BiomacromoleculesPub Date : 2025-03-10Epub Date: 2025-02-05DOI: 10.1021/acs.biomac.4c01234
Wacili Da, Xiangtian Deng, Quan Chen, Yang Yang, Shenghu Jiang, Xiaoting Chen, Gonggong Lu, Bin Shen
{"title":"Metformin-Loaded Tannic Acid Nanoparticles Attenuate Osteoarthritis by Promoting Chondrocyte Mitochondria Homeostasis Based on Mitocytosis.","authors":"Wacili Da, Xiangtian Deng, Quan Chen, Yang Yang, Shenghu Jiang, Xiaoting Chen, Gonggong Lu, Bin Shen","doi":"10.1021/acs.biomac.4c01234","DOIUrl":"10.1021/acs.biomac.4c01234","url":null,"abstract":"<p><p>The oxidative stress microenvironment and mitochondrial dysfunction in chondrocytes are key mechanisms in the development of osteoarthritis (OA). Metformin (Met) has demonstrated multiple effects on mitochondria and is regarded as a potential therapeutic agent for OA. The low blood flow characteristics in the joint cavity make targeted local delivery of metformin crucial for its clinical application. In this study, tannic acid (TA), with its natural antioxidant and anti-inflammatory properties, was used to prepare self-assemble Met-loaded TA nanoparticles (NPs). The NPs exhibit excellent reactive oxygen scavenging capability, stability in various media, and an acid-responsive release of Met. In Vitro experiments showed that NPs possess excellent biocompatibility, effectively protecting chondrocyte viability in OA's pathological environment and preventing the senescence phenotype. In addition, NPs promoted the expression of antioxidant elements in chondrocytes, restored mitochondrial membrane potential, and enhanced mitocytosis to improve mitochondrial quality. In vivo experiments further confirmed that intra-articular injection of NPs in rats with post-traumatic OA improves cartilage matrix degradation, osteophyte formation, and subchondral bone sclerosis over 8 weeks. Tissue staining further confirmed the protective effects of NPs on chondrocyte mitochondria. Importantly, both in vivo and in vitro experiments revealed that NPs provided superior cellular protection compared to TA or Met alone. Overall, this study demonstrates that NPs effectively against OA cartilage degeneration, with the advantages of easy preparation, high efficiency, and biosafety.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":"1507-1519"},"PeriodicalIF":5.5,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143254030","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}
BiomacromoleculesPub Date : 2025-03-10Epub Date: 2025-02-17DOI: 10.1021/acs.biomac.4c01371
Yu Ikushima, Tatsuya Oshima
{"title":"Development of a Pillar[6]arene Carboxylic Acid Derivative for the Extraction of a Cationic Protein.","authors":"Yu Ikushima, Tatsuya Oshima","doi":"10.1021/acs.biomac.4c01371","DOIUrl":"10.1021/acs.biomac.4c01371","url":null,"abstract":"<p><p>Pillararenes are macrocyclic compounds that can have multiple functional groups and can provide a platform to develop multivalent ligands. Herein, a pillar[6]arene carboxylic acid derivative (OctP[6]CH<sub>2</sub>COOH) was prepared to extract the cationic protein cytochrome c (Cyt-c) into organic solvents. OctP[6]CH<sub>2</sub>COOH was synthesized by the condensation of ethyl 2-(4-octoxyphenoxy) acetate to obtain the pillar[6]arene derivative, followed by alkali hydrolysis. OctP[6]CH<sub>2</sub>COOH showed high extractability for Cyt-c, while a monomer analog and a neutral pillar[6]arene ester derivative did not. The lysine-rich protein Cyt-c was selectively extracted using OctP[6]CH<sub>2</sub>COOH over other cationic proteins because the complexation was a result of the inclusion of the NH<sub>3</sub><sup>+</sup> groups of the lysine residues by the macrocyclic molecule. Cyt-c complexed with OctP[6]CH<sub>2</sub>COOH partially underwent a structural change and exhibited peroxidase activity in organic solvents. This is the first report of protein extraction using pillararene derivatives that can be applied for the separation and modification of proteins.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":"1571-1579"},"PeriodicalIF":5.5,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143439381","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}
{"title":"Material Design, Fabrication Strategies, and the Development of Multifunctional Hydrogel Composites Dressings for Skin Wound Management.","authors":"Ziteng Wu, Dongdong Lu, Shuo Sun, Manqi Cai, Lin Lin, Mingning Zhu","doi":"10.1021/acs.biomac.4c01715","DOIUrl":"10.1021/acs.biomac.4c01715","url":null,"abstract":"<p><p>The skin is fragile, making it very vulnerable to damage and injury. Untreated skin wounds can pose a serious threat to human health. Three-dimensional polymer network hydrogels have broad application prospects in skin wound dressings due to their unique properties and structure. The therapeutic effect of traditional hydrogels is limited, while multifunctional composite hydrogels show greater potential. Multifunctional hydrogels can regulate wound moisture through formula adjustment. Moreover, hydrogels can be combined with bioactive ingredients to improve their performance in wound healing applications. Stimulus-responsive hydrogels can respond specifically to the wound environment and meet the needs of different wound healing stages. This review summarizes the material types, structure, properties, design considerations, and formulation strategies for multifunctional hydrogel composite dressings used in wound healing. We discuss various types of recently developed hydrogel dressings, highlights the importance of tailoring their physicochemical properties, and addresses potential challenges in preparing multifunctional hydrogel wound dressings.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":"1419-1460"},"PeriodicalIF":5.5,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143439382","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}
BiomacromoleculesPub Date : 2025-03-10Epub Date: 2025-02-24DOI: 10.1021/acs.biomac.4c01572
Jun Wu, Tiantian Tan, Jinghua Chen, Yan Zhang
{"title":"pH-Responsive Conformational-Switching Cationic Fusion Protein for Promoted Plasmid DNA Delivery and Transfection.","authors":"Jun Wu, Tiantian Tan, Jinghua Chen, Yan Zhang","doi":"10.1021/acs.biomac.4c01572","DOIUrl":"10.1021/acs.biomac.4c01572","url":null,"abstract":"<p><p>Gene therapy holds great promise for treating various diseases, but challenges such as delivery efficiency, immune response, and long-term effects still remain. Protamine is a frequently used gene delivery vector for its strong nucleic acid binding capacity, but its application is constrained by inadequate nucleic acid release, resulting in low transfection efficiency. Here, we introduce a fusion protein by integrating LAH4 peptides on both ends of protamine's DNA-binding motif. This fusion protein exhibits lower cytotoxicity compared to protamine. At pH 7.4, its uniform charge distribution and α-helical structure enable robust DNA condensation and DNase resistance. Under acidic conditions (pH 5.8), the conformational change of the protein weakens its DNA binding, facilitating controlled release in endosomes/lysosomes. Simultaneously, it interacts with the endosomal membrane to form pores, aiding in the endosomal escape of the nucleic acids, thereby significantly improving transfection efficiency. This fusion protein offers the potential for efficient and safe nucleic acid delivery.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":"1788-1798"},"PeriodicalIF":5.5,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143490314","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}
BiomacromoleculesPub Date : 2025-03-10Epub Date: 2025-02-18DOI: 10.1021/acs.biomac.4c01621
Keiji Numata
{"title":"The Biology of Natural Polymers Accelerates and Expands the Science of Biomacromolecules: A Focus on Structural Proteins.","authors":"Keiji Numata","doi":"10.1021/acs.biomac.4c01621","DOIUrl":"10.1021/acs.biomac.4c01621","url":null,"abstract":"<p><p>This Perspective explores the use of biomacromolecules in natural materials synthesized by living organisms, such as spider silk, in the development of sustainable synthetic materials. Currently employed synthetic polymers lack the hierarchical complexity and unique properties of natural materials composed of biomacromolecules. By understanding the composition of these natural materials, it may be able to reproduce their properties synthetically. Additionally, research directions involving the use of renewable resources such as nitrogen and carbon dioxide from the air and seawater to develop biomacromolecules such as spider silk and biopolyester via photosynthetic organisms are reviewed. Next-generation biomacromolecule research will aid in the creation of a sustainable global society, advancing fields such as biomanufacturing, agriculture, aquaculture, and other industries.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":"1393-1403"},"PeriodicalIF":5.5,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11898061/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143447441","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}
BiomacromoleculesPub Date : 2025-03-10Epub Date: 2025-02-24DOI: 10.1021/acs.biomac.4c01294
Pedro Augusto Invernizzi Sponchiado, Maryanne Trafani Melo, Juçara G Cominal, Milena Martelli Tosi, Pietro Ciancaglini, Ana Paula Ramos, Bianca Chieregato Maniglia
{"title":"Biomembranes Based on Potato Starch Modified by Dry Heating Treatment: One Sustainable Strategy to Amplify the Use of Starch as a Biomaterial.","authors":"Pedro Augusto Invernizzi Sponchiado, Maryanne Trafani Melo, Juçara G Cominal, Milena Martelli Tosi, Pietro Ciancaglini, Ana Paula Ramos, Bianca Chieregato Maniglia","doi":"10.1021/acs.biomac.4c01294","DOIUrl":"10.1021/acs.biomac.4c01294","url":null,"abstract":"<p><p>The exceptional biocompatibility of polymeric membranes drives their use in biomaterials, but structural modifications are needed to improve their mechanical properties. This study investigated dry heating treatment (DHT) as an ecofriendly and cost-effective approach to modifying potato starch for biomembrane fabrication. DHT-treated starch (2 h) produced biomembranes with a denser structure, smoother surfaces, and significantly improved mechanical properties, including higher tensile strength (∼6×), rigidity (∼15×), and relative crystallinity (∼2×) while reducing flexibility (∼5×), compared to native starch membranes. These membranes also exhibited lower moisture content, reduced hydrophilicity, higher surface energy, decreased biodegradability, and enhanced bioactivity, as shown by hydroxyapatite formation in simulated body fluid. Importantly, they were nontoxic to osteoblasts, emphasizing their potential for medical applications. This study highlights DHT as a sustainable and innovative method for modifying starch to develop advanced biomaterials for medical applications.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":"1530-1540"},"PeriodicalIF":5.5,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11898047/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143490306","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}
BiomacromoleculesPub Date : 2025-03-10Epub Date: 2025-02-04DOI: 10.1021/acs.biomac.4c01394
Ning Wang, Chenxi Qiao, Jun Liu, Guohua Liu, Kun Zhang, Mao Li
{"title":"Acetylation of Short Glycopeptides Enables Phase Separation.","authors":"Ning Wang, Chenxi Qiao, Jun Liu, Guohua Liu, Kun Zhang, Mao Li","doi":"10.1021/acs.biomac.4c01394","DOIUrl":"10.1021/acs.biomac.4c01394","url":null,"abstract":"<p><p>Liquid-liquid phase separation (LLPS) of biomacromolecules is crucial for regulating cellular functions. To explore their molecular mechanisms, peptide-based coacervates mimicking natural proteins have been developed, but the role of side chain modifications such as glycosylation remains underexplored. Here, we demonstrate that acetylation of short glycopeptides can induce pH- and concentration-dependent phase separation, while removing acetyl groups abolishes this behavior. Circular dichroism spectroscopy revealed a strong link between peptide structural ordering and the phase separation propensity. Peptides capable of forming liquid droplets displayed a significant ellipticity change at 205 nm upon changing solution pH. Moreover, these peptide coacervates can interact with cells and enhance the antiproliferative property of doxorubicin. Therefore, this work highlights the critical role of O-acetylation in LLPS and provides a valuable tool for studying the parameters regulating LLPS and its implications in cellular processes.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":"1595-1603"},"PeriodicalIF":5.5,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143187551","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}
BiomacromoleculesPub Date : 2025-03-10Epub Date: 2025-02-05DOI: 10.1021/acs.biomac.4c01331
Huan Liu, Ronger Ai, Bizhi Liu, Li He
{"title":"Dual ROS/Glucose-Responsive Quercetin-Loaded Supramolecular Hydrogel for Diabetic Wound Healing.","authors":"Huan Liu, Ronger Ai, Bizhi Liu, Li He","doi":"10.1021/acs.biomac.4c01331","DOIUrl":"10.1021/acs.biomac.4c01331","url":null,"abstract":"<p><p>Diabetic wound healing remains a significant challenge due to complex pathological mechanisms, including prolonged inflammation, excessive reactive oxygen species (ROS) accumulation, angiogenesis dysfunction, and increased susceptibility to bacterial infection. In this study, we developed a dual ROS/glucose-responsive quercetin-loaded supramolecular hydrogel (GPQ hydrogel) for treating diabetic wounds. The hydrogel was fabricated by incorporating quercetin (QUE) into a guanosine-phenylboronic acid (GP) hydrogel network through dynamic borate ester bonds. Structural characterization revealed the formation of a typical G-quadruplex structure in the GPQ hydrogel. The dual responsiveness to ROS and glucose enabled the controlled release of QUE, effectively addressing the abnormal wound microenvironment in diabetes. <i>In vitro</i> studies demonstrated the excellent antibacterial, antioxidant, anti-inflammatory, and pro-angiogenic properties of the GPQ hydrogel. Furthermore, the <i>in vivo</i> diabetic wound healing study using a full-thickness wound model in streptozotocin-induced diabetic rats showed that the GPQ hydrogel significantly accelerated wound closure, enhanced re-epithelialization and collagen deposition, and promoted angiogenesis compared to the control and GP hydrogel groups. Immunofluorescence analysis confirmed the superior antioxidant and pro-angiogenic effects of the GPQ hydrogel in the wound microenvironment. This study presents a promising multifunctional biomaterial for effectively managing diabetic wounds.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":"1541-1554"},"PeriodicalIF":5.5,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143253981","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}
BiomacromoleculesPub Date : 2025-03-10Epub Date: 2025-02-05DOI: 10.1021/acs.biomac.4c01453
Ruxia Ning, Chi Feng, Fenglun Zhang, Shiyu Zong, Jianxin Jiang
{"title":"Synthesis and Characterization of Superhigh Moisturizing Carboxymethyl Tamarind Xyloglucan and Its Potential Application in Cosmetics.","authors":"Ruxia Ning, Chi Feng, Fenglun Zhang, Shiyu Zong, Jianxin Jiang","doi":"10.1021/acs.biomac.4c01453","DOIUrl":"10.1021/acs.biomac.4c01453","url":null,"abstract":"<p><p>Carboxymethyl tamarind xyloglucan (CMTXG) was synthesized by xyloglucan with sodium chloroacetate in 50% ethanol. The effects of carboxymethylation on the structure and properties of xyloglucan were studied, and its application potential in cosmetics was evaluated. The results showed that carboxymethylation increased the molecular weight, enhanced water solubility and stability, decreased apparent viscosity, and promoted xyloglucan's application in cosmetics. The CMTXG with moderate substitution (CMT-M) exhibited superior hygroscopic and moisturizing effects, indicating that CMTXG does not need to pursue high degree of substitution. The moisturizing rate of CMT-M was 81.08% after 12 h, surpassing that of sodium hyaluronate (55.79%) and glycerin (59.52%). The CMT-M exhibited enhanced antioxidant and antibacterial activity after modification. Toxicity assessment indicated that CMT-M can improve the long-term tolerance of larvae zebrafish. Furthermore, the CMT-M cream demonstrated a long-term moisturizing effect compared to commercial creams. The research findings are expected to provide an effective bioactive moisturizer candidate for the daily chemical industry.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":"1647-1658"},"PeriodicalIF":5.5,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143254084","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}
{"title":"Metallo-Polyampholyte Hydrogel Based on a Y-Shaped Amphoteric Monomer with Robust Antibacterial and Antifouling Performance.","authors":"Qianyi Fang, Jing Yan, Weiwei Wang, Xueting Wang, Jingjie Chen, Yunxin Xu, Xudong Deng, Peng Li, Shixin Fa, Qiuyu Zhang, Yi Yan","doi":"10.1021/acs.biomac.4c01226","DOIUrl":"10.1021/acs.biomac.4c01226","url":null,"abstract":"<p><p>A Y-shaped metallo-amphoteric monomer with cobaltocenium as the cation and sulfonyl as the anion was synthesized and used to prepare the corresponding metallo-polyampholyte hydrogel (PAH). The cobaltocenium in the amphoteric system and its Y-shape may introduce tunable supramolecular interactions, providing regulation of hydration properties and biomedical performance. Such metallo-PAH showed a higher water swelling ratio and comparable mechanical performance in comparison with its organic counterpart, polysulfobetaine methacrylate hydrogel (SBMA-PAH). Moreover, the metallo-PAH showed a good inhibitory effect against Gram-negative bacteria, Gram-positive bacteria, as well as corresponding drug-resistant bacteria. Interestingly, it was found that the metallo-PAH achieved as high as 95% antifouling property against different proteins in both short-term (2 h) and long-term (24 h) tests, which is much better than that of the SBMA-PAH (<50%). It is believed that the concept of \"metallo-polyampholyte\" may expand the field of classical polyampholytes and related materials, thus opening up a new avenue to design powerful antifouling materials.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":"1498-1506"},"PeriodicalIF":5.5,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143424620","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}