BiomacromoleculesPub Date : 2025-04-06DOI: 10.1021/acs.biomac.4c01707
Wafaa Aljuhani, Matthew P Wylie, Rudra N Purusottam, Colin P McCoy, Steven E J Bell
{"title":"Probing the Coupled Equilibria between Metal Nanoparticles, Antibiotics and Components of the Extracellular Matrix in Biofilms with SERS.","authors":"Wafaa Aljuhani, Matthew P Wylie, Rudra N Purusottam, Colin P McCoy, Steven E J Bell","doi":"10.1021/acs.biomac.4c01707","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01707","url":null,"abstract":"<p><p>Understanding the interplay between nanoparticles, biomaterials and drug molecules in biological environments is important but studying these interactions in complex systems such as biofilms is challenging. Here, surface-enhanced Raman spectroscopy (SERS) with gold nanostars (NS) was used to monitor how biofilm components influence the binding and SERS signals of two antibiotics, levofloxacin (Levo) and ampicillin (Amp). The SERS signals of both antibiotics were reduced by approximately 70% (Levo) and 90% (Amp) in biofilm environments. Investigations of mixtures of model biofilm components: adenine (nucleic acids), alginate (polysaccharides) and albumin (proteins), revealed that their interactions with NS are governed by coupled equilibria. This gave surprising results, for example, alginate reduced the interference from adenine and albumin, so adding alginate increased the intensity of the antibiotic signals 4x. These findings highlight the importance of matrix component interactions in modulating detection sensitivity and show that these effects are critical in allowing clinically relevant detection levels to be achieved.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-04-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143794058","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":"High-Performance Multiscale LNPs from Black Liquor as Repulpable Paper Coatings with Enhanced Water, Oil, and Vapor Resistance","authors":"Wen Chen, Zhenyu Zhou, Dahang Zha, Ruihao Zhang, Ren’ai Li, Yunfeng Cao, Zhulan Liu* and Huining Xiao*, ","doi":"10.1021/acs.biomac.5c0000510.1021/acs.biomac.5c00005","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00005https://doi.org/10.1021/acs.biomac.5c00005","url":null,"abstract":"<p >Technical lignin in alkaline pulping black liquor is usually combusted for energy in a soda recovery unit. To improve resource utilization, multiscale lignin nanoparticles (LNPs) were acid precipitated from black liquor and combined with gelatinized starch (SS) to produce a series of uniformly mixed surface coating agents to enhance the barrier properties of paper materials including water, oil, and water vapor resistance. The coating with 20%SS and 50%LNPs (based on oven-dried SS) with a diameter of 276 nm could significantly improve the barrier properties of the coated paper. Cobb 60 decreased by 79.6% from 67.98 to 13.86 g/m<sup>2</sup>, Kit rating improved from 0 to 10, and water vapor transmission reduced from ≥3000 to 441.69 g/m<sup>2</sup>·day. The coated paper presented superior mechanical properties, thermal stability, repulpability, and biodegradability. This work provides an effective strategy for the high-value application of pulping black liquor and holds promise for paper-based packaging.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 4","pages":"2500–2512 2500–2512"},"PeriodicalIF":5.5,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143825215","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":"Preparation, Conformational Structure, and Proteolytic Activity of Papain Covalently Conjugated to Poly(ethylene glycol)-Tethered Lipid Bilayer Membranes.","authors":"Yuya Takahashi, Kyohei Kubota, Makoto Yoshimoto, Noriko Yoshimoto","doi":"10.1021/acs.biomac.4c01324","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01324","url":null,"abstract":"<p><p>Conjugation of enzymes to lipid membranes is a key approach to reconstitute fascinating features of cell organelles and to deduce the nature of membrane-involved biological events. In this work, papain was covalently conjugated via a cross-linker to phospholipid vesicles (liposomes) tethered with poly(ethylene glycol) (PEG) at 25 °C and pH = 7.0, followed by chromatographic purification. The size of the PEG moiety and the type of cross-linker were optimized to obtain PEG-tethered liposome-conjugated papain (liposome-PEG-papain). Slight conformational changes of the membrane-conjugated papain in both its secondary and tertiary structures were revealed using circular dichroism and intrinsic fluorescence measurements. Notably, heat treatment of a liposome-PEG-papain dispersion at 77 or 84 °C caused permeabilization of the lipid membranes to 5(6)-carboxyfluorescein. Furthermore, liposome-PEG-papain exhibited the digestion activity of casein at 37 °C and pH = 7.6. The structural flexibility of liposomes as enzyme carriers may provide the opportunity to functionalize the membrane-conjugated biomacromolecules.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143770722","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 : 2025-04-02DOI: 10.1021/acs.biomac.4c01847
Xinghan Wu, Wenxin Xu, Xuantao Huang, Nianhua Dan, Yining Chen, Zhengjun Li, Yunbing Wang
{"title":"Engineering High-Performance Multifunctional Scaffolds from the Acellular Dermal Matrix for Abdominal Wall Defects Repair via a Dopamine Progressive Permeation-Cross-Linking Strategy.","authors":"Xinghan Wu, Wenxin Xu, Xuantao Huang, Nianhua Dan, Yining Chen, Zhengjun Li, Yunbing Wang","doi":"10.1021/acs.biomac.4c01847","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01847","url":null,"abstract":"<p><p>Emergency repair of complicated full-thickness abdominal wall defects remains one of the most common and challenging surgical emergencies globally. Here, an integrated polydopamine permeating-cross-linking strategy was innovatively proposed to convert porcine acellular dermal matrix (pADM) into versatile, degradation-resistant biopatches (PDA-pADM) for efficiently repairing full-thickness abdominal wall defects. The strategy significantly addresses the challenge that natural-property improvement and biocompatibility of biomaterials are difficult to balance. Molecularly, dopamine (DA) molecules could fully permeate into the collagen fibers of the acellular dermal matrix and then automatically trigger the interfacial in situ polymerization of dopamine monomers among collagen fibers to achieve the efficient cross-linking of pADM. Surprisingly, the enzymatic durability of the biopatch shows significant improvements, extending the original duration from 3 to 20 d. Comprehensive in vivo experiments have shown that PDA-pADM can effectively promote angiogenesis and inhibit inflammatory response, so as to achieve regeneration and repair of abdominal wall damage.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143762489","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 : 2025-04-02DOI: 10.1021/acs.biomac.4c0132410.1021/acs.biomac.4c01324
Yuya Takahashi, Kyohei Kubota, Makoto Yoshimoto and Noriko Yoshimoto*,
{"title":"Preparation, Conformational Structure, and Proteolytic Activity of Papain Covalently Conjugated to Poly(ethylene glycol)-Tethered Lipid Bilayer Membranes","authors":"Yuya Takahashi, Kyohei Kubota, Makoto Yoshimoto and Noriko Yoshimoto*, ","doi":"10.1021/acs.biomac.4c0132410.1021/acs.biomac.4c01324","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01324https://doi.org/10.1021/acs.biomac.4c01324","url":null,"abstract":"<p >Conjugation of enzymes to lipid membranes is a key approach to reconstitute fascinating features of cell organelles and to deduce the nature of membrane-involved biological events. In this work, papain was covalently conjugated via a cross-linker to phospholipid vesicles (liposomes) tethered with poly(ethylene glycol) (PEG) at 25 °C and pH = 7.0, followed by chromatographic purification. The size of the PEG moiety and the type of cross-linker were optimized to obtain PEG-tethered liposome-conjugated papain (liposome-PEG-papain). Slight conformational changes of the membrane-conjugated papain in both its secondary and tertiary structures were revealed using circular dichroism and intrinsic fluorescence measurements. Notably, heat treatment of a liposome-PEG-papain dispersion at 77 or 84 °C caused permeabilization of the lipid membranes to 5(6)-carboxyfluorescein. Furthermore, liposome-PEG-papain exhibited the digestion activity of casein at 37 °C and pH = 7.6. The structural flexibility of liposomes as enzyme carriers may provide the opportunity to functionalize the membrane-conjugated biomacromolecules.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 4","pages":"2131–2145 2131–2145"},"PeriodicalIF":5.5,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.biomac.4c01324","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143825183","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":"High-Performance Multiscale LNPs from Black Liquor as Repulpable Paper Coatings with Enhanced Water, Oil, and Vapor Resistance.","authors":"Wen Chen, Zhenyu Zhou, Dahang Zha, Ruihao Zhang, Ren'ai Li, Yunfeng Cao, Zhulan Liu, Huining Xiao","doi":"10.1021/acs.biomac.5c00005","DOIUrl":"https://doi.org/10.1021/acs.biomac.5c00005","url":null,"abstract":"<p><p>Technical lignin in alkaline pulping black liquor is usually combusted for energy in a soda recovery unit. To improve resource utilization, multiscale lignin nanoparticles (LNPs) were acid precipitated from black liquor and combined with gelatinized starch (SS) to produce a series of uniformly mixed surface coating agents to enhance the barrier properties of paper materials including water, oil, and water vapor resistance. The coating with 20%SS and 50%LNPs (based on oven-dried SS) with a diameter of 276 nm could significantly improve the barrier properties of the coated paper. Cobb 60 decreased by 79.6% from 67.98 to 13.86 g/m<sup>2</sup>, Kit rating improved from 0 to 10, and water vapor transmission reduced from ≥3000 to 441.69 g/m<sup>2</sup>·day. The coated paper presented superior mechanical properties, thermal stability, repulpability, and biodegradability. This work provides an effective strategy for the high-value application of pulping black liquor and holds promise for paper-based packaging.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143762494","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 : 2025-04-02DOI: 10.1021/acs.biomac.4c0184710.1021/acs.biomac.4c01847
Xinghan Wu, Wenxin Xu, Xuantao Huang, Nianhua Dan, Yining Chen*, Zhengjun Li and Yunbing Wang,
{"title":"Engineering High-Performance Multifunctional Scaffolds from the Acellular Dermal Matrix for Abdominal Wall Defects Repair via a Dopamine Progressive Permeation-Cross-Linking Strategy","authors":"Xinghan Wu, Wenxin Xu, Xuantao Huang, Nianhua Dan, Yining Chen*, Zhengjun Li and Yunbing Wang, ","doi":"10.1021/acs.biomac.4c0184710.1021/acs.biomac.4c01847","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01847https://doi.org/10.1021/acs.biomac.4c01847","url":null,"abstract":"<p >Emergency repair of complicated full-thickness abdominal wall defects remains one of the most common and challenging surgical emergencies globally. Here, an integrated polydopamine permeating-cross-linking strategy was innovatively proposed to convert porcine acellular dermal matrix (pADM) into versatile, degradation-resistant biopatches (PDA-pADM) for efficiently repairing full-thickness abdominal wall defects. The strategy significantly addresses the challenge that natural-property improvement and biocompatibility of biomaterials are difficult to balance. Molecularly, dopamine (DA) molecules could fully permeate into the collagen fibers of the acellular dermal matrix and then automatically trigger the interfacial in situ polymerization of dopamine monomers among collagen fibers to achieve the efficient cross-linking of pADM. Surprisingly, the enzymatic durability of the biopatch shows significant improvements, extending the original duration from 3 to 20 d. Comprehensive in vivo experiments have shown that PDA-pADM can effectively promote angiogenesis and inhibit inflammatory response, so as to achieve regeneration and repair of abdominal wall damage.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 4","pages":"2487–2499 2487–2499"},"PeriodicalIF":5.5,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143825218","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":"MXene-Incorporated Conductive Hydrogel Simulating Myocardial Microenvironment for Cardiac Repair and Functional Recovery.","authors":"Shan Yu, Ling Wang, Mengdie Chen, Yanjun Chen, Zhenbo Peng","doi":"10.1021/acs.biomac.4c01752","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01752","url":null,"abstract":"<p><p>Myocardial infarction (MI) remains one of the leading causes of mortality worldwide, necessitating advanced therapeutic strategies to address the resulting electrical disconnection and pathological remodeling. This study developed a conductive hydrogel by covalently cross-linking silk fibroin and hyaluronic acid, integrating MXene nanosheets to mimic the extracellular matrix (ECM). Results demonstrated that the incorporation of MXene significantly enhanced the hydrogel's conductivity, with SH-M5 exhibiting the highest conductivity of 0.32 S/m. The SH-M5 hydrogel effectively improved electrical signal transmission and enhanced the recovery of the left ventricular function in myocardial infarction. These findings underscore the transformative role of MXene in enhancing the functional properties of hydrogels for myocardial repair. The conductive hydrogel demonstrated a unique capacity to integrate mechanical reinforcement, electrical conductivity, and biocompatibility, presenting a promising platform for treating myocardial infarction and advancing regenerative medicine.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143750171","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":"Elasticity Anisotropy of <i>Bombyx mori</i> Silkworm Silk Fiber by Brillouin Light Spectroscopy.","authors":"Alina Aluculesei, Yuanzhong Zhang, Shifeng Huang, Zuyuan Wang, Yu Cang, Younjin Min, George Fytas","doi":"10.1021/acs.biomac.4c01844","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01844","url":null,"abstract":"<p><p>Silkworm silk has long been an important natural protein fiber for textile and medical applications, where its superior mechanical properties play a crucial role. Despite the many studies by conventional stress-strain tests, our understanding of the mechanical properties of silkworm silk remains limited. This work investigates the complete elastic properties of <i>Bombyx mori</i> silkworm silk in a noncontact, noninvasive manner by conducting Brillouin light spectroscopy experiments. The analysis of the angle-dependent sound velocities leads to the determination of the full elastic tensor and the engineering mechanical properties of the silkworm silk in natural and stretched states. In the natural state, the axial and lateral Young's moduli are 23.4 ± 1.0 and 10.4 ± 0.5 GPa, respectively, giving an elastic anisotropy of 2.3. Different from the strain-hardening behavior of the spider silk, the mechanical properties of the silkworm silk exhibit a weak strain-dependence up to the breakage strain (∼20%).</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.5,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143762487","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 : 2025-04-01DOI: 10.1021/acs.biomac.4c0184410.1021/acs.biomac.4c01844
Alina Aluculesei, Yuanzhong Zhang, Shifeng Huang, Zuyuan Wang, Yu Cang, Younjin Min and George Fytas*,
{"title":"Elasticity Anisotropy of Bombyx mori Silkworm Silk Fiber by Brillouin Light Spectroscopy","authors":"Alina Aluculesei, Yuanzhong Zhang, Shifeng Huang, Zuyuan Wang, Yu Cang, Younjin Min and George Fytas*, ","doi":"10.1021/acs.biomac.4c0184410.1021/acs.biomac.4c01844","DOIUrl":"https://doi.org/10.1021/acs.biomac.4c01844https://doi.org/10.1021/acs.biomac.4c01844","url":null,"abstract":"<p >Silkworm silk has long been an important natural protein fiber for textile and medical applications, where its superior mechanical properties play a crucial role. Despite the many studies by conventional stress–strain tests, our understanding of the mechanical properties of silkworm silk remains limited. This work investigates the complete elastic properties of <i>Bombyx mori</i> silkworm silk in a noncontact, noninvasive manner by conducting Brillouin light spectroscopy experiments. The analysis of the angle-dependent sound velocities leads to the determination of the full elastic tensor and the engineering mechanical properties of the silkworm silk in natural and stretched states. In the natural state, the axial and lateral Young’s moduli are 23.4 ± 1.0 and 10.4 ± 0.5 GPa, respectively, giving an elastic anisotropy of 2.3. Different from the strain-hardening behavior of the spider silk, the mechanical properties of the silkworm silk exhibit a weak strain-dependence up to the breakage strain (∼20%).</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":"26 4","pages":"2479–2486 2479–2486"},"PeriodicalIF":5.5,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.biomac.4c01844","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143825014","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}