{"title":"Virus adsorption and elution using cationic polymer brushes: potential applications for passive sampling in wastewater-based epidemiology†","authors":"Junya Uchida, Miaomiao Liu, Shizuka Matsuyama, Hiroyuki Katayama and Takashi Kato","doi":"10.1039/D3LP00216K","DOIUrl":"https://doi.org/10.1039/D3LP00216K","url":null,"abstract":"<p >Wastewater-based epidemiology (WBE) has been recognized as a promising approach for rapid monitoring of infectious diseases in local communities. Development of adsorption materials that efficiently capture viruses is important in WBE to provide precise information on the prevalence of viral infections. Herein, ionic polymer brushes are synthesized for the tuning of virus adsorption and elution. Quaternary ammonium-based cationic polymer brushes exhibit higher adsorption of enveloped and nonenveloped viruses than a low-molecular-weight amine adduct. Moreover, efficient and selective elution of Aichivirus from the polymer brushes is demonstrated. These cationic polymer brushes may be useful as materials for passive sampling of viruses from water.</p>","PeriodicalId":101139,"journal":{"name":"RSC Applied Polymers","volume":" 4","pages":" 670-677"},"PeriodicalIF":0.0,"publicationDate":"2024-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/lp/d3lp00216k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141725720","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Chun-Yi Chang, Han Nguyen, Ellen Frahm, Keith Kolaczyk and Chien-Chi Lin
{"title":"Triple click chemistry for crosslinking, stiffening, and annealing of gelatin-based microgels†","authors":"Chun-Yi Chang, Han Nguyen, Ellen Frahm, Keith Kolaczyk and Chien-Chi Lin","doi":"10.1039/D3LP00249G","DOIUrl":"https://doi.org/10.1039/D3LP00249G","url":null,"abstract":"<p >Microgels are spherical hydrogels with physicochemical properties ideal for many biomedical applications. For example, microgels can be used as individual carriers for suspension cell culture or jammed/annealed into granular hydrogels with micron-scale pores highly permissive to molecular transport and cell proliferation/migration. Conventionally, laborious optimization processes are often needed to create microgels with different moduli, sizes, and compositions. This work presents a new microgel and granular hydrogel preparation workflow using gelatin-norbornene-carbohydrazide (GelNB-CH). As a gelatin-derived macromer, GelNB-CH presents cell adhesive and degradable motifs while being amenable to three orthogonal click chemistries, namely the thiol-norbornene photo-click reaction, hydrazone bonding, and the inverse electron demand Diels–Alder (iEDDA) click reaction. The thiol-norbornene photo-click reaction (with thiol-bearing crosslinkers) and hydrazone bonding (with aldehyde-bearing crosslinkers) were used to crosslink the microgels and to realize on-demand microgel stiffening, respectively. The tetrazine-norbornene iEDDA click reaction (with tetrazine-bearing crosslinkers) was used to anneal microgels into granular hydrogels. In addition to materials development, we demonstrated the value of the triple-click chemistry granular hydrogels <em>via</em> culturing human mesenchymal stem cells and pancreatic cancer cells.</p>","PeriodicalId":101139,"journal":{"name":"RSC Applied Polymers","volume":" 4","pages":" 656-669"},"PeriodicalIF":0.0,"publicationDate":"2024-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/lp/d3lp00249g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141725719","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Cuc Thu Mai, Harish Gudla, Guiomar Hernández, Kristina Edström and Jonas Mindemark
{"title":"Inherent limitations of the hydrogen-bonding UPy motif as self-healing functionality for polymer electrolytes†","authors":"Cuc Thu Mai, Harish Gudla, Guiomar Hernández, Kristina Edström and Jonas Mindemark","doi":"10.1039/D4LP00017J","DOIUrl":"https://doi.org/10.1039/D4LP00017J","url":null,"abstract":"<p >The development of advanced materials displaying reversible functionalities, such as self-healing is particularly desirable for energy storage devices, since the cycle life of many rechargeable batteries is limited due to the irreversible mechanical damages over the cycling processes. Hydrogen-bonding self-healing polymers functionalized with ureido pyrimidinone (UPy) has received great interest for energy storage applications, particularly for polymer electrolytes. Herein, we design a star-branched poly(ε-caprolactone-<em>co</em>-trimethylene carbonate) end-capped with UPy groups for both reinforced mechanical and desired self-healing properties in the polymer electrolytes. Despite the versatile implementation and strong bonding association, the benefits of hydrogen-bonding UPy functionalities are diminished after the dissolution of LiTFSI salt in the self-healing polymer matrix. Experimental analysis and molecular dynamics simulations were performed to gain insight into the dynamics of the self-healing polymer electrolyte system. FTIR shows a dramatic decrease in the intensities of the hydrogen-bonded C<img>O signals belonging to UPy motifs after adding LiTFSI salt, indicative of a significant reduction in the total number of hydrogen-bonding and more loosened cross-linked polymer network. This is also noticed as a simultaneous deterioration of the mechanical properties. Molecular dynamics simulations reveal that the complex interplay of C<img>O--Li<small><sup>+</sup></small> coordination bonds and hydrogen bonding between TFSI anions and UPy motifs are responsible for the mechanical deterioration of the self-healing polymer electrolytes.</p>","PeriodicalId":101139,"journal":{"name":"RSC Applied Polymers","volume":" 3","pages":" 374-383"},"PeriodicalIF":0.0,"publicationDate":"2024-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/lp/d4lp00017j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141091265","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Valorization of plastic waste via chemical activation and carbonization into activated carbon for functional material applications","authors":"Rachel Blanchard and Tizazu H. Mekonnen","doi":"10.1039/D4LP00016A","DOIUrl":"https://doi.org/10.1039/D4LP00016A","url":null,"abstract":"<p >Addressing the complex issue of plastic waste disposal requires a nuanced approach, as no single solution proves universally effective. This review advocates for a comprehensive strategy, combining mechanical recycling and chemical methods to manage plastic waste while emphasizing the transformative potential of carbonization and activation processes specifically. With a focus on chemical activation, this review explores the synthesis of high surface area activated carbon (AC) from diverse plastic sources including polyesters (<em>e.g.</em>, polyethylene terephthalate), polyolefins (<em>e.g.</em>, polyethylene, polypropylene), and non-recyclable thermoset resins (<em>e.g.</em>, epoxy, phenolics). The resulting AC products exhibit notable potential, with high surface areas exceeding 2000 m<small><sup>2</sup></small> g<small><sup>−1</sup></small> in some cases. Furthermore, the adsorptive behavior of the plastic derived ACs are discussed with respect to common pollutants such as dyes and CO<small><sub>2</sub></small> in addition to emerging pollutants, such as micro/nano-plastics. Overall, this work highlights carbonization and chemical activation as important upcycling methods for plastic wastes that may otherwise end up in landfills or spills into the environment. Given the urgency of plastic waste disposal, it is recommended that the feasibility and scalability of plastic-derived AC production is explored in future work for the potential replacement of conventional AC feedstocks derived from coal or biomass.</p>","PeriodicalId":101139,"journal":{"name":"RSC Applied Polymers","volume":" 4","pages":" 557-582"},"PeriodicalIF":0.0,"publicationDate":"2024-03-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/lp/d4lp00016a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141725728","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Agnes C. Morrissey, Vishakya Jayalatharachchi, Lukas Michalek, Prasanna Egodawatta, Neomy Zaquen, Laura Delafresnaye and Christopher Barner-Kowollik
{"title":"A bioinspired approach to reversibly metal binding interfaces†","authors":"Agnes C. Morrissey, Vishakya Jayalatharachchi, Lukas Michalek, Prasanna Egodawatta, Neomy Zaquen, Laura Delafresnaye and Christopher Barner-Kowollik","doi":"10.1039/D4LP00010B","DOIUrl":"https://doi.org/10.1039/D4LP00010B","url":null,"abstract":"<p >We introduce a bioinspired materials system that is capable of effectively coating surfaces, while concomitantly allowing metal ions to be reversibly bound. Specifically, we prepare a nitrogen-ligand carrying <small>L</small>-3,4-dihydroxyphenylalanine (<small>L</small>-DOPA) derivate, which can readily crosslink in aqueous systems with effective adhesion onto silicon wafers as well as stone wool fibers. Critically, the introduced system allows for reversible binding of the metal species (such as zinc cations) from aqueous solution. The reversibly binding surfaces are carefully assessed towards their metal ion binding efficiency – in contrast to non-ligand carrying coatings or uncoated surfaces – <em>via</em> surface sensitive analytical methods such as X-ray photoelectron spectroscopy, making them highly attractive candidates for applications in urban storm water filtration systems.</p>","PeriodicalId":101139,"journal":{"name":"RSC Applied Polymers","volume":" 3","pages":" 490-496"},"PeriodicalIF":0.0,"publicationDate":"2024-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/lp/d4lp00010b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141091299","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ellie G. Puente, Rajalakshmi P. Sivasankaran, Daniele Vinciguerra, Jane Yang, Haillie-Ann C. Lower, Andrea L. Hevener and Heather D. Maynard
{"title":"Uniform trehalose nanogels for glucagon stabilization†","authors":"Ellie G. Puente, Rajalakshmi P. Sivasankaran, Daniele Vinciguerra, Jane Yang, Haillie-Ann C. Lower, Andrea L. Hevener and Heather D. Maynard","doi":"10.1039/D3LP00226H","DOIUrl":"https://doi.org/10.1039/D3LP00226H","url":null,"abstract":"<p >Glucagon is a peptide hormone that acts <em>via</em> receptor-mediated signaling predominantly in the liver to raise glucose levels by hepatic glycogen breakdown or conversion of noncarbohydrate, 3 carbon precursors to glucose by gluconeogenesis. Glucagon is administered to reverse severe hypoglycemia, a clinical complication associated with type 1 diabetes. However, due to low stability and solubility at neutral pH, there are limitations in the current formulations of glucagon. Trehalose methacrylate-based nanoparticles were utilized as the stabilizing and solubilizing moiety in the system reported herein. Glucagon was site-selectively modified to contain a cysteine at amino acid number 24 to covalently attach to the methacrylate-based polymer containing pyridyl disulfide side chains. PEG<small><sub>2000</sub></small> dithiol was employed as the crosslinker to form uniform nanoparticles. Glucagon nanogels were monitored in Dulbecco's phosphate-buffered saline (DPBS) pH 7.4 at various temperatures to determine its long-term stability in solution. Glucagon nanogels were stable up to at least 5 months by size uniformity when stored at −20 °C and 4 °C, up to 5 days at 25 °C, and less than 12 hours at 37 °C. When glucagon stability was studied by either HPLC or thioflavin T assays, the glucagon was intact for at least 5 months at −20 °C and 4 °C within the nanoparticles at −20 °C and 4 °C and up to 2 days at 25 °C. Additionally, the glucagon nanogels were studied for toxicity and efficacy using various assays <em>in vitro</em>. The findings indicate that the nanogels were nontoxic to fibroblast cells and nonhemolytic to red blood cells. The glucagon in the nanogels was as active as glucagon alone. These results demonstrate the utility of trehalose nanogels towards a glucagon formulation with improved stability and solubility in aqueous solutions, particularly useful for storage at cold temperatures.</p>","PeriodicalId":101139,"journal":{"name":"RSC Applied Polymers","volume":" 3","pages":" 473-482"},"PeriodicalIF":0.0,"publicationDate":"2024-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/lp/d3lp00226h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141091297","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Ultrathin redox active hydrogel electrolytes for high performance flexible supercapacitors†","authors":"Mengmeng Xun, Xiuting Shi, Haiping Wang, Xiaoyan Li, Wenxing Miao, Xiangbing Wang, Kanjun Sun, Hui Peng, Guofu Ma and Yuxi Xu","doi":"10.1039/D4LP00007B","DOIUrl":"https://doi.org/10.1039/D4LP00007B","url":null,"abstract":"<p >Flexible supercapacitors (FSCs) based on hydrogel electrolytes have the advantages of high ionic conductivity, no liquid leakage, flexibility and versatility, making them the most promising power sources for wearable devices. Herein, a flexible and stretchable, ultrathin polyvinyl alcohol/carboxymethyl chitosan incorporated with a redox active ionic liquid (PVA/CMCS-[ViEtIm][Br]) hydrogel electrolyte is prepared by a facile coating and freezing/thawing method, which is used to improve the practical performance of supercapacitors. The PVA/CMCS-[ViEtIm][Br] hydrogel film has good mechanical properties. More importantly, the redox reaction caused by [ViEtIm][Br] in the hydrogel electrolyte provides a crucial pseudocapacitive contribution to supercapacitors. Thus, the flexible supercapacitor assembled with the PVA/CMCS-[ViEtIm][Br] hydrogel at a thickness of 0.1 mm has an areal specific capacitance of 314.4 mF cm<small><sup>−2</sup></small> and an energy density of 78.6 μWh cm<small><sup>−2</sup></small> at 540 μW cm<small><sup>−2</sup></small>, with a capacitance retention of 87.5% after 10 000 charge/discharge cycles. Moreover, the flexible supercapacitor can also exhibit stable performance at different bending angles. This work provides a simple and feasible method for realizing ultra-thin flexible capacitors with high energy density.</p>","PeriodicalId":101139,"journal":{"name":"RSC Applied Polymers","volume":" 3","pages":" 483-489"},"PeriodicalIF":0.0,"publicationDate":"2024-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/lp/d4lp00007b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141091298","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Malavika Ramkumar, Woojung Ji, Henry E. Thurber, Madeline E. Clough, Sarena Chirdon and Anne J. McNeil
{"title":"Enhancing microplastic capture efficiencies with adhesive coatings on stainless-steel filters†","authors":"Malavika Ramkumar, Woojung Ji, Henry E. Thurber, Madeline E. Clough, Sarena Chirdon and Anne J. McNeil","doi":"10.1039/D3LP00282A","DOIUrl":"https://doi.org/10.1039/D3LP00282A","url":null,"abstract":"<p >Microplastics have been found in our food, water, and air, raising concerns about their potential health impacts. While environmental remediation may be intractable, we should prioritize minimizing our exposure. In this context, an adhesive-coated stainless-steel filter was developed herein to remove microplastics from water.</p>","PeriodicalId":101139,"journal":{"name":"RSC Applied Polymers","volume":" 3","pages":" 456-460"},"PeriodicalIF":0.0,"publicationDate":"2024-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/lp/d3lp00282a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141091272","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Karolina Kasza, Fadi Soukarieh, Manuel Romero, Kim R. Hardie, Pratik Gurnani, Miguel Cámara and Cameron Alexander
{"title":"Triblock copolymer micelles enhance solubility, permeability and activity of a quorum sensing inhibitor against Pseudomonas aeruginosa biofilms†","authors":"Karolina Kasza, Fadi Soukarieh, Manuel Romero, Kim R. Hardie, Pratik Gurnani, Miguel Cámara and Cameron Alexander","doi":"10.1039/D3LP00208J","DOIUrl":"https://doi.org/10.1039/D3LP00208J","url":null,"abstract":"<p >Antimicrobial resistance is a threat to public health for which new treatments are urgently required. The capability of bacteria to form biofilms is of particular concern as it enables high bacterial tolerance to conventional therapies by reducing drug diffusion through the dense, exopolymeric biofilm matrix and the upregulation of antimicrobial resistance machinery. Quorum sensing (QS), a process where bacteria use diffusible chemical signals to coordinate group behaviour, has been shown to be closely interconnected with biofilm formation and bacterial virulence in many top priority pathogens including <em>Pseudomonas aeruginosa</em>. Inhibition of QS pathways therefore pose an attractive target for new therapeutics. We have recently reported a new series of <em>pqs</em> quorum sensing inhibitors (QSIs) that serve as potentiators for antibiotics in <em>P. aeruginosa</em> infections. The impact on biofilms of some reported QSIs was however hindered by their poor penetration through the bacterial biofilm, limiting the potential for clinical translation. In this study we developed a series of poly(β-amino ester) (PBAE) triblock copolymers and evaluated their ability to form micelles, encapsulate a QSI and enhance subsequent delivery to <em>P. aeruginosa</em> biofilms. We observed that the QSI could be released from polymer micelles, perturbing the <em>pqs</em> pathway in planktonic <em>P. aeruginosa</em>. In addition, one of the prepared polymer variants increased the QSIs efficacy, leading to an enhanced potentiation of ciprofloxacin (CIP) action and therefore improved reduction in biofilm viability, compared to the non-encapsulated QSI. Thus, we demonstrate QSI encapsulation in polymeric particles can enhance its efficacy through improved biofilm penetration.</p>","PeriodicalId":101139,"journal":{"name":"RSC Applied Polymers","volume":" 3","pages":" 444-455"},"PeriodicalIF":0.0,"publicationDate":"2024-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/lp/d3lp00208j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141091271","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Priyanka Sahariah, Francesco Papi, Koi L. Merz, Olafur E. Sigurjonsson, Rikke Loiuse Meyer and Cristina Nativi
{"title":"Chitosan–saccharide conjugates for eradication of Pseudomonas aeruginosa biofilms†","authors":"Priyanka Sahariah, Francesco Papi, Koi L. Merz, Olafur E. Sigurjonsson, Rikke Loiuse Meyer and Cristina Nativi","doi":"10.1039/D3LP00263B","DOIUrl":"https://doi.org/10.1039/D3LP00263B","url":null,"abstract":"<p >The problem of antibiotic resistance has raised serious concerns globally and hence the development of new materials which can combat these drug-resistant strains has gained a great deal of attention. Herein, we report the use of a biocompatible material, chitosan, as a scaffold to graft saccharides which can specifically target <em>Pseudomonas aeruginosa</em>. We realized this by synthesizing <em>N</em>-functionalized chitosan conjugates by coupling chitosan to fucose and galactose moieties which intercept <em>Pseudomonas aeruginosa</em> lectins and target the bacterial biofilms. A series of six conjugates containing similar proportions of cationic and sugar moieties were synthesized by direct modification of the chitosan backbone using a method that is highly efficient and reproducible. The conjugates showed a bactericidal effect against both Gram positive and Gram negative bacterial strains. An investigation into the antibiofilm activity of the conjugates revealed the optimum combination of the type and positioning of the functionalities that were highly effective in eradicating <em>Pseudomonas aeruginosa</em> biofilms. 2D and 3D imaging of the conjugate-treated biofilms using confocal laser scanning microscopy (CLSM) allowed us to determine that the conjugates not only acted on the surface but also dispersed into deep layers of the biofilm. Interaction between the conjugates and individual bacterial cells in the biofilm was further confirmed by fluorescence labelling of the conjugates and imaging by CLSM.</p>","PeriodicalId":101139,"journal":{"name":"RSC Applied Polymers","volume":" 3","pages":" 461-472"},"PeriodicalIF":0.0,"publicationDate":"2024-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/lp/d3lp00263b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141091273","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}