{"title":"AgCuTe 热电材料中含碲间隙原子和银/铜空位的纳米级区域的高密度排列","authors":"Bin Xiao, He Yang, Jianbo Li, Jun Wang","doi":"10.1021/acsaem.4c01701","DOIUrl":null,"url":null,"abstract":"The rigid crystalline sublattice of Te ions in AgCuTe provides an effective electrical transport channel, enabling AgCuTe to exhibit good electrical properties. However, the appearance of vacancies or interstitial atoms within the Te<sup>2–</sup> rigid anionic framework poses significant challenges both theoretically and experimentally. Here, we are the first to discover the existence of localized Te<sub>i</sub>, V<sub>Cu</sub>, and V<sub>Ag</sub> multiple defects in the AgCuTe phase, as well as a highly ordered arrangement of V<sub>Cu</sub> in the Cu<sub>2</sub>Te phase of AgCuTe<sub>1–<i>z</i></sub> samples, by only fine-tuning the Te stoichiometric ratio. The formation of these localized defects arises from the excess precipitation of Ag and Cu during the process, which enhances phonon scattering and reduces thermal conductivity. Simultaneously, the total cation content in AgCuTe<sub>1–<i>z</i></sub> samples increases relative to the anion, thereby optimizing total intrinsic vacancies and carrier concentration. As a result, there is a 311% increase in the power factor and a 44% decrease in the lattice thermal conductivity at room temperature, leading to a 54% net increase in <i>ZT</i> compared to that of pristine AgCuTe. This approach is expected to be a universal modification strategy for enhancing the thermoelectric properties of other Te-based anionic framework superionic conductor materials.","PeriodicalId":4,"journal":{"name":"ACS Applied Energy Materials","volume":"33 1","pages":""},"PeriodicalIF":5.4000,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"High-Density Arrangement of Nanoscale Regions with Tellurium Interstitial Atoms and Silver/Copper Vacancies in AgCuTe Thermoelectric Materials\",\"authors\":\"Bin Xiao, He Yang, Jianbo Li, Jun Wang\",\"doi\":\"10.1021/acsaem.4c01701\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The rigid crystalline sublattice of Te ions in AgCuTe provides an effective electrical transport channel, enabling AgCuTe to exhibit good electrical properties. However, the appearance of vacancies or interstitial atoms within the Te<sup>2–</sup> rigid anionic framework poses significant challenges both theoretically and experimentally. Here, we are the first to discover the existence of localized Te<sub>i</sub>, V<sub>Cu</sub>, and V<sub>Ag</sub> multiple defects in the AgCuTe phase, as well as a highly ordered arrangement of V<sub>Cu</sub> in the Cu<sub>2</sub>Te phase of AgCuTe<sub>1–<i>z</i></sub> samples, by only fine-tuning the Te stoichiometric ratio. The formation of these localized defects arises from the excess precipitation of Ag and Cu during the process, which enhances phonon scattering and reduces thermal conductivity. Simultaneously, the total cation content in AgCuTe<sub>1–<i>z</i></sub> samples increases relative to the anion, thereby optimizing total intrinsic vacancies and carrier concentration. As a result, there is a 311% increase in the power factor and a 44% decrease in the lattice thermal conductivity at room temperature, leading to a 54% net increase in <i>ZT</i> compared to that of pristine AgCuTe. This approach is expected to be a universal modification strategy for enhancing the thermoelectric properties of other Te-based anionic framework superionic conductor materials.\",\"PeriodicalId\":4,\"journal\":{\"name\":\"ACS Applied Energy Materials\",\"volume\":\"33 1\",\"pages\":\"\"},\"PeriodicalIF\":5.4000,\"publicationDate\":\"2024-09-18\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Energy Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1021/acsaem.4c01701\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Energy Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1021/acsaem.4c01701","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
High-Density Arrangement of Nanoscale Regions with Tellurium Interstitial Atoms and Silver/Copper Vacancies in AgCuTe Thermoelectric Materials
The rigid crystalline sublattice of Te ions in AgCuTe provides an effective electrical transport channel, enabling AgCuTe to exhibit good electrical properties. However, the appearance of vacancies or interstitial atoms within the Te2– rigid anionic framework poses significant challenges both theoretically and experimentally. Here, we are the first to discover the existence of localized Tei, VCu, and VAg multiple defects in the AgCuTe phase, as well as a highly ordered arrangement of VCu in the Cu2Te phase of AgCuTe1–z samples, by only fine-tuning the Te stoichiometric ratio. The formation of these localized defects arises from the excess precipitation of Ag and Cu during the process, which enhances phonon scattering and reduces thermal conductivity. Simultaneously, the total cation content in AgCuTe1–z samples increases relative to the anion, thereby optimizing total intrinsic vacancies and carrier concentration. As a result, there is a 311% increase in the power factor and a 44% decrease in the lattice thermal conductivity at room temperature, leading to a 54% net increase in ZT compared to that of pristine AgCuTe. This approach is expected to be a universal modification strategy for enhancing the thermoelectric properties of other Te-based anionic framework superionic conductor materials.
期刊介绍:
ACS Applied Energy Materials is an interdisciplinary journal publishing original research covering all aspects of materials, engineering, chemistry, physics and biology relevant to energy conversion and storage. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important energy applications.