Diogo Lopes , Miguel A. Vieira , Nuno M. Ferreira , Vladimir V. Shvartsman , Oscar J. Dura , Francisco Q. Batista , Andrei N. Salak , Sergey Mikhalev , Florinda Costa , Andrei V. Kovalevsky
{"title":"激光浮区制备供体取代钛酸锶基复合材料的高热电性能","authors":"Diogo Lopes , Miguel A. Vieira , Nuno M. Ferreira , Vladimir V. Shvartsman , Oscar J. Dura , Francisco Q. Batista , Andrei N. Salak , Sergey Mikhalev , Florinda Costa , Andrei V. Kovalevsky","doi":"10.1016/j.jallcom.2025.180106","DOIUrl":null,"url":null,"abstract":"<div><div>Oxide thermoelectrics, made from abundant, eco-friendly materials, can withstand high-temperature gradients, making them highly promising for high-temperature waste heat harvesting. Recent advancements in the efficiency of thermoelectric material families have been driven by composite approaches, fostering synergistic effects between materials, further enhanced by advanced processing techniques. Accordingly, this study explores the design of oxide-based thermoelectric composites, involving the redistribution of a common substituting cation between composite phases, driven by laser floating zone (LFZ) processing. Niobium substituted strontium titanate/rutile composite material with a nominal composition Sr<sub>0.97</sub>Ti<sub>0.8</sub>Nb<sub>0.2</sub>O<sub>3</sub> / 0.15Ti<sub>0.95</sub>Nb<sub>0.05</sub>O<sub>2</sub> was processed by LFZ at various pulling rates (50, 100, and 200 mm/h), followed by post-thermal treatment under highly reducing conditions. The obtained samples showed inhomogeneous niobium distribution between perovskite and rutile phases shaped by strongly non-equilibrium conditions inherent to the LFZ processing, in contrast to the conventional solid-state route. Adjusting the pulling rate enabled a certain degree of control over niobium incorporation into both phases. Primarily driven by an enhanced Seebeck coefficient, the LFZ-processed and thermally treated samples demonstrated high power factors, reaching 1350–820 μW·K<sup>−2</sup>·m<sup>−1</sup> at 473–1173 K, respectively. An appealing ZT of 0.52 at 1173 K was achieved for the composite sample processed at 100 mm/h and subjected to thermal treatment. This performance is attributed to a combination of a high power factor and low thermal conductivity (∼2 W·m<sup>−1</sup>·K<sup>−1</sup> at 1173 K), enabled by phase and compositional inhomogeneities, as well as residual porosity introduced by LFZ processing. The LFZ technique offers considerable potential for optimisation and has proven to be a powerful tool for designing ceramic composite thermoelectric materials.</div></div>","PeriodicalId":344,"journal":{"name":"Journal of Alloys and Compounds","volume":"1024 ","pages":"Article 180106"},"PeriodicalIF":6.3000,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"High thermoelectric performance in donor-substituted strontium titanate-based composites processed by laser floating zone\",\"authors\":\"Diogo Lopes , Miguel A. Vieira , Nuno M. Ferreira , Vladimir V. Shvartsman , Oscar J. Dura , Francisco Q. Batista , Andrei N. Salak , Sergey Mikhalev , Florinda Costa , Andrei V. Kovalevsky\",\"doi\":\"10.1016/j.jallcom.2025.180106\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Oxide thermoelectrics, made from abundant, eco-friendly materials, can withstand high-temperature gradients, making them highly promising for high-temperature waste heat harvesting. Recent advancements in the efficiency of thermoelectric material families have been driven by composite approaches, fostering synergistic effects between materials, further enhanced by advanced processing techniques. Accordingly, this study explores the design of oxide-based thermoelectric composites, involving the redistribution of a common substituting cation between composite phases, driven by laser floating zone (LFZ) processing. Niobium substituted strontium titanate/rutile composite material with a nominal composition Sr<sub>0.97</sub>Ti<sub>0.8</sub>Nb<sub>0.2</sub>O<sub>3</sub> / 0.15Ti<sub>0.95</sub>Nb<sub>0.05</sub>O<sub>2</sub> was processed by LFZ at various pulling rates (50, 100, and 200 mm/h), followed by post-thermal treatment under highly reducing conditions. The obtained samples showed inhomogeneous niobium distribution between perovskite and rutile phases shaped by strongly non-equilibrium conditions inherent to the LFZ processing, in contrast to the conventional solid-state route. Adjusting the pulling rate enabled a certain degree of control over niobium incorporation into both phases. Primarily driven by an enhanced Seebeck coefficient, the LFZ-processed and thermally treated samples demonstrated high power factors, reaching 1350–820 μW·K<sup>−2</sup>·m<sup>−1</sup> at 473–1173 K, respectively. An appealing ZT of 0.52 at 1173 K was achieved for the composite sample processed at 100 mm/h and subjected to thermal treatment. This performance is attributed to a combination of a high power factor and low thermal conductivity (∼2 W·m<sup>−1</sup>·K<sup>−1</sup> at 1173 K), enabled by phase and compositional inhomogeneities, as well as residual porosity introduced by LFZ processing. The LFZ technique offers considerable potential for optimisation and has proven to be a powerful tool for designing ceramic composite thermoelectric materials.</div></div>\",\"PeriodicalId\":344,\"journal\":{\"name\":\"Journal of Alloys and Compounds\",\"volume\":\"1024 \",\"pages\":\"Article 180106\"},\"PeriodicalIF\":6.3000,\"publicationDate\":\"2025-04-03\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Alloys and Compounds\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0925838825016640\",\"RegionNum\":2,\"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":"Journal of Alloys and Compounds","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0925838825016640","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
High thermoelectric performance in donor-substituted strontium titanate-based composites processed by laser floating zone
Oxide thermoelectrics, made from abundant, eco-friendly materials, can withstand high-temperature gradients, making them highly promising for high-temperature waste heat harvesting. Recent advancements in the efficiency of thermoelectric material families have been driven by composite approaches, fostering synergistic effects between materials, further enhanced by advanced processing techniques. Accordingly, this study explores the design of oxide-based thermoelectric composites, involving the redistribution of a common substituting cation between composite phases, driven by laser floating zone (LFZ) processing. Niobium substituted strontium titanate/rutile composite material with a nominal composition Sr0.97Ti0.8Nb0.2O3 / 0.15Ti0.95Nb0.05O2 was processed by LFZ at various pulling rates (50, 100, and 200 mm/h), followed by post-thermal treatment under highly reducing conditions. The obtained samples showed inhomogeneous niobium distribution between perovskite and rutile phases shaped by strongly non-equilibrium conditions inherent to the LFZ processing, in contrast to the conventional solid-state route. Adjusting the pulling rate enabled a certain degree of control over niobium incorporation into both phases. Primarily driven by an enhanced Seebeck coefficient, the LFZ-processed and thermally treated samples demonstrated high power factors, reaching 1350–820 μW·K−2·m−1 at 473–1173 K, respectively. An appealing ZT of 0.52 at 1173 K was achieved for the composite sample processed at 100 mm/h and subjected to thermal treatment. This performance is attributed to a combination of a high power factor and low thermal conductivity (∼2 W·m−1·K−1 at 1173 K), enabled by phase and compositional inhomogeneities, as well as residual porosity introduced by LFZ processing. The LFZ technique offers considerable potential for optimisation and has proven to be a powerful tool for designing ceramic composite thermoelectric materials.
期刊介绍:
The Journal of Alloys and Compounds is intended to serve as an international medium for the publication of work on solid materials comprising compounds as well as alloys. Its great strength lies in the diversity of discipline which it encompasses, drawing together results from materials science, solid-state chemistry and physics.