Dong Wu, Jie Zhu, Jiayin Xu, Xinran Zhao, Oushuo Jiang, Xiayun Huang, Zhihong Nie, Daoyong Chen
{"title":"Recyclable Amphiphilic Magnetic-responsive Mixed-Shell Nanoparticles With High Interfacial Activity Comparable to Janus Particles for Oily Water Purification.","authors":"Dong Wu, Jie Zhu, Jiayin Xu, Xinran Zhao, Oushuo Jiang, Xiayun Huang, Zhihong Nie, Daoyong Chen","doi":"10.1002/marc.202400734","DOIUrl":"https://doi.org/10.1002/marc.202400734","url":null,"abstract":"<p><p>Amphiphilic magnetic-responsive mixed-shell nanoparticles (Mag-MSNPs) with tailorable compositions are synthesized by electrostatic-mediated cross-linking of core-forming blocks of two diblock copolymers, followed by in situ growth of magnetite in the cross-linked core. The Mag-MSNPs have a magnetic-responsive core and hydrophilic/lipophilic mixed shells, firmly anchoring at the oil-water interface of emulsified oil droplets due to their high interfacial activity (13.1 mN m<sup>-1</sup> at a rather low emulsifier concentration of 1.2 mg mL<sup>-1</sup> in the n-hexane/water system), outperforming most of Janus particles. Driven by the magnetic field, the emulsified oil droplets with Mag-MSNPs at the interface are drawn to one side for collection. The oil-water separation efficiency reaches 99.5%, manifesting their excellent ability to remove emulsified oil droplets from oily water. After five separation and regeneration cycles, the separation efficiency remains at 98.8%, showcasing their potential for recyclable oily water purification.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e2400734"},"PeriodicalIF":4.2,"publicationDate":"2024-11-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142694926","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sarah R Sergi, James J Hastie, Finlay J M Smith, Abigail G Devlin, Elizabeth G Bury, Mara L Paterson, Sophia B Kosednar, Lauren S Sefcik, Melissa B Gordon
{"title":"Swelling-Shrinking Behavior of a Hydrogel with a CO<sub>2</sub>-Switchable Volume Phase Transition Temperature.","authors":"Sarah R Sergi, James J Hastie, Finlay J M Smith, Abigail G Devlin, Elizabeth G Bury, Mara L Paterson, Sophia B Kosednar, Lauren S Sefcik, Melissa B Gordon","doi":"10.1002/marc.202400772","DOIUrl":"https://doi.org/10.1002/marc.202400772","url":null,"abstract":"<p><p>Macromolecules exhibit rich phase behavior that may be exploited for advanced material design. In particular, the volume phase transition in certain crosslinked hydrogels is a key property controlling the transition between a collapsed/dehydrated and a swollen/hydrated state, thereby regulating the release and absorption of water via a temperature change. In this work, a simple and tunable system exhibiting a carbon dioxide (CO<sub>2</sub>)-switchable volume phase transition is introduced, which displays isothermal swelling-shrinking behavior that is activated by addition and removal of CO<sub>2,</sub> respectively. Through systematic compositional studies, shifts in phase transition temperatures of up to 8.6 °C are measured upon CO<sub>2</sub> exposure, which enables pronounced isothermal swelling in response to CO<sub>2</sub>, reaching up to a fivefold increase in mass. The shift in transition temperature and the extent of swelling are controlled by the hydrogel composition, thus enabling the transition temperature and swelling degree to be tuned a priori for a particular application. Controlled release experiments from these gels upon a CO<sub>2</sub>-induced phase transition suggest viability for drug delivery applications. It is anticipated that this work will motivate and expand efforts to exploit phase behavior for smart material development.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e2400772"},"PeriodicalIF":4.2,"publicationDate":"2024-11-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142694929","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Stretchable and Self-Adhesive Conductors for Smart Epidermal Electronics.","authors":"Lin Wang, Desheng Kong","doi":"10.1002/marc.202400774","DOIUrl":"https://doi.org/10.1002/marc.202400774","url":null,"abstract":"<p><p>Epidermal electronics utilize deformable devices that are seamlessly integrated into the body for various cutting-edge applications. Stretchable conductors are essential for creating electrodes in these devices, allowing them to interface with the skin for sensing and stimulation. Despite considerable progress in improved deformability, these conductors may not easily adhere to the skin for long-term use. There is a growing interest in imparting self-adhesive properties to epidermal devices to ensure secure integration with the body. This article focuses on the emerging field of stretchable and self-adhesive conductors. It explores the design strategy required to enable stretchability and conformability in these materials and discusses their pivotal applications in smart epidermal electronics. Additionally, this article also addresses the current challenges and future directions in this dynamic area of research.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e2400774"},"PeriodicalIF":4.2,"publicationDate":"2024-11-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142694927","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yuhan Qiao, Dongxin Li, Qianqian Liang, Ming Kang, Yewei Xu, Li Yang, Guanjun Chang
{"title":"Large-scale Conformational Changes of Diindole Functional Groups Driven by Cation-π Interactions and the Toughening Mechanism of Thermosets.","authors":"Yuhan Qiao, Dongxin Li, Qianqian Liang, Ming Kang, Yewei Xu, Li Yang, Guanjun Chang","doi":"10.1002/marc.202400823","DOIUrl":"https://doi.org/10.1002/marc.202400823","url":null,"abstract":"<p><p>This is described that a new concept for the design of toughening supramolecular thermosets by incorporating diindole groups, which are functionalized via cation-π interactions in covalently crosslinked networks. Large-scale conformational changes of the diindole functional groups could occur under external forces, endowing the thermosets with excellent toughening properties.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e2400823"},"PeriodicalIF":4.2,"publicationDate":"2024-11-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142694924","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"The Trade-Off between Dechlorination and Polymerization for Facile Fabrication of Electronic Grade Epoxidized Cardol.","authors":"Fengyan Zhang, Zihao Tian, Liangyong Chu, Wenxiao Lv, Liming Shen, Xiaoyan Zhang, Xiaobao Li, Ningzhong Bao","doi":"10.1002/marc.202400489","DOIUrl":"https://doi.org/10.1002/marc.202400489","url":null,"abstract":"<p><p>The dechlorination of epoxidized Cardol (E-Cardol), which is a high-performance and sustainable adhesive and packaging material for electronics, remains challenging. The previous work proposed a new alcohol-sodium refining method to efficiently remove the chlorine of E-Cardol. However, this method is strongly limited by the trade-off between the dechlorination efficiency and its polymerization side effect, which leads to the viscosity as well as the epoxy equivalent increase of E-Cardol. Based on the detailed analysis of the refining process using fourier transform infrared spectroscopy (FTIR), simultaneous thermal analysis (STA), and nuclear magnetic resonance spectrometer (NMR) epoxidized Cardol (E-Cardol), this trade-off is studied. It is found that the dechlorination efficiency increases with the increase of the usage of the alcohol sodium. Meanwhile, when the residual alcohol-sodium content after refining exceeds 3000 ppm, the viscosity of the E-Cardol increases significantly due to the increased polymerization of E-Cardol by epoxy ring-opening reaction. It is demonstrated that the alcohol-sodium refining method can efficiently reduce the chlorine content of E-Cardol with the initial hydrolyzable chlorine content not higher than 3000 ppm to below 300 ppm without influencing their epoxy equivalent and viscosity. This paper thoroughly explores the mechanism and application range of the proposed alcohol-sodium refining method, which is crucial for the facile preparation of electronic-grade E-Cardol materials.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e2400489"},"PeriodicalIF":4.2,"publicationDate":"2024-11-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142694931","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yuanbo Liu, Yi Lu, Yuxin Hou, Xiao Xiao, Huijuan Yue, Xiaoming Liu
{"title":"Fully Conjugated Microporous Polymers as Metal-Free Heterogeneous Photocatalysts for Organic Transformations.","authors":"Yuanbo Liu, Yi Lu, Yuxin Hou, Xiao Xiao, Huijuan Yue, Xiaoming Liu","doi":"10.1002/marc.202400743","DOIUrl":"https://doi.org/10.1002/marc.202400743","url":null,"abstract":"<p><p>Photoactive conjugated microporous polymers (CMPs) have recently received huge attention in photocatalytic organic transformations owing to their adjustable structure and functionality. However, commonly reported CMPs are synthesized through metal catalyzed coupling reactions, which require complicated product separation and result in increased costs. In this study, two sp<sup>2</sup> carbon-linked CMPs are constructed by organic base induced Knoevenagel reaction using 2,6-dimethylbenzo[1,2-d:4,5-d']bisoxazole and aromatic polyaldehydes as co-monomers. The new benzobisoxazole-based polymer materials feature fully π-conjugated skeleton with broad visible-light absorption, permanent porosity as well as outstanding stability. Importantly, they can effectively induce many organic reactions such as C-3 thiocyanation of indoles under visible-light illumination and show broad substrate applicability and superior recyclability.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e2400743"},"PeriodicalIF":4.2,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142685459","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Giovanni Mattiotti, Manuel Micheloni, Lorenzo Petrolli, Lorenzo Rovigatti, Luca Tubiana, Samuela Pasquali, Raffaello Potestio
{"title":"Molecular Dynamics Characterization of the Free and Encapsidated RNA2 of CCMV with the oxRNA Model.","authors":"Giovanni Mattiotti, Manuel Micheloni, Lorenzo Petrolli, Lorenzo Rovigatti, Luca Tubiana, Samuela Pasquali, Raffaello Potestio","doi":"10.1002/marc.202400639","DOIUrl":"https://doi.org/10.1002/marc.202400639","url":null,"abstract":"<p><p>The cowpea chlorotic mottle virus (CCMV) has emerged as a model system to assess the balance between electrostatic and topological features of single-stranded RNA viruses, specifically in the context of the viral self-assembly. Yet, despite its biophysical significance, little structural data on the RNA content of the CCMV virion is available. Here, the conformational dynamics of the RNA2 fragment of CCMV was assessed via coarse-grained molecular dynamics simulations, employing the oxRNA2 force field. The behavior of RNA2 was characterized both as a freely-folding molecule and within a mean-field depiction of the capsid. For the former, the role of the salt concentration, the temperature and of ad hoc constraints on the RNA termini was verified on the equilibrium properties of RNA2. For the latter, a multi-scale approach was employed to derive a potential profile of the viral cavity from atomistic structures of the CCMV capsid in solution. The conformational ensembles of the encapsidated RNA2 were significantly altered with respect to the freely-folding counterparts, as shown by the emergence of long-range motifs and pseudoknots. Finally, the role of the N-terminal tails of the CCMV subunits is highlighted as a critical feature in the construction of a proper electrostatic model of the CCMV capsid.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e2400639"},"PeriodicalIF":4.2,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142685465","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sandra Kalem, David Siefker, Mingsheng Ji, Jean-Michel Guigner, Ralf Schweins, Sandrine Pensec, Jutta Rieger, Laurent Bouteiller, Erwan Nicol, Olivier Colombani
{"title":"Supramolecular Janus Nanocylinders: Controlling Their Characteristics by the Self-Assembly Process.","authors":"Sandra Kalem, David Siefker, Mingsheng Ji, Jean-Michel Guigner, Ralf Schweins, Sandrine Pensec, Jutta Rieger, Laurent Bouteiller, Erwan Nicol, Olivier Colombani","doi":"10.1002/marc.202400492","DOIUrl":"https://doi.org/10.1002/marc.202400492","url":null,"abstract":"<p><p>Janus NanoRods (JNR) are anisotropic and non-symmetrical colloids with two faces of different chemical composition. They are difficult to prepare because of their nanometric dimensions and strong anisotropy. Recently, a versatile strategy was developed, allowing the formation of JNR relying on the self-assembly in aqueous medium of two polymers end-functionalized with non-symmetrical and complementary hydrogen bonding stickers. However, the supramolecular JNR prepared following this strategy are out-of-equilibrium (frozen) and therefore their characteristics depend on the self-assembly process. The present study elucidates the formation mechanism of the JNR and the parameters of the self-assembly process influencing their characteristics. The polymers are initially dissolved as unimers in DMSO. Dropwise addition of water triggers the rapid assembly of more and more unimers into long nanocylinders that are unable to grow anymore once formed. Consequently, increasing the dropwise addition rate of water hardly impacts the process, whereas lowering the initial polymer concentration in DMSO reduces both the length and proportion of nanocylinders. Increasing temperature during water addition weakens hydrogen bonds, triggering the formation of a mixture of spheres and nanocylinders. Many supramolecular polymer assemblies are frozen in solution and these findings should help understanding how to control their characteristics, allowing to adapt them to a target application.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e2400492"},"PeriodicalIF":4.2,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142680153","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Thermal Treatment Induced Crystal Development and Crystal Orientation Change in Electrospun Coaxial Fibers Comprising Dual Crystalline Polymers.","authors":"Yu-Rong Hu, Hsin-Yu Lin, Chieh-Tsung Lo","doi":"10.1002/marc.202400731","DOIUrl":"10.1002/marc.202400731","url":null,"abstract":"<p><p>This study investigates the crystallization behavior of electrospun coaxial fibers composed of crystalline poly(ethylene oxide) (PEO) in the core and crystalline poly(L-lactide) (PLLA) in the sheath. The influence of cold crystallization temperature and premelting temperature on the crystallization of PEO and PLLA is investigated. At a cold crystallization temperature of ≤60 °C, PLLA remained immobile. PEO crystallization is hard-confined, leading to a low degree of crystallinity. At a cold crystallization temperature of >60 °C, PEO melted, whereas PLLA crystallized. An increase in cold crystallization temperature results in an increase in the crystallite size and crystallinity of PLLA. Furthermore, the melt crystallization behavior of PEO in the coaxial fibers is strongly influenced by its premelting temperature and crystallization temperature. A higher premelting temperature leads to enhanced interdiffusion between PEO and PLLA. This increased confinement results in a decrease in PEO's crystallizability. Additionally, premelting relaxes the PEO chains, causing a shift in crystal orientation from parallel to the fiber axis (observed in as-electrospun fibers) to perpendicular to the fiber axis (observed in melt-crystallized fibers). Moreover, at a low melt crystallization temperature, demixing between PEO and PLLA is observed. This, coupled with a higher degree of supercooling, leads to an increase in PEO's crystallizability.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e2400731"},"PeriodicalIF":4.2,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142666168","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yirixiatijiang Amier, Wenke Ji, Yang Xun, Xiao Yu, Zhiyuan Zhu, Jingyi Rao
{"title":"pH-Responsive Protein-Polycation Nanocarriers for Efficient Eradication of Bacterial Biofilms and Intracellular Bacteria.","authors":"Yirixiatijiang Amier, Wenke Ji, Yang Xun, Xiao Yu, Zhiyuan Zhu, Jingyi Rao","doi":"10.1002/marc.202400809","DOIUrl":"10.1002/marc.202400809","url":null,"abstract":"<p><p>Bacterial biofilms and intracellular pathogens pose significant challenges in eradication, often leading to persistent infections that are difficult to treat. To address this issue, the hydrophobic biofilm dispersant D-tyrosine is encapsulated within protein-polycation nanoparticles, designed using a mannose-terminated cationic polymer and concanavalin through electrostatic interactions. Thermodynamic studies reveal that free mannosyl groups on the nanoparticle surface promote spontaneous binding to receptor molecules mimicking those on bacterial biofilms and host cells. Under mildly acidic conditions, the nanoparticles reduce in size from 550 to ≈48 nm within 2 h, releasing 76% of encapsulated D-tyrosine. The combination of mannose targeting, particle size reduction, and controlled D-tyrosine release enable the nanoparticles to eliminate 70%-80% of the Pseudomonas aeruginosa and Staphylococcus aureus biofilm biomass at minimum bactericidal concentration (MBC) and 2MBC while eradicating 8 log of bacteria embedded within the biofilm. In an intracellular Pseudomonas aeruginosa infection model using RAW 264.7 macrophages, the nanoparticles at 2MBC eliminate over 95% of the intracellular bacteria without inducing an increase in the inflammatory cytokine interleukin-6. These protein-polycation nanoparticles, which activate their antimicrobial properties under acidic conditions, efficiently penetrate bacterial biofilms and host cell barriers via their mannose-rich surface, offering a promising strategy for the treatment of persistent infections.</p>","PeriodicalId":205,"journal":{"name":"Macromolecular Rapid Communications","volume":" ","pages":"e2400809"},"PeriodicalIF":4.2,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646384","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}