Article
Chemistry, Multidisciplinary
John Eymann, Lionel Joucla, Guy Jacob, Jean Raynaud, Chaza Darwich, Emmanuel Lacote
Summary: New energetic polymers based on polytetrazenes have direct incorporation of energetic groups in the polymer backbone, with decomposition temperature at around 130 degrees Celsius and glass transition temperatures ranging from -34.2 to 0.2 degrees Celsius, lowering to -61 degrees Celsius with a new diazidotetrazene plasticizer. Complete room-temperature depolymerization within 1 week is achieved using hexafluoroisopropanol (HFIP), enabling recycling of pyrotechnic compositions with these new binders.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Yunyan Sun, William J. Neary, Zachary P. Burke, Hai Qian, Lingyang Zhu, Jeffrey S. Moore
Summary: Polymers that release small molecules under mechanical stress have potential applications in catalysis, sensing, and mechanochemical dynamic therapy. In this study, a dual mechanophore based on a unique mechanochemical reaction involving norborn-2-en-7-one (NEO) is demonstrated. The polymers can release carbon monoxide (CO) and exhibit bright cyan emission upon mechanical activation.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
David Nieto-Castro, Felipe A. Garces-Pineda, Andrea Moneo-Corcuera, Irene Sanchez-Molina, Jose Ramon Galan-Mascaros
Summary: Bistable multifunctional materials have great potential in various devices, but the direct use of spin crossover materials in electronic devices is limited. Incorporating SCO spin crossover materials as probes in conducting organic polymer matrices can lead to low-resistance conductors with memory effect.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Christoph Baumann, Maria Stratigaki, Silvia P. Centeno, Robert Gostl
Summary: The fracture of polymer materials is a complex multiscale process, and a new approach involving fluorescent molecular force probes has been developed to track intact and cleaved bonds, allowing for a quantitative description of the fracture processes in various materials.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Takuma Watabe, Hideyuki Otsuka
Summary: We present a new method for achieving swelling-induced mechanochemistry using a multinetwork (MN) strategy, which allows polymer networks to repeatedly swell with monomers and solvents. The isotropic expansion of the first network (FN) provides sufficient force to drive the mechanochemical scission of a radical-based mechanophore, difluorenylsuccinonitrile (DFSN). The MN polymers not only demonstrate the ability to modify networks through swelling force, but also show tunable reactivity of the dissociative unit through hierarchical network architecture design.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Davide Campagna, Robert Goestl
Summary: This study reports a mechanochemical protecting group for secondary amines that can be activated in polymers through force-induced reactions. The research demonstrates that this protecting group can produce free amines in polymers through bond scission, similar to its photochemical counterpart. Additionally, the protecting group is applied in a force-activated organocatalytic reaction.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Jingsong Yuan, Gavin J. Giardino, Jia Niu
Summary: A novel class of enyne self-immolative polymers with 1,6-enyne structures have been reported to undergo metathesis cascade-triggered depolymerization efficiently. The introduction of a terminal alkene to the chain end of the enyne SIPs improved depolymerization efficiency, showing potential as stimuli-responsive materials.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Parishmita Sarma, Kashyap Kumar Sarmah, Dharittri Kakoti, Sanjeev Pran Mahanta, Nadeesh Madusanka Adassooriya, Goutam Nandi, Pranab Jyoti Das, Dejan-Kresimir Bucar, Ranjit Thakuria
Summary: A novel nitrogen-rich amorphous porous organic polymer has been synthesized using microwave-assisted process, exhibiting high chemical stability and reusability. It can serve as a metal-free heterogeneous catalyst for C-C bond formation under environmentally benign conditions at ambient temperature.
CATALYSIS COMMUNICATIONS
(2021)
Article
Chemistry, Multidisciplinary
Jess M. Clough, Cedric Kilchoer, Bodo D. Wilts, Christoph Weder
Summary: This paper reports a new type of mechanochromic material that overcomes the limitations of traditional mechanochromic polymers by combining photonic structures with covalent mechanophores. These materials can change their reflection spectra upon deformation and provide quantitative detection of the range of changes, with a broad strain detection range.
Review
Chemistry, Multidisciplinary
Fabian Eisenreich
Summary: Shaping a sustainable future is closely tied to advanced plastic recycling technologies. Low global recycling rates result in the incineration or landfill disposal of post-consumer plastics, causing severe environmental risks and a loss of chemical resources. Recent breakthroughs in photocatalytic methods offer a solution by converting polymers into valuable organic molecules under environmentally benign conditions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Polymer Science
Eunsong Jung, Daniel Yim, Hyungjun Kim, Gregory I. Peterson, Tae-Lim Choi
Summary: In this study, ball-mill grinding (BMG) was found to effectively depolymerize poly(alpha-methyl styrene) (PMS) with minimal side products. Mechanochemical chain scission was identified as the mechanism for the depolymerization, which was supported by constrained geometries simulate external force (CoGEF) simulations and radical trapping experiments. The depolymerization proceeded even at temperatures below the ceiling temperature of PMS. This research provides a starting point for further development of BMG as a mild method for depolymerizing vinyl polymers.
JOURNAL OF POLYMER SCIENCE
(2023)
Review
Polymer Science
Cesar A. Barbero, Diego F. Acevedo
Summary: This review discusses the mechanochemical synthesis of polyanilines (PANIs) through oxidative polymerization of anilines. The effects of different parameters on the properties of conducting polymers are analyzed, including molecular weight, degradation, doping/oxidation level, conductivity, and nanostructure. The production of acids during polymerization and the comparison of PANI nanostructures made by mechanochemical polymerization (MCP) and solution are also investigated. The extensive work on the production of nanocomposites by MCP of anilines together with different nanomaterials is described.
Article
Polymer Science
Han Hu, Jiayi Li, Qianfeng Wang, Xingyu Ouyang, Jinggang Wang, Yi-Lei Zhao, Cheng Kang, Ruoyu Zhang, Jin Zhu
Summary: A series of PBXI copolyesters with outstanding mechanical properties were successfully synthesized, showing good degradation performance in experiments，providing a new strategy for the synthesis of potentially biodegradable copolymers.
Article
Chemistry, Multidisciplinary
Takumi Yamamoto, Sota Kato, Daisuke Aoki, Hideyuki Otsuka
Summary: This study introduces an innovative strategy to detect mechanoradicals visually and quantitatively, using a fluorescent molecular probe that generates relatively stable radicals. Mechanoradicals generated by ball milling of polystyrene samples were successfully detected through this radical chain-transfer mechanism, enabling visualization and quantitative evaluation of mechanoradicals generated by polymer-chain scission.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Hajime Sugita, Yi Lu, Daisuke Aoki, Hideyuki Otsuka, Koichiro Mikami
Summary: In this study, the synthesis and characterization of two series of arylfluorene-based mechanophores were reported. Density functional theory (DFT) calculations revealed the importance of thermodynamic stability and oxygen tolerance for the functions and applicability of these materials. Furthermore, the mechanochromism of a polymer containing one of the mechanophores was demonstrated through ball-milling.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Polymer Science
Gregory I. Peterson, Jaeho Lee, Tae-Lim Choi
Article
Polymer Science
Gregory I. Peterson, Jinkyung Noh, Ki-Taek Bang, Hyunji Ma, Kyoung Taek Kim, Tae-Lim Choi
Article
Chemistry, Multidisciplinary
Jung-Ah Song, Gregory Peterson, Ki-Taek Bang, Tonia S. Ahmed, Jong-Chan Sung, Robert H. Grubbs, Tae-Lim Choi
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2020)
Article
Chemistry, Multidisciplinary
Antonio Rizzo, Gregory I. Peterson, Atanu Bhaumik, Cheol Kang, Tae-Lim Choi
Summary: Enyne monomers derived from D-xylose underwent living cascade polymerizations to prepare new polymers with a ring-opened sugar and degradable linkage incorporated into every repeat unit of the backbone. The polymerizations were well-controlled and had living character, which enabled the preparation of high molecular weight polymers with narrow molecular weight dispersity values and a block copolymer. By tuning the type of acid-sensitive linkage, the degradation profile of the polymer and the identity of the resulting degradation products could be changed.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Polymer Science
Gregory Peterson, Wonyoung Ko, Ye-Jin Hwang, Tae-Lim Choi
Editorial Material
Chemistry, Multidisciplinary
Gregory I. Peterson, Sanghee Yang, Tae-Lim Choi
Article
Polymer Science
Gregory Peterson, Jinkyung Noh, Min Young Ha, Sanghee Yang, Won Bo Lee, Tae-Lim Choi
Summary: The study found that higher grafting density increases the extension of polymer backbone and arms, as well as enhances arm-arm interactions. At higher grafting density, faster scission rates for backbone and arms were observed, with PS and PMA arms showing opposite trends in scission rates.
Article
Chemistry, Multidisciplinary
Jinkyung Noh, Gregory I. Peterson, Tae-Lim Choi
Summary: The study investigated the mechanochemical degradation of bottlebrush and dendronized polymers in solution and solid states, revealing different backbone scission behaviors based on their elongated conformations in solution and arm architecture in solid state. The results suggest important implications for the development of new mechanoresponsive materials.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Antonio Rizzo, Eunsong Jung, Hojoon Song, Yunhyeong Cho, Gregory I. Peterson, Tae-Lim Choi
Summary: Cascade polymerization of unique polycyclic enyne monomers was explored, with modifications to monomer structure parameters allowing control over polymerization performance and efficiency. By analyzing degradation products under mild acidic conditions, the cascade efficiency could be calculated, leading to controlled living cascade polymerizations of multiple monomers with high efficiency.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Polymer Science
Eunsong Jung, Daniel Yim, Hyungjun Kim, Gregory I. Peterson, Tae-Lim Choi
Summary: In this study, ball-mill grinding (BMG) was found to effectively depolymerize poly(alpha-methyl styrene) (PMS) with minimal side products. Mechanochemical chain scission was identified as the mechanism for the depolymerization, which was supported by constrained geometries simulate external force (CoGEF) simulations and radical trapping experiments. The depolymerization proceeded even at temperatures below the ceiling temperature of PMS. This research provides a starting point for further development of BMG as a mild method for depolymerizing vinyl polymers.
JOURNAL OF POLYMER SCIENCE
(2023)
Article
Polymer Science
Seung-Hwan Jin, Chanseo Lee, Youngrok Kim, Jinwoo Jeon, Gregory I. Peterson, Ye-Jin Hwang
Summary: The conjugated polymer PTB7 was found to undergo flow-induced chain scission, suggesting that polymer degradation is a crucial side reaction in flow synthesis. Increasing the residence time leads to an initial increase in molecular weight, but longer times result in declines. The extent of degradation is influenced by reactor temperature, polymer molecular weight, and concentration.
POLYMER DEGRADATION AND STABILITY
(2023)
Article
Chemistry, Multidisciplinary
Gue Seon Lee, Hyo Won Lee, Hyun Sub Lee, Taeyang Do, Jean-Louis Do, Jeewoo Lim, Gregory Peterson, Tomislav Friscic, Jeung Gon Kim
Summary: Ruthenium-alkylidene initiated ring-opening metathesis polymerization has been successfully achieved under solid-state conditions using a mechanochemical ball milling method. This method offers a green approach and expands the range of mechano-exclusive products. The Grubbs 3(rd)-generation complex based on carbene and pyridine catalysts outperforms other catalysts and retains similar mechanistic features as solution-phase reactions. High-speed ball milling provides sufficient mixing and energy to minimize or eliminate the use of solvents. The addition of a small amount of liquid additive enables the synthesis of high-molecular-weight polymers by minimizing chain-degradation.
Article
Chemistry, Multidisciplinary
Gregory Peterson, Tae-Lim Choi
Summary: This Feature Article summarizes recent developments in utilizing polymer architecture to modulate mechanochemical reactions within polymers. Various well-defined architectures have been explored, including cyclic, intramolecularly cross-linked, dendritic, star, bottlebrush, and dendronized polymers. The focus is on describing the enhancement or suppression of mechanochemical reactivity, with respect to analogous linear polymers, as well as differences in solution- and solid-state behavior.
CHEMICAL COMMUNICATIONS
(2021)
Article
Polymer Science
Gregory Peterson, Sanghee Yang, Tae-Lim Choi
Summary: Polymer self-assembly using conjugated polymers, known as INCP, offers a simplified method for obtaining stable nano-objects with various morphologies, which have potential applications in optoelectronics. This approach eliminates the need for challenging post-polymerization treatment steps.
Article
Chemistry, Multidisciplinary
Gregory Peterson, Tae-Lim Choi
