ChemistryEurope最新文献_第6页

Pore Nanoarchitectonics of Carbon Nitrides for the Excited-State Deactivation of Confined Methylene Blue 氮化碳纳米孔结构对受限亚甲基蓝激发态失活的影响

ChemistryEurope Pub Date : 2023-10-18 DOI: 10.1002/ceur.202300031

Dr. Chunyu Li, Dr. Erik Troschke, Dr. Carolin Müller, Anindita Dasgupta, Prof. Dr. Christian Eggeling, Prof. Dr. Martin Oschatz, Prof. Dr. Benjamin Dietzek-Ivanšić

{"title":"Pore Nanoarchitectonics of Carbon Nitrides for the Excited-State Deactivation of Confined Methylene Blue","authors":"Dr. Chunyu Li, Dr. Erik Troschke, Dr. Carolin Müller, Anindita Dasgupta, Prof. Dr. Christian Eggeling, Prof. Dr. Martin Oschatz, Prof. Dr. Benjamin Dietzek-Ivanšić","doi":"10.1002/ceur.202300031","DOIUrl":"10.1002/ceur.202300031","url":null,"abstract":"The confinement of organic chromophores within mesoporous material architectures can exert a considerable alteration on their physico-chemical properties. This study presents a detailed spectroscopic investigation of methylene blue (MB) entrapped in mesoporous polymeric carbon nitrides (mPCNs) with different pore architecturesusing transient absorption spectroscopy (TAS). The spatial confinement of MB molecules results in a prominent change in absorption spectra, characterized by both redshifts and the appearance of additional shoulder peaks, arising from the formation of MB dimers (MB2) concomitant with a distortion of the MB structure. Upon photoexcitation, entrapped MB molecules exhibit a notable altered excited-state absorption feature, along with a drastic excited-state quenching within 2 ns compared to molecues in bulk solutions. In contrast to the ultrafast quenching of sole MB2 with a lifetime of ~3.6 ps in highly concentrated solutions, the concentration-dependent quenching behavior of MB aggregates in confined environments suggests the effect is caused by excimers formed in close proximity. The findings of this work highlight the impact of constrained environments and intermolecular interactions on the relaxation pathways of the excited states in photoactive molecules.","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"1 3","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202300031","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135885230","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

An Aminoisoxazole-Based Proto-RNA 基于氨基异恶唑的原rna

ChemistryEurope Pub Date : 2023-10-12 DOI: 10.1002/ceur.202300057

Felix Xu, Dr. Stefan Wiedemann, Dr. Jonas Feldmann, Dr. Sidney Becker, Prof. Dr. Thomas Carell

引用次数: 0

Toward a Traceless Tag for the Thiol-Mediated Uptake of Proteins 巯基介导的蛋白质摄取的无迹标记

ChemistryEurope Pub Date : 2023-10-11 DOI: 10.1002/ceur.202300029

Dr. John R. J. Maynard, Dr. Saidbakhrom Saidjalolov, Marie-Claire Velluz, Stefania Vossio, Prof. Charlotte Aumeier, Dr. Dimitri Moreau, Dr. Naomi Sakai, Prof. Stefan Matile

{"title":"Toward a Traceless Tag for the Thiol-Mediated Uptake of Proteins","authors":"Dr. John R. J. Maynard, Dr. Saidbakhrom Saidjalolov, Marie-Claire Velluz, Stefania Vossio, Prof. Charlotte Aumeier, Dr. Dimitri Moreau, Dr. Naomi Sakai, Prof. Stefan Matile","doi":"10.1002/ceur.202300029","DOIUrl":"10.1002/ceur.202300029","url":null,"abstract":"The emergence of thiol-mediated uptake (TMU) as a powerful strategy to penetrate cells calls for the development of practical small-molecule TMU tools for traceless delivery. Toward this goal, esters are explored here as bioreversible linkers between dynamic covalent cascade exchangers accounting for TMU and the protein of interest (POI). The method relies on α-aryl-α-diazoamides that react with carboxylic acids of the POI to form esters that can be enzymatically hydrolyzed inside cells to release the native POI. A two-step protocol is established for bioreversible conjugation of TMU tags to the POI. Despite the small number of tags attached to POIs to prevent isoelectric precipitation, POIs with traceless TMU tags are shown to efficiently enter cells not only in 2D culture but also in 3D spheroids mimicking deep tissue, confirming a key advantage of TMU. Uptake inhibition by various thiol-reactive agents confirms the participation of cell-surface thiols in cell penetration, i. e., the occurrence of TMU.","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"1 3","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202300029","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"136213434","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

Actinide-Pnictide Chemistry: A Uranium Primary Alkyl Stibinide and a Diuranium Hexaantimonide-Tetralithium Zintl Cluster 锕系-镍系化学:一个铀伯系烷基硬binide和一个二铀六锑化物-四锂锌团簇

ChemistryEurope Pub Date : 2023-10-02 DOI: 10.1002/ceur.202300067

Dr. Thomas M. Rookes, Dr. Gábor Balázs, Dr. Benedict M. Gardner, Dr. Ashley J. Wooles, Prof. Dr. Manfred Scheer, Prof. Dr. Stephen T. Liddle

{"title":"Actinide-Pnictide Chemistry: A Uranium Primary Alkyl Stibinide and a Diuranium Hexaantimonide-Tetralithium Zintl Cluster","authors":"Dr. Thomas M. Rookes, Dr. Gábor Balázs, Dr. Benedict M. Gardner, Dr. Ashley J. Wooles, Prof. Dr. Manfred Scheer, Prof. Dr. Stephen T. Liddle","doi":"10.1002/ceur.202300067","DOIUrl":"10.1002/ceur.202300067","url":null,"abstract":"Structurally characterised U−Sb bonds are rare. Here, the synthesis and characterisation of [U(TrenDMBS){Sb(H)C(H)(SiMe3)2}] (5, TrenDMBS=N(CH2CH2NSiMe2But)3) and [{U(TrenTIPS)}2{Sb3(μ6-Li)(μ-Li[THF]2)3Sb3}] (6, TrenTIPS=N(CH2CH2NSiPri3)3) are reported. Complex 5 is an unprecedented primary stibinide actinide complex and 6 can be formulated as containing a unique triple decker 20 skeletal-electron distorted closo tricapped Zintl cluster (Sb3Li4Sb3)2− that is analogous to the D3h closo tricapped trigonal prism form of [Ge9]2−. Quantum chemical calculations emphasise polar U−Sb bonding in 5 and 6, and that viewing (Sb3Li4Sb3)2− as a single unit rather than two distinct but contiguous (Sb3)3− units, themselves unprecedented in molecular actinide chemistry, is valid due to the presence of three weak (Sb3)⋯(Sb3) (3, −1)-bond critical points. Complexes 5 and 6 highlight the challenges of preparing polar U−Sb bonds and the underlying tendency for unpredictable cluster formation with Sb.","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"1 3","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202300067","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135899230","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

Hydrophobic Interfacing of Fluorescent Membrane Probes 荧光膜探针的疏水界面

ChemistryEurope Pub Date : 2023-10-02 DOI: 10.1002/ceur.202300041

Felix Bayard, Dr. Xiao-Xiao Chen, Dr. Juan Manuel García-Arcos, Prof. Aurelien Roux, Dr. Naomi Sakai, Prof. Stefan Matile

{"title":"Hydrophobic Interfacing of Fluorescent Membrane Probes","authors":"Felix Bayard, Dr. Xiao-Xiao Chen, Dr. Juan Manuel García-Arcos, Prof. Aurelien Roux, Dr. Naomi Sakai, Prof. Stefan Matile","doi":"10.1002/ceur.202300041","DOIUrl":"10.1002/ceur.202300041","url":null,"abstract":"Fluorescent flippers have been introduced as small-molecule probes to image membrane tension in living systems. While the hydrophilic headgroup region has been modified extensively for intracellular targeting, little is known about the hydrophobic interfacing with the surrounding membrane. To tackle this challenge, the design, synthesis and evaluation of a glutamine-derived flipper collection is reported. Considering the importance of tension-induced phase separation for tension imaging, this study is focused on how to modulate the distribution of functional flippers between ordered and disordered microdomains. Also of interest was control over intermembrane transfer without loss of function for the specific labeling of plasma and intracellular membranes. Evidence is presented for a two-step insertion mechanism through more accessible disordered domains into better matching ordered domains. This process also explains differences between partition coefficients and bioimaging. It is further demonstrated that interdomain and intermembrane distribution can be regulated by hydrophobic interfacing to control brightness in fluorescence lifetime imaging microscopy and responsiveness to membrane tension. Irreversible partitioning inhibits intermembrane transfer and coincides with internalization into cells. These results demonstrate that hydrophobic interfacing can improve probe performance and provide guidelines on how to proceed.","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"1 3","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202300041","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135899450","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

Conformational Selection and Induced Fit: The Behavior of Two Homologous Proteases 构象选择与诱导拟合:两种同源蛋白酶的行为

ChemistryEurope Pub Date : 2023-09-29 DOI: 10.1002/ceur.202300060

Hannah Maus, Gerald Hinze, Stefan J. Hammerschmidt, Prof. Dr. Tanja Schirmeister, Prof. Dr. Thomas Basché

{"title":"Conformational Selection and Induced Fit: The Behavior of Two Homologous Proteases","authors":"Hannah Maus, Gerald Hinze, Stefan J. Hammerschmidt, Prof. Dr. Tanja Schirmeister, Prof. Dr. Thomas Basché","doi":"10.1002/ceur.202300060","DOIUrl":"10.1002/ceur.202300060","url":null,"abstract":"Protein-ligand interactions are crucial for many cellular processes, with details of the binding mechanism being discussed as essential for biological functions. Interestingly, protein binding often involves conformational changes between two or more states, whereby different binding mechanisms are possible even with a simple two-state description. Two models are widely used to portray protein-ligand interactions: Induced fit and conformational selection. However, distinguishing them experimentally is challenging. Single-molecule Förster resonance energy transfer (smFRET) has emerged as a powerful tool to resolve structural dynamics at the level of single proteins. Here, we investigated immobilized Zika virus (ZIKV) and dengue virus (DENV2) NS2B-NS3 proteases using smFRET to compare their conformational changes upon binding to competitive small molecule inhibitors. The analysis of the smFRET data allowed us to distinguish between induced fit and conformational selection models and assign the binding mechanism from the kinetic parameters obtained. Although DENV and ZIKV protease are proteins with high structural similarities, our results reveal that they have opposite binding mechanisms for competitive ligands. While the protein-ligand interaction in the ZIKV protease follows an induced fit mechanism, the DENV protease follows the conformational selection mechanism.","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"1 3","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202300060","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135244044","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

Synthesis and Enzymatic Conversion of Amino Acids Equipped with the Silanetriol Functionality: A Prelude to Silicon Biodiversification 具有硅三醇功能的氨基酸的合成和酶转化:硅生物多样化的前奏

ChemistryEurope Pub Date : 2023-09-27 DOI: 10.1002/ceur.202300058

Dr. Jade Dussart-Gautheret, Dr. Julie Rivollier, Dr. Cédric Simon, Dr. Alessandro De Simone, Dr. Jérôme Berthet, Prof. Stéphanie Delbaere, Régina Maruchenko, Claire Troufflard, Dr. Denis Lesage, Dr. Yves Gimbert, Dr. Gilles Lemière, Dr. Philippe Marlière, Prof. Louis Fensterbank

{"title":"Synthesis and Enzymatic Conversion of Amino Acids Equipped with the Silanetriol Functionality: A Prelude to Silicon Biodiversification","authors":"Dr. Jade Dussart-Gautheret, Dr. Julie Rivollier, Dr. Cédric Simon, Dr. Alessandro De Simone, Dr. Jérôme Berthet, Prof. Stéphanie Delbaere, Régina Maruchenko, Claire Troufflard, Dr. Denis Lesage, Dr. Yves Gimbert, Dr. Gilles Lemière, Dr. Philippe Marlière, Prof. Louis Fensterbank","doi":"10.1002/ceur.202300058","DOIUrl":"10.1002/ceur.202300058","url":null,"abstract":"Synthetic routes are reported for the three analogues of the simplest L-2-amino-dicarboxylic acids, aspartate, glutamate, and aminoadipate, in which the silanetriol group (Si(OH)3) replaces the distal carboxyl group (CO2H). Direct access to the silanetriol amino acids relied either on catalytic hydrosilylation of a terminal alkene using triethoxysilane, or on alkylation of a glycine equivalent anion by triallyl(iodomethyl)silane. In both cases, acid hydrolysis afforded the silanetriol amino acids. These were shown to self-assemble into siloxane Si-O clusters as their concentration in water increased in the pH range of 1–12. Such reversible cross-linking did not prevent silanetriol amino acids from serving as substrates of an aminotransferase enzyme, boding well for their utilization as microbial nutrients to encompass silicon in future stages of metabolism and polypeptide edifices.","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"1 3","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202300058","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135537776","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

Controlling the Assembly of PdII/Bianthryl-Based Monomeric and Dimeric Interlocked Cages by Steric Effects 空间效应控制PdII/Bianthryl基单体和二聚体连锁笼的组装

ChemistryEurope Pub Date : 2023-09-26 DOI: 10.1002/ceur.202300047

Sota Watanabe, Dr. Masahiro Yamashina, Dr. Eiji Tsurumaki, Prof. Dr. Shinji Toyota

{"title":"Controlling the Assembly of PdII/Bianthryl-Based Monomeric and Dimeric Interlocked Cages by Steric Effects","authors":"Sota Watanabe, Dr. Masahiro Yamashina, Dr. Eiji Tsurumaki, Prof. Dr. Shinji Toyota","doi":"10.1002/ceur.202300047","DOIUrl":"10.1002/ceur.202300047","url":null,"abstract":"In the energy landscape of coordination-driven self-assembly processes, the isolation of kinetically formed supramolecular cages has long been identified as a challenging task. This study reports a reliable strategy for the selective isolation of kinetically or thermodynamically preferred stable coordination cages, whose formation depends on the degree of steric protection offered by the exterior side chains. The combination of PdII ions with arc-shaped 2,2′-bianthryl-based ligands that contain different numbers of methoxyethoxy side chains led to the quantitative formation of both kinetically favorable monomeric M2L4 cages and thermodynamically favorable dimeric (M2L4)2 interlocked cages. These assemblies were structurally fully characterized via NMR spectroscopy, mass spectrometry, and single-crystal X-ray diffraction analysis. Although the monomeric cages with fewer exterior side chains can reassemble into interlocked cages, the cages with more exterior substituents remain monomeric cages under similar conditions. A computational study revealed that this different behavior is mainly governed by the destabilization of the interlocking assemblies due to the steric repulsion among the side chains on the overcrowded exterior. Furthermore, the kinetically stabilized monomeric M2L4 cages exhibit permanent host abilities toward sulfonate guests, while the cages with lower steric protection undergo dimerization accompanied by guest release.","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"1 3","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202300047","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"134960011","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: N-Doped Octagon-Containing HBC as Redox and pH Chiroptical Switch in the NIR (ChemistryEurope 2/2023) 封面特征：含HBC的N掺杂八角形作为氧化还原剂和近红外pH Chiropoptical开关（ChemistryEurope2/2023）

ChemistryEurope Pub Date : 2023-09-12 DOI: 10.1002/ceur.202300061

Dr. Miguel A. Medel, Lidia Hortigüela, Dr. Vega Lloveras, José Catalán-Toledo, Prof. Delia Miguel, Prof. Antonio J. Mota, Prof. Núria Crivillers, Prof. Araceli G. Campaña, Dr. Sara P. Morcillo

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Front Cover: Complexities of the Interaction of NiII, PdII and PtII Pyrrole-Imine Chelates with Human Serum Albumin (ChemistryEurope 2/2023) 封面：NiII、PdII和PtII吡咯亚胺螯合物与人血清白蛋白相互作用的络合作用（ChemistryEurope2/2023）

ChemistryEurope Pub Date : 2023-09-04 DOI: 10.1002/ceur.202300056

Sheldon Sookai, Prof. Dr. Orde Q. Munro

引用次数: 0