Article
Chemistry, Multidisciplinary
Taeyang An, Hanseul Ryu, Tae-Lim Choi
Summary: This study presents a versatile approach to improve the alternation and degradability of 2,3-dihydrofuran (DHF) copolymers by carefully controlling the reactivity of both the Ru initiators and the monomers. The DHF copolymers showed outstanding A, B-alternation and could be broken down to a single repeat unit level under acidic conditions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Polymer Science
Mohammad Yasir, Andreas F. M. Kilbinger
Summary: Norbornene and cyclohexene show different polymerization behaviors using Grubbs' catalysts due to their varying ring strain energy levels; a sequence-selective cascade polymerization of a monomer containing both rings resulted in polymers with moderate molecular weight dispersities and good control over molecular weight.
Review
Polymer Science
Jiaxi Xu, Nikos Hadjichristidis
Summary: The incorporation of heteroatom-containing weak bonds along polymer backbones has become a popular tool to accelerate degradation. Many methods have been reported for the synthesis of degradable heteroatom-containing polymers based on step-growth polymerization and chain-growth ring-opening polymerization. Ring-opening metathesis polymerization has emerged as an approach for the synthesis of various types of degradable polymers. This review covers the synthesis of different heteroatom-containing degradable polymers via ring-opening metathesis polymerization and their degradation mechanisms under different conditions.
PROGRESS IN POLYMER SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Phong K. Quach, Jesse H. Hsu, Ivan Keresztes, Brett P. Fors, Tristan H. Lambert
Summary: The ring-opening metathesis polymerization of cyclopropenes using hydrazonium initiators was investigated. The initiators, formed by condensing 2,3-diazabicyclo[2.2.2]octane and an aldehyde, polymerize cyclopropene monomers through a sequence of [3+2] cycloaddition and cycloreversion reactions. The study showed that the monomer to initiator ratio had a positive correlation with the degree of polymerization.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Polymer Science
Yujin Cha, JiHyeon Hwang, Luis Ramos, Huina Lin, Tianyu Zhu, Chuanbing Tang
Summary: The synthesis of cyclic cobaltocenium and its application in the synthesis of high-performance copolymers have been reported.
Article
Polymer Science
Sebla Onbulak, Marc A. Hillmyer
Summary: The synthesis of sequence-controlled poly(ethylene-co-styrene) copolymers is challenging due to limitations in catalytic olefin polymerizations. An alternative method using ROMP of cyclic olefins followed by hydrogenation can generate ethylene copolymers with regioregularity. Investigating the ROMP of low-strain cyclododecenes provided useful information for mechanistic aspects of polymerization.
Article
Polymer Science
Ankita Mandal, Subhajit Pal, Andreas F. M. Kilbinger
Summary: A new heterocyclic monomer is synthesized via Diels-Alder reaction and exhibits reluctant polymerization in dichloromethane (DCM) but facile polymerization in tetrahydrofuran using Grubbs' third generation catalyst (G3), with excellent control over molecular weight and dispersities. The removal of tert-butoxycarbonyl group from the polymeric backbone yields a water-soluble ring opening metathesis polymerization (ROMP) polymer. In DCM, this monomer can also copolymerize with 2,3-dihydrofuran under catalytic living ROMP conditions to produce backbone degradable polymers. All synthesized polymers are characterized by size exclusion chromatography (SEC) and nuclear magnetic resonance (NMR) spectroscopy. This new method for preparing water-soluble ROMP homopolymers and cost-effective degradable copolymers and block-copolymers may have potential applications in biomedicine.
MACROMOLECULAR RAPID COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Ki-Young Yoon, Jinkyung Noh, Quan Gan, Julian P. Edwards, Robert Tuba, Tae-Lim Choi, Robert H. Grubbs
Summary: The study presents a continuous circular process for the scalable synthesis of pure cyclic polymers. This process utilizes silica-supported ruthenium catalysts and newly designed glassware to enable polymerization, polymer separation, and catalyst recovery in situ. The process minimizes manual labor, maximizes catalyst security, and guarantees the purity of cyclic polymers.
Article
Chemistry, Multidisciplinary
Dmitry S. Belov, Logesh Mathivathanan, Melanie J. Beazley, William Blake Martin, Konstantin V. Bukhryakov
Summary: The study explores the capability of an iron-based catalyst in performing ring-opening metathesis polymerization of olefins, demonstrating that the use of in situ prepared heteroleptic iron catalysts significantly enhances polymerization rate and selectivity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Polymer Science
Huiqun Wang, Sebla Onbulak, Steven Weigand, Frank S. Bates, Marc A. Hillmyer
Summary: The researchers synthesized a series of polyethylene-graft-aPP graft copolymers and found that increasing aPP content led to decreased melting temperatures and glass transition temperatures of PE, as well as decreased crystallinity. Additionally, the linear viscoelastic behavior of the PE-g-aPP graft copolymers exhibited greatly enhanced dynamic modulus and complex viscosity, with the effect increasing as side chain number and/or length increased.
Review
Chemistry, Applied
Nina Guy, Olivia Giani, Sebastien Blanquer, Julien Pinaud, Jean-Jacques Robin
Summary: Photopolymerization is gaining interest in both industrial and academic fields due to its high reaction kinetics, low emissions of organic solvents, and reduced shrinking stress. This method has mainly been developed for radical polymerization of vinyl monomers and to a lesser extent for ring-opening polymerization (ROP). With the emergence of new initiating systems, the photopolymerization of various cyclic monomers has expanded beyond epoxides, which were the first monomers polymerized by cationic ring-opening polymerization (CROP).
PROGRESS IN ORGANIC COATINGS
(2021)
Article
Polymer Science
Chia-Jung Lin, Yi-Hao Lin, Tai-Chin Chiang, Chin-Yang Yu
Summary: Well-defined norbornene-based homopolymers and block copolymers with low polydispersity index and close to theoretical molecular weight were synthesized using the third-generation Grubbs' initiator. These polymers exhibit aggregation-induced emission characteristics and high emission in solid and aggregate states. They show strong sensing ability for aniline in the aggregated state with a detection limit of 5 x 10-6 M.
Article
Polymer Science
Francis O. Boadi, Nicole S. Sampson
Summary: Bicyclo[4.2.0]oct-6-ene-7-carboxamide can form an alternating copolymer with cyclohexene in the presence of N-heterocyclic carbene-ruthenium catalyst. By creating a gradient copolymer with two different monomers, specific surface hydrophobicity, topology, and thermal properties can be controlled.
Article
Polymer Science
Mohammad Yasir, Manvendra Singh, Andreas F. M. Kilbinger
Summary: A mechanistically unique and efficient method for preparing heterotelechelic polymers through ring-opening metathesis polymerization using a single functionalization agent is reported. This method offers simplicity and efficiency, as different functionalization agents can be synthesized from inexpensive commercial starting materials to achieve the synthesis of heterotelechelic polymers.
Article
Chemistry, Multidisciplinary
Zhen Yu, Meng Wang, Xu-Man Chen, Shuai Huang, Hong Yang
Summary: The novel macrobicyclic olefin system shows good selectivity and high stereoselectivity in ROMP, with sacrificial cleavage of the silyloxide bridge providing clean-structured, non-auxiliaried polymers.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Polymer Science
Michael Kuepfert, Eman Ahmed, Marcus Weck
Summary: This study reports on thermoresponsive core-shell micelles as catalyst supports, which exhibit different lower critical solution temperature behavior and nanostructure size in water, demonstrating the efficiency by which the molecular brushes self-assemble into micelles. It was also found that molecular brushes with an extended backbone show higher activity and selectivity.
Article
Biochemistry & Molecular Biology
Annarita Falanga, Valentina Del Genio, Elizabeth A. Kaufman, Carla Zannella, Gianluigi Franci, Marcus Weck, Stefania Galdiero
Summary: Novel antiviral nanotherapeutics combining different antiviral peptides showed biocompatibility and effectively inhibited Herpes simplex virus type 1 by inactivating the virus and blocking it from entering host cells.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2021)
Article
Infectious Diseases
Xinxin Yang, Matthew F. Wipperman, Sharon Nachman, Nicole S. Sampson
Summary: Current TB diagnostic methods developed for adults are not suitable for children, especially those who are co-infected with HIV. This study established an ELISA assay to detect modified lipoprotein in plasma, which showed lower levels of TLP in active TB patients. This suggests that TLP has potential as a biomarker for TB detection in children.
BMC INFECTIOUS DISEASES
(2022)
Review
Chemistry, Multidisciplinary
Peiyuan Qu, Jacob W. Cleveland, Eman Ahmed, Fangbei Liu, Sage Dubrawski, Christopher W. Jones, Marcus Weck
Summary: The development of nonorthogonal tandem catalysis allows for the rapid synthesis of complex products using a combination of arbitrary catalysts. Compartmentalising molecular catalysts is key to overcoming incompatibilities and ensuring efficient reactions. Design principles and future directions in the field emphasize the importance of functional materials for compartmentalisation.
CHEMICAL SOCIETY REVIEWS
(2022)
Article
Polymer Science
Ru Deng, Chengyuan Wang, Marcus Weck
Summary: We report a hydrogen-bonded supramolecular miktoarm star polymer containing three distinct helical arms. The assembly is driven by the hydrogen bonding between Hamilton Wedge (HW) and barbituric acid (Ba). This modular approach provides a strategy for preparing nonlinear supramolecular ensembles with topologically diverse building blocks.
Article
Chemistry, Organic
Fangbei Liu, Peiyuan Qu, Marcus Weck
Summary: We successfully achieved substrate-selective asymmetric transfer hydrogenation of aromatic ketones using rhodium complexes immobilized on a photoresponsive nanoreactor. The morphology of the nanoreactor can be switched by light irradiation in a wavelength-selective manner. The gated behavior in the cross-linking layer plays a crucial role in discriminating among substrates and reagents during catalysis. Under ultraviolet light irradiation, the nanoreactor exhibits substrate selectivity and converts smaller ketone substrates to corresponding secondary alcohols faster.
Article
Polymer Science
Xiaoxi Yu, Guofang Li, Bingqian Zheng, Gyusaang Youn, Ting Jiang, Suan P. Quah, Scott T. Laughlin, Nicole S. Sampson, Surita R. Bhatia
Summary: This study investigates the interfacial rheology of sequence-controlled copolymers and finds that an increase in microblock size enhances the interfacial storage modulus, thereby tuning surface and interfacial properties. The research indicates that microblock size can be utilized to control the interfacial rheology of amphiphilic copolymers, providing a new strategy for controlling the dynamics of fluid interfaces through precision sequence-controlled polymers.
MACROMOLECULAR CHEMISTRY AND PHYSICS
(2022)
Article
Polymer Science
Arielle Mann, Marcus Weck
Summary: This contribution describes the synthesis of a novel unsymmetrical substituted tetraalkoxy[2.2]paracyclophane-1,9-diene and its polymerization to produce copolymers with alternating cis,trans-poly(p-phenylenevinylene)s. The synthesized polymers exhibit unique optical properties.
Article
Chemistry, Physical
Veronica Grebe, Mingzhu Liu, Marcus Weck
Summary: This paper introduces an algorithm that analyzes the dynamic assembly process of ellipsoidal particles and extracts quantitative data from qualitative media. By analyzing the data generated by the algorithm, a better understanding of the dynamic nature of particle chain formation can be obtained. This algorithm can quantitatively analyze the dynamic assembly behavior of particles of different shapes and is expected to be used for studying biological samples and nanoparticles.
COLLOID AND INTERFACE SCIENCE COMMUNICATIONS
(2022)
Review
Polymer Science
Arielle Mann, Matthew D. Hannigan, Marcus Weck
Summary: Poly(p-phenylene vinylene)s and poly(arylene vinylene)s are important materials for various applications. Recent advances in catalysts have allowed for the synthesis of PPVs with control over dispersity and solubility. The development of living ring-opening metathesis polymerization (ROMP) has enabled the incorporation of different end-groups and control over the number of repeat units.
MACROMOLECULAR CHEMISTRY AND PHYSICS
(2023)
Article
Engineering, Biomedical
Alessandra Zanut, Rui Li, Ru Deng, Xiangyu Liu, Martin Rejhon, Weiqiang Chen, Marcus Weck, Giuseppe Maria de Peppo, Elisa Riedo
Summary: Reproducing the multiscale physical features of human tissues in vitro provides new biomedical opportunities and fundamental understanding of cell-environment interfaces and interactions. A platform for tuning the stiffness of a biocompatible polymeric interface up to values characteristic of human bone is reported, enabling better adhesion, proliferation, and osteogenic differentiation. The platform allows rapid and simple fabrication of stiffness patterns and gradients, offering innovative applications in biosensors, single-cell patterning, and lab-on-a-chip devices.
ADVANCED HEALTHCARE MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Francis O. Boadi, Nicole S. Sampson
Summary: This study investigates the rates of ruthenium-catalyzed alternating ring opening metathesis (AROM) of cyclohexene using two different Ru-cyclohexylidenecarbenes derived from bicyclo[4.2.0]oct-6-ene-7-carboxamides with different side chains. The substitution of the amide directly affects the rate of ring opening of the bicyclo[4.2.0]oct-6-ene-7-carboxamide and the reaction rate of the resulting carbene with cyclohexene. Different factors, such as the stability of ligated complexes and the relative rates of ring opening reactions, are considered to determine the kinetics and gradient copolymer structures.
ACS ORGANIC & INORGANIC AU
(2023)
Article
Chemistry, Medicinal
Joshua M. Werman, Yu-Ching Chen, Tianao Yuan, Xinxin Yang, Nicole S. Sampson
Summary: By studying the effects of 6-azasteroid analogs on Mycobacterium tuberculosis and Mycobacterium marinum, we can enhance the antimycobacterial activity and gain a better understanding of the mechanism behind the potentiation of the antituberculosis drug bedaquiline.
ACS INFECTIOUS DISEASES
(2023)
Article
Chemistry, Physical
Fangyuan Dong, Samira Munkaila, Veronica Grebe, Marcus Weck, Michael D. Ward
Summary: This study presents a synthetic strategy for creating metallodielectric particles with spatially segregated amine-functionalized lobes, which can be selectively coated with gold. The researchers also found that dielectrophoretic forces exerted by an AC field can generate aggregate structures of different shapes and lobe arrangements.
Article
Chemistry, Multidisciplinary
Eman Ahmed, Jinwon Cho, Lulu Friedmann, Seung Soon Jang, Marcus Weck
Summary: This article presents the self-assembly behavior of multicompartment micelles in water and their use as supports for aqueous catalysis. The morphologies of the micelles and their catalytic activities were investigated, and the results showed that micelle morphology plays an important role in catalytic activity.
