简便合成咪唑烷基苯酚支撑的双铜(II/II)配合物：以 MeOCO2- 的形式活化和固定大气中的二氧化碳，显示外源桥调制磁交换耦合

IF 2.7 3区化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Inorganica Chimica Acta Pub Date : 2024-08-04 DOI:10.1016/j.ica.2024.122298

{"title":"简便合成咪唑烷基苯酚支撑的双铜(II/II)配合物：以 MeOCO2- 的形式活化和固定大气中的二氧化碳，显示外源桥调制磁交换耦合","authors":"","doi":"10.1016/j.ica.2024.122298","DOIUrl":null,"url":null,"abstract":"<div>Two imidazolidine grafted Schiff bases H3L2 and H3L3 have been utilized to fasten the Cu2 core in four new complexes [Cu2(μ-L2)(μ-O2CMe)]·H2O (1·H2O), [Cu2(μ-L2)(μ-O2COMe)]·H2O (2·H2O), [Cu2(μ-L2)(μ-NO3)]·H2O (3·H2O) and [Cu2L3(μ-OAc)]·5H2O (4·5H2O). Room temperature solution reaction of H3L2 with Cu2(OAc)4·2H2O provided 1·H2O in good yield. Follow-up reaction of 1·H2O with Et4NOH in air replaces μ-O2CMe (acetato) bridge by MeOCO2− (monomethyl carbonato) linker in 2·H2O. Single crystal X-ray structure established the individual complexes and confirmed the fixation of atmospheric CO2. Variable temperature (2 to 300 K) magnetic susceptibility measurements recognized the antiferromagnetic exchange interactions between the adjacent copper(II) centers in complexes 2 and 3. The amount of spin–spin interactions are found to be higher for ancillary NO3− bridge (−284 cm−1) compared to the in situ transformed MeOCO2− bridged (−1.64 cm−1).</div>","PeriodicalId":13599,"journal":{"name":"Inorganica Chimica Acta","volume":null,"pages":null},"PeriodicalIF":2.7000,"publicationDate":"2024-08-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Facile synthesis of imidazolidinyl phenolate supported Dicopper(II/II) Complexes: Activation and fixation of atmospheric CO2 as MeOCO2− showing exogenous bridge modulating magnetic exchange coupling\",\"authors\":\"\",\"doi\":\"10.1016/j.ica.2024.122298\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div>Two imidazolidine grafted Schiff bases H3L2 and H3L3 have been utilized to fasten the Cu2 core in four new complexes [Cu2(μ-L2)(μ-O2CMe)]·H2O (1·H2O), [Cu2(μ-L2)(μ-O2COMe)]·H2O (2·H2O), [Cu2(μ-L2)(μ-NO3)]·H2O (3·H2O) and [Cu2L3(μ-OAc)]·5H2O (4·5H2O). Room temperature solution reaction of H3L2 with Cu2(OAc)4·2H2O provided 1·H2O in good yield. Follow-up reaction of 1·H2O with Et4NOH in air replaces μ-O2CMe (acetato) bridge by MeOCO2− (monomethyl carbonato) linker in 2·H2O. Single crystal X-ray structure established the individual complexes and confirmed the fixation of atmospheric CO2. Variable temperature (2 to 300 K) magnetic susceptibility measurements recognized the antiferromagnetic exchange interactions between the adjacent copper(II) centers in complexes 2 and 3. The amount of spin–spin interactions are found to be higher for ancillary NO3− bridge (−284 cm−1) compared to the in situ transformed MeOCO2− bridged (−1.64 cm−1).</div>\",\"PeriodicalId\":13599,\"journal\":{\"name\":\"Inorganica Chimica Acta\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":2.7000,\"publicationDate\":\"2024-08-04\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Inorganica Chimica Acta\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S002016932400389X\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, INORGANIC & NUCLEAR\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Inorganica Chimica Acta","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S002016932400389X","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, INORGANIC & NUCLEAR","Score":null,"Total":0}

引用次数: 0

摘要

两种咪唑烷接枝希夫碱 H3L2 和 H3L3 被用来固定四种新配合物 [Cu2(μ-L2)(μ-O2CMe)]-H2O (1-H2O) 中的 Cu2 核心、[Cu2(μ-L2)(μ-O2COMe)]-H2O（2-H2O）、[Cu2(μ-L2)(μ-NO3)]-H2O（3-H2O）和[Cu2L3(μ-OAc)]-5H2O（4-5H2O）。H3L2 与 Cu2(OAc)4-2H2O 的室温溶液反应生成了 1-H2O，收率很高。1-H2O 与 Et4NOH 在空气中发生后续反应，在 2-H2O 中，MeOCO2-（碳一甲基）连接体取代了 μ-O2CMe （乙酰基）桥。单晶 X 射线结构确定了单个复合物，并证实了对大气中 CO2 的固定作用。变温（2 至 300 K）磁感应强度测量确认了络合物 2 和 3 中相邻铜（II）中心之间的反铁磁交换相互作用。与原位转化的 MeOCO2- 桥接（-1.64 cm-1）相比，辅助 NO3- 桥接（-284 cm-1）的自旋-自旋相互作用量更高。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

摘要图片

查看原文

微信好友朋友圈 QQ好友复制链接

本刊更多论文

Facile synthesis of imidazolidinyl phenolate supported Dicopper(II/II) Complexes: Activation and fixation of atmospheric CO2 as MeOCO2− showing exogenous bridge modulating magnetic exchange coupling

Two imidazolidine grafted Schiff bases H₃L₂ and H₃L₃ have been utilized to fasten the Cu₂ core in four new complexes [Cu₂(μ-L₂)(μ-O₂CMe)]·H₂O (1·H₂O), [Cu₂(μ-L₂)(μ-O₂COMe)]·H₂O (2·H₂O), [Cu₂(μ-L₂)(μ-NO₃)]·H₂O (3·H₂O) and [Cu₂L₃(μ-OAc)]·5H₂O (4·5H₂O). Room temperature solution reaction of H₃L₂ with Cu₂(OAc)₄·2H₂O provided 1·H₂O in good yield. Follow-up reaction of 1·H₂O with Et₄NOH in air replaces μ-O₂CMe (acetato) bridge by MeOCO₂⁻ (monomethyl carbonato) linker in 2·H₂O. Single crystal X-ray structure established the individual complexes and confirmed the fixation of atmospheric CO₂. Variable temperature (2 to 300 K) magnetic susceptibility measurements recognized the antiferromagnetic exchange interactions between the adjacent copper(II) centers in complexes 2 and 3. The amount of spin–spin interactions are found to be higher for ancillary NO₃⁻ bridge (−284 cm⁻¹) compared to the in situ transformed MeOCO₂⁻ bridged (−1.64 cm⁻¹).

求助全文

通过发布文献求助，成功后即可免费获取论文全文。去求助

来源期刊

Inorganica Chimica Acta 化学-无机化学与核化学

CiteScore

6.00

自引率

3.60%

发文量

440

审稿时长

35 days

期刊介绍： Inorganica Chimica Acta is an established international forum for all aspects of advanced Inorganic Chemistry. Original papers of high scientific level and interest are published in the form of Articles and Reviews. Topics covered include: • chemistry of the main group elements and the d- and f-block metals, including the synthesis, characterization and reactivity of coordination, organometallic, biomimetic, supramolecular coordination compounds, including associated computational studies; • synthesis, physico-chemical properties, applications of molecule-based nano-scaled clusters and nanomaterials designed using the principles of coordination chemistry, as well as coordination polymers (CPs), metal-organic frameworks (MOFs), metal-organic polyhedra (MPOs); • reaction mechanisms and physico-chemical investigations computational studies of metalloenzymes and their models; • applications of inorganic compounds, metallodrugs and molecule-based materials. Papers composed primarily of structural reports will typically not be considered for publication.