ChemPlusChem最新文献

{"title":"Cover Feature: Piercing the Shadows: Exploring the Influence of Signal Preprocessing on Interpreting Ultrasensitive Bioelectronic Sensor Data (ChemPlusChem 2/2025)","authors":"Mariapia Caputo,&nbsp;Lucia Sarcina,&nbsp;Cecilia Scandurra,&nbsp;Michele Catacchio,&nbsp;Matteo Piscitelli,&nbsp;Cinzia Di Franco,&nbsp;Paolo Bollella,&nbsp;Gaetano Scamarcio,&nbsp;Luisa Torsi,&nbsp;Eleonora Macchia","doi":"10.1002/cplu.202580202","DOIUrl":"https://doi.org/10.1002/cplu.202580202","url":null,"abstract":"<p><b>A single-molecule with a large transistor</b> (SiMoT) array is used to explore the impact of data preprocessing on electronic biosensor outcomes. Cyst fluid and plasma samples from 37 patients with pancreatic precursor cyst lesions are analyzed. New strategies to mitigate these effects are provided, ensuring that data interpretation remains accurate and reflective of the underlying biochemical information in the samples. More details can be found in the Research Article by Luisa Torsi, Eleonora Macchia, and co-workers (DOI: 10.1002/cplu.202400520).<figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":148,"journal":{"name":"ChemPlusChem","volume":"90 2","pages":""},"PeriodicalIF":3.0,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cplu.202580202","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143404334","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}

{"title":"Front Cover: Artificial Compartments Encapsulating Enzymatic Reactions: Towards the Construction of Artificial Organelles (ChemPlusChem 2/2025)","authors":"Peng Lin,&nbsp;Shiwei Zhang,&nbsp;Futa Komatsubara,&nbsp;Hiroaki Konishi,&nbsp;Eiji Nakata,&nbsp;Takashi Morii","doi":"10.1002/cplu.202580201","DOIUrl":"https://doi.org/10.1002/cplu.202580201","url":null,"abstract":"<p><b>The front cover shows</b> the artificial compartments constructed using liposomes, polymersomes, proteins, DNA nanostructures, and hybrid materials. Enzymes have been incorporated, assembled, or spatially organized into the membrane or membraneless compartments to efficiently carry out the enzymatic reactions or metabolic pathways and to understand the chemistry behind the compartment function. These compartments can be the building blocks to construct the artificial organelles with the target functions. More details can be found in the Review by Takashi Morii and co-workers (DOI: 10.1002/cplu.202400483).<figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":148,"journal":{"name":"ChemPlusChem","volume":"90 2","pages":""},"PeriodicalIF":3.0,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cplu.202580201","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143404714","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}

{"title":"Phenoxazinone Synthase-Like Catalytic Activity of Bi- and Trinuclear Copper(II) Complexes with 2-Benzylethanolamine: Experimental and Theoretical Investigations.","authors":"Oksana V Nesterova, Olena E Bondarenko, Armando J L Pombeiro, Dmytro S Nesterov","doi":"10.1002/cplu.202400613","DOIUrl":"10.1002/cplu.202400613","url":null,"abstract":"<p><p>The self-assembly reaction of 2-benzylaminoethanol (Hbae) with CuCl₂ or Cu(NO₃)₂ leads to the formation of binuclear [Cu₂(bae)₂(Cl)₂] (1) and [Cu₂(Hbae)₂(bae)₂](NO₃)₂ (2) complexes, while the trinuclear [Cu₃(Hbae)₂(bae)₂(dmba)₂](NO₃)₂ (3) compound was obtained using the auxiliar bulky substituted 2,2-dimethylbutyric acid (Hdmba). Crystallographic studies reveal the molecular structures of 1 and 2 based on the similar {Cu₂(μ-O)₂} core, while the structure of 3 features the {Cu₃(μ-O)₂} core with consecutive arranement of the metal centres, supported by the additional carboxylate bridges. The strong intermolecular hydrogen bonds join the molecular structures into 1D (for 1 and 3) or 2D (for 2) architectures. All three compounds act as catalysts for the aerobic oxidation of 2-aminophenol to the phenoxazinone chromophore (phenoxazinone synthase-like activity) with the maximum reaction rates up to 2.3×10^-8 M s^-1. The substrate scope involves methyl-, nitro- and chloro-substituted 2-aminophenols, disclosing the negligible activity of nitro-derivatives, while the 6-amino-m-cresol substrate shows the highest activity with the initial reaction rate of 5.8×10^-8 M s^-1. The mechanism of the rate-limiting reaction step (copper-catalysed formation of 2-aminophenoxyl radicals) was investigated at the DFT level. The combined DFT and CASSCF studies of the copper superoxo Cu^II-OO⋅ radical species as possible unconventional reaction intermediates resulted in a rational mechanism of H-atom abstraction, where the activation energies follow the experimental reactivity of substituted 2-aminophenols. The TDDFT and STEOM-DLPNO-CCSD theoretical calculations of the absorption spectra of substrates, phenoxazinone chromophores and putative polynuclear species containing 2-aminophenoxo ligand are reported.</p>","PeriodicalId":148,"journal":{"name":"ChemPlusChem","volume":" ","pages":"e202400613"},"PeriodicalIF":3.0,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143389483","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}

{"title":"A Computational Design of Covalently Bonded Mixed Stacking Cocrystals.","authors":"Lam H Nguyen, Thanh N Truong","doi":"10.1002/cplu.202500028","DOIUrl":"10.1002/cplu.202500028","url":null,"abstract":"<p><p>In this study, a computational design of a new type of donor-acceptor mixed stacking cocrystals is introduced. Our approach involves functionalizing trisilasumanene frameworks with electron-donating groups (-CH₃, -OH, -NH₂) and electron-withdrawing groups (-F, -CN), and then stacking donors and acceptors alternatively while connecting them either by sp³- and sp-carbon chains. Using the B3LYP-D3/6-31+G(d) level of theory, we demonstrate that these covalently bonded cocrystals can overcome the issue of thermal and mechanical instabilities observed in the non-covalently mixed stacking. Furthermore, modifying donor and acceptor groups can vary the bandgaps, approximated by the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) gaps, from 1.50 to 3.50 eV. The results also predict the covalently bonded mixed stacking cocrystals having much larger conductance via Yoshizawa model. In addition, variations in bridge lengths were found to have a small effect on the HOMO-LUMO gaps but allow for a new control parameter regarding the porosity of the materials. These results encourage experimental explorations.</p>","PeriodicalId":148,"journal":{"name":"ChemPlusChem","volume":" ","pages":"e202500028"},"PeriodicalIF":3.0,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143381332","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}

{"title":"Sustainable One-Pot Electrochemical Approach for Entrapment of Multi-Enzymes and Biocompatible Redox Mediator.","authors":"Hathaichanok Seelajaroen, Felix Mayr, Dominik Wielend, Munise Cobet, Christoph Ulbricht, Niyazi Serdar Sariciftci, Serpil Tekoglu","doi":"10.1002/cplu.202400577","DOIUrl":"10.1002/cplu.202400577","url":null,"abstract":"<p><p>Enzyme immobilization is regarded as a key factor for their effective utilization in various fields such as biofuel production, wastewater treatment, and biosensors. Designing new electrodes with biocompatible support matrices is essential to improve the stability in bioelectrocatalysis. Modified carbon felt electrodes were prepared and tested as bioelectrocatalyst under mild conditions - aqueous media at room temperature and basically neutral pH. Co-immobilization of dehydrogenase enzymes and neutral red (NR) dye at carbon felt electrodes was successfully achieved during electropolymerization of pyrrole in a facile one-step approach. Neutral red was incorporated to operate as a redox mediator supporting efficient electron transfer to the enzymes' active sites. Electrodes modified with alcohol dehydrogenase (ADH) have been employed to reduce acetaldehyde to ethanol in a chronoamperometic setting with Faradaic efficiency (FE) of up to 33 %. By incorporating the cascade reaction with three enzymes - ADH, formate dehydrogenase, and formaldehyde dehydrogenase - an electroreduction sequence could be established to produce methanol from CO₂ reaching a FE of 10 %. The proposed approach shows good stability. Together with the simple implementation and application, this process is promising for employment in enzymatic electrocatalysis.</p>","PeriodicalId":148,"journal":{"name":"ChemPlusChem","volume":" ","pages":"e202400577"},"PeriodicalIF":3.0,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143363352","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}

{"title":"Inorganic Nanoparticles in Reproduction Biology: Opportunities and Challenges.","authors":"Stephan Barcikowski, Sangita Kundu, Christoph Rehbock, Wilfried A Kues","doi":"10.1002/cplu.202400554","DOIUrl":"https://doi.org/10.1002/cplu.202400554","url":null,"abstract":"<p><p>The development of inorganic metal and metal oxide nanoparticles (MNPs) has attracted significant attention in  biomedical and biotechnological fields. An emerging field in this context is the use of MNPs  in reproduction biology. Here, we review the development of MNPs in the field of reproduction  by focusing on their interactions with highly delicate and specialized germ cells like spermatozoa and oocytes as well as developing embryos. By their unique physicochemical properties, MNPs are good candidates for targeted imaging and delivery of biofunctional molecules  to the specific sites of the gametes and reproductive cells. Furthermore, functionalized MNPs can serve as transfection vectors for the generation of transgenic animals by sperm-mediated gene transfer (SMGT) in artificial insemination or in vitro fertilization. In addition, MNPs have shown great promise in application fields such as semen collection, nano-purification, cryopreservation, and sex sorting of sperm in the livestock industry. The article includes an in-depth discussion on the uptake, translocation mechanism, and bioresponse of the MNPs to reproduction-relevant sites on the clinical, cellular, and molecular levels. Based on these promising achievements, the current challenges and prospects of the development of these functionalized MNPs for clinical research in conjunction with the reproductive system will be discussed.</p>","PeriodicalId":148,"journal":{"name":"ChemPlusChem","volume":" ","pages":"e202400554"},"PeriodicalIF":3.0,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143363351","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}

{"title":"Redox-Responsive Side Chain Structural Changes in a Seven-Membered Cyclic α,α-Disubstituted α-Amino Acid with a Disulfide Bond Enable Reversible Conformational Changes in Peptides.","authors":"Makoto Oba, Hikaru Nonaka, Tomohiro Umeno, Takuma Kato, Mitsunobu Doi, Atsushi Ueda, Masakazu Tanaka","doi":"10.1002/cplu.202400772","DOIUrl":"https://doi.org/10.1002/cplu.202400772","url":null,"abstract":"<p><p>We report the development of a redox-responsive system that induces reversible conformational changes in peptides through the design of a seven-membered cyclic α,α-disubstituted α-amino acid with a disulfide bond, 5-amino-1,2-dithiepane-5-carboxylic acid (Dtp). Upon reduction, the disulfide bond in Dtp was cleaved to form thiols, converting Dtp into (2-mercaptoethyl)homocysteine (Mhc), and this process was reversed by oxidation. Dtp-containing peptides predominantly adopted 3₁₀-helical conformation in solution, whereas Mhc-containing peptides exhibited a mixture of helical and other conformations. This redox-responsive mechanism allows for precise control over peptide secondary structures, making it a promising approach for designing functional helical peptides capable of acting molecular switches in response to intracellular reductive environments.</p>","PeriodicalId":148,"journal":{"name":"ChemPlusChem","volume":" ","pages":"e202400772"},"PeriodicalIF":3.0,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143187832","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}

{"title":"Thermodynamic Insights on the Structure-Property Relationships in Substituted Benzenes: Are the Pairwise Interactions in Tri-Substituted Methyl-Nitro-Benzoic Acids Still Valid?","authors":"José M Silva Ferraz, Vladimir N Emel'yanenko, Dzmitry H Zaitsau, Artemiy A Samarov, Bruno Brunetti, Andrea Ciccioli, Stefano Vecchio Ciprioti, Sergey P Verevkin","doi":"10.1002/cplu.202400703","DOIUrl":"10.1002/cplu.202400703","url":null,"abstract":"<p><p>A comprehensive experimental thermochemical study of nine methyl-substituted nitrobenzoic acids was carried out, leading to the final standard molar enthalpies of formation in the gas phase. The combustion energies were measured using high-precision combustion calorimetry, and the enthalpies of formation of the crystal phase were derived. The sublimation enthalpies were obtained from the vapor pressure-temperature dependencies measured using the classic Knudsen effusion mass loss and the transpiration methods. The standard molar enthalpies of vaporisation were derived from the temperature dependence of the mass-loss rates measured using the non-isothermal thermogravimetry. The thermal behaviour, including melting temperatures and standard molar enthalpies of fusion, was investigated by DSC. The high-level quantum chemical G* methods were used for the mutual validation of the experimental and theoretical gas phase enthalpies of formation of methyl-substituted nitrobenzoic acids. The consistent set of experimental properties at the reference temperature T=298 K was evaluated and recommended for thermochemical calculations. The pairwise interactions of the substituents on the benzene ring were derived from nitro-toluenes, methyl-benzoic acids and nitro-benzoic acids available in the literature, and the additivity of the contributions when three substituents are placed simultaneously in the benzene ring was discussed.</p>","PeriodicalId":148,"journal":{"name":"ChemPlusChem","volume":" ","pages":"e202400703"},"PeriodicalIF":3.0,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143078079","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}

{"title":"Automated Investigation of Metal-Ligand Interactions by a Newly Established Robotic Workflow for Titrations.","authors":"Michael Ringleb, Lukas Klähn, Stefan Zechel, Ulrich S Schubert","doi":"10.1002/cplu.202400686","DOIUrl":"10.1002/cplu.202400686","url":null,"abstract":"<p><p>In this work, we present a new workflow to set up an automated platform for the investigation of metal complex formation in solutions. With the utilization of this robot titration platform, the generation of an abundancy of solvated metal complexes in differing coordination number is possible in a simple manner. The generated complexes can subsequently be sampled into differing vessels to examine them in detail. We present sampling for UV/Vis and NMR spectroscopy at chosen model systems, however, the platform can easily be adapted to provide samples for other techniques, e. g., for infrared spectroscopy.</p>","PeriodicalId":148,"journal":{"name":"ChemPlusChem","volume":" ","pages":"e202400686"},"PeriodicalIF":3.0,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143121789","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}

{"title":"Heteroleptic (NHC/MIC) Biscarbene Ag(I) and Au(I) Complexes: Synthesis, Characterization and Catalytic Applications.","authors":"Francisco J Ruiz-Mendoza, Emmanuel Campos-Dominguez, M Guadalupe Torres-Salazar, Alejandro Álvarez-Hernández, Daniel Mendoza-Espinosa","doi":"10.1002/cplu.202400765","DOIUrl":"10.1002/cplu.202400765","url":null,"abstract":"<p><p>A series of hetero-biscarbene silver(I) and gold(I) complexes of the general formula [NHC-M-MIC]PF₆ (NHC=imidazol-2-ylidene, MIC=1,2,3-triazol-5-ylidene) have been prepared via the treatment of NHC-M-Cl precursors in reaction with an in situ generated mesoionic carbene (MIC). The new heteroleptic complexes have been fully characterized including NMR spectroscopy, elemental analysis, melting points and single crystal X-ray diffraction. The silver(I) derivatives were employed successfully in the solvent free KA² (ketone-alkyne-amine) coupling for the preparation of a series of quaternary carbon-containing propargyl amines while, the gold(I) biscarbenes, demonstrated a good performance in the A³ (aldehyde, amine, alkyne) coupling and the benzylic oxidation processes under low catalyst loadings.</p>","PeriodicalId":148,"journal":{"name":"ChemPlusChem","volume":" ","pages":"e202400765"},"PeriodicalIF":3.0,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143062836","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}