Polymer Journal最新文献

筛选
英文 中文
Coordination polymerization of (Z)-1-phenyl[3]dendralene by a neodymium catalyst 钕催化剂配位聚合(Z)-1-苯基[3]树突烯
IF 2.7 4区 化学
Polymer Journal Pub Date : 2025-05-02 DOI: 10.1038/s41428-025-01044-6
Haruto Tanaka, Tomoyuki Toda, Katsuhiko Takenaka
{"title":"Coordination polymerization of (Z)-1-phenyl[3]dendralene by a neodymium catalyst","authors":"Haruto Tanaka, Tomoyuki Toda, Katsuhiko Takenaka","doi":"10.1038/s41428-025-01044-6","DOIUrl":"10.1038/s41428-025-01044-6","url":null,"abstract":"The control of the microstructure of polymers derived from conjugated dienes was investigated using coordination polymerization. In this work, we conducted coordination polymerization of (Z)-1-phenyl[3]dendralene (1Z-P3D) as a diene monomer. The polymerization of 1Z-P3D using a homogeneous neodymium catalyst yielded poly(1Z-P3D) with predominantly 4,6-structures (~100%). Coordination polymerization of (Z)-1-phenyl[3]dendralene(1Z-P3D) was investigated using by homogeneous neodymium catalyst. The polymer was obtained under the appropriate polymerization condition and the most part of polymer became insoluble in the progress of isolation. The microstructure of poly(1Z-P3D) prepared by neodymium catalyst was only 4,6-structure whereas poly(1Z-P3D) prepared by anionic initiator contained a predominant amount of 1,4-structure.","PeriodicalId":20302,"journal":{"name":"Polymer Journal","volume":"57 9","pages":"1043-1048"},"PeriodicalIF":2.7,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144990859","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A deeper dive into primitive polylactate polymerization and microdroplet assembly under restrictive early Earth conditions 深入研究早期地球条件下的原始聚乳酸聚合和微滴组装
IF 2.7 4区 化学
Polymer Journal Pub Date : 2025-04-30 DOI: 10.1038/s41428-025-01048-2
Mahendran Sithamparam, Ming-Jing He, Navaniswaran Tharumen, Rehana Afrin, Niannian Ding, Chen Chen, Ruiqin Yi, Po-Hsiang Wang, Tony Z. Jia, Kuhan Chandru
{"title":"A deeper dive into primitive polylactate polymerization and microdroplet assembly under restrictive early Earth conditions","authors":"Mahendran Sithamparam, Ming-Jing He, Navaniswaran Tharumen, Rehana Afrin, Niannian Ding, Chen Chen, Ruiqin Yi, Po-Hsiang Wang, Tony Z. Jia, Kuhan Chandru","doi":"10.1038/s41428-025-01048-2","DOIUrl":"10.1038/s41428-025-01048-2","url":null,"abstract":"Alpha hydroxy acids (AHAs) play various roles in modern biology such as in metabolism, but could have played different roles as “non-biomolecules” at the origins of life. Specifically, lactic acid (LA) and other AHAs can polymerize into polyesters and subsequently assemble into membraneless microdroplets (MMDs) upon dehydration-rehydration cycles, suggesting that polyester MMDs could have been relevant protocell models on early Earth. However, in particular, how the harsh conditions of early Earth, namely salinity and decreased reactant volume/concentration, could have affected primitive LA polymerization and subsequent MMD assembly is unclear. In this study, we found that while monovalent salts such as NaCl and KCl did not inhibit LA polymerization and MMD assembly even at high concentrations (up to 1 M), divalent salts such as MgCl2 and CaCl2 were inhibitory at much lower concentrations. Additionally, we found that lower reaction volumes and concentrations, potentially simulating confined microenvironments on early Earth, still supported LA polymerization and MMD assembly to some extent, albeit with decreased efficiency. These results suggest that early Earth’s environmental conditions could have still supported the polymerization of LA and the formation of MMD-based protocells in a variety of settings despite being quite harsh and variable. Lactic acid (LA), likely abundant on early Earth, can polymerize into polyesters and assemble into membraneless microdroplets (MMDs). However, how the harsh conditions of early Earth could have affected primitive LA polymerization and subsequent MMD assembly is unclear. In this study, we probed the effect of salinity, reaction volume, and reaction concentration on primitive LA polymerization and subsequent MMD assembly, and find that early Earth’s harsh environmental conditions could have still supported the formation of LA-based MMD protocells in a variety of settings.","PeriodicalId":20302,"journal":{"name":"Polymer Journal","volume":"57 8","pages":"897-910"},"PeriodicalIF":2.7,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41428-025-01048-2.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774178","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Liquid‒liquid phase separation induced by i-motif DNA under molecular crowding conditions 分子拥挤条件下i-motif DNA诱导的液-液相分离
IF 2.7 4区 化学
Polymer Journal Pub Date : 2025-04-30 DOI: 10.1038/s41428-025-01047-3
Ryosuke Suzuki, Mitsuki Tsuruta, Sumit Shil, Kosei Morohashi, Keiko Kawauchi, Daisuke Miyoshi
{"title":"Liquid‒liquid phase separation induced by i-motif DNA under molecular crowding conditions","authors":"Ryosuke Suzuki, Mitsuki Tsuruta, Sumit Shil, Kosei Morohashi, Keiko Kawauchi, Daisuke Miyoshi","doi":"10.1038/s41428-025-01047-3","DOIUrl":"10.1038/s41428-025-01047-3","url":null,"abstract":"Cytosine-rich sequences can fold into a four-stranded structure called the i-motif. These i-motif-forming DNA sequences are enriched in the promoter regions of cancer-related genes and telomeres, indicating their biological importance. Interestingly, an i-motif-forming DNA oligonucleotide derived from telomeres was reported to undergo liquid‒liquid phase separation (LLPS), suggesting that i-motifs regulate cellular processes involving gene expression via LLPS. However, it is still unclear whether i-motifs are able to undergo LLPS under physiological conditions because i-motif structures are thermodynamically stable only under acidic conditions. In this study, we systematically studied the thermodynamics of a series of i-motif-forming oligonucleotides and their ability to undergo LLPS under molecular crowding conditions that mimic the conditions inside cells at various pH values. The thermodynamic analyses revealed that crowding reagents with higher molecular weights stabilize the i-motif structure and increase its pKa. Moreover, we demonstrated that i-motif structures stabilized by molecular crowding undergo LLPS under neutral and even basic conditions. On the other hand, mutated oligonucleotides that do not form stable i-motif structures did not undergo LLPS. These results indicate that i-motif-forming DNAs can robustly and widely undergo LLPS depending on cellular environmental factors such as the solution pH, composition of crowding reagents and degree of molecular crowding in living cells. We showed that various i-motif-forming DNAs undergo LLPS with cationic peptide in acidic conditions. Considering cellular condition, we further investigated LLPS of DNAs in the molecular crowding conditions at physiological pH. LLPS is promoted by molecular crowding conditions at even in basic pH through stabilization of i-motif structure by molecular crowding condition.","PeriodicalId":20302,"journal":{"name":"Polymer Journal","volume":"57 8","pages":"931-940"},"PeriodicalIF":2.7,"publicationDate":"2025-04-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41428-025-01047-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774177","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Exploring the self-assembly of silk proteins through liquid-liquid phase separation 利用液-液相分离技术探索丝蛋白的自组装
IF 2.7 4区 化学
Polymer Journal Pub Date : 2025-04-28 DOI: 10.1038/s41428-025-01040-w
Michelle Gracia Lay, Nur Alia Oktaviani, Ali D. Malay, Keiji Numata
{"title":"Exploring the self-assembly of silk proteins through liquid-liquid phase separation","authors":"Michelle Gracia Lay, Nur Alia Oktaviani, Ali D. Malay, Keiji Numata","doi":"10.1038/s41428-025-01040-w","DOIUrl":"10.1038/s41428-025-01040-w","url":null,"abstract":"Silk fibers have been used by humans for millennia to create textiles and have recently gained the attention of scientists due to their unsurpassed mechanical properties. These properties arise from a sophisticated process by which the starting material, a liquid feedstock consisting of high-molecular-weight silk proteins, is rapidly converted within silk glands into solid fibers with a multi-scale hierarchical structure that is responsible for the material’s incredible robustness. Recently, liquid-liquid phase separation (LLPS) has emerged as a powerful framework for understanding the self-assembly behavior of silk proteins. Interestingly, LLPS-associated proteins typically exhibit disordered or dynamic conformations and have sequences rich in low-complexity multivalent repeats, reminiscent of silk protein sequences. In this review, we explore the evidence indicating that LLPS is a major aspect of silk fiber storage and assembly in both lepidopteran and spider systems. We discuss insights derived from comparative analyses of amino acid sequences, specific chemical triggers, and potential chemical interactions and contextualize the results from recent empirical investigations based on native and recombinant silk materials. We also discuss how LLPS mechanisms might be applied to the sustainable production of silk-like materials that replicate native hierarchical structures. Finally, we outline important areas for future investigations and speculate on how findings from the field of silk research may help illuminate the more general field of biomolecular condensates. The production of silk in spiders and silkworms involves the transformation of concentrated liquid protein feedstock into hierarchically organized solid fibers through a highly controlled mechanism facilitated by their respective glandular spinning apparatus. Recent insights suggest that liquid–liquid phase separation (LLPS) plays a central role in organizing the initially disordered silk protein chains into dense yet dynamic condensates, which is a key step towards rapid fiber formation. This hierarchical assembly process underlies the remarkable mechanical properties of silk fibers.","PeriodicalId":20302,"journal":{"name":"Polymer Journal","volume":"57 8","pages":"799-814"},"PeriodicalIF":2.7,"publicationDate":"2025-04-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41428-025-01040-w.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774181","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Supercharging design of an anti-lysozyme Fab antibody to regulate ligand-dependent reversible aggregation 抗溶菌酶Fab抗体调节配体依赖性可逆聚集的增压设计
IF 2.7 4区 化学
Polymer Journal Pub Date : 2025-04-25 DOI: 10.1038/s41428-025-01046-4
Keisuke Kasahara, Makoto Nakakido, Daisuke Kuroda, Satoru Nagatoishi, Kouhei Tsumoto
{"title":"Supercharging design of an anti-lysozyme Fab antibody to regulate ligand-dependent reversible aggregation","authors":"Keisuke Kasahara, Makoto Nakakido, Daisuke Kuroda, Satoru Nagatoishi, Kouhei Tsumoto","doi":"10.1038/s41428-025-01046-4","DOIUrl":"10.1038/s41428-025-01046-4","url":null,"abstract":"Protein aggregation and liquid‒liquid phase separation (LLPS), as key physicochemical processes, orchestrate protein behavior and function, and engineering a protein surface charge offers a robust approach to modulate protein‒protein interactions and, consequently, aggregation and phase separation. Among protein surface engineering methods, supercharging leads to a drastic increase in the protein net charge by replacing surface residues with charged amino acid residues. Previous studies have reported that some physicochemical properties of proteins are improved by supercharging, and changing the surface charge is considered to affect intermolecular interactions. In this study, we designed a new supercharged antigen-binding fragment (Fab) antibody mutant and investigated its aggregation behavior. Upon examination of the physicochemical properties of the designed supercharged antibody, the thermal stability, structure, and ligand binding affinity of the antibody were retained despite having the same charge pairing of both the antibody and the antigen. Furthermore, we revealed that the antibody exhibited reversible ligand- and salt concentration-dependent aggregation. Our study demonstrated how supercharging can potentially modulate protein aggregation and LLPS. It is expected that this approach can be extended to other proteins, through which its applicability in various biological and biotechnological fields can be explored. Protein aggregation and liquid‒liquid phase separation (LLPS) orchestrate protein behavior and function. Engineering protein surface charge offers a robust approach to modulating these phenomena, and supercharging, which replaces surface residues with charged ones, leads to a drastic change in the protein net charge. In this study, we designed a new supercharged antigen-binding fragment antibody mutant and investigated its aggregation behavior. We revealed that the antibody exhibited reversible ligand- and salt concentration-dependent aggregation while retaining the physicochemical properties. Our study demonstrated how supercharging can potentially modulate protein aggregation and LLPS.","PeriodicalId":20302,"journal":{"name":"Polymer Journal","volume":"57 8","pages":"923-930"},"PeriodicalIF":2.7,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41428-025-01046-4.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774183","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Polymer-engineered condensates for enzyme activation 用于酶活化的聚合物工程凝聚物
IF 2.7 4区 化学
Polymer Journal Pub Date : 2025-04-25 DOI: 10.1038/s41428-025-01042-8
Tomoto Ura, Toya Yoshida, Tsutomu Mikawa, Kentaro Shiraki
{"title":"Polymer-engineered condensates for enzyme activation","authors":"Tomoto Ura, Toya Yoshida, Tsutomu Mikawa, Kentaro Shiraki","doi":"10.1038/s41428-025-01042-8","DOIUrl":"10.1038/s41428-025-01042-8","url":null,"abstract":"Enzyme condensates are powerful tools for controlling enzymatic reactions in living cells. Recent advances in polymer science have enabled the design of artificial enzyme condensates in vitro, providing a promising approach to enhance enzymatic activity and stability for various biotechnological applications. In this review, we describe a systematic approach to engineering enzyme condensates through polymer-based strategies. First, we consider the design principles for tailoring the state of the enzyme condensates using charged polymers, including approaches that utilize enzymes as scaffolds or clients, and compare these condensates with other enzyme activation methods, highlighting the advantages and potential limitations of enzyme condensates. Second, we review the major factors that affect enzyme performance within the condensates, including size-dependent effects and local environmental changes. These data are supported by recent mechanistic studies using various enzyme systems, including oxidoreductases. Finally, we focus on possible applications and outline the key challenges in expanding the utility of enzyme condensates from single-enzyme to multienzyme systems and from solution-based to surface-bound architectures. Our comprehensive overview of enzyme condensate engineering provides a new perspective to bridge cellular organization principles and innovations in enzyme catalysis. This review highlights recent advances in engineering artificial enzyme condensates in vitro using charged polymers. Based on our recent findings, we describe strategies for designing condensates through interactions between polymers and enzymes or coenzymes. We then summarize enzyme activation mechanisms triggered by enzyme condensates, including size-dependent effects and conformational changes in enzymes. We also discuss potential applications and future directions, including multienzyme systems, integration with solid surfaces, and combination with rational enzyme design.","PeriodicalId":20302,"journal":{"name":"Polymer Journal","volume":"57 8","pages":"885-896"},"PeriodicalIF":2.7,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41428-025-01042-8.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774168","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Oxidation-responsive coacervates composed of oligo(ethylene glycol) bearing benzyl sulfide groups 含苯硫醚基团的低聚乙二醇组成的氧化反应性凝聚体
IF 2.7 4区 化学
Polymer Journal Pub Date : 2025-04-25 DOI: 10.1038/s41428-025-01038-4
Ryutaro Fujimoto, Sayuri L. Higashi, Yuki Shintani, Koichiro M. Hirosawa, Kenichi G. N. Suzuki, Masato Ikeda
{"title":"Oxidation-responsive coacervates composed of oligo(ethylene glycol) bearing benzyl sulfide groups","authors":"Ryutaro Fujimoto, Sayuri L. Higashi, Yuki Shintani, Koichiro M. Hirosawa, Kenichi G. N. Suzuki, Masato Ikeda","doi":"10.1038/s41428-025-01038-4","DOIUrl":"10.1038/s41428-025-01038-4","url":null,"abstract":"Herein, we describe the construction of coacervates composed of an oligo(ethylene glycol) derivative bearing benzyl sulfide groups. The obtained liquid-like coacervates (droplets) can undergo oxidation-responsive disassembly through the conversion of the sulfide groups to the sulfoxide groups. Moreover, the coacervates selectively encapsulate hydrophobic molecules; therefore, oxidation-responsive disassembly can lead to the controlled release of the encapsulated molecules. The construction of coacervates composed of an oligo(ethylene glycol) derivative bearing benzyl sulfide groups is presented. The obtained liquid-like coacervates (droplets) can undergo oxidation-responsive disassembly through the conversion of the sulfide groups to the sulfoxide groups. Moreover, the coacervates selectively encapsulate hydrophobic molecules; therefore, oxidation-responsive disassembly can lead to the controlled release of the encapsulated molecules.","PeriodicalId":20302,"journal":{"name":"Polymer Journal","volume":"57 8","pages":"941-947"},"PeriodicalIF":2.7,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41428-025-01038-4.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774182","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Durable dual-repellent coatings with anti-fouling and anti-icing performance 耐久的双驱涂层,具有防污和防冰性能
IF 2.7 4区 化学
Polymer Journal Pub Date : 2025-04-25 DOI: 10.1038/s41428-025-01034-8
Shuyang Xing, Xin Wang, Wei Kuang, Xinyu Wang, Huilin Tian, Jianhan Huang, Ruiyi Luo
{"title":"Durable dual-repellent coatings with anti-fouling and anti-icing performance","authors":"Shuyang Xing, Xin Wang, Wei Kuang, Xinyu Wang, Huilin Tian, Jianhan Huang, Ruiyi Luo","doi":"10.1038/s41428-025-01034-8","DOIUrl":"10.1038/s41428-025-01034-8","url":null,"abstract":"The development of environmentally sustainable preparation methods is crucial for developing coatings that combine high mechanical strength with superior antifouling properties. Herein, a dual-repellent coating (PKF-SiO2) was fabricated through an epoxy ring-opening reaction in an aqueous environment using γ-glycidoxypropyltrimethoxysilane (KH560), nanosilica (SiO2), and 1H,1H,2H,2H-perfluorodecyltrimethoxysilane (PFAS) as raw materials. The resulting PKF-SiO2 coating exhibited exceptional mechanical robustness and antifouling properties. Remarkably, liquids such as n-hexadecane, soybean oil, and glycerin showed no adhesion to the coating surface even after being subjected to 1000 cycles of friction or bending tests. Anti-icing evaluations further demonstrated that the ice adhesion pressure on the PKF-SiO2 coating was reduced to 17 kPa, whereas the freezing time of the water droplets was extended to 1167 s, representing a 9-min delay compared with that of the bare substrate. These findings underscore the promising potential of the PKF-SiO2 coating for enhancing antifouling and self-cleaning protection in diverse fields, such as textiles and construction. γ-glycidoxypropyltrimethoxysilane was used as a bridge between hydrophobic particles and polyurethane to prepare dual-repellent coating in aqueous environment. This coating demonstrates superior mechanical strength, antifouling properties, and self-cleaning capabilities. In comparison to the uncoated substrate, the amphiphobic coating exhibited a 9-minute delay in freezing time and a reduced adhesion strength of 17 kPa. These results highlight the promising potential of the PKF-SiO2 coating for enhancing antifouling and self-cleaning functionalities in various applications, including textiles and construction","PeriodicalId":20302,"journal":{"name":"Polymer Journal","volume":"57 9","pages":"1003-1013"},"PeriodicalIF":2.7,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144990813","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Liquid‒liquid phase separation of spider silk proteins 蜘蛛丝蛋白的液-液相分离
IF 2.7 4区 化学
Polymer Journal Pub Date : 2025-04-24 DOI: 10.1038/s41428-025-01039-3
Lisa Zeußel, Hendrik Bargel, Gregory P. Holland, Thomas Scheibel
{"title":"Liquid‒liquid phase separation of spider silk proteins","authors":"Lisa Zeußel, Hendrik Bargel, Gregory P. Holland, Thomas Scheibel","doi":"10.1038/s41428-025-01039-3","DOIUrl":"10.1038/s41428-025-01039-3","url":null,"abstract":"Liquid‒liquid phase separation (LLPS) is a phenomenon relevant in the multicomponent settings of many biological processes, including compartmentation, pathological conditions such as Alzheimer’s disease, and protein assembly. LLPS also plays a key role in spider silk fiber formation. Many spider silk fibers display properties such as elasticity in combination with high mechanical strength, which result in an outstanding toughness exceeding that of steel or Kevlar. A thorough understanding of the natural silk spinning process is thus vital for translation to artificial spinning techniques to achieve biomimetic fibers with properties superior to those of other fibrous materials. This focus review summarizes the milestones of research on spider silk assembly, starting from two initial theories, i.e., the liquid crystal theory and the micelle theory, followed by evidence for the importance of LLPS in this process. Ex vivo studies and experiments utilizing recombinant spider silk proteins have highlighted the importance of LLPS during spider silk assembly. Here, we provide a consolidated view of the previously separate theories as a concerted, transitional concept, and describe practical implications showcasing the importance of this unifying concept for technical silk spinning. The process of spider silk assembly is a concerted, transitional process that combines liquid‒liquid phase separation (LLPS), liquid‒crystal (LC) and liquid‒solid phase separation (LSP), yielding fibers with outstanding mechanical properties. Spider silk proteins form micelle-like assemblies that undergo LLPS to form larger droplets, which are highly relevant for preorientation and permit intra- and intermolecular interactions, leading to a dimerized protein network and a nematic crystal phase of β-sheet-rich nanofibrils. The final solid fiber is drawn via LSP.","PeriodicalId":20302,"journal":{"name":"Polymer Journal","volume":"57 8","pages":"831-843"},"PeriodicalIF":2.7,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.com/articles/s41428-025-01039-3.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144774170","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Effects of β-Cyclodextrin Introduced by Different Methods on the Immobilized Phenol-Degrading Bacteria in Photocrosslinked Spherical Hydrogels 不同方法引入β-环糊精对光交联球形水凝胶中固定化酚降解菌的影响
IF 2.7 4区 化学
Polymer Journal Pub Date : 2025-04-23 DOI: 10.1038/s41428-025-01032-w
Hirohito Yamasaki, Yasu-yuki Nagasawa, Narumi Uchida, Taiji Ito, Kimitoshi Fukunaga
{"title":"Effects of β-Cyclodextrin Introduced by Different Methods on the Immobilized Phenol-Degrading Bacteria in Photocrosslinked Spherical Hydrogels","authors":"Hirohito Yamasaki, Yasu-yuki Nagasawa, Narumi Uchida, Taiji Ito, Kimitoshi Fukunaga","doi":"10.1038/s41428-025-01032-w","DOIUrl":"10.1038/s41428-025-01032-w","url":null,"abstract":"In this study, we developed two types of lattice-type β-cyclodextrin (β-CyD)-containing spherical hydrogels to immobilize phenol (PhOH)-degrading bacteria. One type, ENTG-mix-βCyD/HDI, consists of mixed-type spherical hydrogels containing β-CyD ring-bearing polymer microparticles embedded within the gel matrix. The other type, ENTG-co-PSβCyD, consists of copolymerized spherical hydrogels in which β-CyD-substituted monomers are copolymerized and crosslinked. The former features an aggregated distribution of β-CyD rings, whereas the latter exhibits a uniform distribution. Continuous PhOH degradation experiments revealed that both of the β-CyD-containing spherical hydrogel catalysts exhibited catalytic activity exceeding that of the ENTG spherical catalyst without β-CyD. Immobilized bacteria were distributed both on the surface and within the structure of the copolymerized carrier, whereas in the mixed carrier, many bacteria were dispersed throughout. Analysis of the PhOH-degrading flora revealed that Pseudomonas putida formed a niche in the copolymerized hydrogels, whereas Sphingomonas sp. formed a niche in the mixed hydrogels. Batch experiments using p-xylene instead of PhOH demonstrated that the degradation rates of the copolymerized and mixed gels were 2.4 times and 1.6 times greater than that of the ENTG gel, respectively. The copolymerized gel exhibited a faster p-xylene degradation rate due to the reactivity of P. putida. Continuous phenol (PhOH) decomposition experiments were carried out with PhOH-degrading bacteria immobilized in a copolymerized spherical hydrogel (ENTG-co-PSβCyD) and a mixed spherical hydrogel (ENTG-mix-βCyD/HDI). Similar to the results obtained from the batch PhOH degradation experiments, both β-CyD-containing spherical hydrogels, which feature cylindrical hydrophobic intramolecular spaces, exhibited higher activity than the ENTG spherical hydrogels lacking β-CyD. The bacterial cells were extensively distributed on the surface and inside the copolymerized carrier and throughout the entire mixed carrier, while only a small amount of bacteria were found on the surface of the ENTG carrier. Furthermore, the PhOH-degrading bacterial flora (microflora) in the copolymerized and mixed spherical gel matrices were identified. Pseudomonas putida formed a niche in the copolymerized spherical hydrogel, and Sphingomonas sp. formed a niche in the mixed hydrogel. In the continuous PhOH degradation experiment, the performance of both hydrogels was almost identical because the ability of both strains to degrade PhOH is similar. However, in the batch removal experiment using p-xylene as the substrate instead of PhOH, the rates of substrate removal by the copolymerized gel and mixed gel 2.4 times and 1.6 times greater than that of the ENTG gel, respectively. This occurred because the bacterial species in the mixed gel was Sphingomonas sp. instead of P. putida, and the high substrate removal by the copolymerized gel was a result of the high r","PeriodicalId":20302,"journal":{"name":"Polymer Journal","volume":"57 9","pages":"949-958"},"PeriodicalIF":2.7,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144990844","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
0
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
相关产品
×
本文献相关产品
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术官方微信