ORCID Profile
0000-0002-4564-4702
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Research Topics
In Research Link Australia (RLA), "Research Topics" refer to ANZSRC FOR and SEO codes. These topics are either sourced from ANZSRC FOR and SEO codes listed in researchers' related grants or generated by a large language model (LLM) based on their publications.
Top 5 Research Topics
ANZSRC Field of Research (FoR)
Synthesis of Materials | Macromolecular and Materials Chemistry | Chemical Engineering Design | Chemical Engineering | Nanochemistry and Supramolecular Chemistry | Functional materials | Functional Materials | Nanotechnology | Nanomaterials | Nanomedicine | Macromolecular and Materials Chemistry not elsewhere classified | Systems engineering | Materials engineering | Synthesis Of Macromolecules | Condensed Matter Physics | Polymerisation Mechanisms | Characterisation Of Macromolecules | Polymers and plastics | Macromolecular and materials chemistry | Composite and hybrid materials | Macromolecular Chemistry Not Elsewhere Classified | Materials Engineering | Medicinal and Biomolecular Chemistry not elsewhere classified | Composite and Hybrid Materials | Chemical engineering design | Macromolecular materials | Colloid and Surface Chemistry | Nanoscale Characterisation | Civil engineering | Chemical Engineering not elsewhere classified | Surfaces and Structural Properties of Condensed Matter | Fire safety engineering | Nanobiotechnology | Condensed Matter Characterisation Technique Development
ANZSRC Socio-Economic Objective (SEO)
Expanding Knowledge in the Chemical Sciences | Expanding Knowledge in Engineering | Expanding Knowledge in Technology | Polymeric Materials (e.g. Paints) | Human Diagnostics | Mining and Extraction of Titanium Minerals, Zircon, and Rare Earth Metal Ores (e.g. Monazite) | Prevention—biologicals (e.g. vaccines) | Health not elsewhere classified | Diagnostics | Management of Greenhouse Gas Emissions from Manufacturing Activities | Treatments (e.g. chemicals, antibiotics) | Coated Metal and Metal-Coated Products | Expanding Knowledge in the Medical and Health Sciences | Hydrogen Production from Renewable Energy | Solar-Photovoltaic Energy | Plastic Products (incl. Construction Materials) | Expanding Knowledge in the Physical Sciences | Expanding Knowledge in the Biological Sciences |
Related Links
Publications
Seeing the Light: Advancing Materials Chemistry through Photopolymerization
Publisher: Wiley
Date: 11-02-2019
Abstract: The application of photochemistry to polymer and material science has led to the development of complex yet efficient systems for polymerization, polymer post-functionalization, and advanced materials production. Using light to activate chemical reaction pathways in these systems not only leads to exquisite control over reaction dynamics, but also allows complex synthetic protocols to be easily achieved. Compared to polymerization systems mediated by thermal, chemical, or electrochemical means, photoinduced polymerization systems can potentially offer more versatile methods for macromolecular synthesis. We highlight the utility of light as an energy source for mediating photopolymerization, and present some promising ex les of systems which are advancing materials production through their exploitation of photochemistry.
Rapid High‐Resolution 3D Printing and Surface Functionalization via Type I Photoinitiated RAFT Polymerization
Publisher: Wiley
Date: 26-02-2021
100th Anniversary of Macromolecular Science Viewpoint: Photochemical Reaction Orthogonality in Modern Macromolecular Science
Publisher: American Chemical Society (ACS)
Date: 19-06-2019
DOI: 10.1021/ACSMACROLETT.9B00292
Abstract: The ability to perform multiple chemical reactions independently (orthogonally) in a single reaction vessel can allow simplified reaction protocols for intricate chemical syntheses. Light is an especially advantageous external stimuli to enact such orthogonal chemical reactions due to its independence with other stimuli, instantaneous spatiotemporal control, and material penetrability. The potential to combine orthogonal chemistry and polymerization is also very appealing, as these systems may open the door for polymeric materials to find applications in emerging and high-tech fields, including biotechnology, microelectronics, sensors, energy, and others. We highlight the use of light in orthogonal polymerization protocols, particularly for living and controlled polymerization, and explore potential future directions and challenges for this technology.
Forced gradient copolymerisation: a simplified approach for polymerisation-induced self-assembly
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D0PY00889C
Abstract: In this work, a novel and versatile gradient copolymerisation approach to simplify polymeric nanoparticle synthesis through polymerisation-induced self-assembly (PISA) is reported.
Frontispiz: A Versatile 3D and 4D Printing System through Photocontrolled RAFT Polymerization
Publisher: Wiley
Date: 02-12-2019
A Photoinduced Dual‐Wavelength Approach for 3D Printing and Self‐Healing of Thermosetting Materials
Publisher: Wiley
Date: 14-12-2021
Abstract: Vat photopolymerization‐based 3D printing techniques have been widely used to produce high‐resolution 3D thermosetting materials. However, the lack of repairability of these thermosets leads to the production of waste. In this study, reversible addition fragmentation chain transfer (RAFT) agents are incorporated into resin formulations to allow visible light (405 nm) mediated 3D printing of materials with self‐healing capabilities. The self‐healing process is based on the reactivation of RAFT agent embedded in the thermosets under UV light (365 nm), which enables reformation of the polymeric network. The self‐healing process can be performed at room temperature without prior deoxygenation. The impact of the type and concentration of RAFT agents in the polymer network on the healing efficiency is explored. Resins containing RAFT agents enable 3D printing of thermosets with self‐healing properties, broadening the scope of future applications for polymeric thermosets in various fields.
Sustained A1 Adenosine Receptor Antagonist Drug Release from Nanoparticles Functionalized by a Neural Tracing Protein
Publisher: American Chemical Society (ACS)
Date: 21-10-2021
DOI: 10.1021/ACSCHEMNEURO.1C00538
Abstract: Respiratory dysfunction is a major cause of death in people with spinal cord injury (SCI). A remaining unsolved problem in treating SCI is the intolerable side effects of the drugs to patients. In a significant departure from conventional targeted nanotherapeutics to overcome the blood-brain barrier (BBB), this work pursues a drug-delivery approach that uses neural tracing retrograde transport proteins to bypass the BBB and deliver an adenosine A1 receptor antagonist drug, 1,3-dipropyl-8-cyclopentyl xanthine, exclusively to the respiratory motoneurons in the spinal cord and the brainstem. A single intradiaphragmatic injection at one thousandth of the native drug dosage induces prolonged respiratory recovery in a hemisection animal model. To translate the discovery into new treatments for respiratory dysfunction, we carry out this study to characterize the purity and quality of synthesis, stability, and drug-release properties of the neural tracing protein (wheat germ agglutinin chemically conjugated to horseradish peroxidase)-coupled nanoconjugate. We show that the batch-to-batch particle size and drug dosage variations are less than 10%. We evaluate the nanoconjugate size against the spatial constraints imposed by transsynaptic transport from pre to postsynaptic neurons. We determine that the nanoconjugate formulation is capable of sustained drug release lasting for days at physiologic pH, a prerequisite for long-distance transport of the drug from the diaphragm muscle to the brainstem. We model the drug-release profiles using a first-order reaction model and the Noyes-Whitney diffusion model. We confirm via biological electron microscopy that the nanoconjugate particles do not accumulate in the tissues at the injection site. We define the nanoconjugate storage conditions after monitoring the solution dispersion stability under various conditions for 4 months. This study supports further development of neural tracing protein-enabled nanotherapeutics for treating respiratory problems associated with SCI.
Effect of hydrophilic groups on the bioactivity of antimicrobial polymers
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1PY01075A
Abstract: Antimicrobial polymers have recently been investigated as potential treatments to combat multidrug-resistant pathogens.
Photo‐Enhanced Antimicrobial Activity of Polymers Containing an Embedded Photosensitiser
Publisher: Wiley
Date: 04-10-2021
Abstract: This work presents the synthesis of a novel photosensitive acrylate monomer for use as both a self‐catalyst in the photoinduced electron/energy transfer–reversible addition fragmentation chain transfer (PET‐RAFT) polymerisation process and a photosensitiser (PS) for antibacterial applications. Hydrophilic, cationic, and antimicrobial formulations are explored to compare the antibacterial effects between charged and non‐charged polymers. Covalent attachment of the catalyst to well‐defined linear polymer chains has no effect on polymerisation control or singlet oxygen generation. The addition of the PS to polymers provides activity against S. aureus for all polymer formulations, resulting in up to a 99.99999 % killing efficacy in 30 min. Antimicrobial peptide mimetic polymers previously active against P. aeruginosa , but not S. aureus , gain significant bactericidal activity against S. aureus through the inclusion of PS groups, with 99.998 % killing efficiency after 30 min incubation with light. Thus, a broader spectrum of antimicrobial activity is achieved using two distinct mechanisms of bactericidal activity via the incorporation of a photosensitiser monomer into an antimicrobial polymer.
RAFT-mediated, visible light-initiated single unit monomer insertion and its application in the synthesis of sequence-defined polymers
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C7PY00713B
Abstract: In this communication, we report a catalyst-free methodology for single unit monomer insertion (SUMI) into reversible addition–fragmentation chain transfer (RAFT) agents initiated by low intensity visible light.
3D Printed Solid Polymer Electrolytes with Bicontinuous Nanoscopic Domains for Ionic Liquid Conduction and Energy Storage
Publisher: Wiley
Date: 03-02-2023
Abstract: Solid polymer electrolytes (SPEs) offer several advantages compared to their liquid counterparts, and much research has focused on developing SPEs with enhanced mechanical properties while maintaining high ionic conductivities. The recently developed polymerization‐induced microphase separation (PIMS) technique offers a straightforward pathway to fabricate bicontinuous nanostructured materials in which the mechanical properties and conductivity can be independently tuned. In this work SPEs with tunable mechanical properties and conductivities are prepared via digital light processing 3D printing, exploiting the PIMS process to achieve nanostructured ion‐conducting materials for energy storage applications. A rigid crosslinked poly(isobornyl acrylate‐ stat ‐trimethylpropane triacrylate) scaffold provided materials with room temperature shear modulus above 400 MPa, while soft poly(oligoethylene glycol methyl ether acrylate) domains containing the ionic liquid 1‐butyl‐3‐methylimidazolium bis‐(trifluoromethyl sulfonyl)imide endowed the material with ionic conductivity up to 1.2 mS cm −1 at 30 °C. These features make the 3D‐printed SPE very competitive for applications in all solid energy storage devices, including supercapacitors.
Dual Role of Doxorubicin for Photopolymerization and Therapy
Publisher: American Chemical Society (ACS)
Date: 29-07-2020
Divergent Synthesis of Graft and Branched Copolymers through Spatially Controlled Photopolymerization in Flow Reactors
Publisher: American Chemical Society (ACS)
Date: 17-03-2021
Towards Sequence‐Controlled Antimicrobial Polymers: Effect of Polymer Block Order on Antimicrobial Activity
Publisher: Wiley
Date: 15-03-2018
Abstract: Synthetic polymers have shown promise in combating multidrug‐resistant bacteria. However, the biological effects of sequence control in synthetic antimicrobial polymers are currently not well understood. As such, we investigate the antimicrobial effects of monomer distribution within linear high‐order quasi‐block copolymers consisting of aminoethyl, phenylethyl, and hydroxyethyl acrylamides made in a one‐pot synthesis approach via photoinduced electron transfer–reversible addition–fragmentation chain transfer polymerisation (PET‐RAFT). Through different combinations of monomer olymer block order, antimicrobial and haemolytic activities are tuneable in a manner comparable to antimicrobial peptides.
Application of oxygen tolerant PET-RAFT to polymerization-induced self-assembly
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C7PY00442G
Abstract: The inhibitory effects of molecular oxygen in PET-RAFT polymerization can be overcome by the addition of singlet oxygen quenchers. This oxygen tolerant approach is compatible with a range of organic solvents and can be used to synthesize nanoparticles according to a PISA process.
Design of an Oxygen‐Tolerant Photo‐RAFT System for Protein‐Polymer Conjugation Achieving High Bioactivity
Publisher: Wiley
Date: 27-09-2023
Fire-Resistant Flexible Polyurethane Foams via Nature-Inspired Chitosan-Expandable Graphite Coatings
Publisher: American Chemical Society (ACS)
Date: 08-07-2021
RAFT iniferter polymerization in miniemulsion using visible light
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C7PY00939A
Abstract: Methodology for the successful implementation of RAFT (4-cyano-4[(dodecylsulfanylthiocarbonyl)sulfanyl]pentanoic acid (CDTPA)) iniferter polymerization of butyl methacrylate in miniemulsion using visible light (green light λ max = 530 nm) has been developed.
Flow mediated metal-free PET-RAFT polymerisation for upscaled and consistent polymer production
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C9RE00014C
Abstract: A slug flow process has been utilised in conjunction with metal-free photopolymerisation to produce well-defined polymers with outstanding consistency.
Frontispiz: Synthesis of Discrete Oligomers by Sequential PET‐RAFT Single‐Unit Monomer Insertion
Publisher: Wiley
Date: 05-07-2017
Recent developments of hybrid piezo–triboelectric nanogenerators for flexible sensors and energy harvesters
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1NA00501D
Abstract: Hybrid piezo–triboelectric nanogenerators constitute a new class of self-powered systems that exploit the synergy of piezoelectric and triboelectric mechanisms to address the energy and power needs for portable and wearable electronic devices.
Effect of Cationic Groups on the Selectivity of Ternary Antimicrobial Polymers
Publisher: Wiley
Date: 02-08-2022
Abstract: Antimicrobial polymers (AMPs) have emerged as a promising approach to combat multidrug‐resistant pathogens. Developed from binary polymers, which contain cationic and hydrophobic groups, ternary polymers are enhanced by adding neutral hydrophilic monomers to improve their biocompatibility. Cationic groups have attracted significant attention owing to their pivotal role in AMPs. Although many studies have investigated the effect of cationic groups on antimicrobial activity of binary AMPs, there is a lack of comprehensive and systematic evaluation for ternary AMPs. Therefore, a library of 31 statistical hiphilic ternary polymers containing different cationic groups, including primary amine, guanidine, and sulfonium groups is prepared to investigate the impact of cationic groups on antimicrobial activity and biocompatibility. It is shown that the cationic balance appears to be a critical factor influencing polymers' antibacterial activity and selectivity. The results reveal that the polymers that have the ratio of the cationic groups ranging between 50% and 60%, coupled with a cationic/hydrophobic ratio in the range of [1.4–2] and an appropriate neutral hydrophilic/hydrophobic balance, exhibited the highest selectivity toward mammalian cells. This study elucidates a structure–property‐performance relationship for ternary AMPs, which contributes to the development of AMPs capable of selectively targeting gram‐negative pathogens.
Controlling Molecular Weight Distributions through Photoinduced Flow Polymerization
Publisher: American Chemical Society (ACS)
Date: 23-10-2017
A Versatile 3D and 4D Printing System through Photocontrolled RAFT Polymerization
Publisher: Wiley
Date: 09-12-2019
Abstract: Reversible addition-fragmentation chain-transfer (RAFT) polymerization is a valuable tool for synthesizing macromolecules with controlled topologies and erse chemical functionalities. However, the application of RAFT polymerization to additive-manufacturing processes has been prevented due to the slow polymerization rates of typical systems. In this work, we developed and optimized a rapid visible (green) light mediated RAFT polymerization process and applied it to an open-air 3D printing system. The reaction components are non-toxic, metal free and environmentally friendly, which tailors these systems toward biomaterial fabrication. The inclusion of RAFT agent in the photosensitive resin provided control over the mechanical properties of 3D printed materials and allowed these materials to be post-functionalized after 3D printing. Additionally, photoinduced spatiotemporal control of the network structure provided a one-pass approach to 4D printed materials. This RAFT-mediated 3D and 4D printing process should provide access to a range of new functional and stimuli-responsive materials.
Discrete and Stereospecific Oligomers Prepared by Sequential and Alternating Single Unit Monomer Insertion
Publisher: American Chemical Society (ACS)
Date: 19-09-2018
DOI: 10.1021/JACS.8B08386
Abstract: Natural biopolymers, such as DNA and proteins, have uniform microstructures with defined molecular weight, precise monomer sequence, and stereoregularity along the polymer main chain that affords them unique biological functions. To reproduce such structurally perfect polymers and understand the mechanism of specific functions through chemical approaches, researchers have proposed using synthetic polymers as an alternative due to their broad chemical ersity and relatively simple manipulation. Herein, we report a new methodology to prepare sequence-controlled and stereospecific oligomers using alternating radical chain growth and sequential photoinduced RAFT single unit monomer insertion (photo-RAFT SUMI). Two families of cyclic monomers, the indenes and the N-substituted maleimides, can be alternatively inserted into RAFT agents, one unit at a time, allowing the monomer sequence to be controlled through sequential and alternating monomer addition. Importantly, the stereochemistry of cyclic monomer insertion into the RAFT agents is found to be trans-selective along the main chains due to steric hindrance from the repeating monomer units. All investigated cyclic monomers provide such trans-selectivity, but analogous acyclic monomers give a mixed cis- and trans-insertion.
Copolymers with Controlled Molecular Weight Distributions and Compositional Gradients through Flow Polymerization
Publisher: American Chemical Society (ACS)
Date: 07-06-2018
High-Throughput Synthesis of Antimicrobial Copolymers and Rapid Evaluation of Their Bioactivity
Publisher: American Chemical Society (ACS)
Date: 17-05-2019
An aqueous photo-controlled polymerization under NIR wavelengths: synthesis of polymeric nanoparticles through thick barriers
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2SC03952D
Abstract: Taking advantage of high penetration and reduced light scattering of NIR wavelengths, we demonstrate the syntheses of polymeric nanoparticles with consistent morphologies through thick barriers.
Near‐Infrared Light‐Induced Reversible Deactivation Radical Polymerization: Expanding Frontiers in Photopolymerization
Publisher: Wiley
Date: 26-09-2023
Effect of Thiocarbonylthio Compounds on Visible-Light-Mediated 3D Printing
Publisher: American Chemical Society (ACS)
Date: 29-01-2021
More than skin deep: using polymers to facilitate topical delivery of nitric oxide
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D0BM01197E
Abstract: Polymers can facilitate delivery of nitric oxide, improving stability and control of release for effective treatment of common skin disorders.
Strategies for Achieving Oxygen Tolerance in Reversible Addition–Fragmentation Chain Transfer Polymerization
Publisher: Wiley
Date: 26-07-2023
Abstract: Reversible addition–fragmentation chain transfer polymerization (RAFT) is a popular method for the synthesis of well‐defined macromolecules, but its sensitivity to oxygen is a major limitation for many industrial applications. Recent research has focused on developing strategies to confer oxygen tolerance onto RAFT polymerization, eliminating the need for deoxygenation steps and allowing for simpler reaction conditions. This minireview highlights several promising approaches to achieve oxygen tolerance in RAFT polymerization, including enzyme‐mediated, alkylborane‐initiated, and photomediated methods. The potential applications of oxygen‐tolerant RAFT polymerization are also discussed, demonstrating the promise for significant advances in large‐scale industrial polymer synthesis.
Enhancing the triboelectricity of stretchable electrospun piezoelectric polyvinylidene fluoride/boron nitride nanosheets composite nanofibers
Publisher: Elsevier BV
Date: 12-2020
Designing Nanostructured 3D Printed Materials by Controlling Macromolecular Architecture
Publisher: Wiley
Date: 18-07-2022
Abstract: Nanostructured polymeric materials play important roles in many advanced applications, however, controlling the morphologies of polymeric thermosets remains a challenge. This work uses multi‐arm macroCTAs to mediate polymerization‐induced microphase separation (PIMS) and prepare nanostructured materials via photoinduced 3D printing. The characteristic length scale of microphase‐separated domains is determined by the macroCTA arm length, while nanoscale morphologies are controlled by the macroCTA architecture. Specifically, using 2‐ and 4‐ arm macroCTAs provides materials with different morphologies compared to analogous monofunctional linear macroCTAs at similar compositions. The mechanical properties of these nanostructured thermosets can also be tuned while maintaining the desired morphologies. Using multi‐arm macroCTAs can thus broaden the scope of accessible nanostructures for extended applications, including the fabrication of actuators and potential drug delivery devices.
Photoinduced Oxygen Reduction for Dark Polymerization
Publisher: American Chemical Society (ACS)
Date: 24-02-2017
S-Nitrosothiol Plasma-Modified Surfaces for the Prevention of Bacterial Biofilm Formation
Publisher: American Chemical Society (ACS)
Date: 25-09-2019
Polymerization Induced Microphase Separation of ABC Triblock Copolymers for 3D Printing Nanostructured Materials
Publisher: Wiley
Date: 03-09-2023
Well-Defined Polymers for Nonchemistry Laboratories using Oxygen Tolerant Controlled Radical Polymerization
Publisher: American Chemical Society (ACS)
Date: 02-01-2020
Rapid Oxygen Tolerant Aqueous RAFT Photopolymerization in Continuous Flow Reactors
Publisher: American Chemical Society (ACS)
Date: 07-02-2019
Manganese-Based Magnetic Layered Double Hydroxide Nanoparticle: A pH-Sensitive and Concurrently Enhanced T1/T2-Weighted Dual-Mode Magnetic Resonance Imaging Contras
Publisher: American Chemical Society (ACS)
Date: 25-03-2019
Synthesis of Light-Responsive Pyrene-Based Polymer Nanoparticles via Polymerization-Induced Self-Assembly.
Publisher: Wiley
Date: 03-09-2019
Abstract: The use of an in situ, one-pot polymerization-induced self-assembly method to synthesize light-responsive pyrene-containing nanoparticles is reported. The strategy is based on the chain extension of a hydrophilic macromolecular chain transfer agent, poly(oligo(ethylene glycol) methyl ether methacrylate), using a light-responsive monomer, 1-pyrenemethyl methacrylate (PyMA), via a reversible addition-fragmentation chain transfer dispersion polymerization yielding nanoparticles of various morphologies (spherical micelles and worm-like micelles). In this process, addition of comonomers, such as butyl methacrylate (BuMA) or methyl methacrylate (MMA), are required to obtain high PyMA monomer conversion (>80% in 24 h). The addition of comonomers reduces the π-π stacking of the pyrene moieties, which facilitates the diffusion of monomers in the nanoparticle core. The addition of BuMA (as a comonomer) offers P(PyMA-co-BuMA) core-forming chains with high mobility that enables the reorganization of chains and then the evolution of morphology to form vesicles. In contrast, when MMA comonomer is used, kinetically trapped spheres are obtained this is due to the low mobility of the core-forming chains inhibiting in situ morphological evolution. Finally, the UV-light-induced dissociation of these light-responsive nanoparticles due to the gradual cleavage of the pyrene moieties and the subsequent hydrophobic-to-hydrophilic transitions of the core-forming blocks is demonstrated.
Porphyrinic Zirconium Metal–Organic Frameworks (MOFs) as Heterogeneous Photocatalysts for PET-RAFT Polymerization and Stereolithography
Publisher: Wiley
Date: 15-01-2021
Abstract: In this study, porphyrinic zirconium (Zr) MOFs were investigated as heterogeneous photocatalysts for photoinduced electron transfer‐reversible addition‐fragmentation chain transfer (PET‐RAFT) polymerization of various monomers under a broad range of wavelengths, producing polymers with high monomer conversions, narrow molecular weight distributions, low dispersity and good chain‐end fidelity. Screening of various porphyrinic Zr‐MOFs (Zn) containing Zn‐metalled porphyrinic ligands demonstrated that MOF‐525 (Zn) with the smallest size had the best photocatalytic activity in PET‐RAFT polymerization, due to enhanced dispersion and light penetration. Oxygen tolerance and temporal control were also demonstrated during MOF catalysed PET‐RAFT. Results suggested that the polymerization rates were significantly affected by changing the size and surface area of MOFs, and the heterogeneous MOF photocatalysts could be easily separated and recycled for up to five independent PET‐RAFT polymerizations without an obvious decrease in efficiency. Finally, the MOF photocatalysts were utilized to create three‐dimensional polymeric objects with high resolution via visible light mediated stereolithography in an open‐air environment.
How Do Reaction and Reactor Conditions Affect Photoinduced Electron/Energy Transfer Reversible Addition–Fragmentation Transfer Polymerization?
Publisher: American Chemical Society (ACS)
Date: 13-03-2018
Synthesis of polymeric nano-objects of various morphologies based on block copolymer self-assembly using microporous membranes
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C7RE00032D
Abstract: Polymeric nano-objects of a range of morphologies have been prepared using a novel approach based on the use of microporous membranes for mixing of a solvent (containing a diblock copolymer) and a non-solvent.
Oxygen tolerant photopolymerization for ultralow volumes
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C7PY00007C
Abstract: A benchtop approach is developed for the synthesis of various polymeric architectures using an aqueous Reversible Addition–Fragmentation chain Transfer (RAFT) photopolymerization technique.
Exploiting NIR Light-Mediated Surface-Initiated PhotoRAFT Polymerization for Orthogonal Control Polymer Brushes and Facile Postmodification of Complex Architecture through Opaque Barriers
Publisher: American Chemical Society (ACS)
Date: 22-09-2023
Copper-Doped Metal-Organic Frameworks for the Controlled Generation of Nitric Oxide from Endogenous S-nitrosothiols
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D0TB02709J
Abstract: We report the synthesis of a catalyst, copper-doped zeolitic imidazolate framework ZIF-8, that generates nitric oxide from naturally occurring endogenous nitric oxide donors, S -nitrosoglutathione and S -nitrosocysteine.
A Versatile 3D and 4D Printing System through Photocontrolled RAFT Polymerization
Publisher: Wiley
Date: 15-11-2019
Screening RAFT agents and photocatalysts to mediate PET-RAFT polymerization using a high throughput approach
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1PY01258D
Abstract: We report a high throughput approach for the screening of RAFT agents and photocatalysts to mediate photoinduced electron/energy transfer-reversible addition–fragmentation chain transfer (PET-RAFT) polymerization.
Nitric Oxide-Loaded Antimicrobial Polymer for the Synergistic Eradication of Bacterial Biofilm
Publisher: American Chemical Society (ACS)
Date: 04-05-2018
Nanostructure Control in 3D Printed Materials
Publisher: Wiley
Date: 06-12-2022
Abstract: Currently, there are no straightforward methods to 3D print materials with nanoscale control over morphological and functional properties. Here, a novel approach for the fabrication of materials with controlled nanoscale morphologies using a rapid and commercially available Digital Light Processing 3D printing technique is demonstrated. This process exploits reversible deactivation radical polymerization to control the in‐situ‐polymerization‐induced microphase separation of 3D printing resins, which provides materials with complex architectures controllable from the macro‐ to nanoscale, resulting in the preparation of materials with enhanced mechanical properties. This method does not require specialized equipment or process conditions and thus represents an important development in the production of advanced materials via additive manufacturing.
Particle Size Control in Miniemulsion Polymerization via Membrane Emulsification
Publisher: American Chemical Society (ACS)
Date: 12-06-2019
Chlorophyll a crude extract: efficient photo-degradable photocatalyst for PET-RAFT polymerization
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C7CC07663K
Abstract: This work demonstrates use of spinach extracts for living radical polymerization bypassing catalyst synthesis urification, degassing and catalyst removal procedures.
Antibiofilm Nitric Oxide-Releasing Polydopamine Coatings
Publisher: American Chemical Society (ACS)
Date: 28-01-2019
Abstract: The growing number of patient morbidity related to nosocomial infections has placed an importance on the development of new antibacterial coatings for medical devices. Here, we utilize the versatile adhesion property of polydopamine (pDA) to design an antibacterial coating that possesses low-fouling and nitric oxide (NO)-releasing capabilities. To demonstrate this, glass substrates were functionalized with pDA via immersion in alkaline aqueous solution containing dopamine, followed by grafting of low-fouling polymer (poly(ethylene glycol) (PEG)) via Michael addition and subsequent formation of N-diazeniumdiolate functionalities (NO precursors) by purging with NO gas. X-ray photoelectron spectroscopy confirmed the successful grafting of PEG and formation of N-diazeniumdiolate on polydopamine-coated substrates. NO release from the coating was observed over 2 days, and NO loading is tunable by the pDA film thickness. The antibacterial efficiency of the coatings was assessed using Gram-negative Pseudomonas aeruginosa (i.e., wild-type PAO1 and multidrug-resistant PA37) and Gram-positive Staphylococcus aureus (ATCC 29213). The NO-releasing PEGylated pDA film inhibited biofilm attachment by 96 and 70% after exposure to bacterial culture solution for 24 and 36 h, respectively. In contrast, films that do not contain NO failed to prevent biofilm formation on the surfaces at these time points. Furthermore, this coating also showed 99.9, 97, and 99% killing efficiencies against surface-attached PAO1, PA37, and S. aureus bacteria. Overall, the combination of low-fouling PEG and antibacterial activity of NO in pDA films makes this coating a potential therapeutic option to inhibit biofilm formation on medical devices.
Guiding the Design of Organic Photocatalyst for PET-RAFT Polymerization: Halogenated Xanthene Dyes
Publisher: American Chemical Society (ACS)
Date: 20-12-2018
Releasable antimicrobial polymer-silk coatings for combating multidrug-resistant bacteria
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1PY01219C
Abstract: Controlled release of synthetic cationic antimicrobial polymers from silk-based coating for preventing bacterial biofilm formation on the surface and for killing planktonic bacteria cells.
A Process for Well-Defined Polymer Synthesis through Textile Dyeing Inspired Catalyst Immobilization
Publisher: American Chemical Society (ACS)
Date: 17-09-2018
Bioactive Synthetic Polymers
Publisher: Wiley
Date: 05-10-2021
Abstract: Synthetic polymers are omnipresent in society as textiles and packaging materials, in construction and medicine, among many other important applications. Alternatively, natural polymers play a crucial role in sustaining life and allowing organisms to adapt to their environments by performing key biological functions such as molecular recognition and transmission of genetic information. In general, the synthetic and natural polymer worlds are completely separated due to the inability for synthetic polymers to perform specific biological functions in some cases, synthetic polymers cause uncontrolled and unwanted biological responses. However, owing to the advancement of synthetic polymerization techniques in recent years, new synthetic polymers have emerged that provide specific biological functions such as targeted molecular recognition of peptides, or present antiviral, anticancer, and antimicrobial activities. In this review, the emergence of this generation of bioactive synthetic polymers and their bioapplications are summarized. Finally, the future opportunities in this area are discussed.
A synthetic peptide mimic killsCandida albicansand synergistically prevents infection
Publisher: Cold Spring Harbor Laboratory
Date: 25-09-2023
Living Additive Manufacturing
Publisher: American Chemical Society (ACS)
Date: 30-01-2017
Porphyrinic Zirconium Metal–Organic Frameworks (MOFs) as Heterogeneous Photocatalysts for PET‐RAFT Polymerization and Stereolithography
Publisher: Wiley
Date: 20-01-2021
Abstract: In this study, porphyrinic zirconium (Zr) MOFs were investigated as heterogeneous photocatalysts for photoinduced electron transfer‐reversible addition‐fragmentation chain transfer (PET‐RAFT) polymerization of various monomers under a broad range of wavelengths, producing polymers with high monomer conversions, narrow molecular weight distributions, low dispersity and good chain‐end fidelity. Screening of various porphyrinic Zr‐MOFs (Zn) containing Zn‐metalled porphyrinic ligands demonstrated that MOF‐525 (Zn) with the smallest size had the best photocatalytic activity in PET‐RAFT polymerization, due to enhanced dispersion and light penetration. Oxygen tolerance and temporal control were also demonstrated during MOF catalysed PET‐RAFT. Results suggested that the polymerization rates were significantly affected by changing the size and surface area of MOFs, and the heterogeneous MOF photocatalysts could be easily separated and recycled for up to five independent PET‐RAFT polymerizations without an obvious decrease in efficiency. Finally, the MOF photocatalysts were utilized to create three‐dimensional polymeric objects with high resolution via visible light mediated stereolithography in an open‐air environment.
The Emergence of Reversible–Deactivation Radical Polymerization in 3D Printing
Publisher: Wiley
Date: 18-09-2023
Abstract: The majority of materials 3D printed using vat photopolymerization techniques are prepared by uncontrolled polymerization methods and cannot be easily modified to introduce additional functionality these materials can be considered as effectively “dead” materials. Fortunately, a suite of photocontrolled reversible–deactivation radical polymerization (photoRDRP) techniques is recently implemented in 3D printing. In addition to their fast polymerization rate and oxygen tolerance, the high livingness imparted by photoRDRP methods is beginning to disrupt the field of 3D printing by providing access to materials with advanced properties, including on‐demand editing of surface and bulk properties, self‐healing, and control over nanostructuration and mechanical properties. This mini‐review analyzes the development of photoRDRP techniques in the field of photoinduced 3D printing with an emphasis on the advanced and highly tailorable materials possible through these techniques.
Large Hexosomes from Emulsion Droplets: Particle Shape and Mesostructure Control
Publisher: American Chemical Society (ACS)
Date: 15-10-2018
DOI: 10.1021/ACS.LANGMUIR.8B02638
Abstract: Soft, rotationally symmetric particles of dispersed hexagonal liquid crystalline phase are produced using a method previously developed for cubosome microparticle production. The technique forms hexosome particles via removal of ethanol from emulsion droplets containing monoolein, water, and one of the various hydrophobic molecules: vitamin E, hexadecane, oleic acid, cyclohexane, or inylbenzene. The unique rotational symmetry of the particles is characterized by optical microscopy and small-angle X-ray scattering to link particle phase, shape, and structure to composition. Rheology of the soft particles can be varied independently of shape, enabling control of transport, deformation, and biological response by controlling composition and molecular structure of the additives. The direct observations of formation, and the resultant hexosome shapes, link the particle-scale and mesoscale properties of these novel self-assembled particles and broaden their applications. The micron-scale hexosomes provide a route to understanding the effects of particle size, crystallization rate, and rheology on the production of soft particles with liquid crystalline structure and unique shape and symmetry.
PNIPAM-immobilized gold-nanoparticles with colorimetric temperature-sensing and reusable temperature-switchable catalysis properties
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1PY01180D
Abstract: The temperature-responsive core–shell hybrid nanoparticles PNIPAMs-AuNP have dual-functional applications as colorimetric temperature-sensors and reusable temperature-switchable catalysts.
Antibiofilm Platform based on the Combination of Antimicrobial Polymers and Essential Oils
Publisher: American Chemical Society (ACS)
Date: 28-10-2020
DOI: 10.1021/ACS.BIOMAC.9B01278
Abstract: The development of potent strategies to counter microbial biofilm is an urgent priority in healthcare. The majority of bacterial infections in humans are biofilm related, however, effective treatments are still lacking especially for combating multidrug-resistant (MDR) strains. Herein, we report an effective antibiofilm platform based on the use of synthetic antimicrobial polymers in combination with essential oils, where the antimicrobial polymers play a secondary role as delivery vehicle for essential oils. Two ternary antimicrobial polymers consisting of cationic primary amines, low-fouling oligo(ethylene glycol) and hydrophobic ethylhexyl groups were synthesized in the form of random and block copolymers, and mixed with either carvacrol or eugenol. Coadministration of these compounds improved the efficacy against
Versatile oligomers and polymers from flavonoids-a new approach to synthesis
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C7PY00325K
Abstract: Antioxidant oligomers and polymers have been prepared from two flavonoids, catechin and quercetin, using a new facile technique.
Silk Sponges with Surface Antimicrobial Activity
Publisher: American Chemical Society (ACS)
Date: 16-12-2021
3D printing of polymeric materials based on photo-RAFT polymerization
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/C9PY01419E
Abstract: For the first time, we report 3D printing of RAFT-based formulations to fabricate functional objects in a layer-by-layer fashion.
Design of Antimicrobial Polymers
Publisher: Wiley
Date: 09-2022
Abstract: Antibiotic resistance has become a critical issue, alarming the healthcare and agriculture sectors worldwide. Thanks to rapid advancements in polymer science, antimicrobial polymers (AMPs) have been developed as a mimic version of host‐defense peptides (a part of natural immune systems of multicellular organisms) to mitigate antibiotic resistance. By exploiting advanced polymerization techniques, polymer structures are easily manipulated in a well‐defined controlled manner, enabling precise and accurate evaluation of the structure–activity relationship. Recent years have witnessed the blossoming of antimicrobial polymer development. This review provides comprehensive insight into antimicrobial polymers from concept to structure design, to biofunction control. Along with the optimization of intrinsic factors, including compositional and topological features, external factors like induced conformation upon exposure to specific targeting pathogens should be considered in AMP design and optimization. Furthermore, the new design approaches of smart response platforms (or bacterial‐induced triggering systems) and targeting specific administration dosage forms for specific pathogens are also discussed as prospective strategies to address the remaining challenge of toxicity while maintaining or even enhancing antimicrobial potency.
Rational Design of Single-Chain Polymeric Nanoparticles That Kill Planktonic and Biofilm Bacteria
Publisher: American Chemical Society (ACS)
Date: 08-02-2017
DOI: 10.1021/ACSINFECDIS.6B00203
Abstract: Infections caused by multidrug-resistant bacteria are on the rise and, therefore, new antimicrobial agents are required to prevent the onset of a postantibiotic era. In this study, we develop new antimicrobial compounds in the form of single-chain polymeric nanoparticles (SCPNs) that exhibit excellent antimicrobial activity against Gram-negative bacteria (e.g., Pseudomonas aeruginosa) at micromolar concentrations (e.g., 1.4 μM) and remarkably kill ≥99.99% of both planktonic cells and biofilm within an hour. Linear random copolymers, which comprise oligoethylene glycol (OEG), hydrophobic, and amine groups, undergo self-folding in aqueous systems due to intramolecular hydrophobic interactions to yield these SCPNs. By systematically varying the hydrophobicity of the polymer, we can tune the extent of cell membrane wall disruption, which in turn governs the antimicrobial activity and rate of resistance acquisition in bacteria. We also show that the incorporation of OEG groups into the polymer design is essential in preventing complexation with proteins in biological medium, thereby maintaining the antimicrobial efficacy of the compound even in in vivo mimicking conditions. In comparison to the last-resort antibiotic colistin, our lead agents have a higher therapeutic index (by ca. 2-3 times) and hence better biocompatibility. We believe that the SCPNs developed here have potential for clinical applications and the information pertaining to their structure-activity relationship will be valuable toward the general design of synthetic antimicrobial (macro)molecules.
Synthetic copolymer conjugates of docetaxel andin vitroassessment of anticancer efficacy
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0NJ03425H
Abstract: Docetaxel (DTX) is a widely used chemotherapy drug that is associated with numerous side effects and limited bioavailability. We show synthetic copolymer conjugates of docetaxel with drug loading up to 20% and assess their efficacy in MCF-7 cells.
Photo‐RAFT Polymerization for Hydrogel Synthesis through Barriers and Development of Light‐Regulated Healable Hydrogels under NIR Irradiation
Publisher: Wiley
Date: 27-04-2023
NIR/blue light emission optimization of NaY1−(x+y)YbxF4:Tmy upconversion nanoparticles via Yb3+/Tm3+ dopant balancing
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C7DT04768A
Abstract: A data driven approach provides better understanding of the role of dopant balancing in the upconversion process and presents an effective strategy to enhance the optical properties of upconversion nanoparticles.
Miniemulsion photopolymerization in a continuous tubular reactor: particle size controlviamembrane emulsification
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0PY00654H
Abstract: Synthesis of polymeric nanoparticles of adjustable size in the submicron-range 200–950 nm has been conducted via membrane emulsification combined with photoinduced miniemulsion polymerization in a continuous tubular flow reactor.
Computer-Guided Discovery of a pH-Responsive Organic Photocatalyst and Application for pH and Light Dual-Gated Polymerization
Publisher: American Chemical Society (ACS)
Date: 22-04-2019
DOI: 10.1021/JACS.9B01096
Abstract: In this work, we adopted a fully computer-guided strategy in discovering an efficient pH-switchable organic photocatalyst (OPC), unprecedentedly turning colorless at pH 5 and recovering strong visible-light absorption and photoactivity at pH 7. This is the first ex le of an OPC design fully guided by comprehensive density functional theory (DFT) studies covering electrostatic, electrochemical, and photophysical predictions. Characterization of the designed OPC after synthesis confirmed the computational predictions. We applied this OPC to mediate an aqueous photoinduced electron/energy transfer-reversible addition-fragmentation chain transfer (PET-RAFT) polymerization under green LED light (nominal emission wavelength: 530 nm, 5 mW/cm
Synergy between Synthetic Antimicrobial Polymer and Antibiotics: A Promising Platform To Combat Multidrug-Resistant Bacteria
Publisher: American Chemical Society (ACS)
Date: 02-04-2019
DOI: 10.1021/ACSINFECDIS.9B00049
Abstract: The failure of many antibiotics in the treatment of chronic infections caused by multidrug-resistant (MDR) bacteria necessitates the development of effective strategies to combat this global healthcare issue. Here, we report an antimicrobial platform based on the synergistic action between commercially available antibiotics and a potent synthetic antimicrobial polymer that consists of three key functionalities: low-fouling oligoethylene glycol, hydrophobic ethylhexyl, and cationic primary amine groups. Checkerboard assays with
2D Porphyrinic Metal–Organic Framework Nanosheets as Multidimensional Photocatalysts for Functional Materials
Publisher: Wiley
Date: 14-09-2021
Abstract: Ultrathin porphyrinic 2D MOFs, ZnTCPP nanosheets (TCPP: 5,10,15,20‐(tetra‐4‐carboxyphenyl) porphyrin) were employed as heterogeneous photocatalysts to activate PET‐RAFT polymerization under various wavelengths ranging from violet to orange light. High polymerization rates, oxygen tolerance, and precise temporal control were achieved. The polymers showed narrow molecular weight distributions and good chain‐end fidelity. The 2D ZnTCPP nanosheets were applied as photocatalysts in stereolithographic 3D printing in an open‐air environment under blue light to yield well‐defined 3D printed objects. Apart from providing an efficient catalytic system, 2D ZnTCPP nanosheets reinforced the mechanical properties of the 3D printed materials. The presence of ZnTCPP embedded in the materials conferred effective antimicrobial activity under visible light by production of singlet oxygen, affording 98 % and 93 % anti‐bacterial efficiency against Gram‐positive and Gram‐negative bacteria, respectively.
Effect of Macromolecular Structure on Phase Separation Regime in 3D Printed Materials
Publisher: Wiley
Date: 19-06-2023
Abstract: In this study, the fabrication of 3D‐printed polymer materials with controlled phase separation using polymerization induced microphase separation (PIMS) via photoinduced 3D printing is demonstrated. While many parameters affecting the nanostructuration in PIMS processes are extensively investigated, the influence of the chain transfer agent (CTA) end group, i.e., Z‐group, of macromolecular chain transfer agent (macroCTA) remains unclear as previous research has exclusively employed trithiocarbonate as the CTA end group. Herein, the effect of macroCTAs containing four different Z‐groups on the formation of nanostructure of 3D printed materials is explored. The results show that the different Z‐groups lead to distinct network formation and phase separation behaviors between the resins, influencing both the 3D printing process and the resulting material properties. Specifically, less reactive macroCTAs toward acrylic radical addition, such as O ‐alkyl xanthate and N ‐alkyl‐ N ‐aryl dithiocarbamate, result in translucent and brittle materials with macrophase separation morphology. In contrast, more reactive macroCTAs such as S ‐alkyl trithiocarbonate and 4‐chloro‐3,5‐dimethylpyrazo dithiocarbamate produce transparent and rigid materials with nano‐scale morphology. Findings of this study provide a novel approach to manipulate the nanostructure and properties of 3D printed PIMS materials, which can have important implications for materials science and engineering.
Effective Utilization of NIR Wavelengths for Photo‐Controlled Polymerization: Penetration Through Thick Barriers and Parallel Solar Syntheses
Publisher: Wiley
Date: 12-12-2019
Abstract: This contribution details an efficient and controlled photopolymerization regulated by far-red (λ=680 nm) and NIR (λ=780 and 850 nm) light in the presence of aluminium phthalocyanine and aluminium naphthalocyanine. Initiating radicals are generated by photosensitization of peroxides affording an effective strategy that provides controlled polymerization of a variety of monomers with excellent living characteristics. Critically, long wavelength irradiation provides penetration through thick barriers, affording unprecedented rates of controlled polymerization that can open new and exciting applications. Furthermore, a more optimized approach to performing solar syntheses is presented. By combining the narrow Q-bands of these photocatalysts with others possessing complementary absorptions, layered, independent polymerizations and organic transformations may be performed in parallel under a single broadband emission source, such as sunlight.
Reversible Deactivation Radical Polymerization: From Polymer Network Synthesis to 3D Printing
Publisher: Wiley
Date: 21-01-2021
Abstract: 3D printing has changed the fabrication of advanced materials as it can provide customized and on‐demand 3D networks. However, 3D printing of polymer materials with the capacity to be transformed after printing remains a great challenge for engineers, material, and polymer scientists. Radical polymerization has been conventionally used in photopolymerization‐based 3D printing, as in the broader context of crosslinked polymer networks. Although this reaction pathway has shown great promise, it offers limited control over chain growth, chain architecture, and thus the final properties of the polymer networks. More fundamentally, radical polymerization produces dead polymer chains incapable of postpolymerization transformations. Alternatively, the application of reversible deactivation radical polymerization (RDRP) to polymer networks allows the tuning of network homogeneity and more importantly, enables the production of advanced materials containing dormant reactivatable species that can be used for subsequent processes in a postsynthetic stage. Consequently, the opportunities that (photoactivated) RDRP‐based networks offer have been leveraged through the novel concepts of structurally tailored and engineered macromolecular gels, living additive manufacturing and photoexpandable/transformable‐polymer networks. Herein, the advantages of RDRP‐based networks over irreversibly formed conventional networks are discussed.
Designing Nanostructured 3D Printed Materials by Controlling Macromolecular Architecture
Publisher: Wiley
Date: 18-07-2022
Abstract: Nanostructured polymeric materials play important roles in many advanced applications, however, controlling the morphologies of polymeric thermosets remains a challenge. This work uses multi‐arm macroCTAs to mediate polymerization‐induced microphase separation (PIMS) and prepare nanostructured materials via photoinduced 3D printing. The characteristic length scale of microphase‐separated domains is determined by the macroCTA arm length, while nanoscale morphologies are controlled by the macroCTA architecture. Specifically, using 2‐ and 4‐ arm macroCTAs provides materials with different morphologies compared to analogous monofunctional linear macroCTAs at similar compositions. The mechanical properties of these nanostructured thermosets can also be tuned while maintaining the desired morphologies. Using multi‐arm macroCTAs can thus broaden the scope of accessible nanostructures for extended applications, including the fabrication of actuators and potential drug delivery devices.
Selective and Rapid Light-Induced RAFT Single Unit Monomer Insertion in Aqueous Solution
Publisher: Wiley
Date: 10-11-2020
Abstract: The photocatalyst Zn(II) meso-tetra(4-sulfonatophenyl)porphyrin (ZnTPPS) is found to substantially accelerate visible-light-initiated (red, yellow, green light) single unit monomer insertion (SUMI) of N,N-dimethylacrylamide into the reversible addition-fragmentation chain transfer (RAFT) agent, 4-((((2-carboxyethyl)thio)carbonothioyl)thio)-4-cyanopentanoic acid (RAFT
Polydopamine Shell as a Ga3+ Reservoir for Triggering Gallium–Indium Phase Separation in Eutectic Gallium–Indium Nanoalloys
Publisher: American Chemical Society (ACS)
Date: 06-10-2021
Unravelling an oxygen-mediated reductive quenching pathway for photopolymerisation under long wavelengths
Publisher: Springer Science and Business Media LLC
Date: 20-01-2021
DOI: 10.1038/S41467-020-20640-Z
Abstract: Photomediated-reversible-deactivation radical polymerisation (photo-RDRP) has a limited scope of available photocatalysts (PCs) due to multiple stringent requirements for PC properties, limiting options for performing efficient polymerisations under long wavelengths. Here we report an oxygen-mediated reductive quenching pathway (O-RQP) for photoinduced electron transfer reversible addition-fragmentation chain transfer (PET-RAFT) polymerisation. The highly efficient polymerisations that are performed in the presence of ambient air enable an expanded scope of available PCs covering a much-broadened absorption spectrum, where the oxygen tolerance of PET-RAFT allows high-quality polymerisation by preventing the existence of O 2 in large amounts and efficient O-RQP is permitted due to its requirement for only catalytic amounts of O 2 . Initially, four different porphyrin dyes are investigated for their ability to catalyse PET-RAFT polymerisation via an oxidative quenching pathway (OQP), reductive quenching pathway (RQP) and O-RQP. Thermodynamic studies with the aid of (time-dependent) density functional theory calculations in combination with experimental studies, enable the identification of the thermodynamic constraints within the OQP, RQP and O-RQP frameworks. This knowledge enables the identification of four phthalocyanine photocatalysts, that were previously thought to be inert for PET-RAFT, to be successfully used for photopolymerisations via O-RQP. Well-controlled polymerisations displaying excellent livingness are performed at wavelengths in the red to near-infrared regions. The existence of this third pathway O-RQP provides an attractive pathway to further expand the scope of photocatalysts compatible with the PET-RAFT process and facile access to photopolymerisations under long wavelengths.
Mediating Reaction Orthogonality in Polymer and Materials Science
Publisher: Wiley
Date: 17-09-2020
Abstract: Selective control of chemical reactions is critical for the proper regulation of processes ranging from intricate biological systems to large scale industrial manufacturing. The progression of synthetic chemistry toward the complexity seen in Nature requires increased control over many concurrent chemical reactions in a non‐interfering (orthogonal) fashion. Fortunately, the practically endless pool of synthetic chemical reactions developed to date can often be combined in an orthogonal manner to provide elegant solutions to complex chemical problems. In this review, we first highlight some of the many photochemical reactions that have been applied in orthogonal reaction protocols the highly selective nature of photochemical reactions makes them well‐suited for independent activation in the presence of other reaction components. The application of these orthogonal reactions, especially photochemical reactions, for the synthesis and modification of polymers and polymeric materials is also summarized. Importantly, the use of orthogonal chemical reactions can provide additional opportunities for synthesizing advanced and functional polymeric materials compared to traditional synthetic procedures.
An Oxygen Paradox
Publisher: Wiley
Date: 11-10-2019
Abstract: A peculiar radical polymerization reaction is presented in which oxygen serves as a cocatalyst, alongside triethylamine, to provide activation with light in the far-red (690 nm, 3 mW cm
Synthesis of Discrete Oligomers by Sequential PET‐RAFT Single‐Unit Monomer Insertion
Publisher: Wiley
Date: 07-12-2016
Abstract: Uniform synthetic polymers with precisely defined molar mass and monomer sequence (primary structure) have many potential high-value applications. However, a robust and versatile synthetic strategy for these materials remains one of the great challenges in polymer synthesis. Herein we describe proof-of-principle experiments for a modular strategy to produce discrete oligomers by a visible-light-mediated radical chain process. We utilize the high selectivity provided by photo-induced electron/energy transfer (PET) activation to develop efficient single unit monomer insertion (SUMI) into reversible addition-fragmentation chain-transfer (RAFT) agents. A variety of discrete oligomers (single unit species, dimers, and, for the first time, trimers) have been synthesized by sequential SUMI in very high yield under mild reaction conditions. The trimers were used as building blocks for the construction of uniform hexamers and graft copolymers with precisely defined branches.
High-Throughput Process for the Discovery of Antimicrobial Polymers and Their Upscaled Production via Flow Polymerization
Publisher: American Chemical Society (ACS)
Date: 16-01-2020
Photo-responsive supramolecular hyaluronic acid hydrogels for accelerated wound healing
Publisher: Elsevier BV
Date: 07-2020
Precise synthesis of poly(N-acryloyl amino acid) through photoinduced living polymerization
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8PY00366A
Abstract: A library of N -acryloylamino acid polymers with controlled molecular weights and narrow molecular weight distributions ( M w / M n 1.20) was created by a universal and versatile photoinduced living radical polymerization technique.
Oxygen Tolerant PET-RAFT Facilitated 3D Printing of Polymeric Materials under Visible LEDs
Publisher: American Chemical Society (ACS)
Date: 24-01-2020
Pushing the Limits of High Throughput PET-RAFT Polymerization
Publisher: American Chemical Society (ACS)
Date: 20-09-2018
An Oxygen Paradox: Catalytic Use of Oxygen in Radical Photopolymerization
Publisher: Wiley
Date: 11-10-2019
Polymers for Fluorescence Imaging of Formaldehyde in Living Systems via the Hantzsch Reaction
Publisher: American Chemical Society (ACS)
Date: 22-10-2018
The effects of polymer topology and chain length on the antimicrobial activity and hemocompatibility of amphiphilic ternary copolymers
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C7PY01069A
Abstract: Hyperbranched random copolymers that consist of ethylhexyl hydrophobic groups have the best selectivity compared to linear random and block copolymers.
Alcohol-based PISA in batch and flow: exploring the role of photoinitiators
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C9PY00166B
Abstract: Polymerization-induced self-assembly (PISA) via PhotoRAFT (photoinduced reversible addition–fragmentation radical transfer) was investigated in polar solvents via continuous flow reactors.
Towards Sequence-Controlled Antimicrobial Polymers: Effect of Polymer Block Order on Antimicrobial Activity
Publisher: Wiley
Date: 15-03-2018
Abstract: Synthetic polymers have shown promise in combating multidrug‐resistant bacteria. However, the biological effects of sequence control in synthetic antimicrobial polymers are currently not well understood. As such, we investigate the antimicrobial effects of monomer distribution within linear high‐order quasi‐block copolymers consisting of aminoethyl, phenylethyl, and hydroxyethyl acrylamides made in a one‐pot synthesis approach via photoinduced electron transfer–reversible addition–fragmentation chain transfer polymerisation (PET‐RAFT). Through different combinations of monomer olymer block order, antimicrobial and haemolytic activities are tuneable in a manner comparable to antimicrobial peptides.
A Comprehensive Platform for the Design and Synthesis of Polymer Molecular Weight Distributions
Publisher: American Chemical Society (ACS)
Date: 08-10-2020
Liquid Metal-Triggered Assembly of Phenolic Nanocoatings with Antioxidant and Antibacterial Properties
Publisher: American Chemical Society (ACS)
Date: 22-02-2021
Frontispiz: A Photoinduced Dual‐Wavelength Approach for 3D Printing and Self‐Healing of Thermosetting Materials
Publisher: Wiley
Date: 27-02-2022
Controlling mechanical properties of 3D printed polymer composites through photoinduced reversible addition–fragmentation chain transfer (RAFT) polymerization
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D1PY01283E
Abstract: Reversible addition–fragmentation chain-transfer (RAFT) polymerization has been exploited to design silica-nanoparticle-incorporated photocurable resins for 3D printing of materials with enhanced mechanical properties and complex structures.
Frontispiece: Synthesis of Discrete Oligomers by Sequential PET‐RAFT Single‐Unit Monomer Insertion
Publisher: Wiley
Date: 05-07-2217
Photo‐Enhanced Antimicrobial Activity of Polymers Containing an Embedded Photosensitiser
Publisher: Wiley
Date: 04-10-2021
Abstract: This work presents the synthesis of a novel photosensitive acrylate monomer for use as both a self‐catalyst in the photoinduced electron/energy transfer–reversible addition fragmentation chain transfer (PET‐RAFT) polymerisation process and a photosensitiser (PS) for antibacterial applications. Hydrophilic, cationic, and antimicrobial formulations are explored to compare the antibacterial effects between charged and non‐charged polymers. Covalent attachment of the catalyst to well‐defined linear polymer chains has no effect on polymerisation control or singlet oxygen generation. The addition of the PS to polymers provides activity against S. aureus for all polymer formulations, resulting in up to a 99.99999 % killing efficacy in 30 min. Antimicrobial peptide mimetic polymers previously active against P. aeruginosa , but not S. aureus , gain significant bactericidal activity against S. aureus through the inclusion of PS groups, with 99.998 % killing efficiency after 30 min incubation with light. Thus, a broader spectrum of antimicrobial activity is achieved using two distinct mechanisms of bactericidal activity via the incorporation of a photosensitiser monomer into an antimicrobial polymer.
A photocatalyst immobilized on fibrous and porous monolithic cellulose for heterogeneous catalysis of controlled radical polymerization
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C7PY01690E
Abstract: Fibrous and porous monolithic cellulose was employed to immobilize a photocatalyst for heterogeneously catalysing controlled radical polymerization, which provides superior catalyst recyclability.
2-(Methylthio)ethyl Methacrylate: A Versatile Monomer for Stimuli Responsiveness and Polymerization-Induced Self-Assembly in the Presence of Air
Publisher: American Chemical Society (ACS)
Date: 24-10-2017
PET-RAFT polymerisation: towards green and precision polymer manufacturing
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8CC02783H
Abstract: Photoinduced electron/energy transfer-reversible addition–fragmentation chain transfer (PET-RAFT) process has opened up a new way of precision polymer manufacturing to satisfy the concept of green chemistry.
A Photoinduced Dual‐Wavelength Approach for 3D Printing and Self‐Healing of Thermosetting Materials
Publisher: Wiley
Date: 14-12-2021
Abstract: Vat photopolymerization‐based 3D printing techniques have been widely used to produce high‐resolution 3D thermosetting materials. However, the lack of repairability of these thermosets leads to the production of waste. In this study, reversible addition fragmentation chain transfer (RAFT) agents are incorporated into resin formulations to allow visible light (405 nm) mediated 3D printing of materials with self‐healing capabilities. The self‐healing process is based on the reactivation of RAFT agent embedded in the thermosets under UV light (365 nm), which enables reformation of the polymeric network. The self‐healing process can be performed at room temperature without prior deoxygenation. The impact of the type and concentration of RAFT agents in the polymer network on the healing efficiency is explored. Resins containing RAFT agents enable 3D printing of thermosets with self‐healing properties, broadening the scope of future applications for polymeric thermosets in various fields.
Exploiting the Versatility of Polydopamine-Coated Nanoparticles to Deliver Nitric Oxide and Combat Bacterial Biofilm
Publisher: Wiley
Date: 28-05-2018
Abstract: In this study, an antimicrobial platform in the form of nitric oxide (NO) gas-releasing polydopamine (PDA)-coated iron oxide nanoparticles (IONPs) is developed for combating bacterial biofilms. NO is bound to the PDA-coated IONPs via the reaction between NO and the secondary amine moieties on PDA to form N-diazeniumdiolate (NONOate) functionality. To impart colloidal stability to the nanoparticles in aqueous solutions (e.g., phosphate buffered saline (PBS) and bacteria cell culture media M9), a polymer bearing hydrophilic and amine pendant groups, P(OEGMA)-b-P(ABA), is synthesized via reversible addition-fragmentation chain transfer (RAFT) polymerization and is subsequently grafted onto the PDA-coated IONPs by employing the Schiff base/Michael addition reaction between o-quinone and a primary amine. These nanoparticles are able to effectively disperse Pseudomonas aeruginosa biofilms (up to 79% dispersal) at submicromolar NO concentrations. In addition, the nanoparticles demonstrate excellent bactericidal activity toward P. aeruginosa planktonic and biofilm cells (up to 5-log
Insight into Bioactivity of In‐situ Trapped Enzyme‐Covalent‐Organic Frameworks
Publisher: Wiley
Date: 03-05-2023
Abstract: Selecting a suitable support material for enzyme immobilization with excellent biocatalytic activity and stability is a critical aspect in the development of functional biosystems. The highly stable and metal‐free properties of covalent‐organic frameworks (COFs) make them ideal supports for enzyme immobilization. Herein, we constructed three kinds of COFs via a biofriendly and one‐pot synthetic strategy at room temperature in aqueous solution. Among the three developed COFs (COF‐LZU1, RT‐COF‐1 and ACOF‐1), the horseradish peroxidase (HRP)‐incorporated COF‐LZU1 is found to retain the highest activity. Structural analysis reveals that a weakest interaction between the hydrated enzyme and COF‐LZU1, an easiest accessibility by the COF‐LZU1 to the substrate, as well as an optimal conformation of enzyme together promote the bioactivity of HRP‐COF‐LZU1. Furthermore, the COF‐LZU1 is revealed to be a versatile nanoplatform for encapsulating multiple enzymes. The COF‐LZU1 also offers superior protection for the immobilized enzymes under harsh conditions and during recycling. The comprehensive understanding of interfacial interactions of COF host and enzyme guest, the substrate diffusion, as well as the enzyme conformation alteration within COF matrices represents an opportunity to design the ideal biocatalysts and opens a broad range of applications of these nanosystems.
Effect of Hydrophobic Groups on Antimicrobial and Hemolytic Activity: Developing a Predictive Tool for Ternary Antimicrobial Polymers
Publisher: American Chemical Society (ACS)
Date: 13-11-2020
Visible Light-Mediated Polymerization-Induced Self-Assembly Using Continuous Flow Reactors
Publisher: American Chemical Society (ACS)
Date: 06-07-2018
Designing with Light: Advanced 2D, 3D, and 4D Materials
Publisher: Wiley
Date: 12-2019
Abstract: Recent achievements and future opportunities for the design of 2D, 3D, and 4D materials using photochemical reactions are summarized. Light is an attractive stimulus for material design due to its outstanding spatiotemporal control, and its ability to mediate rapid polymerization under moderate reaction temperatures. These features have been significantly enhanced by major advances in light generation/manipulation with light-emitting diodes and optical fiber technologies which now allows for a broad range of cost-effective fabrication protocols. This combination is driving the preparation of sophisticated 2D, 3D, and 4D materials at the nano-, micro-, and macrosize scales. Looking ahead, future challenges and opportunities that will significantly impact the field and help shape the future of light as a versatile and tunable design tool are highlighted.
3D Printing Nanostructured Solid Polymer Electrolytes with High Modulus and Conductivity
Publisher: Wiley
Date: 22-09-2022
Abstract: The development of advanced solid‐state energy‐storage devices is contingent upon finding new ways to produce and manufacture scalable, high‐modulus solid‐state electrolytes that can simultaneously provide high ionic conductivity and robust mechanical integrity. In this work, an efficient one‐step process to manufacture solid polymer electrolytes composed of nanoscale ion‐conducting channels embedded in a rigid crosslinked polymer matrix via Digital Light Processing 3D printing is reported. A visible‐light‐mediated polymerization‐induced microphase‐separation approach is utilized, which produces materials with two chemically independent nanoscale domains with highly tunable nanoarchitectures. By producing materials containing a poly(ethylene oxide) domain swelled with an ionic liquid, robust solid polymer electrolytes with outstanding room‐temperature (22 °C) shear modulus ( G ’ 10 8 Pa) and ionic conductivities up to σ = 3 × 10 −4 S cm −1 are achieved. The nanostructured 3D‐printed electrolytes are fabricated into a custom geometry and employed in a symmetric carbon supercapacitor, demonstrating the scalability of the fabrication and the functionality of the electrolyte. Critically, these high‐performance materials are manufactured on demand using inexpensive and commercially available 3D printers, which allows the facile modular design of solid polymer electrolytes with custom geometries.
Seeing the Light: Advancing Materials Chemistry through Photopolymerization
Publisher: Wiley
Date: 11-02-2019
Water Soluble Antioxidant Dextran–Quercetin Conjugate with Potential Anticancer Properties
Publisher: Wiley
Date: 07-02-2018
Abstract: Quercetin, a naturally occurring potent antioxidant, is limited in therapeutic use, owing to its poor water solubility and stability. Herein, a method of conjugating quercetin to an aldehyde functionalized dextran via an HCl catalyzed condensation reaction to yield a water soluble quercetin functionalized polymer is reported. The prepared conjugate is characterized by
Controlled Direct Growth of Polymer Shell on Upconversion Nanoparticle Surface via Visible Light Regulated Polymerization
Publisher: American Chemical Society (ACS)
Date: 15-09-2017
Interconvertible and switchable cationic/PET-RAFT copolymerization triggered by visible light
Publisher: Springer Science and Business Media LLC
Date: 26-08-2019
Customized Nanostructured Ceramics via Microphase Separation 3D Printing
Publisher: Wiley
Date: 26-09-2023
Recent advances in nitric oxide delivery for antimicrobial applications using polymer-based systems
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8TB00299A
Abstract: The present review highlights the recent developments in NO-releasing polymeric biomaterials for antimicrobial applications.
Frontispiece: A Versatile 3D and 4D Printing System through Photocontrolled RAFT Polymerization
Publisher: Wiley
Date: 09-12-2019
Two colours of light drive PET–RAFT photoligation
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0PY01078B
Abstract: By fusing the realms of photopolymerisation and photoligation, our contribution exploits two orthogonal wavelengths of visible light to readily synthesise and functionalise well defined polymers from a unique dual functionality RAFT agent.
PET-RAFT facilitated 3D printable resins with multifunctional RAFT agents
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D0QM00961J
Abstract: The application of reversible addition–fragmentation chain-transfer (RAFT) agents in stereolithographic 3D printing has been seldom reported due to their tendency to reduce polymerization rates.
Influence of Molecular Weight Distribution on the Thermoresponsive Transition of Poly(N‐isopropylacrylamide)
Publisher: Wiley
Date: 13-06-2021
Abstract: A series of poly( N ‐isopropylacrylamide) (PNIPAm) homopolymers with narrow molecular weight distributions (MWDs) is prepared via photoinduced electron/energy transfer–reversible addition‐fragmentation chain transfer (PET–RAFT) polymerization. The thermal transition temperature of these polymer s les is analyzed via turbidity measurements in water/ N , N' ‐dimethylformamide mixtures, which show that the cloud point temperatures are inversely proportional to the weight average molecular weight ( M w ). Binary mixtures of the narrowly distributed PNIPAm s les are also prepared and the statistical parameters for the MWDs of these blends are determined. Very interestingly, for binary blends of the PNIPAm s les, the thermoresponsive transition is not only dependent on the M w , which has been shown previously, but also on higher order statistical parameters of the MWDs. Specifically, at very high values of skewness and kurtosis, the polymer blends deviate from a single sharp thermoresponsive transition toward a broader thermal response, and eventually to a regime of two more distinct transitions. This work highlights the importance of in‐depth characterization of polymer MWDs for thermoresponsive polymers.
Soft polyhedral particles based on cubic liquid crystalline emulsion droplets
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C7SM01521F
Abstract: Soft polyhedral particles based on variations of the cubic symmetry group are produced from a precursor emulsion by extracting solvent to grow facets on the droplets.
In the Limelight: 2D and 3D Materials via Photo-Controlled Radical Polymerization
Publisher: Elsevier BV
Date: 08-2020
Insight into Bioactivity of In‐situ Trapped Enzyme‐Covalent‐Organic Frameworks
Publisher: Wiley
Date: 03-05-2023
Abstract: Selecting a suitable support material for enzyme immobilization with excellent biocatalytic activity and stability is a critical aspect in the development of functional biosystems. The highly stable and metal‐free properties of covalent‐organic frameworks (COFs) make them ideal supports for enzyme immobilization. Herein, we constructed three kinds of COFs via a biofriendly and one‐pot synthetic strategy at room temperature in aqueous solution. Among the three developed COFs (COF‐LZU1, RT‐COF‐1 and ACOF‐1), the horseradish peroxidase (HRP)‐incorporated COF‐LZU1 is found to retain the highest activity. Structural analysis reveals that a weakest interaction between the hydrated enzyme and COF‐LZU1, an easiest accessibility by the COF‐LZU1 to the substrate, as well as an optimal conformation of enzyme together promote the bioactivity of HRP‐COF‐LZU1. Furthermore, the COF‐LZU1 is revealed to be a versatile nanoplatform for encapsulating multiple enzymes. The COF‐LZU1 also offers superior protection for the immobilized enzymes under harsh conditions and during recycling. The comprehensive understanding of interfacial interactions of COF host and enzyme guest, the substrate diffusion, as well as the enzyme conformation alteration within COF matrices represents an opportunity to design the ideal biocatalysts and opens a broad range of applications of these nanosystems.
Synthesis of Discrete Oligomers by Sequential PET‐RAFT Single‐Unit Monomer Insertion
Publisher: Wiley
Date: 07-12-2016
Nano- to macro-scale control of 3D printed materials via polymerization induced microphase separation
Publisher: Springer Science and Business Media LLC
Date: 22-06-2022
DOI: 10.1038/S41467-022-31095-9
Abstract: Although 3D printing allows the macroscopic structure of objects to be easily controlled, controlling the nanostructure of 3D printed materials has rarely been reported. Herein, we report an efficient and versatile process for fabricating 3D printed materials with controlled nanoscale structural features. This approach uses resins containing macromolecular chain transfer agents (macroCTAs) which microphase separate during the photoinduced 3D printing process to form nanostructured materials. By varying the chain length of the macroCTA, we demonstrate a high level of control over the microphase separation behavior, resulting in materials with controllable nanoscale sizes and morphologies. Importantly, the bulk mechanical properties of 3D printed objects are correlated with their morphologies transitioning from discrete globular to interpenetrating domains results in a marked improvement in mechanical performance, which is ascribed to the increased interfacial interaction between soft and hard domains. Overall, the findings of this work enable the simplified production of materials with tightly controllable nanostructures for broad potential applications.
Aqueous RAFT Photopolymerization with Oxygen Tolerance
Publisher: American Chemical Society (ACS)
Date: 14-12-2016
Selective Photoactivation of Trithiocarbonates Mediated by Metal Naphthalocyanines and Overcoming Activation Barriers Using Thermal Energy
Publisher: American Chemical Society (ACS)
Date: 10-01-2022
DOI: 10.1021/JACS.1C11700
Abstract: Metal naphthalocyanines (MNcs) were demonstrated to be efficient photocatalysts to activate photoinduced electron-transfer reversible addition-fragmentation chain transfer (PET-RAFT) polymerization, enabling well-controlled polymerization of (meth)acrylates under near-infrared (λ = 780 nm) light. Owing to their lower redox potential compared to previously explored photocatalysts, the activation of trithiocarbonate RAFT agents exhibited a unique selectivity that was dependent on the nature of the R group. Specifically, MNcs were capable in activating tertiary R group trithiocarbonates, whereas no activation of the trithiocarbonate possessing a secondary R group was observed. The combination of density functional theory calculations and experimental studies have revealed new mechanistic insights into the factors governing a PET-RAFT mechanism and explained this unique selectivity of MNcs toward tertiary carbon trithiocarbonates. Interestingly, by increasing the reaction temperature moderately (i.e., ∼15 °C), the energy barrier prohibiting the photoactivation of the trithiocarbonate with a secondary R group was overcome, enabling their successful activation.
Frontispiece: A Photoinduced Dual‐Wavelength Approach for 3D Printing and Self‐Healing of Thermosetting Materials
Publisher: Wiley
Date: 27-02-2022
Synthetic Antimicrobial Polymers in Combination Therapy: Tackling Antibiotic Resistance
Publisher: American Chemical Society (ACS)
Date: 12-01-2021
Planar polymer electrolyte membrane fuel cells: powering portable devices from hydrogen
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/C9SE00861F
Abstract: An air breathing planar PEMFC has thin geometry, open cathode and minimum peripheral devices.
Scalable Aqueous Reversible Addition–Fragmentation Chain Transfer Photopolymerization-Induced Self-Assembly of Acrylamides for Direct Synthesis of Polymer Nanoparticles for Potential Drug Delivery App
Publisher: American Chemical Society (ACS)
Date: 16-05-2019
What happens in the dark? Assessing the temporal control of photo‐mediated controlled radical polymerizations
Publisher: Wiley
Date: 08-11-2018
DOI: 10.1002/POLA.29247
Gesteuerte Reaktionsorthogonalität in der Polymer‐ und Materialwissenschaft
Publisher: Wiley
Date: 23-09-2020
Abstract: Die selektive Steuerung chemischer Reaktionen ist entscheidend für die genaue Regelung von Prozessen, die von komplizierten biologischen Systemen bis hin zur industriellen Fertigung in großem Maßstab reichen. Die Entwicklung der synthetischen Chemie hin zu einer Komplexität, wie sie in der Natur zu beobachten ist, erfordert eine erhöhte Kontrolle über viele konkurrierende chemische Reaktionen in einer nicht interferierenden (orthogonalen) Weise. Glücklicherweise kann der praktisch unerschöpfliche Pool der bisher entwickelten synthetischen chemischen Reaktionen oft auf orthogonale Weise kombiniert werden, um elegante Lösungen für komplexe chemische Probleme zu finden. In diesem Aufsatz werden zunächst einige der vielen photochemischen Reaktionen hervorgehoben, die in orthogonalen Reaktionsführungen angewendet wurden die hochselektive Natur der photochemischen Reaktionen macht sie gut geeignet für eine unabhängige Aktivierung in Gegenwart anderer Reaktionskomponenten. Die Anwendung solcher orthogonalen Reaktionen, insbesondere der photochemischen Reaktionen, für die Synthese und Modifikation von Polymeren und polymeren Materialien wird ebenfalls zusammengefasst. Hervorzuheben ist, dass die Anwendung orthogonaler chemischer Reaktionen im Vergleich zu traditionellen Syntheseverfahren zusätzliche Möglichkeiten für die Synthese moderner und funktioneller Polymermaterialien bieten kann.
Rational Design of Photocatalysts for Controlled Polymerization: Effect of Structures on Photocatalytic Activities
Publisher: American Chemical Society (ACS)
Date: 04-01-2022
DOI: 10.1021/ACS.CHEMREV.1C00409
Abstract: Over the past decade, the use of photocatalysts (PCs) in controlled polymerization has brought new opportunities in sophisticated macromolecular synthesis. However, the selection of PCs in these systems has been typically based on laborious trial-and-error strategies. To tackle this limitation, computer-guided rational design of PCs based on knowledge of structure-property-performance relationships has emerged. These rational strategies provide rapid and economic methodologies for tuning the performance and functionality of a polymerization system, thus providing further opportunities for polymer science. This review provides an overview of PCs employed in photocontrolled polymerization systems and summarizes their progression from early systems to the current state-of-the-art. Background theories on electronic transitions are also introduced to establish the structure-property-performance relationships from a perspective of quantum chemistry. Typical ex les for each type of structure-property relationships are then presented to enlighten future design of PCs for photocontrolled polymerization.
Polydiacetylene for the Detection of α-Hemolysin in Milk toward the Diagnosis of Bovine Mastitis
Publisher: American Chemical Society (ACS)
Date: 18-09-2020
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