Pub Date : 2025-02-10DOI: 10.1021/acs.biomac.4c01802
Olga Lidia Torres-Rocha, Julien Pinaud, Patrick Lacroix-Desmazes, Pascale Champagne, Michael F Cunningham
Cellulose nanocrystals (CNC) offer unique mechanical and optical properties but face challenges that often prevent its commercial development, foremost its high hydrophilicity, which makes it incompatible with most polymers. Covalent polymer graft modification can address this issue; however, these processes are often complex and expensive. We present a simple, inexpensive route for the noncovalent modification of a CNC surface with block copolymers. Five new block copolymers, composed of a butyl vinyl imidazolium bromide anchoring (cationic) and a nonionic stabilizing block, were synthesized via nitroxide-mediated polymerization. The degree of polymerization (DPn) of the stabilizing and anchoring blocks was systematically varied. Dispersibility of modified CNC in various organic solvents was evaluated. It was found that the DPn of both the anchoring and stabilizing blocks has a significant impact on the amount of the polymer that can be noncovalently bound to the CNC surface as well as in dispersibility in various solvents.
{"title":"Cellulose Nanocrystals Modified with Cationic Block Copolymers.","authors":"Olga Lidia Torres-Rocha, Julien Pinaud, Patrick Lacroix-Desmazes, Pascale Champagne, Michael F Cunningham","doi":"10.1021/acs.biomac.4c01802","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01802","url":null,"abstract":"<p><p>Cellulose nanocrystals (CNC) offer unique mechanical and optical properties but face challenges that often prevent its commercial development, foremost its high hydrophilicity, which makes it incompatible with most polymers. Covalent polymer graft modification can address this issue; however, these processes are often complex and expensive. We present a simple, inexpensive route for the noncovalent modification of a CNC surface with block copolymers. Five new block copolymers, composed of a butyl vinyl imidazolium bromide anchoring (cationic) and a nonionic stabilizing block, were synthesized via nitroxide-mediated polymerization. The degree of polymerization (DPn) of the stabilizing and anchoring blocks was systematically varied. Dispersibility of modified CNC in various organic solvents was evaluated. It was found that the DPn of both the anchoring and stabilizing blocks has a significant impact on the amount of the polymer that can be noncovalently bound to the CNC surface as well as in dispersibility in various solvents.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143389496","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-10DOI: 10.1021/acs.biomac.4c01252
Huan Liu, Yang Yu
The development of biobased polyesters with the combination of high UV shielding and degradability is a significant challenge. Herein, three 4-membered cyclic monomers containing two pyrrolidone and two furan rings were prepared by the aza-Michael addition of biobased bifuran diamine and dimethyl itaconate (DMI). They were available in melt polycondensation reactions with various diols to synthesize biobased polyesters. The bifuran structure endowed the polyesters with ultrahigh UV-shielding cutoff values of up to 443 nm, which achieved the highest UV-shielding results among the commercial polyesters. The bipyrrolidone structure conferred high hydrolysis sensitivity to the polyesters, which facilitated hydrolytic degradation of the polyester in an aqueous environment. The variability of the link structure between the multirings of the three monomers can regulate the various properties of the polyesters. Overall, the 4-membered cyclic monomers are promising precursors for sustainable biobased materials in providing high UV shielding and hydrolysis sensitivity.
{"title":"Biobased Polyesters with Ultrahigh UV Shielding and Water Degradation Derived from Multifunctional Tetracyclic Diesters","authors":"Huan Liu, Yang Yu","doi":"10.1021/acs.biomac.4c01252","DOIUrl":"10.1021/acs.biomac.4c01252","url":null,"abstract":"<div><div>The development of biobased polyesters with the combination of high UV shielding and degradability is a significant challenge. Herein, three 4-membered cyclic monomers containing two pyrrolidone and two furan rings were prepared by the aza-Michael addition of biobased bifuran diamine and dimethyl itaconate (DMI). They were available in melt polycondensation reactions with various diols to synthesize biobased polyesters. The bifuran structure endowed the polyesters with ultrahigh UV-shielding cutoff values of up to 443 nm, which achieved the highest UV-shielding results among the commercial polyesters. The bipyrrolidone structure conferred high hydrolysis sensitivity to the polyesters, which facilitated hydrolytic degradation of the polyester in an aqueous environment. The variability of the link structure between the multirings of the three monomers can regulate the various properties of the polyesters. Overall, the 4-membered cyclic monomers are promising precursors for sustainable biobased materials in providing high UV shielding and hydrolysis sensitivity.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (66KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 2","pages":"Pages 943-953"},"PeriodicalIF":5.5,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142925801","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-10DOI: 10.1021/acs.biomac.4c01639
Li Fu , Ya Liu , Jingjing Guo , Xueqing Zhang , Wenqiang Li , Jiayue Zhao , Ziying Zhen , Yu Chen
Green separation of protein (e.g., bovine serum albumin (BSA)) by low-melting mixture solvents (LoMMSs) depends on the underlying mechanism between BSA and LoMMSs. Here, we for the first time find that eco-friendly biomass-derived LoMMSs could be potentially used for the efficient and green purification of BSA protein by enthalpy-driven interactions. Biomass-derived LoMMSs possess the merits of high biocompatibility, high degradability, high abundance, and low cost. A single high-affinity binding site via hydrogen bonding and van der Waals forces is observed between BSA and LoMMSs by fluorescence and thermodynamic analysis. Experimental results from circular dichroism and infrared spectra demonstrate that the addition of LoMMSs stabilizes the secondary structure of the BSA protein. This work provides a valuable indication for the design of eco-friendly and cost-effective LoMMSs for the purification of protein.
{"title":"Enthalpy-Driven Interaction between Bovine Serum Albumin and Biomass-Derived Low-Melting Mixture Solvents (LoMMSs) for Efficient and Green Purification of Protein","authors":"Li Fu , Ya Liu , Jingjing Guo , Xueqing Zhang , Wenqiang Li , Jiayue Zhao , Ziying Zhen , Yu Chen","doi":"10.1021/acs.biomac.4c01639","DOIUrl":"10.1021/acs.biomac.4c01639","url":null,"abstract":"<div><div>Green separation of protein (e.g., bovine serum albumin (BSA)) by low-melting mixture solvents (LoMMSs) depends on the underlying mechanism between BSA and LoMMSs. Here, we for the first time find that eco-friendly biomass-derived LoMMSs could be potentially used for the efficient and green purification of BSA protein by enthalpy-driven interactions. Biomass-derived LoMMSs possess the merits of high biocompatibility, high degradability, high abundance, and low cost. A single high-affinity binding site via hydrogen bonding and van der Waals forces is observed between BSA and LoMMSs by fluorescence and thermodynamic analysis. Experimental results from circular dichroism and infrared spectra demonstrate that the addition of LoMMSs stabilizes the secondary structure of the BSA protein. This work provides a valuable indication for the design of eco-friendly and cost-effective LoMMSs for the purification of protein.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (102KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 2","pages":"Pages 1274-1282"},"PeriodicalIF":5.5,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142941445","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-10DOI: 10.1021/acs.biomac.4c01516
Eugenia Apuzzo , Marilina Cathcarth , Agustín S. Picco , Catalina von Bilderling , Omar Azzaroni , Maximiliano L. Agazzi , Santiago E. Herrera
The study of the phase behavior of polyelectrolyte complex coacervates has attracted significant attention in recent years due to their potential use as membrane-less organelles, microreactors, and drug delivery platforms. In this work, we investigate the mechanism of protein loading in chain-length asymmetric complex coacervates composed of a polyelectrolyte and an oppositely charged multivalent ion. Unlike the symmetric case (polycation + polyanion), we show that protein loading is highly selective based on the protein’s net charge: only proteins with charges opposite to the polyelectrolyte can be loaded. Through a series of systematic experiments, we identified that the protein loading process relies on the formation of a neutral three-component coacervate in which both the protein and the multivalent ion serve as complexing agents for the polyelectrolyte. Lastly, we demonstrated that this mechanism extends to the sequestration of other charged small molecules, offering valuable insights into designing functional multicomponent coacervates.
{"title":"Insights into the Mechanism of Protein Loading by Chain-Length Asymmetric Complex Coacervates","authors":"Eugenia Apuzzo , Marilina Cathcarth , Agustín S. Picco , Catalina von Bilderling , Omar Azzaroni , Maximiliano L. Agazzi , Santiago E. Herrera","doi":"10.1021/acs.biomac.4c01516","DOIUrl":"10.1021/acs.biomac.4c01516","url":null,"abstract":"<div><div>The study of the phase behavior of polyelectrolyte complex coacervates has attracted significant attention in recent years due to their potential use as membrane-less organelles, microreactors, and drug delivery platforms. In this work, we investigate the mechanism of protein loading in chain-length asymmetric complex coacervates composed of a polyelectrolyte and an oppositely charged multivalent ion. Unlike the symmetric case (polycation + polyanion), we show that protein loading is highly selective based on the protein’s net charge: only proteins with charges opposite to the polyelectrolyte can be loaded. Through a series of systematic experiments, we identified that the protein loading process relies on the formation of a neutral three-component coacervate in which both the protein and the multivalent ion serve as complexing agents for the polyelectrolyte. Lastly, we demonstrated that this mechanism extends to the sequestration of other charged small molecules, offering valuable insights into designing functional multicomponent coacervates.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (160KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 2","pages":"Pages 1171-1183"},"PeriodicalIF":5.5,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142976832","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-10DOI: 10.1021/acs.biomac.4c01168
Carlo Kupfernagel , Mohammed Rahman , Rosalie Cresswell , Morwenna J. Spear , Andrew Pitman , Steven P. Brown , Graham A. Ormondroyd
Wood modification using low molecular weight thermosetting resins improves the biological durability and dimensional stability of wood while avoiding increasingly regulated biocides. During the modification process, resin monomers diffuse from the cell lumen to the cell wall, occupying micropore spaces before in situ curing at 150 °C. This study investigated the mechanism of cell wall diffusion at multiple scales, comparing two test groups where diffusion was either facilitated or restricted. Antiswelling efficiency tests demonstrated improved dimensional stability when diffusion was facilitated. Differential scanning calorimetry showed that bound water was excluded more effectively from the cell wall if cell wall diffusion was enabled. Solid-state NMR spectroscopy (1H MAS and 13C MAS) with relaxation time analysis indicated that resin migrated to distinct locations within the cell wall, influenced by diffusion and drying conditions. These findings highlight how optimizing cell wall diffusion can significantly improve the performance of wood modification processes using thermosetting resins.
{"title":"Investigating Cell Wall Diffusion in Wood Modified with Phenol Urea Formaldehyde Resin in Different Length Scales","authors":"Carlo Kupfernagel , Mohammed Rahman , Rosalie Cresswell , Morwenna J. Spear , Andrew Pitman , Steven P. Brown , Graham A. Ormondroyd","doi":"10.1021/acs.biomac.4c01168","DOIUrl":"10.1021/acs.biomac.4c01168","url":null,"abstract":"<div><div>Wood modification using low molecular weight thermosetting resins improves the biological durability and dimensional stability of wood while avoiding increasingly regulated biocides. During the modification process, resin monomers diffuse from the cell lumen to the cell wall, occupying micropore spaces before <em>in situ</em> curing at 150 °C. This study investigated the mechanism of cell wall diffusion at multiple scales, comparing two test groups where diffusion was either facilitated or restricted. Antiswelling efficiency tests demonstrated improved dimensional stability when diffusion was facilitated. Differential scanning calorimetry showed that bound water was excluded more effectively from the cell wall if cell wall diffusion was enabled. Solid-state NMR spectroscopy (<sup>1</sup>H MAS and <sup>13</sup>C MAS) with relaxation time analysis indicated that resin migrated to distinct locations within the cell wall, influenced by diffusion and drying conditions. These findings highlight how optimizing cell wall diffusion can significantly improve the performance of wood modification processes using thermosetting resins.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (77KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 2","pages":"Pages 900-913"},"PeriodicalIF":5.5,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11825066/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142976836","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-10DOI: 10.1021/acs.biomac.4c01545
Xuelian Hu , Sai Li , Yuji Pu , Bin He
Hemostasis is the initial step in wound healing, yet significant challenges, such as massive bleeding and infection, often arise. In this study, we developed amphiphilic biodegradable polyester-based segmented polyurethane (SPU) microspheres modified with epigallocatechin gallate (EGCG)-Ag nanoparticles and calcium-alginate cross-linking shell, combining blood absorption with the pro-coagulation properties of Ca2+ and the negative charge of EGCG for synergistic hemostatic effects across various stages of the coagulation cascade. The in vitro blood clotting time of the SPU@EAg@CaAlg microsphere (328.7 s) was reduced by half compared to the SPU microsphere (685.0 s). SPU@EAg@CaAlg exhibited a reduced hemostatic time and blood loss in three rat hemostatic models. Additionally, EGCG-Ag nanoparticles imparted strong antibacterial and anti-inflammatory properties both in vitro and in vivo. In vivo infected wound model demonstrated that SPU@EAg@CaAlg effectively eliminated bacteria and reduced the levels of pro-inflammatory factors, thereby promoting wound healing. Thus, the modified SPU microspheres present a promising candidate for effective hemostatic applications.
{"title":"Biodegradable Polymeric Microspheres with Enhanced Hemostatic and Antibacterial Properties for Wound Healing","authors":"Xuelian Hu , Sai Li , Yuji Pu , Bin He","doi":"10.1021/acs.biomac.4c01545","DOIUrl":"10.1021/acs.biomac.4c01545","url":null,"abstract":"<div><div>Hemostasis is the initial step in wound healing, yet significant challenges, such as massive bleeding and infection, often arise. In this study, we developed amphiphilic biodegradable polyester-based segmented polyurethane (SPU) microspheres modified with epigallocatechin gallate (EGCG)-Ag nanoparticles and calcium-alginate cross-linking shell, combining blood absorption with the pro-coagulation properties of Ca<sup>2+</sup> and the negative charge of EGCG for synergistic hemostatic effects across various stages of the coagulation cascade. The in vitro blood clotting time of the SPU@EAg@CaAlg microsphere (328.7 s) was reduced by half compared to the SPU microsphere (685.0 s). SPU@EAg@CaAlg exhibited a reduced hemostatic time and blood loss in three rat hemostatic models. Additionally, EGCG-Ag nanoparticles imparted strong antibacterial and anti-inflammatory properties both in vitro and in vivo. In vivo infected wound model demonstrated that SPU@EAg@CaAlg effectively eliminated bacteria and reduced the levels of pro-inflammatory factors, thereby promoting wound healing. Thus, the modified SPU microspheres present a promising candidate for effective hemostatic applications.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (92KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 2","pages":"Pages 1207-1218"},"PeriodicalIF":5.5,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142996198","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-10DOI: 10.1021/acs.biomac.4c01544
Ying Luo , Yiping Zhao , Li Chen , Ying Guan , Yongjun Zhang
Antioxidant hydrogels that can provide a moist environment and scavenge reactive oxygen species have emerged as highly potential wound dressing materials. In situ-forming and good tissue adhesiveness will make them more desirable, as they can fill the irregular wound defect, stick to the wound, and offer intimate contact with the wound. Herein, a hydrogel dressing combining in situ-forming, good tissue adhesiveness, and excellent antioxidant capabilities was developed by simply conjugating dopamine onto carboxymethyl chitosan. The introduction of dopamine allows in situ gelation of the polymer under mild conditions using an HRP-catalyzed cross-linking reaction. The introduction of dopamine also endows the hydrogels with suitable tissue-adhesion properties. Excellent antioxidant properties were also imparted as a result of the introduction of dopamine. Thanks to the favorable moist environment provided by the hydrogel and the effectively mitigated oxidative stress at wound sites, accelerated healing and reduced scar formation were observed in a rat full-thickness skin wound model.
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{"title":"In Situ-Forming, Adhesive, and Antioxidant Chitosan Hydrogels for Accelerated Wound Healing","authors":"Ying Luo , Yiping Zhao , Li Chen , Ying Guan , Yongjun Zhang","doi":"10.1021/acs.biomac.4c01544","DOIUrl":"10.1021/acs.biomac.4c01544","url":null,"abstract":"<div><div>Antioxidant hydrogels that can provide a moist environment and scavenge reactive oxygen species have emerged as highly potential wound dressing materials. In situ-forming and good tissue adhesiveness will make them more desirable, as they can fill the irregular wound defect, stick to the wound, and offer intimate contact with the wound. Herein, a hydrogel dressing combining in situ-forming, good tissue adhesiveness, and excellent antioxidant capabilities was developed by simply conjugating dopamine onto carboxymethyl chitosan. The introduction of dopamine allows in situ gelation of the polymer under mild conditions using an HRP-catalyzed cross-linking reaction. The introduction of dopamine also endows the hydrogels with suitable tissue-adhesion properties. Excellent antioxidant properties were also imparted as a result of the introduction of dopamine. Thanks to the favorable moist environment provided by the hydrogel and the effectively mitigated oxidative stress at wound sites, accelerated healing and reduced scar formation were observed in a rat full-thickness skin wound model.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (58KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 2","pages":"Pages 1219-1233"},"PeriodicalIF":5.5,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143057536","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-10DOI: 10.1021/acs.biomac.4c01273
Sagar Bag , Arunava Seth , Desoshree Ghosh , Rupak Datta , Priyadarsi De
The present investigation aims to develop a reactive oxygen species (ROS) and esterase-responsive biodegradable mannosylated polyurethane to effectively deliver the encapsulated antileishmanial drug amphotericin B (AmB) selectively to infected macrophage cells. Owing to suitable amphiphilic balance, the as-synthesized glycosylated polyurethane (PU2M) with aryl boronic ester-based diol (M2) moiety as ROS-trigger, water-soluble mannose pendants, and fluorescent 4,4-difluoro-4-bora-3a,4a-diaza-s-indacene (BODIPY) chain ends for bioimaging formed nanoaggregates in an aqueous medium as confirmed by 1H NMR spectroscopy, dynamic light scattering (DLS), field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), and critical aggregation concentration (CAC) measurements. Aided by two endogenous stimuli present in phagolysosome, ROS and esterase, AmB-encapsulated polymeric nanoaggregates as drug delivery vehicles achieved an efficient reduction of both L. donovani and L. major intracellular amastigote burden compared to the free AmB. Overall, this work illustrated a promising therapeutic application of dual endogenous stimuli-triggered degradable theranostic polyurethane for target-specific drug delivery of AmB, to mitigate leishmaniasis.
{"title":"Degradable Theranostic Polyurethane for Macrophage-Targeted Antileishmanial Drug Delivery","authors":"Sagar Bag , Arunava Seth , Desoshree Ghosh , Rupak Datta , Priyadarsi De","doi":"10.1021/acs.biomac.4c01273","DOIUrl":"10.1021/acs.biomac.4c01273","url":null,"abstract":"<div><div>The present investigation aims to develop a reactive oxygen species (ROS) and esterase-responsive biodegradable mannosylated polyurethane to effectively deliver the encapsulated antileishmanial drug amphotericin B (AmB) selectively to infected macrophage cells. Owing to suitable amphiphilic balance, the as-synthesized glycosylated polyurethane (<strong>PU2M</strong>) with aryl boronic ester-based diol (<strong>M2</strong>) moiety as ROS-trigger, water-soluble mannose pendants, and fluorescent 4,4-difluoro-4-bora-3a,4a-diaza-<em>s</em>-indacene (BODIPY) chain ends for bioimaging formed nanoaggregates in an aqueous medium as confirmed by <sup>1</sup>H NMR spectroscopy, dynamic light scattering (DLS), field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), and critical aggregation concentration (CAC) measurements. Aided by two endogenous stimuli present in phagolysosome, ROS and esterase, AmB-encapsulated polymeric nanoaggregates as drug delivery vehicles achieved an efficient reduction of both L. donovani and L. major intracellular amastigote burden compared to the free AmB. Overall, this work illustrated a promising therapeutic application of dual endogenous stimuli-triggered degradable theranostic polyurethane for target-specific drug delivery of AmB, to mitigate leishmaniasis.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (142KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 2","pages":"Pages 967-980"},"PeriodicalIF":5.5,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142925802","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-10DOI: 10.1021/acs.biomac.4c01467
Dallin L. Smith , Danixa Rodriguez-Melendez , Maya D. Montemayor , Miguel O. Convento , Jaime C. Grunlan
Chitosan is one of the most abundant biopolymers on earth. It is used as a nontoxic alternative in a wide range of medicines, packaging, adhesives, and flame retardants. Chitosan is poorly soluble in neutral or alkaline solutions, but it dissolves in solutions of weak acids, such as acetic acid or citric acid, both of which occur naturally. As a replacement for formaldehyde-containing resins in engineered wood, a chitosan-acid mixture acts as a low-cost, nontoxic adhesive for natural wood that also offers fire protection by forming a char barrier. Pentaerythritol was studied as an additive due to its similarity to glycerol (a common plasticizer for chitosan) and its potential flame retardant benefit. The properties of chitosan adhesives produced with acetic acid and citric acid are compared, and moderate thermal treatment is applied to facilitate covalent bonding (e.g., Maillard reaction) that improves water resistance. Tensile shear strengths of >1 MPa are obtained on lap joints. The unique combination of fire protection and adhesion for wood makes these low cost, biobased systems very appealing.
{"title":"Fire Resistant Adhesive from Chitosan","authors":"Dallin L. Smith , Danixa Rodriguez-Melendez , Maya D. Montemayor , Miguel O. Convento , Jaime C. Grunlan","doi":"10.1021/acs.biomac.4c01467","DOIUrl":"10.1021/acs.biomac.4c01467","url":null,"abstract":"<div><div>Chitosan is one of the most abundant biopolymers on earth. It is used as a nontoxic alternative in a wide range of medicines, packaging, adhesives, and flame retardants. Chitosan is poorly soluble in neutral or alkaline solutions, but it dissolves in solutions of weak acids, such as acetic acid or citric acid, both of which occur naturally. As a replacement for formaldehyde-containing resins in engineered wood, a chitosan-acid mixture acts as a low-cost, nontoxic adhesive for natural wood that also offers fire protection by forming a char barrier. Pentaerythritol was studied as an additive due to its similarity to glycerol (a common plasticizer for chitosan) and its potential flame retardant benefit. The properties of chitosan adhesives produced with acetic acid and citric acid are compared, and moderate thermal treatment is applied to facilitate covalent bonding (e.g., Maillard reaction) that improves water resistance. Tensile shear strengths of >1 MPa are obtained on lap joints. The unique combination of fire protection and adhesion for wood makes these low cost, biobased systems very appealing.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (81KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 2","pages":"Pages 1141-1148"},"PeriodicalIF":5.5,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11815856/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142929890","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-10DOI: 10.1021/acs.biomac.4c01334
Lei Wang, Yue Wang, Simin Peng, Shuangyan Li, Silong Wu
Silk fibroin (SF) hydrogel has been proven to have excellent applications in the field of pressure sensors, but its sensing performance still needs improvement. A flexible hydrogel prepared from natural macromolecular materials was developed, and lignin nanoparticles (LNPs) were introduced during the preparation of the SF hydrogel. When LNPs account for 3% of SF, the sensing unit of the SF-LNPs3% hydrogel exhibits high stress sensitivity (1.32 kPa–1), fast response speed (<0.1 s), and superior cycle stability (≥8000 cycles). The sensor can detect human motion information, such as finger bending, elbow bending, and pulse signals. When worn at the vocal cord position, it can detect the peak value of the characteristic signal during the wearer speaks. This work demonstrates that the SF-LNPs3% hydrogel has high sensitivity and shows great potential in the field of pressure sensors.
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