Article
Polymer Science
Wangmeng Hou, Xiuzhe Yin, Yao Chen, Jianzhong Du, Yongming Chen, Yi Shi
Summary: A novel aqueous ring-opening metathesis polymerization method named ME-ROMP is proposed. It involves injecting a small amount of a CH2Cl2 solution of the Grubbs' third-generation catalyst into the aqueous solution of water-soluble monomers, allowing high efficiency and controlled polymerization without deoxygenation. This method enables the synthesis of well-defined water-soluble polynorbornenes with various compositions and architectures.
Article
Polymer Science
Henry L. Cater, Iana Balynska, Marshall J. Allen, Benny D. Freeman, Zachariah A. Page
Summary: This paper presents a systematic study on ROMP with endo-norbornene monomers using stable chelated Ru-alkylidene initiators. The study shows that ROMP with endo-norbornene monomers is versatile and robust, providing access to polymers with excellent molecular weight control, low dispersities, good functional group tolerance, and high chain-end fidelity. The process is oxygen-tolerant and can be performed under ambient conditions, allowing for the synthesis of mechanically robust thermoplastics with high glass transition and decomposition temperatures.
Article
Polymer Science
Sarah E. Blosch, Mohammed Alaboalirat, Cabell B. Eades, Samantha J. Scannelli, John B. Matson
Summary: This study investigates the influence of solvent choice and purity on the propagation rate and termination reactions in ring-opening metathesis polymerization (ROMP) reactions. It was found that the choice of solvent and its purity level can significantly affect the propagation rate and termination reactions in ROMP reactions.
Article
Chemistry, Multidisciplinary
Indradip Mandal, Ankita Mandal, Md Atiur Rahman, Andreas F. M. Kilbinger
Summary: In this study, the metathesis activity of conjugated 1,3 diene derivatives in ring opening metathesis polymerization (ROMP) using Grubbs' 3rd generation catalyst (G3) was investigated. Monosubstituted 1,3 dienes showed similar reactivities towards G3-alkylidenes as norbornene derivatives, making them suitable for chain transfer agents in catalytic ROMP. This unprecedented reactivity allowed for the synthesis of mono-end-functional poly(norborneneimide)s on a large scale. Additionally, more complex architectures such as star-shaped polymers could be synthesized catalytically via ROMP. This method was also utilized for the synthesis of ROMP block copolymers and ROMP-PEG diblock copolymer.
Article
Polymer Science
Shoichiro Uchiyama, Taichi Sotani, Toshiko Mizokuro, Hiromitsu Sogawa, Kenneth B. Wagener, Fumio Sanda
Summary: The functionalization of polymer chain ends is a hot topic in synthetic polymer chemistry. This study demonstrates the incorporation of a platinum complex at the terminal of a polynorbornene derivative for the first time. The modified polymers exhibited enhanced absorption and photoluminescence properties compared to the unmodified polymer. The weight residues of the functionalized polymers at high temperatures were higher than the unmodified polymer.
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
Ankita Mandal, Indradip Mandal, Andreas F. M. Kilbinger
Summary: Single chain transfer agents are used to synthesize narrowly distributed heterotelechelic ROMP polymers in one pot, exploiting a new mechanistic and synthetic approach. The strategy allows for excellent control over molecular weight and dispersity of the resulting polymers, showcasing a straightforward and efficient method for synthesizing heterotelechelic ROMP polymers.
Article
Polymer Science
Tianqi Zhang, Xuelin Sui, Will R. Gutekunst
Summary: This report discusses the use of enyne-containing branching agents in synthesizing star and miktoarm star polymers through a convergent synthesis pathway using ring-opening metathesis polymerization (ROMP). By introducing these agents into a living ROMP, control over the degree of polymerization of the star arms, the number of star arms, and chain extension can be achieved to produce functional asymmetric miktoarm star polymers.
Article
Biochemistry & Molecular Biology
Ervin Kovacs, Bence Balterer, Nguyen Anh Duc, Gyorgyi Szarka, Michael C. Owen, Attila Domjan, Bela Ivan
Summary: A large number of organic solvents contaminate the environment on a daily basis worldwide. This study demonstrates that benzotrifluoride can be used as a suitable solvent for olefin metathesis reactions, providing high yields and similar or even higher reaction rates compared to dichloromethane.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
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
Polymer Science
Toshiki Sonoda, Shingo Kobayashi, Masaru Tanaka
Summary: The successful utilization of regioselective ring-opening metathesis polymerization to synthesize polymers modified with tertiary amino groups has demonstrated unique properties in hydration, crystallization, and coating stability under physiological aqueous environment.
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
Multidisciplinary Sciences
Thomas G. Pattison, Shuo Wang, Robert D. Miller, Gang-yu Liu, Greg G. Qiao
Summary: Macroscale additive manufacturing has developed significantly, but nanoscale formation of polymeric features from the bottom-up is not yet achieved. This study demonstrates a rapid crosslinking technique using an atomic force microscope, enabling fast curing of crosslinkable polymers in the presence of catalysts.
NATURE COMMUNICATIONS
(2022)
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
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
Chemistry, Multidisciplinary
Elena J. Cassella, Emma L. K. Spooner, Timothy Thornber, Mary E. O'Kane, Thomas E. Catley, James E. Bishop, Joel A. Smith, Onkar S. Game, David G. Lidzey
Summary: Self-assembled monolayers (SAMs) are widely used as hole-selective layers in perovskite solar cells. Ultrasonic spray coating and airbrush coating are effective methods for depositing carbazole-based SAMs. Solvent rinsing protocols overcome the dewetting issue of hybrid perovskite precursor solutions. Air-knife gas-quenching is used to remove volatile solvents, allowing fabrication of high-efficiency p-i-n devices with large-area roll-to-roll manufacturing.
Article
Chemistry, Multidisciplinary
Jincheng Tong, Amadou Doumbia, Raja U. Khan, Aiman Rahmanudin, Michael L. Turner, Cinzia Casiraghi
Summary: Quantitative measurements of molecular dynamics at the solid-liquid interface are crucial. However, the commonly used analytical techniques have limited sensitivity. By using electrolyte-gated organic field-effect transistors (EGOFETs), it is possible to monitor the crystallization process in real-time and quantify changes in solute concentration and molecular transport rate at the solid-liquid interface.
Article
Nanoscience & Nanotechnology
Amadou Doumbia, Michelle Webb, Jonathan M. Behrendt, Richard J. Wilson, Michael L. Turner
Summary: Electrolyte-gated organic field-effect transistors (EGOFETs) have great potential in biosensing applications. They can sensitively and selectively quantify various chemical and biological molecules, but the real-time monitoring of analyte-receptor interactions has been rarely explored. In this study, an EGOFET array integrated with a microfluidic device is presented for the real-time detection of DNA hybridization. The integrated devices exhibit highly reproducible electrical performance and can operate under different electrical stresses for extended periods of time.
ADVANCED ELECTRONIC MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Kezia Sasitharan, Rachel C. Kilbride, Emma L. K. Spooner, Jenny Clark, Ahmed Iraqi, David G. Lidzey, Jonathan A. Foster
Summary: This study demonstrates a broadly applicable approach to improve the morphology of bulk heterojunction OPV devices using metal-organic nanosheets as additives. The addition of nanosheets leads to remarkable improvements in power conversion efficiency of semi-crystalline polymer devices.
Article
Energy & Fuels
Dominic Blackburn, Thomas Routledge, Mary O'Kane, Elena J. Cassella, Onkar S. Game, Thomas E. Catley, Christopher J. Wood, Trevor McArdle, David George Lidzey
Summary: Tin oxide (SnOx) electron-extraction layers were fabricated using a reactive electron-beam evaporation process, achieving power conversion efficiencies up to 19.3% in standard perovskite solar cells. The deposition process of SnOx can be done at low temperature and does not require subsequent high-temperature annealing, demonstrating its potential compatibility with roll-to-roll processing on flexible polymeric substrates.
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
Nanoscience & Nanotechnology
Armando Genco, Cristina Cruciano, Matteo Corti, Kirsty E. McGhee, Benedetto Ardini, Luca Sortino, Ludwig Huettenhofer, Tersilla Virgili, David G. Lidzey, Stefan A. Maier, Andrea Bassi, Gianluca Valentini, Giulio Cerullo, Cristian Manzoni
Summary: Fourier-plane microscopy is a powerful tool for measuring the angular optical response of materials and devices. A new hyperspectral microscope technique is introduced, allowing angle- and wavelength-resolved imaging of photoluminescent organic microcavities in just one measurement. This technique provides a complete optical characterization for materials and devices with nontrivial angle-/wavelength-dependent properties.
Article
Polymer Science
Van Hoang-Khang Phan, Yi-Hsin Tai, Tai-Chin Chiang, Chin-Yang Yu
Summary: This article focuses on the synthesis and properties of random copolymers poly(l-lactide-r-glycolide) and block copolymers poly(l-lactide-b-glycolide). The results show that block copolymers have better thermal stability and crystallinity compared to random copolymers, and also exhibit higher hydrophilicity.
JOURNAL OF APPLIED POLYMER SCIENCE
(2023)
Article
Polymer Science
Yurachat Janpatompong, Andrew M. Spring, Venukrishnan Komanduri, Raja U. Khan, Michael L. Turner
Summary: This article reports the synthesis of 2,3-dialkoxyphenylenevinylene polymers by ring contraction and ring-opening metathesis polymerization, as well as the preparation of block copolymers of phenylene vinylene polymers, and the properties of the polymers were studied.
Article
Materials Science, Multidisciplinary
Vanessa Tischler, Piotr Dudek, Jayawan Wijekoon, Leszek A. Majewski, Yasunori Takeda, Shizuo Tokito, Michael L. Turner
Summary: This paper reports the fabrication of a simple neuromorphic circuit using solution-processed organic field-effect transistors (OFETs). The circuit has predictable behavior and allows for customized design, providing the basis for various flexible neuromorphic circuit designs.
ORGANIC ELECTRONICS
(2023)
Article
Nanoscience & Nanotechnology
Emma L. K. Spooner, Elena J. Cassella, Joel A. Smith, Thomas E. Catley, Sam Burholt, David G. Lidzey
Summary: The introduction of Y-series non-fullerene acceptors has greatly improved the power conversion efficiencies of organic solar cells. This study demonstrates, for the first time, the deposition of a Y-series-based system using ultrasonic spray coating, which has the potential for significantly faster deposition speeds than traditional methods. The use of an air-knife enables rapid removal of the casting solvent and overcomes film reticulation, resulting in spray-coated PM6:DTY6 devices with PCEs of up to 14.1%. The study also highlights the challenges of scalable coating for Y-series-based solar cells, particularly the influence of slower drying times on blend morphology and crystallinity. The compatibility of ultrasonic spray coating with high-speed roll-to-roll OSC manufacturing techniques is demonstrated.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Polymer Science
Yurachat Janpatompong, Kamil Suwada, Michael L. Turner, Guillaume De Bo
Summary: Understanding the stability of conjugated polymers towards mechanical stimuli is crucial for optimizing their use in electronic and optoelectronic devices. Mechanochemistry is a field that aims to control mechanical forces for chemical changes, and it can also be used to study the stability of conjugated polymers. Ultrasonication is a technique that can be used to test the mechanical integrity of phenylenevinylene block copolymers and demonstrate their stability to mechanical forces, making them suitable for flexible organic electronics.
Article
Chemistry, Organic
Yurachat Janpatompong, Venukrishnan Komanduri, Raja U. U. Khan, Michael L. L. Turner
Summary: ortho-Diethylhexyloxyphenylene benzothiadiazole paracyclophane-1,9-diene, a mixture of diastereomers, was synthesized through benzyne-induced Stevens rearrangement, oxidation, and pyrolysis. These cyclophanedienes, when reacted with Grubbs catalyst, can be opened to alternating cis,trans-phenylenevinylene polymers. In situ NMR experiments showed that one isomer polymerized to 90% conversion, while the other isomer gave only 9% conversion due to steric hindrance. The resulting polymers can be easily isomerized to all-trans isomer using visible light, and their optical and electrochemical properties were investigated by theory and experiment.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2023)
Article
Energy & Fuels
Elena J. Cassella, Timothy Thornber, Robert D. J. Oliver, Mary E. O'Kane, Emma L. K. Spooner, Rachel C. Kilbride, Thomas E. Catley, Onkar S. Game, Alexandra J. Ramadan, David G. Lidzey
Summary: Defect management in perovskite solar cells through surface passivation is crucial for improving stability and efficiency. This study demonstrates the use of spray-coating technology to deposit iso-butylammonium bromide, resulting in the formation of a quasi-2D perovskite layer and significant improvement in device performance.
Article
Materials Science, Multidisciplinary
Kirsty E. McGhee, Rahul Jayaprakash, Kyriacos Georgiou, Stephanie L. Burg, David G. Lidzey
Summary: Researchers fabricated dielectric microcavities containing a molecular dye, demonstrating strong coupling despite the broad absorption line. They successfully generated polariton condensation from a strongly-coupled microcavity in air and at room temperature, showing high photostability of the dye.
JOURNAL OF MATERIALS CHEMISTRY C
(2022)