Yuanyuan Chen, Emma J Murphy, Zhi Cao, Ciara Buckley, Yvonne Cortese, Bor Shin Chee, Thomas Scheibel
{"title":"Electrospinning Recombinant Spider Silk Fibroin-Reinforced PLGA Membranes: A Biocompatible Scaffold for Wound Healing Applications.","authors":"Yuanyuan Chen, Emma J Murphy, Zhi Cao, Ciara Buckley, Yvonne Cortese, Bor Shin Chee, Thomas Scheibel","doi":"10.1021/acsbiomaterials.4c01605","DOIUrl":"10.1021/acsbiomaterials.4c01605","url":null,"abstract":"<p><p>Polylactide-polyglycolide (PLGA) is one of the most attractive polymeric biomaterials used to fabricate medical devices for drug delivery and tissue engineering applications. Nevertheless, the utilization of PLGA in load-bearing applications is restricted due to its inadequate mechanical properties. This study examines the potential of recombinant silk fibroin (eADF4), a readily producible biomaterial, as a reinforcing agent for PLGA. The PLGA/eADF4 composite membranes were developed by using the process of electrospinning. The spinnability of the electrospinning solutions and the physicochemical, mechanical, and thermal properties of the composite membranes were characterized. The addition of eADF4 increased the viscosity of the electrospinning solutions and enhanced both the mechanical characteristics and the thermal stability of the composites. This study demonstrates that PLGA membranes reinforced with recombinant spider silk fibroin are noncytotoxic, significantly enhance cell migration and wound closure, and do not trigger an inflammatory response, making them ideal candidates for advanced wound healing applications.</p>","PeriodicalId":8,"journal":{"name":"ACS Biomaterials Science & Engineering","volume":" ","pages":"7144-7154"},"PeriodicalIF":5.4,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142453189","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Form Equals Function: Influence of Coacervate Architecture on Drug Delivery Applications.","authors":"Chaeyoung Lim, Whitney C Blocher McTigue","doi":"10.1021/acsbiomaterials.4c01105","DOIUrl":"10.1021/acsbiomaterials.4c01105","url":null,"abstract":"<p><p>Complex coacervates, formed through electrostatic interactions between oppositely charged polymers, present a versatile platform for drug delivery, providing rapid assembly, selective encapsulation, and responsiveness to environmental stimuli. The architecture and properties of coacervates can be tuned by controlling structural and environmental design factors, which significantly impact the stability and delivery efficiency of the drugs. While environmental design factors such as salt, pH, and temperature play a crucial role in coacervate formation, structural design factors such as polymer concentration, polymer structure, mixing ratio, and chain length serve as the core framework that shapes coacervate architecture. These elements modulate the phase behavior and material properties of coacervates, allowing for a highly tunable system. In this review, we primarily analyze how these structural design factors contribute to the formation of diverse coacervate architecture, ranging from bulk coacervates to polyion complex micelles, vesicles, and cross-linked gels, though environmental design factors are considered. We then examine the effectiveness of these architectures in enhancing the delivery and efficacy of drugs across various administration routes, such as noninvasive (e.g., oral and transdermal) and invasive delivery. This review aims to provide foundational insights into the design of advanced drug delivery systems by examining how the origin and chemical structure of polymers influence coacervate architecture, which in turn defines their material properties. We then explore how the architecture can be tailored to optimize drug delivery for specific administration routes. This approach leverages the intrinsic properties derived from the coacervate architecture to enable targeted, controlled, and efficient drug release, ultimately enhancing therapeutic outcomes in precision medicine.</p>","PeriodicalId":8,"journal":{"name":"ACS Biomaterials Science & Engineering","volume":" ","pages":"6766-6789"},"PeriodicalIF":5.4,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11558567/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142453190","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Megh Prajapati, Karan Vishwanath, Lingting Huang, Marshall Colville, Heidi Reesink, Matthew Paszek, Lawrence J Bonassar
{"title":"Specific Degradation of the Mucin Domain of Lubricin in Synovial Fluid Impairs Cartilage Lubrication.","authors":"Megh Prajapati, Karan Vishwanath, Lingting Huang, Marshall Colville, Heidi Reesink, Matthew Paszek, Lawrence J Bonassar","doi":"10.1021/acsbiomaterials.4c00908","DOIUrl":"10.1021/acsbiomaterials.4c00908","url":null,"abstract":"<p><p>Progressive cartilage degradation, synovial inflammation, and joint lubrication dysfunction are key markers of osteoarthritis. The composition of synovial fluid (SF) is altered in OA, with changes to both hyaluronic acid and lubricin, the primary lubricating molecules in SF. Lubricin's distinct bottlebrush mucin domain has been speculated to contribute to its lubricating ability, but the relationship between its structure and mechanical function in SF is not well understood. Here, we demonstrate the application of a novel mucinase (StcE) to selectively degrade lubricin's mucin domain in SF to measure its impact on joint lubrication and friction. Notably, StcE effectively degraded the lubricating ability of SF in a dose-dependent manner starting at nanogram concentrations (1-3.2 ng/mL). Further, the highest StcE doses effectively degraded lubrication to levels on par with trypsin, suggesting that cleavage at the mucin domain of lubricin is sufficient to completely inhibit the lubrication mechanism of the collective protein component in SF. These findings demonstrate the value of mucin-specific experimental approaches to characterize the lubricating properties of SF and reveal key trends in joint lubrication that help us better understand cartilage function in lubrication-deficient joints.</p>","PeriodicalId":8,"journal":{"name":"ACS Biomaterials Science & Engineering","volume":" ","pages":"6915-6926"},"PeriodicalIF":5.4,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142453196","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Thermo-controlled Water Microenvironment Inducing Fluorescence Enhancement of Chalcone Nanohydrogels for Mitochondrial Temperature Sensing.","authors":"Qing-Pu Zhang, Qingqing Zhang, Yu-Ling Sun, Xin Tao, Yu-Ting Zhao, Fei Guo, Zhen-Ke Li, Zhen Wang, Zi-Hui Liang, Chang-Hai Yi","doi":"10.1021/acsbiomaterials.4c01427","DOIUrl":"10.1021/acsbiomaterials.4c01427","url":null,"abstract":"<p><p>Developing aggregation-induced emission (AIE)-based hydrogels that exhibit fluorescence enhancement as to thermal properties is an interesting and challenging task. In this work, we employed the fluorophore 2'-hydroxychalcone (HC), fluorescence properties of which are easily influenced by the excited-state intramolecular proton transfer and twisted intramolecular charge transfer (TICT) effects, to develop a novel type of temperature-sensitive polymers, hydroxychalcone-based polymers (HCPs). By controlling the temperature-dependent water microenvironments in HCPs, the intramolecular hydrogen bonds between water and HCPs can be regulated, thereby influencing the TICT process and leading to thermo-induced fluorescence enhancement, which shows a contrary tendency compared to typical AIEgens that always exhibit fluorescence attenuation as the thermal energy accelerates the molecular motion. Following the decoration with triphenylphosphine, the resulting polymer P-HCP assembled into nanohydrogels and served as a fluorescent probe for intracellular mitochondrial temperature sensing.</p>","PeriodicalId":8,"journal":{"name":"ACS Biomaterials Science & Engineering","volume":" ","pages":"7167-7175"},"PeriodicalIF":5.4,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142453198","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sepideh Azarmgin, Bahman Torabinejad, Rooja Kalantarzadeh, Heriberto Garcia, Carlo Alberto Velazquez, Gino Lopez, Marisol Vazquez, Gabriel Rosales, Behzad Shiroud Heidari, Seyed Mohammad Davachi
{"title":"Polyurethanes and Their Biomedical Applications.","authors":"Sepideh Azarmgin, Bahman Torabinejad, Rooja Kalantarzadeh, Heriberto Garcia, Carlo Alberto Velazquez, Gino Lopez, Marisol Vazquez, Gabriel Rosales, Behzad Shiroud Heidari, Seyed Mohammad Davachi","doi":"10.1021/acsbiomaterials.4c01352","DOIUrl":"10.1021/acsbiomaterials.4c01352","url":null,"abstract":"<p><p>The tunable mechanical properties of polyurethanes (PUs), due to their extensive structural diversity and biocompatibility, have made them promising materials for biomedical applications. Scientists can address PUs' issues with platelet absorption and thrombus formation owing to their modifiable surface. In recent years, PUs have been extensively utilized in biomedical applications because of their chemical stability, biocompatibility, and minimal cytotoxicity. Moreover, addressing challenges related to degradation and recycling has led to a growing focus on the development of biobased polyurethanes as a current focal point. PUs are widely implemented in cardiovascular fields and as implantable materials for internal organs due to their favorable biocompatibility and physicochemical properties. Additionally, they show great potential in bone tissue engineering as injectable grafts or implantable scaffolds. This paper reviews the synthesis methods, physicochemical properties, and degradation pathways of PUs and summarizes recent progress in applying different types of polyurethanes in various biomedical applications, from wound repair to hip replacement. Finally, we discuss the challenges and future directions for the translation of novel polyurethane materials into biomedical applications.</p>","PeriodicalId":8,"journal":{"name":"ACS Biomaterials Science & Engineering","volume":" ","pages":"6828-6859"},"PeriodicalIF":5.4,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142453195","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Mohamad Mokhtarzadegan, Saba Amini, Aida Iraji, Mehdi Kian, Cambyz Irajie, Seyyed Sajad Daneshi, Shekofeh Abbaspour, Shahrokh Zare, Akram Jamshidzadeh, Ali Feiz, Nadiar M Mussin, Nader Tanideh, Amin Tamadon
{"title":"Enhanced Mandibular Bone Repair Using Poly Lactic-<i>co</i>-glycolic Acid Combined with Nanohydroxyapatite Scaffold Loaded by Mesenchymal Stromal/Stem Cells and Curcumin in Male Rats.","authors":"Mohamad Mokhtarzadegan, Saba Amini, Aida Iraji, Mehdi Kian, Cambyz Irajie, Seyyed Sajad Daneshi, Shekofeh Abbaspour, Shahrokh Zare, Akram Jamshidzadeh, Ali Feiz, Nadiar M Mussin, Nader Tanideh, Amin Tamadon","doi":"10.1021/acsbiomaterials.4c00608","DOIUrl":"10.1021/acsbiomaterials.4c00608","url":null,"abstract":"<p><p>This study aimed to investigate the healing effect of a polylactic-<i>co</i>-glycolic acid (PLGA) scaffold containing nanohydroxyapatite (NHA) along with curcumin (CCM), loaded with adipose-derived mesenchymal stem cells (AD-MSCs), on mandibular bone defects. The designed PLGA scaffolds containing NHA were evaluated for their mechanical and structural properties. Forty rats were divided into five groups (<i>n</i> = 8) based on the treatment: Sham, PLGA scaffolds containing NHA, PLGA scaffolds containing NHA + CCM, PLGA scaffolds containing NHA + AD-MSCs, and PLGA scaffolds containing NHA + CCM + AD-MSCs. After 8 weeks' follow-up, mandible bones were isolated for histomorphometry evaluation. Data were analyzed using SPSS version 21, with <i>p</i>-values <0.05 considered statistically significant. SEM evaluation showed that the designed nanocomposite scaffold had 80% porosity. Histomorphometry results indicated a significant difference in osteocyte, osteoblast, bone area, and vascular area parameters in the group treated with scaffolds loaded with AD-MSCs + CCM compared to the other groups (<i>p</i> < 0.05). The PLGA-containing NHA-CCM nanocomposite scaffold demonstrated good porosity and dispersion, suitable for treating bone defects. Rats treated with scaffolds containing AD-MSCs and CCM showed better therapeutic results than the other groups. Further research is needed to evaluate its anti-inflammatory, antioxidant properties, osteogenesis, and therapeutic effects in larger animal models.</p>","PeriodicalId":8,"journal":{"name":"ACS Biomaterials Science & Engineering","volume":" ","pages":"7043-7053"},"PeriodicalIF":5.4,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142520293","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Quantum Insights into Partially Molecular Imprinted Microspheres for Anticancer Therapeutics: Experimental and Theoretical Studies.","authors":"Sreejith Thrivikraman Nair, Vishnu Vr, Kaladhar Kamalasanan, Aneesh Thankappan Presanna","doi":"10.1021/acsbiomaterials.4c01249","DOIUrl":"10.1021/acsbiomaterials.4c01249","url":null,"abstract":"<p><p>Drug solubility is a determining factor for controlled release, and solubility-dependent release kinetics can be modified by changing the drug's state in the polymer matrix through partial molecular imprinting (PMI), although research in this area remains limited. This novel PMI approach creates nanocavities within the polymer by partially retaining the imprinting molecule and trapping the drug. Such a method holds promise for developing advanced biomaterial-based drug delivery systems for anticancer therapies. In this study, we developed microspheres designed for anticancer drug delivery utilizing PMI to enhance controlled release properties. Poly(vinyl alcohol) (PVA) microspheres were partially imprinted with aspirin (ASP) to create nanocavities for gemcitabine (GEM) molecules, inducing a polymorphic shift of GEM within the polymer matrix. This novel PMI approach enhanced drug release properties by enabling control over the drug crystallinity and release rate. The PVA-ASP-GEM complex showed zero-order release kinetics, releasing 21.6% of GEM over 48 h, maintaining steady state release profile. In contrast, nonimprinted PVA-GEM microspheres exhibited first-order kinetics with a faster release of 46.85% in the same period. Quantum insights from density functional theory (DFT) calculations revealed the superior stability of the PVA-ASP-GEM complex, with a binding free energy of -56.03 kcal/mol, compared to -29.07 kcal/mol for PVA-GEM. Molecular dynamics (MD) simulations demonstrated that ASP's presence created nanocavities that restricted GEM's movement, further contributing to the controlled release. Experimental validation through differential scanning calorimetry (DSC), thermogravimetric analysis (TGA), X-ray diffraction (XRD), and Raman spectroscopy confirmed the polymorphic transitions within the PVA-ASP-GEM complex. This PMI-based approach offers a promising method for modulating drug release kinetics and improving the stability of anticancer therapeutics, paving the way for innovative biomaterial-based drug delivery systems.</p>","PeriodicalId":8,"journal":{"name":"ACS Biomaterials Science & Engineering","volume":" ","pages":"7005-7017"},"PeriodicalIF":5.4,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142370164","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Weiye Du, Yunping Yang, Jinkun Liu, Yan Zhu, Tao Shen, Qinghua Chen, Toshiki Miyazaki
{"title":"In Situ Synthesis and Characterizations of a Strontium-Substituted Dicalcium Phosphate Anhydrous/Hydroxyapatite Biphasic Whisker and Its Properties Evaluation.","authors":"Weiye Du, Yunping Yang, Jinkun Liu, Yan Zhu, Tao Shen, Qinghua Chen, Toshiki Miyazaki","doi":"10.1021/acsbiomaterials.4c00306","DOIUrl":"10.1021/acsbiomaterials.4c00306","url":null,"abstract":"<p><p>Dicalcium phosphate anhydrous (DCPA) presents good biomineralization ability, the strontium element is known for superior bone affinity, and a whisker possesses good mechanical strength; all these are beneficial for improving the drawbacks of hydroxyapatite (HAP) like weaker mechanical properties, poor biomineralization, and slower degradation/absorption. Therefore, a homogeneous precipitation was adopted to synthesize Sr-substituted and DCPA and HAP coexisting whiskers. The composition, structure, and morphology based on urea dosage and substitution content were characterized, and the roles of DCPA, Sr, and whisker shape were investigated. It turned out that Sr-DCPA/HAP biphasic products contained about 19% DCPA and 81% HAP, and both phases occupied the outer and inner parts of the whisker, respectively. Increasing the urea dosage made the morphology transform from a sea urchin shape to fiber clusters and then whiskers, while Sr substitution brought the whisker back to the porous microsphere shape. Only 5% of Sr content and 15 g of urea could maintain the whisker shape. Sr could promote the proliferation of MC3T3-E1 cells even at a higher extract concentration of 10 mg/mL. The cells stayed in a healthy state whether cocultured with the whisker or the microsphere. The unstable DCPA combined with the decreased crystallinity brought by Sr doping contributed to shortening the apatite deposition period to within 7 days. The whisker morphology enhanced the compressive strength of acrylic resin, and the apatite layer helped to reduce the strength loss during soaking. The Sr-DCPA/HAP biphasic whisker with enhanced overall properties possessed more promising potential for biomedical application.</p>","PeriodicalId":8,"journal":{"name":"ACS Biomaterials Science & Engineering","volume":" ","pages":"6874-6886"},"PeriodicalIF":5.4,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142379389","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}