The Ce-Ni-Si system as a representative of the rare earth-Ni-Si family: Isothermal section and new rare-earth nickel silicides

doi:10.1016/j.jssc.2016.09.001

Journal of Solid State Chemistry

Volume 243, November 2016, Pages 290-303

https://doi.org/10.1016/j.jssc.2016.09.001 Get rights and content

Highlights

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Ce-Ni-Si isothermal section was obtained at 870/1070 K.
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Twenty one known ternary cerium nickel silicides were confirmed in Ce-Ni-Si.
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Five new cerium nickel silicides were detected in Ce-Ni-Si.
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Eleven new rare earth nickel silicides were detected in R-Ni-Si.
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Magnetic properties of eight rare earth nickel silicides were investigated.

Abstract

The Ce-Ni-Si system has been investigated at 870/1070 K by X-ray and microprobe analyses. The existence of the known compounds, i.e.: Ce₂Ni_15.8Si_1.2 (Th₂Ni₁₇-type), Ce₂Ni_15-14Si_2-3 (Th₂Zn₁₇-type), CeNi_8.6Si_2.4 (BaCd₁₁-type), CeNi_8.8Si_4.2 (LaCo₉Si₄-type), CeNi₆Si₆ (CeNi₆Si₆-type), CeNi₅Si_1-0.3 (TbCu₇-type), CeNi₄Si (YNi₄Si-type), CeNi₂Si₂ (CeGa₂Al₂-type), Ce₂Ni₃Si₅ (U₂Co₃Si₅-type), Ce₃Ni₆Si₂ (Ce₃Ni₆Si₂-type), Ce₃Ni₄Si₄ (U₃Ni₄Si₄-type), CeNiSi₂ (CeNiSi₂-type), ~CeNi_1.3Si_0.7 (unknown type structure), Ce₆Ni₇Si₄ (Pr₆Ni₇Si₄-type), CeNiSi (LaPtSi-type), CeNi_0.8-0.3Si_1.2-1.7 (AlB₂-type), ~Ce₂Ni₂Si (unknown type structure), ~Ce_4.5Ni_3.5Si₂ (unknown type structure), Ce₁₅Ni₇Si₁₀ (Pr₁₅Ni₇Si₁₀-type), Ce₅Ni_1.85Si₃ (Ce₅Ni_1.85Si₃-type), Ce₆Ni_1.4Si_3.4 (Ce₆Ni_1.67Si₃-type), Ce₇Ni₂Si₅ (Ce₇Ni₂Si₅-type) and Ce₃NiSi₃ (Y₃NiSi₃-type) has been confirmed in this section.

Moreover, the type structure has been determined for ~Ce₂Ni₂Si (Mo₂NiB₂-type Ce₂Ni_2.5Si_0.5) and ~Ce_4.5Ni_3.5Si₂ (W₃CoB₃-type Ce₃Ni_3-2.7Si_1-1.3) and new ternary phases Ce₂Ni_6.25Si_0.75 (Gd₂Co₇-type), CeNi_7-7.6Si_6-5.4 (GdNi₇Si₆-type) and ~Ce₂₇Ni₄₂Si₃₁ (unknown type structure) have been identified in this system.

Quasi-binary phases, solid solutions, were detected at 870/1070 K for CeNi₅, CeNi₃ and CeSi₂; while no appreciable solubility was observed for the other binary compounds of the Ce-Ni-Si system.

As a prolongation of Rare Earth-Ni-Si system’s isostructural rows, LaNi₇Si₆ and YNi_6.6Si_6.1 (GdNi₇Si₆-type), ScNi₆Si₆ (YCo₆Ge₆-type), NdNi₆Si₆ (YNi₆Si₆-type), {Tb, Ho}₂Ni₁₅Si₂ (Th₂Zn₁₇-type), Nd₂Ni_2.3Si_0.7 and Sm₂Ni_2.2Si_0.8 (Mo₂NiB₂-type), Nd₃Ni_2.55Si_1.45 (W₃CoB₃-type) and {Tb, Dy}₇Ni₅₀Si₁₉ (Y₇Ni₄₉Si₂₀-type) compounds were synthesized and investigated.

Magnetic properties of the CeNi₆Si₆, CeNi₇Si₆, CeNi_8.8Si_4.2, Ce₆Ni₇Si₄, CeNi₅Si, Ce₂Ni_2.5Si_0.5, Nd₂Ni_2.3Si_0.7 and Dy₇Ni₅₀Si₁₉ compounds have also been investigated and are presented here.

Graphical abstract

Introduction

The Ce-containing compounds are interesting since they often exhibit the mixed valent state [1], [2], Kondo effect and heavy-fermion behavior [3], [4]. The Ce-Ni-Si system and ternary compounds of this system supplement the series of R-Ni-Si sections with ternary rare earth silicides [5], [6], [7], [8], [9], [10], [11], [12], [13], [14], [15], [16], [17], [18], [19], [20], including recently reported Y₇Ni₄₉Si₂₀-type Y₇(Ni_1−xSi_x)₆₉ (x≈0.287) compound by Demchenko et al. [14].

The study of the phase diagrams or isothermal cross-sections of rare earth (R) systems, along with the full characterization of the crystal structure of the formed compounds and the investigation of their magnetic properties is an important step towards both fundamental and practical goals in the materials science, solid state chemistry and physics.

The isothermal section of Ce-Ni-Si at 870 K was early investigated by Bodak et al. [21], [22]. The ternary compounds CeNi_8.5Si_4.5 [23], CeNi₈Si₅ [21], CeNi_8.6Si_2.4 [24], Ce₂Ni₁₅Si₂ [25], CeNi₄Si [26], Ce₃Ni₂Si₈ [27], CeNi₂Si₂ [28], CeNiSi₂ [29], Ce₃Ni₆Si₂ [30], CeNiSi [31], Ce₃Ni₄Si₄ [22], CeNi_0.5Si_1.5 [32], Ce₆Ni₇Si₄ [21], Ce₇Ni₂Si₅ [33], Ce₁₅Ni_4-9Si_13-8 [11], [13], [28], [34], Ce₅Ni_2−xSi₃ [35], [43], [44] and Ce₆Ni_2−xSi₃ [36] were detected in this ternary system at 670 K and 1070 K, like the compounds with unknown type structure ~CeNi_1.3Si_0.7, ~Ce₂Ni₂Si, ~Ce_4.5Ni_3.5Si₂, and Ce₁₀Ni₃Si₇. Later, Ce₂Ni₁₅Si₂ compound has been found to have Th₂Zn₁₇-type structure [37] and ~Ce₁₀Ni₃Si₇ has been found to have Y₃NiSi₃-type structure [38]. Also Ce₁₄Ni₈Si₉-type Ce₁₄Ni₈Si₉ [11], [12], [13], YNi₄Si-type CeNi₄Si [18], [19], tetragonal derivative of NaZn₁₃-type structure, the CeNi₆Si₆ [20], U₂Co₃Si₅-type Ce₂Ni₃Si₅ [39] and TbCu₇-type CeNi₅Si [40] compounds were detected in Ce-Ni-Si system.

These data allow careful re-investigation of Ce-Ni-Si system with using of Ce-Ni, Ce-Si and Ni-Si binary systems that have been studied in detail and published in several works [11], [12], [13], [41].

As shown in [42] for rare earth nickel germanides, as a rule, the rare-earth sequence Eu-La-Ce-Pr-Nd-Sm-Gd-Tb-Y-Dy-Ho-Er-Tm-Yb-Lu-Sc) corresponds to the continuous row of isostructural compounds (rule of isostructural rows) with decrease in their unit cell parameters when Ce and Yb are in the trivalent state. This sequence corresponds to the W→α-La→Sm→Mg structural sequence observed for rare-earth metals and one could argue that this sequence correlates with the structure of the binary and ternary compounds. Thus, the series of known ternary rare-earth compounds can be used to predict the formation of isostoichiometric and isostructural compounds in other systems including R-Ni-Si as used and shown in the present work (Table 1).

The magnetic, thermoelectric and Kondo effect properties of several ternary compounds pertaining to the Ce-Ni-Si systems were also investigated [9], [11], [18], [19], [20], [23], [43], [44], [45], [46], [47], [48], [49], [50], [51], like the magnetic properties of other ternary rare earth nickel silicides [see e.g. [9], [10], [15], [16], [17], [18], [19], [20]].

As new compounds were detected in Ce-Ni-Si system, a careful reinvestigation of the isothermal section of the Ce-Ni-Si system at 870/1070 K, together with an updated assessment of the existing phases, was considered necessary. Moreover, as a part of this work, magnetic properties of some ternary rare earth nickel silicides have been also established.

The newly identified compounds of R-Ni-Si systems partially supplement the isostructural rows of known rare earth compounds. On the other hand, the results obtained from the magnetic measurements give supplementary information on the magnetic data of ternary rare earth compounds.

Section snippets

Experimental details

Alloys with a total mass of 1–2 g were prepared by arc-melting in an electric arc furnace (90 V, 150 A) under argon (99.992 vol%) using a non-consumable tungsten electrode and on a water-cooled copper hearth. Pieces of rare earth metals (purity 99.9 wt%), silicon (99.99 wt%) and nickel (99.95 wt%) were used as starting components. A titanium button was used as a getter during arc-melting and the alloys were remelted three times. The arc-melted samples were then annealed in argon at 1070 K (±2 K) for

Ce-Ni-Si system at 870/1070 K

Based on the Rietveld analysis of the powder X-ray diffraction data and microprobe results obtained on nearly 40 samples (SEM micrographs of some of the representative samples are shown in Fig. 1 and example of Rietveld refinement of X-ray powder pattern is given in Fig. 1s), the isothermal section of the Ce-Ni-Si system at 870/1070 K was constructed (Fig. 2). The nominal composition of the prepared samples is shown as square dots in Fig. 2. The estimated equilibria are represented by dotted

Discussion

The present Ce-Ni-Si section at 870/1070 K supplements the Ce-Ni-Si sections at 670/1070 K [21], [22] and R-Ni-Si sections with ternary and pseudo-binary rare earth silicides.

From the point of view of isostructural rows in R-Ni-Si systems (see Table 1):

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GdNi₇Si₆-type {Pr, Nd, Sm}Ni₇Si₆ should exist and GdNi₇Si₆-type {Eu, Yb, Lu}Ni₇Si₆ compounds also are possible to synthesize.
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PrNi₆Si₆ may crystallize in YNi₆Si₆- or CeNi₆Si₆-type structure and YNi₆Si₆- or YCo₆Ge₆-type structure is possible for LuNi₆

Conclusion

The isothermal section of the Ce-Ni-Si system at 870/1070 K has been investigated. The crystal structure of the pseudo-binary phases as well as the ternary compounds has been studied and some new compounds of R-Ni-Si systems have been detected. Certainly, the family of these compounds may be expanded via variation of preparation methods and synthesis conditions. Magnetic properties of a few ternary compounds have been also investigated. The present work constitutes a further contribution to the

Acknowledgments

This work was supported by the Indo-Russian Fund for Basic Research through the Project no. 15-53-45129-a and Russian Fund for Basic Research through the Project no. 16-03-00666-a. S.K.M. thanks CAPES for the award of a fellowship, MEC and MCTI (Brazil) for financial support during the course of this work. This work supported by a ICDD (USA) Grant N 05-07. The unit cell data of CeNi₇Si₆, CeNi₆Si₆, CeNi₄Si, Ce₂Ni_2.5Si_0.5, Ce₃Ni₃Si, Ce₅Ni_1.85Si₃, LaNi₇Si₆, YNi_6.6Si_6.1, NdNi₆Si₆, Dy₂Ni₁₅Si₂, Ho₂Ni

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The Ce-Ni-Si system as a representative of the rare earth-Ni-Si family: Isothermal section and new rare-earth nickel silicides

Highlights

Abstract

Graphical abstract

Introduction

Section snippets

Experimental details

Ce-Ni-Si system at 870/1070 K

Discussion

Conclusion

Acknowledgments

Mater. Res. Bull.

Phys. Lett. A

J. Magn. Magn. Mater.

Phys. Soc. Jpn.

J. Alloy. Compd.

J. Alloy. Compd.

J. Solid State Chem.

J. Solid State Chem.

J. Solid State Chem.

J. Solid State Chem.

J. Solid State Chem.

J. Magn. Magn. Mater.

J. Solid State Chem.

J. Alloy. Compd.

J. Alloy. Compd.

J. Less Common Met.

J. Alloy. Compd.

J. Alloy. Compd.

J. Less Common Met.

J. Alloy. Compd.

J. Alloy. Compd.

J. Solid State Chem.

J. Solid State Chem.

Solid State Sci.

J. Alloy. Compd.

J. Alloy. Compd.

J. Magn. Magn. Mater.

J. Alloy. Compd.