Leonardo Tacconi, Anna Schannong Manvell, Matteo Briganti, Dominik Czernia, Hogni Weihe, Piotr Konieczny, Jesper Bendix, Mauro Perfetti
{"title":"利用高阶磁各向异性开发先进的磁致冷剂","authors":"Leonardo Tacconi, Anna Schannong Manvell, Matteo Briganti, Dominik Czernia, Hogni Weihe, Piotr Konieczny, Jesper Bendix, Mauro Perfetti","doi":"10.1002/anie.202417582","DOIUrl":null,"url":null,"abstract":"Three new 3d-4f complexes of general formula trans-[MF2(py)4][LnDOTA] (M = Cr3+ or Co3+, Ln = Dy3+ or Y3+, py = pyridine and DOTA = tetraazacyclododecane-N,N′,N″,N‴-tetraacetate) have been synthetised. The fluoride-bridged systems were designed to achieve perfect tetragonal symmetry by combining four-fold symmetric lanthanide and transition metal building blocks. From single crystal measurements, an unprecedented switch of the tetragonal anisotropy of the Dy3+ complexes has been observed. A combination of spectroscopic observations, magnetometry measurements and ab initio calculations allowed us to pinpoint the origin of this phenomenon, which is related to the peculiar energy level structure of the complexes. Moreover, the fourfold anisotropy of the complex has been exploited to design a rotating magnetocaloric experiment showing that tetragonal anisotropy holds great potential to engineer a new class of more efficient magnetic refrigerants.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"248 1","pages":""},"PeriodicalIF":16.1000,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Exploiting High Order Magnetic Anisotropy for Advanced Magnetocaloric Refrigerants\",\"authors\":\"Leonardo Tacconi, Anna Schannong Manvell, Matteo Briganti, Dominik Czernia, Hogni Weihe, Piotr Konieczny, Jesper Bendix, Mauro Perfetti\",\"doi\":\"10.1002/anie.202417582\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Three new 3d-4f complexes of general formula trans-[MF2(py)4][LnDOTA] (M = Cr3+ or Co3+, Ln = Dy3+ or Y3+, py = pyridine and DOTA = tetraazacyclododecane-N,N′,N″,N‴-tetraacetate) have been synthetised. The fluoride-bridged systems were designed to achieve perfect tetragonal symmetry by combining four-fold symmetric lanthanide and transition metal building blocks. From single crystal measurements, an unprecedented switch of the tetragonal anisotropy of the Dy3+ complexes has been observed. A combination of spectroscopic observations, magnetometry measurements and ab initio calculations allowed us to pinpoint the origin of this phenomenon, which is related to the peculiar energy level structure of the complexes. Moreover, the fourfold anisotropy of the complex has been exploited to design a rotating magnetocaloric experiment showing that tetragonal anisotropy holds great potential to engineer a new class of more efficient magnetic refrigerants.\",\"PeriodicalId\":125,\"journal\":{\"name\":\"Angewandte Chemie International Edition\",\"volume\":\"248 1\",\"pages\":\"\"},\"PeriodicalIF\":16.1000,\"publicationDate\":\"2024-11-18\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Angewandte Chemie International Edition\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1002/anie.202417582\",\"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":"Angewandte Chemie International Edition","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1002/anie.202417582","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
我们合成了通式为反式-[MF2(py)4][LnDOTA]（M = Cr3+ 或 Co3+，Ln = Dy3+ 或 Y3+，py = 吡啶，DOTA = 四氮杂环十二烷-N,N′,N″,N‴-四乙酸酯）的三种新的 3d-4f 复合物。氟化物桥接系统是通过将四倍对称的镧系元素和过渡金属构筑模块结合在一起而设计出来的，以实现完美的四方对称性。通过单晶测量，我们观察到 Dy3+ 复合物的四方各向异性发生了前所未有的变化。结合光谱观察、磁力测量和 ab initio 计算，我们确定了这一现象的起源，它与复合物的特殊能级结构有关。此外，我们还利用复合物的四重各向异性设计了一个旋转磁致冷实验，表明四方各向异性在设计一类新型高效磁制冷剂方面具有巨大潜力。
Exploiting High Order Magnetic Anisotropy for Advanced Magnetocaloric Refrigerants
Three new 3d-4f complexes of general formula trans-[MF2(py)4][LnDOTA] (M = Cr3+ or Co3+, Ln = Dy3+ or Y3+, py = pyridine and DOTA = tetraazacyclododecane-N,N′,N″,N‴-tetraacetate) have been synthetised. The fluoride-bridged systems were designed to achieve perfect tetragonal symmetry by combining four-fold symmetric lanthanide and transition metal building blocks. From single crystal measurements, an unprecedented switch of the tetragonal anisotropy of the Dy3+ complexes has been observed. A combination of spectroscopic observations, magnetometry measurements and ab initio calculations allowed us to pinpoint the origin of this phenomenon, which is related to the peculiar energy level structure of the complexes. Moreover, the fourfold anisotropy of the complex has been exploited to design a rotating magnetocaloric experiment showing that tetragonal anisotropy holds great potential to engineer a new class of more efficient magnetic refrigerants.
期刊介绍：
Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
京公网安备 11010802042870号
京ICP备2023020795号-1
分享
求助内容：
应助结果提醒方式：
扫码关注我们
