Nitroxide-Mediated Polymerization: A Versatile Tool for the Engineering of Next Generation Materials

Lamontagne, Halynne R.; Lessard, Benoît H.

doi:10.1021/acsapm.0c00888

Cited by 69 publications

(55 citation statements)

References 193 publications

(357 reference statements)

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“…All experimental conditions and formulations can be found in the Experimental Section (Table S1). Nitroxide mediated polymerization (NMP) is a controlled polymerization technique that can lead to well-defined molecular architectures without the need for transition metal catalysts or laborious purification techniques; making it an ideal technique for the development of functional polymers for printable electronics. − Therefore, a single large batch of narrow dispersity and pseudoliving poly(styrene) (poly(S)) macroinitiator ( M̅ w / M̅ n = 1.06; M̅ n = 22.5 kg·mol –1 , Table ) was synthesized by NMP, ensuring to stop the reaction at low-conversion to maintain a high-degree of livingness, with a target number average molecular weight (similar to our previous works. ,, Chain extension of the poly(S) macroinitiators was performed using chloromethyl styrene (CMS) and poly(ethylene glycol)methyl ether methacrylate (PEGMA) comonomers in varying comonomer feed ratios and with different target molecular weights (Table ). We obtained nine different poly(S)- b -poly(CMS- r -PEGMA) diblock copolymers with unimodal molecular weight distributions ranging from M̅ w / M̅ n = 1.07–1.24 with M̅ n values ranging from 24.5–39.6 kg·mol –1 (Table ).…”

Section: Resultsmentioning

confidence: 99%

Ionic Liquid Containing Block Copolymer Dielectrics: Designing for High-Frequency Capacitance, Low-Voltage Operation, and Fast Switching Speeds

Peltekoff

Brixi

Niskanen

et al. 2021

JACS Au

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Polymerized ionic liquids (PILs) are a potential solution to the large-scale production of low-power consuming organic thin-film transistors (OTFTs). When used as the device gating medium in OTFTs, PILs experience a double-layer capacitance that enables thickness independent, low-voltage operation. PIL microstructure, polymer composition, and choice of anion have all been reported to have an effect on device performance, but a better structure property relationship is still required. A library of 27 well-defined, poly(styrene) -b- poly(1-(4-vinylbenzyl)-3-butylimidazolium- random -poly(ethylene glycol) methyl ether methacrylate) (poly(S)- b -poly(VBBI + [X]- r -PEGMA)) block copolymers, with varying PEGMA/VBBI + ratios and three different mobile anions (where X = TFSI – , PF 6 – or BF 4 – ), were synthesized, characterized and integrated into OTFTs. The fraction of VBBI + in the poly(VBBI + [X]- r -PEGMA) block ranged from to 100 mol % and led to glass transition temperatures ( T g ) between −7 and 55 °C for that block. When VBBI + composition was equal or above 50 mol %, the block copolymer self-assembled into well-ordered domains with sizes between 22 and 52 nm, depending on the composition and choice of anion. The block copolymers double-layer capacitance ( C DL ) and ionic conductivity (σ) were found to correlate to the polymer self-assembly and the T g of the poly(VBBI + [X]- r -PEGMA) block. Finally, the block copolymers were integrated into OTFTs as the gating medium that led to n-type devices with threshold voltages of 0.5–1.5 V while maintaining good electron mobilities. We also found that the greater the σ of the PIL, the greater the OTFT operating frequency could reach. However, we also found that C DL is not strictly proportional to OTFT output currents.

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Section: Resultsmentioning

confidence: 99%

Ionic Liquid Containing Block Copolymer Dielectrics: Designing for High-Frequency Capacitance, Low-Voltage Operation, and Fast Switching Speeds

Peltekoff

Brixi

Niskanen

et al. 2021

JACS Au

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“…In other frequently used methods such as nitroxide mediated polymerization (NMP) or atom transfer radical polymerization (ATRP) the propagation is driven by activation of a dormant species, followed by reversible deactivation, usually with an equilibrium favoring the dormant side. [ 21 ] Here, the radical species, necessary for polymerization are generated by homolytic bond cleavage (NMP) [ 22 ] or by a redox process (ATRP). [ 23 ] RAFT polymerization on the other hand relies on a degenerative chain transfer mechanism of growing chains.…”

Section: Mechanism Of Conventional Raft‐polymerizationsmentioning

confidence: 99%

Photo‐Iniferter RAFT Polymerization

Hartlieb

2021

Macromol. Rapid Commun.

101

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Light‐mediated polymerization techniques offer distinct advantages over polymerization reactions fueled by thermal energy, such as high spatial and temporal control as well as the possibility to work under mild reaction conditions. Reversible addition‐fragmentation chain‐transfer (RAFT) polymerization is a highly versatile radical polymerization method that can be utilized to control a variety of monomers and produce a vast number of complex macromolecular structures. The use of light to drive a RAFT‐polymerization is possible via multiple routes. Besides the use of photo‐initiators, or photo‐catalysts, the direct activation of the chain transfer agent controlling the RAFT process in a photo‐iniferter (PI) process is an elegant way to initiate and control polymerization reactions. Within this review, PI‐RAFT polymerization and its advantages over the conventional RAFT process are discussed in detail.

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“…Other controlled/“living” polymerization techniques, such as ring-opening metathesis polymerizations (ROMP), as well as nitroxide-mediated polymerization (NMP), can also be used [ 114 , 115 , 116 ]. The mechanism for ROMP [ 117 , 118 ] and MNP [ 119 , 120 , 121 ] have been briefly described.…”

Section: Polymersomes As a Platform For Anticancer Therapeutic Deliverymentioning

confidence: 99%

Light-Triggered Polymersome-Based Anticancer Therapeutics Delivery

et al. 2022

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Polymersomes are biomimetic cell membrane-like model structures that are self-assembled stepwise from amphiphilic copolymers. These polymeric (nano)carriers have gained the scientific community’s attention due to their biocompatibility, versatility, and higher stability than liposomes. Their tunable properties, such as composition, size, shape, and surface functional groups, extend encapsulation possibilities to either hydrophilic or hydrophobic cargoes (or both) and their site-specific delivery. Besides, polymersomes can disassemble in response to different stimuli, including light, for controlling the “on-demand” release of cargo that may also respond to light as photosensitizers and plasmonic nanostructures. Thus, polymersomes can be spatiotemporally stimulated by light of a wide wavelength range, whose exogenous response may activate light-stimulable moieties, enhance the drug efficacy, decrease side effects, and, thus, be broadly employed in photoinduced therapy. This review describes current light-responsive polymersomes evaluated for anticancer therapy. It includes light-activable moieties’ features and polymersomes’ composition and release behavior, focusing on recent advances and applications in cancer therapy, current trends, and photosensitive polymersomes’ perspectives.

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Nitroxide-Mediated Polymerization: A Versatile Tool for the Engineering of Next Generation Materials

Cited by 69 publications

References 193 publications

Ionic Liquid Containing Block Copolymer Dielectrics: Designing for High-Frequency Capacitance, Low-Voltage Operation, and Fast Switching Speeds

Ionic Liquid Containing Block Copolymer Dielectrics: Designing for High-Frequency Capacitance, Low-Voltage Operation, and Fast Switching Speeds

Photo‐Iniferter RAFT Polymerization

Light-Triggered Polymersome-Based Anticancer Therapeutics Delivery

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