ACS Omega最新文献

{"title":"An Efficient and Accessible Hectogram-Scale Synthesis for the Selective O-GlcNAcase Inhibitor Thiamet-G","authors":"Viktor Holicek,&nbsp;Matthew Deen,&nbsp;Sandeep Bhosale,&nbsp;Roger A. Ashmus and David J. Vocadlo*,&nbsp;","doi":"10.1021/acsomega.4c0614110.1021/acsomega.4c06141","DOIUrl":"https://doi.org/10.1021/acsomega.4c06141https://doi.org/10.1021/acsomega.4c06141","url":null,"abstract":"<p >Altered levels of intracellular protein glycosylation with O-linked β-N-acetylglucosamine (O-GlcNAc) have emerged as being involved in various cancers and neurodegenerative diseases. OGA inhibitors have proven critically useful as tools to help understand the roles of O-GlcNAc, yet accessing large quantities of inhibitors necessary for many animal studies remains a challenge. Herein is described a scalable method to produce Thiamet-G, a potent, selective, and widely used brain-permeable OGA inhibitor. This synthetic route begins with inexpensive precursor, requires no column chromatography, employs simple nontoxic reagents, and in a single campaign can furnish several hundred grams of crystalline Thiamet-G in an overall yield of 44% over six steps.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":"9 50","pages":"49223–49228 49223–49228"},"PeriodicalIF":3.7,"publicationDate":"2024-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsomega.4c06141","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842105","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Charging and Discharging of Poly(m-aminophenylboronic Acid) Doped with Phytic Acid for Enzyme-Free Real-Time Monitoring of Human Sweat Lactate","authors":"Ryujiro Kishi,&nbsp;Shoichi Nishitani,&nbsp;Hiroyuki Kudo and Toshiya Sakata*,&nbsp;","doi":"10.1021/acsomega.4c0667110.1021/acsomega.4c06671","DOIUrl":"https://doi.org/10.1021/acsomega.4c06671https://doi.org/10.1021/acsomega.4c06671","url":null,"abstract":"<p >In this study, we realized a real-time and enzyme-free measurement of lactate in sweat in the same way as an enzyme-based amperometric method. A conductive polymer, which is based on polyaniline (PANI), was strongly coated on a glassy carbon electrode as a poly <i>m</i>-aminophenylboronic acid (PANI–PBA) membrane by drop-casting, which is a convenient method, owing to adhesive phytic acid (PA) molecules with negative charges included as a dopant. This polymer membrane had a functional structure with PBA in the PANI main chain, which expectedly induced electrical charges upon diol binding to lactate, owing to the formation of deprotonated boronate esters with negative charges. This indicates that PBA served as the self-dopant and as the site of binding to lactate. On the basis of the fundamental electrochemical characteristics such as the membrane resistance, the change in the current density of the PA-doped PANI–PBA electrode was quantitatively monitored with the change in lactate concentration from 1 to 300 mM under acidic conditions in real time, considering pH and interfering substances in sweat. Moreover, the sweat lactate concentration was determined to be ca. 60 mM using the PA-doped PANI–PBA electrode in a microfluidic system in measurements using sweat samples collected during exercise load. A change in current density induced a change in the density of charges in the capacitive PA-doped PANI–PBA membrane. This means that the detection mechanism for the change in the lactate concentration in sweat was based on repeated charging and discharging in the PA-doped PANI–PBA electrode.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":"9 50","pages":"49368–49376 49368–49376"},"PeriodicalIF":3.7,"publicationDate":"2024-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsomega.4c06671","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842726","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Room-Temperature Deposition of δ-Ni5Ga3 Thin Films and Nanoparticles via Magnetron Sputtering","authors":"Filippo Romeggio*,&nbsp;Rasmus Bischoff,&nbsp;Clara B. Møller,&nbsp;Victor L. Jensen,&nbsp;Esteban Gioria,&nbsp;Rikke Egeberg Tankard,&nbsp;Rasmus S. Nielsen,&nbsp;Ole Hansen,&nbsp;Ib Chorkendorff,&nbsp;Jakob Kibsgaard and Christian D. Damsgaard*,&nbsp;","doi":"10.1021/acsomega.4c0840510.1021/acsomega.4c08405","DOIUrl":"https://doi.org/10.1021/acsomega.4c08405https://doi.org/10.1021/acsomega.4c08405","url":null,"abstract":"<p >Magnetron sputtering is a versatile method for investigating model system catalysts thanks to its simplicity, reproducibility, and chemical-free synthesis process. It has recently emerged as a promising technique for synthesizing δ-Ni₅Ga₃ thin films. Physically deposited thin films have significant potential to clarify certain aspects of catalysts by eliminating parameters such as particle size dependence, metal–support interactions, and the presence of surface ligands. In this work, we demonstrate the potential of magnetron sputtering for the synthesis and analysis of thin film catalysts, using Ni₅Ga₃ as a model system. Initially, deposition conditions were optimized by varying the deposition pressure, followed by an investigation of the temperature effects, aiming to map a structure zone dependence on temperature and pressure as in the Thornton model. The evolution of film crystallinity was monitored using a combination of grazing incidence X-ray diffraction (GI-XRD) and high-resolution scanning electron microscopy (HR-SEM). Additionally, ultrathin films were synthesized and annealed in H₂ at high temperatures to demonstrate the possibility of producing size-controlled nanoparticles by adjusting the annealing conditions. This work demonstrates the full potential of magnetron sputtering as a technique for synthesizing model system catalysts in various forms, opening new avenues for the research and development of additional catalytic systems.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":"9 50","pages":"49759–49766 49759–49766"},"PeriodicalIF":3.7,"publicationDate":"2024-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsomega.4c08405","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142850367","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Electrorefining of Crude Solder for the Production of Fine Solder in Methanesulfonic Acid Medium: Electrolyte Conductivity and Electrorefining Process.","authors":"Yuhui Zhang, Kunyun He, Bingjie Jin, Jin Luan","doi":"10.1021/acsomega.4c08470","DOIUrl":"https://doi.org/10.1021/acsomega.4c08470","url":null,"abstract":"<p><p>At present, the refining of crude solder has many drawbacks such as high energy consumption, high environmental pollution, equipment corrosion, and low current efficiency. Therefore, a new technique for refining crude solder is of great practical importance. In this work, the electrorefining of crude solder in methanesulfonic acid (MSA) medium was studied. The conductivities of tin-MSA solutions had been measured and modeled to characterize the electrolyte. The effects of the electrorefining conditions on the electrorefining process were investigated systematically. The cell voltage, current efficiency, and fine solder appearance were used to characterize the electrorefining performance. Some operating parameters of the electrorefining process are established as follows: current density 207 A/m², tin concentration 120-160 g/L, free-MSA concentration 90-120 g/L, electrode spacing 4 cm, and temperature 305.15-315.15 K. Under these conditions, the average cell voltage is 0.30 V and the current efficiency is 99.31%. The total content of tin and lead of the fine solder with good product appearance is >99.99%. This technique offers low energy consumption, high productivity, and low environmental pollution.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":"9 50","pages":"49778-49785"},"PeriodicalIF":3.7,"publicationDate":"2024-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11656602/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142875364","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Tunneling Times in an Asymmetric Harmonic Double-Well with Application to Electron Transfers in Biological Macromolecules","authors":"João Marcos Costa Monteiro*,&nbsp; and ,&nbsp;Elso Drigo Filho,&nbsp;","doi":"10.1021/acsomega.4c0862210.1021/acsomega.4c08622","DOIUrl":"https://doi.org/10.1021/acsomega.4c08622https://doi.org/10.1021/acsomega.4c08622","url":null,"abstract":"<p >Tunneling times were calculated in electron transfer processes using an asymmetric harmonic double-well model. The simplicity of a direct variational calculation in the approximate solution of the Schrödinger equation, along with the interpretation of tunneling times within the probabilistic framework of a two-level system, allows for the efficient and accurate determination of tunneling times with minimal computational cost. These calculations were applied to electron transfer processes in the study of the photosynthetic reaction center and in the context of catalysis in UV-induced DNA lesion repair and are in agreement with the experimental, computational, and theoretical results with which they were compared. It was seen that the donor–acceptor distance needed to be adjusted for closer agreement between the calculated and experimentally observed times. However, the adjusted values for this distance remain close to those reported in the literature.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":"9 50","pages":"49832–49838 49832–49838"},"PeriodicalIF":3.7,"publicationDate":"2024-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsomega.4c08622","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842730","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Three Dihydroquinolin-4-one Derivatives as Potential Biodiesel Additives: From the Molecular Structure to Machine Learning Approach","authors":"Leonardo R. de Almeida*,&nbsp;Antônio S. N. Aguiar,&nbsp;Alex B. R. M. da Anunciação,&nbsp;Giulio D. C. d’Oliveira,&nbsp;Wesley F. Vaz,&nbsp;Jean M. F. Custódio,&nbsp;Caridad N. Pérez and Hamilton B. Napolitano*,&nbsp;","doi":"10.1021/acsomega.4c0574210.1021/acsomega.4c05742","DOIUrl":"https://doi.org/10.1021/acsomega.4c05742https://doi.org/10.1021/acsomega.4c05742","url":null,"abstract":"<p >Biodiesel offers an alternative to fossil fuels, primarily because it is derived from renewable sources, with the potential to mitigate issues such as pollutant and greenhouse gas emissions, resource scarcity, and the market instability of petroleum derivatives. However, lower durability and stability pose challenges. To address this, researchers worldwide are exploring technologies that employ specific molecules to slow down biodiesel’s oxidation process, thereby preserving its key physicochemical properties. This study investigates heterocyclic dihydroquinolinone derivatives as potential additives to enhance the oxidative stability of diesel-biodiesel blends. Comprehensive structural and computational analyses were carried out by density functional theory to investigate the reactivity aspects of these compounds as potential additive candidates. The supramolecular arrangements were predominantly stabilized by weak molecular interactions, such as C–H···O and C–H···π, which are associated with antioxidant and antibacterial properties. We demonstrate that these groups can act as electron-donating or electron-withdrawing substituents. We explored frontier molecular orbitals, which provide insights into chemical reactivity, acidity, basicity, and the best oxidizing and reducing agents. Finally, the molecular chemical potential maps indicate the nucleophilic and electrophilic regions and the Fukui indices show the sites of nucleophilic, electrophilic, and radical attacks. This comprehensive study paves the way to understanding how dihydroquinolinone-based compounds serve as alternatives for fuel additives.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":"9 50","pages":"49188–49204 49188–49204"},"PeriodicalIF":3.7,"publicationDate":"2024-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsomega.4c05742","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842104","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Metal-Free Synthesis of Functionalized Indolizines via a Cascade Michael/SN2/Aromatization Reaction of 2-Alkylazaarene Derivatives with Bromonitroolefins","authors":"Kangbiao Chen,&nbsp;Rui Zhou,&nbsp;Gaofeng Zhu,&nbsp;Lei Tang,&nbsp;Lu Huang* and Qing He*,&nbsp;","doi":"10.1021/acsomega.4c0929510.1021/acsomega.4c09295","DOIUrl":"https://doi.org/10.1021/acsomega.4c09295https://doi.org/10.1021/acsomega.4c09295","url":null,"abstract":"<p >A transition metal-free domino Michael/S_N2/aromatization annulation of 2-pyridylacetates with bromonitroolefins has been developed. A wide range of substrates containing various substituted groups was compatible with the present methodology and afforded functionalized indolizines with moderate to excellent yield (up to 99% yield). In addition, the potential practicality of the method stood out through scale-up reactions and further transformations to other valuable compounds. In our view, this study is an essential complement for the rapid construction of indolizine derivatives through a metal-free strategy.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":"9 50","pages":"49980–49985 49980–49985"},"PeriodicalIF":3.7,"publicationDate":"2024-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsomega.4c09295","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842737","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"An Efficient and Accessible Hectogram-Scale Synthesis for the Selective O-GlcNAcase Inhibitor Thiamet-G.","authors":"Viktor Holicek, Matthew Deen, Sandeep Bhosale, Roger A Ashmus, David J Vocadlo","doi":"10.1021/acsomega.4c06141","DOIUrl":"https://doi.org/10.1021/acsomega.4c06141","url":null,"abstract":"<p><p>Altered levels of intracellular protein glycosylation with O-linked β-N-acetylglucosamine (O-GlcNAc) have emerged as being involved in various cancers and neurodegenerative diseases. OGA inhibitors have proven critically useful as tools to help understand the roles of O-GlcNAc, yet accessing large quantities of inhibitors necessary for many animal studies remains a challenge. Herein is described a scalable method to produce Thiamet-G, a potent, selective, and widely used brain-permeable OGA inhibitor. This synthetic route begins with inexpensive precursor, requires no column chromatography, employs simple nontoxic reagents, and in a single campaign can furnish several hundred grams of crystalline Thiamet-G in an overall yield of 44% over six steps.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":"9 50","pages":"49223-49228"},"PeriodicalIF":3.7,"publicationDate":"2024-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11656354/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142875316","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Electrorefining of Crude Solder for the Production of Fine Solder in Methanesulfonic Acid Medium: Electrolyte Conductivity and Electrorefining Process","authors":"Yuhui Zhang,&nbsp;Kunyun He,&nbsp;Bingjie Jin* and Jin Luan,&nbsp;","doi":"10.1021/acsomega.4c0847010.1021/acsomega.4c08470","DOIUrl":"https://doi.org/10.1021/acsomega.4c08470https://doi.org/10.1021/acsomega.4c08470","url":null,"abstract":"<p >At present, the refining of crude solder has many drawbacks such as high energy consumption, high environmental pollution, equipment corrosion, and low current efficiency. Therefore, a new technique for refining crude solder is of great practical importance. In this work, the electrorefining of crude solder in methanesulfonic acid (MSA) medium was studied. The conductivities of tin─MSA solutions had been measured and modeled to characterize the electrolyte. The effects of the electrorefining conditions on the electrorefining process were investigated systematically. The cell voltage, current efficiency, and fine solder appearance were used to characterize the electrorefining performance. Some operating parameters of the electrorefining process are established as follows: current density 207 A/m², tin concentration 120–160 g/L, free-MSA concentration 90–120 g/L, electrode spacing 4 cm, and temperature 305.15–315.15 K. Under these conditions, the average cell voltage is 0.30 V and the current efficiency is 99.31%. The total content of tin and lead of the fine solder with good product appearance is &gt;99.99%. This technique offers low energy consumption, high productivity, and low environmental pollution.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":"9 50","pages":"49778–49785 49778–49785"},"PeriodicalIF":3.7,"publicationDate":"2024-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsomega.4c08470","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142850368","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Cooperative Molecular Interaction-Based Highly Efficient Capturing of Ultrashort- and Short-Chain Emerging Per- and Polyfluoroalkyl Substances Using Multifunctional Nanoadsorbents.","authors":"Avijit Pramanik, Olorunsola Praise Kolawole, Sanchita Kundu, Kaelin Gates, Shivangee Rai, Manoj K Shukla, Paresh Chandra Ray","doi":"10.1021/acsomega.4c07159","DOIUrl":"https://doi.org/10.1021/acsomega.4c07159","url":null,"abstract":"<p><p>The short-chain (C₄ to C₇) and ultrashort-chain (C₃ to C₂) per- and polyfluoroalkyl substances (PFAS) are bioaccumulative, carcinogenic to humans, and harder to remove using current technologies, which are often detected in drinking and environmental water samples. Herein, we report the development of nonafluorobutanesulfonyl (NFBS) and polyethylene-imine (PEI)-conjugated Fe₃O₄ magnetic nanoparticle-based magnetic nanoadsorbents and demonstrated that the novel adsorbent has the capability for highly efficient removal of six different short- and ultrashort-chain PFAS from drinking and environmental water samples. Reported experimental data indicates that by capitalizing the cooperative hydrophobic, fluorophilic, and electrostatic interaction processes, NFBS-PEI-conjugated magnetic nanoadsorbents can remove ∼100% short-chain perfluorobutanesulfonic acid within 30 min from the water sample with a maximum absorption capacity <i>q</i> _m of ∼234 mg g^-1. Furthermore, to show how cooperative interactions are necessary for effective capturing of ultrashort and short PFAS, a comparative study has been performed using PEI-attached magnetic nanoadsorbents without NFBS and acid-functionalized magnetic nanoadsorbents without PEI and NFBS. Reported data show that the ultrashort-chain perfluoropropanesulfonic acid capture efficiency is the highest for the NFBS-PEI-attached nanoadsorbent (<i>q</i> _m ∼ 187 mg g^-1) in comparison to the PEI-attached nanoadsorbent (<i>q</i> _m ∼ 119 mg g^-1) or carboxylic acid-attached nanoadsorbent (<i>q</i> _m ∼ 52 mg g^-1). In addition, the role of cooperative molecular interactions in highly efficient removal of ultrashort-chain PFAS has been analyzed in detail. Moreover, reported data demonstrate that nanoadsorbents can be used for effective removal of short-chain PFAS (<92%) and ultrashort-chain PFAS (<70%) simultaneously from reservoir, lake, tape, and river water samples within 30 min, which shows the potential of nanoadsorbents for real-life PFAS remediation.</p>","PeriodicalId":22,"journal":{"name":"ACS Omega","volume":"9 50","pages":"49452-49462"},"PeriodicalIF":3.7,"publicationDate":"2024-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11656356/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142875338","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}