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
Polymer Science
Hao Guo, Kun Qian, Mesfin Tsige
Summary: This study investigates the conformational properties of [2]catenane polymers in solution, revealing their dependence on solvent quality and molecular weight. The findings show that [2]catenane polymers have a lower theta-temperature compared to linear and ring counterparts, and their conformation significantly deviates from an analogous ring polymer in a poor solvent condition.
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)
Review
Chemistry, Organic
Milo D. Cornelissen, Simone Pilon, Jan H. van Maarseveen
Summary: Mechanically interlocked molecules, such as catenanes and rotaxanes, exhibit unique properties and have potential applications as artificial molecular machines and drug discovery targets. Covalent and non-covalent strategies each have their own advantages and limitations, but combining them may lead to new research opportunities.
SYNTHESIS-STUTTGART
(2021)
Article
Chemistry, Multidisciplinary
Kenji Caprice, David Pal, Celine Besnard, Bartomeu Galmes, Antonio Frontera, Fabien B. L. Cougnon
Summary: This study demonstrates the amplification of a mechanically chiral (P)-catenane by binding to (R)-1,1'-binaphthyl 2,2'-disulfonate, with a diastereomeric excess of 85%. The chirality of the [2]catenane was confirmed by single crystal X-ray diffraction and NMR/CD spectroscopies, establishing a basis for the development of new synthetic approaches to enantioenriched mechanically chiral [2]catenanes.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
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
Eoin P. McCarney, June I. Lovitt, Thorfinnur Gunnlaugsson
Summary: This study reports the efficient self-templated formation of optically active btp homocircuit [2]catenane enantiomers through X-ray diffraction crystallography for structural characterization. The self-assembly reaction was closely monitored in solution, facilitating the characterization of the pseudo-rotaxane reaction intermediate prior to mechanically interlocking the pre-organised system via ring-closing metathesis.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Organic
Richard C. Knighton, Paul D. Beer
Summary: A novel method was used to construct a mechanically interlocked ion-pair binding [2]catenane, with the heteroditopic binding mode elucidated by single-crystal X-ray crystallography, revealing an unprecedented 'macrocycle separated' ion-pair configuration with alkali-metal sodium cation.
ORGANIC CHEMISTRY FRONTIERS
(2021)
Article
Chemistry, Organic
Shinya Tajima, Atsuya Muranaka, Masaya Naito, Noriho Taniguch, Mei Harada, Shinobu Miyagawa, Masahiro Ueda, Hikaru Takaya, Nagao Kobayashi, Masanobu Uchiyama, Yuji Tokunaga
Summary: In this study, a [2]rotaxane with both mechanically planar chiral and axially chiral properties was synthesized, consisting of a symmetrical biscrown ether with a biphenyl moiety as the macrocyclic component and a symmetrical bis-ammonium salt as the dumbbell-shaped component.
Article
Multidisciplinary Sciences
Xue Yang, Lin Cheng, Zhaoming Zhang, Jun Zhao, Ruixue Bai, Zhewen Guo, Wei Yu, Xuzhou Yan
Summary: This study presents mechanically interlocked networks with densely rotaxanated backbones as a model system to understand the integration and amplification of molecular-level motion in macroscopic mechanical properties. The motion of mechanical bonds leads to the expansion of the network, imparting stretchability and puncture resistance to the materials. Similarly, the dissociation and sliding motion contribute to the toughness and damping capacity of the materials. This research provides insights into the relationship between microscopic motion and macroscopic mechanical performance.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Ata Utku Ozkan, Donus Tuncel, Aykut Erbas
Summary: Rotaxanes can exhibit stimuli-responsive behavior by allowing positional fluctuations of their rota groups in response to physiochemical conditions such as the changes in solution pH. However, ionic strength of the solution also affects the molecular conformation by altering the charge state of the entire molecule, coupling the stimuli-responsiveness of rotaxanes with their conformation.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Chemistry, Multidisciplinary
Jun-Tao Shi, Xian-Hui Chen, Yuan-Yuan Peng, Gui-Ping Wang, Guang-Yan Du, Quan Li
Summary: In this study, a novel mechanically bonded amphiphile was designed and synthesized. It showed pH-responsive emissions in both solution and aggregated states, and the morphology of the aggregates could be controlled by adjusting the pH value. This research has potential implications for the development of smart materials with unique functions.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Simone Pilon, Steen Ingemann Jorgensen, Jan H. van Maarseveen
Summary: Despite advances in synthesizing mechanically interlocked molecules, a universally applicable approach for interlocked natural products like lasso peptides has not yet been established. By using an ester-functionalized, aromatic delta-amino acid as a central template unit, researchers successfully synthesized both a [2]catenane and a [2]rotaxane, representing a significant step towards future synthetic peptide-based interlocked products.
Article
Chemistry, Multidisciplinary
Rebecca L. L. Spicer, Curtis C. C. Shearman, Nicholas H. H. Evans
Summary: This study presents the synthesis of two mechanically chiral rotaxanes with urea and squaramide motifs, with yields of 33% and 22% respectively. H-1 NMR spectroscopic titrations reveal the possibility of shuttling the macrocycle, detectable through modulation of mechanical chirality expression in the NMR spectrum, by the addition of achiral chloride anions, which can be reversed by the addition of sodium cations.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Organic
Manisha Prakashni, Rasendra Shukla, Suvankar Dasgupta
Summary: A facile, rapid, and high yield synthesis of [23]crown ether (X23C7) has been developed from commercially available starting materials in one step with good to excellent yield. The X23C7 macrocycle formed strong association with a dibenzylammonium ion (DBA(+)), leading to the synthesis of a high yield [2]catenane using a threading-followed-ring-closing-metathesis approach. The reaction was completed in 6 hours under room temperature conditions, with the highest yield reaching 81%.
JOURNAL OF ORGANIC CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Jun Zhao, Zhaoming Zhang, Lin Cheng, Ruixue Bai, Dong Zhao, Yongming Wang, Wei Yu, Xuzhou Yan
Summary: Mechanically interlocked vitrimers (MIVs) are a new class of MINs that combine vitrimer chemistry with mechanically interlocked structures to address challenges. Experimental results demonstrate that MIVs exhibit improved mechanical performance, including Young's modulus, toughness, and damping capacity.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Polymer Science
Ruixue Bai, Hao Zhang, Xue Yang, Jun Zhao, Yongming Wang, Zhaoming Zhang, Xuzhou Yan
Summary: Supramolecular polymer networks based on host-guest recognition play a crucial role in the development of smart supramolecular materials. This study focuses on the rarely explored bulk SPNs and demonstrates their tough characteristics, dynamic behaviors, and responsiveness to pH. The host-guest recognition acts as a sacrificial bond, enabling notable strength, ductility, and high toughness. The findings deepen the understanding of bulk SPNs and promote the development of supramolecular materials with emergent functions and applications.
Article
Multidisciplinary Sciences
Zhaoming Zhang, Jun Zhao, Zhewen Guo, Hao Zhang, Hui Pan, Qian Wu, Wei You, Wei Yu, Xuzhou Yan
Summary: This study presents mechanically interlocked networks cross-linked by a molecular necklace, which possess unique architectural and dynamic features and endow the materials with robust yet mechanically adaptive properties. Additionally, the materials exhibit abundant active properties, responding to stimuli such as K+ and Br-. These findings demonstrate the untapped potential of molecular necklaces as cross-linkers and open up new possibilities for their advanced applications in intelligent supramolecular materials.
NATURE COMMUNICATIONS
(2022)
Article
Nanoscience & Nanotechnology
Yuchen Guo, Yuhang Liu, Xinyang Zhao, Jun Zhao, Yongming Wang, Xinhai Zhang, Zhewen Guo, Xuzhou Yan
Summary: Network topologies have a significant impact on the properties of polymer materials, but achieving such structures at the macromolecular level remains a challenge. This study presents a platform using synergistic covalent-and-supramolecular polymers to prepare interwoven polymer networks. The resulting networks exhibit mechanically robust yet dynamic properties, as well as stimuli-responsive behavior.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Yuhang Liu, Xuzhou Yan
Summary: This article summarizes and discusses the recent progress and related strategies in constructing woven polymer networks, and provides an outlook on the future opportunities and challenges in the development of both molecularly woven structures and molecularly woven functional materials.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Zhaoming Zhang, Wei You, Peitong Li, Jun Zhao, Zhewen Guo, Tingjie Xu, Jieqi Chen, Wei Yu, Xuzhou Yan
Summary: Mimicking filament sliding in sarcomeres using artificial molecular muscles has sparked interest in developing advanced polymeric materials. By decoupling a bistable [c2]daisy chain into individual extended and contracted ones, the relationship between microscopic motion and macroscopic mechanical properties of mechanically interlocked networks (MINs) is established.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Xue Yang, Lin Cheng, Zhaoming Zhang, Jun Zhao, Ruixue Bai, Zhewen Guo, Wei Yu, Xuzhou Yan
Summary: This study presents mechanically interlocked networks with densely rotaxanated backbones as a model system to understand the integration and amplification of molecular-level motion in macroscopic mechanical properties. The motion of mechanical bonds leads to the expansion of the network, imparting stretchability and puncture resistance to the materials. Similarly, the dissociation and sliding motion contribute to the toughness and damping capacity of the materials. This research provides insights into the relationship between microscopic motion and macroscopic mechanical performance.
NATURE COMMUNICATIONS
(2022)
Article
Polymer Science
Xue Yang, Ruixue Bai, Zhaoming Zhang, Yangang Liu, Xuzhou Yan
Summary: Supramolecular polymer networks (SPNs) have garnered significant research attention for their excellent performance in the preparation of adaptable materials. This study focuses on controlling the distribution of supramolecular interactions within SPNs, which has received limited attention. By constructing two triblock copolymers in ABA and BAB forms, the study demonstrates that the location of supramolecular interactions can significantly influence the mechanical properties of SPNs. These findings deepen our understanding of SPNs and hold promise for the development of supramolecular block copolymers with unique functions and applications.
JOURNAL OF POLYMER SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Yuhang Liu, Junjun Wan, Xinyang Zhao, Jun Zhao, Yuchen Guo, Ruixue Bai, Zhaoming Zhang, Wei Yu, Harry W. Gibson, Xuzhou Yan
Summary: Cryptand/paraquat host-guest recognition motifs as cross-links can be used to prepare highly strong and tough supramolecular polymer networks with enhanced mechanical properties and abundant dynamic properties.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Yuhang Liu, Zhewen Guo, Yuchen Guo, Guangfeng Li, Shengbing Yang, Xuzhou Yan, Yi Shen, Jinbing Wang
Summary: A selective formation of a barrel-shaped or a ball-shaped fluorescent metallacage was achieved by controlling the shape and stoichiometry of the building blocks. The ball-shaped metallacage exhibited stronger and blue-shifted fluorescence compared to the barrel-shaped one in dilute solutions, while a reversal of fluorescence intensities was observed in the aggregation process. This work demonstrates the impact of subtle geometrical factors on the photophysical properties of supramolecular coordination complexes.
CHINESE CHEMICAL LETTERS
(2023)
Article
Multidisciplinary Sciences
Weichen Wang, Yuanwen Jiang, Donglai Zhong, Zhitao Zhang, Snehashis Choudhury, Jian-Cheng Lai, Huaxin Gong, Simiao Niu, Xuzhou Yan, Yu Zheng, Chien -Chung Shih, Rui Ning, Qing Lin, Deling Li, Yun-Hi Kim, Jingwan Kim, Yi-Xuan Wang, Chuanzhen Zhao, Chengyi Xu, Xiaozhou Ji, Yuya Nishio, Hao Lyu, Jeffrey B. -H. Tok, Zhenan Bao
Summary: Through rational design and engineering, we have developed a soft prosthetic electronic skin that mimics the sensory feedback and mechanical properties of natural skin. It is capable of multimodal perception, neuromorphic pulse-train signal generation, and closed-loop actuation. Our e-skin has achieved low subthreshold swing, low operation voltage, low power consumption, and medium-scale circuit integration complexity for stretchable organic devices, thanks to a trilayer, high-permittivity elastomeric dielectric.
Article
Chemistry, Multidisciplinary
Jingxi Deng, Ruixue Bai, Jun Zhao, Guoquan Liu, Zhaoming Zhang, Wei You, Wei Yu, Xuzhou Yan
Summary: Simultaneously introducing covalent and supramolecular cross-links into one system to construct dually cross-linked networks has proven to be an effective approach for preparing high-performance materials. This study investigates the features and advantages of dually cross-linked networks compared to those with individual covalent or supramolecular cross-linking points. The results reveal that the dual cross-linking strategy endows the dually cross-linked polymer network (DPN) with the integrated advantages of covalent polymer networks (CPN) and supramolecular polymer networks (SPN). The DPN exhibits excellent toughness and ductility similar to SPN due to the energy dissipative ability of host-guest complexes, while the covalent cross-links contribute to the structural stability and quick deformation recovery capacity comparable to CPN. Moreover, the DPN demonstrates the strongest breaking stress and puncture resistance, showcasing the unique property advantages of the dual cross-linking method.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
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
Polymer Science
Xintian Xie, Liang Wu, Huai Sun, Xuzhou Yan, Xinyuan Zhu
Summary: In this study, coarse-grained molecular dynamics simulation is used to investigate the thermodynamics and phase behavior of [2]catenane. The mechanical bond in [2]catenane not only destabilizes the packing between molecular rings but also provides additional internal degrees of freedom. The [2]catenane molecule undergoes a conformation transition from free-rolling to cross-stacking with respect to density increase, and exhibits a smectic layering structure with high free volume, showing cubatic ordering due to the interpenetration of macrocycles.
Article
Chemistry, Multidisciplinary
Yongming Wang, Hao Zhang, Zhaoming Zhang, Jun Zhao, Ruixue Bai, Yuhang Liu, Xinhai Zhang, Xuzhou Yan
Summary: In this study, a thermo-responsive macromolecular metamorphosis was achieved by coupling covalent polymers and supramolecular polymers. The researchers successfully transformed brittle materials into tough materials through the topological transformation, demonstrating the potential of supramolecular polymers in designing smart materials.
