Biomacromolecules最新文献

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Hydrogels Based on Polyelectrolyte Complexes: Underlying Principles and Biomedical Applications
IF 5.5 2区 化学
Biomacromolecules Pub Date : 2024-11-18 DOI: 10.1021/acs.biomac.4c0124010.1021/acs.biomac.4c01240
Belynn Sim, Jun Jie Chang, Qianyu Lin, Joey Hui Min Wong, Valerie Ow, Yihao Leow, Yi Jing Wong, Yi Jian Boo, Rubayn Goh* and Xian Jun Loh*, 
{"title":"Hydrogels Based on Polyelectrolyte Complexes: Underlying Principles and Biomedical Applications","authors":"Belynn Sim,&nbsp;Jun Jie Chang,&nbsp;Qianyu Lin,&nbsp;Joey Hui Min Wong,&nbsp;Valerie Ow,&nbsp;Yihao Leow,&nbsp;Yi Jing Wong,&nbsp;Yi Jian Boo,&nbsp;Rubayn Goh* and Xian Jun Loh*,&nbsp;","doi":"10.1021/acs.biomac.4c0124010.1021/acs.biomac.4c01240","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01240https://doi.org/10.1021/acs.biomac.4c01240","url":null,"abstract":"<p >Ionic complexes of electrostatically charged biomacromolecules are key players in various biological processes like nucleotide transportation, organelle formation, and protein folding. These complexes, abundant in biological systems, contribute to the function, responsiveness, and mechanical properties of organisms. Coherent with these natural phenomena, hydrogels formed through the complexation of oppositely charged polymers exhibit unique attributes, such as rapid self-assembly, hierarchical microstructures, tunable properties, and protective encapsulation. Consequently, polyelectrolyte complex (PEC) hydrogels have garnered considerable interest, emerging as an up-and-coming platform for various biomedical applications. This review outlines the underlying principles governing PEC hydrogels. The classification of polyelectrolytes and the self-assembly of PEC hydrogels are discussed, including the factors influencing their self-assembly process. Recent developments of PEC hydrogels for biomedical applications, including drug delivery, tissue engineering, wound healing and management, and wearable sensors, are summarized. This review concludes with the prospective directions for the next generation of PEC hydrogel research.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"25 12","pages":"7563–7580 7563–7580"},"PeriodicalIF":5.5,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842993","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
Single-Step Synthesis of Highly Sensitive 19F MRI Tracers by Gradient Copolymerization-Induced Self-Assembly
IF 5.5 2区 化学
Biomacromolecules Pub Date : 2024-11-18 DOI: 10.1021/acs.biomac.4c0091510.1021/acs.biomac.4c00915
Vyshakh M. Panakkal, Dominik Havlicek, Ewa Pavlova, Klara Jirakova, Daniel Jirak and Ondrej Sedlacek*, 
{"title":"Single-Step Synthesis of Highly Sensitive 19F MRI Tracers by Gradient Copolymerization-Induced Self-Assembly","authors":"Vyshakh M. Panakkal,&nbsp;Dominik Havlicek,&nbsp;Ewa Pavlova,&nbsp;Klara Jirakova,&nbsp;Daniel Jirak and Ondrej Sedlacek*,&nbsp;","doi":"10.1021/acs.biomac.4c0091510.1021/acs.biomac.4c00915","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c00915https://doi.org/10.1021/acs.biomac.4c00915","url":null,"abstract":"<p >Amphiphilic gradient copolymers are promising alternatives to block copolymers for self-assembled nanomaterials due to their straightforward synthesis via statistical copolymerization of monomers with different reactivities and hydrophilicity. By carefully selecting monomers, nanoparticles can be synthesized in a single step through gradient copolymerization-induced self-assembly (gPISA). We synthesized highly sensitive <sup>19</sup>F MRI nanotracers via aqueous dispersion gPISA of hydrophilic poly(ethylene glycol) methyl ether methacrylate (PEGMA) with core-forming <i>N</i>,<i>N</i>-(2,2,2-trifluoroethyl)acrylamide (TFEAM). The PPEGMA-grad-PTFEAM nanoparticles were optimized to achieve spherical morphology and exceptional <sup>19</sup>F MRI performance. Noncytotoxicity was confirmed in Panc-1 cells. In vitro <sup>19</sup>F MR relaxometry and imaging demonstrated their diagnostic imaging potential. Notably, these gradient copolymer nanotracers outperformed block copolymer analogs in <sup>19</sup>F MRI performance due to their gradient architecture, enhancing <sup>19</sup>F relaxivity. The synthetic versatility and superior <sup>19</sup>F MRI performance of gradient copolymers highlight their potential in advanced diagnostic imaging applications.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"25 12","pages":"7685–7694 7685–7694"},"PeriodicalIF":5.5,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.biomac.4c00915","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142843138","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}
引用次数: 0
The Improved Redispersibility of Cellulose Nanocrystals Using Hydroxypropyl Cellulose and Structure Color from Redispersed Cellulose Nanocrystals
IF 5.5 2区 化学
Biomacromolecules Pub Date : 2024-11-15 DOI: 10.1021/acs.biomac.4c0127710.1021/acs.biomac.4c01277
Huan Wang, Lukuan Guo*, Mingfeng Wu, Guang Chu, Wenyuan Zhu, Junlong Song and Jiaqi Guo*, 
{"title":"The Improved Redispersibility of Cellulose Nanocrystals Using Hydroxypropyl Cellulose and Structure Color from Redispersed Cellulose Nanocrystals","authors":"Huan Wang,&nbsp;Lukuan Guo*,&nbsp;Mingfeng Wu,&nbsp;Guang Chu,&nbsp;Wenyuan Zhu,&nbsp;Junlong Song and Jiaqi Guo*,&nbsp;","doi":"10.1021/acs.biomac.4c0127710.1021/acs.biomac.4c01277","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01277https://doi.org/10.1021/acs.biomac.4c01277","url":null,"abstract":"<p >Cellulose nanocrystals (CNC) have been significantly developed as a building block material for the design of novel functional materials in many fields such as biomedicine, nanotechnology, and materials science due to their excellent optical properties, biocompatibility, and sustainability. Improving the redispersibility of CNC in the sustainable processing of nanocellulose has been a challenge because intense hydrogen bond interaction leads to irreversible aggregation, making CNC difficult to redisperse and increasing the cost of storage and transportation of CNC. Hydroxypropyl cellulose (HPC) is an important hydroxy propylated cellulose ether. As a water-soluble cellulose derivative, HPC has a polyhydroxy structure similar to that of CNC, which leads to good compatibility and high affinity between HPC and CNC. In this work, HPC of different molecular weights was comixed with CNC of different contents, which was then dried using different methods, and the dried samples were redispersed in water. The addition of HPC improved the redispersibility of the CNC. Finally, the redispersed suspension was also redried to form a film, which was found to retain its structure color. These results provide an important avenue for the redispersion of dried CNC and for the development of functional materials from redispersed CNC.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"25 12","pages":"8006–8015 8006–8015"},"PeriodicalIF":5.5,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142843002","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
Adhesive, Stretchable, and Photothermal Antibacterial Hydrogel Dressings for Wound Healing of Infected Skin Burn at Joints 用于关节处感染性皮肤烧伤伤口愈合的粘性、可伸缩和光热抗菌水凝胶敷料
IF 5.5 2区 化学
Biomacromolecules Pub Date : 2024-11-14 DOI: 10.1021/acs.biomac.4c0102310.1021/acs.biomac.4c01023
Chen Zhang, Hua Zhao, Shanshan Geng, Chenghao Li, Jingmei Liu, Yuxin Chen, Ming Yi, Yuntong Liu, Fangxia Guan* and Minghao Yao*, 
{"title":"Adhesive, Stretchable, and Photothermal Antibacterial Hydrogel Dressings for Wound Healing of Infected Skin Burn at Joints","authors":"Chen Zhang,&nbsp;Hua Zhao,&nbsp;Shanshan Geng,&nbsp;Chenghao Li,&nbsp;Jingmei Liu,&nbsp;Yuxin Chen,&nbsp;Ming Yi,&nbsp;Yuntong Liu,&nbsp;Fangxia Guan* and Minghao Yao*,&nbsp;","doi":"10.1021/acs.biomac.4c0102310.1021/acs.biomac.4c01023","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01023https://doi.org/10.1021/acs.biomac.4c01023","url":null,"abstract":"<p >Dressings for infectious skin burn wounds at joints should have therapeutic functions as well as high tissue-adhesion, stretching, and self-healing properties. This makes it difficult for most hydrogel dressings to simultaneously meet the above-mentioned requirements. In this study, poly(vinyl alcohol), anhydrous sodium borax, epigallocatechin gallate, and copper chloride were used to prepare a hydrogel dressing (PBEC) for the infected burn wound healing at joints. The PBEC hydrogel can adhere to a variety of substrates, has a stretching capacity, and quickly self-healing after being damaged. Additionally, the PBEC hydrogel has the properties of reactive oxygen species scavenging, photothermal sterilization, hemostatic ability, and biocompatibility. Finally, the hydrogel could accelerate the process of wound healing in vivo, especially with the assistance of near-infrared radiation. Therefore, the hydrogel dressing shows great potential for clinical application in the healing of infected burn wounds at joints.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"25 12","pages":"7750–7766 7750–7766"},"PeriodicalIF":5.5,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142843287","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-Promoted TiO2-Loaded Double-Network Hydrogels for Dye Removal and Wearable Sensors
IF 5.5 2区 化学
Biomacromolecules Pub Date : 2024-11-14 DOI: 10.1021/acs.biomac.4c0128610.1021/acs.biomac.4c01286
Wei Gao, Huichun Kang, Ming Zhong*, Lijuan Han, Xue Guo, Bitao Su* and Ziqiang Lei, 
{"title":"Chitosan-Promoted TiO2-Loaded Double-Network Hydrogels for Dye Removal and Wearable Sensors","authors":"Wei Gao,&nbsp;Huichun Kang,&nbsp;Ming Zhong*,&nbsp;Lijuan Han,&nbsp;Xue Guo,&nbsp;Bitao Su* and Ziqiang Lei,&nbsp;","doi":"10.1021/acs.biomac.4c0128610.1021/acs.biomac.4c01286","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01286https://doi.org/10.1021/acs.biomac.4c01286","url":null,"abstract":"<p >The loading of photocatalysts on hydrogels can significantly reduce the loss of catalysts and effectively prevent secondary contamination, thus demonstrating great application potential and advantages in the field of wastewater treatment, especially in the removal of dyes. Herein, the semiconductor TiO<sub>2</sub> was successfully loaded into a polyacrylic acid/chitosan (PAA/CS) double-network (DN) hydrogel, which exhibited superior removal of dyes in wastewater such as MG, MB, MV, and RhB. The dye degradation process followed first-order kinetics, and the first-order rate constants for dye degradation were further calculated under UV light irradiation. Furthermore, the photocatalytic mechanism of the hydrogel was explored and analyzed. More interestingly, the PAA/CS-TiO<sub>2</sub> DN hydrogel has excellent tensile properties and superior electrical conductivity, which can be assembled into flexible sensors for real-time monitoring of mechanical deformations and human joint motions. It is envisioned that these excellent properties make hydrogel photocatalysts promising for a wide range of applications.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"25 12","pages":"8016–8025 8016–8025"},"PeriodicalIF":5.5,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142843107","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
Self-Healing, Electrically Conductive, Antibacterial, and Adhesive Eutectogel Containing Polymerizable Deep Eutectic Solvent for Human Motion Sensing and Wound Healing 自愈性、导电性、抗菌性和粘性共晶凝胶,含有可聚合的深共晶溶剂,用于人体运动传感和伤口愈合
IF 5.5 2区 化学
Biomacromolecules Pub Date : 2024-11-14 DOI: 10.1021/acs.biomac.4c0096010.1021/acs.biomac.4c00960
Shaghayegh Vakili, Zahra Mohamadnia* and Ebrahim Ahmadi*, 
{"title":"Self-Healing, Electrically Conductive, Antibacterial, and Adhesive Eutectogel Containing Polymerizable Deep Eutectic Solvent for Human Motion Sensing and Wound Healing","authors":"Shaghayegh Vakili,&nbsp;Zahra Mohamadnia* and Ebrahim Ahmadi*,&nbsp;","doi":"10.1021/acs.biomac.4c0096010.1021/acs.biomac.4c00960","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c00960https://doi.org/10.1021/acs.biomac.4c00960","url":null,"abstract":"<p >Flexible electronic devices such as wearable sensors are essential to advance human–machine interactions. Conductive eutectogels are promising for wearable sensors, despite their challenges in self-healing and adhesion properties. This study introduces a multifunctional eutectogel based on a novel polymerizable deep eutectic solvent (PDES) prepared by the incorporation of diallyldimethylammonium chloride (DADMAC) and glycerol in the presence of polycyclodextrin (PCD)/dopamine-grafted gelatin (Gel-DOP)/oxidized sodium alginate (OSA). The synthesized eutectogel has reversible Schiff-base bonds, hydrogen bonds, and host–guest interactions, which enable rapid self-healing upon network disruption. GPDO-15 eutectogel has significant tissue adhesion, high stretchability (419%), good ionic conductivity (0.79 mS·cm<sup>–1</sup>), and favorable antibacterial and self-healing properties. These eutectogels achieve 90% antibacterial effect, show excellent biocompatibility, and can be used as sensors to monitor human activities with strong stability and durability. The <i>in vivo</i> studies indicate that the eutectogels can improve the wound healing process which makes them an effective option for biological dressings.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"25 12","pages":"7704–7722 7704–7722"},"PeriodicalIF":5.5,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142843286","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
Antimicrobial Activity of Copolymer Structures from Bio-Based Monomers
IF 5.5 2区 化学
Biomacromolecules Pub Date : 2024-11-14 DOI: 10.1021/acs.biomac.4c0120310.1021/acs.biomac.4c01203
Mónica C. S. Fernandes, Rita Branco, Patrícia Pereira, Jorge F. J. Coelho, Paula V. Morais and Arménio C. Serra*, 
{"title":"Antimicrobial Activity of Copolymer Structures from Bio-Based Monomers","authors":"Mónica C. S. Fernandes,&nbsp;Rita Branco,&nbsp;Patrícia Pereira,&nbsp;Jorge F. J. Coelho,&nbsp;Paula V. Morais and Arménio C. Serra*,&nbsp;","doi":"10.1021/acs.biomac.4c0120310.1021/acs.biomac.4c01203","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01203https://doi.org/10.1021/acs.biomac.4c01203","url":null,"abstract":"<p >The urgent need for new antimicrobial compounds has led scientists to explore antimicrobial peptides (AMPs) and antimicrobial polymers as solutions for multidrug resistance. In this study, we synthesized copolymers with cationic and hydrophobic moieties by free-radical polymerization (FRP) using a chain transfer agent to control molecular weights. The potential of natural products as part of the hydrophobic moiety was evaluated, along with variations in their monomer content (13–25%) and the molecular weight (MW) of the copolymer (5000–20,000 g·mol<sup>–1</sup>). Hydrophobicity was evaluated using the theoretical Log <i>P</i><sub>oct</sub> values and surface areas (SAs). Biological assays included antimicrobial activity against <i>Escherichia coli</i> and <i>Staphylococcus aureus</i> standard strains, hemolytic activity in red blood cells (RBC), and cytotoxicity tests against HEK293T cells. Keys findings indicate that copolymers with tropolone moieties, lower MWs, and an optimal balance between hydrophobic and cationic moieties show a promising basis for future generations of antimicrobials.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"25 12","pages":"7915–7925 7915–7925"},"PeriodicalIF":5.5,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142850473","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
Alkylated RALA-Derived Peptides for Efficient Gene Delivery
IF 5.5 2区 化学
Biomacromolecules Pub Date : 2024-11-13 DOI: 10.1021/acs.biomac.4c0135510.1021/acs.biomac.4c01355
Xuelin Zhang, Yexi Zhang, Xi Rong, Chuanmei Tang, Huiye Liu, Lei Yue, Rongxin Su, Yuefei Wang* and Wei Qi*, 
{"title":"Alkylated RALA-Derived Peptides for Efficient Gene Delivery","authors":"Xuelin Zhang,&nbsp;Yexi Zhang,&nbsp;Xi Rong,&nbsp;Chuanmei Tang,&nbsp;Huiye Liu,&nbsp;Lei Yue,&nbsp;Rongxin Su,&nbsp;Yuefei Wang* and Wei Qi*,&nbsp;","doi":"10.1021/acs.biomac.4c0135510.1021/acs.biomac.4c01355","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01355https://doi.org/10.1021/acs.biomac.4c01355","url":null,"abstract":"<p >RALA is an amphipathic cationic peptide demonstrated to be a low-toxicity and high-efficiency delivery platform for the systemic delivery of nucleic acid therapeutics. This work reports three RALA-derived peptides modified with N-terminal palmitic acid, engineered through amino acid substitutions and truncated sequences. All three peptides have good nucleic acid encapsulation, release and uptake, biocompatibility, and endolysosome escape. The siRNA transfection efficiency is about 90%, and the silencing rate of GA (C16-GLFWHHHARLARALARHLARALRA) exceeds that of lipofectamine 2000 (siRNA concentration = 50 nM). Truncating the peptide chain while retaining a certain amount of arginine ensures an effective particle size. Replacing glutamic acid with three histidines ensures an effective zeta potential and accelerates the endosome escape process through the proton sponge phenomenon. Introducing phenylalanine enhances the carrier–cell interaction. We believe that they are powerful carriers of siRNA therapy and may have good application prospects in treating various diseases.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"25 12","pages":"8046–8057 8046–8057"},"PeriodicalIF":5.5,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849892","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
Customizable Glycopolymers as Adjuvants for Cancer Immunotherapy: From Branching Degree Optimization to Cell Surface Engineering
IF 5.5 2区 化学
Biomacromolecules Pub Date : 2024-11-13 DOI: 10.1021/acs.biomac.4c0123010.1021/acs.biomac.4c01230
Zhichen Zhu, Xingyu Heng, Fangjian Shan, He Yang, Yichen Wang, Hengyuan Zhang, Gaojian Chen* and Hong Chen*, 
{"title":"Customizable Glycopolymers as Adjuvants for Cancer Immunotherapy: From Branching Degree Optimization to Cell Surface Engineering","authors":"Zhichen Zhu,&nbsp;Xingyu Heng,&nbsp;Fangjian Shan,&nbsp;He Yang,&nbsp;Yichen Wang,&nbsp;Hengyuan Zhang,&nbsp;Gaojian Chen* and Hong Chen*,&nbsp;","doi":"10.1021/acs.biomac.4c0123010.1021/acs.biomac.4c01230","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01230https://doi.org/10.1021/acs.biomac.4c01230","url":null,"abstract":"<p >Engineering dendritic cell (DC) maturation is paramount for robust T-cell responses and immunological memory, critical for cancer immunotherapy. This work unveils a novel strategy using precisely controlled branching in synthetic glycopolymers to optimize DC activation. Using the distinct copolymerization kinetics of 2-(methacrylamido) glucopyranose (MAG) and diethylene glycol dimethacrylate (DEGDMA) in a RAFT polymerization, unique glycopolymers with varying branching degrees are created. These strategically produced gradient branched glycopolymers with sugar moieties on the outer chain potently promote DC maturation. Strikingly, low-branched glycopolymers demonstrate superior activity, both in pure form and when engineered on tumor cell surfaces. Quartz crystal microbalance and theoretical simulations elucidate the crucial role of branching in modulating glycopolymer–DC receptor interactions. Low-branched gradient glycopolymers have shown a notable advantage and are promising adjuvants in DC-based cancer immunotherapy.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"25 12","pages":"7975–7984 7975–7984"},"PeriodicalIF":5.5,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849891","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
Noncanonical Amino Acid Incorporation Modulates Condensate States of Intrinsically Disordered Proteins in Escherichia coli Cells. 非顺式氨基酸整合调节大肠杆菌细胞中内在紊乱蛋白质的凝结状态
IF 5.5 2区 化学
Biomacromolecules Pub Date : 2024-11-11 Epub Date: 2024-10-11 DOI: 10.1021/acs.biomac.4c00864
Ya-Jiao Zhu, Sheng-Chen Huang, Xiao-Xia Xia, Zhi-Gang Qian
{"title":"Noncanonical Amino Acid Incorporation Modulates Condensate States of Intrinsically Disordered Proteins in <i>Escherichia coli</i> Cells.","authors":"Ya-Jiao Zhu, Sheng-Chen Huang, Xiao-Xia Xia, Zhi-Gang Qian","doi":"10.1021/acs.biomac.4c00864","DOIUrl":"10.1021/acs.biomac.4c00864","url":null,"abstract":"<p><p>Biomolecular condensates are distinct subcellular structures with on-demand material states and dynamics in living cells. However, strategies for modulating their material states and physicochemical properties are lacking. Here, we report a chemical strategy for modulating the condensate states of intrinsically disordered proteins in bacterial <i>Escherichia coli</i> cells. This is achieved by noncanonical amino acid (DOPA) incorporation into model resilin-like proteins (RLPs) to endow autonomous oxidative and coordinative cross-linking mechanisms. Biogenesis of spherical gel-like condensates is achieved upon heterologous expression of the DOPA-incorporated RLP in the cells at 30 °C. We reveal that liquid-liquid phase separation underlies the formation of liquid condensates, and this liquid-like state is metastable and its dynamics is compromised by the oxidative and coordinative cross-linkings that ultimately drive the liquid-to-gel transition. Therefore, this study has deepened our understanding of biomolecular condensation and offers a new chemical strategy to expand the landscape of condensation phenotypes of living cells.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":"7191-7201"},"PeriodicalIF":5.5,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142398690","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
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