{"title":"Identification and Characterization of the Starch Granule-Associated Proteins of Cereal Starches after Alkali Treatment","authors":"Zekun Xu, , , Zhiqian Wu, , , Xinyu Zhang, , , Mengting Ma, , , Zhongquan Sui*, , and , Harold Corke, ","doi":"10.1021/acs.biomac.5c01158","DOIUrl":"10.1021/acs.biomac.5c01158","url":null,"abstract":"<p >Starch granule-associated proteins (SGAPs) of four cereal starches subjected to different alkali treatments were investigated. Starch synthesis-related proteins were identified as the major SGAPs in normal and waxy maize starches. In rice starch, seed storage proteins were the majority of SGAPs. A concentric ring pattern of the SGAPs distribution was found in normal maize starch and normal rice starch, related to the granule-bound starch synthases. SGAPs of waxy maize starch mainly occur in starch channels, identified as starch synthases and starch branching enzymes. Alkali treatment decreased SGAPs by facilitating protein solubility and degrading the protein structure. Hydrothermal treatment promoted the effect of the alkali. After alkali treatment, the proportion of starch synthesis-related proteins in total SGAPs significantly increased, indicating that these were more resistant to alkali, as they were tightly bound to starch granules. This study revealed the heterogeneity of SGAPs in starch granules and their response to the alkaline treatment.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 10","pages":"6843–6853"},"PeriodicalIF":5.4,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145147085","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":"Glucose/Glucuronate Copolymers Stripped from Oxidized Cell Wall Cellulose by Mechanical Shearing","authors":"Takumi Haruno, , , Yoshinori Doi, , , Tomoki Ito, , , Kazuho Daicho, , , Ryosuke Kusumi, , , Hiroyuki Watanabe, , , Shuji Fujisawa, , and , Tsuguyuki Saito*, ","doi":"10.1021/acs.biomac.5c01254","DOIUrl":"10.1021/acs.biomac.5c01254","url":null,"abstract":"<p >Alternating copolymers often exhibit specific physical properties, such as a narrow glass transition temperature range and a highly uniform micelle size. Alternating copolymers are, however, synthesized from only limited combinations of monomers. Herein, we report the semisynthesis of copolymers with a basic skeleton composed of alternating glucose (G)/glucuronate (U) units via the regioselective surface oxidation of plant cellulose crystallites, followed by mechanical shearing of the oxidized crystallites in water. The molecular weights and yields of the resulting G/U copolymers exhibited variation depending on the degree of oxidation (DO) of the crystallites and the conditions of mechanical shearing, with the values ranging from approximately 8000–15000 g/mol and 4–31%, respectively. Interestingly, the molecular chain length distributions of the G/U copolymers were in good agreement with the length distributions of the dent defects formed on the crystallite surfaces. These results show that the oxidized surface molecules of the crystallites were stripped during the mechanical shearing process to yield the G/U copolymers, and these parts of the surfaces were identified as crystallite defects. We demonstrate that novel biobased alternating copolymers are produced via the chemical functionalization of plant cellulose crystallites utilizing the 2-fold helix structure of the surface molecules as a template.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 10","pages":"6940–6947"},"PeriodicalIF":5.4,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.biomac.5c01254","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145147096","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
BiomacromoleculesPub Date : 2025-09-26DOI: 10.1021/acs.biomac.5c01188
Jeffrey E. Thompson, , , Isabela T. Coutinho, , , Nicholas F. Pietra, , , Louis A. Madsen, , , Robert B. Moore, , and , Kevin J. Edgar*,
{"title":"Well-Defined Amylose Acetate-graft-polylactide Graft Polymers as Compatibilizers for Renewable Polymer Blends","authors":"Jeffrey E. Thompson, , , Isabela T. Coutinho, , , Nicholas F. Pietra, , , Louis A. Madsen, , , Robert B. Moore, , and , Kevin J. Edgar*, ","doi":"10.1021/acs.biomac.5c01188","DOIUrl":"10.1021/acs.biomac.5c01188","url":null,"abstract":"<p >Regioselectively substituted amylose acetate-<i>graft</i>-polylactide (AmAc-<i>g</i>-PLA) graft polymers were synthesized via grafting-to “click” reaction between C6-azide functionalized AmAc and alkyne-terminated PLA. Alkyne-terminated PLA synthesized through organocatalytic ring-opening polymerization (ROP) permitted control over graft degree of polymerization (DP) and stereochemistry, while azide functionalized AmAc with tailorable C6-azide degree of substitution (DS) allowed graft density control. This describes the first synthesis of polysaccharide-based graft polymers with exclusive C6 grafting and controllable topology. Thermal analysis indicates that glass transition temperatures (<i>T</i><sub>g</sub>) of AmAc and PLA segments are affected after grafting-to coupling, with poly(<span>l</span>-lactide) (PLLA) grafts maintaining crystallizability. AmAc-<i>graft</i>-poly(<span>d</span>,<span>l</span>-lactide) (PDLLA) graft polymers were effective compatibilizers for immiscible blends of starch acetate (StAc) and PDLLA as evidenced by small-angle laser light scattering (SALLS) and phase contrast optical microscopy (PCOM). This method permits the determination of structure–property relationships with regard to the effect of graft polymer topology on blend compatibilization, which will be invaluable in designing compatibilized biobased polymer blends as sustainable materials.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 10","pages":"6893–6905"},"PeriodicalIF":5.4,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acs.biomac.5c01188","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145147140","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Simultaneous Removal of Endotoxin and Circulating Histones by Heparin-Grafted Chitosan-Cellulose Composite Microspheres for Multitargeted Hemoperfusion in Septic Blood","authors":"Yu Cheng, , , Yu Chen, , , Tao Song, , , Luojia Jiang, , , Yuhan He, , , Yupei Li*, , , Weifeng Zhao, , and , Baihai Su*, ","doi":"10.1021/acs.biomac.5c01085","DOIUrl":"10.1021/acs.biomac.5c01085","url":null,"abstract":"<p >Endotoxin and circulating histones form a pathogenic loop, driving immune dysregulation in sepsis. A multitargeted extracorporeal blood purification combining endotoxin adsorption with histone neutralization may represent a critical therapeutic approach to improve the clinical outcomes of septic patients. However, existing hemoperfusion adsorbents are often heparin-dependent and single-target and exhibit limited hemocompatibility. Herein, we developed self-anticoagulant heparin-grafted chitosan/cellulose composite microspheres (CSCEHEP) for the simultaneous adsorption of endotoxin and circulating histones. The obtained CSCEHEP microspheres significantly prolonged plasma coagulation time while maintaining excellent hemocompatibility, owing to the heparin coating. In vitro, CSCEHEP microspheres exhibited adsorption capacities of 251.0 EU/g (81.8% clearance) for endotoxin and 288.6 μg/g (62.8% clearance) for histones, respectively. Meanwhile, CSCEHEP microspheres effectively adsorbed histones in whole blood and counteracted histone-induced endothelial and kidney epithelial cytotoxicity, erythrocyte fragility, and thrombocytopenia. In conclusion, CSCEHEP microspheres are promising adsorbents for hemoperfusion to simultaneously remove endotoxins and circulating histones in septic blood.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 10","pages":"6787–6801"},"PeriodicalIF":5.4,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145147207","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 : 2025-09-25DOI: 10.1021/acs.biomac.5c01458
Erfan Dinjoo, , , Michaël W. Kulka, , , Peyman Malek Mohammadi Nouri, , , Iren Constantinescu, , , Haifeng Ji, , , Arshdeep Gill, , and , Jayachandran N. Kizhakkedathu*,
{"title":"A-BioHPG: A Hydrophilic Biodegradable and Hemocompatible Hyperbranched/Dendritic Polyketal Polyglycerol with Tunable Degradation","authors":"Erfan Dinjoo, , , Michaël W. Kulka, , , Peyman Malek Mohammadi Nouri, , , Iren Constantinescu, , , Haifeng Ji, , , Arshdeep Gill, , and , Jayachandran N. Kizhakkedathu*, ","doi":"10.1021/acs.biomac.5c01458","DOIUrl":"10.1021/acs.biomac.5c01458","url":null,"abstract":"<p >We report the design and synthesis of a biodegradable hyperbranched polyether polyketal polyol, containing acid-labile ketal groups with controlled degradation, high water solubility, excellent hemocompatibility, and cell compatibility. For this, we have developed a new AB<sub>2</sub>-type acid-labile monomer, 2-((4-(2-(oxiran-2-ylmethoxy) ethoxy)tetrahydro-2H-pyran-4-yl)oxy)ethan-1-ol (OTPE). The OTPE monomer is copolymerized with glycidol through anionic ring-opening multibranching polymerization generating OTPE-incorporated hyperbranched polyglycerol (A-BioHPG) with varying degradable monomer content. Gel permeation chromatography assisted degradation studies indicated polymer stability at physiological pH, while controlled degradation is observed under acidic pH, and the data support the homogeneous distribution of the OTPE monomer throughout the polymer. The hemocompatibility of A-BioHPG is assessed by blood coagulation, platelet activation, red blood cell lysis and aggregation, and cell compatibility with endothelial cells. Our findings show that A-BioHPG is a promising candidate for use in multitude of biomedical applications, including but not limited to solubility enhancement, drug delivery, tissue engineering, and bioconjugation.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 10","pages":"7108–7124"},"PeriodicalIF":5.4,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145147079","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 : 2025-09-25DOI: 10.1021/acs.biomac.5c00948
Sisi Ma, , , Yingbo Zhang, , , Linlin Du, , , Mingwen Wang, , , Wenying Shi*, , and , Hongbin Li,
{"title":"Coral-Inspired Polyrotaxane Dynamic Antifouling Membrane Simultaneously Enhances Flux and Antifouling Performance","authors":"Sisi Ma, , , Yingbo Zhang, , , Linlin Du, , , Mingwen Wang, , , Wenying Shi*, , and , Hongbin Li, ","doi":"10.1021/acs.biomac.5c00948","DOIUrl":"10.1021/acs.biomac.5c00948","url":null,"abstract":"<p >Inspired by soft coral’s self-cleaning properties, a polyrotaxane-based membrane (EVOH-PR) with sliding α-cyclodextrin rings was designed to enhance flux and antifouling performance. The sliding-ring structure, synthesized via click chemistry, mimics coral’s dynamic motion to induce hydration layers and steric hindrance. Molecular dynamics simulations confirmed the dynamic behavior of PR and the dynamic antifouling mechanism. The EVOH-PR membrane achieved a high flux recovery rate (95.1%), low flux decline rate (7.54%), and maximum flux (720 L/(m<sup>2</sup>·h)). Stability tests showed unchanged hydrophilicity and separation efficiency after multiple cycles. Synergy between movable rings, hydration layers, and steric hindrance enabled dynamic antifouling. This work provides a proactive dynamic antifouling strategy through coral-inspired molecular motion.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 10","pages":"6684–6701"},"PeriodicalIF":5.4,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145147112","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":"Phosphorus–Nitrogen Synergistic Flame-Retardant Cellulose Nanofibers from a Reactive Ternary Deep Eutectic Solvent Containing Guanidine Phosphate","authors":"Yutong Zhang, , , Lebin Zhao, , , Yun Liu, , , Xujuan Huang, , , Kaitao Zhang*, , and , Henrikki Liimatainen*, ","doi":"10.1021/acs.biomac.5c01396","DOIUrl":"10.1021/acs.biomac.5c01396","url":null,"abstract":"<p >Phosphorylation is considered one of the most effective strategies for enhancing the flame retardancy of cellulose materials. Herein, a pretreatment based on a reactive deep eutectic solvent (RDES) containing guanidine phosphate was developed and used for facilitating cellulose nanofibrillation and synthesizing phosphorylated cellulose nanofibers (P-CNFs) with superior phosphorus–nitrogen synergistic flame-retardancy properties and extremely small average diameter (≈3 nm), eliminating external flame retardants. Compared with unmodified softwood pulp, the peak heat release rate (PHRR) and total heat release (THR) of P-CNFs were reduced by 87.2% and 75.3%, respectively. Moreover, the limiting oxygen index (LOI) of P-CNFs increased to 62.7%. The fabricated P–CNF films exhibited remarkable self-extinguishing behavior and demonstrated outstanding mechanical properties, (maximum tensile strength >188 MPa) and exceptional optical transparency (visible light transmittance >90%). This study presents an innovative and efficient strategy for the development of ecofriendly and flame-retardant nanocellulose materials with enhanced mechanical properties, demonstrating significant potential for fire-safe flexible electronics and transparent coatings.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 10","pages":"7085–7096"},"PeriodicalIF":5.4,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145147202","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":"Sodium Alginate-Based Frost-Resistant and Antidry Conductive Hydrogel for Human Motion Monitoring and Human–Computer Interaction","authors":"Xiaomin Zhang*, , , Zhuoya Zhang, , , Weilei Tang, , , Yuanfeng Ye*, , , Xiaoli Yang*, , , Guangshui Li, , , Mei Chen, , , Xinyan Zhang, , and , Guozhao Ning, ","doi":"10.1021/acs.biomac.5c01503","DOIUrl":"10.1021/acs.biomac.5c01503","url":null,"abstract":"<p >Wearable devices characterized by their flexibility are garnering significant interest, particularly in light of the emergence of notable conductive hydrogels. Although many of these hydrogels are highly conductive, they often lack adhesion. The ideal hydrogel should possess superior adhesive properties and a wide range of responsiveness. This study introduces a distinctive interpenetrating network conductive hydrogel, synthesized via a single-pot method employing lignosulfonate sodium and sodium alginate. The hydrogel’s high mechanical strength (∼196 kPa modulus, ∼435 kPa tensile) and conductivity stem from its dynamic hydrogen bonds, electrostatic interactions, and 3D network. Furthermore, the hydrogel exhibits adhesive properties due to sulfonic, phenolic hydroxyl, carboxyl, and hydroxyl groups from lignosulfonate sodium and sodium alginate, enabling it to adhere to various material surfaces. It also detects human physiological signals with wireless monitoring capability, demonstrating a rapid response (∼100 ms) and high sensitivity, with a maximum gauge factor of 4 at strains of 0–10%.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 10","pages":"7140–7151"},"PeriodicalIF":5.4,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145147222","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":"Spider-Silk-Like Alginate Fibers with Outstanding Photomodulating Mechanical Properties upon Molecular Motion","authors":"Lei Zhang, , , Zhongtao Wu, , , Xue Zhou, , , Luyang Wang, , , Yue Li, , , Tianci Zhang, , , Xiangyu Wang, , and , Xiliang Luo*, ","doi":"10.1021/acs.biomac.5c01156","DOIUrl":"10.1021/acs.biomac.5c01156","url":null,"abstract":"<p >Spider silks exhibit extraordinary mechanical performances by combining strength and toughness together. However, spider-silk-like materials hardly achieve great modulation of mechanical properties under the trigger of external stimuli. Herein, a molecular designing strategy for synthesizing spider silk-like fibers is developed by cross-linking alginate molecules with the designed merocyanine-containing ammonium surfactant as flexible contact points. Through establishing an electrostatic complexation between alginate and surfactant, the noncovalent cohesive network imparts the fibers with an outstanding strength of 1.54 GPa and a toughness of 121.12 MJ/m<sup>3</sup>. Assisted by the isomerization of merocyanine, the strength and toughness of such fibers could be light-modulated to be 0.67 GPa and 16.87 MJ/m<sup>3</sup>. The spider silk-like and photoresponsive mechanical properties, reversible color change, and good resistance to various conditions could support the use of such alginate fibers in wide-application scenarios. This study provides a new design strategy for fabricating smart biomaterials with high mechanical performances.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 10","pages":"6880–6892"},"PeriodicalIF":5.4,"publicationDate":"2025-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145129576","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}
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