Article
Chemistry, Multidisciplinary
Yi Lu, Hajime Sugita, Koichiro Mikami, Daisuke Aoki, Hideyuki Otsuka
Summary: Exploration of mechanochemical reactions has opened up new opportunities for designing functional materials, such as the synthesis and application of BMPF as a mechanophore in stress-responsive materials with excellent potential for applications.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Polymer Science
Sourabh Kumar, Baris Demir, Alexander Dellwisch, Lucio Colombi Ciacchi, Tim Neudecker
Summary: This study introduces a multiscale mechanochemical model that establishes a connection between bulk deformation and mechanophore activation. By combining quantum mechanical and molecular mechanical simulations, the activation of mechanophores in polymer networks under different strain conditions is simulated.
Article
Chemistry, Multidisciplinary
Hang Shen, Yunzheng Cao, Miaojiang Lv, Qinxin Sheng, Zhengbiao Zhang
Summary: The field of force-induced release of small cargoes within polymeric materials has grown rapidly in the past decade, achieving diversified functional materials and investigating force-coupled reactivity of mechanophores. By discussing different types of mechanophores and their mechanochemical reactions, it is possible to release acids, gases, fluorophores, drugs, iron ions, and more. The challenges and future targets in this growing field are also discussed.
CHEMICAL COMMUNICATIONS
(2022)
Review
Polymer Science
Daniel E. Martinez-Tong, Jose A. Pomposo, Ester Verde-Sesto
Summary: Polymer mechanochemistry has focused on using advanced force application methods like ultrasonication and single-molecule force spectroscopy (SMFS) to study the mechanophores' responses, exploring the mechanochemical properties of stress-responsive motifs. Recent research has emphasized the importance of the fundamental parameters of single-molecule force spectroscopy technique for triggering specific force responses, as well as the measurement of force-extension curves for single- and multi-mechanophore polymers.
MACROMOLECULAR RAPID COMMUNICATIONS
(2021)
Review
Medicine, Research & Experimental
Bohan Yin, Junguo Ni, Claire E. Witherel, Mo Yang, Jason A. Burdick, Chunyi Wen, Siu Hong Dexter Wong
Summary: Osteoarthritis is a common chronic whole-joint disease, and the secretion of extracellular vesicles plays a role in its pathogenesis. Extracellular vesicles derived from mesenchymal stem cells or platelet-rich plasma have high therapeutic value for treating osteoarthritis and can be modified or incorporated into biomaterials for enhanced targeting and prolonged retention. By analyzing pathological biomarkers associated with osteoarthritis, we discuss current diagnostic and therapeutic methods and propose the potential of using extracellular vesicles for the diagnosis and treatment of osteoarthritis in the future.
Article
Chemistry, Medicinal
Shiji Zhao, Andrew J. Schaub, Shiou-Chuan Tsai, Ray Luo
Summary: The development of the Pantetheine Force Field (PFF) library allows for the modeling of systems containing PCLs in silico, supporting various applications including protein engineering and drug discovery. Validation studies have shown promising performance in molecular dynamics simulations compared to experimental data of representative systems.
JOURNAL OF CHEMICAL INFORMATION AND MODELING
(2021)
Review
Gastroenterology & Hepatology
Laura E. McCoubrey, Moe Elbadawi, Mine Orlu, Simon Gaisford, Abdul W. Basit
Summary: Seminal microbiome research in the past twenty years has shown the intrinsic relationship between microbiota and human health, with imbalanced microbiomes linked to diseases. Machine learning offers powerful techniques for analyzing and predicting microbiome big data, facilitating the development of new therapeutics.
Article
Chemistry, Multidisciplinary
Yaoli Zhao, Patatri Chakraborty, Ali Passian, Thomas Thundat
Summary: Molecular-level spectroscopy is essential for sensing and imaging applications, but the detection and quantification of minuscule quantities of chemicals are challenging, particularly when they adsorb in low numbers. In this study, a photothermal spectroscopic technique utilizing a microfabricated nanoscale thermocouple junction integrated into a microcantilever was introduced for high selectivity sensing of adsorbates with an attogram detection limit. The temperature variation driving the thermoelectric junction is caused by the nonradiative decay of molecular adsorbates' vibrational states on the tip. The detection of photothermal spectra of physisorbed trinitrotoluene (TNT) and dimethyl methylphosphonate (DMMP) molecules, as well as representative polymers, with an estimated mass of 10^(-18) g was demonstrated.
Review
Biotechnology & Applied Microbiology
Alexander Honkala, Sanjay Malhotra, Shivaani Kummar, Melissa R. Junttila
Summary: Recent advances in understanding molecular basis, identifying therapeutic targets, and evolving regulatory landscape have made oncology drug development an exciting time, yet challenges like high costs and high attrition rates persist. Alignment of patient tumor biology with preclinical models is crucial for developing effective treatments, enhancing translational research in both forward and reverse directions.
NATURE REVIEWS DRUG DISCOVERY
(2022)
Article
Pharmacology & Pharmacy
Roberto Oliva, Giovanna Ginestra, Anna Piperno, Antonino Mazzaglia, Antonia Nostro, Angela Scala
Summary: This study developed a novel PLA-PEG NPs for the delivery of Linezolid against MRSA. The encapsulation efficiency of LNZ in PLA-PEG NPs was 15% with a 10:3 polymer to drug mass ratio, and sustained release kinetics with 65% of the antibiotic released within 80 h. The NPs exhibited antimicrobial activity against various Gram-positive bacteria including MRSA, and showed inhibitory activity on both planktonic growth and preformed biofilm of MRSA.
INTERNATIONAL JOURNAL OF PHARMACEUTICS
(2023)
Article
Chemistry, Multidisciplinary
Ankita Das, Ayan Datta
Summary: Mechanical force can release small molecules from macromolecular carriers in a predictable and precise manner. Using mechanochemical simulations, this study demonstrates that norborn-2-en-7-one (NEO) and its derivatives can selectively release CO, N-2, and SO2 to generate two distinct products A and B. The regioselectivity in the pulling points enables the exclusive formation of either A or B. Through changing the rigidity of the NEO scaffold and tuning the pulling groups, control over the selective formation of B is achieved. The diradical intermediate formed during the conversion of I to A is predicted to be persistent for approximately 150 fs. Structural design plays a crucial role in balancing the mechanochmeical rigidity and lability.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Engineering, Biomedical
Kun Xue, FuKe Wang, Ady Suwardi, Ming-Yong Han, Peili Teo, Pei Wang, Shijie Wang, Enyi Ye, Zibiao Li, Xian Jun Loh
Summary: Biomaterials research can accelerate success through machine learning techniques, leading to faster commercialization. Transitioning from unstructured empirical approaches to data-driven development strategies can bring about many potential benefits.
MATERIALS TODAY BIO
(2021)
Review
Pharmacology & Pharmacy
Zhaokui Jin, Qi Gao, Keke Wu, Jiang Ouyang, Weisheng Guo, Xing-Jie Liang
Summary: The lack of effective treatments for pulmonary diseases is a significant global health burden. Inhaled nanomedicines offer promise for precise and localized drug delivery, but face multifaceted challenges. This review summarizes the barriers associated with pulmonary diseases, the effects of physicochemical properties and drug formulations, and the advantages of nanomedicine in overcoming these barriers.
ADVANCED DRUG DELIVERY REVIEWS
(2023)
Article
Chemistry, Multidisciplinary
Raphael Hertel, Wafa Maftuhin, Michael Walter, Michael Sommer
Summary: In this study, we used a series of thiophene-flanked quinoxalines as molecular torsional springs for force sensing in bulk polymers at room temperature. Through detailed spectroscopy and calculations, we identified the thiophene ring flip as the major part of the overall mechanochromic response. The thiophene ring flip requires much smaller forces than planarization of the DAD spring, allowing for sensing of tiny forces and expanding the sensitivity and force range of conformational mechanochromophores.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Anton O. Razgoniaev, Logan M. Glasstetter, Tatiana B. Kouznetsova, Kacey C. Hall, Matias Horst, Stephen L. Craig, Katherine J. Franz
Summary: The experimental characterization of the mechanochemical scission of metal-NHC bonds in N-heterocyclic carbene mechanophores has been reported. The study reveals a force-coupled rate constant for ligand dissociation and supports a dissociative mechanism of ligand displacement, with the rate-limiting scission of Pd-NHC bond followed by rapid dissociation of the pyridine moiety from Pd.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Xiaoran Hu, Tian Zeng, Corey C. Husic, Maxwell J. Robb
Summary: A general mechanophore platform based on masked 2-furylcarbinol derivatives is described in this study, which can spontaneously decompose under mild conditions upon liberation via a mechanically triggered reaction, resulting in the release of functionally diverse molecular cargo with adjustable release kinetics. The platform demonstrates good selectivity and control, and efficient release of various cargo molecules can be triggered by ultrasound-induced mechanical force.
ACS CENTRAL SCIENCE
(2021)
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)