ChemSystemsChem最新文献_第4页

Spatially Coded Transformations in Gradient-Dependent Protocell Morphogenesis 梯度依赖的原始细胞形态发生中的空间编码转换

IF 3.1

ChemSystemsChem Pub Date : 2024-10-22 DOI: 10.1002/syst.202400064

Shuqi Wu, Wei Ji, Mei Li, Stephen Mann, Liangfei Tian

{"title":"Spatially Coded Transformations in Gradient-Dependent Protocell Morphogenesis","authors":"Shuqi Wu, Wei Ji, Mei Li, Stephen Mann, Liangfei Tian","doi":"10.1002/syst.202400064","DOIUrl":"10.1002/syst.202400064","url":null,"abstract":"Chemical gradients provide spatiotemporal signaling fields in various cellular processes, driving complex dynamic behaviours such as differentiation and spatial organization. Here we employ opposing gradients of two artificial morphogens (sodium dodecyl sulfate (SDS) and sodium phosphotungstate (polyoxometalate; POM)) to systematically investigate morphological differentiation in organized populations of coacervate microdroplet-based protocells. Using a matrix of 16 sets of counter-diffusive gradients, we classify the differentiated protocells into five phenotypes and encode their spontaneous organization into different spatially patterned protocell consortia using a 3-bit binary information system. We show that a predominant SDS gradient produces a diversity of differentiated phenotypes to generate complex spatially coded 2D protocell organizations. In contrast, a prevailing POM gradient decreases morphological differentiation, resulting in population homogenization. Our results improve our understanding of gradient concentration-dependent collective responses in synthetic microscale agents and provide a step to a new spatially resolved information encoding method with 3-bit binary outputs.","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"7 1","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143118057","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

The Role of Kinetic Asymmetry in Chemical and Thermodynamic Coupling 动力学不对称在化学和热力学耦合中的作用

IF 3.1

ChemSystemsChem Pub Date : 2024-10-15 DOI: 10.1002/syst.202400066

R. Dean Astumian

引用次数: 0

A Pseudo-catalytic Network Motif for Thiol-based Chemical Reaction Networks 巯基化学反应网络的伪催化网络基序

IF 3.1

ChemSystemsChem Pub Date : 2024-10-14 DOI: 10.1002/syst.202400072

Ekaterina A. Zhigileva, Ilia A. Puchkin, Sergey N. Semenov

{"title":"A Pseudo-catalytic Network Motif for Thiol-based Chemical Reaction Networks","authors":"Ekaterina A. Zhigileva, Ilia A. Puchkin, Sergey N. Semenov","doi":"10.1002/syst.202400072","DOIUrl":"10.1002/syst.202400072","url":null,"abstract":"The construction of chemical reaction networks (CRNs) is a formidable challenge because of their holistic and nonlinear nature. One approach to constructing CRNs involves combining fragments with distinctive properties, known as network motifs. Thiol chemistry is widely used in the construction of CRNs, with motifs available for positive and negative feedback loops. However, a simple catalytic motif has been lacking. Here, we developed a pseudo-catalytic motif using the reaction between cystamine and organic thiocyanates, which operates through a nucleophilic chain mechanism. Although similar to thiol autocatalytic systems, this reaction does not involve a doubling of the number of thiol species at any stage. The reaction is high-yielding and produces 2-amino-2-thiazoline. Its pseudo-catalytic nature manifests itself in the nearly linear relationship between the reaction rate and the amount of free thiols added at the beginning of the reaction. We demonstrated that this reaction can be regulated by external, time-dependent thiol signals and integrated into larger CRNs. We believe that this system will be a valuable addition to thiol chemistry, enabling the construction of CRNs with interesting functionalities.","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"7 2","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/syst.202400072","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143629916","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

Non-Uniform Electric Field Manipulation of Chromogenic Peptide Amphiphile Assemblies 非均匀电场操纵显色肽两亲体组装

IF 3.1

ChemSystemsChem Pub Date : 2024-10-09 DOI: 10.1002/syst.202400061

Kiara L. Lacy, Sujeung Lim, Emil M. Lundqvist, Yuyao Kuang, Harrison C. Jeong, Tayloria N. G. Adams, Herdeline Ann M. Ardoña

{"title":"Non-Uniform Electric Field Manipulation of Chromogenic Peptide Amphiphile Assemblies","authors":"Kiara L. Lacy, Sujeung Lim, Emil M. Lundqvist, Yuyao Kuang, Harrison C. Jeong, Tayloria N. G. Adams, Herdeline Ann M. Ardoña","doi":"10.1002/syst.202400061","DOIUrl":"10.1002/syst.202400061","url":null,"abstract":"This work investigates the influence of dielectrophoretic forces on the structural features and the resulting aggregates of a chromogenic model system, peptide-diacetylene (D3GV-DA) amphiphiles. Here, we systematically investigate how non-uniform electric fields impact the (i) peptide-directed supramolecular assembly stage and (ii) topochemical photopolymerization stage of polydiacetylenes (PDAs) in a quadrupole-based dielectrophoresis (DEP) device, as well as the (iii) manipulation of D3GV-DA aggregates in a light-induced DEP (LiDEP) platform. The conformation-dependent chromatic phases of peptide-PDAs are utilized to probe the chain-level effect of DEP exposure after the supramolecular assembly or after the topochemical photopolymerization stage. Steady-state spectroscopic and microscopy analyses show that structural features such as the chirality and morphologies of peptidic 1-D nanostructures are mostly conserved upon DEP exposure, but applying mild, non-uniform fields at the self-assembly stage is sufficient for fine-tuning the chromatic phase ratio in peptide-PDAs and manipulating their aggregates via LiDEP. Overall, this work provides insights into how non-uniform electric fields offer a controllable approach to fine-tune or preserve the molecularly preset assembly order of DEP-responsive supramolecular or biopolymeric assemblies, as well as manipulate their aggregates using light projections, which have future implications for the precision fabrication of macromolecular systems with hierarchical structure-dependent function.","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"7 3","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/syst.202400061","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144091247","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

Charge-Mediated Interactions Affect Enzymatic Reactions in Peptide Condensates 电荷介导的相互作用影响肽凝聚物中的酶反应

IF 3.1

ChemSystemsChem Pub Date : 2024-10-04 DOI: 10.1002/syst.202400055

Rif Harris, Nofar Berman, Ayala Lampel

{"title":"Charge-Mediated Interactions Affect Enzymatic Reactions in Peptide Condensates","authors":"Rif Harris, Nofar Berman, Ayala Lampel","doi":"10.1002/syst.202400055","DOIUrl":"10.1002/syst.202400055","url":null,"abstract":"Biomolecular condensates, formed through liquid-liquid phase separation (LLPS), serve as enzymatic reaction centers in cells by increasing local concentrations of enzymes and substrates, thereby facilitating reaction kinetics and regulatory mechanisms. Inspired by these natural systems, synthetic condensates are being developed for diverse applications, including payload delivery, sensing, and as microreactors where enzymatic reaction kinetics can be modulated by factors like pH, viscosity, and enzyme-substrate co-localization. Here, we investigate how the physicochemical properties of enzymes and substrates influence condensate formation and function as microreactors. Focusing on cellulase and alkaline phosphatase, which differ in molecular weight and isoelectric point, we employed a minimalistic complex coacervation system of oppositely charged LLPS-promoting peptides. Our findings show how electrostatic forces within condensates influence their role as microreactors. Specifically, the ability of condensates to encapsulate or exclude phosphatase, cellulase, and their substrates, which is pivotal for the regulation of reaction kinetics, is determined by the enzyme surface charge, substrate charge, and condensate charge stoichiometry. These results highlight the potential of utilizing electrostatic forces within condensates to modulate enzymatic reactions, providing critical insights for developing synthetic condensates as microreactors in biotechnology and materials science.","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"7 1","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/syst.202400055","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143111993","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

Empowering Chemical AI Through Systems Chemistry 通过系统化学提高化学人工智能的能力

IF 3.1

ChemSystemsChem Pub Date : 2024-09-19 DOI: 10.1002/syst.202400054

Prof. Pier Luigi Gentili, Prof. Pasquale Stano

引用次数: 0

Prebiotic Environmental Conditions Impact the Type of Iron-Sulfur Cluster Formed 益生元环境条件对铁硫团簇形成类型的影响

IF 3.1

ChemSystemsChem Pub Date : 2024-09-18 DOI: 10.1002/syst.202400051

Luca Valer, Yin Juan Hu, Alberto Cini, Marco Lantieri, Craig R. Walton, Oliver Shorttle, Maria Fittipaldi, Sheref S. Mansy

{"title":"Prebiotic Environmental Conditions Impact the Type of Iron-Sulfur Cluster Formed","authors":"Luca Valer, Yin Juan Hu, Alberto Cini, Marco Lantieri, Craig R. Walton, Oliver Shorttle, Maria Fittipaldi, Sheref S. Mansy","doi":"10.1002/syst.202400051","DOIUrl":"10.1002/syst.202400051","url":null,"abstract":"Iron-sulfur clusters are ancient cofactors that could have played a role in the prebiotic chemistry leading to the emergence of protometabolism. Previous research has shown that certain iron-sulfur clusters can form from prebiotically plausible components, such as cysteine-containing oligopeptides. However, it is unclear if these iron-sulfur clusters could have survived in prebiotically plausible environments. To begin exploring this possibility, we tested the stability of iron-sulfur clusters coordinated to a tripeptide and to N-acetyl-L-cysteine methyl ester in a variety of solutions meant to mimic prebiotically plausible environments. We also assessed the impact of individual chemical components on stability. We find that iron-sulfur clusters form over a wide variety of conditions but that the type of iron-sulfur cluster formed is strongly impacted by the chemical environment and the coordinating scaffold. These findings support the general hypothesis that iron-sulfur clusters were present on the prebiotic Earth and that different types of iron-sulfur cluster predominated in different environments.","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"7 1","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/syst.202400051","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143116266","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

Front Cover: Effect of Temperature on Calcium-Based Chemical Garden Growth (ChemSystemsChem 5/2024) 封面：温度对钙基化学花园生长的影响（ChemSystemsChem 5/2024）

IF 3.1

ChemSystemsChem Pub Date : 2024-09-13 DOI: 10.1002/syst.202480501

Dr. Pamela Knoll, Dr. Corentin C. Loron

引用次数: 0

Oscillations of the Local pH Reverses Silver Micromotors in H2O2 局部 pH 值的振荡可逆转 H2O2 中的银微电机

IF 3.1

ChemSystemsChem Pub Date : 2024-09-09 DOI: 10.1002/syst.202400046

Xianghong Liu, Yixin Peng, Zuyao Yan, Dezhou Cao, Shifang Duan, Wei Wang

{"title":"Oscillations of the Local pH Reverses Silver Micromotors in H2O2","authors":"Xianghong Liu, Yixin Peng, Zuyao Yan, Dezhou Cao, Shifang Duan, Wei Wang","doi":"10.1002/syst.202400046","DOIUrl":"10.1002/syst.202400046","url":null,"abstract":"Asymmetric chemical reactions on the surfaces of colloidal particles are known to propel them into directional motion. The dynamics of such chemical micromotors are sensitive to their local chemical environments, which also continually evolve with the reactions on motor surfaces. This two-way coupling between the motor dynamics and the local environment may result in complex nonlinear behaviors. As an example, we report that Janus Ag microspheres, which self-propel in hydrogen peroxide (H2O2), spontaneously reverse their direction of motion two or more times. We hypothesize that two distinct chemical reactions between Ag and H2O2 drive the micromotor in opposite directions, and which reaction dominates depends on the local pH. Interestingly, the local pH near a Ag micromotor oscillates spontaneously in H2O2, likely due to a complex interplay between the kinetics of the reaction between Ag and H2O2 and the diffusion of chemical species. Consequently, the pH-sensitive Ag micromotor reverses its direction of motion in response to these pH oscillations. This study introduces a new mechanism for regulating the speed and directionality of micromotors, highlights the potential of Ag micromotors in chemical sensing, and sheds new light on the interplay between chemical kinetics and micromotor dynamics.","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"6 6","pages":""},"PeriodicalIF":3.1,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142665742","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

Transport-Limited Growth of Flow-Driven Rare-Earth Silicate Tubes 流动驱动的稀土硅酸盐管的传输限制生长

IF 3.1

ChemSystemsChem Pub Date : 2024-09-04 DOI: 10.1002/syst.202400053

Panna E. Farkas, Emese Lantos, Dezső Horváth, Agota Tóth

引用次数: 0