Article
Chemistry, Multidisciplinary
Tian Zeng, Xiaoran Hu, Maxwell J. Robb
Summary: In this study, a new mechanophore platform based on a masked 2-furylcarbinol derivative was reported, which efficiently releases phenol and arylamine payloads following mechanical activation. This platform incorporates a 5-aryloxy group as an electron-rich substituent to accelerate molecular release.
CHEMICAL COMMUNICATIONS
(2021)
Article
Chemistry, Medicinal
Anna Carbery, Rachael Skyner, Frank von Delft, Charlotte M. Deane
Summary: Current fragment-based drug design relies on structurally diverse libraries of small fragments to explore chemical space. However, structurally dissimilar compounds can be functionally similar. By analyzing the 3D structures of fragments bound to multiple targets, we found a better strategy for selecting fragments for screening libraries. Ranking fragments based on the number of novel interactions they generated, we discovered that functionally diverse selections of fragments can greatly increase the amount of information recovered for unseen targets. Using these findings, we designed small functionally efficient libraries that provide more information about new protein targets compared to structurally diverse libraries of similar size.
JOURNAL OF MEDICINAL CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Hye-Seon Jeong, Eunseo Kim, Changwoo Nam, Yoon Choi, You-Jeong Lee, David A. Weitz, Hyomin Lee, Chang-Hyung Choi
Summary: A hydrogel microcapsule with an intermediate thin oil layer is developed for smart release of diverse cargoes triggered by stimuli. The oil layer acts as an effective diffusion barrier, allowing encapsulation of various small cargoes within a porous hydrogel shell until a stimulus destabilizes the oil layer for on-demand release.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Review
Chemistry, Multidisciplinary
Alejandro Lopez-Moreno, Julia Villalva, Emilio M. Perez
Summary: SWNTs are a highly interesting nanomaterial, where chemical modifications can enhance their intrinsic properties. The mechanical bond is appealing for materials science and SWNTs. Making MINTs has potential advantages compared to covalent or classic supramolecular derivatives.
CHEMICAL SOCIETY REVIEWS
(2022)
Article
Biochemistry & Molecular Biology
Fatima Amanat, Mahima Thapa, Tinting Lei, Shaza M. Sayed Ahmed, Daniel C. Adelsberg, Juan Manuel Carreno, Shirin Strohmeier, Aaron J. Schmitz, Sarah Zafar, Julian Q. Zhou, Willemijn Rijnink, Hala Alshammary, Nicholas Borcherding, Ana Gonzalez Reiche, Komal Srivastava, Emilia Mia Sordillo, Harm van Bakel, Jackson S. Turner, Goran Bajic, Viviana Simon, Ali H. Ellebedy, Florian Krammer
Summary: After receiving the SARS-CoV-2 spike mRNA vaccine, individuals showed robust polyclonal antibody responses, with a majority of vaccine-induced antibodies lacking neutralizing activity. However, vaccine-induced RBD binding antibodies may offer substantial protection against viral variants carrying single E484K RBD mutations.
Article
Chemistry, Multidisciplinary
Hayato Anetai, Yoshitaka Matsushita, Takahito Ohmura, Masayuki Takeuchi
Summary: Single crystals of simple benzene derivatives with different substituents were prepared and the flexibility of these crystals was investigated. The crystals can be classified into three types based on their bending behavior, which depends on the substituents. Furthermore, density functional theory calculation and nanoindentation test revealed the mechanical properties of the bendable crystals.
CRYSTAL GROWTH & DESIGN
(2023)
Article
Chemistry, Multidisciplinary
Emile R. Engel, Satoshi Takamizawa
Summary: Phase diagram mapping is a useful method for predicting and rationalizing crystal transition phenomena. A comprehensive phase diagram has been presented for pimelic acid, explaining its three different mechanical responses: jumping/fragmentation, superelasticity, and ferroelasticity.
CRYSTAL GROWTH & DESIGN
(2022)
Article
Multidisciplinary Sciences
Ying Lai, Giorgio Fois, Jose R. Flores, Michael J. Tuvim, Qiangjun Zhou, Kailu Yang, Jeremy Leitz, John Peters, Yunxiang Zhang, Richard A. Pfuetzner, Luis Esquivies, Philip Jones, Manfred Frick, Burton F. Dickey, Axel T. Brunger
Summary: Membrane fusion triggered by Ca2+ is important for synaptic neurotransmitter release and mucin secretion. A designed peptide can disrupt Ca2+-triggered membrane fusion, reduce stimulated mucin secretion, and alleviate mucus occlusion of mouse airways.
Article
Chemistry, Applied
Jundan Huang, Wenjing Wei, Bian Li, Tao Liu, Xiaofang Chen
Summary: This study synthesized a series of biphenyl-based cyanostilbenic compounds with mechanofluorochromic properties, and further investigated their photocycloaddition reaction process, finding that they exhibited good photochromic fluorescent response in the amorphous state. The results of this study can be used to monitor the photoreaction process and quantitatively analyze the products.
Article
Chemistry, Multidisciplinary
Miao Luo, Juan Zhao, Yanyan Liu, Zhu Mao, Sheng Wang, Zhenguo Chi
Summary: Three novel all-visible-light triggered fluorescent molecular photoswitches have been designed and prepared, achieving reversible photochromic and fluorescent switching in dilute solutions, films, and powder states. Solvent polarity can alter the photochromic abilities of two distinct conformations, and the size difference between the two conformations is one of the largest changes among photochromic molecules based on dithienylethene. The accompanying conformational changes provide insights into the relationship between solvent characteristics, crystal structure, and intermolecular interaction in solid state for all-visible-light triggered photoswitching molecules.
ADVANCED FUNCTIONAL MATERIALS
(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
Chemistry, Inorganic & Nuclear
Yun-Rui Chen, Meng-Ze Jia, Jia-Qi Pan, Bin Tan, Jie Zhang
Summary: In this study, photoinduced bending behavior triggered by [2 + 2] cycloaddition of a photoactive complex was successfully achieved, accompanied by photochromic and fluorescence changes. The introduction of flexible methylene groups and cation-pi interactions provided convenience for long-distance observation of photomechanical motion.
DALTON TRANSACTIONS
(2022)
Article
Biochemistry & Molecular Biology
Wafa Soudani, Fatima Zohra Hadjadj-Aoul, Mohammed Bouachrine, Hanane Zaki
Summary: This study focused on the molecular modelling of 2-chloroethylnitrosoureas into 2-chloroethylnitrososulfamides derived from Carmustine, evaluating the pharmacodynamic profile through molecular docking. The results showed a better chemical affinity of CENS to the biological target and stability of the ligand-DNA complex, indicating potential inter-strand crosslinking. The molecular docking study provided insights into the therapeutic mode of action of CENS.
JOURNAL OF BIOMOLECULAR STRUCTURE & DYNAMICS
(2021)
Article
Nanoscience & Nanotechnology
Rui Huang, Ruochen Lan, Chen Shen, Zhongping Zhang, Zichen Wang, Jinying Bao, Zizheng Wang, Lanying Zhang, Wei Hu, Zhan Yu, Siquan Zhu, Lei Wang, Huai Yang
Summary: Responsive smart nanocarriers are a promising class of materials for drug delivery and tissue engineering. This study introduces a novel strategy to impart light responsivity to internal drugs in microcapsules, enabling accelerated drug release with the help of UV light and molecular motors. The cooperative effect of liquid crystalline mesogens facilitates molecular-scale geometric changes, leading to microscale disturbances and faster drug delivery.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Multidisciplinary
Yue Hua, Han Yin, Xiaoyang Liu, Jinbing Xie, Wenjun Zhan, Gaolin Liang, Yang Shen
Summary: In this study, a supramolecular hydrogel capable of responsive release of a SIK2 inhibitor was developed for ovarian cancer therapy. Cell and animal experiments demonstrated its therapeutic efficacy and potential clinical application.
Article
Polymer Science
Anna C. Overholts, Molly E. McFadden, Maxwell J. Robb
Summary: Accurate and quantitative characterization of structure-mechanochemical activity relationships is crucial for understanding mechanochemical reactivity and advancing the field of polymer mechanochemistry. Ultrasound-induced mechanical activation of polymers is a common method for studying mechanophore reactivity, but traditional methods for analyzing chain scission kinetics from GPC measurements may provide misleading results. This study demonstrates the importance of spectroscopic analysis in accurately determining mechanophore activation rates, highlighting the need for a unified approach to kinetic analysis in polymer mechanochemistry.
Article
Polymer Science
Anna C. Overholts, Maxwell J. Robb
Summary: In this study, we investigated the activation efficiency of different mechanophores under ultrasound-induced mechanical force and found that the characteristics of the mechanophore and its position in the polymer chain play crucial roles in determining the selectivity of ultrasound-induced mechanophore activation.
Article
Polymer Science
Corey C. Husic, Xiaoran Hu, Maxwell J. Robb
Summary: This study presents a new design of mechanophore polymer container that can release chemical payloads efficiently in non-proton solvent environments. The design incorporates a tethered primary alcohol and an intramolecular hydrogen bonding interaction between the alcohol and the carbonyl oxygen of a carbonate, reducing the activation energy for carbonate fragmentation and enabling molecular release. This design expands the application range of mechanically triggered release.
Article
Chemistry, Multidisciplinary
Molly E. McFadden, Skylar K. Osler, Yan Sun, Maxwell J. Robb
Summary: Multimodal mechanophores can distinguish between different stress states through color changes. In this study, we covalently linked polymer chains to naphthodipyran and generated the dual ring-opened dimerocyanine product with unique near-infrared absorption properties using mechanical force.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Anna C. Overholts, Wendy Granados Razo, Maxwell J. Robb
Summary: Mechanophores are stress-sensitive molecules that undergo productive chemical transformations under mechanical force. A new platform has been introduced to achieve mechanically gated multicolour chromogenic reactivity. This platform is based on an activated furan precursor, which, when mechanochemically activated, generates a diverse range of color variations. This system has been applied to create a complex multicolour composite image through localized compression and reaction with different secondary amines.
Article
Chemistry, Multidisciplinary
Hui-Qi Ni, Malkanthi K. Karunananda, Tian Zeng, Shenghua Yang, Zhen Liu, K. N. Houk, Peng Liu, Keary M. Engle
Summary: Multistep organic synthesis allows the conversion of simple chemical feedstocks into more complex products with specific functions. This study introduces a novel approach to organic reactions that can generate multiple valuable products with different carbon skeletons in a single operation. Through a palladium-catalyzed reaction, a single alkene starting material can be converted into two structurally distinct products, demonstrating the potential for simultaneous access to diverse compounds. The findings of this study provide insights into the mechanistic details of this unique catalytic system and establish a new method for small-molecule library synthesis.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Infectious Diseases
Mingrong Yin, Zhipeng Tang, Xiaoran Hu, Yuyan Li, Longzong Guo, Xiaolong Sun, Shuang Chang, Peng Zhao, Yixin Wang
Summary: A cluster of artificially bred vultures in a zoo in Shandong Province, China exhibited emaciation and mortality, suggesting the presence of an immunosuppressive pathogen. Nucleic acid testing confirmed the presence of chicken infectious anemia virus (CIAV) in the dead vulture tissue. The isolated CIAV strain, SDTY2021-TJ, showed high pathogenicity in SPF chickens, causing significant mortality and immunosuppressive effects.
TRANSBOUNDARY AND EMERGING DISEASES
(2023)
Article
Polymer Science
Molly E. McFadden, Anna C. Overholts, Skylar K. Osler, Maxwell J. Robb
Summary: Understanding the relationship between structure and mechanochemical reactivity is crucial for designing new stimuli-responsive polymers. In this study, we validate an initial rates method that accurately determines rate constants for ultrasound-induced mechanochemical transformations. The experimental results support the effectiveness of this method in deconvoluting the kinetics of specific mechanophore activation from nonspecific chain scission.
Article
Chemistry, Multidisciplinary
Xuancheng Fu, Boyu Zhu, Xiaoran Hu
Summary: This paper presents a mechanical approach to induce atropisomerization in a parallel diarylethene molecule, resulting in distinct chemical reactivity of its antiparallel diastereomers. Under ultrasound-induced force field, a congested parallel diarylethene mechanophore in (R(a), S(a)) configuration with mirror symmetry is atropisomerized to antiparallel diastereomers with C(2) symmetry. The obtained stereochemistry-converted material exhibits symmetry-allowed reactivity towards conrotatory photocyclization.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Polymer Science
Skylar K. Osler, Molly E. McFadden, Tian Zeng, Maxwell J. Robb
Summary: Multi-modal mechanophores that react under mechanical force to produce unique absorption properties are of interest for force-sensing polymer design. In this study, a 2H-bis-naphthopyran mechanophore was investigated for its reactivity in generating thermally stable mono- and bis-merocyanine products upon mechanical activation. The force-mediated ester bond scission reaction followed by intramolecular hydrogen bonding plays a role in locking one merocyanine subunit in the open form, leading to the formation of an unusual trans merocyanine isomer. Unexpectedly, density functional theory calculations suggest a thermally reversible retro-cyclization reaction that may explain the mechanochemical generation of this isomer.
Article
Polymer Science
Stella M. Luo, Ross W. Barber, Anna C. Overholts, Maxwell J. Robb
Summary: Our understanding of mechanochemical reactivity has significantly improved over the past two decades. However, limited knowledge of structure-activity relationships and governing principles hampers molecular design. Simple computational tools like CoGEF have aided the experimental development of mechanophores, allowing the extraction of quantitative metrics like rupture force to estimate reactivity.
Article
Chemistry, Multidisciplinary
Tian Zeng, Xiaoran Hu, Maxwell J. Robb
Summary: In this study, a new mechanophore platform based on a masked 2-furylcarbinol derivative was reported, which efficiently releases phenol and arylamine payloads following mechanical activation. This platform incorporates a 5-aryloxy group as an electron-rich substituent to accelerate molecular release.
CHEMICAL COMMUNICATIONS
(2021)