Biomacromolecules最新文献_第2页

Lipid-Modified PEI Derivative-Based Binary/Ternary Polyplex Formulations for the Delivery of pDNA and mRNA in Primary Cells.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-03-27 DOI: 10.1021/acs.biomac.5c00169

Amarnath Praphakar Rajendran, Daniel Nisakar Meenakshi Sundaram, Luis Carlos Morales, Cezary Kucharski, Mohammad Nasrullah, Burcak Bulut, Pavlo Michailo Tsisar, Aislinn D Maguire, Bradley J Kerr, Hasan Uludağ

{"title":"Lipid-Modified PEI Derivative-Based Binary/Ternary Polyplex Formulations for the Delivery of pDNA and mRNA in Primary Cells.","authors":"Amarnath Praphakar Rajendran, Daniel Nisakar Meenakshi Sundaram, Luis Carlos Morales, Cezary Kucharski, Mohammad Nasrullah, Burcak Bulut, Pavlo Michailo Tsisar, Aislinn D Maguire, Bradley J Kerr, Hasan Uludağ","doi":"10.1021/acs.biomac.5c00169","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00169","url":null,"abstract":"A previous study has demonstrated the benefit of modification of polyethylenimine (PEI1.2k) by lipids through a p-hydroxyphenylacetic acid (PHPA) linker and polyanion (PA), which is now extended in this report to several primary cells. The formulated binary (lipopolymer/NAs) and ternary (lipopolymer/NAs/PA) complexes displayed no significant toxicity (MTT/hemolysis assay). The pDNA/mRNA complexes with PEI1.2k-PHPA-Lin9 and PEI1.2k-PHPA-Lau5-Ole5 lipopolymers showed gene expression levels higher than those of other lipopolymers. The transfection efficiencies of the ternary polyplexes of these lipopolymers possessed higher gene expression than those of the binary polyplexes. The serum-stable ternary polyplexes of PEI1.2k-PHPA-Lau5-Ole5 maintained high levels of mRNA expression in the lungs along with the spleen after intravenous injection. As in in vitro studies, transgene expression was relatively weak with binary complexes in muscle; however, a 10-fold higher efficiency was obtained with ternary complexes. Overall, our results provide improved gene formulations for the transfections of primary cells in vitro, as well as in in vivo animal models.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143727021","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

Hyperstable and Fibril-Forming Collagen-Mimetic Peptides in Shortest Triple Helices: Empowering the Capping by π-systems.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-03-27 DOI: 10.1021/acs.biomac.4c01455

Smriti Mukherjee, Vijayakumar Varshashankari, Ancy Feba, Niraikulam Ayyadurai, Kanagasabai Balamurugan, Ganesh Shanmugam

{"title":"Hyperstable and Fibril-Forming Collagen-Mimetic Peptides in Shortest Triple Helices: Empowering the Capping by π-systems.","authors":"Smriti Mukherjee, Vijayakumar Varshashankari, Ancy Feba, Niraikulam Ayyadurai, Kanagasabai Balamurugan, Ganesh Shanmugam","doi":"10.1021/acs.biomac.4c01455","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01455","url":null,"abstract":"Developing collagen-mimetic peptides (CMPs) with short triple helices and fibril-forming ability remains challenging. Herein, we stabilized short CMPs (3-6 GPO repeats) by attaching extended aromatic π-system─fluorenyl groups at the N-terminus and tyrosine at the C-terminus. These modifications promoted triple helix folding through π-π interactions, acting as a \"glue\" to stabilize the structure and facilitate fibrillation. A single fluorenyl cap required 5 GPO repeats for helix formation, while double fluorenyl capping reduced this to 4 repeats. Notably, at pH 5.5, triple helices formed with only 3 GPO repeats. The double-capped CMPs exhibited hyperstability (Tm = 76 °C) and formed fibrillar networks at physiological pH. Biophysical and computational studies confirmed the role of π-π and CH-π interactions, along with hydrogen bonding, in stabilization. The minimalistic CMPs supported cell viability, demonstrating their potential for biomedical applications. This strategy offers a method to design highly stable, short CMPs that form robust fibrillar networks.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143727020","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

Bioactive Polymeric Scaffolds: Multivalent Functionalization by Thermal Azide-Alkyne Cycloaddition with Alkynyl Dicarbamates.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-03-26 DOI: 10.1021/acs.biomac.5c00038

Maun H Tawara, Juan Correa, Emma Leire, Bruno Delgado Gonzalez, Samuel Parcero-Bouzas, Flonja Liko, Eduardo Fernandez-Megia

{"title":"Bioactive Polymeric Scaffolds: Multivalent Functionalization by Thermal Azide-Alkyne Cycloaddition with Alkynyl Dicarbamates.","authors":"Maun H Tawara, Juan Correa, Emma Leire, Bruno Delgado Gonzalez, Samuel Parcero-Bouzas, Flonja Liko, Eduardo Fernandez-Megia","doi":"10.1021/acs.biomac.5c00038","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00038","url":null,"abstract":"Multivalency enables interactions with higher affinities and specificities than monovalent interactions. The strategy exploited by nature to modulate biorecognition has inspired the design of multivalent conjugates with therapeutic properties. However, chemical functionalization often requires coupling agents, additives, or metal catalysts that complicate isolation and purification. Herein, azide-alkyne cycloaddition (AAC) with alkynyl dicarbamates (Alk-R) is presented as a flexible, reliable, atom-economical, and user-friendly strategy for the multivalent functionalization of polymeric scaffolds. Alk-R functionalized with biologically relevant ligands have been prepared and used for the multivalent AAC functionalization of azide-bearing dendrimers and block copolymers. The resulting polymers with double multivalency reveal a platform for the development of bioinspired functional systems with promising applications in drug delivery: block copolymer micelles and multifunctional nanocarriers with synergistically integrated probes-ligands-drugs. The extension of this strategy to other ligands and scaffolds is expected to open up a wide range of therapeutic and diagnostic opportunities.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143727016","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

Diboronate-Modified Hyaluronic Acid for Glucose-Responsive Insulin Delivery.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-03-26 DOI: 10.1021/acs.biomac.5c00144

Sijie Xian, Yuanhui Xiang, Katarína Mitrová, Jiří Jiráček, Matthew J Webber

{"title":"Diboronate-Modified Hyaluronic Acid for Glucose-Responsive Insulin Delivery.","authors":"Sijie Xian, Yuanhui Xiang, Katarína Mitrová, Jiří Jiráček, Matthew J Webber","doi":"10.1021/acs.biomac.5c00144","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00144","url":null,"abstract":"Diabetes requires precise insulin management to maintain glycemic control and prevent severe complications. Glucose-responsive delivery systems envision an autonomous approach to improve insulin therapy. Here, a glucose-sensitive insulin delivery system comprising hyaluronic acid conjugated with a diboronate glucose binder as a carrier for diol-modified insulin is shown. This approach seeks improved precision in insulin delivery, leveraging bidentate glucose binding to achieve enhanced glucose affinity and specificity. Modification of insulin with a diol motif preserves its native conformation and function. These insulin formulations correct blood glucose in diabetic mice, including glucose-responsive function when subjected to a glucose challenge. However, the absence of secondary interactions, such as electrostatic complexation, ultimately limits the duration of function relative to that of previous platforms. Integrating complementary interactions alongside dynamic-covalent glucose binders therefore enhances the functional duration and therapeutic efficacy in the design of glucose-responsive polymeric carriers, offering design insights into the development of new carriers for glucose-responsive insulin delivery.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143717596","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

NO-Releasing Metal-Organic Framework-Based Composite Coatings with Heparin-Mimicking Copolymers on Titanium Substrates: Impact on Vascular Cell Behavior.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-03-26 DOI: 10.1021/acs.biomac.5c00016

Denghai Sheng, Shuaihang Guo, Aiqing Li, Qiulian Wu, Mengying Zhan, Xiaoli Liu, Hong Chen

引用次数: 0

Enhancing Biodegradable Bone Plate Performance: Stereocomplex Polylactic Acid for Improved Mechanical Properties and Near-Infrared Transparency.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-03-25 DOI: 10.1021/acs.biomac.4c01768

Su Jeong Park, Ho-Kyung Lim, Sung-Jae Lee, Seung Hyuk Im, Jong Min Lee, Youngmee Jung, Soo Hyun Kim, Ji-Seok Shim, Jong-Eun Won, Justin J Chung, In-Seok Song

{"title":"Enhancing Biodegradable Bone Plate Performance: Stereocomplex Polylactic Acid for Improved Mechanical Properties and Near-Infrared Transparency.","authors":"Su Jeong Park, Ho-Kyung Lim, Sung-Jae Lee, Seung Hyuk Im, Jong Min Lee, Youngmee Jung, Soo Hyun Kim, Ji-Seok Shim, Jong-Eun Won, Justin J Chung, In-Seok Song","doi":"10.1021/acs.biomac.4c01768","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01768","url":null,"abstract":"The use of biodegradable materials in bone plates offers remarkable advantages; however, their application in bone fixation is limited by their brittleness. Moreover, treatments tailored to patient conditions are needed in orthopedics. In this study, bone plates were fabricated with stereocomplex polylactic acid (scPLA) and the effects of poly(d-lactic acid) molecular weight and scPLA blending ratios were analyzed. Although modulus values of poly(l-lactic acid) (PLLA) and scPLA were similar, strain resistance improved at higher scPLA proportions. The enhanced elongation was owing to the presence of tie molecules within the scPLA as opposed to single PLA chains. The fabricated scPLA bone plates exhibited improved mechanical properties and transparency in the optical and near-infrared ranges. scPLA was characterized by a smaller crystallite size. These properties of scPLA combined with its biocompatibility indicate potential for various diagnostic and therapeutic orthopedic applications. Comparisons with commercial PLLA-based bone plates show no significant differences in in vivo bone-healing ability.","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":"143699088","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

Improving Complex Coacervate Tissue Adhesive Performance Using Bridging Polymer Chains.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-03-25 DOI: 10.1021/acs.biomac.4c01801

Ayla N Kwant, Julien S Es Sayed, Nawal Aledlbi, Hanna Pryshchepa, Pieter J van der Zaag, Janette K Burgess, Dirk-Jan Slebos, Simon D Pouwels, Marleen Kamperman

{"title":"Improving Complex Coacervate Tissue Adhesive Performance Using Bridging Polymer Chains.","authors":"Ayla N Kwant, Julien S Es Sayed, Nawal Aledlbi, Hanna Pryshchepa, Pieter J van der Zaag, Janette K Burgess, Dirk-Jan Slebos, Simon D Pouwels, Marleen Kamperman","doi":"10.1021/acs.biomac.4c01801","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01801","url":null,"abstract":"Complex coacervates have emerged as promising tissue adhesives due to their excellent wet adhesion and tunable properties. However, maintaining stable adhesion on soft, dynamic tissues remains challenging. In this study, the use of a bridging polymer was investigated to enhance the adhesive properties of a complex coacervate adhesive (CCA) composed of poly(allylamine hydrochloride) (pAH) and polysulfopropyl methacrylate (pSPMA). The CCA undergoes solidification as a result of a change in salt concentration, forming a robust adhesive under physiological conditions. Pretreatment with pAH, but not pSPMA, significantly improved adhesion energy on both model hydrogels and biological tissues by forming a polymer-rich bridging layer at the interface. The beneficial effect was driven by accumulation of pAH in superficial layers of both the CCA and the substrates. This enabled the CCA to withstand higher deformation before adhesive failure. These findings underscore the potential of bridging polymers to improve CCAs and other tissue adhesives for biomedical 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":"143699089","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

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