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Heterotrimetallic Mixed-Valent Molecular Precursors Containing Periodic Table Neighbors: Assignment of Metal Positions and Oxidation States.
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-03-12 , DOI: 10.1002/anie.202001083
Haixiang Han 1, 2 , Jesse C Carozza 1 , Audra P Colliton 1 , Yuxuan Zhang 1 , Zheng Wei 1 , Alexander S Filatov 3 , Yu-Sheng Chen 4 , Melisa Alkan 5 , Andrey Yu Rogachev 5 , Evgeny V Dikarev 1
Affiliation  

A known trinuclear structure was used to design the heterobimetallic mixed‐valent, mixed‐ligand molecule [CoII(hfac)3−Na−CoIII(acac)3] (1 ). This was used as a template structure to develop heterotrimetallic molecules [CoII(hfac)3−Na−FeIII(acac)3] (2 ) and [NiII(hfac)3−Na−CoIII(acac)3] (3 ) via isovalent site‐specific substitution at either of the cobalt positions. Diffraction methods, synchrotron resonant diffraction, and multiple‐wavelength anomalous diffraction were applied beyond simple structural investigation to provide an unambiguous assignment of the positions and oxidation states for the periodic table neighbors in the heterometallic assemblies. Molecules of 2 and 3 are true heterotrimetallic rather than a statistical mixture of two heterobimetallic counterparts. Trinuclear platform 1 exhibits flexibility in accommodating a variety of di‐ and trivalent metals, which can be further utilized in the design of molecular precursors for the NaMM′O4 functional oxide materials.

中文翻译:

含有周期表邻居的杂三金属混合价分子前体:金属位置和氧化态的分配。

已知的三核结构用于设计异双金属混合价,混合配体分子[Co II(hfac)3 -Na-Co III(acac)3 ](1)。将其用作开发杂三金属分子[Co II(hfac)3 -Na-Fe III(acac)3 ](2)和[Ni II(hfac)3 -Na-Co III(acac)3 ](3)通过任一钴位置的等价位点特异性取代。除简单的结构研究外,还应用了衍射方法,同步加速器共振衍射和多波长异常衍射,以为异金属组件中的元素周期表邻居提供明确的位置和氧化态分配。23的分子是真正的异三金属,而不是两个异双金属对应物的统计混合物。三核平台1在适应各种二价和三价金属方面表现出灵活性,可以进一步用于设计NaMM'O 4功能性氧化物材料的分子前体。
更新日期:2020-03-12
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