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

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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 Gd ₂Co ₁₇based intermetallic compound, and the effect of high configuration entropy on the structural stabilization and room-temperature magnetic properties of Gd ₂Co ₁₇based 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 Gd ₂Co ₁₇based 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 Gd ₂Co ₁₇based intermetallics can be stabilized into rhombohedral Th ₂Zn ₁₇-type with R _A> 1.416 or hexagonal Th ₂Ni ₁₇-type with R _A< 1.4105. According to thermodynamic calculations of entropized Gd ₂Co ₁₇intermeatllics, the atomic radius difference Δ rranges 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.

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

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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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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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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

DownLoad: CSV

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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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

DownLoad: CSV

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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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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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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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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