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Beyond Single-Cycle Autonomous Molecular Machines: Light-Powered Shuttling in a Multi-Cycle Reaction Network.
Yang, Zhiyao; Wang, Xirui; Penocchio, Emanuele; Ragazzon, Giulio; Chen, Xinnan; Lu, Shuai; Zhou, Yidan; Fu, Kuirong; Liu, Zejiang; Cai, Yimin; Yu, Xiujun; Li, Xiaopeng; Li, Xiaowei; Feng, Wen; Yuan, Lihua.
Afiliación
  • Yang Z; College of Chemistry, Key Laboratory of Radiation Physics and Technology of Ministry of Education, Sichuan University, Chengdu, Sichuan 610064, China.
  • Wang X; College of Chemistry, Key Laboratory of Radiation Physics and Technology of Ministry of Education, Sichuan University, Chengdu, Sichuan 610064, China.
  • Penocchio E; Department of Chemistry, Northwestern University, Evanston, IL 60208, USA.
  • Ragazzon G; Institut de Science et d'Ingénierie Supramoléculaires (ISIS), CNRS UMR 7006, University of Strasbourg, 67000, Strasbourg, France.
  • Chen X; College of Chemistry, Key Laboratory of Radiation Physics and Technology of Ministry of Education, Sichuan University, Chengdu, Sichuan 610064, China.
  • Lu S; College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, Guangdong 518060, China.
  • Zhou Y; College of Chemistry, Key Laboratory of Radiation Physics and Technology of Ministry of Education, Sichuan University, Chengdu, Sichuan 610064, China.
  • Fu K; College of Chemistry, Key Laboratory of Radiation Physics and Technology of Ministry of Education, Sichuan University, Chengdu, Sichuan 610064, China.
  • Liu Z; College of Chemistry, Key Laboratory of Radiation Physics and Technology of Ministry of Education, Sichuan University, Chengdu, Sichuan 610064, China.
  • Cai Y; College of Chemistry, Key Laboratory of Radiation Physics and Technology of Ministry of Education, Sichuan University, Chengdu, Sichuan 610064, China.
  • Yu X; College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, Guangdong 518060, China.
  • Li X; College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen, Guangdong 518060, China.
  • Li X; College of Chemistry, Key Laboratory of Radiation Physics and Technology of Ministry of Education, Sichuan University, Chengdu, Sichuan 610064, China.
  • Feng W; College of Chemistry, Key Laboratory of Radiation Physics and Technology of Ministry of Education, Sichuan University, Chengdu, Sichuan 610064, China.
  • Yuan L; College of Chemistry, Key Laboratory of Radiation Physics and Technology of Ministry of Education, Sichuan University, Chengdu, Sichuan 610064, China.
Angew Chem Int Ed Engl ; : e202414072, 2024 Aug 16.
Article en En | MEDLINE | ID: mdl-39152651
ABSTRACT
Biomolecular machines autonomously convert energy into functions, driving systems away from thermodynamic equilibrium. This energy conversion is achieved by leveraging complex, kinetically asymmetric chemical reaction networks that are challenging to characterize precisely. In contrast, all known synthetic molecular systems in which kinetic asymmetry has been quantified are well described by simple single-cycle networks. Here, we report on a unique light-driven [2]rotaxane that enables the autonomous operation of a synthetic molecular machine with a multi-cycle chemical reaction network. Unlike all prior systems, the present one exploits a photoactive macrocycle, which features a different photoreactivity depending on the binding sites at which it resides. Furthermore, E to Z isomerization reverses the relative affinity of the macrocycle for two binding sites on the axle, resulting in a multi-cycle network. Building on the most recent theoretical advancements, this work quantifies kinetic asymmetry in a multi-cycle network for the first time. Our findings represent the simplest rotaxane capable of autonomous shuttling developed so far and offer a general strategy to generate and quantify kinetic asymmetry beyond single-cycle systems.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Alemania
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
Buscar en Google

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Alemania