Article
Chemistry, Multidisciplinary
Zhen Luo, Xinhai Zhang, Jun Zhao, Ruixue Bai, Chunyu Wang, Yuanhao Wang, Dong Zhao, Xuzhou Yan
Summary: Mechanical bonds have been used to construct mechanically interlocked aerogels (MIAs) with adaptivity and multifunctionality. However, fabricating MIAs with precise chemical structures and dynamic features is still challenging. In this study, we present MIAs carrying dense [2]rotaxane units, which provide stability and flexibility to the aerogel network. The chemical structure of [2]rotaxane allows for the fabrication of precise and full-scale mechanically interlocked networks using diverse solvents. Furthermore, the dynamic nature of [2]rotaxane allows for modulation of the morphologies and mechanical performances of MIAs under chemical stimuli. We hope that understanding the structure-property relationship in MIAs will contribute to the development of mechanically interlocked materials and provide new opportunities for constructing smart materials with multifunctionalities.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Inorganic & Nuclear
Weibin Yu, Feng-Yi Qiu, Shi-Ting Luo, Hua-Tian Shi, Guozan Yuan, Xianwen Wei
Summary: Researchers have successfully constructed a triply interlocked [2]catenane with confirmed solid-state structure and solution properties, showing potential applications in drug delivery systems.
INORGANIC CHEMISTRY FRONTIERS
(2021)
Article
Chemistry, Multidisciplinary
Ying-Ying Zhang, Feng-Yi Qiu, Hua-Tian Shi, Weibin Yu
Summary: By tuning the widths of organometallic dinuclear building blocks, two fascinating triply interlocked catenanes and one simple triangular prism metallacage were constructed. Interestingly, the interlocked architectures were disassembled in the presence of large aromatic molecules to form their corresponding monomeric host-guest complexes.
CHEMICAL COMMUNICATIONS
(2021)
Article
Chemistry, Organic
Jiang-Xiong Yang, Ze Li, Xu-Hai Gu, Tian-Guang Zhan, Jiecheng Cui, Kang-Da Zhang
Summary: In this study, a photoswitchable [2]rotaxane with unique photogated macrocyclic shuttling was constructed, enabling control over the shuttling movement through photoisomerization and cycloaddition reactions. This provides a new approach to improve the switching controllability of rotaxane, beneficial for fabricating high-performance rotaxane-based nanosystems and materials.
Article
Materials Science, Multidisciplinary
Jingxi Zheng, Ziteng Yang, Yutong Sang, Fengrunze Zhang, Yixi Zhang, Peng Zhang
Summary: This study proposes a simple and efficient method to prepare rotaxane cross-linker (RC) using gamma-Cyclodextrin (gamma-CD), which requires only one-step chemical reaction. Comparing the swelling ratios and deformation properties of hydrogels prepared by RC and traditional cross-linker, it is shown that hydrogels prepared by RC exhibit better performance. Additionally, the effects of mineralization degrees and cross-linker content on the properties of hydrogels are investigated.
MATERIALS TODAY COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Yu-Ping Tang, Yi-Er Luo, Jun-Feng Xiang, Yan-Mei He, Qing-Hua Fan
Summary: A novel pH-responsive molecular shuttle based on a [2]rotaxane with a phosphine ligand has been designed and synthesized, enabling substrate-selective hydrogenation with high ON/OFF ratios. Mechanistic studies revealed that Rh-III-hydride species are formed in a H-2 atmosphere when the catalyst is in the OFF state, leading to heterolytic activation of dihydrogen and subsequent homolytic splitting to achieve substrate selectivity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Review
Chemistry, Multidisciplinary
Liya Chen, Xinru Sheng, Guangfeng Li, Feihe Huang
Summary: Mechanically interlocked polymers (MIPs) are a type of polymeric material with mechanically interlocked structures, known for their unique properties and potential applications in emerging fields.
CHEMICAL SOCIETY REVIEWS
(2022)
Article
Chemistry, Multidisciplinary
Lei-Min Zhao, Li-Shuo Zheng, Xiaoping Wang, Wei Jiang
Summary: This study reports a molecular shuttle based on a rotaxane, which is influenced by an acid-responsive asymmetric macrocycle. Upon protonation induced by trifluoroacetic acid (TFA), the macrocycle translocates and the shuttling kinetics are hindered by steric hindrance. The shuttling kinetics depend on the concentration of TFA and a kinetic intermediate can be captured.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Materials Science, Multidisciplinary
Zewen Zhu, Sara West, Hengxi Chen, Guan-Hui Lai, Shuntaro Uenuma, Kohzo Ito, Masaya Kotaki, Hung-Jue Sue
Summary: A mechanically interlocked vitrimer (MIV) based on a benzoxazine monomer and polyrotaxane has been developed through dynamic covalent bond chemistry. The MIV exhibited enhanced mechanical performance, including ductility and tensile strength, while maintaining high Young's modulus and glass transition temperature. Reprocessing the MIV did not compromise its mechanical performance and thermal stability. This study demonstrates the potential of high-performance eco-friendly thermosetting vitrimers.
ACS APPLIED POLYMER MATERIALS
(2023)
Article
Chemistry, Organic
Dagninet Yeshiwas Alene, Venkatesan Srinivasadesikan, Ming-Chang Lin, Wen-Sheng Chung
Summary: In this study, a multistimuli responsive [2]rotaxane system was designed, synthesized, and analyzed for its optical behaviors. The system was constructed through noncovalent interactions between diarylethene-based axle and tetraphenylethene-based macrocycle. The shuttling behavior of the macrocycle between different stations and the switching between open-form rotaxanes were achieved using acid-base stimuli. The rotaxane systems exhibited enhanced blue fluorescence in their aggregation states and showed excellent photochromic and fluorescent properties, making them suitable for various applications.
JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Rosemary J. Goodwin, Andrew Docker, Hugo MacDermott-Opeskin, Heather M. Aitken, Megan L. O'Mara, Paul D. Beer, Nicholas G. White
Summary: This article describes the synthesis of two [2]rotaxanes containing interlocked three-dimensional binding cavities, with one receptor showing a higher selectivity preference for chloride ions. X-ray crystal structures showed the encapsulation of chloride ions within the binding cavity, with computational simulations indicating secondary intermolecular interactions.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Ayan Dhara, Anton Dmitrienko, Rahaf N. N. Hussein, Ariel Sotomayor, Benjamin H. H. Wilson, Stephen J. J. Loeb
Summary: A rigid H-shaped [2]rotaxane molecular shuttle was synthesized, which consists of an axle containing benzimidazole recognition sites and a central bipyridyl group interlocked with a 24-crown-8 wheel. The central bipy unit acts as a speed bump that raises the barrier to shuttling for the [2]rotaxane. Coordination of a PtCl2 moiety to the bipy unit creates a steric barrier to shuttling, while addition of Zn(II) ions allows shuttling to occur through a ligand exchange mechanism.
Article
Chemistry, Multidisciplinary
Jamie T. T. Wilmore, Yuen Cheong Tse, Andrew Docker, Caspar Whitehead, Charlotte K. K. Williams, Paul D. D. Beer
Summary: A series of dynamic metalloporphyrin [2]rotaxane molecular shuttles were synthesized with high yield using active metal template synthetic methodology. The dynamic macrocycle translocation is controlled by an inter-component co-ordination interaction between the macrocycle pyridyl and axle Zn(II) metalloporphyrin. The shuttling behavior can be inhibited by a neutral Lewis base, but can be tuned through rotaxane demetallation or subsequent metallation.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Biochemical Research Methods
Peiqiao Wu, Bhushan Dharmadhikari, Prabir Patra, Xingguo Xiong
Summary: In this study, molecular simulation was performed to investigate the switching mechanism of [2]rotaxane molecules. The results show that the solvent environment plays an important role in the switching characteristics of [2]rotaxane molecules. The switching behavior of [2]rotaxane is stable, controllable, reversible, and repeatable, indicating the potential for molecular memory and logic applications.
JOURNAL OF MOLECULAR GRAPHICS & MODELLING
(2022)
Article
Chemistry, Organic
Jesus de Maria Perez, Julio Puigcerver, Tainara Orlando, Aurelia Pastor, Marcos A. P. Martins, Mateo Alajarin, Alberto Martinez-Cuezva, Jose Berna
Summary: In this study, a series of succinamide-based hydrogen-bonded [2]rotaxanes with acyclic secondary amine as the catalytically active sites were synthesized and evaluated for their catalytic activity in an iminium-type process. The presence of an interlocked polyamide macrocycle notably increased the catalytic efficiency of the entwined organocatalysts by rapidly forming a reactive iminium intermediate with the aldehyde. The hydrogen-bonding interaction between the macrocycle and the electrophile plays a crucial role in the rapid formation and stabilization of the key intermediate.
ORGANIC CHEMISTRY FRONTIERS
(2021)
Review
Chemistry, Multidisciplinary
Dan He, Yawen Li, Fuwen Zhao, Yuze Lin
Summary: High trap density in organic solar cells leads to localized charge carriers and reduced carrier lifetime, limiting device efficiency. This feature article summarizes the recent advances of trap suppression by material design and device engineering.
CHEMICAL COMMUNICATIONS
(2024)
Review
Chemistry, Multidisciplinary
Olivier Monfort, Arshitha Madhusudhan, Martin Motola
Summary: This article presents the advantages of coupling photocatalysis and Fenton-based processes for environmental remediation and discusses their synergy. It critically examines the simultaneous triggering of these two processes and provides insights into research approaches. The study aims to enhance understanding of this complex process and highlight the potential integration of new catalysts in current wastewater treatment technology.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Manideepa Dhar, Chittaranjan Mishra, Avijit Das, Uttam Manna
Summary: An approach of 'polymerization of monomers in its aggregated form' has been introduced to tailor the water wettability of fibrous and porous substrates, achieving hydrophobicity to superhydrophobicity transition, as well as patterned wettability. This facile chemical method provides a durable coating with adjustable and patterned wettability for various potential applications.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Saswat Ranjan Bhoi, Chhanda Debnath, Shikha Gandhi
Summary: In this article, a novel catalytic reaction using Pd(0) and Bronsted acid is reported for the synthesis of biologically important imidazolidinone-fused N-heterocycles through redox-neutral intramolecular N-allylation of indoles and pyrroles with alkynes. This atom-economical method is applicable to a wide range of substrates and eliminates the need for leaving groups or oxidizing agents commonly used in traditional allylation reactions.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Longkun Chen, Mingshuai Zhang, Meichen Liu, Zhuoyuan Liu, Yuetong Qiu, Zhilai Zhang, Fuchao Yu, Jiuzhong Huang
Summary: In this study, an efficient Rh(III)-catalyzed selective mono- and dual-C-H bond functionalization/cyclization with iodonium ylide as the sole coupling partner was demonstrated. Fused benzodiazepine skeletons were obtained in excellent yields, providing an improved approach to dual C-H unsymmetrical functionalization.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Alice Kennett, Sven Epple, Gabriella van der Valk, Irene Georgiou, Evelyne Gout, Romain R. Vives, Angela J. Russell
Summary: This study presents the design and synthesis of sulfated disaccharide inhibitors based on IdoA(2S)-GlcNS(6S), which showed potent inhibition of Sulf-2. The results suggest that IdoA(2S)-GlcNS(6S) is the shortest fragment size required for effective inhibition of Sulfs, and a trisulfated disaccharide is identified as the minimal fragment size of heparan sulfate for effective endosulfatase inhibition.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Mauro Garbini, Andrea Brunetti, Riccardo Pedrazzani, Magda Monari, Massimo Marcaccio, Giulio Bertuzzi, Marco Bandini
Summary: The self-adaptability of galvanostatic electrolysis was found to be helpful in a multistage chemo- and diastereoselective electrochemically promoted cyclodimerization of chalcones. Through a series of reductive events, densely functionalized cyclopentanes with five contiguous stereocenters were obtained (25 examples, yields up to 95%, dr values up to >20:1). Further experimental and electrochemical investigations indicated the crucial role of dynamic kinetic resolution of the aldol intermediate in the reaction mechanism.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Dhananjay S. Nipate, Neha Meena, Prakash N. Swami, Krishnan Rangan, Anil Kumar
Summary: In this study, the synthesis of functionalized benzo[a]phenazines and indazolo[2,3-a]quinolines was achieved through Rh(III)-catalyzed oxidative annulation of 2-arylquinoxalines and 2-aryl-2H-indazoles with allyl alcohols. The method showed a wide substrate scope, excellent functional group tolerance, good to high yields of annulated products, and the capability for scaled-up synthesis. A tentative mechanism of the annulation reaction was proposed based on a preliminary mechanistic investigation.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Ruonan Zhang, Abudukadi Tudi, Xia Yang, Xuping Wang, Zhihua Yang, Shujuan Han, Shilie Pan
Summary: A new lead tellurium borate material with a unique fundamental building block [B4O10] was synthesized and found to exhibit high birefringence. The structure-property relationship was discussed using first-principles calculations.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Amresh Kumar Singh, Baishali Thakurta, Anupam Giri, Monalisa Pal
Summary: This study introduces three key concepts for the quick synthesis of large-scale high-quality 2D materials films and their utilization in device fabrication.
CHEMICAL COMMUNICATIONS
(2024)
Article
Chemistry, Multidisciplinary
Reina Hagiwara, Shun Nishimura, Kosuke Okeyoshi
Summary: A copolymer-conjugated nanocatalytic system has been developed to improve electron transfer and enhance photoinduced H2 generation.
CHEMICAL COMMUNICATIONS
(2024)