Biomacromolecules最新文献_第8页

Programmable Fabrics of Enzyme-Responsive Amphiphiles: A Multiscale Platform for Hierarchical Mesophase Transformations 酶反应性两亲植物的可编程结构：分层中间相转化的多尺度平台。

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-06-09 DOI: 10.1021/acs.biomac.4c01649

Nicole Edelstein-Pardo , Shira Kutchinsky , Amit Sitt , Roey J. Amir

{"title":"Programmable Fabrics of Enzyme-Responsive Amphiphiles: A Multiscale Platform for Hierarchical Mesophase Transformations","authors":"Nicole Edelstein-Pardo , Shira Kutchinsky , Amit Sitt , Roey J. Amir","doi":"10.1021/acs.biomac.4c01649","DOIUrl":"10.1021/acs.biomac.4c01649","url":null,"abstract":"<div><div>Systems capable of undergoing a controlled cascade of mesophase transitions across hierarchical scales represent a novel class of dynamic materials. Here, we describe an electrospun polymeric fabric composed of enzyme-responsive di- and triblock copolymers that undergoes a hierarchical cascade of four distinct mesophases. Initially, on immersion in water, the macroscale fabric dissolves, forming nanoscale micelles. Enzymatic degradation of the diblock components triggers a transition into a triblock-based hydrogel. Finally, the enzymatic degradation of the hydrogel into hydrophilic polymers leads to complete dissolution. By adjusting the di- and triblock ratios, we can finely tune the fabric’s dissolution rate. Moreover, the fibers can encapsulate hydrophobic agents, which are retained within the micelle and hydrogel phases, enabling their controlled release. This cascade of mesophase transitions, from a macroscopic solid to nanoscale assemblies, organized hydrogels, and eventual molecular dissolution, demonstrates sophisticated hierarchical control, unlocking new opportunities for biomedical applications of programmable materials.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (84KB)</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 6","pages":"Pages 3281-3290"},"PeriodicalIF":5.5,"publicationDate":"2025-06-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143955842","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}

引用次数: 0

Polydopamine-Modified Composite Bone Cement for Cancellous Bone Repair: Synergism of Bioactivity, Antibacterial Properties, and Biodegradability 用于松质骨修复的多多巴胺改性复合骨水泥：生物活性、抗菌性能和生物降解性的协同作用。

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-06-09 DOI: 10.1021/acs.biomac.5c00157

Yalan Ouyang , Rongguang Zhang , Qiyi Zhang , Yonggang Yan

{"title":"Polydopamine-Modified Composite Bone Cement for Cancellous Bone Repair: Synergism of Bioactivity, Antibacterial Properties, and Biodegradability","authors":"Yalan Ouyang , Rongguang Zhang , Qiyi Zhang , Yonggang Yan","doi":"10.1021/acs.biomac.5c00157","DOIUrl":"10.1021/acs.biomac.5c00157","url":null,"abstract":"<div><div>Infection-prone bone defects require multifunctional materials. We developed a novel degradable composite bone cement: polydopamine-modified calcium polyphosphate (CPP@PDA) combined with tricalcium silicate (C<sub>3</sub>S). CPP@PDA provides bioactivity and antibacterial effects, while C<sub>3</sub>S ensures sustained bioactive ion release. The cement exhibited >74% antibacterial efficacy (Staphylococcus aureus, Escherichia coli), with bacterial survival at 15.9 ± 1.2% and 26.1 ± 0.8%. Controlled degradation released Ca<sup>2+</sup> and silicon species, stimulating osteogenesis, shown by increased alkaline phosphatase (ALP) activity and upregulated <em>RUNX2</em>, <em>COL1</em>, and <em>OPN</em> markers. The material also demonstrated antioxidant and antiinflammatory properties, reducing oxidative stress and modulating immune responses to support bone regeneration. This CPP@PDA composite cement, with synergistic antibacterial, biodegradable, and osteogenic functionalities, shows significant potential for treating infection-prone cancellous bone defects.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (298KB)</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 6","pages":"Pages 3538-3551"},"PeriodicalIF":5.5,"publicationDate":"2025-06-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144092051","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}

引用次数: 0

Transformation from Suspension to Anisotropic Microfiber in the System of the Cholesteric Liquid Crystalline Phase of Chitin-Nanowhisker with the Surface Modified by Chitosan 壳聚糖改性甲壳素纳米晶须胆甾相液晶体系中悬浮液向各向异性微纤维的转变。

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-06-09 DOI: 10.1021/acs.biomac.4c01705

Phanicha Wiwatsamphan , Kohji Tashiro , Sono Sasaki , Thanit Kertsomboon , Patakorn Pilasen , Fanatchanon Maneechot , Suwabun Chirachanchai

{"title":"Transformation from Suspension to Anisotropic Microfiber in the System of the Cholesteric Liquid Crystalline Phase of Chitin-Nanowhisker with the Surface Modified by Chitosan","authors":"Phanicha Wiwatsamphan , Kohji Tashiro , Sono Sasaki , Thanit Kertsomboon , Patakorn Pilasen , Fanatchanon Maneechot , Suwabun Chirachanchai","doi":"10.1021/acs.biomac.4c01705","DOIUrl":"10.1021/acs.biomac.4c01705","url":null,"abstract":"<div><div>The strength of natural fibers is attributed to the anisotropic alignment of nano/microfibrils. To mimic this, the present work proposes a concentration-induced cholesteric liquid crystalline (CLC) phase for a suspension of chitin nanowhiskers surface-modified with chitosan (CTWK-CS). This phase enables the wet-spinning process to produce anisotropic microfibers. Although shear forces during spinning are expected to disturb the CLC structure, birefringent colors and TEM cross sections confirm its partial retention in the microfibers. Fiber tenacity is tunable through poststretching. Fiber dissolution in acetic acid indicates that inter- and intramolecular hydrogen bonding contribute critically to the structural integrity. This work demonstrates that the preorganization of nanowhiskers into a CLC phase allows the direct formation of ordered microfibers from colloidal suspension.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (79KB)</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 6","pages":"Pages 3309-3321"},"PeriodicalIF":5.5,"publicationDate":"2025-06-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144092077","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}

引用次数: 0

Cation-Driven Modulation of Tau Condensates: Insights into Liquid–Liquid Phase Separation and Rheological Properties 阳离子驱动的Tau凝聚物调制：对液-液相分离和流变特性的见解。

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-06-09 DOI: 10.1021/acs.biomac.5c00193

Nahuel N. Foressi , Leandro Cruz Rodríguez , Natalia Wilke , M. Soledad Celej

{"title":"Cation-Driven Modulation of Tau Condensates: Insights into Liquid–Liquid Phase Separation and Rheological Properties","authors":"Nahuel N. Foressi , Leandro Cruz Rodríguez , Natalia Wilke , M. Soledad Celej","doi":"10.1021/acs.biomac.5c00193","DOIUrl":"10.1021/acs.biomac.5c00193","url":null,"abstract":"<div><div>The formation of biocondensates through liquid–liquid phase separation (LLPS) has emerged as a vital and ubiquitous phenomenon contributing to the spatiotemporal coordination of cellular processes. Additionally, dysregulation of LLPS is increasingly implicated as a previously overlooked driver of diseases. LLPS typically involves multivalent noncovalent interactions among biomolecules, yet the role of solvent molecules, particularly water, in this process has received increasing attention. Metal ions are essential for life and exist in varying concentrations within cells. Both the concentration and type of metal ions significantly influence the phase separation of biomolecules. Ions with different degrees of hydration can uniquely alter the structure of water, which, in turn, affects LLPS. In this study, we use hyperspectral imaging (HSI) analysis and optical tweezers to investigate the effects of cations with different degrees of hydration on solvent properties within Tau condensates, an intrinsically disordered protein involved in Alzheimer’s disease. We first demonstrate that the environment within Tau droplets is more structured than the diluted phase. Then, we show that highly hydrated cations enhance phase separation, increase the proportion of restricted water within Tau droplets, and slow down their relaxation dynamics, suggesting a correlation between water structuring and rheological properties. By connecting solvent properties with the stability and dynamics of phase-separated droplets, this research provides insights into the molecular mechanisms governing LLPS and how environmental factors, such as metal ions and water structure, influence this process.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (53KB)</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 6","pages":"Pages 3605-3616"},"PeriodicalIF":5.5,"publicationDate":"2025-06-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144172096","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}

引用次数: 0

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-06-09

Wenqian Chen, Zi Ye, Lixiong Gao, Yuhang Jiang, Yue Wei, Xuejun Chen, Liqin Li*, Tengfei Mao* and Zhaohui Li*,

引用次数: 0

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-06-09

Iuliia Pilipenko*, Teemu Sorsa, Annika Valtari, Susanna Posio, Kati-Sisko Vellonen, Astrid Subrizi, Sami Hietala, Marika Ruponen and Arto Urtti,

引用次数: 0

Gas-Driven Porosity Control in Cellulose Acetate Membranes: Comparing Nitrogen and Carbon Dioxide for Micropore Formation 醋酸纤维素膜气驱孔隙控制：氮气和二氧化碳对微孔形成的影响。

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-06-09 DOI: 10.1021/acs.biomac.5c00257

Haram Ryu, Sang Wook Kang

{"title":"Gas-Driven Porosity Control in Cellulose Acetate Membranes: Comparing Nitrogen and Carbon Dioxide for Micropore Formation","authors":"Haram Ryu, Sang Wook Kang","doi":"10.1021/acs.biomac.5c00257","DOIUrl":"10.1021/acs.biomac.5c00257","url":null,"abstract":"<div><div>Cellulose acetate (CA) is a widely used porous material in various industrial applications, and its processing methods have evolved. This study presents a novel approach to enhancing pore formation efficiency by substituting nitrogen (N<sub>2</sub>) with carbon dioxide (CO<sub>2</sub>), a gas with a higher quadrupole moment. This method was employed to fabricate lactic acid-plasticized CA membranes coated on polypropylene substrates, enabling control over pore size and porosity. Surface morphology was analyzed using scanning electron microscopy to observe structural changes before and after gas permeation, with respect to the type of gas used. Fourier-transform infrared spectroscopy was used to assess molecular changes induced by lactic acid addition and to investigate gas-specific differences in pore formation. Thermal stability was evaluated via thermogravimetric analysis in relation to pore development. Additionally, the porosity, Gurley values, and gas permeance were measured to compare the effects of N<sub>2</sub> and CO<sub>2</sub> on the physical properties of the membranes.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (189KB)</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 6","pages":"Pages 3680-3688"},"PeriodicalIF":5.5,"publicationDate":"2025-06-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143951389","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}

引用次数: 0

The Hidden Isodimorphic Crystallization of Poly(ε-Caprolactone-Ran-ω-Pentadecalactone) Copolymers 聚（ε-己内酯- ran -ω-五内酯）共聚物的隐性同二晶化。

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-06-09 DOI: 10.1021/acs.biomac.5c00075

Juan Torres-Rodríguez , Ricardo A. Pérez-Camargo , Yunxiang Shi , Kaojin Wang , Yong-Guang Jia , X. X. Zhu , Alejandro J. Müller

{"title":"The Hidden Isodimorphic Crystallization of Poly(ε-Caprolactone-Ran-ω-Pentadecalactone) Copolymers","authors":"Juan Torres-Rodríguez , Ricardo A. Pérez-Camargo , Yunxiang Shi , Kaojin Wang , Yong-Guang Jia , X. X. Zhu , Alejandro J. Müller","doi":"10.1021/acs.biomac.5c00075","DOIUrl":"10.1021/acs.biomac.5c00075","url":null,"abstract":"<div><div>Poly(ε-caprolactone-<em>ran</em>-ω-pentadecalactone) (PCL<sub> <em>x</em> </sub>-PPDL<sub> <em>y</em> </sub>) copolymers were synthesized by using ring-opening polymerization with Candida antarctica lipase B as a catalyst across various compositions. The aim was to study their crystallization behavior and ascertain whether they are isomorphic or isodimorphic. Differential scanning calorimetry, polarized light optical microscopy, <em>in situ</em> wide- and small-angle X-ray scattering, and Fourier-transform infrared spectroscopy were employed to assess the crystallization mode. Various crystallization conditions were used to investigate their influence on the comonomer inclusion/exclusion balance. The copolymers exhibited pseudoeutectic behavior across all compositions, crystallizing in either PPDL-type or PCL-type unit cells and conformations, independent of crystallization conditions. This indicates that they are isodimorphic, contrary to previous reports. Self-nucleation tests showed that the <em>Domain II</em> width decreases with increasing comonomer content, supporting isodimorphism. The pseudoeutectic point was observed at CL contents above 83%, which explains the previously unrecognized isodimorphic character of these copolyesters.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (75KB)</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 6","pages":"Pages 3446-3462"},"PeriodicalIF":5.5,"publicationDate":"2025-06-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144074916","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}

引用次数: 0

Intracellular Nanodelivery of DNA with Enzyme-Degradable and pH-Responsive Peptide Dendrons 酶降解和ph响应肽树突的细胞内纳米DNA递送。

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-06-09 DOI: 10.1021/acs.biomac.5c00013

M. A. Urello , H. J. Vaughan , L. T. Dockery , A. J. Ciciriello , Y. Rui , B. Keyser , I. Ramos , E. E. Bosco , N. Peterson , C. Webster , J. Anand Subramony , M. Rice , M. Marelli , R. James Christie

{"title":"Intracellular Nanodelivery of DNA with Enzyme-Degradable and pH-Responsive Peptide Dendrons","authors":"M. A. Urello , H. J. Vaughan , L. T. Dockery , A. J. Ciciriello , Y. Rui , B. Keyser , I. Ramos , E. E. Bosco , N. Peterson , C. Webster , J. Anand Subramony , M. Rice , M. Marelli , R. James Christie","doi":"10.1021/acs.biomac.5c00013","DOIUrl":"10.1021/acs.biomac.5c00013","url":null,"abstract":"<div><div>Effective DNA delivery requires functional materials to package and transport genetic cargo into cells. However, many synthetic systems rely on heterogeneous mixtures, lack biodegradability, and pose toxicity concerns. Here, we introduce a peptide dendron single-molecule transfection reagent that enables targeted DNA delivery via pH-responsive, degradable nanoparticles with minimal toxicity. Peptide dendrons for intracellular delivery (PDIDs) incorporate ionizable non-natural amino acids for DNA binding and pH sensitivity. PDIDs formed stable nanoparticles that released DNA upon lysosomal acidification, facilitating cytoplasmic entry and subsequent gene expression. Rationally designed triamino acid blocks promoted protease degradation, reducing toxicity in preclinical models. Targeting ligands further enhanced the transfection efficiency by increasing cell uptake. In a lung metastasis model, targeted PDID-DNA nanoparticles selectively delivered therapeutic gene cargo to the lung, reducing tumor burden and extending survival. This platform demonstrates the potential to integrate natural and non-natural peptide features to enable safe and efficient DNA delivery in vivo.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (125KB)</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 6","pages":"Pages 3410-3422"},"PeriodicalIF":5.5,"publicationDate":"2025-06-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144085559","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}

引用次数: 0

Thermoresponsive Hydrogels with Tunable Viscoelasticity for Extended Ocular Drug Delivery 具有可调粘弹性的热响应性水凝胶用于延长眼部给药。

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-06-09 DOI: 10.1021/acs.biomac.5c00292

Iuliia Pilipenko , Teemu Sorsa , Annika Valtari , Susanna Posio , Kati-Sisko Vellonen , Astrid Subrizi , Sami Hietala , Marika Ruponen , Arto Urtti

{"title":"Thermoresponsive Hydrogels with Tunable Viscoelasticity for Extended Ocular Drug Delivery","authors":"Iuliia Pilipenko , Teemu Sorsa , Annika Valtari , Susanna Posio , Kati-Sisko Vellonen , Astrid Subrizi , Sami Hietala , Marika Ruponen , Arto Urtti","doi":"10.1021/acs.biomac.5c00292","DOIUrl":"10.1021/acs.biomac.5c00292","url":null,"abstract":"<div><div>The conformation of charged polymers is heavily dependent on interactions with the surrounding salt ions. By adding calcium ions to hyaluronan–Pluronic F-127 complexes, we prepared colloidal coacervates with decreased viscosity at cold temperatures (<em>G</em>′ of 10 Pa) and enhanced mechanical properties at physiological temperatures (<em>G</em>′ of 19 kPa) that improved the stability of the gel and prolonged drug release. The release of ophthalmic drugs, brinzolamide, dorzolamide, and dexamethasone, was tuned from 2 weeks to four months by changing drug lipophilicity. The low-viscosity hydrogel enabled topical ocular administration as eye drops and injections via thin needles (29G) under the conjunctiva. The precorneal residence time of glaucoma drug brinzolamide was extended over 48 h after topical administration and over 23 days after subconjunctival injections in rabbits. These findings suggest an approach to improve the viscoelasticity of eye drops and injectables, as well as to prolong drug delivery times via hydrogel systems.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (168KB)</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 6","pages":"Pages 3721-3731"},"PeriodicalIF":5.5,"publicationDate":"2025-06-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144172102","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}

引用次数: 0