Square-Planar Ruthenium(II) Complexes: Control of Spin State by Pincer Ligand Functionalization

Askevold Bjorn; Khusniyarov Marat M.; Kroener Wolfgang; Gieb Klaus; Mueller Paul; Herdtweck Eberhardt; Heinemann Frank W.; Diefenbach Martin; Holthausen Max C.; Vieru Veacheslav; Chibotaru Liviu F.; Schneider Sven

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Square-Planar Ruthenium(II) Complexes: Control of Spin State by Pincer Ligand Functionalization

机译：方平面钌（II）配合物：通过钳配体配体化功能控制自旋状态。

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Functionalization of the PNP pincer ligand backbone allows for a comparison of the dialkyl amido, vinyl alkyl amido, and divinyl amido ruthenium(II) pincer complex series [RuCl{N(CH2CH2PtBu2)(2)}], [RuCl{N(CHCHPtBu2)(CH2CH2PtBu2)}], and [RuCl{N(CHCHPtBu2)(2)}], in which the ruthenium( II) ions are in the extremely rare square-planar coordination geometry. Whereas the dialkylamido complex adopts an electronic singlet (S=0) ground state and energetically low-lying triplet (S=1) state, the vinyl alkyl amido and the divinyl amido complexes exhibit unusual triplet (S=1) ground states as confirmed by experimental and computational examination. However, essentially non-magnetic ground states arise for the two intermediate-spin complexes owing to unusually large zero-field splitting (D> +200 cm(-1)). The change in ground state electronic configuration is attributed to tailored pincer ligand-to-metal pi-donation within the PNP ligand series.

机译：PNP夹钳配体主链的功能允许比较二烷基酰胺基，乙烯基烷基酰胺基和二乙烯基酰胺基钌（II）钳形复合物系列[RuCl {N（CH2CH2PtBu2）（2）}]，[RuCl {N（CHCHPtBu2）（CH2CH2PtBu2）}]和[RuCl {N（CHCHPtBu2）（2）}]，其中钌（II）离子处于极为罕见的方平面配位几何结构中。尽管二烷基酰胺基络合物采用电子单重态（S = 0）基态和低能三重态（S = 1）态，但乙烯基烷基酰胺基和二乙烯基酰胺基络合物表现出不寻常的三重态（S = 1）基态，如实验和计算检查。但是，由于异常大的零场分裂（D> +200 cm（-1）），两个中间自旋复合物基本上会出现非磁性基态。基态电子构型的变化归因于PNP配体系列中量身定制的从钳子到金属的pi-donation。

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来源
《Chemistry: A European journal》 |2015年第2期|共11页
作者
Askevold Bjorn; Khusniyarov Marat M.; Kroener Wolfgang; Gieb Klaus; Mueller Paul; Herdtweck Eberhardt; Heinemann Frank W.; Diefenbach Martin; Holthausen Max C.; Vieru Veacheslav; Chibotaru Liviu F.; Schneider Sven;
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正文语种 eng
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computer chemistry; ligands; magnetic properties; NMR spectroscopy; ruthenium;

机译：计算机化学;配体;磁性;NMR光谱;钌;

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1. Square-Planar Ruthenium(II) Complexes: Control of Spin State by Pincer Ligand Functionalization [J] . Askevold Bjorn, Khusniyarov Marat M., Kroener Wolfgang, Chemistry: A European journal . 2015,第2期

机译：方平面钌（II）配合物：通过钳配体配体化功能控制自旋状态。
2. Synthesis and characterization of a family of M2+ complexes supported by a trianionic ONO3- pincer-type ligand: towards the stabilization of high-spin square-planar complexes [J] . Pascualini M. E., Stoian S. A., Ozarowski A., Dalton transactions: An international journal of inorganic chemistry . 2015,第46期

机译：三阴离子ONO3-钳型配体支持的M2 +配合物家族的合成与表征：稳定高纺丝方平面配合物
3. Ruthenium(II) and osmium(II) complexes bearing bipyridine and the N-heterocyclic carbene-based C^N^C pincer ligand: An experimental and density functional theory study [J] . Chung L.-H., Cho K.-S., England J., Inorganic Chemistry: A Research Journal that Includes Bioinorganic, Catalytic, Organometallic, Solid-State, and Synthetic Chemistry and Reaction Dynamics . 2013,第17期

机译：带有联吡啶和基于N-杂环卡宾的C ^ N ^ C钳位配体的钌（II）和（II）配合物：实验和密度泛函理论研究
4. Preparation of Transition Metal Complexes Based on NNN-Type Pincer Ligand Incorporating Imidazo1,5-apyridine Moiety and Their Photofunctionality [C] . Fumitoshi Yagishita, Shun Ikami, Souta Shimokawa 日本化学会春季年会講演予稿集 . 2018

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5. IRON AND RUTHENIUM COMPLEXES POSSESSING UNUSUAL ELECTRONIC PROPERTIES. PART I: SYNTHESIS AND SPIN STATE STUDIES OF GAMMA-SUBSTITUTED TRIS(BETA-DIKETONATO)IRON(III) COMPLEXES AND THEIR BETA-KETOIMINE ANALOGUES DERIVED FROM TRIETHYLENETETRAMINE. PART II: A DIRECT MEASUREMENT OF DYNAMIC SPIN INTERCONVERSION RATES IN THE SPIN EQUILIBRIUM PROTEIN FERRIC MYOGLOBIN HYDROXIDE. PART III: SYNTHESIS, PHOTOEMISSION, AND ELECTROCHEMICAL STUDIES OF. [D] . DOSE, ERIC VON. 1978

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6. A high-spin square-planar Fe(ii) complex stabilized by a trianionic pincer-type ligand and conclusive evidence for retention of geometry and spin state in solution [O] . M. E. Pascualini, N. V. Di Russo, A. E. Thuijs, 2015

机译：由三阴离子钳型配体稳定的高纺丝方平面Fe（ii）配合物并在溶液中保留了几何形状和自旋态的确凿证据
7. A high-spin square-planar Fe(ii) complex stabilized by a trianionic pincer-type ligand and conclusive evidence for retention of geometry and spin state in solution [O] . M. E. Pascualini, N. V. Di Russo, A. E. Thuijs, 2015

机译：通过Traianion inpiner型配体稳定的高旋转正方形Fe（II）复合物，以及确定溶液中的几何形状和旋转状态的确凿证据
8. Unique Spectroscopic Properties of Mixed-Ligand Complexes with 2,2'-Dipyridylamine: A Dual Luminescence from a Ruthenium(II) Complex [R] . Blakley, R. L., DeArmond, M. K. 1987

机译：具有2,2'-二吡啶胺的混合配体配合物的独特光谱性质：来自钌（II）配合物的双重发光

Square-Planar Ruthenium(II) Complexes: Control of Spin State by Pincer Ligand Functionalization

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