A Radically Configurable Six-State Compound

被引:141
作者
Barnes, Jonathan C. [1 ,5 ,6 ]
Fahrenbach, Albert C. [1 ,5 ,6 ]
Cao, Dennis [1 ,5 ,6 ]
Dyar, Scott M. [1 ]
Frasconi, Marco [1 ]
Giesener, Marc A. [1 ]
Benitez, Diego [4 ]
Tkatchouk, Ekaterina [4 ]
Chernyashevskyy, Oleksandr [3 ]
Shin, Weon Ho [5 ,6 ]
Li, Hao [1 ]
Sampath, Srinivasan [1 ,5 ,6 ]
Stern, Charlotte L. [1 ]
Sarjeant, Amy A. [1 ]
Hartlieb, Karel J. [1 ]
Liu, Zhichang [1 ]
Carmieli, Raanan [1 ]
Botros, Youssry Y. [1 ,2 ,7 ,8 ]
Choi, Jang Wook [5 ,6 ]
Slawin, Alexandra M. Z. [9 ]
Ketterson, John B. [3 ]
Wasielewski, Michael R. [1 ]
Goddard, William A., III [4 ,5 ,6 ]
Stoddart, J. Fraser [1 ,5 ,6 ]
机构
[1] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA
[2] Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA
[3] Northwestern Univ, Dept Phys, Evanston, IL 60208 USA
[4] CALTECH, Mat & Proc Simulat Ctr, Pasadena, CA 91125 USA
[5] Korea Adv Inst Sci & Technol, NanoCentury KAIST Inst, Taejon 305701, South Korea
[6] Korea Adv Inst Sci & Technol, Grad Sch EEWS WCU, Taejon 305701, South Korea
[7] Intel Labs, Santa Clara, CA 95054 USA
[8] King Abdulaziz City Sci & Technol, Natl Ctr Nano Technol Res, Riyadh 11442, Saudi Arabia
[9] Univ St Andrews, EaStCHEM Sch Chem, St Andrews KY16 9ST, Fife, Scotland
基金
美国国家科学基金会; 英国工程与自然科学研究理事会;
关键词
OXIDATION-REDUCTION; MOLECULAR MATERIALS; ELECTRON-TRANSFER; BUILDING-BLOCKS; REDOX CENTERS; METHYLVIOLOGEN; VIOLOGEN; CATION; INCLUSION; NITROXIDE;
D O I
10.1126/science.1228429
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Most organic radicals possess short lifetimes and quickly undergo dimerization or oxidation. Here, we report on the synthesis by radical templation of a class of air- and water-stable organic radicals, trapped within a homo[2]catenane composed of two rigid and fixed cyclobis (paraquat-p-phenylene) rings. The highly energetic octacationic homo[2] catenane, which is capable of accepting up to eight electrons, can be configured reversibly, both chemically and electrochemically, between each one of six experimentally accessible redox states (0, 2+, 4+, 6+, 7+, and 8+) from within the total of nine states evaluated by quantum mechanical methods. All six of the observable redox states have been identified by electrochemical techniques, three (4+, 6+, and 7+) have been characterized by x-ray crystallography, four (4+, 6+, 7+, and 8+) by electron paramagnetic resonance spectroscopy, one (7+) by superconducting quantum interference device magnetometry, and one (8+) by nuclear magnetic resonance spectroscopy.
引用
收藏
页码:429 / 433
页数:5
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