Biomacromolecules最新文献

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 : 2025-05-17 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":"https://doi.org/10.1021/acs.biomac.5c00013","url":null,"abstract":"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.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-05-17","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

Compositional Control of Stereocomplexed Hydrogel Microparticle Network Formation and Physical Properties. 立体络合水凝胶微粒网络形成及物理性质的组成控制。

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-05-17 DOI: 10.1021/acs.biomac.5c00443

Gianna Tutoni, Annette Lu, Matthew E Bonacci, Tony Jun Huang, Matthew L Becker

{"title":"Compositional Control of Stereocomplexed Hydrogel Microparticle Network Formation and Physical Properties.","authors":"Gianna Tutoni, Annette Lu, Matthew E Bonacci, Tony Jun Huang, Matthew L Becker","doi":"10.1021/acs.biomac.5c00443","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00443","url":null,"abstract":"Granular hydrogel scaffolds composed of many discrete hydrogel microparticles (HMPs) have demonstrated significant advantages over bulk hydrogels, including injectability and the flexibility to incorporate diverse chemistries, physical properties, and bioactive payloads. Herein, we demonstrate the ability to tune HMP properties through varying the length of poly(ethylene glycol) (PEG) arms and stereocomplexed poly(lactic acid) (SC PLA) cross-links within PEG-based HMPs to further understand the networks' structure-property relationships and utility in a model prodrug delivery system. DSC and WAXS revealed that hydrogels with shorter PEG arms were able to form stereocomplex domains to a greater extent than longer PEG arms. Additionally, as the SC PLA length increased, the HMPs were more thermally and mechanically stable. HMPs were also loaded with model prodrug, doxorubicin, to characterize compositional variations' effects on release profiles. These studies suggest that variations in the cross-linker concentration influence the crystallinity of each HMP formulation, allowing for tunable drug loading and release.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144085555","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

Enhanced Near-Infrared Light-Mediated Hydrogel Curing Using Photoinitiator Integrated Upconversion Particles as Nano Initiator for 3D Bioprinting. 利用光引发剂集成上转换粒子作为纳米引发剂增强近红外光介导的水凝胶固化用于生物3D打印。

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-05-17 DOI: 10.1021/acs.biomac.4c01775

Xiong Xiao, Ziwei Huang, Hongying Duan, Liping Yang, Yuchu Yang, Yushang Lai, Chenxi Li, Li Feng

{"title":"Enhanced Near-Infrared Light-Mediated Hydrogel Curing Using Photoinitiator Integrated Upconversion Particles as Nano Initiator for 3D Bioprinting.","authors":"Xiong Xiao, Ziwei Huang, Hongying Duan, Liping Yang, Yuchu Yang, Yushang Lai, Chenxi Li, Li Feng","doi":"10.1021/acs.biomac.4c01775","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01775","url":null,"abstract":"In vivo three-dimensional (3D) bioprinting is a promising strategy that can enable personalized organ repair with minimal injury. The current in vivo 3D bioprinting based on upconversion nanoparticles (UCNPs) mediating near-infrared (NIR) light curing is still limited by the low hydrogel cross-linking efficiency. Herein, we introduced a bioink system that allows enhanced NIR light curing by utilizing thiol-ene cross-linkable polymers and photoinitiator-modified UCNPs@LAP nano initiator. The norbornene functionalized hyaluronic acid (NorHA) and thiolated gelatin (GelSH) were first synthesized to prepare the thiol-ene polymer solution. Compared to radical cross-linkable gelatin methacryloyl (GelMA), the NorHA/GelSH exhibited much higher reactivity under weak photoinitiating conditions. With the addition of surface-modified UCNPs@LAP nano initiator, the bioinks showed improved NIR curing performances, which is beneficial to reduce potential thermal damage. Furthermore, in vitro evaluation showed that the NIR light-cured 3D scaffolds preserved excellent bioactivity, suggesting that the hybrid bioink holds great promise to serve as a candidate for in vivo 3D bioprinting.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144085557","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

Effect of Poly(l-serine) Additives with Different Primary Structures on the Mechanical Properties of Poly(vinyl alcohol) Films. 不同一级结构的聚l-丝氨酸添加剂对聚乙烯醇薄膜力学性能的影响。

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-05-16 DOI: 10.1021/acs.biomac.5c00277

Ruka Ito, Takamasa Sakai, Kousuke Tsuchiya

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 : 2025-05-15 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":"https://doi.org/10.1021/acs.biomac.5c00075","url":null,"abstract":"Poly(ε-caprolactone-ran-ω-pentadecalactone) (PCLx-PPDLy) 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, in situ 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 Domain II 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.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-05-15","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

Heterotypic Droplet Formation by Pro-Inflammatory S100A9 and Neurodegenerative Disease-Related α-Synuclein. 促炎性S100A9和神经退行性疾病相关α-突触核蛋白形成异型液滴。

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-05-15 DOI: 10.1021/acs.biomac.5c00130

Dominykas Veiveris, Aurimas Kopustas, Darius Sulskis, Kamile Mikalauskaite, Mohammad Nour Alsamsam, Marijonas Tutkus, Vytautas Smirnovas, Mantas Ziaunys

{"title":"Heterotypic Droplet Formation by Pro-Inflammatory S100A9 and Neurodegenerative Disease-Related α-Synuclein.","authors":"Dominykas Veiveris, Aurimas Kopustas, Darius Sulskis, Kamile Mikalauskaite, Mohammad Nour Alsamsam, Marijonas Tutkus, Vytautas Smirnovas, Mantas Ziaunys","doi":"10.1021/acs.biomac.5c00130","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00130","url":null,"abstract":"Liquid-liquid phase separation of proteins and nucleic acids is a rapidly emerging field of study, aimed at understanding the process of biomolecular condensate formation. Recently, it has been discovered that different neurodegenerative disease-related proteins, such as α-synuclein and amyloid-β are capable of forming heterotypic droplets. Other reports have also shown non-LLPS cross-interactions between various amyloidogenic proteins and the resulting influence on their amyloid fibril formation. This includes the new discovery of pro-inflammatory S100A9 affecting the aggregation of both amyloid-β, as well as α-synuclein. In this study, we explore the formation of heterotypic droplets by S100A9 and α-synuclein. We show that their mixture is capable of assembling into both homotypic and heterotypic condensates and that this cross-interaction alters the aggregation mechanism of α-synuclein. These results provide insight into the influence of S100A9 on the process of neurodegenerative disease-related protein LLPS and aggregation.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144074914","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

Chitosan-Based Thermal-Coagulation Hydrogel System Driven by Multiple Interactions: Oxidation-Induced Fast Gelation and Enhanced Performance. 基于壳聚糖的多重相互作用驱动的热凝水凝胶体系：氧化诱导的快速凝胶化和性能增强。

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-05-14 DOI: 10.1021/acs.biomac.5c00304

Yifan Liu, Guoyin Chen, Tianyu Zhou, Xiaohui Mao, Junfen Sun, Liping Zhu, Long Chen, Meifang Zhu

{"title":"Chitosan-Based Thermal-Coagulation Hydrogel System Driven by Multiple Interactions: Oxidation-Induced Fast Gelation and Enhanced Performance.","authors":"Yifan Liu, Guoyin Chen, Tianyu Zhou, Xiaohui Mao, Junfen Sun, Liping Zhu, Long Chen, Meifang Zhu","doi":"10.1021/acs.biomac.5c00304","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00304","url":null,"abstract":"The application of the chitosan/β-glycerophosphate (CS/β-GP) system is limited due to its weak mechanical performance, high concentration of β-GP, and slow gelation. To revitalize this thermal-coagulation system, we used catechol-chitosan (CS-C) and systematically investigated the influence of modification. By controlling the grafting rate, it was found that the solution pH and pKa of CS-C were both affected by the decrease of the amino groups, whereas the gelation time and the required β-GP content for gelling significantly decreased. Using the oxidative properties of the catechol groups, the CS-C/β-GP hydrogel showed a 10-fold increment in stiffness, rapid gelation (1-2 min), and a much lower β-GP content (2-6 wt %). In addition, the hydrogel performed well in antimicrobial and biocompatibility tests. This is the first work to elucidate the thermal-coagulation mechanism of modified chitosan systems, making the application of chitosan-based thermal-coagulation systems in the field of biomedicine and tissue repair possible.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143952908","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

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 : 2025-05-14 DOI: 10.1021/acs.biomac.5c00257

Haram Ryu, Sang Wook Kang

引用次数: 0

Direct Quantification of PEGylation for Intact Bioconjugates and Nanoparticles by the Colorimetric Barium/Iodide Assay. 用钡碘比色法直接定量完整生物偶联物和纳米颗粒的聚乙二醇化。

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-05-14 DOI: 10.1021/acs.biomac.5c00274

Kevin Coutu, Amatus Ngabonziza Sangwa, Nicolas Gaudreault, Seyed Saeid Tayebi, Todd Hoare, Prashant Mhaskar, Nicolas Bertrand, Andrea A Greschner, Marc A Gauthier

{"title":"Direct Quantification of PEGylation for Intact Bioconjugates and Nanoparticles by the Colorimetric Barium/Iodide Assay.","authors":"Kevin Coutu, Amatus Ngabonziza Sangwa, Nicolas Gaudreault, Seyed Saeid Tayebi, Todd Hoare, Prashant Mhaskar, Nicolas Bertrand, Andrea A Greschner, Marc A Gauthier","doi":"10.1021/acs.biomac.5c00274","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00274","url":null,"abstract":"Several methods are available to determine the average number of methoxy poly(ethylene glycol) (mPEG) chains grafted to a protein or peptide, referred to as the degree of PEGylation. Nevertheless, the development of simple, versatile, and multiplexable methods for determining PEGylation remains desirable. Childs and Kurfürst have respectfully reported the quantitative and qualitative use of a colored 'barium-iodide-PEG' complex for the titration of PEG in solutions and to stain PEG-containing bands on electrophoresis gels. Remarkably, this assay has yet to be employed to directly determine the extent of PEGylation of protein bioconjugates or intact nanoparticles. This study validates this assay for these purposes, via libraries of 54 mPEG-protein conjugates and 10 polymeric nanoparticles. The effect of mPEG molecular weight, terminal functional groups, and architecture were analyzed, among other parameters. Practical details and known artifacts are discussed to enhance the accuracy and reproducibility of the assay.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143951236","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

Hydrogen Bond and Hydrophobic Interaction Reinforced Tough and Antiswelling Hydrogels via Polymerization-Induced Microphase Separation. 氢键和疏水相互作用通过聚合诱导的微相分离增强坚韧和抗膨胀的水凝胶。

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-05-14 DOI: 10.1021/acs.biomac.5c00480

Kaixuan Ren, Xinyan Quanji, Xiao Du, Chengfeng Cai, Jinyu Luo, Jingbo Yin

{"title":"Hydrogen Bond and Hydrophobic Interaction Reinforced Tough and Antiswelling Hydrogels via Polymerization-Induced Microphase Separation.","authors":"Kaixuan Ren, Xinyan Quanji, Xiao Du, Chengfeng Cai, Jinyu Luo, Jingbo Yin","doi":"10.1021/acs.biomac.5c00480","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00480","url":null,"abstract":"Polymerization-induced microphase separation strategy offers an effective approach for designing hydrogels with microphase-separated structure. In this study, a kind of microphase-separated hydrogels was fabricated by copolymerizing histidine methacrylamide and methacrylic acid monomers. Spontaneous microphase separation occurred during the polymerization process, which was driven by the strong hydrogen bonding interactions between imidazole and carboxyl groups, stabilizing by the hydrophobic interactions of methyl groups. The microphase-separated hydrogels exhibited significantly enhanced mechanical properties, achieving stiffness of 67 MPa, tensile strength of 2.2 MPa, toughness of 8.3 MJ/m3, fracture energy of 7.0 kJ/m2, and superior energy dissipation capabilities. These hydrogels also exhibited remarkable antiswelling performance across a broad pH range (pH 3-11). Notably, the microphase-separated hydrogels remained in a glassy state at room temperature. Moreover, the hydrogels displayed excellent cytocompatibility. This study provides valuable insights into the design of microphase-separated hydrogels, paving the way for their practical applications in biomedical engineering.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143955836","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