品的磁晶各向异性场　(a) Gd₂(Co_1/2Fe_1/2)₁₇; (b) Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇; (c) Gd₂(Co_1/4Fe_1/4Ni_1/4Mn_1/4)₁₇

Figure 7. Magnetic anisotropy field of field aligned Gd₂(T₁, T₂, ···, T_n)₁₇: (a) Gd₂(Co_1/2Fe_1/2)₁₇; (b) Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇; (c) Gd₂(Co_1/4Fe_1/4Ni_1/4Mn_1/4)₁₇.

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图 8 Gd₂Co₁₇系列取向样品的拟合磁化曲线　(a) Gd₂(Fe_1/2Co_1/2)₁₇; (b) Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇; (c) Gd₂(Co_1/4Fe_1/4Ni_1/4Mn_1/4)₁₇; (d) (Gd_1/2Tb_1/2)₂Co₁₇; (e) (Gd_1/3Tb_1/3Dy_1/3)₂Co₁₇; (f) (Gd_1/4Tb_1/4Dy_1/4Ho_1/4)₂Co₁₇

Figure 8. Fitted magnetization curves of field aligned entropized Gd₂Co₁₇: (a) Gd₂(Co_1/2Fe_1/2)₁₇; (b) Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇; (c) Gd₂(Co_1/4Fe_1/4Ni_1/4Mn_1/4)₁₇; (d) (Gd_1/2Tb_1/2)₂Co₁₇; (e) (Gd_1/3Tb_1/3Dy_1/3)₂Co₁₇; (f) (Gd_1/4Tb_1/4Dy_1/4Ho_1/4)₂Co₁₇.

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表 1 熵调控Gd₂Co₁₇系列样品热力学参数

Table 1. Thermodynamic parameters of entropized Gd₂Co₁₇ intermetallic compounds.

样品	原子半径差 ${{\Delta } }r$/%	${\rm{混} }{\rm{合} }{\rm{焓} }\Delta {{\boldsymbol{H}}}_{ {\rm{m} }{\rm{i} }{\rm{x} } }$/(kJ·mol^–1)			混合熵 $\Delta {S}_{ {\rm{mix} } } /R$
样品	原子半径差 ${{\Delta } }r$/%	稀土位	金属位	稀土位-金属位	混合熵 $\Delta {S}_{ {\rm{mix} } } /R$
Gd₂Co₁₇	—	—	—	–8.29	0
Gd₂(Co_1/2Fe_1/2)₁₇	0.79	—	–1.00	–5.13	0.69
Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇	0.99	—	–1.33	–7.85	1.10
Gd₂(Co_1/4Fe_1/4Ni_1/4Mn_1/4)₁₇	1.81	—	–4.00	–8.38	1.39
(Gd_1/2Tb_1/2)₂Co₁₇	0.55	0	—	–8.48	0.69
(Gd_1/3Tb_1/3Dy_1/3)₂Co₁₇	0.69	0	—	–8.54	1.10
(Gd_1/4Tb_1/4Dy_1/4Ho_1/4)₂Co₁₇	0.83	0	—	–8.48	1.39

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表 2 熵调控Gd₂Co₁₇系列样品晶格参数、品质因子和可信度因子

Table 2. Lattice parameter, merit factors M and smith factor F of entropized Gd₂Co₁₇ intermetallic compounds.

样品	a/Å	c/Å	V/Å³	M(20)	F(20)
Gd₂Co₁₇	8.378(0)	12.206(6)	742.0(0)	28	27
Gd₂(Co_1/2Fe_1/2)₁₇	8.458(0)	12.409(6)	768.8(2)	17	14
Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇	8.444(4)	12.254(1)	756.6(7)	23	23
Gd₂(Co_1/4Fe_1/4Ni_1/4Mn_1/4)₁₇	8.507(0)	8. 267(8)	518.1(7)	49	39
(Gd_1/2Tb_1/2)₂Co₁₇	8.332(3)	8.133(1)	489.0(1)	46	52
(Gd_1/3Tb_1/3Dy_1/3)₂Co₁₇	8.363(1)	12.203(0)	739.1(5)	28	28
(Gd_1/4Tb_1/4Dy_1/4Ho_1/4)₂Co₁₇	8.333(6)	8.125(6)	488.7(1)	44	45

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表 3 选取样品的元素组成

Table 3. Element compositions of typical samples.

元素	Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇		Gd₂(Co_1/4Fe_1/4Ni_1/4Mn_1/4)₁₇
元素	质量百分比/%	原子百分比/%	质量百分比/%	原子百分比/%
Gd	24.5	10.6	26.0	11.3
Co	26.1	30.3	18.9	21.9
Fe	24.0	29.4	16.9	20.7
Ni	25.4	29.6	20.1	23.4
Mn	—	—	18.1	22.7

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表 4 具有菱方结构的样品的精修晶体学数据

Table 4. Refined crystallographic data of samples with rhombohedral structure.

样品		Gd₂Co₁₇	Gd₂(Co_1/2Fe_1/2)₁₇	Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇	(Gd_1/3Tb_1/3Dy_1/3)₂Co₁₇
	空间群	${R}\bar3{m}$	${R}\bar3{m}$	${R}\bar{\text{3} }{m}$	${R}\bar3{m}$
	a/Å	8.375(2)	8.454(5)	8.444(7)	8.358(0)
	c/Å	12.200(4)	12.413(7)	12.254(3)	12.185(7)
	V/Å³	741.131(2)	768.436(1)	756.817(0)	737.200(9)
	稀土位	Gd	Gd	Gd	Gd, Tb, Dy
	6c (0, 0, z)	(z = 0.34369)	(z = 0.34188)	(z = 0.33731)	(z = 0.34197)
	占位率/%	100	100	100	各33.33
	金属位	Co	Co, Fe	Fe, Co, Ni	Co
	6c (0, 0, z)	(z = 0.09431)	(z = 0.08016)	(z = 0.08100)	(z = 0.09567)
	占位率/%	100	各50	各33.33	100
	9d (1/2, 0, 1/2)	—	—	—	—
	占位率/%	100	各50	各33.33	100
	18f (x, 0, 0)	(x = 0.28942)	(x = 0.30352)	(x = 0.30607)	(x = 0.29175)
	占位率/%	100	各50	各33.33	100
	18h (x, 1–x, z)	(x = 0.16826; z = 0.48728)	(x = 0.50226; z = 0.15830)	(x = 0.16629; z = 0.49090)	(x = 0.16783; z = 0.48701)
	占位率/%	100	各50	各33.33	100
	R_p/%	5.144	8.110	8.830	5.605
	R_WP/%	6.865	10.611	12.690	7.057

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表 5 具有六方结构的样品的精修晶体学数据

Table 5. Refined crystallographic data of samples with hexagonal structure.

样品	Gd₂(Co_1/4Fe_1/4Ni_1/4Mn_1/4)₁₇	(Gd_1/2Tb_1/2)₂Co₁₇	(Gd_1/4Tb_1/4Dy_1/4Ho_1/4)₂Co₁₇
空间群	P6₃/mmc	P6₃/mmc	P6₃/mmc
a/Å	8.501(6)	8.329(5)	8.332(9)
c/Å	8.265(3)	8.130(4)	8.124(4)
V/Å³	517.357(3)	488.512(1)	488.561(0)
稀土位	Gd	Gd, Tb	Gd, Tb, Dy, Ho
2b (0, 0, 1/4)	—	—	—
占位率/%	100	各50	各25
2d (1/3, 2/3, 3/4)	—	—	—
占位率/%	100	各50	各25
金属位	Fe, Co, Ni, Mn	Co	Co
4f (1/3, 2/3, z)	(z = 0.14285)	(z = 0.12127)	(z = 0.13757)
占位率/%	各25	100	100
6g (1/2, 0, 0)	—	—	—
占位率/%	各25	100	100
12j (x, y, 1/4)	(x = 0.32333; y = –0.02248)	(x = 0.33032; y = 0.96090)	(x = 0.32409; y = 0.96806)
占位率/%	各25	100	100
12k (x, 2x, z)	(x = 0.16182; z = –0.11890)	(x = 0.16585; z = 0.98326)	(x = 0.16655; z = 0.98716)
占位率/%	各25	100	100
R_p/%	7.006	8.07	9.07
R_WP/%	8.942	10.50	11.80

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表 6 熵调控Gd₂Co₁₇系列样品有效原子半径R_A

Table 6. Effective radius ratio R_A of entropized Gd₂Co₁₇ intermetallic compounds.

样品	晶体结构	有效原子半径R_A
Gd₂Co₁₇	菱方	1.4262
Gd₂(Co_1/2Fe_1/2)₁₇	菱方	1.4330
Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇	菱方	1.4334
Gd₂(Co_1/4Fe_1/4Ni_1/4Mn_1/4)₁₇	六方	1.3996
(Gd_1/2Tb_1/2)₂Co₁₇	六方	1.4166
(Gd_1/3Tb_1/3Dy_1/3)₂Co₁₇	菱方	1.4105
(Gd_1/4Tb_1/4Dy_1/4Ho_1/4)₂Co₁₇	六方	1.4056

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表 7 熵调控Gd₂Co₁₇系列取向样品磁化曲线拟合参数

Table 7. Results of fitted magnetization parameters of field aligned entropized Gd₂Co₁₇.

取向样品	拟合度	Nμ/(emu·g^–1)	Nμ/μ_B
Gd₂(Co_1/2Fe_1/2)₁₇	0.99887	109.56395±0.02882	25.30
Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇	0.99630	74.23084±0.03279	17.19
Gd₂(Co_1/4Fe_1/4Ni_1/4Mn_1/4)₁₇	0.99644	68.97675±0.02946	15.87
(Gd_1/2Tb_1/2)₂Co₁₇	0.99985	104.73245±0.01038	24.71
(Gd_1/3Tb_1/3Dy_1/3)₂Co₁₇	0.99844	71.71314±0.01977	16.96
(Gd_1/4Tb_1/4Dy_1/4Ho_1/4)₂Co₁₇	0.99837	83.60305±0.02565	19.81

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表 8 R₂T₁₇金属间化合物的室温磁性能

Table 8. Magnetic properties of R₂T₁₇ at room temperature.

二元R₂T₁₇	晶体结构	饱和磁矩Nμ/μ_B	居里温度T_c/K	磁各向异性
Gd₂Co₁₇	菱方	13.5—14.4	1209—1240	基面
Gd₂Fe₁₇	六方	21—21.5	460—485	基面
Gd₂Ni₁₇	六方	8.8—9.36	187—205	—
Tb₂Co₁₇	菱方	8.4—10.7	1180—1195	基面
Dy₂Co₁₇	六方	7—8.3	1152—1188	基面
Ho₂Co₁₇	六方	5.8—7.7	1173—1183	基面
熵调控Gd₂Co₁₇	晶体结构	饱和磁矩Nμ/μ_B	理论磁矩Nμ/μ_B	磁各向异性
Gd₂(Co_1/2Fe_1/2)₁₇	菱方	25.30	17.25—17.95	易轴
Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇	菱方	17.19	14.43—15.09	易轴
Gd₂(Co_1/4Fe_1/4Ni_1/4Mn_1/4)₁₇	六方	15.87	—	易轴
(Gd_1/2Tb_1/2)₂Co₁₇	六方	24.71	10.95—12.55	基面
(Gd_1/3Tb_1/3Dy_1/3)₂Co₁₇	菱方	16.96	9.63—12.87	基面
(Gd_1/4Tb_1/4Dy_1/4Ho_1/4)₂Co₁₇	六方	19.81	8.68—10.28	基面

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表 9 熵调控Gd₂Co₁₇系列样品饱和磁矩计算结果

Table 9. Calculated moments of entropized Gd₂Co₁₇ intermetallic.

样品	实验磁矩/μ_B	理论磁矩/μ_B	$ {N}_{{\rm{s}}{\rm{p}}}^{\uparrow } $
Gd₂Co₁₇	13.5—14.4	14.40	0.30
Gd₂(Co_1/2Fe_1/2)₁₇	25.30	26.70	0.40
Gd₂(Co_1/3Fe_1/3Ni_1/3)₁₇	17.19	18.20	0.40
Gd₂(Co_1/4Fe_1/4Ni_1/4Mn_1/4)₁₇	15.87	13.95	0.40

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Structures and room-temperature magnetic properties of entropy-modulated Gd₂Co₁₇ based intermetallic compounds

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Structures and room-temperature magnetic properties of entropy-modulated Gd2Co17 based intermetallic compounds

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Structures and room-temperature magnetic properties of entropy-modulated Gd₂Co₁₇ based intermetallic compounds