Biomacromolecules最新文献_第2页

Insights into Protein Unfolding under pH, Temperature, and Shear Using Molecular Dynamics Simulations.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-03-25 DOI: 10.1021/acs.biomac.4c00991

Yinhao Jia, Clare Cocker, Janani Sampath

{"title":"Insights into Protein Unfolding under pH, Temperature, and Shear Using Molecular Dynamics Simulations.","authors":"Yinhao Jia, Clare Cocker, Janani Sampath","doi":"10.1021/acs.biomac.4c00991","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c00991","url":null,"abstract":"Protein biologics hold immense potential in therapeutic applications, but their ephemeral nature has hindered widespread application. The effects of different stressors on protein folding have long been studied, but whether these stressors induce protein unfolding through different pathways remains unclear. Here, we conduct all-atom molecular dynamics simulations to investigate the unfolding of bovine serum albumin (BSA) under three distinct stressors: high temperature, acidic pH, and shear stress. Our findings reveal that each stressor induces unique unfolding patterns in BSA, indicating stressor-specific unfolding pathways. Structural analyses show that high temperature significantly disrupts the protein's secondary structure, while acidic pH causes alternations in the tertiary structure, leading to domain separation. Shear stress initially perturbs the tertiary structure, initiating structural rearrangements, which causes a loss of secondary structure similar to temperature. These distinct unfolding behaviors suggest that different stabilization strategies are required to enhance protein stability under different denaturation conditions.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143699090","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

Physicochemical Properties of Freeze-Dried Bigel-Based Materials Composed of Sodium Alginate/Whey Protein Isolate Hydrogel and Ethylcellulose/Sunflower Oil Oleogel.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-03-25 DOI: 10.1021/acs.biomac.4c01677

Weronika Walendziak, Timothy E L Douglas, Justyna Kozlowska

{"title":"Physicochemical Properties of Freeze-Dried Bigel-Based Materials Composed of Sodium Alginate/Whey Protein Isolate Hydrogel and Ethylcellulose/Sunflower Oil Oleogel.","authors":"Weronika Walendziak, Timothy E L Douglas, Justyna Kozlowska","doi":"10.1021/acs.biomac.4c01677","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01677","url":null,"abstract":"Freeze-drying bigels is a novel technique for developing functional materials for dermatological and cosmetic use, leveraging the benefits of two structured phases. This study optimized freeze-dried bigels composed of whey protein isolate (WPI)/sodium alginate/glycerin hydrogel and ethylcellulose (EC)/Span 80/sunflower oil oleogel at varying hydrogel/oleogel ratios. The materials showed swelling ratios from 50% to 255%, with higher values for a lower oleogel content and higher polymer concentration. The higher oleogel content extended the degradation from a few hours to 7 days. The polymer concentrations and hydrogel/oleogel ratios influenced Young's modulus (1.25-3.7 MPa). Porosity varied from 35% to 58%, and density varied from 100 to 200 mg/mL. The residual moisture content (5% to 20%) increased with EC content and decreased with WPI and oleogel content. These findings underscore the role of polymer concentrations and phase ratios in tuning the physicochemical properties of freeze-dried gels, positioning them as promising biomaterials for skincare and cosmetic applications.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143699091","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

Biobased Physicochemical Reversible Dual-Cross-Linked Hydrogel: Self-Healing, Antibacterial, Antioxidant, and Hemostatic Properties for Diabetic Wound Healing.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-03-24 DOI: 10.1021/acs.biomac.5c00087

Hanzhang Wang, Bin Lu, Junyi Zhou, Jieying Lai, Xue Zheng, Shuang-Zhuang Guo, Li-Ming Zhang

{"title":"Biobased Physicochemical Reversible Dual-Cross-Linked Hydrogel: Self-Healing, Antibacterial, Antioxidant, and Hemostatic Properties for Diabetic Wound Healing.","authors":"Hanzhang Wang, Bin Lu, Junyi Zhou, Jieying Lai, Xue Zheng, Shuang-Zhuang Guo, Li-Ming Zhang","doi":"10.1021/acs.biomac.5c00087","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00087","url":null,"abstract":"Skin wound healing remains challenging due to a lack of ideal wound dressings suitable for acute and chronic wounds. This study introduced a biocompatible hydrogel wound dressing, synthesized through a green chemistry approach, specifically designed to meet the dual needs of acute and chronic wound care. The innovative strategy utilized sustainable biomaterials, soy protein, and vanillin, to construct a physical-reversible chemical dual-cross-linked hydrogel exhibiting high mechanical strength, excellent adhesion, and toughness. Schiff base reversible covalent bonds enabled rapid self-healing within 10 s, significantly improving durability. In a rat liver hemorrhage model, the hydrogel rapidly sealed wounds, achieving effective hemostasis, indicating great potential for acute wound care. Furthermore, vanillin imparted the hydrogel with antimicrobial and antioxidant properties, effectively accelerating diabetic chronic wound healing. This safe and efficient advanced biobased hydrogel offers a novel perspective for wound treatment and holds significant promise for clinical applications.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143699086","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 Photosensitizer-Embedded Glycopolymers through Self-Catalytic PET-RAFT Polymerization for Targeted PDT.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-03-24 DOI: 10.1021/acs.biomac.5c00090

Jiaoyang Zhu, Jiahui Lin, Ruili Wang, Zhiyuan Ma, Weiwei Zuo, Meifang Zhu

{"title":"Enhanced Photosensitizer-Embedded Glycopolymers through Self-Catalytic PET-RAFT Polymerization for Targeted PDT.","authors":"Jiaoyang Zhu, Jiahui Lin, Ruili Wang, Zhiyuan Ma, Weiwei Zuo, Meifang Zhu","doi":"10.1021/acs.biomac.5c00090","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00090","url":null,"abstract":"PET-RAFT polymerization enables precise polymer synthesis, yet conventional systems require an excess chain transfer agent (CTA) over unbound photocatalysts (PCs). Herein, a self-catalyzed strategy employing polymerizable porphyrin MTPPZnH as a dual-functional PC effectively embeds high photosensitizer content into glycopolymers for photodynamic therapy (PDT). Three galactose-bearing monomers (acrylate, methacrylate, 4-vinylbenzoate) were polymerized via PET-RAFT under optimized light conditions, achieving satisfactory Mn and relatively narrow Đ. Mechanistic studies revealed that photoexcited MTPPZnH transfers electrons/energy to CTA via a PET process, initiating polymerization, with DMSO enhancing oxygen depletion. Water-soluble glycopolymeric photosensitizers exhibited high fluorescence and singlet oxygen quantum yield. In vitro, galactose-bearing photosensitizers showed superior ASGPR-mediated endocytosis in HepG2 cells over Huh-7 and MCF-7 cells, enabling targeted PDT. The incorporation of MTPPZnH contributes to an effective multifunctional strategy, offering a promising approach for the development of high photosensitizer-embedded polymeric photosensitizers for potential PDT applications.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143699087","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 Whole Tumor Cell-Based Vaccines by a RAFT and Protein Fusion Strategy for Tumor Immunotherapy.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-03-21 DOI: 10.1021/acs.biomac.5c00115

He Yang, Ruyan Feng, Xingyu Heng, Fangjian Shan, Yichen Wang, Lihua Yao, Sujian Wang, Gaojian Chen, Hong Chen

{"title":"Enhanced Whole Tumor Cell-Based Vaccines by a RAFT and Protein Fusion Strategy for Tumor Immunotherapy.","authors":"He Yang, Ruyan Feng, Xingyu Heng, Fangjian Shan, Yichen Wang, Lihua Yao, Sujian Wang, Gaojian Chen, Hong Chen","doi":"10.1021/acs.biomac.5c00115","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00115","url":null,"abstract":"Inactivated whole tumor cell-based vaccines (WTVs) are a promising strategy for tumor immunotherapy, but have exhibited limited antitumor effects clinically. Aiming at constructing enhanced WTVs, we developed glycopolymer-engineered WTVs (G-WTVs) using a Halo-Tag protein (HTP) fusion technique and reversible addition-fragmentation chain transfer (RAFT) polymerization. In our study, G-WTVs with varying molecular weights of glycopolymers were constructed. Compared to unmodified tumor cells, all G-WTVs effectively induced the polarization of macrophages toward the M1 phenotype and promoted the secretion of pro-inflammatory cytokines. This enhanced immune response was attributed to the improved interactions between G-WTVs and the macrophages. Among the G-WTVs, the medium molecular weight variant demonstrated the most pronounced enhancement of antitumor immune responses. Notably, the administration of optimized G-WTVs effectively inhibited the growth of B16 melanoma in mice. Our findings provide a new approach to enhance the antitumor efficacy of WTVs via cell membrane glycopolymer engineering, offering a promising strategy for tumor immunotherapy.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672905","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

Hybrid Pectin-Fibroin Microgels with Supramolecular and Covalent Cross-Links.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-03-21 DOI: 10.1021/acs.biomac.4c01658

Gokul Kamaraju, Julian Karl, Selin Bulut, Maria Pieper, Nabanita Hazra, Gurudas Chakraborty, Alexander Boes, Andreas Herrmann, Ulrich Schwaneberg, Andrij Pich

{"title":"Hybrid Pectin-Fibroin Microgels with Supramolecular and Covalent Cross-Links.","authors":"Gokul Kamaraju, Julian Karl, Selin Bulut, Maria Pieper, Nabanita Hazra, Gurudas Chakraborty, Alexander Boes, Andreas Herrmann, Ulrich Schwaneberg, Andrij Pich","doi":"10.1021/acs.biomac.4c01658","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01658","url":null,"abstract":"Sugar beet pectin, an anionic polysaccharide, and silk fibroin, a high molecular weight protein, undergo gelation through ionic interactions and conformational changes, leading to hydrogel formation. Although many studies have focused on bulk gel systems involving polysaccharides and proteins, more research is needed to investigate their properties at the microscale level. In this context, we have developed a microgel system based on a pectin/fibroin combination and investigated its properties. We focused on two gelation mechanisms: physical cross-linking and enzymatic covalent cross-linking. The pectin/fibroin microgels were fabricated using droplet-based microfluidics, and the secondary structure, mechanical properties, and degradation profiles were investigated. Our experimental results show that the microgels exhibit an ordered β-sheet structure, a Young's modulus in the range of 10 to 20 kPa, and that degradation can be promoted using protease enzymes. Finally, the biocompatibility of the microgels is assessed using the Alamar Blue cell viability assay with human pulmonary fibroblasts (HPFs). This research presents a highly functional hybrid biomaterial produced from waste products and a structural protein, demonstrating its cell compatibility and potential in tissue engineering applications.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143672908","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

ROS-Responsive Cationic Polymers with Intrinsic Anti-Inflammatory Activity for Intracellular Protein Delivery. 具有内在抗炎活性的 ROS 反应性阳离子聚合物用于细胞内蛋白质输送。

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-03-20 DOI: 10.1021/acs.biomac.4c01593

Yongming Wang, Yangcan Ming, Zhichao Yu, Zhenjin Xu, Minglang Zou, Cuiping Chen, Fang Luo, Da Huang, Na Wang, Zhenyu Lin, Zuquan Weng

{"title":"ROS-Responsive Cationic Polymers with Intrinsic Anti-Inflammatory Activity for Intracellular Protein Delivery.","authors":"Yongming Wang, Yangcan Ming, Zhichao Yu, Zhenjin Xu, Minglang Zou, Cuiping Chen, Fang Luo, Da Huang, Na Wang, Zhenyu Lin, Zuquan Weng","doi":"10.1021/acs.biomac.4c01593","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01593","url":null,"abstract":"The intracellular delivery of protein drugs via nanocarriers offers significant potential for expanding their therapeutic applications. However, the unintended activation of innate immune responses and inflammation triggered by the carriers presents a major challenge, often compromising therapeutic efficacy. Here, we present oligoethylenimine-thioketal (OEI-TK), a reactive oxygen species-responsive cationic polymer with intrinsic anti-inflammatory properties, to overcome this challenge. OEI-TK self-assembles electrostatically with bovine serum albumin (BSA) to form stable nanoparticles (OTB NPs) with excellent encapsulation efficiency. In vitro studies confirmed that OTB NPs retained OEI-TK's antioxidant and anti-inflammatory properties, enhanced biocompatibility, and efficiently delivered BSA into cells. Furthermore, OEI-TK facilitated the intracellular delivery of β-galactosidase while preserving its enzymatic activity, demonstrating its potential for functional protein transport. These findings highlight OEI-TK as a promising platform with dual benefits of inflammation modulation and intracellular protein delivery, holding potential for the synergistic treatment of inflammation-related diseases.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143668580","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

An Antibacterial Hydrogel Based on Silk Sericin Cross-Linking Glycyrrhizic Acid and Silver for Infectious Wound Healing.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-03-18 DOI: 10.1021/acs.biomac.4c01687

Xiang Li, Yurong Li, Akoumay Tehoungue, Qianyan Wang, Hui Yan, Guozheng Zhang, Yeshun Zhang

{"title":"An Antibacterial Hydrogel Based on Silk Sericin Cross-Linking Glycyrrhizic Acid and Silver for Infectious Wound Healing.","authors":"Xiang Li, Yurong Li, Akoumay Tehoungue, Qianyan Wang, Hui Yan, Guozheng Zhang, Yeshun Zhang","doi":"10.1021/acs.biomac.4c01687","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01687","url":null,"abstract":"Bioactive hydrogels are garnering increasing interest in wound management due to their porous structural features and versatile intrinsic biological activities. Importantly, the antibacterial capacity is a crucial requirement for hydrogel dressings in chronically infected wounds. In this study, we report an antibacterial hydrogel constructed from silk sericin (SS) cross-linked with glycyrrhizic acid (GA) and integrated with silver ions (Ag+) to accelerate the healing of bacterial-infected wounds. The resultant sericin-glycyrrhizic acid-Ag+ hydrogel (SGA) demonstrates favorable mechanical properties, effectively preventing secondary injury to wounds. Moreover, in vitro studies indicated that the SGA hydrogel possesses excellent swelling ratios, degradability, and cytocompatibility, promoting cell growth and proliferation. Notably, the SGA hydrogel exhibited effective antibacterial activity against both Gram-positive and Gram-negative bacteria through the release of Ag+. In a Staphylococcus aureus-infected wound model, the SGA hydrogel efficiently eradicated bacteria, thus promoting wound repair. Overall, our work establishes a novel strategy for developing multifunctional hydrogel dressings based on natural materials for managing bacteria-infected wounds.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143655464","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 Role and Future of Functional Graphenic Materials in Biomedical and Human Health Applications.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-03-18 DOI: 10.1021/acs.biomac.4c01431

Anne M Arnold, Juhi Singh, Stefanie A Sydlik

引用次数: 0

Fabricating N-Cadherin Mimetic Peptide-Based Diverse Self-Assembled Hydrogels in the Presence of Biologically Relevant Cations.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-03-18 DOI: 10.1021/acs.biomac.4c01579

Sweta Mohanty, Sangita Roy

{"title":"Fabricating N-Cadherin Mimetic Peptide-Based Diverse Self-Assembled Hydrogels in the Presence of Biologically Relevant Cations.","authors":"Sweta Mohanty, Sangita Roy","doi":"10.1021/acs.biomac.4c01579","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01579","url":null,"abstract":"N-cadherin, a crucial extracellular matrix protein, is crucial in mediating cellular interactions and promoting cell migration. Herein, we have attempted to create N-cadherin mimetic peptide (NcMP) hydrogel scaffolds by incorporating cations as the external stimulus to create a suitable interface for favorable cellular interactions. Inspired by the Hofmeister series, we selected four biologically significant cations, classified as kosmotropes and chaotropes, and varied their concentrations to investigate how increasing ionic strength affects the self-assembly of the NcMP. Interestingly, the incorporation of these ions greatly influenced the self-assembling propensity of the Fmoc-HAVDI hydrogel, which resulted in diverse structural and mechanical properties. Such diverse physical properties led to differential cellular responses. Thus, we were able to access diverse physical and biological properties in a single gelator molecule by simply changing the nature and concentration of the biologically relevant cations. We anticipate that these diverse hydrogel systems hold great potential in various biomedical applications.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143646495","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