Abstract

Defects and defect engineering are at the core of many regimes of material research, including the field of thermoelectric study. The 60‐year history of V2VI3 thermoelectric materials is a prime example of how a class of semiconductor material, considered mature several times, can be rejuvenated by better understanding and manipulation of defects. This review aims to provide a systematic account of the underexplored intrinsic point defects in V2VI3 compounds, with regard to (i) their formation and control, and (ii) their interplay with other types of defects towards higher thermoelectric performance. We herein present a convincing case that intrinsic point defects can be actively controlled by extrinsic doping and also via compositional, mechanical, and thermal control at various stages of material synthesis. An up‐to‐date understanding of intrinsic point defects in V2VI3 compounds is summarized in a (χ, r)‐model and applied to elucidating the donor‐like effect. These new insights not only enable more innovative defect engineering in other thermoelectric materials but also, in a broad context, contribute to rational defect design in advanced functional materials at large.

Highlights

  • V2VI3 compounds (V = Group V elements Sb and Bi, and VI = Group VI elements S, Se and Te) and their derivatives constito characterize intrinsic point defects and their interplay with other defects in V2VI3 materials; reversely, a better understanding of intrinsic point defects and their interplay with other defects enables us to further optimize the TE performance of tute an important class of semiconductor material in renewable V2VI3 compounds

  • Harman et al proposed that the dominant intrinsic point defects in the asgrown Bi2Te3 ingot are negatively charged antisite defects Bi′Te on the Te-deficient side and positively charged antisite defects TeiBi on the Te-rich side.[46]

  • Liu et al recently conducted a systematic study of n-type Bi2Te3–Bi2Se3–Bi2S3 system.[134]. These results showed that Bi2Te2S1 has a peak zT value ≈ 0.8 at 573 K and Bi2Se1S2 ≈ 0.8 at 773 K upon high energy ball milling (BM) followed by the hot pressed (HP) process

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Summary

Introduction

(TE) materials.[1] Recently they became a focus in the study of mopower), electrical conductivity, total thermal conductivity bulk quantum topological insulators.[2] In this review we intend to address the fundamental yet underexplored role of intrinsic point defects in V2VI3 compounds. While this gap of knowledge has led to ambiguities in the synthesis-structure-property (including the lattice component, κph, and carrier component, κel), the absolute temperature, and the power factor (PF), respectively.

Formation of Intrinsic Point Defects in V2VI3 Binary Compounds
Manipulation of Intrinsic Point Defects
Compositional Control in Cation-Rich V2VI3 Compounds
E AS k bTm
Synthesis Environment Control
Mechanical Control
Thermal Control via the Recovery Effect
Role of Intrinsic Point Defect towards Higher zT
Optimizing Electron Band Structure
Reduced Lattice Thermal Conductivity
Intrinsic Point Defect Engineering
Reassessment of Optimal Compositions
Room Temperature Refrigeration
Mid-Temperature Power Generation
Low-Temperature Power Generation
Approaches beyond Intrinsic Point Defect Engineering
Findings
Conclusions
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