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Dissipative Cyclic Reaction Networks: Mechanistic Insights into a Minor Enantiomer Recycling Process 耗散循环反应网络:小对映体回收过程的机理启示
ChemSystemsChem Pub Date : 2023-11-27 DOI: 10.1002/syst.202300045
Dr. Cristiana Margarita, Dr. Anna Laurell Nash, David A. Ahlstrand, Prof. Dr. Mårten S. G. Ahlquist, Prof. Dr. Ola F. Wendt, Dr. Linda Fransson, Prof. Dr. Christina Moberg
{"title":"Dissipative Cyclic Reaction Networks: Mechanistic Insights into a Minor Enantiomer Recycling Process","authors":"Dr. Cristiana Margarita,&nbsp;Dr. Anna Laurell Nash,&nbsp;David A. Ahlstrand,&nbsp;Prof. Dr. Mårten S. G. Ahlquist,&nbsp;Prof. Dr. Ola F. Wendt,&nbsp;Dr. Linda Fransson,&nbsp;Prof. Dr. Christina Moberg","doi":"10.1002/syst.202300045","DOIUrl":"10.1002/syst.202300045","url":null,"abstract":"<p>An analysis of an out-of-equilibrium cyclic reaction network which continuously converts a minor undesired product enantiomer to the desired major enantiomer by irreversible addition of chemical fuel and irreversible elimination of spent fuel is presented. The reaction network is maintained as long as fuel is added; interrupted fuel addition drives the system towards equilibrium, but the cyclic process restarts upon resumed fuel addition, as demonstrated by three consecutive fuel cycles. The process is powered by the hydrolysis of methyl cyanoformate to HCN and monomethyl carbonic acid, which decomposes to CO<sub>2</sub> and MeOH. The time it takes to reach steady state depends on the rate of conversion of the fuel and decreases with increased conversion rate. Three catalysts, one metal catalyst and two enzymes, together constitute an efficient regulation system allowing control of the forward, backward and waste-forming steps, thereby assuring the production of high yields of products with high enantiopurity.</p>","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"6 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-11-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/syst.202300045","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139227990","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
Instructing Liquid-Liquid Phase Separation Inside Membranous Protocells 在膜原生细胞内指导液-液相分离
ChemSystemsChem Pub Date : 2023-11-23 DOI: 10.1002/syst.202300040
Xintao Lv, Jiawei Liu, Peiyong Song, Prof. Li Zhao, Prof. Yiyang Lin
{"title":"Instructing Liquid-Liquid Phase Separation Inside Membranous Protocells","authors":"Xintao Lv,&nbsp;Jiawei Liu,&nbsp;Peiyong Song,&nbsp;Prof. Li Zhao,&nbsp;Prof. Yiyang Lin","doi":"10.1002/syst.202300040","DOIUrl":"10.1002/syst.202300040","url":null,"abstract":"<p>The bottom-up fabrication of compartmentalized cell-like entities represents a promising avenue for reconstituting hierarchical organization within cells and emulating life-like behaviors. Integrating the creation of semipermeable membranes and membraneless artificial organelles has recently garnered significant attention, aiming to achieve cytomimetic properties. We briefly describe the concept of liquid-liquid phase separation and review approaches for the fabrication of cell-sized membranous protocells (e. g., giant unilamellar vesicles, polymersomes and proteinosomes). Three strategies are emphasized for the construction of advanced cell-like structures consisting of liquid-like subcompartments enclosed by a membrane: (i) adsorption and assembly of organic or inorganic species onto the surface of preformed coacervate microdroplets; (ii) interfacial assembly of a lipid or polymer bilayer on the surface of an aqueous pool containing preformed microdroplets; and (ii) triggering phase separation within a preformed semipermeable membrane with chemical or physical stimuli. This review underscores the significance of the hierarchical organization of these synthetic cellular structures in mimicking cytomimetic functions, including transmembrane signaling, protocell communication, prototissue formation, and their compelling biomedical applications.</p>","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"6 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-11-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139242870","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
Emergence of Cell Behavior Through Feedback Control of Polymersome Membrane Transport 通过聚合体膜运输的反馈控制实现细胞行为的产生
ChemSystemsChem Pub Date : 2023-11-17 DOI: 10.1002/syst.202300044
Omar Rifaie-Graham
{"title":"Emergence of Cell Behavior Through Feedback Control of Polymersome Membrane Transport","authors":"Omar Rifaie-Graham","doi":"10.1002/syst.202300044","DOIUrl":"10.1002/syst.202300044","url":null,"abstract":"<p>Artificial cell and organelle construction has recently gained substantial attention to generate simplified models for understanding of biological phenomena, or micro- and nanomachines for biomedical and biotechnological applications. A wide array of building blocks has been employed to build these systems as membraneless structures with the ability to compartmentalize chemical reactions by enhanced partitioning, or as membrane-defined entities that provide a physical barrier that inhibits the interference of external factors. While these systems present unique properties that enable high fidelity to biological processes, they present limited ability to recreate the high selectivity and specificity of small molecule trafficking observed in biological membranes. Owing to their high chemical versatility, polymers can be leveraged to generate 3D structures that resemble biological membranes while providing transmembrane chemical motifs that enable responsiveness to a wide array of stimuli. This Concept Article discusses the ability to control membrane transport facilitating the emergence of out-of-equilibrium feedback mechanisms that ultimately modulate enzymatic rates. This can be employed to engineer future artificial cells and organelles that display homeostasis as a mechanism of self-adaptation to continuously evolving environments.</p>","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"6 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/syst.202300044","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139263899","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
Bidirectional Communication between Droplet Interface Bilayers Driven by Cell-Free Quorum Sensing Gene Circuits 无细胞群体感应基因电路驱动的液滴界面双层双向通信
ChemSystemsChem Pub Date : 2023-10-30 DOI: 10.1002/syst.202300041
Dr. David T. Gonzales, Surased Suraritdechachai, Dr. Christoph Zechner, Dr. T.-Y. Dora Tang
{"title":"Bidirectional Communication between Droplet Interface Bilayers Driven by Cell-Free Quorum Sensing Gene Circuits","authors":"Dr. David T. Gonzales,&nbsp;Surased Suraritdechachai,&nbsp;Dr. Christoph Zechner,&nbsp;Dr. T.-Y. Dora Tang","doi":"10.1002/syst.202300041","DOIUrl":"https://doi.org/10.1002/syst.202300041","url":null,"abstract":"<p>The front cover artwork is provided by David T. Gonzales of the Max Planck Institute of Molecular Cell Biology and Genetics. The image shows a collection of aqueous water-in-oil droplets with lipid bilayer interfaces. Inside each droplet is a cell-free expression system that is capable of gene expression or intercellular communication. Read the full text of the Research Article at 10.1002/syst.202300029.</p>","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"5 6","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/syst.202300041","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"109176012","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
1,3-Acetonedicarboxylic Acid as a Simple Stimulus for Reversible Time-Controlled pH Modulation 1,3-丙酮二羧酸作为可逆时控 pH 值调节的简单刺激物
ChemSystemsChem Pub Date : 2023-10-27 DOI: 10.1002/syst.202300037
Vincent Verdoot, Dr. Adrien Quintard
{"title":"1,3-Acetonedicarboxylic Acid as a Simple Stimulus for Reversible Time-Controlled pH Modulation","authors":"Vincent Verdoot,&nbsp;Dr. Adrien Quintard","doi":"10.1002/syst.202300037","DOIUrl":"10.1002/syst.202300037","url":null,"abstract":"<p>Implementation of new activated carboxylic acids is crucial to switch reversibly chemical systems over time in a safer manner. By applying cheap 1,3-acetonedicarboxylic acid, the pH of aqueous solutions can be decreased before autonomously evolving over time back again to a higher value upon diacid decarboxylation. This decarboxylation can be catalysed by different species such as simple amines or simple metals such as iron and copper salts. This process generates 2 molecules of CO<sub>2</sub> and acetone as single waste, considerably decreasing the toxicity associated with such activated acids. The potential of this weak diacid was confirmed by reversibly disrupting a strong gel upon diacid addition and opens the way to the application in complex chemically fuelled systems.</p>","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"6 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-10-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"136262528","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
Polylysine-Coated Surfaces Drive Competition in Chemical Reaction Networks to Enable Molecular Information Processing 聚赖氨酸涂层表面推动化学反应网络竞争,实现分子信息处理
ChemSystemsChem Pub Date : 2023-10-22 DOI: 10.1002/syst.202300030
A. Hazal Koyuncu, Dr. Jacopo Movilli, Dr. Sevil Sahin, Dmitrii V. Kriukov, Prof. Jurriaan Huskens, Dr. Albert S. Y. Wong
{"title":"Polylysine-Coated Surfaces Drive Competition in Chemical Reaction Networks to Enable Molecular Information Processing","authors":"A. Hazal Koyuncu,&nbsp;Dr. Jacopo Movilli,&nbsp;Dr. Sevil Sahin,&nbsp;Dmitrii V. Kriukov,&nbsp;Prof. Jurriaan Huskens,&nbsp;Dr. Albert S. Y. Wong","doi":"10.1002/syst.202300030","DOIUrl":"10.1002/syst.202300030","url":null,"abstract":"<p>This work describes a competing activation network, which is regulated by chemical feedback at the liquid-surface interface. Feedback loops dynamically tune the concentration of chemical components in living systems, thereby controlling regulatory processes in neural, genetic, and metabolic networks. Advances in systems chemistry demonstrate that chemical feedback could be designed based on similar concepts of using activation and inhibition processes. Most efforts, however, are focused on temporal feedback whereas biological networks are maintained by the interplay between temporal and spatial organization. Here, we designed a feedback system comprising a simple acid-base equilibrium that can be perturbed by two opposing activation processes. Crucially, one of the processes is immobilized on the surface of a microfluidic channel using poly-<span>l</span>-lysine (PLL). We measured the capacity of the PLL-coated channels to resist changes in pH in flow using a pH-sensitive indicator, phenol red, and showed that this capacity can be increased by employing polyelectrolyte multilayers. Specifically, we found that the rate of local activation (<i>i. e</i>., the deprotonation of the immobilized lysine residues) could be significantly increased to delay the otherwise fast equilibrium. This effect allowed for encoding read and write operations, providing the potential to bestow CRNs with the capacity of molecular information processing.</p>","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"6 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/syst.202300030","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"134993615","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: Bidirectional Communication between Droplet Interface Bilayers Driven by Cell-Free Quorum Sensing Gene Circuits (ChemSystemsChem 6/2023) 封面:无细胞群体感应基因电路驱动的液滴界面双层之间的双向通信(chemsystemscheme 6/2023)
ChemSystemsChem Pub Date : 2023-10-05 DOI: 10.1002/syst.202300042
Dr. David T. Gonzales, Surased Suraritdechachai, Dr. Christoph Zechner, Dr. T.-Y. Dora Tang
{"title":"Front Cover: Bidirectional Communication between Droplet Interface Bilayers Driven by Cell-Free Quorum Sensing Gene Circuits (ChemSystemsChem 6/2023)","authors":"Dr. David T. Gonzales,&nbsp;Surased Suraritdechachai,&nbsp;Dr. Christoph Zechner,&nbsp;Dr. T.-Y. Dora Tang","doi":"10.1002/syst.202300042","DOIUrl":"https://doi.org/10.1002/syst.202300042","url":null,"abstract":"<p><b>The Front Cover</b> shows collections of communicating synthetic cells composed of water-in-oil droplets separated and stabilized by lipid bilayer interfaces and containing cell-free expression system with quorum sensing gene circuits. Cover design by David T. Gonzales. More information can be found in the Research Article by T.-Y. Dora Tang and co-worker.\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"5 6","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-10-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/syst.202300042","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"109163637","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
Cover Feature: Peptide and Peptidomimetic Assemblies in Dynamic Combinatorial Chemistry (ChemSystemsChem 6/2023) 封面专题:动态组合化学中的肽和拟肽组装(chemsystemscheme 6/2023)
ChemSystemsChem Pub Date : 2023-10-05 DOI: 10.1002/syst.202300043
Ashmi Rodrigues, Dr. Lou Rocard, Dr. Roba Moumné
{"title":"Cover Feature: Peptide and Peptidomimetic Assemblies in Dynamic Combinatorial Chemistry (ChemSystemsChem 6/2023)","authors":"Ashmi Rodrigues,&nbsp;Dr. Lou Rocard,&nbsp;Dr. Roba Moumné","doi":"10.1002/syst.202300043","DOIUrl":"https://doi.org/10.1002/syst.202300043","url":null,"abstract":"<p><b>The Cover Feature</b> illustrates three strategies for the generation of dynamic combinatorial libraries (DCLs) of peptide or peptidomimetic-based assemblies. Exploring their self-adaptative potential can lead to the discovery of smart nanomaterials, drug nanocarriers or drugs for untreated diseases. Cover design by Ashmi Rodrigues. More information can be found in the Review by Ashmi Rodrigues, Lou Rocard and Roba Moumné.\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"5 6","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-10-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/syst.202300043","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"109163780","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
Equilibrium and Non-equilibrium Reaction Schemes for Prebiotic Polymerization of Ribonucleotides 核糖核苷酸前生物聚合的平衡和非平衡反应方案
ChemSystemsChem Pub Date : 2023-09-21 DOI: 10.1002/syst.202300033
Varun Kitson, Quentin Sanders, Dr. Avinash V. Dass, Prof. Paul G. Higgs
{"title":"Equilibrium and Non-equilibrium Reaction Schemes for Prebiotic Polymerization of Ribonucleotides","authors":"Varun Kitson,&nbsp;Quentin Sanders,&nbsp;Dr. Avinash V. Dass,&nbsp;Prof. Paul G. Higgs","doi":"10.1002/syst.202300033","DOIUrl":"10.1002/syst.202300033","url":null,"abstract":"<p>The RNA World theory for the origin of life requires polymers to be generated initially by abiotic reactions. Experiments have studied polymerization of 5′-monophosphates, 2′,3′-cyclic phosphates, and 5′-triphosphates. We consider theoretical models of polymerization in solution illustrating the differences between these cases. We consider (i) a basic model where all monomers undergo reversible joining and breaking; (ii) a model where 2′,3′-cyclic phosphates can join, and breaking regenerates the cyclic phosphate; (iii) a model where 5′-triphosphates can join irreversibly, in addition to the joining and breaking of 2′,3′-cyclic phosphates. In cases (i) and (ii) there is an equilibrium steady state with balance between making and breaking bonds. In case (iii) there is a circular reaction flux in which monomers are activated by an external phosphate source, activated monomers form polymers, and polymers break to release non-activated monomers. The mean length can be calculated as a function of concentration. In case (iii), the mean length switches from a low-concentration regime controlled by the 5′-triphosphates to a high-concentration regime controlled by the 2′,3′-cyclic phosphates. The circular reaction flux is reminiscent of a metabolism. If formation of 5’-triphosphates was already in place for RNA synthesis, ATP could subsequently been coopted for metabolism.</p>","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"6 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/syst.202300033","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135944293","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
Assembly of Multi-Compartment Cell Mimics by Droplet-Based Microfluidics 基于微流控的多室细胞模拟装配
ChemSystemsChem Pub Date : 2023-09-08 DOI: 10.1002/syst.202300034
Tsvetomir Ivanov, Dr. Shoupeng Cao, Dr. Thao P. Doan-Nguyen, Heloísa Bremm Madalosso, Dr. Lucas Caire da Silva, Prof. Dr. Katharina Landfester
{"title":"Assembly of Multi-Compartment Cell Mimics by Droplet-Based Microfluidics","authors":"Tsvetomir Ivanov,&nbsp;Dr. Shoupeng Cao,&nbsp;Dr. Thao P. Doan-Nguyen,&nbsp;Heloísa Bremm Madalosso,&nbsp;Dr. Lucas Caire da Silva,&nbsp;Prof. Dr. Katharina Landfester","doi":"10.1002/syst.202300034","DOIUrl":"https://doi.org/10.1002/syst.202300034","url":null,"abstract":"<p>In recent years, there has been a growing interest in multi-compartment systems as a means of developing materials that mimic the structure and function of biological cells. These hierarchical systems, including artificial cells and cell-like reactors, can efficiently perform biochemical tasks by exploiting compartmentalization inspired by biological systems. However, the bottom-up design of cell mimics presents significant challenges due to the need for precise and efficient assembly of components. This short review examines recent advances in droplet-based microfluidics (DBM), which has emerged as a powerful technique for creating cell-like systems with multi-compartment architectures, precise composition, and biomimetic functionality. DBM has proven to be a reliable method for generating populations of cell-mimics with a compartment-in-compartment structure, some of which have adaptable properties that resemble the dynamic properties of natural cells. Notable examples will be discussed to illustrate how droplet-based microfluidics provides a versatile approach to create, manipulate, and study cell-mimics.</p>","PeriodicalId":72566,"journal":{"name":"ChemSystemsChem","volume":"5 6","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/syst.202300034","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"109165941","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
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