Pub Date : 2025-11-10DOI: 10.1021/acs.biomac.5c01432
Jinwei Wang , Yue Chang , Jiayuan Liu , Cuiping Wang , Jinglin Yu , Les Copeland , Shujun Wang
Previous studies have shown that starch interacts with fatty acids, monoglycerides, or diglycerides to form starch-lipid complexes. Triacylglycerols (TAG) have been considered incapable of forming complexes with starch. Here, we describe a novel complexation strategy using octenyl succinic anhydride-modified maize starch (OSAMS) and glyceryl tridodecanoate (TLG) to form OSAMS-TAG complexes for the first time. MD simulations showed that the three hydrocarbon tails of the TLG molecule were encapsulated together by amylose helices, mainly through van der Waals forces. Structural analyses showed the OSAMS-TLG complexes to have a typical V-type crystalline pattern, with higher DS of OSAMS being more favorable for the formation of V-type complexes. The OSAMS-TLG complexes showed superior resistance to enzymatic hydrolysis and lipid oxidation than straight mixtures of native maize starch and TLG. This is the first study to show that OSA-starch can interact with TAG to form starch-lipid complexes, highlighting their potential for developing nutritionally functional starchy foods.
{"title":"Strategy for Fabricating Starch-Triacylglycerol Complexes with Resistance to Amylolysis and Lipid Oxidation","authors":"Jinwei Wang , Yue Chang , Jiayuan Liu , Cuiping Wang , Jinglin Yu , Les Copeland , Shujun Wang","doi":"10.1021/acs.biomac.5c01432","DOIUrl":"10.1021/acs.biomac.5c01432","url":null,"abstract":"<div><div>Previous studies have shown that starch interacts with fatty acids, monoglycerides, or diglycerides to form starch-lipid complexes. Triacylglycerols (TAG) have been considered incapable of forming complexes with starch. Here, we describe a novel complexation strategy using octenyl succinic anhydride-modified maize starch (OSAMS) and glyceryl tridodecanoate (TLG) to form OSAMS-TAG complexes for the first time. MD simulations showed that the three hydrocarbon tails of the TLG molecule were encapsulated together by amylose helices, mainly through van der Waals forces. Structural analyses showed the OSAMS-TLG complexes to have a typical V-type crystalline pattern, with higher DS of OSAMS being more favorable for the formation of V-type complexes. The OSAMS-TLG complexes showed superior resistance to enzymatic hydrolysis and lipid oxidation than straight mixtures of native maize starch and TLG. This is the first study to show that OSA-starch can interact with TAG to form starch-lipid complexes, highlighting their potential for developing nutritionally functional starchy foods.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (111KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 11","pages":"Pages 7998-8006"},"PeriodicalIF":5.4,"publicationDate":"2025-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145353034","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}
Pub Date : 2025-11-10DOI: 10.1021/acs.biomac.5c00321
Nanami Fujisawa , Mitsuhiro Ebara , James J. Lai
As a stimulus-responsive drug release system, we developed Diels–Alder (DA) induction-activated magnetic nanoparticles (DiMaN). Functionalization of polymer-coated magnetic nanoparticles (mNPs) with drugs via thermoreversible DA coupling enabled release through retro-Diels–Alder (rDA) cleavage upon heating. The (pDMAm-co-pFMA)-b-pAAc polymer supported mNP formation and drug binding. DA coupling with maleimide-functionalized drugs was verified by 1H NMR, showing distinct exo (3.23 ppm) and endo (3.48 ppm) signals after 72 h at 37 °C. Approximately 70% release was observed within 15 min at 80 °C, while the complex maintained stability at 40 °C. The superparamagnetic mNPs generated localized heating under an alternating current magnetic field (192 kHz, 480 A), raising the solution temperature by 6 °C within 5 min. The biotin-maleimide complex demonstrated higher release by rDA from furan-containing mNPs (approximately 150 μM) compared to the control group (approximately 103 μM). These results highlight DiMaN as a promising platform for magnetic-controlled, on-demand drug release.
{"title":"Magnetic Induction Heating Enables On-Demand Drug Release via Diels–Alder Polymeric Nanocarriers","authors":"Nanami Fujisawa , Mitsuhiro Ebara , James J. Lai","doi":"10.1021/acs.biomac.5c00321","DOIUrl":"10.1021/acs.biomac.5c00321","url":null,"abstract":"<div><div>As a stimulus-responsive drug release system, we developed Diels–Alder (DA) induction-activated magnetic nanoparticles (DiMaN). Functionalization of polymer-coated magnetic nanoparticles (mNPs) with drugs via thermoreversible DA coupling enabled release through retro-Diels–Alder (rDA) cleavage upon heating. The (pDMAm-<em>co</em>-pFMA)-<em>b</em>-pAAc polymer supported mNP formation and drug binding. DA coupling with maleimide-functionalized drugs was verified by <sup>1</sup>H NMR, showing distinct exo (3.23 ppm) and endo (3.48 ppm) signals after 72 h at 37 °C. Approximately 70% release was observed within 15 min at 80 °C, while the complex maintained stability at 40 °C. The superparamagnetic mNPs generated localized heating under an alternating current magnetic field (192 kHz, 480 A), raising the solution temperature by 6 °C within 5 min. The biotin-maleimide complex demonstrated higher release by rDA from furan-containing mNPs (approximately 150 μM) compared to the control group (approximately 103 μM). These results highlight DiMaN as a promising platform for magnetic-controlled, on-demand drug release.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (77KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 11","pages":"Pages 7265-7274"},"PeriodicalIF":5.4,"publicationDate":"2025-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145353083","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}
Pub Date : 2025-11-10DOI: 10.1021/acs.biomac.5c00805
Xinyu Zhang , Zhiqian Wu , Xiaoning Liu , Mengting Ma , Zhongquan Sui , Harold Corke
This study explored dynamic changes in starch granule-associated lipids (SGALs) during rice grain filling, including granule surface lipids (GSLs) and internal lipids (GILs). SGAL content increased from 0.335% at 6 days after anthesis (DAA) to 0.684% at DAA 46. Lipidomics identified 423 lipids in GSLs and 148 lipids in GILs, with triglycerides being the most abundant. In GSLs, 23 lipids, including phosphatidic acid (5:0_16:0), monoacylglycerol (18:1), and lysophosphatidylglycerol (14:0), were upregulated from DAA 6 to 22. The GSLs showing changes during grain filling may be related to amyloplast membrane metabolism. For GILs, 7 lipids were upregulated from DAA 6 to 22, with only acyl carnitine (25:8) upregulated between DAA 22 and 46. Triglycerides (11:0_8:0_10:0) and (P-10:0_16:2) increased first and then decreased, suggesting changes in intracellular lipid dynamics related to carbon partitioning. This study detailed changes in SGALs during rice grain filling, revealing their potential roles in starch biosynthesis.
{"title":"Lipidomics Reveals Dynamic Changes of Starch Granule-Associated Lipids during Rice Grain Filling","authors":"Xinyu Zhang , Zhiqian Wu , Xiaoning Liu , Mengting Ma , Zhongquan Sui , Harold Corke","doi":"10.1021/acs.biomac.5c00805","DOIUrl":"10.1021/acs.biomac.5c00805","url":null,"abstract":"<div><div>This study explored dynamic changes in starch granule-associated lipids (SGALs) during rice grain filling, including granule surface lipids (GSLs) and internal lipids (GILs). SGAL content increased from 0.335% at 6 days after anthesis (DAA) to 0.684% at DAA 46. Lipidomics identified 423 lipids in GSLs and 148 lipids in GILs, with triglycerides being the most abundant. In GSLs, 23 lipids, including phosphatidic acid (5:0_16:0), monoacylglycerol (18:1), and lysophosphatidylglycerol (14:0), were upregulated from DAA 6 to 22. The GSLs showing changes during grain filling may be related to amyloplast membrane metabolism. For GILs, 7 lipids were upregulated from DAA 6 to 22, with only acyl carnitine (25:8) upregulated between DAA 22 and 46. Triglycerides (11:0_8:0_10:0) and (P-10:0_16:2) increased first and then decreased, suggesting changes in intracellular lipid dynamics related to carbon partitioning. This study detailed changes in SGALs during rice grain filling, revealing their potential roles in starch biosynthesis.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (166KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 11","pages":"Pages 7331-7342"},"PeriodicalIF":5.4,"publicationDate":"2025-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144705763","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}
Pub Date : 2025-11-10DOI: 10.1021/acs.biomac.5c01510
Robert Forster , Bellinda Lantzberg , Annabelle Weldert , Laura Rosenberger , Yanira Zeyn , Danuta Kowalczyk , Seah Ling Kuan , Christian Kersten , Matthias Bros , Tanja Weil , Tanja Schirmeister , Till Opatz
Actively targeted delivery of nanocarriers (NC) modified with targeting structures (TS) binding to cell surface receptors, specific to target cells, enables enhanced selectivity and efficacy of cellular uptake. This is influenced by the ligand density on the NC surface. Herein, the impact of type, valency, and surface density of high-mannan derived TS on the C-type lectin receptor (CLR)-mediated uptake of human serum albumin (HSA)-based NCs in immune cell populations was investigated. Monovalent and trivalent TSs were prepared via efficient synthesis protocols and investigated regarding their affinity versus isolated carbohydrate recognition domains (CRD) of CD206 and CD209 within a NanoDSF study. Conjugation to HSA resulted in low valency and saturated NCs with a well-defined mannose epitope count. An in vitro study with bone-marrow-derived dendritic cells and splenic immune cells revealed the impact of the NC surface modification on cellular uptake and cell selectivity, allowing insights into the design of TSs and NCs.
{"title":"Surface Density of Mono- and Trivalent High-Mannan-Derived Targeting Structures with Different Affinities Impacts Cellular Uptake of Human Serum Albumin-Derived Nanocarriers","authors":"Robert Forster , Bellinda Lantzberg , Annabelle Weldert , Laura Rosenberger , Yanira Zeyn , Danuta Kowalczyk , Seah Ling Kuan , Christian Kersten , Matthias Bros , Tanja Weil , Tanja Schirmeister , Till Opatz","doi":"10.1021/acs.biomac.5c01510","DOIUrl":"10.1021/acs.biomac.5c01510","url":null,"abstract":"<div><div>Actively targeted delivery of nanocarriers (NC) modified with targeting structures (TS) binding to cell surface receptors, specific to target cells, enables enhanced selectivity and efficacy of cellular uptake. This is influenced by the ligand density on the NC surface. Herein, the impact of type, valency, and surface density of high-mannan derived TS on the C-type lectin receptor (CLR)-mediated uptake of human serum albumin (HSA)-based NCs in immune cell populations was investigated. Monovalent and trivalent TSs were prepared via efficient synthesis protocols and investigated regarding their affinity versus isolated carbohydrate recognition domains (CRD) of CD206 and CD209 within a NanoDSF study. Conjugation to HSA resulted in low valency and saturated NCs with a well-defined mannose epitope count. An <em>in vitro</em> study with bone-marrow-derived dendritic cells and splenic immune cells revealed the impact of the NC surface modification on cellular uptake and cell selectivity, allowing insights into the design of TSs and NCs.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (261KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 11","pages":"Pages 8087-8102"},"PeriodicalIF":5.4,"publicationDate":"2025-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145243314","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}
Pub Date : 2025-11-10DOI: 10.1021/acs.biomac.5c00598
Victor Lehot , Ondřej Lidický , Julien Most , Marc Nothisen , Stéphane Erb , Igor Dovgan , Artem Osypenko , Oleksandr Koniev , Sergii Kolodych , Lenka Kotrchová , Guilhem Chaubet , Sarah Cianférani , Tomáš Etrych , Alain Wagner
In the past two decades, antibody–drug conjugates (ADCs) have emerged as highly effective targeted therapeutics against cancers. One current path to improve ADCs is to increase the amount of cytotoxic payload delivered to cancer cells by conjugating antibodies with a soluble polymer bearing several drug molecules. However, this approach is challenging due to the high molecular weight of the polymer and the need to strictly control the degree of conjugation to maintain favorable pharmacokinetic and binding profiles. Here, we build from the recent development brought to our automated stoichiometric conjugation device to tackle this challenge. We produced a new format of ADC-like targeted therapy: monoconjugated Antibody–Polymer–Drug Conjugates (APDCs) with enzyme-cleavable linkers, designed to achieve selective delivery of the cytotoxic MMAE to HER2+ cancer cells. We showed the selectivity of our conjugates for HER2+ over HER2– cells in vitro and demonstrated their efficiency in vivo in a SKBR-3-xenografted mouse (NOD-SCID) model.
{"title":"Stoichiometric Antibody–Polymer–Drug Conjugate for Effective Low-Dose Treatment of Breast Cancer","authors":"Victor Lehot , Ondřej Lidický , Julien Most , Marc Nothisen , Stéphane Erb , Igor Dovgan , Artem Osypenko , Oleksandr Koniev , Sergii Kolodych , Lenka Kotrchová , Guilhem Chaubet , Sarah Cianférani , Tomáš Etrych , Alain Wagner","doi":"10.1021/acs.biomac.5c00598","DOIUrl":"10.1021/acs.biomac.5c00598","url":null,"abstract":"<div><div>In the past two decades, antibody–drug conjugates (ADCs) have emerged as highly effective targeted therapeutics against cancers. One current path to improve ADCs is to increase the amount of cytotoxic payload delivered to cancer cells by conjugating antibodies with a soluble polymer bearing several drug molecules. However, this approach is challenging due to the high molecular weight of the polymer and the need to strictly control the degree of conjugation to maintain favorable pharmacokinetic and binding profiles. Here, we build from the recent development brought to our automated stoichiometric conjugation device to tackle this challenge. We produced a new format of ADC-like targeted therapy: monoconjugated Antibody–Polymer–Drug Conjugates (APDCs) with enzyme-cleavable linkers, designed to achieve selective delivery of the cytotoxic MMAE to HER2<sup>+</sup> cancer cells. We showed the selectivity of our conjugates for HER2<sup>+</sup> over HER2<sup>–</sup> cells in vitro and demonstrated their efficiency in vivo in a SKBR-3-xenografted mouse (NOD-SCID) model.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (100KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 11","pages":"Pages 7309-7318"},"PeriodicalIF":5.4,"publicationDate":"2025-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145285065","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}
Pub Date : 2025-11-10DOI: 10.1021/acs.biomac.5c00450
Uxia Gato-Diaz , Sandra Blanco-Garcia , Diana Peixoto , Angel Concheiro , Carmen Alvarez-Lorenzo , Barbara Blanco-Fernandez
Pancreatic ductal adenocarcinoma is one of the cancers with the least favorable survival prognosis worldwide. It is characterized by a high desmoplastic stroma rich in collagen I, which regulates pancreatic cancer cells’ behavior. There is a critical need to develop desmoplastic 3D models for preclinical testing. In this study, bioinks that imitate the biochemical characteristics of pancreatic ductal adenocarcinoma were developed to observe the influence that the desmoplastic extracellular matrix has on cancer cells. The bioinks were made of gelatin methacrylamide, alginate, and different concentrations of collagen I. Cancer cells were able to proliferate in all bioinks, presenting high paclitaxel resistance and a high expression of desmoplasia and extracellular matrix remodeling markers. The designed bioinks can play a crucial role in developing more clinically relevant cancer models for chemotherapeutic drug screening. Furthermore, they have significant potential for studying the influence of desmoplasia and for improving advanced treatment approaches for pancreatic cancer.
{"title":"A 3D Bioprinted Pancreatic Cancer Model Using Collagen-Gelatin Methacrylamide-Alginate Bioinks to Mimic the Desmoplastic Microenvironment","authors":"Uxia Gato-Diaz , Sandra Blanco-Garcia , Diana Peixoto , Angel Concheiro , Carmen Alvarez-Lorenzo , Barbara Blanco-Fernandez","doi":"10.1021/acs.biomac.5c00450","DOIUrl":"10.1021/acs.biomac.5c00450","url":null,"abstract":"<div><div>Pancreatic ductal adenocarcinoma is one of the cancers with the least favorable survival prognosis worldwide. It is characterized by a high desmoplastic stroma rich in collagen I, which regulates pancreatic cancer cells’ behavior. There is a critical need to develop desmoplastic 3D models for preclinical testing. In this study, bioinks that imitate the biochemical characteristics of pancreatic ductal adenocarcinoma were developed to observe the influence that the desmoplastic extracellular matrix has on cancer cells. The bioinks were made of gelatin methacrylamide, alginate, and different concentrations of collagen I. Cancer cells were able to proliferate in all bioinks, presenting high paclitaxel resistance and a high expression of desmoplasia and extracellular matrix remodeling markers. The designed bioinks can play a crucial role in developing more clinically relevant cancer models for chemotherapeutic drug screening. Furthermore, they have significant potential for studying the influence of desmoplasia and for improving advanced treatment approaches for pancreatic cancer.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (129KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 11","pages":"Pages 7275-7288"},"PeriodicalIF":5.4,"publicationDate":"2025-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145285096","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}
Pub Date : 2025-11-10DOI: 10.1021/acs.biomac.5c00955
Shahar Tevet , Michal Brodsky , Roey J. Amir
A key challenge in designing enzyme-responsive micellar nanocarriers lies in balancing their stability and enzymatic degradation. While it has been widely assumed that the micelle–unimer exchange governs enzyme accessibility to the hydrophobic blocks, this relationship had not been directly demonstrated. Here, to uncover this long-assumed mechanistic link, we synthesized a set of triblock amphiphiles that convert by an in situ transition to diblock amphiphiles via reductive cleavage of a central disulfide bond. In parallel, hydrophobicity was independently tuned by modifying the aliphatic end-groups. Enzymatic degradation studies and Förster resonance energy transfer (FRET)-based exchange assays showed two consistent trends across all systems: increasing hydrophobicity led to slower micelle–unimer exchange and reduced enzymatic degradation rates, while transition to diblock consistently enhanced both. These results provide direct evidence that exchange kinetics govern enzymatic degradation and lay the mechanistic foundation for overcoming the stability–degradability barrier for enzyme-responsive micelles by applying architectural transitions as a molecular programming tool.
{"title":"Unimer Exchange as a Tool for Programming Enzymatic Degradation through Micellar Dynamics","authors":"Shahar Tevet , Michal Brodsky , Roey J. Amir","doi":"10.1021/acs.biomac.5c00955","DOIUrl":"10.1021/acs.biomac.5c00955","url":null,"abstract":"<div><div>A key challenge in designing enzyme-responsive micellar nanocarriers lies in balancing their stability and enzymatic degradation. While it has been widely assumed that the micelle–unimer exchange governs enzyme accessibility to the hydrophobic blocks, this relationship had not been directly demonstrated. Here, to uncover this long-assumed mechanistic link, we synthesized a set of triblock amphiphiles that convert by an in situ transition to diblock amphiphiles via reductive cleavage of a central disulfide bond. In parallel, hydrophobicity was independently tuned by modifying the aliphatic end-groups. Enzymatic degradation studies and Förster resonance energy transfer (FRET)-based exchange assays showed two consistent trends across all systems: increasing hydrophobicity led to slower micelle–unimer exchange and reduced enzymatic degradation rates, while transition to diblock consistently enhanced both. These results provide direct evidence that exchange kinetics govern enzymatic degradation and lay the mechanistic foundation for overcoming the stability–degradability barrier for enzyme-responsive micelles by applying architectural transitions as a molecular programming tool.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (97KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 11","pages":"Pages 7423-7433"},"PeriodicalIF":5.4,"publicationDate":"2025-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145273114","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}
Pub Date : 2025-11-10DOI: 10.1021/acs.biomac.5c01417
Liangliang Zhang , Xvyue Zhou , Xinmeng Li , Kun Wang , Peng Zhou , Weixiao Ding , Jian Cui , Yalei Qiao , Shudai Huang , Chao Luan , Lei Zhang , Kun Chen , Jiaan Zhang
Psoriasis is a chronic, inflammatory skin disorder driven by dysregulated keratinocyte-immune interactions and oxidative stress. To address limitations of conventional therapies, we engineered a sulfated bacterial cellulose/chitosan hydrogel that integrates intrinsic bioactivity with controlled methotrexate delivery (MTX-SBC/CS Gel). Sulfonation introduced sulfonic groups, conferring potent ROS-scavenging activity while optimizing drug compatibility and release kinetics. Chitosan enabled self-healing and bioadhesion through hydrogen-bonding networks. Molecular simulations and experiments revealed how sulfonic groups modulate drug-polymer interactions. In imiquimod-induced psoriatic models, MTX-SBC/CS Gel exhibited therapeutic efficacy comparable to that of the clinical standard betamethasone, with SBC alone showing beneficial effects; both accelerated epidermal normalization, and cytokine suppression. Transcriptomics identified SBC’s multimodal mechanism: downregulation of IL-23/Th17 axis components, inhibition of keratinocyte hyperproliferation, and restoration of redox homeostasis via HSP90α-mediated pathways. The synergistic integration of sulfonation-enabled ROS scavenging, and optimized MTX release kinetics establishes this engineered hydrogel as a promising platform for the management of dermatoses.
{"title":"Engineered Sulfonated Bacterial Cellulose Hydrogel with Dual Bioactive-Drug Delivery Functions for Precision Treatment of Psoriasis","authors":"Liangliang Zhang , Xvyue Zhou , Xinmeng Li , Kun Wang , Peng Zhou , Weixiao Ding , Jian Cui , Yalei Qiao , Shudai Huang , Chao Luan , Lei Zhang , Kun Chen , Jiaan Zhang","doi":"10.1021/acs.biomac.5c01417","DOIUrl":"10.1021/acs.biomac.5c01417","url":null,"abstract":"<div><div>Psoriasis is a chronic, inflammatory skin disorder driven by dysregulated keratinocyte-immune interactions and oxidative stress. To address limitations of conventional therapies, we engineered a sulfated bacterial cellulose/chitosan hydrogel that integrates intrinsic bioactivity with controlled methotrexate delivery (MTX-SBC/CS Gel). Sulfonation introduced sulfonic groups, conferring potent ROS-scavenging activity while optimizing drug compatibility and release kinetics. Chitosan enabled self-healing and bioadhesion through hydrogen-bonding networks. Molecular simulations and experiments revealed how sulfonic groups modulate drug-polymer interactions. In imiquimod-induced psoriatic models, MTX-SBC/CS Gel exhibited therapeutic efficacy comparable to that of the clinical standard betamethasone, with SBC alone showing beneficial effects; both accelerated epidermal normalization, and cytokine suppression. Transcriptomics identified SBC’s multimodal mechanism: downregulation of IL-23/Th17 axis components, inhibition of keratinocyte hyperproliferation, and restoration of redox homeostasis via HSP90α-mediated pathways. The synergistic integration of sulfonation-enabled ROS scavenging, and optimized MTX release kinetics establishes this engineered hydrogel as a promising platform for the management of dermatoses.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (185KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 11","pages":"Pages 7974-7988"},"PeriodicalIF":5.4,"publicationDate":"2025-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145306348","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}
Pub Date : 2025-11-10DOI: 10.1021/acs.biomac.5c01565
Ji Hyun Lee , Eun Seo Lee , Un Jung Chae , Sung Ok Han , Jeong Eun Hyeon
Bioplastics offer eco-friendly alternatives to conventional plastics. This study aimed to expand the application scope of bioplastics by developing a functional material with enhanced conductivity. We recombined the SpyCatcher–SpyTag system from Streptococcus pyogenes with leghemoglobin from Glycine max to generate SpyCatcher-GmLegC2-SpyTag, SpyCatcher-GmLegC2-SpyCatcher, and SpyTag-GmLegC2-SpyTag proteins, which assembled into a conductive polymer. This polymer exhibited electrical conductivity 2.5 times higher than free hemin in aqueous solution when mixed with hemin. For improved stability, SpyCatcher-GmLegC2 was fused with a carbohydrate-binding module from Clostridium cellulovorans and integrated into bacterial cellulose scaffolds. The resulting composite showed a 141-fold increase in conductivity compared to free hemin and exhibited uniform, stable performance. This eco-friendly conductive bioplastic demonstrates strong potential for applications in wearable sensors, electronic devices, and sustainable conductive materials.
{"title":"Boosting Conductive Bioplastic Applications with SpyCatcher–SpyTag Technology and Cellulose Scaffolds","authors":"Ji Hyun Lee , Eun Seo Lee , Un Jung Chae , Sung Ok Han , Jeong Eun Hyeon","doi":"10.1021/acs.biomac.5c01565","DOIUrl":"10.1021/acs.biomac.5c01565","url":null,"abstract":"<div><div>Bioplastics offer eco-friendly alternatives to conventional plastics. This study aimed to expand the application scope of bioplastics by developing a functional material with enhanced conductivity. We recombined the SpyCatcher–SpyTag system from Streptococcus pyogenes with leghemoglobin from <em>Glycine max</em> to generate SpyCatcher-GmLegC<sub>2</sub>-SpyTag, SpyCatcher-GmLegC<sub>2</sub>-SpyCatcher, and SpyTag-GmLegC<sub>2</sub>-SpyTag proteins, which assembled into a conductive polymer. This polymer exhibited electrical conductivity 2.5 times higher than free hemin in aqueous solution when mixed with hemin. For improved stability, SpyCatcher-GmLegC<sub>2</sub> was fused with a carbohydrate-binding module from Clostridium cellulovorans and integrated into bacterial cellulose scaffolds. The resulting composite showed a 141-fold increase in conductivity compared to free hemin and exhibited uniform, stable performance. This eco-friendly conductive bioplastic demonstrates strong potential for applications in wearable sensors, electronic devices, and sustainable conductive materials.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (99KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 11","pages":"Pages 8160-8166"},"PeriodicalIF":5.4,"publicationDate":"2025-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145342091","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}
Pub Date : 2025-11-10DOI: 10.1021/acs.biomac.5c01715
Yasuyuki Maki , Koichi Matsuo , Masahiko Annaka
It is well-known that sugars such as sucrose increase the gelling temperature and mechanical properties of gelatin. In this study, the effects of sucrose and sucralose, a sucrose derivative obtained by the chlorination of sucrose, on the gelation behavior of gelatin were investigated. The gelation of gelatin, monitored by rheological properties and helix formation, was enhanced by the addition of sucrose but inhibited by the addition of sucralose. For both sucrose and sucralose, the gelation kinetics were governed by the undercooling from the gelling temperature. To gain insights into the mechanisms by which sucrose and sucralose stabilize and destabilize gelatin gels, respectively, the preferential solvation of a collagen model peptide in aqueous solutions of sucrose or sucralose was measured using small-angle X-ray scattering. The observed preferential solvation behavior of the peptide was consistent with the results of the effect of these sugars on the gelation behavior of gelatin.
{"title":"Effect of Sucrose and Sucralose on the Gelation of Gelatin","authors":"Yasuyuki Maki , Koichi Matsuo , Masahiko Annaka","doi":"10.1021/acs.biomac.5c01715","DOIUrl":"10.1021/acs.biomac.5c01715","url":null,"abstract":"<div><div>It is well-known that sugars such as sucrose increase the gelling temperature and mechanical properties of gelatin. In this study, the effects of sucrose and sucralose, a sucrose derivative obtained by the chlorination of sucrose, on the gelation behavior of gelatin were investigated. The gelation of gelatin, monitored by rheological properties and helix formation, was enhanced by the addition of sucrose but inhibited by the addition of sucralose. For both sucrose and sucralose, the gelation kinetics were governed by the undercooling from the gelling temperature. To gain insights into the mechanisms by which sucrose and sucralose stabilize and destabilize gelatin gels, respectively, the preferential solvation of a collagen model peptide in aqueous solutions of sucrose or sucralose was measured using small-angle X-ray scattering. The observed preferential solvation behavior of the peptide was consistent with the results of the effect of these sugars on the gelation behavior of gelatin.</div></div><div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (89KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span></div></div>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 11","pages":"Pages 8280-8288"},"PeriodicalIF":5.4,"publicationDate":"2025-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145248921","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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