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Investigating Impacts of Amino Acids on the Structural Stability of Anionic Biomembranes 研究氨基酸对阴离子生物膜结构稳定性的影响
IF 3.1
ChemSystemsChem Pub Date : 2025-01-08 DOI: 10.1002/syst.202400065
Arslan Siddique, Lauren A. Lowe, Soumya Kanti De, Daniel W. K. Loo, Anton P. Le Brun, Andrew R. J. Nelson, Anna Wang
{"title":"Investigating Impacts of Amino Acids on the Structural Stability of Anionic Biomembranes","authors":"Arslan Siddique,&nbsp;Lauren A. Lowe,&nbsp;Soumya Kanti De,&nbsp;Daniel W. K. Loo,&nbsp;Anton P. Le Brun,&nbsp;Andrew R. J. Nelson,&nbsp;Anna Wang","doi":"10.1002/syst.202400065","DOIUrl":"10.1002/syst.202400065","url":null,"abstract":"<p>Anionic biomembranes are vital features of all living cells and were perhaps key components of the earliest cell-like structures – protocells. In the absence of evolved protein machinery, any protocell membranes would have had their properties heavily influenced by the ambient environment, posing a systems chemistry challenge to understanding how such membranes functioned. Here we use a range of techniques to examine the effect of glycine and lysine, representative neutral and cationic amino acids, on the properties of model anionic membranes composed of equimolar POPC and POPG. Using QCM−D and neutron reflectometry, we find that unlike glycine, lysine strongly binds to the membrane, resulting in significant lipid loss and changes in the scattering length density and volume fraction of the lipids in the bilayer. Interestingly, we also find that even though lysine causes substantial changes in the physicochemical and structural properties of the anionic membrane, permeability studies show that lysine cannot permeate while glycine can, highlighting a disconnect between the structural changes observed for low curvature systems and the permeability trends observed in high curvature systems. This research provides mechanistic insights into single amino acid-anionic biomembrane interactions, and how they could have impacted evolving protocell membrane functions and stability.</p>","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"7 2","pages":""},"PeriodicalIF":3.1,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/syst.202400065","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143629798","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Aqueous Synthesis of Membrane Lipids via Amide Formation between Amphiphilic Amines and Thioacids 两亲胺和硫酸之间形成酰胺的膜脂水合成
IF 3.1
ChemSystemsChem Pub Date : 2024-12-29 DOI: 10.1002/syst.202400077
Jiyue Chen, Dr. Lalita Tanwar, Dr. Peng Ji, Prof. Roberto J. Brea, Prof. Neal K. Devaraj
{"title":"Aqueous Synthesis of Membrane Lipids via Amide Formation between Amphiphilic Amines and Thioacids","authors":"Jiyue Chen,&nbsp;Dr. Lalita Tanwar,&nbsp;Dr. Peng Ji,&nbsp;Prof. Roberto J. Brea,&nbsp;Prof. Neal K. Devaraj","doi":"10.1002/syst.202400077","DOIUrl":"10.1002/syst.202400077","url":null,"abstract":"<p>Protocell membranes were likely formed through primitive metabolic reactions that synthesized more complex membrane lipid species from simpler precursors. Thioacids have been shown to be prebiotically plausible and chemoselective <i>N</i>-acylating reagents. They have been successfully employed for the acylation of peptides and RNA. However, the ability of thioacids to acylate lipid species has not yet been explored. Here, we demonstrate <i>N</i>-acylation of natural amine-containing amphiphiles using fatty thioacids. This reaction occurs spontaneously in aqueous conditions and is chemoselective,and traceless. The synthesis of several natural sphingolipids via direct <i>N</i>-acylation is possible and their subsequent de novo formation into vesicular membranes is shown. Aqueous thioacid coupling provides a route for generating membrane-forming lipids in the context of protocells and for the in situ synthesis of relevant sphingolipid species.</p>","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"7 3","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-12-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144091615","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Coacervate-Droplet Cased Synthetic Cells Regulated By Activated Carboxylic Acids (ACAs) 活化羧酸(ACAs)调控的凝聚体-液滴壳状合成细胞
IF 3.1
ChemSystemsChem Pub Date : 2024-11-27 DOI: 10.1002/syst.202400083
Matteo Valentini, Stefano Di Stefano, Job Boekhoven
{"title":"Coacervate-Droplet Cased Synthetic Cells Regulated By Activated Carboxylic Acids (ACAs)","authors":"Matteo Valentini,&nbsp;Stefano Di Stefano,&nbsp;Job Boekhoven","doi":"10.1002/syst.202400083","DOIUrl":"10.1002/syst.202400083","url":null,"abstract":"<p>Regulating the formation and dissolution of active complex coacervate droplets with chemical reactions offers a powerful synthetic cell model. Such active droplets are also helpful in understanding the non-equilibrium nature of membrane-less organelles. Like many membrane-less organelles, these droplets rely on high-chemical potential reagents, like ATP, to maintain their transient nature. This study explores Activated Carboxylic Acids (ACAs) as a high-chemical potential fuel to modulate the lifetime of peptide-based coacervates through transient pH changes. We demonstrate that nitroacetic acid, a commonly used ACA, can effectively induce the formation and dissolution of coacervates by transiently altering the solution′s pH. The system, comprising the zwitterionic peptide Ac-FRGRGD-OH and polyanions, forms coacervates upon protonation at low pH and dissolves as the pH returns to neutral. Our findings indicate that the lifetime of these synthetic cells can be fine-tuned by varying the amount of ACA added, and the system can be refueled multiple times without significant interference from by-products. This ACA-driven reaction cycle is versatile, accommodating various coacervate compositions and enabling the uptake of diverse compounds, making it a valuable model for compartmentalization. The study underscores the potential of ACA-fueled coacervates as a platform for investigating biomolecular condensates and developing synthetic life systems.</p>","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"7 3","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-11-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/syst.202400083","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144091791","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Spatial Shifting of Biocondensate Assembly Zone in a Microfluidic Gradient of Dissipative Condition 耗散条件下微流体梯度下生物凝析液聚集区的空间移动
IF 3.1
ChemSystemsChem Pub Date : 2024-11-26 DOI: 10.1002/syst.202400084
Sakshi Juneja, Neetu Sivoria, Subhabrata Maiti
{"title":"Spatial Shifting of Biocondensate Assembly Zone in a Microfluidic Gradient of Dissipative Condition","authors":"Sakshi Juneja,&nbsp;Neetu Sivoria,&nbsp;Subhabrata Maiti","doi":"10.1002/syst.202400084","DOIUrl":"10.1002/syst.202400084","url":null,"abstract":"<p>Pursuing non-equilibrium chemistry with (bio)molecules is of utmost importance for the design of life-like dynamic materials that emerge in a constant flux of energy. Herein, we explore spatial localization of dissipative self-assembly of biocondensate (DNA-histone) via passing chemical fuel (histone) and one fuel-degrading agent (trypsin) through two arms of the Y-shaped microfluidic chip. In this case, a continuous supply of fuel and fuel-degrading agent results self-assembly of biocondensate, maintaining a non-equilibrium steady state (NESS). We find in the presence of gradient of dissipating conditions, the formation zone of biocondensate drifts towards fuel-rich zone (away from dissipating zone). In absence of fuel-degrading agent, diffusive transport of free DNA towards histone channel (perpendicular to advection) is restricted as it formed much larger micron-sized biocondensate at the center of the channel (the meeting point of two flows). However, this sidewise DNA diffusion is operative in the presence of fuel-degrading agent and therefore, the formation zone shifted to histone-rich zone. Furthermore, we demonstrate that in the presence of trypsin, catalytic DNA's peroxidase reactivity can be moved to histone-rich region. Transposition of self-assembly process in a gradient of dissipative conditions will be of importance in the development of spatially-controlled chemistry, reaction-diffusion processes.</p>","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"7 3","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144091667","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Easy, Rapid and High-Throughput Production of Single and Multicompartment Liposomes by Vortex Emulsification 漩涡乳化法简便、快速、高通量生产单室和多室脂质体
IF 3.1
ChemSystemsChem Pub Date : 2024-11-25 DOI: 10.1002/syst.202400085
Zhen-Hong Luo, Gong-Yu Shi, Nan-Nan Deng
{"title":"Easy, Rapid and High-Throughput Production of Single and Multicompartment Liposomes by Vortex Emulsification","authors":"Zhen-Hong Luo,&nbsp;Gong-Yu Shi,&nbsp;Nan-Nan Deng","doi":"10.1002/syst.202400085","DOIUrl":"10.1002/syst.202400085","url":null,"abstract":"<p>Cell-sized liposomes, the self-assembled phospholipid vesicles with bilayer membranes, have garnered substantial attention across various fields, particularly as cell mimics. In this study, we introduce a simplified method for rapidly producing single- and multicompartment liposomes using a common laboratory vortex mixer. The simplicity of our method has the potential to greatly facilitate artificial cell and tissue-related research, potentially leading to broader applications of liposomes.</p>","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"7 3","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144091799","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Front Cover: Photostimuli Reach a Selective Intermediate in a Microflow: One-Shot Transformation from a Supramolecular Co-Polymer to a Micro-Disk Structure (ChemSystemsChem 6/2024) 封面光刺激到达微流中的选择性中间体:从超分子共聚物到微盘结构的一次性转化(ChemSystemsChem 6/2024)
IF 3.1
ChemSystemsChem Pub Date : 2024-11-16 DOI: 10.1002/syst.202480601
Akira Kaneyoshi, Shota Nomura, Takato Maeda, Dr. Takahiro Kusukawa, Dr. Yoshihiro Kikkawa, Dr. Munenori Numata
{"title":"Front Cover: Photostimuli Reach a Selective Intermediate in a Microflow: One-Shot Transformation from a Supramolecular Co-Polymer to a Micro-Disk Structure (ChemSystemsChem 6/2024)","authors":"Akira Kaneyoshi,&nbsp;Shota Nomura,&nbsp;Takato Maeda,&nbsp;Dr. Takahiro Kusukawa,&nbsp;Dr. Yoshihiro Kikkawa,&nbsp;Dr. Munenori Numata","doi":"10.1002/syst.202480601","DOIUrl":"10.1002/syst.202480601","url":null,"abstract":"<p>In the Research Article by Munenori Numata and co-workers a <b>dissipative self-assembly system</b> powered by flow and light is demonstrated. Supramolecular co-polymerization and rolling-up from the forward polymer's end led to the creation of discrete micrometer-sized supramolecular architecture featuring both molecular-level inner complexity and long-range order over molecular scale.\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"6 6","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/syst.202480601","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665971","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Interfacing Complex Coacervates with Natural Cells 复杂凝聚体与天然细胞的接合
IF 3.1
ChemSystemsChem Pub Date : 2024-11-15 DOI: 10.1002/syst.202400071
He Meng, Yanglimin Ji, Yan Qiao
{"title":"Interfacing Complex Coacervates with Natural Cells","authors":"He Meng,&nbsp;Yanglimin Ji,&nbsp;Yan Qiao","doi":"10.1002/syst.202400071","DOIUrl":"10.1002/syst.202400071","url":null,"abstract":"<p>Coacervates have been investigated as protocells or synthetic cells, as well as subcellular compartments for the creation of new materials, thus bridging the gap between living and non-living systems in materials science, synthetic biology, and bioengineering. Given the design flexibility and simplicity of coacervates, along with the functionality and complexity of natural cells, the interfacing of complex coacervates with natural cells is considered significant for various biotechnological and biomedical applications. In this review, the fundamental mechanisms and underlying theories of coacervate systems are introduced. Recent efforts to interface coacervates with natural cells are summarized in three key scenarios: (i) the integration of coacervates with natural cell components for the living material assembly into protocells; (ii) communication between therapeutic synthetic cells and natural cells for drug delivery and cell repair; and (iii) the formation of intracellular condensates for metabolic regulation, followed by the regulation of their phase transitions for pathological elucidation. Finally, the potential of coacervate-natural cell interfaces is discussed in the context of developing living/synthetic cell constructs, creating precise disease therapy strategies, and advancing programmable metabolic engineering networks.</p>","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"7 2","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143629847","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Designing and Controlling Transient Supramolecular Gels 瞬态超分子凝胶的设计与控制
IF 3.1
ChemSystemsChem Pub Date : 2024-11-05 DOI: 10.1002/syst.202400073
Emma L. Bowley, Simona Bianco, Fin Hallam Stewart, Chloe M. Wallace, Rebecca E. Ginesi, Alex S. Loch, Martin Rosenthal, Andrew J. Smith, Dave J. Adams
{"title":"Designing and Controlling Transient Supramolecular Gels","authors":"Emma L. Bowley,&nbsp;Simona Bianco,&nbsp;Fin Hallam Stewart,&nbsp;Chloe M. Wallace,&nbsp;Rebecca E. Ginesi,&nbsp;Alex S. Loch,&nbsp;Martin Rosenthal,&nbsp;Andrew J. Smith,&nbsp;Dave J. Adams","doi":"10.1002/syst.202400073","DOIUrl":"10.1002/syst.202400073","url":null,"abstract":"<p>Supramolecular systems are often designed such that a steady state exists. However, the ability to design systems with pre-determined changes in state can lead to highly dynamic materials, with evolving supramolecular structures and adaptable material properties. This approach is of great interest from the perspective of designing adaptive systems as well as from a broader systems chemistry perspective. Here, we report how a transient system can be altered to access different mechanical properties and transitions by varying the trigger and temperature. The aging of these systems is also explored, as the networks continually evolve long past the common cut-off point of analysis of one day. We therefore provide new insights into the control of transient gels, as well as an understanding as to the underpinning supramolecular structures and how they evolve with time.</p>","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"7 2","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/syst.202400073","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143629806","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Supramolecular Systems Chemistry Based on the Interplay Between Peptides and Porphyrins 基于多肽和卟啉相互作用的超分子系统化学
IF 3.1
ChemSystemsChem Pub Date : 2024-10-23 DOI: 10.1002/syst.202400068
Yue Fu, Lian Zhang, Xuehai Yan, Kai Liu
{"title":"Supramolecular Systems Chemistry Based on the Interplay Between Peptides and Porphyrins","authors":"Yue Fu,&nbsp;Lian Zhang,&nbsp;Xuehai Yan,&nbsp;Kai Liu","doi":"10.1002/syst.202400068","DOIUrl":"10.1002/syst.202400068","url":null,"abstract":"<p>The functions of living organisms are emergent from networks of biomolecules. In this review, we discuss the creation of synthetic life-like systems based on the interplay of peptides and porphyrins in the supramolecular chemical systems. In particular, we focus on the spatiotemporal control of self-assembly processes, which allows for the development of hierarchical structures for biomimetic catalysis and adaptive dynamics for stimulus-responsive structural transformations. Notably, when operating in a nonequilibrium regime–characterized by kinetic traps, feedback loops, and dissipative conditions–the structural landscape expands and system-level properties emerge, including transient catalysis, metabolic self-replication, and Darwinian-like evolution. Controlling these systems at the biointerface would facilitate intelligent therapeutic interventions in the anti-tumor phototherapy. Supramolecular systems chemistry provides a valuable framework for exploring new physicochemical spaces of peptides and porphyrins, and may offer distinct advantages and extensive applications across diverse fields.</p>","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"7 2","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143629776","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Shape Analysis of Biomimetic and Plasma Membrane Vesicles 仿生囊泡与质膜囊泡的形态分析
IF 3.1
ChemSystemsChem Pub Date : 2024-10-23 DOI: 10.1002/syst.202400052
Rajni Kudawla, Harshmeet Kaur, Tanmay Pandey, Tripta Bhatia
{"title":"Shape Analysis of Biomimetic and Plasma Membrane Vesicles","authors":"Rajni Kudawla,&nbsp;Harshmeet Kaur,&nbsp;Tanmay Pandey,&nbsp;Tripta Bhatia","doi":"10.1002/syst.202400052","DOIUrl":"10.1002/syst.202400052","url":null,"abstract":"<p>Giant membrane vesicles (GUVs) and Giant plasma membrane vesicles (GPMVs) are used as models to study membrane properties. We conducted a comparative study to examine how reducing the volume of vesicles with different lipid compositions, solution symmetries, solution asymmetries, and membrane charges affects their morphology. We used three-dimensional visualization techniques to study the shape of the vesicles. Although the vesicles may not be perfectly spherical, they exhibit some fluctuations in their shape. To understand these variations, we used confocal image stacks for visualization. Our experimental observations show that the membrane′s charge influences the deflation of the GUVs in the presence of trans-bilayer sugar asymmetries. The lipid bilayers of our GUVs have a uniform distribution of lipids in both leaflets, indicating no asymmetry in lipid composition. We induce trans-bilayer asymmetries by exposing each leaflet of the bilayer to different solution compositions. We also estimated and compared the deformation of GPMV extracted from HEK-293 cells with trans-bilayer buffer asymmetries and inherent leaflet compositional asymmetry with biomimetic membranes.</p>","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"7 1","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143118671","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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