Structural stability and thermoelectric performance of high quality synthetic and natural pyrites (FeS<sub>2</sub>)

Zuñiga-Puelles, E.; Cardoso‐Gil, Raúl; Bobnar, Matej; Veremchuk, Igor; Himcinschi, Cameliu; Hennig, Christoph; Kortus, Jens; Heide, G.; Gumeniuk, Roman

doi:10.1039/c9dt01902b

Cited by 18 publications

(22 citation statements)

References 53 publications

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“…In terms of lattice parameters, we use a = 5.418 Å, u = 0.3850 for pyrite (space group

) and a = 4.443 Å, b = 5.425 Å, c = 3.387 Å, u = 0.2005, v = 0.3783 for marcasite (space group Pnnm ). These values follow the results from X-ray diffraction experiments at ambient conditions ( Brostigen and Kjekshus, 1969 ; Brostigen et al, 1973 ; Chattopadhyay and Von Schnering, 1985 ; Zuñiga-Puelles et al, 2019 ). The corresponding S-S bond lengths in the two polymorphs are 2.16 and 2.21 Å, respectively.…”

Section: Theory and Methodssupporting

confidence: 84%

Accurate Prediction of Band Structure of FeS2: A Hard Quest of Advanced First-Principles Approaches

Zhang

Jiang

2021

Front. Chem.

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The pyrite and marcasite polymorphs of FeS2 have attracted considerable interests for their potential applications in optoelectronic devices because of their appropriate electronic and optical properties. Controversies regarding their fundamental band gaps remain in both experimental and theoretical materials research of FeS2. In this work, we present a systematic theoretical investigation into the electronic band structures of the two polymorphs by using many-body perturbation theory with the GW approximation implemented in the full-potential linearized augmented plane waves (FP-LAPW) framework. By comparing the quasi-particle (QP) band structures computed with the conventional LAPW basis and the one extended by high-energy local orbitals (HLOs), denoted as LAPW + HLOs, we find that one-shot or partially self-consistent GW (G0W0 and GW0, respectively) on top of the Perdew-Burke-Ernzerhof (PBE) generalized gradient approximation with a converged LAPW + HLOs basis is able to remedy the artifact reported in the previous GW calculations, and leads to overall good agreement with experiment for the fundamental band gaps of the two polymorphs. Density of states calculated from G0W0@PBE with the converged LAPW + HLOs basis agrees well with the energy distribution curves from photo-electron spectroscopy for pyrite. We have also investigated the performances of several hybrid functionals, which were previously shown to be able to predict band gaps of many insulating systems with accuracy close or comparable to GW. It is shown that the hybrid functionals considered in general fail badly to describe the band structures of FeS2 polymorphs. This work indicates that accurate prediction of electronic band structure of FeS2 poses a stringent test on state-of-the-art first-principles approaches, and the G0W0 method based on semi-local approximation performs well for this difficult system if it is practiced with well-converged numerical accuracy.

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“…In terms of lattice parameters, we use a = 5.418 Å, u = 0.3850 for pyrite (space group

Section: Theory and Methodssupporting

confidence: 84%

Accurate Prediction of Band Structure of FeS2: A Hard Quest of Advanced First-Principles Approaches

Zhang

Jiang

2021

Front. Chem.

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“…The cumulative effect of noted improvement in the electrical transport and a considerable suppression of the thermal transport (phonon) with cobalt doping is obviously enhancing the zT (Figure 2f). The Co substituted sample with the composition of x = 0.05 exhibited the highest zT ~ 0.004 at 573 K, which is few orders of magnitude greater than that of related pristine pyrite that was reported very recently [31]. However, it must be noted that these zT values are too low for any potential industrial application.…”

Section: Resultsmentioning

confidence: 68%

Exploring the thermoelectric behavior of spark plasma sintered Fe7-xCoxS8 compounds

Simon

Guélou

Srinivasan

et al. 2020

Journal of Alloys and Compounds

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Sulfide-based materials are emerging as viable alternatives for the current state-of-the-art thermoelectric materials, which usually are composed of toxic, expensive and scarce elements. Here, a systematic study of one such inexpensive and environmentally friendly sulfide-based system, i.e. Fe7-xCoxS8 pyrrhotitetype compounds that were synthesized by solid-state reaction and densified by Spark Plasma Sintering are investigated for their structural and thermoelectric properties. We report that substitution of Co for Fe in pyrrhotites: (i) induces structural transition from monoclinic 4C superstructure to trigonal 3C superstructure; (ii) modifies the magnetic behavior by decreasing the magnetic ordering temperature and magnetization; (iii) alters the type of dominant charge carriers (from p-to n-type) and enhances their electrical transport properties; (iv) mitigates the phonon contribution to the thermal conductivity; and (v) amplifies the thermoelectric figure of merit when compared with that of pristine pyrrhotites.

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“…Tetrahedrites are cheap and easily available mineral sulfosalts that present large figures of merit and are seen as having good potential for thermoelectric applications (Lu & Morelli, 2016). Pyrite (FeS 2 ) is low cost sulfide with simple synthesis and moderate thermoelectric properties (Harada, 1998;Zuñiga Puelles et al, 2019). In this compound, the large electrical resistivity and thermal conductivity observed in the pristine material are the major constraints to their practical use.…”

Section: Introductionmentioning

confidence: 99%

Preparation, thermal stability and electrical transport properties of vaesite, NiS₂

Ferreira

Lopes

Malta

et al. 2019

PeerJ Materials Science

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Vaesite, a nickel chalcogenide with NiS2 formula, has been synthetized and studied by theoretical and experimental methods. NiS2 was prepared by solid-state reaction under vacuum and densified by hot-pressing, at different consolidation conditions. Dense single-phase pellets (relative densities >94%) were obtained, without significant lattice distortions for different hot-pressing conditions. The thermal stability of NiS2 was studied by thermogravimetric analysis. Both as-synthetized and hot-pressed NiS2 have a single phase nature, although some hot-pressed samples had traces of the sulfur deficient phase, Ni1-xS (<1%vol), due to the strong desulfurization at T > 340 °C. The electronic band structure and density of states were calculated by Density Functional Theory (DFT), indicating a metallic behavior. However, the electronic transport measurements showed p-type semiconductivity for bulk NiS2, verifying its characteristic behavior has a Mott insulator. The consolidation conditions strongly influence the electronic properties, with the best room-temperature Seebeck coefficient, electrical resistivity and power factor being 182 µVK−1, 2,257 µΩ m and 14.1 µWK−2 m−1, respectively, pointing this compound as a good starting point for a new family of thermoelectric materials.

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Structural stability and thermoelectric performance of high quality synthetic and natural pyrites (FeS₂)

Abstract: Single crystalline pyrite of high quality reveals good thermal- and bad electrical conductivities resulting in poor thermoelectric performance.

Cited by 18 publications

References 53 publications

Accurate Prediction of Band Structure of FeS2: A Hard Quest of Advanced First-Principles Approaches

Accurate Prediction of Band Structure of FeS2: A Hard Quest of Advanced First-Principles Approaches

Exploring the thermoelectric behavior of spark plasma sintered Fe7-xCoxS8 compounds

Preparation, thermal stability and electrical transport properties of vaesite, NiS₂

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Structural stability and thermoelectric performance of high quality synthetic and natural pyrites (FeS2)

Abstract: Single crystalline pyrite of high quality reveals good thermal- and bad electrical conductivities resulting in poor thermoelectric performance.

Cited by 18 publications

References 53 publications

Accurate Prediction of Band Structure of FeS2: A Hard Quest of Advanced First-Principles Approaches

Accurate Prediction of Band Structure of FeS2: A Hard Quest of Advanced First-Principles Approaches

Exploring the thermoelectric behavior of spark plasma sintered Fe7-xCoxS8 compounds

Preparation, thermal stability and electrical transport properties of vaesite, NiS2

Contact Info

Product

Resources

About

Structural stability and thermoelectric performance of high quality synthetic and natural pyrites (FeS₂)

Preparation, thermal stability and electrical transport properties of vaesite, NiS₂