Tuning linkage isomerism and magnetic properties of bi- and tri-metallic cage silsesquioxanes by cation and solvent effects

Bilyachenko Alexey N.; Korlyukov Alexander A.; Vologzhanina Anna V.; Khrustalev Victor N.; Kulakova Alena N.; Long Jerome; Larionova Joulia; Guari Yannick; Dronova Marina S.; Tsareva Ulyana S.; Dorovatovskii Pavel V.; Shubina Elena S.; Levitsky Mikhail M.

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Tuning linkage isomerism and magnetic properties of bi- and tri-metallic cage silsesquioxanes by cation and solvent effects

机译：通过阳离子和溶剂效应调节双金属笼式硅烷烷基硅氧烷和三金属笼中的连杆异构性和磁性

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Herein, the effect of replacement of the surrounding solvent and/or the partial substitution of sodium ions in the cage-like copper, sodium phenylsilsesquioxane [(PhSiO1.5) (12)(CuO)(4)(NaO0.5)(4)(n-BuOH)(6)] 1 with a globular structure was investigated; the synthesis of ten new derivatives of complex 1 was performed, and their crystal structures were determined. Solvate replacement of n-butanol in 1 with dimethyl sulfoxide, acetonitrile, 1,4-dioxane/EtOH, and 1,4-dioxane/PhCN afforded the complexes [(PhSiO1.5)(12)(CuO)(4)(NaO0.5)(4)(DMSO)(8)] (2), [(PhSiO1.5)(12)(CuO)(4)(NaO0.5)(4)(MeCN)(6)(H2O)(2)]center dot 2MeCN (3), [(PhSiO1.5)(12)(CuO)(4)(NaO0.5)(4)(C4H8O2)(EtOH)(4)]center dot 0.5EtOH (4), and [(PhSiO1.5)(12)(CuO)(4)(NaO0.5)(4)(C4H8O2)(4)(H2O)(3)]center dot 2PhCN center dot 2C(4)H(8)O(2)center dot H2O (5). In an aqueous solution of EtOH, a rearrangement reaction occurred instead of substitution, which resulted in a new complex, [(PhSiO1.5)(10)(CuO)(2)(NaO0.5)(2)(H2O)(6)] (6), with a cooling tower molecular structure. Transmetalation reactions of 1 with KCl or CsF resulted in the formation of the trimetallic complexes [(PhSiO1.5)(12)(CuO)(4)(NaO0.5)(2) (KO0.5)(2)(DMF)(6)] (7), [(PhSiO1.5)(12)(CuO)(4)(NaO0.5)(CsO0.5)(3)(DMF)(4)(DMSO)(H2O)]center dot 1.5DMF (8), [(PhSiO1.5)(12)(CuO)(4) (NaO0.5)(2)(CsO0.5)(2)(DMF)(8)]center dot 0.5H(2)O (9), and [(PhSiO1.5)(12)(CuO)(4)(NaO0.5)(3)(CsO0.5)(DMF)(4)] (10). The replacement of sodium ions of 1 by the bulky non-metallic cation PhMe3N+ upon the interaction of 1 with PhMe3NCl in a MeCN medium afforded the complex (PhNMe3)(2)[(PhSiO1.5)(12)(CuO)(4)(NaO0.5)(2)(O)(MeCN)(4)]center dot 4MeCN (11). X-ray analysis confirmed the successful replacement of terminal butanol molecules in all complexes and the stability of the globular cage of the parent complex under the reaction conditions, with the exceptions of complexes 6 and 9 that underwent an unprecedented reorganization of cage metallasilsesquioxane (CLMS) units into the cooling tower and sandwich-like cages, respectively. The stability of the cage during substitution reactions provides the first experimental evidence that polynuclear cage metallasilsesquioxanes can act as building blocks for the construction of coordination polymers, opening new ways for the synthesis of hybrid CLMS-based frameworks. In particular, the compounds 4, 6, 7, 9, and 10 are one-dimensional coordination polymers, and 5 and 8 are two-dimensional coordination polymers with a square lattice topology. A magnetism study of the coordination polymer compounds 5, 6, 8, and 9 showed antiferromagnetic behavior between copper centers.

机译：在此，在笼状铜中替换周围溶剂和/或部分取代钠离子，苯基钠喹甲烷[（pHSIO1.5）（12）（CuO）（4）（NaO 0.5）（4研究了（N-BUOH）（6）] 1，具有球状结构;进行了十种复合物1的新衍生物的合成，测定了它们的晶体结构。用二甲醚，乙腈，1,4-二恶烷/ EtOH和1,4-二恶烷/ phcn替代1丁醇的替代丁醇，得到复合物[（phsio1.5）（12）（CuO）（4）（Nao0 .5）（4）（DMSO）（8）]（2），[（PHSIO1.5）（12）（CUO）（4）（NaO 0.5）（4）（Mecn）（6）（H 2 O）（ 2）]中央点2mecn（3），[（pHSiO1.5）（12）（CuO）（4）（NaO 0.5）（4）（C4H8O2）（EtOH）（4）]中心点0.5 - OH（4），[（pHSiO1.5）（12）（CuO）（4）（NaO 0.5）（4）（4）（C4H8O2）（4）（H 2 O）（3）]中心点2phcn中心点2c（4）H（8 ）O（2）中心点H2O（5）。在EtOH的水溶液中，发生重排反应而不是取代，从而导致新的络合物，[（pHSiO1.5）（10）（10）（2）（NaO 0.5）（2）（H 2 O）（6 ）]（6），具有冷却塔的分子结构。用KCl或CSF的1透透透射反应导致粒子复合物[（pHSIO1.5）（12）（CuO）（4）（NaO 0.5）（2）（KO0.5）（2）（DMF）形成（6）]（7），[（PHSIO1.5）（12）（CUO）（4）（NaO 0.5）（CSO 0.5）（3）（DMF）（4）（DMSO）（H2O）]中心点1.5DMF（8），[（PHSIO1.5）（12）（CUO）（4）（NaO 0.5）（2）（CSO 0.5）（2）（DMF）（8）]中心点0.5h（ 2）O（9）和[（pHSiO1.5）（12）（CuO）（4）（NaO 0.5）（3）（CSO 0.5）（DMF）（4）]（10）。在MECN培养基中用PHME3NCL替换庞大的非金属阳离子pHME3N +在镁培养基中的相互作用时替换1的钠离子，得到复合物（PHNME3）（2）[（PHSIO1.5）（12）（CUO）（4）（Nao0.5）（2）（O）（MECN）（4）]中心点4MECN（11）。 X射线分析证实了在反应条件下成功替代所有复合物中的末端丁醇分子和母体复合物的球笼的稳定性，其中复合物6和9的例外，经历了前所未有的笼式金属钠（CLM）的重组单位分别进入冷却塔和夹层状笼子。封闭反应期间笼的稳定性提供了第一种实验证据，即多核笼式金属金属晶晶片喹术料可以充当用于构建配位聚合物的构建块，开启合成混合动力CLMS的框架的新方法。特别地，化合物4,6,7,9和10是一维配位聚合物，5和8是具有方形晶格拓扑的二维配位聚合物。配位聚合物化合物5,6,8和9的磁性研究在铜中心之间显示了铜胶质行为。

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来源
《Dalton transactions: An international journal of inorganic chemistry》 |2017年第38期|共15页
作者
Bilyachenko Alexey N.; Korlyukov Alexander A.; Vologzhanina Anna V.; Khrustalev Victor N.; Kulakova Alena N.; Long Jerome; Larionova Joulia; Guari Yannick; Dronova Marina S.; Tsareva Ulyana S.; Dorovatovskii Pavel V.; Shubina Elena S.; Levitsky Mikhail M.;
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Russian Acad Sci AN Nesmeyanov Inst Organoelement Cpds Vavilov Str 28 Moscow 119991 Russia;

Russian Acad Sci AN Nesmeyanov Inst Organoelement Cpds Vavilov Str 28 Moscow 119991 Russia;

Russian Acad Sci AN Nesmeyanov Inst Organoelement Cpds Vavilov Str 28 Moscow 119991 Russia;

RUDN Univ Peoples Friendship Univ Russia Miklukho Maklay St 6 Moscow 117198 Russia;

Russian Acad Sci AN Nesmeyanov Inst Organoelement Cpds Vavilov Str 28 Moscow 119991 Russia;

Univ Montpellier ENSCM CNRS Inst Charles Gerhardt UMR5253 Ingn Mol &

Nanoobje Pl Eugene Bataillon F-34095 Montpellier 05 France;

Univ Montpellier ENSCM CNRS Inst Charles Gerhardt UMR5253 Ingn Mol &

Nanoobje Pl Eugene Bataillon F-34095 Montpellier 05 France;

Univ Montpellier ENSCM CNRS Inst Charles Gerhardt UMR5253 Ingn Mol &

Nanoobje Pl Eugene Bataillon F-34095 Montpellier 05 France;

Russian Acad Sci AN Nesmeyanov Inst Organoelement Cpds Vavilov Str 28 Moscow 119991 Russia;

Russian Acad Sci AN Nesmeyanov Inst Organoelement Cpds Vavilov Str 28 Moscow 119991 Russia;

Kurchatov Inst Natl Res Ctr Pl Akad Kurchatova 1 Moscow 123098 Russia;

Russian Acad Sci AN Nesmeyanov Inst Organoelement Cpds Vavilov Str 28 Moscow 119991 Russia;

Russian Acad Sci AN Nesmeyanov Inst Organoelement Cpds Vavilov Str 28 Moscow 119991 Russia;

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1. Tuning linkage isomerism and magnetic properties of bi- and tri-metallic cage silsesquioxanes by cation and solvent effects [J] . Bilyachenko Alexey N., Korlyukov Alexander A., Vologzhanina Anna V., Dalton transactions: An international journal of inorganic chemistry . 2017,第38期

机译：通过阳离子和溶剂效应调节双金属笼式硅烷烷基硅氧烷和三金属笼中的连杆异构性和磁性
2. Mono-, bi-, and tri-metallic Ni-based catalysts for the catalytic hydrotreatment of pyrolysis liquids [J] . Wang Yin, Robbie H. Venderbosch, Songbo He, Biomass Conversion and Biorefinery . 2017,第3期

机译：基于单金属Ni的热解液的单金属Ni催化剂
3. Production of hydrogen by catalytic methane decomposition over alumina supported mono-, bi- and tri-metallic catalysts [J] . Al-Fatesh A. S., Fakeeha A. H., Khan W. U., International journal of hydrogen energy . 2016,第48期

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4. Preparation and properties of cage-like octaaminopropyl polyhedral oligomeric silsesquioxane/polyvinyl alcohol hybrid materials [C] . Xiaojing Zhang, Chaojun Wang, Jiashu Sun International Conference on Chemical Engineering and Advanced Materials . 2011

机译：笼状八氨基丙基多面体低聚硅氧烷喹甲酸/聚乙烯醇杂交材料的制备及性能
5. Modification of the electronic properties of inorganic cage compounds: Tuning guest-framework interactions in sodalites and clathrates. [D] . Latturner, Susan Elizabeth. 2000

机译：改变无机笼状化合物的电子性能：调整方钠石和包合物中的客体-框架相互作用。
6. Hyperbranched Polysiloxanes Based on Polyhedral Oligomeric Silsesquioxane Cages with Ultra-High Molecular Weight and Structural Tuneability [O] . Ning Liu, Jianyi Yu, Yaoyong Meng, 2018

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7. Mono-, bi-, and tri-metallic Ni-based catalysts for the catalytic hydrotreatment of pyrolysis liquids [O] . Wang Yin, Robbie H. Venderbosch, Songbo He, 2017

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Tuning linkage isomerism and magnetic properties of bi- and tri-metallic cage silsesquioxanes by cation and solvent effects

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