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Coordination-Driven Self-Assembly of Heterotrimetallic Barrel and Bimetallic Cages Using a Cobalt Sandwich-Based Tetratopic Donor
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2018-01-10 00:00:00 , DOI: 10.1021/acs.inorgchem.7b02653 Nem Singh 1 , Jatinder Singh 1 , Dongwook Kim 2 , Dong Hwan Kim 1 , Eun-Hee Kim 3 , Myoung Soo Lah 2 , Ki-Whan Chi 1
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2018-01-10 00:00:00 , DOI: 10.1021/acs.inorgchem.7b02653 Nem Singh 1 , Jatinder Singh 1 , Dongwook Kim 2 , Dong Hwan Kim 1 , Eun-Hee Kim 3 , Myoung Soo Lah 2 , Ki-Whan Chi 1
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Three-dimensional molecular architectures self-assembled with tripodal and tetratopic donors are valuable because of their encapsulation properties. Here, we present Co(I)–Fe(II)–Pd(II) heterotrimetallic trifacial barrel 1, which was self-assembled using a newly synthesized tetratopic donor [CpCo(CbR4)] [L; Cp = cyclopentadienyl, Cb = cyclobudiene, and R = 4-(4-pyridylphenyl)] and a 90° acceptor [cis-(dppf)Pd(OTf)2] (A1; dppf = (diphenylphosphino)ferrocene and OTf = CF3SO3–). The heterotrimetallic barrel 1 exhibited selective 1:1 interaction with a N,N′-dimethyl-1,4,5,8-naphthalenetetracarboxylic diimide guest, as revealed by 1H NMR analysis. The self-assembly of donor L with two other Ru(II)-based 180° acceptors [(p-cymene)2Ru2(OO∩OO)(OTf)2] [OO∩OO = 6,11-dioxido-5,12-naphthacenedione (A2) and oxalate (A3)] resulted in tetragonal-prismatic cages. Self-assembly using the longer acceptor A2 provided rare isomers of a tetragonal-prismatic cage by varying the orientation of the cyclopentadienyl moiety out–out (2a) or out–in (2b) of the cavity, whereas self-assembly using the shorter acceptor A3 selectively resulted in the tetragonal-prismatic cage 3. The three-dimensional molecular architectures 1–3 were characterized by combined spectroscopic and elemental analyses. The structures of molecular barrel 1 and prismatic cage 3 were elucidated by single-crystal X-ray analysis.
中文翻译：
三钴金属桶和双金属笼子的钴基四元供体的配位驱动自组装。
与三脚架和四位供体自组装的三维分子结构因其封装特性而非常有价值。这里，我们提出的Co（I）-Fe（II）-Pd（II）heterotrimetallic trifacial枪管1，这是使用新合成的供体tetratopic [CpCo（CBR自组装4）] [大号; Cp =环戊二烯基，Cb =环丁二烯，R = 4-（4-吡啶基苯基）]和90°受体[顺式-（dppf）Pd（OTf）2 ]（A1； dppf =（二苯基膦基）二茂铁，OTf = CF 3 SO 3 –）。异质三金属桶1与N，N表现出选择性的1：1相互作用1 H NMR分析表明，′-二甲基-1,4,5,8-萘四甲酸二酰亚胺客体。供体L与另外两个基于Ru（II）的180°受体[（p- Cymene）2 Ru 2（OO∩OO）（OTf）2 ]的自组装[OO∩OO= 6,11-dioxido-5 ，12-萘二甲酮（A2）和草酸盐（A3）]形成四方棱柱形笼。通过使用更长的受体A2进行自组装，可以通过改变环戊二烯基部分的取向（向外（2 a）或向外（2 b））来提供四方棱柱形笼的稀有异构体）的腔，而使用较短的受体A3的自组装选择性地导致四方棱柱形笼3。三维分子结构1 - 3通过组合光谱和元素分析进行表征。通过单晶X射线分析阐明了分子桶1和棱柱形笼3的结构。
更新日期：2018-01-10
中文翻译：
三钴金属桶和双金属笼子的钴基四元供体的配位驱动自组装。
与三脚架和四位供体自组装的三维分子结构因其封装特性而非常有价值。这里，我们提出的Co（I）-Fe（II）-Pd（II）heterotrimetallic trifacial枪管1，这是使用新合成的供体tetratopic [CpCo（CBR自组装4）] [大号; Cp =环戊二烯基，Cb =环丁二烯，R = 4-（4-吡啶基苯基）]和90°受体[顺式-（dppf）Pd（OTf）2 ]（A1； dppf =（二苯基膦基）二茂铁，OTf = CF 3 SO 3 –）。异质三金属桶1与N，N表现出选择性的1：1相互作用1 H NMR分析表明，′-二甲基-1,4,5,8-萘四甲酸二酰亚胺客体。供体L与另外两个基于Ru（II）的180°受体[（p- Cymene）2 Ru 2（OO∩OO）（OTf）2 ]的自组装[OO∩OO= 6,11-dioxido-5 ，12-萘二甲酮（A2）和草酸盐（A3）]形成四方棱柱形笼。通过使用更长的受体A2进行自组装，可以通过改变环戊二烯基部分的取向（向外（2 a）或向外（2 b））来提供四方棱柱形笼的稀有异构体）的腔，而使用较短的受体A3的自组装选择性地导致四方棱柱形笼3。三维分子结构1 - 3通过组合光谱和元素分析进行表征。通过单晶X射线分析阐明了分子桶1和棱柱形笼3的结构。
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