Relative Unidirectional Translation in an Artificial Molecular Assembly Fueled by Light

被引：108

作者：

Li, Hao ^{[1
]}

Cheng, Chuyang ^{[1
]}

McGonigal, Paul R. ^{[1
]}

Fahrenbach, Albert C. ^{[1
,4
]}

Frasconi, Marco ^{[1
]}

Liu, Wei-Guang ^{[5
]}

Zhu, Zhixue ^{[1
]}

Zhao, Yanli ^{[6
,7
]}

Ke, Chenfeng ^{[1
]}

Lei, Juying ^{[1
]}

Young, Ryan M. ^{[1
,2
]}

Dyar, Scott M. ^{[1
]}

Co, Dick T. ^{[1
,2
]}

Yang, Ying-Wei ^{[1
,4
]}

Botros, Youssry Y. ^{[1
,3
,8
,9
]}

Goddard, William A., III ^{[5
,10
,11
]}

Wasielewski, Michael R. ^{[1
,2
]}

Astumian, R. Dean ^{[12
]}

Stoddart, J. Fraser ^{[1
]}

机构：

[1] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA

[2] Northwestern Univ, Argonne Northwestern Solar Energy Res Ctr, Evanston, IL 60208 USA

[3] Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA

[4] Jilin Univ, State Key Lab Supramol Struct & Mat, Coll Chem, Changchun 130012, Peoples R China

[5] CALTECH, Mat & Proc Simulat Ctr, Pasadena, CA 91125 USA

[6] Nanyang Technol Univ, Sch Phys & Math Sci, Div Chem & Biol Chem, Singapore 637371, Singapore

[7] Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore

[8] King Abdulaziz City Sci & Technol, Natl Ctr Nano Technol Res, Riyadh 11442, Saudi Arabia

[9] Intel Labs, Santa Clara, CA 95054 USA

[10] Korea Adv Inst Sci & Technol, NanoCentury KAIST Inst, Taejon 305701, South Korea

[11] Korea Adv Inst Sci & Technol, Grad Sch EEWS WCU, Taejon 305701, South Korea

[12] Univ Maine, Dept Phys, Orono, ME 04469 USA

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2013年 / 135卷 / 49期

基金：

美国国家科学基金会;

关键词：

DRIVEN TRANSPORT; ROTARY MOTOR; MOTION; DIRECTION; PROTEINS; SWITCHES; TRANSIT; PHYSICS; AXLE; WALK;

D O I：

10.1021/ja4094204

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Motor molecules present in nature convert energy inputs, such as a chemical fuel or incident photons of light, into directed motion and force biochemical systems away from thermal equilibrium. The ability not only to control relative movements of components in molecules but also to drive their components preferentially in one direction relative to each other using versatile stimuli is one of the keys to future technological applications. Herein, we describe a wholly synthetic small-molecule system that, under the influence of chemical reagents, electrical potential, or visible light, undergoes unidirectional relative translational motion. Altering the redox state of a cyclobis(paraquat-p-phenylene) ring simultaneously (i) inverts the relative heights of kinetic barriers presented by the two termini-one a neutral 2-isopropylphenyl group and the other a positively charged 3,5-dimethylpyridinium unit-of a constitutionally asymmetric dumbbell, which can impair the threading/dethreading of a [2]pseudorotaxane, and (ii) controls the ring's affinity for a 1,5-dioxynaphthalene binding site located in the dumbbell's central core. The formation and subsequent dissociation of the [2]pseudorotaxane by passage of the ring over the neutral and positively charged termini of the dumbbell component in one, and only one, direction relatively defined has been demonstrated by (i) spectroscopic (H-1 NMR and UV/vis) means and cyclic voltammetry as well as with (ii) DFT calculations and by (iii) comparison with control compounds in the shape of constitutionally symmetrical [2]pseudorotaxanes, one with two positively charged ends and the other with two neutral ends. The operation of the system relies solely on reversible, yet stable, noncovalent bonding interactions. Moreover, in the presence of a photosensitizer, visible-light energy is the only fuel source that is needed to drive the unidirectional molecular translation, making it feasible to repeat the operation numerous times. without the buildup of byproducts.

引用

页码：18609 / 18620

页数：12

共 74 条

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