量子化学计算研究自由基相互作用的双稳态轮烷的穿梭机理*

doi:10.7523/j.ucas.2022.055

中国科学院大学学报

量子化学计算研究自由基相互作用的双稳态轮烷的穿梭机理^*

王涛, 李晓毅^†

中国科学院大学材料科学与光电技术学院材料科学与光电技术中心,北京 100049

收稿日期:2022-04-14 修回日期:2022-05-10 发布日期:2022-05-12
通讯作者: † E-mail:lixy@ucas.ac.cn
基金资助:
* 国家自然科学基金（21274164）资助

Study on shuttling mechanism the bistable rotaxane based on the radical interaction by quantum chemical calculations

WANG Tao, LI Xiaoyi

Center of Materials Science and Optoelectronics Engineering, College of Materials Science and Opto-Electronic Technology,University of Chinese Academy of Sciences,Beijing 100049,China

Received:2022-04-14 Revised:2022-05-10 Published:2022-05-12

摘要/Abstract

摘要： 我们设计了一种氧化还原驱动的可切换的双稳态轮烷。以双百草枯-对苯双自由基双阳离子环 (CBPQT^2(●+)) 作为大环分子,主链分子上有两个结合位点,即4,4'-联吡啶自由基阳离子BIPY^●+和2,6-二氧亚萘基(DOP)位点。运用密度泛函理论对大环分子在主链分子上的运动机理进行了研究,并通过量子力学理论计算分析了大环分子CBPQT^2(●+)与主链分子上两个结合位点BIPY^●+ 和DOP之间的弱相互作用,证明了氧化还原反应控制自由基络合物的形成和解离可以驱动CBPQT^2(●+)环沿着主链分子的两个结合位点间实现往复运动。

关键词: 分子梭, 双稳态轮烷, 量子力学计算, 自由基相互作用

Abstract: We designed a switchable bistable rotaxane consisted of the cyclobis (paraquat-p-phenylene) bisradical dicationic (CBPQT^2(●+)) ring and a main chain, concluding the recognition sites 4,4′-bipyridinium radical cationic (BIPY^●+ ) and 2,6-dioxynaphthalen(DOP). The density functional theory (DFT) is used to analyze the motion mechanism of ring along the main chain A. Quantum Mechanics calculations are used to analyze the noncovalent interaction between the CBPQT^2(●+) ring and the two recognition sites. It proves that the generation and dissociation of the trisradical tricationic complex controlled by the redox reaction could drive the reciprocating motion of the CBPQT^2(●+) ring along the main chain between the two recognition sites.

Key words: molecular shuttle, bistable rotaxane, Quantum Mechanics Calculation, radical interaction

中图分类号:

O642

王涛, 李晓毅. 量子化学计算研究自由基相互作用的双稳态轮烷的穿梭机理^*[J]. 中国科学院大学学报, DOI: 10.7523/j.ucas.2022.055.

WANG Tao, LI Xiaoyi. Study on shuttling mechanism the bistable rotaxane based on the radical interaction by quantum chemical calculations[J]. Journal of University of Chinese Academy of Sciences, DOI: 10.7523/j.ucas.2022.055.

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量子化学计算研究自由基相互作用的双稳态轮烷的穿梭机理^*

Study on shuttling mechanism the bistable rotaxane based on the radical interaction by quantum chemical calculations

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