BiomacromoleculesPub Date : 2025-06-21DOI: 10.1021/acs.biomac.5c00305
Lang Xiao, Mingzhu Ye, Yirui Fan, Guangyu Liu, Huixia He, Jianxi Xiao
{"title":"Dual-Cross-linked Methylacrylated Collagen-DPPA Bioinks for Precision DLP Bioprinting and Accelerated Skin Wound Healing.","authors":"Lang Xiao, Mingzhu Ye, Yirui Fan, Guangyu Liu, Huixia He, Jianxi Xiao","doi":"10.1021/acs.biomac.5c00305","DOIUrl":"10.1021/acs.biomac.5c00305","url":null,"abstract":"<p><p>Digital light processing (DLP) bioprinting, known for its speed and precision, has become a key tool in disease modeling and regenerative medicine. Yet, creating bioinks with optimal printability, bioactivity, and cell-supporting capacity remains a major challenge. Here, we introduce a novel dual-network collagen-based bioink, methyl acrylated collagen-dimethylphenylphosphonate (CMA-DPPA), which enables the fabrication of mechanically robust and highly printable cell-laden constructs through DLP 3D bioprinting. The CMA-DPPA hydrogel is synthesized by cross-linking collagen with DPPA, followed by photo-crosslinking with CMA; this dual-cross-linking approach markedly improves printing fidelity, mechanical strength, and enzymatic degradation resistance of the 3D-printed constructs. The CMA-DPPA hydrogel exhibits excellent biocompatibility, effectively promoting cell adhesion, proliferation, and migration. In a rat model of full-thickness skin defects, CMA-DPPA hydrogel facilitated organized collagen fiber deposition and accelerated epidermal regeneration, thereby expediting wound closure. CMA-DPPA bioink enables precise, robust scaffold fabrication, showing great promise for DLP-based tissue engineering and regenerative medicine.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-06-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144339691","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}
BiomacromoleculesPub Date : 2025-06-20DOI: 10.1021/acs.biomac.5c00594
Sameen Yousaf, Bahareh Amirloo, Harmesh S Aojula, David J Clarke, Alberto Saiani, Andrew Irwin, Elena V Bichenkova
{"title":"Hydrogel \"Affinity Trap\" for microRNAs with a Self-Assembling Fluorescent \"Split-Probe\" to Monitor Their Expression and Degradation.","authors":"Sameen Yousaf, Bahareh Amirloo, Harmesh S Aojula, David J Clarke, Alberto Saiani, Andrew Irwin, Elena V Bichenkova","doi":"10.1021/acs.biomac.5c00594","DOIUrl":"10.1021/acs.biomac.5c00594","url":null,"abstract":"<p><p>The hydrogel \"affinity trap\" engineered here from peptides and nucleic acids into dynamic supramolecular structures offered the opportunity to measure physiological concentrations of tissue-specific microRNA expression and degradation, which are symptomatic for diseased cells and tissues. Hydrogel size-discriminating properties allowed to segregate microRNAs from complex biological media into a hydrogel matrix and entrap the target sequence via hybridization with a hydrogel-immobilized \"capture\" probe, where it could be detected through fluorescence quenching. We demonstrated the size-selective permeability of the hydrogel that provided a protective microenvironment for microRNAs and detection probes from cellular biological interference and afforded selective self-assembly and detection of oncogenic microRNA-21 (miR-21) in the presence of cell extracts, which is otherwise detrimental for detection in a gel-free solution. We were also able to monitor the degradation of unlabeled miR-21 by natural (RNase A and H) and synthetic (miR-21-RNase) ribonucleases and their synergistic actions, which could be potentially useful in the therapeutic knockdown of pathogenic RNAs.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144332055","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}
BiomacromoleculesPub Date : 2025-06-20DOI: 10.1021/acs.biomac.5c00539
Danni Li, Aiyu Li, Lu Zhang, Yunfei Huang, Rui Guo, Xiangyang Shi, Xueyan Cao
{"title":"Biomimetic Chitosan Nanogels Codeliver Drug/Small Activating RNA for Metastasis-Inhibited Necroptosis Therapy of Ovarian Cancer.","authors":"Danni Li, Aiyu Li, Lu Zhang, Yunfei Huang, Rui Guo, Xiangyang Shi, Xueyan Cao","doi":"10.1021/acs.biomac.5c00539","DOIUrl":"10.1021/acs.biomac.5c00539","url":null,"abstract":"<p><p>Ovarian cancer remains the leading cause of gynecologic malignancy-related deaths. Developing novel nanoplatforms to overcome the low efficacy of chemotherapy and advanced metastasis in ovarian cancer is crucial. Here, we report biomimetic chitosan nanogels (CH NGs) designed to codeliver gambogic acid (GA) and MAS1 small activating RNA (saMAS1). The formed CH NGs/GA/saMAS1 camouflaged with ovarian cancer cell membranes (CM) can release GA in a pH-responsive manner, target cancer cells, and induce the killing effects through GA-mediated necroptosis. Meanwhile, saMAS1 upregulates MAS1 expression, counteracting the activation of angiotensin II receptor type 1 (AGTR1) and thereby inhibiting the renin-angiotensin system (RAS) signaling pathway, subsequently impeding metastasis. The therapeutic efficacy of CH NGs/GA/saMAS1@CM NGs regarding primary tumor killing and metastasis inhibition was further confirmed using ovarian mouse models. These biocompatible CH NGs represent a promising advanced nanomedicine formulation to tackle ovarian cancer through metastasis-inhibited necroptosis following the codelivery of GA and saMAS1.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144332054","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}
BiomacromoleculesPub Date : 2025-06-19DOI: 10.1021/acs.biomac.4c01712
Gaia Pascolo, Bekzod Bekchanov, Mohamed A N Soliman, Eugenia Spessot, Hafiz Ali, Omar Qutachi, Meisam Abdi, Annalisa Tirella, Mohamed A Elsawy
{"title":"Microfluidics Enabling the Controlled Manufacturing of Peptide and Protein Micro and Nano Biomaterials for Biomedical Applications.","authors":"Gaia Pascolo, Bekzod Bekchanov, Mohamed A N Soliman, Eugenia Spessot, Hafiz Ali, Omar Qutachi, Meisam Abdi, Annalisa Tirella, Mohamed A Elsawy","doi":"10.1021/acs.biomac.4c01712","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01712","url":null,"abstract":"<p><p>The intersection of microfluidics (MFs) and biomaterials has opened new avenues for the precise fabrication of micro- and nanostructures with tailored properties. Peptides and proteins are among these biomaterials recently gaining significant attention, offering unique advantages due to their biocompatibility, biodegradability, assembly into biofunctional structures, and potential for targeted interactions. This Review provides a comprehensive overview of advancements in manufacturing of peptide- and protein-based micro- and nanomaterials (PPMNs) using MFs and identifies gaps in current knowledge. We discussed key aspects of MFs systems relevant to the fabrication of micro- and nanostructures, including microchip design and material, as well as manufacturing parameters. By understanding these factors, researchers can optimize MFs systems to precisely tune the size, shape, and composition of the fabricated PPMNs, and get insights into future research directions and address current limitations. Digital approaches and standardization of MFs will accelerate translation of PPMNs for different biomedical applications.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144323843","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}
BiomacromoleculesPub Date : 2025-06-18DOI: 10.1021/acs.biomac.5c00459
Jirayu Boonyakida, Mami Matsuda, Ryosuke Suzuki, Krishna Raja Muthuraman, Enoch Y Park
{"title":"Virus-Like Particle-Based Multiserotype Quartet Vaccine of Dengue Envelope Protein Domain III Elicited Potent Anti-Dengue Responses.","authors":"Jirayu Boonyakida, Mami Matsuda, Ryosuke Suzuki, Krishna Raja Muthuraman, Enoch Y Park","doi":"10.1021/acs.biomac.5c00459","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00459","url":null,"abstract":"<p><p>In this study, we presented two strategies for designing an envelope domain III (EDIII)-based tetravalent dengue virus (DENV) vaccine. The first approach was conjugation of the EDIIIs from all four DENV serotypes to a norovirus-like particle (NoV-LP) scaffold, yielding the NoV::tetEDIII vaccine. The second approach linked the EDIIIs of all four serotypes into a single polypeptide chain, which was also conjugated to the NoV-LP scaffold by using the SpyTag/SpyCatcher system, creating the NoV::quartetEDIII vaccine. These tetravalent DENV vaccines were evaluated for their immunogenicity against all DENV serotypes. Both vaccines elicited strong antibody responses against all serotypes in a prime-and-boost immunization regimen. Furthermore, the single-round infectious particle (SRIP) assay demonstrated that these antibodies had neutralizing capabilities superior to those of traditional subunit vaccines. Our study proposes a promising DENV vaccine strategy that may protect against all four serotypes, potentially promoting public health efforts to prevent and control dengue disease.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144323844","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}
{"title":"Strategic Design of Biocompatible, Glistening-Free, and Foldable Artificial Intraocular Lenses Based on Hydro-Amphiphilic Ternary Copolymers.","authors":"Cheng-Ti Hu, Zhi-Xuan Liang, Jhen-Yu Luo, Po-Hsun Chiu, Annabelle I Day, Chih-Chen Hsieh, Po-Jen Shih, Jia-Han Li, Bo-I Kuo, I-Jong Wang, Jia-Yush Yen, Chi-An Dai","doi":"10.1021/acs.biomac.5c00588","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00588","url":null,"abstract":"<p><p>The increasing prevalence of cataracts underscores the urgent need for intraocular lens (IOL) materials that provide optical clarity, foldability, glistening resistance, and long-term biocompatibility. In this study, we developed hydro-amphiphilic ternary copolymers composed of styrene, hydroxyethyl methacrylate (HEMA), and poly(ethylene glycol) phenyl ether acrylate (PEGPEA) to address these requirements. This rational design integrates the strength and refractive index of hydrophobic styrene with the flexibility and hydrophilicity of HEMA and PEGPEA. The optimized formulation (H3), comprising 50 wt % HEMA, 30 wt % PEGPEA, and 20 wt % styrene, showed excellent transparency after accelerated aging, sufficient modulus and elongation for safe surgical handling, and low cytotoxicity in CCK-8 assays. Cytokine analyses revealed no significant inflammatory response compared to a commercial hydrophobic acrylic IOL. These findings highlight hydro-amphiphilic copolymers as a promising next-generation material platform for IOLs, offering a biocompatible, glistening-free, and foldable solution for enhanced surgical outcomes and long-term patient satisfaction.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144315476","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}
BiomacromoleculesPub Date : 2025-06-16DOI: 10.1021/acs.biomac.5c00289
Sikai Chen, Peng Lin, Jinglin Yuan, Miao Lv, Han Zhang
{"title":"Toward Renewable Water Treatments: Efficient and Sustainable Cationic Cellulose Nanofiber Flocculants Derived from Rice Straw.","authors":"Sikai Chen, Peng Lin, Jinglin Yuan, Miao Lv, Han Zhang","doi":"10.1021/acs.biomac.5c00289","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00289","url":null,"abstract":"<p><p>Flocculants are essential for removing pollutants from wastewater, yet conventional organic and inorganic types often lack renewability and pose risks of secondary pollution. In this study, a cationic cellulose nanofiber (CCNF) flocculant was developed from rice straw, offering enhanced flocculation performance, sustainability, and environmental compatibility. The cellulose nanofiber was extracted and cationically modified under mild conditions. Optimized modification enhanced cationic substitution, yielding a maximum SS removal of 98.9%. CCNF maintained stable performance under both acidic and alkaline conditions and was particularly effective in removing nanoscale SS and treating actual agricultural wastewater. Moreover, cationic modification did not significantly alter the biodegradability of cellulose, with CCNF showing a weight loss similar to that of unmodified CNF after 180 days in soil. The estimated cost of CCNF-3 was approximately 1.13 yuan/g, slightly higher than conventional flocculants, but with considerable environmental benefits.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-06-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144309251","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}
{"title":"Dielectric Properties of Wood-Derived Cellulose Nanofiber Films in 10-40 GHz Band.","authors":"Shennan Wang, Kazuho Daicho, Yoshinori Doi, Marco Beaumont, Tsuguyuki Saito, Junichiro Shiomi","doi":"10.1021/acs.biomac.5c00308","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00308","url":null,"abstract":"<p><p>Wood-derived cellulose nanofiber (CNF) offers excellent electrical insulation, mechanical strength, flexibility, thermal stability, and low thermal expansion, meeting the growing demand for sustainable materials in electronic devices. However, the dielectric properties of CNF-based material crucial for beyond-fifth-generation (B5G) applications at frequencies above 10 GHz remain underexplored. This study investigates dielectric behaviors of CNF films with varying surface functional groups and porosities over 10-40 GHz under controlled humidity. Carboxylated CNF films exhibited distinct dielectric characteristics compared to noncarboxylated CNFs, with moisture sensitivity significantly reduced by substituting proton counterions with hydrophobic tetra-<i>n</i>-butylammonium. Increased porosity led to linear decrease in relative permittivity but increase in loss tangent. The intrinsic permittivity of CNFs also decreased with larger Scherrer crystal size. These findings demonstrate that controlling interfacial polarization and interfibrillar interactions effectively lowers the dielectric response of CNF films, highlighting their potential in B5G and high-frequency electronic applications.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-06-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144309250","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}
BiomacromoleculesPub Date : 2025-06-15DOI: 10.1021/acs.biomac.5c00117
Dmitrii Iudin, Léon J J A Gerridzen, Paulina N Bernal, Carl C L Schuurmans, Myriam Neumann, Lam Nguyen, Mies J van Steenbergen, Jaimie Hak, Wanlu Li, Cristina Casadidio, Anne Metje van Genderen, Rosalinde Masereeuw, Riccardo Levato, Yu Shrike Zhang, Bas G P van Ravensteijn, Tina Vermonden
{"title":"In-Depth Investigation of Electrostatic Interaction-Based Hydrogel Shrinking for Volumetric Printing and Tissue Engineering Applications.","authors":"Dmitrii Iudin, Léon J J A Gerridzen, Paulina N Bernal, Carl C L Schuurmans, Myriam Neumann, Lam Nguyen, Mies J van Steenbergen, Jaimie Hak, Wanlu Li, Cristina Casadidio, Anne Metje van Genderen, Rosalinde Masereeuw, Riccardo Levato, Yu Shrike Zhang, Bas G P van Ravensteijn, Tina Vermonden","doi":"10.1021/acs.biomac.5c00117","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00117","url":null,"abstract":"<p><p>Three-dimensional printing of hydrogels enables the fabrication of complex structures for tissue engineering. Postprinting shrinking via electrostatic interactions offers a promising strategy to better replicate the size and intricacy of native tissues. This study explores hyaluronic acid (HA)-based hydrogels that undergo shrinking upon polycation penetration and complexation focusing on the influence of the HA macromer concentration, molecular weight, cross-linking density, hydrogel initial volume, and polycation properties on shrinking efficiency. To support cell adhesion, RGD peptides were incorporated into the HA network. The polycation concentration strongly affected cell viability: a high concentration of 1 wt % resulted in reduced viability, while 0.1 wt % preserved it with effective shrinkage. Volumetrically printed structures were reduced up to 9 times in volume, achieving features as small as 42 ± 6 μm. This shrinking approach enables the fabrication of hydrogel structures with significantly reduced dimensions, making it a powerful tool for developing high-precision hydrogel structures for tissue engineering.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-06-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144300689","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}
BiomacromoleculesPub Date : 2025-06-13DOI: 10.1021/acs.biomac.5c00360
Golam Mustafa, Sajad Shiekh, Janan Alfehaid, Sineth G Kodikara, Hamza Balci
{"title":"Impact of Molecular Crowding on Accessibility of Telomeric Overhangs Forming Multiple G-Quadruplexes.","authors":"Golam Mustafa, Sajad Shiekh, Janan Alfehaid, Sineth G Kodikara, Hamza Balci","doi":"10.1021/acs.biomac.5c00360","DOIUrl":"10.1021/acs.biomac.5c00360","url":null,"abstract":"<p><p>Molecular crowding─a defining feature of the cellular environment─affects folding kinetics, conformation, and stability of G-quadruplex (GQ) structures. However, its influence on the overall architecture and accessibility of telomeric overhangs containing multiple GQs remains largely unexplored. In this study, we employed single-molecule FRET and FRET-PAINT to address this question. We examined the accessibility of telomeric overhangs, capable of forming 1-6 GQs, to a short complementary peptide nucleic acid (PNA) imager probe in the presence of 200 and 6000 Da polyethylene glycol (PEG) molecules (PEG-200 and PEG-6000). We observed a progressive compaction and architectural condensation of the overhang as PEG concentration increased. At 30% concentration, this compaction was accompanied by approximately 3-fold and 8-fold reduction in probe accessibility in PEG-200 and PEG-6000, respectively. These findings offer new insights into how the crowded cellular environment may compact telomeric overhangs and modulate their structural and functional properties.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-06-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144289315","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}