Review
Polymer Science
Zhaozhao Duan, Fenfen Xu, Xiaohui Huang, Yongchao Qian, Hui Li, Wei Tian
Summary: Supramolecular polymers, constructed through self-assembly of noncovalent interactions like host-guest interaction, have both the advantages of traditional polymers and unique characteristics. Crown ethers, as a widely used host molecule, can be easily modified and derivatized, making them ideal candidates for the fabrication of interesting supramolecular polymers.
MACROMOLECULAR RAPID COMMUNICATIONS
(2022)
Article
Chemistry, Organic
Jing-yang Wang, Qun-yan Wu, Shuai Wang, Zhi-wei Huang, Kong-qiu Hu, Ji-pan Yu, Lei Mei, Meng Zhang, Zhi-fang Chai, Wei-qun Shi
Summary: Research on synthesizing new coordination-driven polyrotaxanes and regulating their structural diversity contributes to the success of macrocycle-based supramolecular materials. By introducing crown ether macrocycles as a new supramolecular element, a different kind of actinide polyrotaxane with intriguing molecular structures and supramolecular assembly behaviors has been created, expanding the research scope of actinide rotaxane coordination polymers.
ORGANIC CHEMISTRY FRONTIERS
(2021)
Article
Chemistry, Inorganic & Nuclear
Caiyun Liu, Chang Gao, Amir Said, Huihui Niu, Dexin Wang, Chen-Ho Tung, Yifeng Wang
Summary: Catenane, rotaxane, and pseudorotaxane molecules based on a cyclic titanium oxide cluster and cyclic/linear alkylammonium cations were synthesized and shown to remain intact in acidic water, promising for assembling inorganic-organic hybrid supramolecular structures in water.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Maxime Gauthier, Frederic Coutrot
Summary: This study synthesized new pH-sensitive [2]rotaxane molecular shuttles and found that the Weinreb amide was not a suitable secondary molecular station for DB24C8, while the ketone was successfully used for this purpose.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Yoko Sakata, Ryosuke Nakamura, Toshihiro Hibi, Shigehisa Akine
Summary: Switching between formation and dissociation of rotaxanes is important for controlling the function of rotaxane-based materials. We developed a convenient strategy called accelerator addition to make a static rotaxane dynamic without affecting the chemical structure. By complexing [PdL2](2+) (L=2,3-diaminotriptycene) with 27C9, a metallorotaxane was quantitatively generated, allowing for tuning of formation and dissociation speed. Addition of Br- accelerated rotaxane formation by 27 times, while Cs+ accelerated dissociation, forming the free axle [PdL2](2+) and the 27C9-Cs+ complex.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Todd N. Poe, Harry Ramanantoanina, Joseph M. Sperling, Hannah B. Wineinger, Brian M. Rotermund, Jacob Brannon, Zhuanling Bai, Benjamin Scheibe, Nicholas Beck, Brian N. Long, Samantha Justiniano, Thomas E. Albrecht-Schonzart, Cristian Celis-Barros
Summary: A study successfully synthesized a divalent plutonium complex and showed that plutonium can be quantitatively reduced to the divalent state and subsequently re-oxidized in solution to form a mixture of divalent and trivalent complexes.
Article
Chemistry, Multidisciplinary
Rupam Roy, Anup Pramanik, Tanoy Dutta, Vikas Sharma, Kovida, Apurba Lal Koner
Summary: This study elucidates the influence of aliphatic biogenic amines on the transient assembly and disassembly of a pyrene dianhydride-based scaffold, and investigates the interaction and stabilization mechanisms, achieving a smooth transition from cyan emission to light blue emission. Additionally, potential biological significance is found in the selective pyrene-biogenic amine conjugates.
MATERIALS CHEMISTRY FRONTIERS
(2022)
Article
Polymer Science
Katalin Czifrak, Csilla Lakatos, Gabriella Szabo, Bence Vadkerti, Lajos Daroczi, Miklos Zsuga, Sandor Keki
Summary: This study reported the preparation and systematic investigation of cross-linked polyurethane-epoxy (PU-EP) polymer systems. The PU-EP polymers were synthesized by reacting NCO-terminated PU prepolymers with diglycidyl ether of bisphenol A (DGEBA)-amine cooligomers. The addition of furfurylamine (FA) or ethanolamine (EA) resulted in the oligomerization of DGEBA and the formation of DGEBA-amine cooligomers. The cross-linking was achieved by adding the DGEBA-amine cooligomer to the PU prepolymers, forming urethane bonds as netpoints. The presence of furfurylamine allowed for the formation of additional thermoreversible bonds, leading to shape memory behavior in the PU-EP networks.
Article
Chemistry, Multidisciplinary
Conghui Wang, Ying-Ming Zhang, Haoran Li, Jin Zhang, Yu Zhou, Guoxing Liu, Xiufang Xu, Yu Liu
Summary: Conformational regulation is not only a main pathway for achieving multiple tasks in complex biological systems, but also a powerful strategy for obtaining stimuli-responsive supramolecular nanoconstructs with tailored physicochemical performance. This study demonstrates that synergistic conformational modulation through intra- and intermolecular interactions can be developed as a generalizable approach to construct more advanced biomimetic nanomaterials.
CHINESE CHEMICAL LETTERS
(2022)
Editorial Material
Chemistry, Multidisciplinary
Daehyun Ahn, Nowshin Kabir, Thirumurugan Prakasam, Ali Trabolsi
Summary: The development of analytical tools over the past three decades has enabled the study of increasingly complex mechanically inter-locked molecules. The first synthesis of a [2]catenane by Edel Wasserman in 1960 was controversial due to the lack of experimental evidence. Recently, Leigh et al. re-examined this pioneering synthesis using modern techniques, confirming its structure in the Journal of the American Chemical Society.
Article
Chemistry, Inorganic & Nuclear
Naoyuki Hisano, Virginia Valderrey, Gemma Aragay, Pablo Ballester
Summary: We report the self-assembly of a di-nuclear tetralactam macrocyle based on two symmetric components and investigate its binding properties with adipamide derivatives. We observe the formation of a weakly bound 1:1 complex with linear alkyl chains and a preferred binding geometry of [2]pseudorotaxane topology. In the presence of bulky stoppers, two different complexes are formed, with the second complex displaying slow exchange kinetics and a [2]rotaxane topology.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Physical
Hui Ma, Dan Luo, Qi Zhao, Rui Liu, Zhenzhou Zhang, Xianglin Hou, Xiaohuan Sun, Yingxiong Wang
Summary: Diffusion-ordered spectroscopy (DOSY) is an efficient technique for analyzing complex mixtures, but often struggles to separate positional isomers. The use of 18C6 and 18C6/K+ complex as matrices can effectively discriminate and identify positional isomeric mixtures, demonstrating superior performance in interacting with different components.
JOURNAL OF MOLECULAR LIQUIDS
(2022)
Article
Chemistry, Multidisciplinary
Hui-Peng Lv, Yi-Rong Li, Xian-Jiang Song, Nan Zhang, Ren-Gen Xiong, Han-Yue Zhang
Summary: This study reports a supramolecular host-guest ferroelectric compound with a remarkable piezoelectric response, which does not require further poling and provides inspiration for optimizing piezoelectricity on molecular materials.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Engineering, Chemical
Sisheng Fang, Hai Tang, Meng Wang, Zhaozan Xu, Nanwen Li
Summary: Amphiphilic copolymers containing hydrophilic crown ether units were synthesized and used in the preparation of high-performance ultrafiltration membranes. The UF membranes exhibited excellent separation performance and antifouling properties. The morphology and properties of the membranes could be controlled by adjusting the content of the hydrophilic crown ether.
JOURNAL OF MEMBRANE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Hendrik Schroeder, Yi Zhang, A. James Link
Summary: The synthesis strategy of mechanically interlocked peptides (MIPs) solely made from peptides was reported in this study. These MIPs were self-assembled in water, breaking the tradition of MIMs usually being prepared in organic solvents. Detailed NMR spectroscopy and mass spectrometry characterization revealed that MIPs exhibit rich conformational dynamics reminiscent of protein folding.
Article
Biochemistry & Molecular Biology
Saravanan Kandasamy, George F. S. Whitehead, Inigo J. Vitorica-Yrezabal, John M. Gardiner
Summary: 5-O-protected and 1,2-acetonide-protected D-glucurono-6,3-lactone furanosides were converted into novel furano-glucuronamides through treatment with ammonia. Different protection and deprotection routes led to primary gluconamide derivatives, while benzylations led to silyl migration, N-benzylation, or reclosure to lactone. The use of 5-O-PMB protection provided a method for obtaining fully protection-differentiated glucofuranamide. Crystal structures of fully protected glucurono-6,3-lactone lactone and glucuronamide derivatives were reported.
CARBOHYDRATE RESEARCH
(2023)
Article
Chemistry, Multidisciplinary
A. R. Bonity J. Lutton-Gething, Lynda T. Nangkam, Jens O. W. Johansson, Ioanna Pallikara, Jonathan M. Skelton, George F. S. Whitehead, Inigo Vitorica-Yrezabal, Martin P. Attfield
Summary: Controlling the mu(2)-X- bridging anion in Ga-MIL-53 [GaX(bdc)] (X-=(OH)(-) or F-, bdc=1, 4-benzenedicarboxylate) can direct the temperature at which breathing transitions of this framework occur. Substituting (OH)(-) with F- stabilizes the large pore (lp) form and decreases the onset temperature of lp to narrow pore (np) transition. In situ diffraction studies provide a plausible crystal structure and reveal a lower temperature pathway for the transition.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Inorganic & Nuclear
William D. Jobbins, Bono van IJzendoorn, Inigo J. Vitorica-Yrezabal, George F. S. Whitehead, Meera Mehta
Summary: The solution-state molecular chemistry of heptapnictogen clusters has not been well established. We investigated the heteroallene capture ability of heavy element derivatives of tetrel functionalized heptapnictogen clusters towards isocyanates and CO2. The experimental results showed that these clusters could capture isocyanates through their tetrel-pnictogen bonds, with different preferences for coordinating with nitrogen or oxygen atoms. This study also used density functional theory to explore the heteroallene insertion at these clusters.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Multidisciplinary
Martin J. Power, David T. J. Morris, Inigo J. Vitorica-Yrezabal, David A. . Leigh
Summary: Challenges in developing effective new superbases include synthesis ease, chemical stability, high basicity, and minimizing nucleophilicity. In this study, a new family of organic superbases called compact amine-crown ether rotaxanes are introduced, which exhibit desirable characteristics in all these aspects. These rotaxanes are synthesized using metal-free active template synthesis, have high basicity, low nucleophilicity, and show excellent stability and selectivity in reactions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Andrei S. Baluna, Albano Galan, David A. . Leigh, Gareth D. Smith, Justin T. J. Spence, Daniel J. Tetlow, Inigo J. Vitorica-Yrezabal, Min Zhang
Summary: We repeated the earliest claimed catenane synthesis reported by Wasserman over 60 years ago to investigate the formation of mechanically interlocked rings through a nontemplate, statistical synthesis. Using modern synthetic methods, we reconstructed Wasserman's deuterium-labeled macrocycle and other building blocks on a scale necessary to generate approximately 1 mg of catenane. We employed advanced spectroscopic and chemical techniques to detect, isolate, and prove the structure of a putative [2]catenane consisting of a 34-membered cyclic hydrocarbon mechanically linked with a 34-membered cyclic alpha-hydroxyketone.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Zhipeng Zhou, Lei Zhang, Yonghang Yang, Inigo J. Vitorica-Yrezabal, Honglei Wang, Fanglin Tan, Li Gong, Yuyao Li, Pohua Chen, Xin Dong, Zihao Liang, Jing Yang, Chao Wang, Yuexian Hong, Yi Qiu, Armin Goelzhaeuser, Xudong Chen, Haoyuan Qi, Sihai Yang, Wei Liu, Junliang Sun, Zhikun Zheng
Summary: This study reports a strategy that utilizes amphiphilic amino-acid derivatives with long hydrophobic chains to produce single-crystal imine-linked COFs in aqueous solutions under ambient conditions. The self-assembled micelles act as dynamic barriers to separate monomers in aqueous solution and hydrophobic compartments, thereby regulating the polymerization and crystallization processes. Five different three-dimensional COFs and a two-dimensional COF were obtained as single crystals on the gram scale, with yields of 92% and above.
Article
Chemistry, Organic
Fahad Ayesh Alharthi, Garrett T. Potter, Gordon C. Jayson, George F. S. Whitehead, Inigo J. Vitorica-Yrezabal, John M. Gardiner
Summary: Reactions of a glucuronic acid (GlcA) beta-thioglyco-side with cyclohexadione result in the formation of two expected all-trans decalin-type O2,O3 and O3,O4 cyclohexane-1,2-diacetals (CDAs), along with an epimer of the main O2,O3 acetal. This trans-cis isomer is then converted to higher amounts of the two all-trans products. Isomerization studies demonstrate slow interconversion between the all-trans CDA acetals, with only one significant interconversion with the minor 2,3-diastereomer. Crystal structures of all three isomers are included. These findings are important for understanding the occurrence and interconversion of apparently disfavored isomers in other uses of CDA protections.
Article
Chemistry, Multidisciplinary
Lorna Binks, Stefan Borsley, Todd R. Gingrich, David A. Leigh, Emanuele Penocchio, Benjamin M. W. Roberts
Summary: The study found that kinetic asymmetry determines the directionality of the information ratchets, while power strokes influence the performance and energy storage form. These findings have important implications for understanding biological ratchets and designing artificial molecular machines.
Article
Chemistry, Multidisciplinary
Luis Martinez-Crespo, Inigo J. Vitorica-Yrezabal, George F. S. Whitehead, Simon J. Webb
Summary: Relaying conformational change over several nanometers is crucial in allosterically regulated proteins. Scientists have successfully replicated this mechanism using nanometer-sized molecules that can reversibly switch between defined shapes in response to signaling molecules. The study demonstrated that a 1.8 nm long rigid rod molecule can serve as a switchable multi-squaramide hydrogen-bond relay, with each relay adopting different orientations based on proton signals and undergoing reversible changes. Additionally, a chemical fuel acted as a dissipative signal, causing the relay to return to its original orientation when consumed.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Selena J. Lockyer, Deepak Asthana, George F. S. Whitehead, Inigo J. Vitorica-Yrezabal, Grigore. A. Timco, Eric J. L. McInnes, Richard E. P. Winpenny
Summary: A synthetic strategy is used to prepare two distinct trimers of antiferromagnetically coupled {Cr7Ni} rings, showing substantial variation in magnetic interactions between spin centers.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Physical
Isabel Abanades Lazaro, Eleni C. Mazarakioti, Eduardo Andres-Garcia, Bruno J. C. Vieira, Joao C. Waerenborgh, Inigo J. Vitorica-Yrezabal, Monica Gimenez-Marques, Guillermo Minguez Espallargas
Summary: Two ultramicroporous 2D and 3D iron-based Metal-Organic Frameworks (MOFs) were synthesized through solvothermal synthesis, using different ratios and concentrations of precursors. These MOFs have reduced pore spaces decorated with pendant pyridine from tangling isonicotinic ligands, enabling them to achieve size-exclusion kinetic gas separation and thermodynamic separation, resulting in efficient and renewable CO2/N2 selectivity for dynamic breakthrough gas separation.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Andrei S. Baluna, Marcel Dommaschk, Burkhard Groh, Salma Kassem, David A. Leigh, Daniel J. Tetlow, Dean Thomas, Loli Varela Lopez
Summary: We report the synthesis and operation of a molecular energy ratchet that transports a crown ether from solution onto a thread, switching on pyrene fluorescence under UV irradiation. The system provides a potential signaling approach for artificial molecular machines.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Organic
David P. Tilly, Catherine McColl, Mingda Hu, Inigo J. Vitorica-Yrezabal, Simon J. Webb
Summary: This article describes the study of two short pentapeptides rich in alpha-aminoisobutyric acid (Aib) as enantioselective organocatalysts. The findings show that folding into a 310 helical structure allows the peptides to transmit chiral information and promote the enantioselectivity of the reaction. This demonstrates the important role of achiral residues in catalysis.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2023)
