{"title":"由二镍(II)金属环和二苄基铵轮轴组成的无螺纹轮轴组件和轮轴型螺纹轮轴组件。","authors":"Yoko Sakata, Seiya Kobayashi, Misato Yamamoto, Katsuya Doken, Mayu Kamezawa, Sachiko Yamaki, Shigehisa Akine","doi":"10.1038/s42004-024-01246-8","DOIUrl":null,"url":null,"abstract":"Rotaxanes are typically prepared using covalent bonds to trap a wheel component onto an axle molecule, and rotaxane-type wheel–axle assembly using only noncovalent interactions has been far less explored. Here we show that a dinickel(II) metallomacrocycle forms two different types of wheel–axle assemblies with a dibenzylammonium axle molecule based only on noncovalent interactions. The non-threaded assembly was obtained by introduction of Ni2+ into the macrocycle before the complexation with the axle molecule (metal-first method). The non-threaded assembly was in rapid equilibrium with each of the components in solution. The threaded assembly was obtained by introduction of Ni2+ after the formation of a pseudorotaxane from the non-metalated wheel and the axle molecule (axle-first method). The threaded assembly was not in equilibrium with the dissociated species even though it was maintained only by noncovalent interactions. Thus, formation of one of the non-threaded and threaded wheel–axle assemblies over the other is governed by the assembly pathway. Mechanically interlocked rotaxanes are typically prepared using covalent bonds to trap a wheel component onto an axle molecule, and rotaxane-type wheel–axle assembly using only noncovalent interactions has been far less explored. Here, a dinickel(II) metallomacrocycle is found to form two different types of wheel–axle assemblies, with a dibenzylammonium axle molecule forming both non-threaded and rotaxane-type threaded assemblies, based only on noncovalent interactions, with formation of one over the other governed by the assembly pathway.","PeriodicalId":10529,"journal":{"name":"Communications Chemistry","volume":null,"pages":null},"PeriodicalIF":5.9000,"publicationDate":"2024-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11289445/pdf/","citationCount":"0","resultStr":"{\"title\":\"Non-threaded and rotaxane-type threaded wheel–axle assemblies consisting of dinickel(II) metallomacrocycle and dibenzylammonium axle\",\"authors\":\"Yoko Sakata, Seiya Kobayashi, Misato Yamamoto, Katsuya Doken, Mayu Kamezawa, Sachiko Yamaki, Shigehisa Akine\",\"doi\":\"10.1038/s42004-024-01246-8\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Rotaxanes are typically prepared using covalent bonds to trap a wheel component onto an axle molecule, and rotaxane-type wheel–axle assembly using only noncovalent interactions has been far less explored. Here we show that a dinickel(II) metallomacrocycle forms two different types of wheel–axle assemblies with a dibenzylammonium axle molecule based only on noncovalent interactions. The non-threaded assembly was obtained by introduction of Ni2+ into the macrocycle before the complexation with the axle molecule (metal-first method). The non-threaded assembly was in rapid equilibrium with each of the components in solution. The threaded assembly was obtained by introduction of Ni2+ after the formation of a pseudorotaxane from the non-metalated wheel and the axle molecule (axle-first method). The threaded assembly was not in equilibrium with the dissociated species even though it was maintained only by noncovalent interactions. Thus, formation of one of the non-threaded and threaded wheel–axle assemblies over the other is governed by the assembly pathway. Mechanically interlocked rotaxanes are typically prepared using covalent bonds to trap a wheel component onto an axle molecule, and rotaxane-type wheel–axle assembly using only noncovalent interactions has been far less explored. Here, a dinickel(II) metallomacrocycle is found to form two different types of wheel–axle assemblies, with a dibenzylammonium axle molecule forming both non-threaded and rotaxane-type threaded assemblies, based only on noncovalent interactions, with formation of one over the other governed by the assembly pathway.\",\"PeriodicalId\":10529,\"journal\":{\"name\":\"Communications Chemistry\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.9000,\"publicationDate\":\"2024-07-31\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11289445/pdf/\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Communications Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.nature.com/articles/s42004-024-01246-8\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Communications Chemistry","FirstCategoryId":"92","ListUrlMain":"https://www.nature.com/articles/s42004-024-01246-8","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Non-threaded and rotaxane-type threaded wheel–axle assemblies consisting of dinickel(II) metallomacrocycle and dibenzylammonium axle
Rotaxanes are typically prepared using covalent bonds to trap a wheel component onto an axle molecule, and rotaxane-type wheel–axle assembly using only noncovalent interactions has been far less explored. Here we show that a dinickel(II) metallomacrocycle forms two different types of wheel–axle assemblies with a dibenzylammonium axle molecule based only on noncovalent interactions. The non-threaded assembly was obtained by introduction of Ni2+ into the macrocycle before the complexation with the axle molecule (metal-first method). The non-threaded assembly was in rapid equilibrium with each of the components in solution. The threaded assembly was obtained by introduction of Ni2+ after the formation of a pseudorotaxane from the non-metalated wheel and the axle molecule (axle-first method). The threaded assembly was not in equilibrium with the dissociated species even though it was maintained only by noncovalent interactions. Thus, formation of one of the non-threaded and threaded wheel–axle assemblies over the other is governed by the assembly pathway. Mechanically interlocked rotaxanes are typically prepared using covalent bonds to trap a wheel component onto an axle molecule, and rotaxane-type wheel–axle assembly using only noncovalent interactions has been far less explored. Here, a dinickel(II) metallomacrocycle is found to form two different types of wheel–axle assemblies, with a dibenzylammonium axle molecule forming both non-threaded and rotaxane-type threaded assemblies, based only on noncovalent interactions, with formation of one over the other governed by the assembly pathway.
期刊介绍:
Communications Chemistry is an open access journal from Nature Research publishing high-quality research, reviews and commentary in all areas of the chemical sciences. Research papers published by the journal represent significant advances bringing new chemical insight to a specialized area of research. We also aim to provide a community forum for issues of importance to all chemists, regardless of sub-discipline.