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An Organic-Inorganic Hybrid Exhibiting Electrical Conduction and Single-Ion Magnetism.
Angewandte Chemie International Edition ( IF 16.6 ) Pub Date : 2020-01-21 , DOI: 10.1002/anie.201910523
Yongbing Shen 1 , Goulven Cosquer 1, 2 , Hiroshi Ito 3 , David C Izuogu 4, 5 , Alex J W Thom 4 , Toshiaki Ina 6 , Tomoya Uruga 6 , Takefumi Yoshida 7 , Shinya Takaishi 1 , Brian K Breedlove 1 , Zhao-Yang Li 8 , Masahiro Yamashita 1, 8, 9
Affiliation  

The first three-dimensional (3D) conductive single-ion magnet (SIM), (TTF)2 [Co(pdms)2 ] (TTF=tetrathiafulvalene and H2 pdms=1,2-bis(methanesulfonamido)benzene), was electrochemically synthesised and investigated structurally, physically, and theoretically. The similar oxidation potentials of neutral TTF and the molecular precursor [HNEt3 ]2 [M(pdms)2 ] (M=Co, Zn) allow for multiple charge transfers (CTs) between the SIM donor [M(pdms)2 ]n- and the TTF.+ acceptor, as well as an intradonor CT from the pdms ligand to Co ion upon electrocrystallisation. Usually TTF functions as a donor, whereas in our system TTF is both a donor and an accepter because of the similar oxidation potentials. Furthermore, the [M(pdms)2 ]n- donor and TTF.+ acceptor are not segregated but strongly interact with each other, contrary to reported layered donor-acceptor electrical conductors. The strong intermolecular and intramolecular interactions, combined with CT, allow for relatively high electrical conductivity even down to very low temperatures. Furthermore, SIM behaviour with slow magnetic relaxation and opening of hysteresis loops was observed. (TTF)2 [Co(pdms)2 ] (2-Co) is an excellent building block for preparing new conductive SIMs.

中文翻译:

具有导电性和单离子磁性的有机-无机杂化体。

电化学合成了第一个三维(3D)导电单离子磁体(SIM)(TTF)2 [Co(pdms)2](TTF = tetrathiafulvalene和H2 pdms = 1,2-双(甲磺酰胺基)苯)并在结构,物理和理论上进行了研究。中性TTF和分子前体[HNEt3] 2 [M(pdms)2](M = Co,Zn)的相似氧化电位可实现SIM供体[M(pdms)2] n-之间的多次电荷转移(CT)。以及TTF。+受体,以及电结晶后从pdms配体到Co离子的供体内CT。通常,TTF充当供体,而在我们的系统中,TTF既是供体又是受体,因为它们的氧化电位相似。此外,[M(pdms)2] n-供体和TTF。+受体没有分离,但彼此之间相互作用很强,与报道的分层供体-受体电导体相反。强大的分子间和分子内相互作用以及CT,即使在非常低的温度下也具有相对较高的电导率。此外,观察到具有缓慢磁弛豫和磁滞回线打开的SIM行为。(TTF)2 [Co(pdms)2](2-Co)是用于制备新的导电SIM的出色构建基块。
更新日期:2020-01-22
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