Aishwarya Mantravadi, Bradyn C. Weaver, Shiya Chen, Shahnaz Mukta, Yao Abusa, Arka Sarkar, Yang Sun, Yaroslav Mudryk, Alexander Gundlach-Graham, Kai-Ming Ho, Oleg I. Lebedev, Julia V. Zaikina
{"title":"当范德瓦耳斯遇到鹿目:具有钒-鹿目网络的二维锑化物","authors":"Aishwarya Mantravadi, Bradyn C. Weaver, Shiya Chen, Shahnaz Mukta, Yao Abusa, Arka Sarkar, Yang Sun, Yaroslav Mudryk, Alexander Gundlach-Graham, Kai-Ming Ho, Oleg I. Lebedev, Julia V. Zaikina","doi":"10.1021/jacs.4c07285","DOIUrl":null,"url":null,"abstract":"2D materials showcase unconventional properties emerging from quantum confinement effects. In this work, a “soft chemical” route allows for the deintercalation of K<sup>+</sup> from the layered antimonide KV<sub>6</sub>Sb<sub>6</sub>, resulting in the discovery of a new metastable 2D-Kagome antimonide K<sub>0.1(1)</sub>V<sub>6</sub>Sb<sub>6</sub> with a van der Waals gap of 3.2 Å. The structure of K<sub>0.1(1)</sub>V<sub>6</sub>Sb<sub>6</sub> was determined via the synergistic techniques, including X-ray pair distribution function analysis, advanced transmission electron microscopy, and density functional theory calculations. The K<sub>0.1(1)</sub>V<sub>6</sub>Sb<sub>6</sub> compound crystallizes in the monoclinic space group <i>C</i>2/<i>m</i> (<i>a</i> = 9.57(2) Å, <i>b</i> = 5.502(8) Å, <i>c</i> = 10.23(2) Å, β = 97.6(2)°, <i>Z</i> = 2). The [V<sub>6</sub>Sb<sub>6</sub>] layers in K<sub>0.1(1)</sub>V<sub>6</sub>Sb<sub>6</sub> are retained upon deintercalation and closely resemble the layers in the parent compound, yet deintercalation results in a relative shift of the adjacent [V<sub>6</sub>Sb<sub>6</sub>] layers. The magnetic properties of the K<sub>0.1(1)</sub>V<sub>6</sub>Sb<sub>6</sub> phase in the 2–300 K range are comparable to those of KV<sub>6</sub>Sb<sub>6</sub> and another Kagome antimonide KV<sub>3</sub>Sb<sub>5</sub>, consistent with nearly temperature-independent paramagnetism. Electronic band structure calculation suggests a nontrivial band topology with flat bands and opening of band crossing afforded by deintercalation. Transport property measurements reveal a metallic nature for K<sub>0.1(1)</sub>V<sub>6</sub>Sb<sub>6</sub> and a low thermal conductivity of 0.6 W K<sup>–1</sup> m<sup>–1</sup> at 300 K. Additionally, ion exchange in KV<sub>6</sub>Sb<sub>6</sub> via a solvothermal route leads to a successful partial exchange of K<sup>+</sup> with <i>A</i><sup>+</sup> (<i>A</i> = Na, Rb, and Cs). This study highlights the tunability of the layered structure of the KV<sub>6</sub>Sb<sub>6</sub> compound, providing a rich playground for the realization of new 2D materials.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":null,"pages":null},"PeriodicalIF":14.4000,"publicationDate":"2024-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"When van der Waals Met Kagome: A 2D Antimonide with a Vanadium-Kagome Network\",\"authors\":\"Aishwarya Mantravadi, Bradyn C. Weaver, Shiya Chen, Shahnaz Mukta, Yao Abusa, Arka Sarkar, Yang Sun, Yaroslav Mudryk, Alexander Gundlach-Graham, Kai-Ming Ho, Oleg I. Lebedev, Julia V. Zaikina\",\"doi\":\"10.1021/jacs.4c07285\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"2D materials showcase unconventional properties emerging from quantum confinement effects. In this work, a “soft chemical” route allows for the deintercalation of K<sup>+</sup> from the layered antimonide KV<sub>6</sub>Sb<sub>6</sub>, resulting in the discovery of a new metastable 2D-Kagome antimonide K<sub>0.1(1)</sub>V<sub>6</sub>Sb<sub>6</sub> with a van der Waals gap of 3.2 Å. The structure of K<sub>0.1(1)</sub>V<sub>6</sub>Sb<sub>6</sub> was determined via the synergistic techniques, including X-ray pair distribution function analysis, advanced transmission electron microscopy, and density functional theory calculations. The K<sub>0.1(1)</sub>V<sub>6</sub>Sb<sub>6</sub> compound crystallizes in the monoclinic space group <i>C</i>2/<i>m</i> (<i>a</i> = 9.57(2) Å, <i>b</i> = 5.502(8) Å, <i>c</i> = 10.23(2) Å, β = 97.6(2)°, <i>Z</i> = 2). The [V<sub>6</sub>Sb<sub>6</sub>] layers in K<sub>0.1(1)</sub>V<sub>6</sub>Sb<sub>6</sub> are retained upon deintercalation and closely resemble the layers in the parent compound, yet deintercalation results in a relative shift of the adjacent [V<sub>6</sub>Sb<sub>6</sub>] layers. The magnetic properties of the K<sub>0.1(1)</sub>V<sub>6</sub>Sb<sub>6</sub> phase in the 2–300 K range are comparable to those of KV<sub>6</sub>Sb<sub>6</sub> and another Kagome antimonide KV<sub>3</sub>Sb<sub>5</sub>, consistent with nearly temperature-independent paramagnetism. Electronic band structure calculation suggests a nontrivial band topology with flat bands and opening of band crossing afforded by deintercalation. Transport property measurements reveal a metallic nature for K<sub>0.1(1)</sub>V<sub>6</sub>Sb<sub>6</sub> and a low thermal conductivity of 0.6 W K<sup>–1</sup> m<sup>–1</sup> at 300 K. Additionally, ion exchange in KV<sub>6</sub>Sb<sub>6</sub> via a solvothermal route leads to a successful partial exchange of K<sup>+</sup> with <i>A</i><sup>+</sup> (<i>A</i> = Na, Rb, and Cs). This study highlights the tunability of the layered structure of the KV<sub>6</sub>Sb<sub>6</sub> compound, providing a rich playground for the realization of new 2D materials.\",\"PeriodicalId\":49,\"journal\":{\"name\":\"Journal of the American Chemical Society\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":14.4000,\"publicationDate\":\"2024-09-21\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of the American Chemical Society\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/jacs.4c07285\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the American Chemical Society","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/jacs.4c07285","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
When van der Waals Met Kagome: A 2D Antimonide with a Vanadium-Kagome Network
2D materials showcase unconventional properties emerging from quantum confinement effects. In this work, a “soft chemical” route allows for the deintercalation of K+ from the layered antimonide KV6Sb6, resulting in the discovery of a new metastable 2D-Kagome antimonide K0.1(1)V6Sb6 with a van der Waals gap of 3.2 Å. The structure of K0.1(1)V6Sb6 was determined via the synergistic techniques, including X-ray pair distribution function analysis, advanced transmission electron microscopy, and density functional theory calculations. The K0.1(1)V6Sb6 compound crystallizes in the monoclinic space group C2/m (a = 9.57(2) Å, b = 5.502(8) Å, c = 10.23(2) Å, β = 97.6(2)°, Z = 2). The [V6Sb6] layers in K0.1(1)V6Sb6 are retained upon deintercalation and closely resemble the layers in the parent compound, yet deintercalation results in a relative shift of the adjacent [V6Sb6] layers. The magnetic properties of the K0.1(1)V6Sb6 phase in the 2–300 K range are comparable to those of KV6Sb6 and another Kagome antimonide KV3Sb5, consistent with nearly temperature-independent paramagnetism. Electronic band structure calculation suggests a nontrivial band topology with flat bands and opening of band crossing afforded by deintercalation. Transport property measurements reveal a metallic nature for K0.1(1)V6Sb6 and a low thermal conductivity of 0.6 W K–1 m–1 at 300 K. Additionally, ion exchange in KV6Sb6 via a solvothermal route leads to a successful partial exchange of K+ with A+ (A = Na, Rb, and Cs). This study highlights the tunability of the layered structure of the KV6Sb6 compound, providing a rich playground for the realization of new 2D materials.
期刊介绍:
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