Enhancing photothermal depolymerization with metalloporphyrin catalyst DOI Creative Commons

Gervase Ng,

Stuart W. Prescott, Almar Postma

et al.

Journal of Polymer Science, Journal Year: 2024, Volume and Issue: 62(17), P. 3920 - 3928

Published: May 22, 2024

Abstract The ability to revert polymers their original monomers represents a crucial chemical recycling technique, promoting sustainability and offering the chance convert used materials into valuable products. In recent years, numerous studies have explored use of synthesized via reversible deactivation radical polymerization (RDRP) techniques facilitate efficient depolymerization reactions. Herein, we report photocatalyst, zinc tetraphenylporphyrin (ZnTPP), along with light irradiation accelerate prepared by addition‐fragmentation chain transfer (RAFT) polymerization. We explore various parameters affecting efficiency, including solvents, reaction temperature (80, 100, 120°C), presence photocatalysts (ZnTPP Eosin Y), type RAFT end‐groups, namely trithiocarbonate, dithiobenzoate, 1 H ‐pyrazole‐1‐carbodithioate. For instance, when PMMA was diluted 25 mM in 1,4‐dioxane heated 120°C under green ZnTPP (200 ppm), rapid exceeding 70% occurred within h. Without ZnTPP, similar conditions, required over 8 h achieve slightly lower yield. Furthermore, this method confers moderate oxygen tolerance system, enabling proceed without need deoxygenation, albeit at rate consequently lesser monomer recovery (31%).

Language: Английский

A comparison of RAFT and ATRP methods for controlled radical polymerization DOI
Nghia P. Truong, Glen R. Jones, Kate G. E. Bradford

et al.

Nature Reviews Chemistry, Journal Year: 2021, Volume and Issue: 5(12), P. 859 - 869

Published: Oct. 18, 2021

Language: Английский

Citations

269
Rational Design of Photocatalysts for Controlled Polymerization: Effect of Structures on Photocatalytic Activities DOI
Chenyu Wu, Nathaniel Corrigan, Chern‐Hooi Lim

et al.

Chemical Reviews, Journal Year: 2022, Volume and Issue: 122(6), P. 5476 - 5518

Published: Jan. 4, 2022

Over the past decade, use of photocatalysts (PCs) in controlled polymerization has brought new opportunities sophisticated macromolecular synthesis. However, selection PCs these systems been typically based on laborious trial-and-error strategies. To tackle this limitation, computer-guided rational design knowledge structure-property-performance relationships emerged. These strategies provide rapid and economic methodologies for tuning performance functionality a system, thus providing further polymer science. This review provides an overview employed photocontrolled summarizes their progression from early to current state-of-the-art. Background theories electronic transitions are also introduced establish perspective quantum chemistry. Typical examples each type structure-property then presented enlighten future polymerization.

Language: Английский

Citations

183
Photocontrolled RAFT polymerization: past, present, and future DOI Creative Commons

Yungyeong Lee,

Cyrille Boyer, Min Sang Kwon

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(9), P. 3035 - 3097

Published: Jan. 1, 2023

In this review, we provide a brief history, progress, and applications, discuss the remaining challenges of photocontrolled reversible addition-fragmentation chain transfer (RAFT) polymerization (i.e., photoinduced electron/energy transfer-RAFT (PET-RAFT), photoiniferter, photomediated cationic RAFT polymerization). Among these, visible-light-driven has attracted particular attention in recent years due to its benefits, including low energy consumption safe reaction procedure. Moreover, incorporation visible-light photocatalysis conferred attractive features, such as spatiotemporal control oxygen tolerance; however, clear understanding mechanism not been completely provided. We also present research efforts elucidate mechanisms with aid quantum chemical calculations combined experimental evidence. This review offers an insight into better design systems for desired applications helps realize full potential both academic- industrial-scale applications.

Language: Английский

Citations

144
Open-air green-light-driven ATRP enabled by dual photoredox/copper catalysis DOI Creative Commons
Grzegorz Szczepaniak, Jaepil Jeong, Kriti Kapil

et al.

Chemical Science, Journal Year: 2022, Volume and Issue: 13(39), P. 11540 - 11550

Published: Jan. 1, 2022

Photoinduced atom transfer radical polymerization (photo-ATRP) has risen to the forefront of modern polymer chemistry as a powerful tool giving access well-defined materials with complex architecture. However, most photo-ATRP systems can only generate radicals under biocidal UV light and are oxygen-sensitive, hindering their practical use in synthesis biohybrids. Herein, inspired by photoinduced electron transfer-reversible addition-fragmentation chain (PET-RAFT) polymerization, we demonstrate dual photoredox/copper catalysis that allows open-air ATRP green irradiation. Eosin Y was used an organic photoredox catalyst (PC) combination copper (X-Cu

Language: Английский

Citations

86
Driving Polymer Brushes from Synthesis to Functioning DOI Creative Commons

Rui Wang,

Qiangbing Wei, Wenbo Sheng

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(27)

Published: March 23, 2023

The great success of controlled radical polymerizations has encouraged researchers to develop more facile and robust approaches for surface-initiated (SIPs) fabricate polymer brushes, even non-experts. In recent years, external-stimuli-mediated polymerization methods have come the fore as SIPs because their less rigorous synthetic procedures high controllability, which expand opportunities synthesizing macromolecules with desired chemical compositions structures, well tailor-made polymers bioconjugates that show broad applicability physiological compatibility. This review discusses latest developments in methods, particular, external-stimuli mediated atom transfer (ATRP), photo-induced polymerizations, reversible addition-fragmentation chain (RAFT) polymerization, other combination application surface grafting. implementation these is interest due unique possibilities temporally control a process, fast straightforward environmentally benign features, lead established emerging applications biolubrication, antifouling, biosensing.

Language: Английский

Citations

62
Fast Bulk Depolymerization of Polymethacrylates by ATRP DOI Creative Commons

Ferdinando De Luca Bossa,

Görkem Yılmaz, Krzysztof Matyjaszewski

et al.

ACS Macro Letters, Journal Year: 2023, Volume and Issue: 12(8), P. 1173 - 1178

Published: Aug. 2, 2023

Fast bulk depolymerization of poly(n-butyl methacrylate) and poly(methyl methacrylate), prepared by atom transfer radical polymerization (ATRP), is reported in the temperature range between 150 230 °C. Depolymerization Cl-terminated polymethacrylates was catalyzed a CuCl2/TPMA complex (0.022 or 0.22 equiv vs P-Cl) studied using TGA, also under isothermal conditions. Relatively rapid 5-20 min observed at 180 The preparative scale reactions were carried out short-path distillation setup with up to 84% within 15

Language: Английский

Citations

60
Advances in Perovskite Nanocrystals and Nanocomposites for Scintillation Applications DOI
Abhinav Anand, Matteo L. Zaffalon, Andrea Erroi

et al.

ACS Energy Letters, Journal Year: 2024, Volume and Issue: 9(3), P. 1261 - 1287

Published: Feb. 28, 2024

In recent years, the field of radiation detection has witnessed a paradigm shift with emergence plastic scintillators incorporating perovskite nanocrystals (PNCs). This innovative class not only capitalizes on superior luminescent properties PNCs but also harnesses flexibility and processability polymers. review explores intricate landscape synthesizing fabricating scintillating nanocomposites, delving into methods employed in their production. From solution-based to solid-state approaches, synthesis for application is explored comprehensively. Furthermore, embedding strategies within polymeric matrices are scrutinized, shedding light various techniques utilized achieve optimal dispersion compatibility. The evaluation final nanocomposites finally discussed, particular emphasis performance hardness. Through meticulous exploration methodologies, techniques, assessments, this Review aims provide multilayered understanding state-of-the-art PNC-based nanoscintillators.

Language: Английский

Citations

29
Oxygen, Light, and Mechanical Force Mediated Radical Polymerization Toward Precision Polymer Synthesis DOI
Zhujun Huang, Jin Dong, Kaiwen Liu

et al.

Chemical Communications, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

This article highlights the advancements in controlled radical polymerization facilitated by three external regulations of oxygen, light, and mechanical force, outlines future directions polymerization.

Language: Английский

Citations

3
Light-accelerated depolymerization catalyzed by Eosin Y DOI Creative Commons
Valentina Bellotti, Kostas Parkatzidis, Hyun Suk Wang

et al.

Polymer Chemistry, Journal Year: 2022, Volume and Issue: 14(3), P. 253 - 258

Published: Dec. 20, 2022

Retrieving the starting monomers from polymers synthesized by reversible deactivation radical polymerization has recently emerged as an efficient way to increase recyclability of such materials and potentially enable their industrial implementation. To date, most methods have primarily focused on utilizing high temperatures (typically 120 °C 180 °C) trigger depolymerization reaction. In this work, we show that, in presence Eosin Y under light irradiation, a much faster made addition-fragmentation chain-transfer (RAFT) can be triggered even at lower temperature (

Language: Английский

Citations

72
An aqueous photo-controlled polymerization under NIR wavelengths: synthesis of polymeric nanoparticles through thick barriers DOI Creative Commons
Zilong Wu,

Wenbo Fang,

Chenyu Wu

et al.

Chemical Science, Journal Year: 2022, Volume and Issue: 13(39), P. 11519 - 11532

Published: Jan. 1, 2022

We report an aqueous and near-infrared (NIR) light mediated photoinduced reversible addition-fragmentation chain transfer (photo-RAFT) polymerization system using tetrasulfonated zinc phthalocyanine (ZnPcS4-) as a photocatalyst. Owing to the high catalytic efficiency excellent oxygen tolerance of this system, well-controlled polyacrylamides, polyacrylates, polymethacrylates were synthesized at fast rates without requiring deoxygenation. Notably, NIR wavelengths possess enhanced penetration through non-transparent barriers compared UV visible light, allowing barriers. Using 6.0 mm pig skin barrier, rate was only reduced from 0.36 0.21 h-1, indicating potential for biomedical applications. Furthermore, longer (higher λ) can be considered ideal source dispersion photopolymerization, especially synthesis large diameter (d) nanoparticles, scattering is proportional d6/λ4. Therefore, photo-RAFT applied polymerization-induced self-assembly (photo-PISA), enabling polymeric nanoparticles with various morphologies, including spheres, worms, vesicles. Taking advantage wavelengths, we demonstrate first syntheses consistent morphologies thick

Language: Английский

Citations

55