Pub Date : 2025-12-08DOI: 10.1021/acs.biomac.5c01431
Nea B. Möttönen , Ruxia Fan , Stefania Aspholm-Tsironi , Salla Keskitalo , Antti Tuhkala , Markku Varjosalo , A. Sesilja Aranko
Phosphorylation is considered to play a role in many of the functional properties of silk proteins, affecting their solubility, environmental adaptability, adhesion, and biocompatibility. However, investigating these effects has been hampered by the difficulty of isolating phosphorylated proteins from natural sources and the limitations of the current in vitro phosphorylation techniques. Here, we present a novel in vivo phosphorylation strategy for recombinant silk proteins in Escherichia coli, utilizing an engineered SpyCatcher/SpyTag system to induce proximity between the target protein and kinase. This scaffolding approach enhances kinase specificity and minimizes off-target effects, increasing the phosphorylation efficiency while preserving cell viability. We demonstrate the applicability of this system to both dragline and aggregate spider silks. Furthermore, we show that polyphosphorylation enhanced the adhesive properties of silk proteins. This modular and tunable strategy provides a powerful platform for producing polyphosphorylated fibrous proteins, offering broad implications for biomaterial design and functional protein engineering.
{"title":"Induced Proximity Approach Enables the Recombinant Production of Polyphosphorylated Silk Proteins with Improved Adhesiveness","authors":"Nea B. Möttönen , Ruxia Fan , Stefania Aspholm-Tsironi , Salla Keskitalo , Antti Tuhkala , Markku Varjosalo , A. Sesilja Aranko","doi":"10.1021/acs.biomac.5c01431","DOIUrl":"10.1021/acs.biomac.5c01431","url":null,"abstract":"<div><div>Phosphorylation is considered to play a role in many of the functional properties of silk proteins, affecting their solubility, environmental adaptability, adhesion, and biocompatibility. However, investigating these effects has been hampered by the difficulty of isolating phosphorylated proteins from natural sources and the limitations of the current <em>in vitro</em> phosphorylation techniques. Here, we present a novel <em>in vivo</em> phosphorylation strategy for recombinant silk proteins in Escherichia coli, utilizing an engineered SpyCatcher/SpyTag system to induce proximity between the target protein and kinase. This scaffolding approach enhances kinase specificity and minimizes off-target effects, increasing the phosphorylation efficiency while preserving cell viability. We demonstrate the applicability of this system to both dragline and aggregate spider silks. Furthermore, we show that polyphosphorylation enhanced the adhesive properties of silk proteins. This modular and tunable strategy provides a powerful platform for producing polyphosphorylated fibrous proteins, offering broad implications for biomaterial design and functional protein engineering.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (106KB)</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 12","pages":"Pages 8594-8605"},"PeriodicalIF":5.4,"publicationDate":"2025-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145601270","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}
The urgent demand for stable and accurate sensors emphasizes the importance of high mechanical and adhesion properties in conductive hydrogels. However, it remains challenging to concurrently enhance these two properties due to the inherent contradiction between internal cohesion and external adhesion. Here, lignin, an underutilized natural resource, is proposed to conquer the design difficulty described above by zwitterionization. Upon π–π aggregation, electronegative lignin readily self-assembles into zwitterionic lignin with a benzyltrimethylammonium cation. The zwitterionic lignin can simultaneously promote supramolecular interactions among lignin, polymer chains (poly(acrylic acid) and gelatin), and adhesive substrates. Hence, the internal cross-linking and external adhesion are enhanced synchronously. Notably, the hydrogel demonstrates a remarkable true stress of 2.34 MPa at a strain of 1597.1%, and the peak adhesion strength of the hydrogel is achieved at 40.87 kPa. By valorizing waste lignin, this work opens up a new path to overcome the inherent design contradiction for high-performance hydrogels in the future.
{"title":"Self-Assembled Zwitterionic Lignin-Induced Joint Enhancement of Mechanics and Adhesion in High-Performance Hydrogels for Flexible Strain Sensors","authors":"Dawei Fang, Jiangping Bian, Yutong Xiang, Yu Wang, Tonglei Zhu, Ying Kang","doi":"10.1021/acs.biomac.5c01574","DOIUrl":"10.1021/acs.biomac.5c01574","url":null,"abstract":"<div><div>The urgent demand for stable and accurate sensors emphasizes the importance of high mechanical and adhesion properties in conductive hydrogels. However, it remains challenging to concurrently enhance these two properties due to the inherent contradiction between internal cohesion and external adhesion. Here, lignin, an underutilized natural resource, is proposed to conquer the design difficulty described above by zwitterionization. Upon π–π aggregation, electronegative lignin readily self-assembles into zwitterionic lignin with a benzyltrimethylammonium cation. The zwitterionic lignin can simultaneously promote supramolecular interactions among lignin, polymer chains (poly(acrylic acid) and gelatin), and adhesive substrates. Hence, the internal cross-linking and external adhesion are enhanced synchronously. Notably, the hydrogel demonstrates a remarkable true stress of 2.34 MPa at a strain of 1597.1%, and the peak adhesion strength of the hydrogel is achieved at 40.87 kPa. By valorizing waste lignin, this work opens up a new path to overcome the inherent design contradiction for high-performance hydrogels in the future.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (274KB)</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 12","pages":"Pages 8652-8667"},"PeriodicalIF":5.4,"publicationDate":"2025-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145429633","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}
Pub Date : 2025-12-08DOI: 10.1021/acs.biomac.5c01269
John A. Terrell, Chengpeng Chen
Recent works in mechanobiology have investigated overarching changes in cell behavior in response to extracellular matrix (ECM) stiffness. Nonetheless, little is known about how key metabolic pathways and critical metabolites are regulated by the ECM microstructures. Glutathione, a tripeptide predominantly synthesized in the liver, is a critical molecule used for the metabolism of certain xenobiotics and the reduction of oxidative species. Here, we report that the ECM microstructures can directly regulate the glutathione bioavailability and synthesis. By preparing a fibrous scaffold to mimic healthy native liver ECM and a flat substrate mimicking severe fibrotic conditions with the same surface chemistry, we found that the fibrous ECM upregulated glutathione levels in hepatocytes with enhanced antioxidation capacity. Mechanistic studies involving reducing and increasing integrin β1 activation suggested that ECM microstructures, integrin β1, and intracellular hepatic glutathione synthesis were mechanistically linked. These results represented an unprecedented discovery in mechanobiology regarding ECM microstructures’ role in regulating the hepatic metabolome, i.e., glutathione bioavailability, which can provide new insights into understanding and treating fibrotic liver diseases.
{"title":"Extracellular Matrix Microstructures Directly Regulate Glutathione Bioavailability in Human Hepatocytes","authors":"John A. Terrell, Chengpeng Chen","doi":"10.1021/acs.biomac.5c01269","DOIUrl":"10.1021/acs.biomac.5c01269","url":null,"abstract":"<div><div>Recent works in mechanobiology have investigated overarching changes in cell behavior in response to extracellular matrix (ECM) stiffness. Nonetheless, little is known about how key metabolic pathways and critical metabolites are regulated by the ECM microstructures. Glutathione, a tripeptide predominantly synthesized in the liver, is a critical molecule used for the metabolism of certain xenobiotics and the reduction of oxidative species. Here, we report that the ECM microstructures can directly regulate the glutathione bioavailability and synthesis. By preparing a fibrous scaffold to mimic healthy native liver ECM and a flat substrate mimicking severe fibrotic conditions with the same surface chemistry, we found that the fibrous ECM upregulated glutathione levels in hepatocytes with enhanced antioxidation capacity. Mechanistic studies involving reducing and increasing integrin β1 activation suggested that ECM microstructures, integrin β1, and intracellular hepatic glutathione synthesis were mechanistically linked. These results represented an unprecedented discovery in mechanobiology regarding ECM microstructures’ role in regulating the hepatic metabolome, i.e., glutathione bioavailability, which can provide new insights into understanding and treating fibrotic liver diseases.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (196KB)</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 12","pages":"Pages 8475-8483"},"PeriodicalIF":5.4,"publicationDate":"2025-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145487137","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}
Pub Date : 2025-12-08DOI: 10.1021/acs.biomac.5c01689
Busra Ozlu , Bong Sup Shim
Polydopamine (PDA), a synthetic analogue of natural biopolymer melanin, possesses a conjugated backbone that theoretically offers conductive pathways. However, the synthesis of conductive PDA has proven to be challenging, with only a few studies successfully achieving structural control during polymerization. In this study, the electrochemical synthesis of conductive PDA using various counterions, including lithium perchlorate (LiClO4), potassium hexafluorophosphate (KPF6), sodium p-toluene sulfonate (Na+-pTS), iron p-toluene sulfonate (Fe3+-pTS), and sodium polystyrenesulfonate, was systematically investigated in terms of their effect on the surface morphology, chemical structure, and electrochemical properties of PDA. To our knowledge, this is the first study to explore the role of counterions during the electropolymerization of PDA, resulting in significant improvements in its structure, hence the electrochemical performance. These findings suggest that the incorporation of counterions can pave the way for developing conductive PDA, which can be tailored for a wide range of bioelectronic applications.
{"title":"Versatile Conductive Polydopamine via Tailoring Counterions","authors":"Busra Ozlu , Bong Sup Shim","doi":"10.1021/acs.biomac.5c01689","DOIUrl":"10.1021/acs.biomac.5c01689","url":null,"abstract":"<div><div>Polydopamine (PDA), a synthetic analogue of natural biopolymer melanin, possesses a conjugated backbone that theoretically offers conductive pathways. However, the synthesis of conductive PDA has proven to be challenging, with only a few studies successfully achieving structural control during polymerization. In this study, the electrochemical synthesis of conductive PDA using various counterions, including lithium perchlorate (LiClO<sub>4</sub>), potassium hexafluorophosphate (KPF<sub>6</sub>), sodium <em>p</em>-toluene sulfonate (Na<sup>+</sup>-pTS), iron <em>p</em>-toluene sulfonate (Fe<sup>3+</sup>-pTS), and sodium polystyrenesulfonate, was systematically investigated in terms of their effect on the surface morphology, chemical structure, and electrochemical properties of PDA. To our knowledge, this is the first study to explore the role of counterions during the electropolymerization of PDA, resulting in significant improvements in its structure, hence the electrochemical performance. These findings suggest that the incorporation of counterions can pave the way for developing conductive PDA, which can be tailored for a wide range of bioelectronic applications.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (221KB)</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 12","pages":"Pages 8713-8725"},"PeriodicalIF":5.4,"publicationDate":"2025-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145493800","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}
Pub Date : 2025-12-08DOI: 10.1021/acs.biomac.5c02106
Lixia Liao, Jiaqi Ding, Xiao Xiong, Fengjiao Quan, Xingxing Liu, Min Zhu, Zehui Chen, Sheng Li, Lian Zhu, Benmei Wei, Juntao Zhang, Haibo Wang
Conductive hydrogels are promising for flexible electronics, yet integrating high conductivity, mechanical robustness, biocompatibility, and environmental stability for flexible supercapacitors (FSCs) and wearable epidermal sensors remains challenging. Herein, a self-healing hydrogel with multiple energy dissipation pathways was constructed using synergistic dynamic borate ester bonds, Schiff base bonds, and hydrogen bonds. Incorporating polydopamine-coated MXene (MP) enhanced the mechanical strength, conductivity, and antibacterial/antioxidant properties. FSCs with the hydrogel electrolyte exhibited excellent electrochemical performance with a specific capacitance of 373.41 mF/cm2, an energy density of 74.67 μWh/cm2, a capacitance retention of 82.43% after 5000 cycles, and high deformation tolerance. As a strain sensor, it effectively detected both large and subtle human motions, including physiological microexpressions and pulse beats due to its high sensitivity (gauge factor = 1.73) and repeatability. Importantly, its notable degradability owing to the inherent degradability of the chitosan framework and the reversible dissociation of dynamic bonds addresses environmental concerns from traditional electronics.
{"title":"Triple-Dynamic-Bond-Engineered Self-Healing Conductive Hydrogels for Deformation-Immune Flexible Supercapacitors and Wearable Epidermal Sensors.","authors":"Lixia Liao, Jiaqi Ding, Xiao Xiong, Fengjiao Quan, Xingxing Liu, Min Zhu, Zehui Chen, Sheng Li, Lian Zhu, Benmei Wei, Juntao Zhang, Haibo Wang","doi":"10.1021/acs.biomac.5c02106","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c02106","url":null,"abstract":"<p><p>Conductive hydrogels are promising for flexible electronics, yet integrating high conductivity, mechanical robustness, biocompatibility, and environmental stability for flexible supercapacitors (FSCs) and wearable epidermal sensors remains challenging. Herein, a self-healing hydrogel with multiple energy dissipation pathways was constructed using synergistic dynamic borate ester bonds, Schiff base bonds, and hydrogen bonds. Incorporating polydopamine-coated MXene (MP) enhanced the mechanical strength, conductivity, and antibacterial/antioxidant properties. FSCs with the hydrogel electrolyte exhibited excellent electrochemical performance with a specific capacitance of 373.41 mF/cm<sup>2</sup>, an energy density of 74.67 μWh/cm<sup>2</sup>, a capacitance retention of 82.43% after 5000 cycles, and high deformation tolerance. As a strain sensor, it effectively detected both large and subtle human motions, including physiological microexpressions and pulse beats due to its high sensitivity (gauge factor = 1.73) and repeatability. Importantly, its notable degradability owing to the inherent degradability of the chitosan framework and the reversible dissociation of dynamic bonds addresses environmental concerns from traditional electronics.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.4,"publicationDate":"2025-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145699301","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}
Pub Date : 2025-12-08DOI: 10.1021/acs.biomac.5c01549
Suqing Shi , Qingyan Kang , Chang Yang , Xudong Liu , Yumeng Zhang , Mengya Sun , Linghan Xiao , Wei Zhu , Yujing Liu
Diabetic wounds suffer from delayed healing due to impaired angiogenesis, bacterial infection, and mechanical damage from dressing changes. This study developed an AP-G-OSA-GB-ICG hydrogel via Schiff base and borate ester bonds. The temperature-responsive conductive system integrates photothermal therapy (PTT) and nitric oxide (NO) release for synergistic antibacterial effects. Graphene oxide-BNN6 (GB) and indocyanine green (ICG) eliminate bacteria via near-infrared (NIR) photothermal effects, while light-triggered NO from BNN6 promotes angiogenesis. Gelatin-based thermal responsiveness enables body temperature-triggered adhesion switching to reduce neotissue damage. Graphene oxide (GO) endows electrical conductivity for potential physiological signal monitoring. In type 1 diabetic SD rats, the hydrogel with NIR irradiation and NO release achieved 100% wound closure at day 14. Masson trichrome staining showed orderly collagen fiber deposition, CD31 and α-SMA immunostaining confirmed a significant increase in vessel density. Hematoxylin and eosin (H&E) staining further revealed the absence of significant inflammatory cell infiltration. This multifunctional system integrates antibacterial activity, angiogenesis promotion, intelligent adhesion, and physiological monitoring, offering a mechanistically innovative and clinically translatable strategy for diabetic wound precision treatment.
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糖尿病伤口由于血管生成受损、细菌感染和换药造成的机械损伤而延迟愈合。本研究通过希夫碱和硼酸酯键制备了ap - g - sa - gb - icg水凝胶。该温度响应传导系统集成了光热疗法(PTT)和一氧化氮(NO)释放,具有协同抗菌作用。氧化石墨烯-BNN6 (GB)和吲哚菁绿(ICG)通过近红外(NIR)光热效应消除细菌,而BNN6的光触发NO促进血管生成。基于明胶的热响应性使体温触发的粘附切换能够减少新组织损伤。氧化石墨烯(GO)具有良好的导电性,可用于监测潜在的生理信号。在1型糖尿病SD大鼠中,近红外照射和NO释放的水凝胶在第14天达到100%的伤口愈合。马松三色染色显示胶原纤维有序沉积,CD31和α-SMA免疫染色证实血管密度明显增加。苏木精和伊红(H&E)染色进一步显示没有明显的炎症细胞浸润。该多功能系统集抗菌活性、促进血管生成、智能粘附和生理监测于一体,为糖尿病伤口精准治疗提供了一种机制创新和临床可翻译的策略。
{"title":"Fault-Tolerant Adhesive Intelligent Hydrogels Accelerate Diabetic Wound Healing through On-Demand Release of Photothermal/Nitric Oxide and Real-Time Monitoring","authors":"Suqing Shi , Qingyan Kang , Chang Yang , Xudong Liu , Yumeng Zhang , Mengya Sun , Linghan Xiao , Wei Zhu , Yujing Liu","doi":"10.1021/acs.biomac.5c01549","DOIUrl":"10.1021/acs.biomac.5c01549","url":null,"abstract":"<div><div>Diabetic wounds suffer from delayed healing due to impaired angiogenesis, bacterial infection, and mechanical damage from dressing changes. This study developed an AP-G-OSA-GB-ICG hydrogel via Schiff base and borate ester bonds. The temperature-responsive conductive system integrates photothermal therapy (PTT) and nitric oxide (NO) release for synergistic antibacterial effects. Graphene oxide-BNN6 (GB) and indocyanine green (ICG) eliminate bacteria via near-infrared (NIR) photothermal effects, while light-triggered NO from BNN6 promotes angiogenesis. Gelatin-based thermal responsiveness enables body temperature-triggered adhesion switching to reduce neotissue damage. Graphene oxide (GO) endows electrical conductivity for potential physiological signal monitoring. In type 1 diabetic SD rats, the hydrogel with NIR irradiation and NO release achieved 100% wound closure at day 14. Masson trichrome staining showed orderly collagen fiber deposition, CD31 and α-SMA immunostaining confirmed a significant increase in vessel density. Hematoxylin and eosin (H&E) staining further revealed the absence of significant inflammatory cell infiltration. This multifunctional system integrates antibacterial activity, angiogenesis promotion, intelligent adhesion, and physiological monitoring, offering a mechanistically innovative and clinically translatable strategy for diabetic wound precision treatment.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (197KB)</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 12","pages":"Pages 8606-8621"},"PeriodicalIF":5.4,"publicationDate":"2025-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145450301","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}
Nanofiber microspheres are widely used in biomedical devices and tissue engineering for their unique structure and nanoscale effects but suffer from complex fabrication and limited biocompatibility. This study prepared hydrogel microspheres (specific surface area: 153.69 m2/g) via electrostatic spraying, using silk nanofibers (SNF) and sodium alginate (SA). These microspheres showed excellent biocompatibility (over 90% viability of human umbilical vein endothelial cells after 7 days of culture). As drug carriers, doxorubicin hydrochloride-loaded ones achieved 60% drug release within 72 h and reduced cancer cell viability to below 40%. Fluorescent peptide-grafted SNF/SA microspheres enhanced protease detection sensitivity (detection limit: 9.75 pM), outperforming conventional probes. Moreover, SNF/SA/hydroxyapatite (HAp) hybrid microspheres (with a hierarchically porous structure) promoted deep cellular migration in 7 days, increased osteoblast differentiation by over 50%, and accelerated proliferation by 30%, offering dual osteogenic activity and biocompatibility. This study provides an innovative strategy for silk fibroin-based biomedical devices and materials.
{"title":"Facial Preparation of Multifunctional Silk Fibroin Nanofiber Hydrogel Microspheres as a Biomedical Platform","authors":"Luyao Zhong , Jiaxin Wang , Renchuan You, Ying Huang, Shuqin Yan, Qiang Zhang","doi":"10.1021/acs.biomac.5c01004","DOIUrl":"10.1021/acs.biomac.5c01004","url":null,"abstract":"<div><div>Nanofiber microspheres are widely used in biomedical devices and tissue engineering for their unique structure and nanoscale effects but suffer from complex fabrication and limited biocompatibility. This study prepared hydrogel microspheres (specific surface area: 153.69 m<sup>2</sup>/g) via electrostatic spraying, using silk nanofibers (SNF) and sodium alginate (SA). These microspheres showed excellent biocompatibility (over 90% viability of human umbilical vein endothelial cells after 7 days of culture). As drug carriers, doxorubicin hydrochloride-loaded ones achieved 60% drug release within 72 h and reduced cancer cell viability to below 40%. Fluorescent peptide-grafted SNF/SA microspheres enhanced protease detection sensitivity (detection limit: 9.75 pM), outperforming conventional probes. Moreover, SNF/SA/hydroxyapatite (HAp) hybrid microspheres (with a hierarchically porous structure) promoted deep cellular migration in 7 days, increased osteoblast differentiation by over 50%, and accelerated proliferation by 30%, offering dual osteogenic activity and biocompatibility. This study provides an innovative strategy for silk fibroin-based biomedical devices and materials.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (209KB)</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 12","pages":"Pages 8370-8381"},"PeriodicalIF":5.4,"publicationDate":"2025-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145511179","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}
Pub Date : 2025-12-08DOI: 10.1021/acs.biomac.5c01633
Haifeng Chen , Zijian Deng , Wenzhu Li , Weimiao Lu , Jingda Huang , Wenbiao Zhang
Polylactic acid (PLA) films are limited in their further applications due to their high brittleness. To enhance the toughness of PLA-based films, UFBC modified with biocohesive agents (TA-ESO) was used, in this study, to improve compatibility and interlocking adhesion with PLA. Benefiting from the effects of TA-ESO in plasticization and interface improvement, TA-ESO-modified UFBC can make PLA more pliable while establishing a stronger mechanical interlocking structure, thus raising the mechanical properties of the system. Compared to pure PLA films, the tensile elongation of TA-ESO-modified UFBC/PLA composite films increased by 189.11%, and the tensile strength remained at a high level of 23.95 MPa, along with an increase in crystallinity (Xc) from 1.09 to 2.05%. Given their excellent strength and toughness, TA-ESO-modified UFBC/PLA composite films are expected to offer various potential applications in the packaging, medical, and agricultural fields.
{"title":"Bio-Modified UFBC Interlocking Structure for Enhanced Interfacial Design of PLA Films with Improved Plasticity and Compatibility","authors":"Haifeng Chen , Zijian Deng , Wenzhu Li , Weimiao Lu , Jingda Huang , Wenbiao Zhang","doi":"10.1021/acs.biomac.5c01633","DOIUrl":"10.1021/acs.biomac.5c01633","url":null,"abstract":"<div><div>Polylactic acid (PLA) films are limited in their further applications due to their high brittleness. To enhance the toughness of PLA-based films, UFBC modified with biocohesive agents (TA-ESO) was used, in this study, to improve compatibility and interlocking adhesion with PLA. Benefiting from the effects of TA-ESO in plasticization and interface improvement, TA-ESO-modified UFBC can make PLA more pliable while establishing a stronger mechanical interlocking structure, thus raising the mechanical properties of the system. Compared to pure PLA films, the tensile elongation of TA-ESO-modified UFBC/PLA composite films increased by 189.11%, and the tensile strength remained at a high level of 23.95 MPa, along with an increase in crystallinity (<em>X</em> <sub>c</sub>) from 1.09 to 2.05%. Given their excellent strength and toughness, TA-ESO-modified UFBC/PLA composite films are expected to offer various potential applications in the packaging, medical, and agricultural fields.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (272KB)</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 12","pages":"Pages 8676-8685"},"PeriodicalIF":5.4,"publicationDate":"2025-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145581590","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}
Pub Date : 2025-12-08DOI: 10.1021/acs.biomac.5c02360
Maike Petermann, Lucie Dianteill, Amal Zeidi, Roméo Vaha Ouloassekpa, Paul Budisavljevic, Claude Le Men, Cédric Montanier, Pierre Roblin, Bernard Cabane, Ralf Schweins, Claire Dumon, Antoine Bouchoux
{"title":"Correction to \"Arabinoxylan in Water through SANS: Single Chain Conformation, Chain Overlap, and Clustering\".","authors":"Maike Petermann, Lucie Dianteill, Amal Zeidi, Roméo Vaha Ouloassekpa, Paul Budisavljevic, Claude Le Men, Cédric Montanier, Pierre Roblin, Bernard Cabane, Ralf Schweins, Claire Dumon, Antoine Bouchoux","doi":"10.1021/acs.biomac.5c02360","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c02360","url":null,"abstract":"","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.4,"publicationDate":"2025-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145699233","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}
Pub Date : 2025-12-08DOI: 10.1021/acs.biomac.5c01178
Pawel Wolski , Chris Oostenbrink , Tomasz Panczyk
Understanding nanoparticle–protein interactions is crucial for designing biocompatible nanocarriers. Here, we performed atomistic molecular dynamics simulations to investigate the binding of human serum albumin (HSA) with carbon quantum dot (CQD)–based nanoparticles functionalized with poly(amidoamine) (PAMAM) dendrimers modified by zwitterionic carboxybetaine acrylamide (CBAA). Three systems with 0% (M0), 50% (M50), and 90% (M90) CBAA modifications were constructed to assess the effect of surface zwitterion density on protein adsorption, hydration, and structural stability. The fully modified M90 nanoparticles exhibited the weakest HSA binding due to reduced electrostatic attraction and steric shielding as well as the formation of a stable, dense hydration layer that hindered protein attachment. Across all systems, HSA retained its secondary structure, confirming its structural compatibility. These findings provide molecular insights into the antifouling mechanisms of CBAA-modified CQD–PAMAM nanocarriers and guide their rational design for enhanced biocompatibility.
{"title":"Tuning Protein–Nanoparticle Interfacial Interactions via Zwitterionic Surface Functionalization: A Molecular Dynamics Study of HSA Adsorption on Dendrimer-Coated Carbon Quantum Dots","authors":"Pawel Wolski , Chris Oostenbrink , Tomasz Panczyk","doi":"10.1021/acs.biomac.5c01178","DOIUrl":"10.1021/acs.biomac.5c01178","url":null,"abstract":"<div><div>Understanding nanoparticle–protein interactions is crucial for designing biocompatible nanocarriers. Here, we performed atomistic molecular dynamics simulations to investigate the binding of human serum albumin (HSA) with carbon quantum dot (CQD)–based nanoparticles functionalized with poly(amidoamine) (PAMAM) dendrimers modified by zwitterionic carboxybetaine acrylamide (CBAA). Three systems with 0% (M0), 50% (M50), and 90% (M90) CBAA modifications were constructed to assess the effect of surface zwitterion density on protein adsorption, hydration, and structural stability. The fully modified M90 nanoparticles exhibited the weakest HSA binding due to reduced electrostatic attraction and steric shielding as well as the formation of a stable, dense hydration layer that hindered protein attachment. Across all systems, HSA retained its secondary structure, confirming its structural compatibility. These findings provide molecular insights into the antifouling mechanisms of CBAA-modified CQD–PAMAM nanocarriers and guide their rational design for enhanced biocompatibility.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (118KB)</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 12","pages":"Pages 8430-8441"},"PeriodicalIF":5.4,"publicationDate":"2025-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145487167","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}