Two dimensional MoS2 accelerates mechanically controlled polymerization and remodeling of hydrogel DOI Creative Commons
Jian Wang,

Han Zhi-jun,

Longfei Zhang

et al.

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Feb. 16, 2025

Self-remodeling material can change their physical properties based on mechanical environment. Recently, mechanically controlled polymerization using mechanoredox catalyst enabled composite materials to undergo a permanent structural change, thereby enhancing strength. However, significant delay in material's response was observed due the sluggish activation of bulk for polymerization. Herein, we report fast, radical water soluble monomers 2D MoS2 as catalyst, studied under various stimuli, including ultrasound, ball milling and low frequency vibrations. Our strategy enables complete within several minutes work. This accelerated process be utilized create hydrogels with ability alter electrical stimuli. has potential applications smart such hydrogel sensors, artificial muscles, implantable biomaterials. Mechanically lead changes structure, but slow. Here, authors use an preparation tuneable properties.

Language: Английский

Recent Progress in Cyclic Aryliodonium Chemistry: Syntheses and Applications DOI Creative Commons
Xiaopeng Peng, Abdur Rahim, Weijie Peng

et al.

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(4), P. 1364 - 1416

Published: Jan. 17, 2023

Hypervalent aryliodoumiums are intensively investigated as arylating agents. They excellent surrogates to aryl halides, and moreover they exhibit better reactivity, which allows the corresponding arylation reactions be performed under mild conditions. In past decades, acyclic aryliodoniums widely explored However, unmet need for is improvement of their notoriously low reaction economy because coproduced iodides during often wasted. Cyclic have intrinsic advantage in terms economy, started receive considerable attention due valuable synthetic applications initiate cascade reactions, can enable construction complex structures, including polycycles with potential pharmaceutical functional properties. Here, we summarizing recent advances made research field cyclic aryliodoniums, nascent design aryliodonium species applications. First, general preparation typical diphenyl iodoniums described, followed by heterocyclic monoaryl iodoniums. Then, initiated arylations coupled subsequent domino summarized construct polycycles. Meanwhile, building biaryls axial atropisomers discussed a systematic manner. Finally, very advance employed halogen-bonding organocatalysts described.

Language: Английский

Citations

72
Dual Nickel(II)/Mechanoredox Catalysis: Mechanical‐Force‐Driven Aryl‐Amination Reactions Using Ball Milling and Piezoelectric Materials DOI

Tamae Seo,

Koji Kubota, Hajime Ito

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(42)

Published: Aug. 28, 2023

Abstract The combination of a nickel(II) catalyst and mechanoredox under ball‐milling conditions promotes mechanical‐force‐driven C−N cross‐coupling reactions. In this nickel(II)/mechanoredox cocatalyst system, the modulation oxidation state nickel center, induced by piezoelectricity, is used to facilitate highly efficient aryl‐amination reaction, which characterized broad substrate scope, an inexpensive catalysts (NiBr 2 BaTiO 3 ), short reaction times, almost negligible quantity solvents. Moreover, can be readily up‐scaled multi‐gram scale, all synthetic operations carried out atmospheric without need for complicated setups. Furthermore, force‐induced system suitable excitation‐energy‐accepting molecules poorly soluble polyaromatic substrates that are incompatible with solution‐based nickel(II)/photoredox cocatalysts.

Language: Английский

Citations

32
Mechanically activated solid state radical polymerization and cross‐linking via piezocatalysis DOI Creative Commons
Mitchell D. Nothling, J. Daniels, Yen Vo

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(20)

Published: March 15, 2023

Abstract Piezocatalysis offers a means to transduce mechanical energy into chemical potential, harnessing physical force drive redox reactions. Working in the solid state, we show here that piezoelectric BaTiO 3 nanoparticles can load flux of reactive radical species capable initiating state free polymerization. Activation powder by ball milling, striking with hammer, or repeated compressive loading generates highly hydroxyl radicals (⋅OH), which readily initiate chain growth and crosslinking acrylamide, acrylate, methacrylate styrenic monomers. Control experiments indicate critical role for chemisorbed water on nanoparticle surface, is oxidized ⋅OH via mechanoredox catalysis. The force‐induced production compressing dry materials represents promising new route harness synthesis.

Language: Английский

Citations

28
Mechanochemically Promoted Functionalization of Postconsumer Poly(Methyl Methacrylate) and Poly(α‐Methylstyrene) for Bulk Depolymerization DOI
James B. Young, Sofia L. Goodrich,

James A. Lovely

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(44)

Published: July 15, 2024

We describe a methodology of post-polymerization functionalization to enable subsequent bulk depolymerization monomer by utilizing mechanochemical macro-radical generation. By harnessing ultrasonic chain-scission in the presence N-hydroxyphthalimide methacrylate (PhthMA), we successfully chain-end functionalize polymers promote bulk, achieving up 82 % poly(methyl methacrylate) (PMMA) and poly(α-methylstyrene) (PAMS) within 30 min. This method yields high-purity that can be repolymerized. Moreover, as compared most common methods depolymerization, this work is efficient with ultra-high molecular weight (UHMW) polymers, establishing potential address highly persistent, non-degradable all-carbon backbone plastic materials. Lastly, demonstrate expansion commercial cell cast PMMA, high degrees from post-consumer waste. first demonstration applying PhthMA-promoted strategies homopolymer PMMA PAMS prepared conventional polymerization methods.

Language: Английский

Citations

10
Piezoelectrically Mediated Reactions: From Catalytic Reactions to Organic Transformations DOI

Ziye Ren,

Yuhao Peng,

Hanliang He

et al.

Chinese Journal of Chemistry, Journal Year: 2022, Volume and Issue: 41(1), P. 111 - 128

Published: Sept. 13, 2022

Comprehensive Summary Recently, piezocatalysis has attracted considerable attention as a new type of renewable mechanical energy conversion technology, which relies on the strain induced polarization piezoelectric material. This technology been extensively applied in applications water splitting, remediation, gas purification and tumor therapy. Despite rapid development piezocatalysis, utilization materials for synthetic purpose is still under exploration. Piezoelectric means to promote organic reactions expand scope piezoelectrically mediated show successes both polymer synthesis. Herein, we provide comprehensive review recent progress reactions, catalytic mechanisms last few years. The limitations future directions this area are also discussed. We believe will insights into underlying mechanism electron transfer process guide design chemistry.

Language: Английский

Citations

36
Resonant acoustic mixing (RAM) for efficient mechanoredox catalysis without grinding or impact media DOI Open Access
Farshid Effaty, Lori Gonnet, Stefan G. Koenig

et al.

Chemical Communications, Journal Year: 2022, Volume and Issue: 59(8), P. 1010 - 1013

Published: Dec. 12, 2022

Resonant acoustic mixing (RAM) enables mechanoredox catalysis with BaTiO3 as the piezoelectric catalyst on model diazonium coupling reactions. RAM proceeds without formal grinding or impact media, is faster than analogous ball-milling strategy, and readily scalable. X-ray diffraction spectroscopy indicate that reusability of a under might be limited by boration.

Language: Английский

Citations

32
CdS nanocages@defective-CoNi-LDH with bilayer porous hollow frameworks toward optimized sono-photocatalytic performance DOI
Bin Fang, Zipeng Xing, Fan Du

et al.

Journal of Materials Chemistry A, Journal Year: 2022, Volume and Issue: 10(31), P. 16439 - 16447

Published: Jan. 1, 2022

HCNs@HD-CoNi-LDH are fabricated via Cd-based Prussian blue analog nanocubes twice sulfidation and epitaxial growth ZIF-67 etching into hollow defective CoNi-LDH strategies, which exhibit excellent sono-photocatalytic performance due to special bilayer porous frameworks.

Language: Английский

Citations

29
Tribochemically Controlled Atom Transfer Radical Polymerization Enabled by Contact Electrification DOI
Chen Wang,

Ruoqing Zhao,

Wenru Fan

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(37)

Published: July 29, 2023

Traditional mechanochemically controlled reversible-deactivation radical polymerization (RDRP) utilizes ultrasound or ball milling to regenerate activators, which induce side reactions because of the high-energy and high-frequency stimuli. Here, we propose a facile approach for tribochemically atom transfer (tribo-ATRP) that relies on contact-electro-catalysis (CEC) between titanium oxide (TiO2 ) particles CuBr2 /tris(2-pyridylmethylamine (TPMA), without any input. Under friction induced by stirring, TiO2 are electrified, continuously reducing /TPMA into CuBr/TPMA, thereby conversing alkyl halides active radicals start ATRP. In addition, effect reaction was elucidated theoretical simulation. The results indicated increasing frequency could reduce energy barrier electron from /TPMA. this study, design tribo-ATRP successfully achieved, enabling CEC (ca. 10 Hz) access variety polymers with predetermined molecular weights, low dispersity, high chain-end fidelity.

Language: Английский

Citations

19
Aerobic mechanochemical reversible-deactivation radical polymerization DOI Creative Commons
Haoyang Feng, Zhe Chen,

Lei Li

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: July 22, 2024

Abstract Polymer materials suffer mechano-oxidative deterioration or degradation in the presence of molecular oxygen and mechanical forces. In contrast, aerobic biological activities combined with stimulus promote tissue regeneration repair various organs. A synthetic approach which energy synergistically initiate polymerization will afford similar robustness polymeric materials. Herein, mechanochemical reversible-deactivation radical was developed by design an organic mechano-labile initiator converts into activators response to ball milling, enabling reaction proceed air low-energy input, operative simplicity, avoidance potentially harmful solvents. addition, this not only complements existing methods access well-defined polymers but also has been successfully employed for controlled (meth)acrylates, styrenic monomers solid acrylamides as well synthesis polymer/perovskite hybrids without solvent at room temperature are inaccessible other means.

Language: Английский

Citations

8
Organic Reactions Enabled by Mechanical Force‐Induced Single Electron Transfer DOI
Ruoxuan Liu,

Xiaochun He,

Tianfen Liu

et al.

Chemistry - A European Journal, Journal Year: 2024, Volume and Issue: 30(47)

Published: June 18, 2024

Mechanochemical reactions, achieved through milling, grinding, or other mechanical actions, have emerged as a solvent-free alternative to traditional solution-based chemistry. Mechanochemistry not only provides the opportunity eliminate bulk solvent use, reducing waste generation, but also unveils new reaction strategy which enables realization of reactions previously inaccessible in solution. While majority organic facilitated by force traditionally follow two-electron transfer pathways similar their counterparts, field mechanochemically induced single-electron (SET) has witnessed rapid development. This review outlines examples mechanochemical SET process, focusing on reagents that initiate SET, thereby positioning mechanochemistry burgeoning within realm

Language: Английский

Citations

7