Thermoelectric performance in disordered Cu2ZnSnSe4 nanostructures driven by ultra-low thermal conductivity

Mukherjee, Binayak; Isotta, Eleonora; Malagutti, Marcelo Augusto; Lohani, Ketan; Rebuffi, Luca; Fanciulli, Carlo; Scardi, Paolo

doi:10.1016/j.jallcom.2022.167756

Cited by 9 publications

(15 citation statements)

References 48 publications

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“…Regarding the CZTS/Se system, the difference between disordered cubic CZTS/Se ( F-43m ) and disordered tetragonal CZTS/Se ( I-42m ) are the superstructure reflections visible through the low-angle Bragg-peaks in XRD and the observed new rings in the SAED patterns [ 45 , 46 , 47 ]. These transitions were also observed in DSC measurements for CZTS/Se [ 20 , 52 ]. The SR-XRD for the monoclinic and cubic CTS at 350 °C is shown in Figure 1 .…”

Section: Structure and Nature Of Disordersupporting

confidence: 56%

“…As discussed, the tetragonal order–disorder transition in CZTS/CZTSe manifests in a variation of the Seebeck value, which sharply increases for CZTS, and moderately decreases for CZTSe at the transition temperatures of ~500 and ~450 K, respectively. This behavior is associated with two different mechanisms, as shown by first-principles calculations [ 20 , 51 ]. In both cases, the disorder contributes to a flattening of the bands (increasing the Seebeck coefficient) and suppression of the band gap (decreasing the resistivity).…”

Section: Electronic Propertiesmentioning

confidence: 98%

“… Temperature-dependent Seebeck coefficient ( a ), electrical resistivity ( b ), and power factor ( c ) curves for CTS, CZTS, and CZTSe polymorphs retrieved from [ 20 , 34 , 51 , 52 ]. …”

Section: Figurementioning

confidence: 99%

“…Such an environment also favors the disordering of these Cu-alloys. Recently, we have synthesized and stabilized various polymorphs of Cu 2 SnS 3 (CTS) [ 9 ], Cu 2 ZnSnS 4 (CZTS) [ 19 ], and Cu 2 ZnSnSe 4 (CZTSe) [ 20 ] through this bottom-up ball-milling technique.…”

Section: Introductionmentioning

confidence: 99%

“…The extrinsic doping with Na [ 46 ], Ag [ 47 ], Ni [ 48 ], and Ga [ 49 ] have also shown significant improvement in the performance of these materials. In addition, the disorder in these systems introduced by temperature [ 50 , 51 ], chemistry [ 45 ], or synthesis method [ 20 , 52 , 53 ] revealed to be critical to their improvement as TE materials.…”

Section: Introductionmentioning

confidence: 99%

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Mechanochemical Synthesis of Sustainable Ternary and Quaternary Nanostructured Cu2SnS3, Cu2ZnSnS4, and Cu2ZnSnSe4 Chalcogenides for Thermoelectric Applications

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Copper-based chalcogenides have emerged as promising thermoelectric materials due to their high thermoelectric performance, tunable transport properties, earth abundance and low toxicity. We have presented an overview of experimental results and first-principal calculations investigating the thermoelectric properties of various polymorphs of Cu2SnS3 (CTS), Cu2ZnSnS4 (CZTS), and Cu2ZnSnSe4 (CZTSe) synthesized by high-energy reactive mechanical alloying (ball milling). Of particular interest are the disordered polymorphs of these materials, which exhibit phonon-glass–electron-crystal behavior—a decoupling of electron and phonon transport properties. The interplay of cationic disorder and nanostructuring leads to ultra-low thermal conductivities while enhancing electronic transport. These beneficial transport properties are the consequence of a plethora of features, including trap states, anharmonicity, rattling, and conductive surface states, both topologically trivial and non-trivial. Based on experimental results and computational methods, this report aims to elucidate the details of the electronic and lattice transport properties, thereby confirming that the higher thermoelectric (TE) performance of disordered polymorphs is essentially due to their complex crystallographic structures. In addition, we have presented synchrotron X-ray diffraction (SR-XRD) measurements and ab initio molecular dynamics (AIMD) simulations of the root-mean-square displacement (RMSD) in these materials, confirming anharmonicity and bond inhomogeneity for disordered polymorphs.

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Section: Structure and Nature Of Disordersupporting

confidence: 56%

Section: Electronic Propertiesmentioning

confidence: 98%

“… Temperature-dependent Seebeck coefficient ( a ), electrical resistivity ( b ), and power factor ( c ) curves for CTS, CZTS, and CZTSe polymorphs retrieved from [ 20 , 34 , 51 , 52 ]. …”

Section: Figurementioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Mechanochemical Synthesis of Sustainable Ternary and Quaternary Nanostructured Cu2SnS3, Cu2ZnSnS4, and Cu2ZnSnSe4 Chalcogenides for Thermoelectric Applications

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Elastic Moduli: a Tool for Understanding Chemical Bonding and Thermal Transport in Thermoelectric Materials

et al. 2023

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The elastic behavior of a material can be a powerful tool to decipher thermal transport. In thermoelectrics, measuring the elastic moduli-directly tied to sound velocity-is critical to understand trends in lattice thermal conductivity, as well as study bond anharmonicity and phase transitions, given the sensitivity of elastic moduli to the chemical bonding. In this review, we introduce the basics of elasticity and explain the origin of high-temperature lattice softening from a bonding perspective. We then review elasticity data throughout classes of thermoelectrics, and explore trends in sound velocity, anharmonicity, and thermal conductivity. We reveal how experimental sound velocities can improve the accuracy of common thermal conductivity models and present a critical discussion of Grüneisen parameter estimates from elastic moduli. Readers will be equipped with tools to leverage elasticity measurements or calculations to accurately interpret thermal transport trends.

show abstract

Elastic Moduli: a Tool for Understanding Chemical Bonding and Thermal Transport in Thermoelectric Materials

et al. 2023

Self Cite

View full text Add to dashboard Cite

The elastic behavior of a material can be a powerful tool to decipher thermal transport. In thermoelectrics, measuring the elastic moduli—directly tied to sound velocity—is critical to understand trends in lattice thermal conductivity, as well as study bond anharmonicity and phase transitions, given the sensitivity of elastic moduli to the chemical bonding. In this review, we introduce the basics of elasticity and explain the origin of high‐temperature lattice softening from a bonding perspective. We then review elasticity data throughout classes of thermoelectrics, and explore trends in sound velocity, anharmonicity, and thermal conductivity. We reveal how experimental sound velocities can improve the accuracy of common thermal conductivity models and present a critical discussion of Grüneisen parameter estimates from elastic moduli. Readers will be equipped with tools to leverage elasticity measurements or calculations to accurately interpret thermal transport trends.

show abstract

Thermoelectric performance in disordered Cu2ZnSnSe4 nanostructures driven by ultra-low thermal conductivity

Cited by 9 publications

References 48 publications

Mechanochemical Synthesis of Sustainable Ternary and Quaternary Nanostructured Cu2SnS3, Cu2ZnSnS4, and Cu2ZnSnSe4 Chalcogenides for Thermoelectric Applications

Mechanochemical Synthesis of Sustainable Ternary and Quaternary Nanostructured Cu2SnS3, Cu2ZnSnS4, and Cu2ZnSnSe4 Chalcogenides for Thermoelectric Applications

Elastic Moduli: a Tool for Understanding Chemical Bonding and Thermal Transport in Thermoelectric Materials

Elastic Moduli: a Tool for Understanding Chemical Bonding and Thermal Transport in Thermoelectric Materials

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