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Tuning the Mesomorphism and Redox Response of Anionic‐Ligand‐Based Mixed‐Valent Nickel(II) Complexes by Alkyl‐Substituted Quaternary Ammonium Cations
Chemistry - A European Journal ( IF 3.9 ) Pub Date : 2018-04-17 , DOI: 10.1002/chem.201706006 Yuichi Nakamura 1 , Takeshi Matsumoto 1 , Yasutaka Sakazume 1 , Junnosuke Murata 1 , Ho‐Chol Chang 1
Chemistry - A European Journal ( IF 3.9 ) Pub Date : 2018-04-17 , DOI: 10.1002/chem.201706006 Yuichi Nakamura 1 , Takeshi Matsumoto 1 , Yasutaka Sakazume 1 , Junnosuke Murata 1 , Ho‐Chol Chang 1
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The combination of the redox‐active mesogenic anion [NiII(Bdt)(BdtSQ)]− (Bdt=1,2‐benzenedithiolato; BdtSQ=1,2‐dithia‐semi‐benzoquinonato) with alkyl‐substituted ammonium cations afforded a series of redox‐active ionic complexes of the type [NR4][NiII(Bdt)(BdtSQ)] [R=nC16H33 (NC164Ni) and C8,10 (NC8,104Ni); C8,10=6‐octylhexadecyl] or [NMe2R2][NiII(Bdt)(BdtSQ)] [R=nC16H33 (NMe2C162Ni) and C8,10 (NMe2C8,102Ni)]. X‐ray crystallographic analyses of NMe2C162Ni and NC164Ni revealed the formation of cation‐dependent integrated ionic layers separated by interdigittated alkyl chains. Complexes NMe2C162Ni and NC164Ni commonly form crystalline phases at room temperature, whereas complexes NMe2C8,102Ni and NC8,104Ni, which contain branched alkyl chains, form a metastable mesophase and an amorphous phase at the same temperature, respectively. Furthermore, complexes NMe2C162Ni, NMe2C8,102Ni, and NC164Ni commonly form a smectic A phase (SmA) at 375, 317, and 342 K, respectively. For the four complexes, well‐defined cyclic voltammetry responses, derived from ligand‐based oxidation and reduction, were observed in solution and the condensed phases, that is, upon casting these complexes on an indium‐doped tin oxide working electrode. The present study demonstrates the tunability of the mesomorphism of ionic molecular assemblies composed of alkyl‐substituted quaternary ammonium cations, while maintaining the well‐defined redox responses of the anions even in the condensed phases.
中文翻译：
通过烷基取代的季铵盐阳离子调节阴离子-配体基混合价镍（II）配合物的同构和氧化还原响应
氧化还原活性的介晶阴离子[Ni II（Bdt）（BdtSQ）] -（Bdt = 1,2-苯二硫代巯基; BdtSQ = 1,2-二硫半-苯并喹啉酮）与烷基取代的铵阳离子的组合类型[NR 4 ] [Ni II（Bdt）（BdtSQ）] [R = n C 16 H 33（NC16 4 Ni）和C8,10（NC8,10 4 Ni）的氧化还原活性离子配合物；C8,10 = 6-辛基十六烷基]或[NMe 2 R 2 ] [Ni II（Bdt）（BdtSQ）] [R = n C 16 H 33（NMe 2 C16 2Ni）和C8,10（NMe 2 C8,10 2 Ni）]。NMe 2 C16 2 Ni和NC16 4 Ni的X射线晶体学分析表明，形成了由阳离子相互交叉的烷基链隔开的依赖阳离子的集成离子层。NMe 2 C16 2 Ni和NC16 4 Ni配合物通常在室温下形成结晶相，而含有支链烷基链的NMe 2 C8,10 2 Ni和NC8,10 4 Ni配合物在界面处形成亚稳中间相和非晶相。相同的温度。此外，络合物NMe 2 C16 2 Ni，NMe2 C8,10 2 Ni和NC16 4 Ni通常分别在375、317和342 K时形成近晶A相（SmA）。对于这四种络合物，在溶液和冷凝相中，即在将这些络合物浇铸在掺铟的氧化锡工作电极上时，观察到了基于配体的氧化和还原得到的明确的循环伏安法响应。本研究证明了由烷基取代的季铵阳离子组成的离子分子组装体的同构性的可调性，同时即使在缩合相中也可保持阴离子的明确定义的氧化还原响应。
更新日期：2018-04-17
中文翻译：
通过烷基取代的季铵盐阳离子调节阴离子-配体基混合价镍（II）配合物的同构和氧化还原响应
氧化还原活性的介晶阴离子[Ni II（Bdt）（BdtSQ）] -（Bdt = 1,2-苯二硫代巯基; BdtSQ = 1,2-二硫半-苯并喹啉酮）与烷基取代的铵阳离子的组合类型[NR 4 ] [Ni II（Bdt）（BdtSQ）] [R = n C 16 H 33（NC16 4 Ni）和C8,10（NC8,10 4 Ni）的氧化还原活性离子配合物；C8,10 = 6-辛基十六烷基]或[NMe 2 R 2 ] [Ni II（Bdt）（BdtSQ）] [R = n C 16 H 33（NMe 2 C16 2Ni）和C8,10（NMe 2 C8,10 2 Ni）]。NMe 2 C16 2 Ni和NC16 4 Ni的X射线晶体学分析表明，形成了由阳离子相互交叉的烷基链隔开的依赖阳离子的集成离子层。NMe 2 C16 2 Ni和NC16 4 Ni配合物通常在室温下形成结晶相，而含有支链烷基链的NMe 2 C8,10 2 Ni和NC8,10 4 Ni配合物在界面处形成亚稳中间相和非晶相。相同的温度。此外，络合物NMe 2 C16 2 Ni，NMe2 C8,10 2 Ni和NC16 4 Ni通常分别在375、317和342 K时形成近晶A相（SmA）。对于这四种络合物，在溶液和冷凝相中，即在将这些络合物浇铸在掺铟的氧化锡工作电极上时，观察到了基于配体的氧化和还原得到的明确的循环伏安法响应。本研究证明了由烷基取代的季铵阳离子组成的离子分子组装体的同构性的可调性，同时即使在缩合相中也可保持阴离子的明确定义的氧化还原响应。
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