Biomacromolecules最新文献_第3页

Internal Secondary Structural Conformational States of Silk Fibroin Studied by Raman Spectroscopy with Band Deconvolution Analysis. 拉曼光谱与频带解卷积分析法研究蚕丝纤维素的内部二级结构构象状态

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-02-21 DOI: 10.1021/acs.biomac.4c01827

Xiang Ben, Xinxin Lu, Gutian Zhao, Zhiyong Wei, Juekuan Yang, Yajing Kan

{"title":"Internal Secondary Structural Conformational States of Silk Fibroin Studied by Raman Spectroscopy with Band Deconvolution Analysis.","authors":"Xiang Ben, Xinxin Lu, Gutian Zhao, Zhiyong Wei, Juekuan Yang, Yajing Kan","doi":"10.1021/acs.biomac.4c01827","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01827","url":null,"abstract":"Silk fibroin (SF) is an extensively utilized biofiber recognized for its excellent mechanical properties across various applications. However, the relationship between its internal structure and mechanical behavior remains inadequately understood. In this work, we employed polarized Raman spectra to investigate how SF's secondary structures respond to external tensile loads. Our results show considerable variations in the amide III band, particularly the 1210 cm-1 random coil subpeak, under tensile stimuli. Subsequent loading-unloading experiments that plotted the peak intensity ratio of I1210 cm-1/I1226 cm-1 against tensile strain produced multiple hysteresis loops, suggesting irreversible structural changes during mechanical cycling. With additional evidence from other characteristic bands, we demonstrate that tensile elongation facilitates the transition of random coils to β-sheets within the SF network, which intrinsically contributes to the fiber's stiffening behavior. This work provides valuable insight into SF's deformation mechanism and highlights the significance of the previously underappreciated amide III band.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143466442","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

Synthesis and Characterization of λ-Carrageenan Oligosaccharide-Based Nanoparticles: Applications in MRI and In Vivo Biodistribution Studies.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-02-21 DOI: 10.1021/acs.biomac.4c01747

Manon Porta-Zapata, Susana Carregal-Romero, Jennifer Saliba, Ainhize Urkola-Arsuaga, Claudia Beatriz Miranda Perez de Alejo, Iñaki Orue, Lydia Martínez-Parra, Desirè Di Silvio, Armel Descamps-Mandine, Clément Daviaud, Maelenn Menard, Ameur Hamami, Benjamin Musnier, Julien Cherfan, Axel Codault, Chanez Manseur, Marc Jeannin, David Castejón, Ingrid Fruitier-Arnaudin, Jesús Ruiz-Cabello, Hugo Groult

{"title":"Synthesis and Characterization of λ-Carrageenan Oligosaccharide-Based Nanoparticles: Applications in MRI and In Vivo Biodistribution Studies.","authors":"Manon Porta-Zapata, Susana Carregal-Romero, Jennifer Saliba, Ainhize Urkola-Arsuaga, Claudia Beatriz Miranda Perez de Alejo, Iñaki Orue, Lydia Martínez-Parra, Desirè Di Silvio, Armel Descamps-Mandine, Clément Daviaud, Maelenn Menard, Ameur Hamami, Benjamin Musnier, Julien Cherfan, Axel Codault, Chanez Manseur, Marc Jeannin, David Castejón, Ingrid Fruitier-Arnaudin, Jesús Ruiz-Cabello, Hugo Groult","doi":"10.1021/acs.biomac.4c01747","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01747","url":null,"abstract":"λ-type carrageenan (λ-CAR) polysaccharides remain overlooked in the preparation of medical nanoparticles (NP) due to their unsuitable rheological properties and undesired biological effects, although they can also offer advantageous properties. To overcome these obstacles, oligosaccharide derivatives (λ-COS) have been successfully applied to the synthesis of stable NP incorporating both, ferrite cores and divalent manganese (Mn2+) releasable ions. The acute pro-inflammatory behavior and anticoagulant activity of native λ-CAR were significantly reduced in the case of λ-COS and λ-COS NP, rendering possible their use for medical applications. In vivo MRI studies in mice showed that the λ-COS NP framework is promising for two applications. The first is partial Mn2+ release into the plasma to achieve intracellular Mn2+-based contrast of the myocardium and imaging of the hepatobiliary system. Second, it serves as a novel sugar-based coating that confers suitable pharmacokinetic properties to NP, making it promising for further targeted therapy applications.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143466405","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Enhanced Bone Targeting of Poly(l-glutamic acid)s through Cationic or Aromatic Substitution. 通过阳离子或芳香族取代增强聚（l-谷氨酸）的骨靶向性

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-02-20 DOI: 10.1021/acs.biomac.4c01714

Xiaoxiong Jin, Wanying Wang, Hui Liu, Jing Zhao, Pengfei Li, Aoting Li, Ziyuan Song

引用次数: 0

Cyclic Poly(2-methyl-2-oxazoline)-Lipid Conjugates Are Good Alternatives to Poly(ethylene glycol)-Lipids for Lipid Nanoparticle mRNA Formulation.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-02-19 DOI: 10.1021/acs.biomac.4c01587

Bianka Golba, Zifu Zhong, Matteo Romio, Ruben Almey, Dieter Deforce, Maarten Dhaenens, Niek N Sanders, Edmondo M Benetti, Bruno G De Geest

{"title":"Cyclic Poly(2-methyl-2-oxazoline)-Lipid Conjugates Are Good Alternatives to Poly(ethylene glycol)-Lipids for Lipid Nanoparticle mRNA Formulation.","authors":"Bianka Golba, Zifu Zhong, Matteo Romio, Ruben Almey, Dieter Deforce, Maarten Dhaenens, Niek N Sanders, Edmondo M Benetti, Bruno G De Geest","doi":"10.1021/acs.biomac.4c01587","DOIUrl":"10.1021/acs.biomac.4c01587","url":null,"abstract":"Lipid nanoparticles (LNPs) with ionizable cationic lipids have revolutionized RNA drug delivery, playing a key role in the success of mRNA-based therapeutics, such as COVID-19 vaccines. A vital component of these LNPs is the poly(ethylene glycol) (PEG)-lipid conjugate, which enhances colloidal stability but may trigger the production of anti-PEG antibodies, resulting in accelerated blood clearance (ABC) and diminished therapeutic efficacy. In this study, we explored poly(2-methyl-2-oxazoline) (PMOXA) as an alternative stabilizing agent for mRNA LNPs. We synthesized both cyclic and linear PMOXA, conjugated them to dialkyl lipids, and created lipid-polymer amphiphiles. We systematically evaluated how polymer topology influenced the physicochemical properties of LNPs, including in vitro cellular uptake, transfection efficiency, and protein corona formation, and directly compared these properties with those of PEG-stabilized counterparts. In vivo experiments in mice further assessed the biodistribution and protein translation efficiency of these LNPs following intravenous administration. Our results showed that cyclic PMOXA conjugates not only matched but potentially surpassed the performance of PEG-based analogues, highlighting their promise as a superior alternative in mRNA-LNP formulations.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143456266","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

Bismuth-Loaded Poly(α-amino acid) Nanoparticles for CT and Fluorescence Bimodal Imaging.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-02-19 DOI: 10.1021/acs.biomac.4c01640

Gege Peng, Guangyao Li, Fei Zhou, Tianlun Shen, Jiali Lyu, Ziyi Liu, Jun Ling, Jihong Sun

{"title":"Bismuth-Loaded Poly(α-amino acid) Nanoparticles for CT and Fluorescence Bimodal Imaging.","authors":"Gege Peng, Guangyao Li, Fei Zhou, Tianlun Shen, Jiali Lyu, Ziyi Liu, Jun Ling, Jihong Sun","doi":"10.1021/acs.biomac.4c01640","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01640","url":null,"abstract":"X-ray computed tomography (CT) offers high spatial resolution and deep tissue penetration, but its low sensitivity limits early disease diagnosis. In contrast, fluorescence imaging (FI) provides high sensitivity, suffering from poor spatial resolution and limited tissue penetration. Combining CT and FI creates a complementary imaging method. Herein, we report bismuth-loaded poly(α-amino acid) nanoparticles (abbreviated as Bi NPs including Bi@POS, Bi@POS-FITC, and Bi@POS-ICG) for CT and fluorescence bimodal imaging. Bi NPs exhibit superior X-ray attenuation and fluorescence emission properties by integrating bismuth complexes with fluorescent dyes, including fluorescein isothiocyanate (FITC) and indocyanine green (ICG). The catechol moieties in poly(α-amino acid)s not only chelate Bi3+ but also exhibit reactive oxygen and nitrogen species (RONS) scavenging activity. In vitro and in vivo experiments demonstrate that Bi NPs have superior bimodal imaging performance, significantly enhanced CT contrast, and prolonged fluorescence signals, suggesting their great potential as bimodal contrast agents for diagnosis applications.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143447438","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

Di-Tyrosine Cross-Linking of Elastin-Like Polypeptides through Ruthenium Photoreaction To Form Scaffolds: Fine Tuning Mechanical Properties and Improving Cytocompatibility.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-02-19 DOI: 10.1021/acs.biomac.4c01376

Iyeswaria K Amma, Rohan S J Ingrole, Ghanesh Kesav Venkatesa Prabhu, Raul Dominquez, Dejie Kong, Satish Chandra Hari Mangalara, Gregory B Mckenna, Harvinder Singh Gill

{"title":"Di-Tyrosine Cross-Linking of Elastin-Like Polypeptides through Ruthenium Photoreaction To Form Scaffolds: Fine Tuning Mechanical Properties and Improving Cytocompatibility.","authors":"Iyeswaria K Amma, Rohan S J Ingrole, Ghanesh Kesav Venkatesa Prabhu, Raul Dominquez, Dejie Kong, Satish Chandra Hari Mangalara, Gregory B Mckenna, Harvinder Singh Gill","doi":"10.1021/acs.biomac.4c01376","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01376","url":null,"abstract":"Ensuring that the mechanical properties of tissue engineering scaffolds align with those of the target tissues is crucial for their successful integration and functional performance. Tyrosine-tyrosine cross-links are found in nature in numerous proteins including resilin that exhibit enhanced toughness and energy storage capacity. Herein, we investigated the potential of tuning the mechanical properties of scaffolds made from elastin-like polypeptides (ELPs) containing tyrosine residues. Ruthenium-based photoreaction was used to form tyrosine cross-links. To enhance the cytocompatibility of the ELP scaffold, a continuous mode of washing was developed to remove residual ruthenium from the scaffolds. The continuous mode of washing was significantly superior in removing ruthenium and did so in a significantly shorter time as compared to batch washing and the conventional semibatch washing (also called dialysis washing). The range of storage moduli of the fabricated scaffolds spanned tens of Pa to hundreds of kPa. Human fibroblast cells were found to grow in the scaffolds and proliferate. Overall, this work offers a rationale for further developing tyrosine cross-linked ELPs for a broad range of tissue engineering applications.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143447439","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

The Biology of Natural Polymers Accelerates and Expands the Science of Biomacromolecules: A Focus on Structural Proteins.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-02-18 DOI: 10.1021/acs.biomac.4c01621

Keiji Numata

引用次数: 0

Coral-Inspired Zinc Acrylate Polymer Utilizing Coumarin as the Fluorescent Unit for Marine Antifouling.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-02-17 DOI: 10.1021/acs.biomac.4c01574

Jianwei Hou, Guobo Chen, Xinghai Hao, Jiali Xu, Geoffrey I N Waterhouse, Zhiming Zhang, Liangmin Yu

{"title":"Coral-Inspired Zinc Acrylate Polymer Utilizing Coumarin as the Fluorescent Unit for Marine Antifouling.","authors":"Jianwei Hou, Guobo Chen, Xinghai Hao, Jiali Xu, Geoffrey I N Waterhouse, Zhiming Zhang, Liangmin Yu","doi":"10.1021/acs.biomac.4c01574","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01574","url":null,"abstract":"The need for low-cost and effective antifouling solutions drives innovation in the fields of chemistry, materials science, and biology. In this work, guided by the antifouling strategies used by fluorescent corals, a series of fluorescent zinc acrylate polymer coatings containing coumarin units (ZAR-coumarin) was successfully prepared. The ZAR-coumarin coatings demonstrated excellent antifouling properties due to the synergistic action of multiple antifouling mechanisms, including fluorescent antifouling, natural bactericidal activity, and self-polishing surface renewal (due to ester group (-COO-Zn-OOC-) cleavage). Compared with zinc acrylate coatings without coumarin units (ZAR), the introduction of coumarin units significantly improved the inhibition efficiency for both bacteria and algae. In marine environment tests, the ZAR-AMCO-1, ZAR-ADMCO-1, and ZAR-CAMCO-1 coatings containing optimized amounts of different types of coumarin units maintained good antifouling properties over a 160-day field test period. This research presents an innovative approach to creating marine antifouling coatings.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143439380","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

Strategy for Making Starch-Polyphenol Complexes with Multifunctional Properties.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-02-17 DOI: 10.1021/acs.biomac.4c01596

Yujue Wang, Chen Chao, Mingyan Zhang, Cuiping Wang, Huilan Zhu, Jinglin Yu, Les Copeland, Shujun Wang

{"title":"Strategy for Making Starch-Polyphenol Complexes with Multifunctional Properties.","authors":"Yujue Wang, Chen Chao, Mingyan Zhang, Cuiping Wang, Huilan Zhu, Jinglin Yu, Les Copeland, Shujun Wang","doi":"10.1021/acs.biomac.4c01596","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01596","url":null,"abstract":"Starch-phenol complexes are of interest due to their potential for health-related functional properties in addition to resistance to enzymic digestion. However, the preparation of such complexes remains a challenge due to the structural features and low solubility of the phenols. The present study sets out a novel protocol to prepare amylose (AM)-polyphenol complexes by forming an AM-lipid complex that incorporates the polyphenol. Three polyphenols (resveratrol, curcumin, and quercetin), which by themselves do not form complexes with AM, were successfully encapsulated by AM through the addition of lauric acid (LA) to form AM-LA-polyphenol complexes. These ternary complexes had a more ordered structure and better functional properties, including antioxidant activity, slower enzymatic digestion, and controlled release of polyphenols, compared with the polyphenols alone or the AM-LA complex. Of the three polyphenols, more curcumin and quercetin were captured through interhelical rather than intrahelical associations. Our study opens up a new way to prepare starch-polyphenol complexes using polyphenols that do not form complexes with AM alone, which will be of great significance for creating novel resistant starches with desirable functionalities.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143439282","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

Development of a Pillar[6]arene Carboxylic Acid Derivative for the Extraction of a Cationic Protein.

IF 5.5 2区化学

Biomacromolecules Pub Date : 2025-02-17 DOI: 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":"https://doi.org/10.1021/acs.biomac.4c01371","url":null,"abstract":"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]CH2COOH) was prepared to extract the cationic protein cytochrome c (Cyt-c) into organic solvents. OctP[6]CH2COOH was synthesized by the condensation of ethyl 2-(4-octoxyphenoxy) acetate to obtain the pillar[6]arene derivative, followed by alkali hydrolysis. OctP[6]CH2COOH 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]CH2COOH over other cationic proteins because the complexation was a result of the inclusion of the NH3+ groups of the lysine residues by the macrocyclic molecule. Cyt-c complexed with OctP[6]CH2COOH 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.","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-02-17","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}

引用次数: 0