ACS Physical Chemistry Au最新文献_第3页

The Effect of Mixtures and Additives on Dissolving Surfactant Lamellar Phases 混合物和添加剂对溶解表面活性剂层状相的影响

IF 3.7

ACS Physical Chemistry Au Pub Date : 2024-07-15 DOI: 10.1021/acsphyschemau.4c0001310.1021/acsphyschemau.4c00013

Mitha Aljabri*, and , Thomas Rodgers,

{"title":"The Effect of Mixtures and Additives on Dissolving Surfactant Lamellar Phases","authors":"Mitha Aljabri*,  and , Thomas Rodgers, ","doi":"10.1021/acsphyschemau.4c0001310.1021/acsphyschemau.4c00013","DOIUrl":"https://doi.org/10.1021/acsphyschemau.4c00013https://doi.org/10.1021/acsphyschemau.4c00013","url":null,"abstract":"Understanding the dissolution process of surfactant solutions is important in formulating product design processes. The main goal of this study is to gain further insights into how additives and mixtures affect surfactant dissolution processes. To achieve this goal, dissipative particle dynamic simulations were used. Lamellar phases at 80% volume of surfactant were initially equilibrated with water. After reaching an equilibrium state, the dissolution simulations were carried out for different surfactant mixtures. To track the dissolution process, different metrics were used, including visual analysis, local concentration analysis, diffusion, and cluster size calculations. Results show that by having a mixture of surfactants, the diffusion of the micelles is not affected only by the size of the micelles as in pure surfactant systems, but there is also an effect due to the composition of the micelles. When oil is added to a surfactant system, the system acts like a longer chain surfactant system, but only when the chain of oil becomes sufficiently long.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsphyschemau.4c00013","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142318293","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

Tailor-Made Design of Three-Dimensional Batteries Using a Simple, Accurate Geometry Optimization Scheme 利用简单精确的几何优化方案量身定制三维电池设计

IF 3.7

ACS Physical Chemistry Au Pub Date : 2024-07-15 DOI: 10.1021/acsphyschemau.4c0003910.1021/acsphyschemau.4c00039

Kaito Miyamoto*,

{"title":"Tailor-Made Design of Three-Dimensional Batteries Using a Simple, Accurate Geometry Optimization Scheme","authors":"Kaito Miyamoto*, ","doi":"10.1021/acsphyschemau.4c0003910.1021/acsphyschemau.4c00039","DOIUrl":"https://doi.org/10.1021/acsphyschemau.4c00039https://doi.org/10.1021/acsphyschemau.4c00039","url":null,"abstract":"In the rapidly evolving Internet of Things (IoT) society, the demand for microbatteries with high areal energy density is surging. As a promising strategy to enhance areal energy density, three-dimensional (3D) batteries have attracted attention. The feature of 3D batteries is the decoupling of the electrode thickness from the ion-transport distance through the modification of the spatial arrangement of the positive and negative electrodes beyond the conventional parallel plates configuration. This allows for the accommodation of a larger amount of active materials without increasing internal resistance. However, identifying the optimal 3D geometry is a complex task, as it depends on printable materials, the resolution of the fabrication equipment, as well as battery usage, which constitutes a multiobjective optimization problem. To overcome this challenge, we propose a novel approach to determine the optimal 3D microbattery geometry. Our innovative method involves a 3D battery optimization system, which integrates an automatic geometry generator with a quick and accurate performance simulator. This approach allows, for the first time, the discovery of material- and discharge-current-dependent optimal geometries. We successfully apply this optimization scheme to two standard electrode pairs (LiFePO4/Li4Ti5O12 and LiNi0.5Mn0.3Co0.2O2/graphite), demonstrating a significant increase in energy density (30%–40% greater than the current state-of-the-art geometry), particularly under high current conditions. These findings underscore the importance of tailor-made batteries for diverse IoT applications and showcase the potential of our approach in realizing such designs.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsphyschemau.4c00039","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142318291","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

Ratiometric Chemosensors That Are Capable of Quantifying Hydrostatic Pressure Stimulus: A Case of Porphyrin Tweezers 能够量化静水压力刺激的比率化学传感器：卟啉镊子案例

IF 3.7

ACS Physical Chemistry Au Pub Date : 2024-07-12 DOI: 10.1021/acsphyschemau.4c00025

Seiya Ono, Tomokazu Kinoshita, Hiroshi Iwasaki, Yoshitane Imai, G. Fukuhara

引用次数: 0

Ratiometric Chemosensors That Are Capable of Quantifying Hydrostatic Pressure Stimulus: A Case of Porphyrin Tweezers 能够量化静水压力刺激的比率化学传感器：卟啉镊子案例

IF 3.7

ACS Physical Chemistry Au Pub Date : 2024-07-12 DOI: 10.1021/acsphyschemau.4c0002510.1021/acsphyschemau.4c00025

Seiya Ono, Tomokazu Kinoshita, Hiroshi Iwasaki, Yoshitane Imai and Gaku Fukuhara*,

{"title":"Ratiometric Chemosensors That Are Capable of Quantifying Hydrostatic Pressure Stimulus: A Case of Porphyrin Tweezers","authors":"Seiya Ono, Tomokazu Kinoshita, Hiroshi Iwasaki, Yoshitane Imai and Gaku Fukuhara*, ","doi":"10.1021/acsphyschemau.4c0002510.1021/acsphyschemau.4c00025","DOIUrl":"https://doi.org/10.1021/acsphyschemau.4c00025https://doi.org/10.1021/acsphyschemau.4c00025","url":null,"abstract":"Investigating chemosensors that are capable of quantifying pressure in solution, particularly hydrostatic pressure, which is one of the mechanical forces, is an attractive challenge in chemistry from the viewpoint of “mechano”-science. Herein, we report the investigation of chiral porphyrin tweezers, Por-Cy and Por-DPhEt, comprising different flexible linkers; Por-Cy and Por-DPhEt displayed distinct ratiometric signaling by using the higher excited S2 state with a standard excited S1 level. A novel operative mechanism using the S1/S2 fluorescence ratio was revealed using hydrostatic pressure-ultraviolet/visible (UV/vis), fluorescence/excitation, circular dichroism spectroscopy, and lifetime measurements, which can be further controlled by the open-closed conformational change inherent in the tweezer skeleton. Furthermore, the fluorescent chiral tweezers exhibited a promising |glum| of 2.9 × 10–3, indicating that they are potential candidates for sensory applications in chiral environments. This study provides opportunities for the development of smart pressure-responsive chemosensors.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsphyschemau.4c00025","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142318290","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

Isomeric Identification of the Nitroindole Chromophore in Indole + NO3 Organic Aerosol 吲哚 + NO3 有机气溶胶中硝基吲哚发色团的异构体鉴定

IF 3.7

ACS Physical Chemistry Au Pub Date : 2024-07-11 DOI: 10.1021/acsphyschemau.4c0004410.1021/acsphyschemau.4c00044

Avery B. Dalton, Lisa M. Wingen and Sergey A. Nizkorodov*,

{"title":"Isomeric Identification of the Nitroindole Chromophore in Indole + NO3 Organic Aerosol","authors":"Avery B. Dalton, Lisa M. Wingen and Sergey A. Nizkorodov*, ","doi":"10.1021/acsphyschemau.4c0004410.1021/acsphyschemau.4c00044","DOIUrl":"https://doi.org/10.1021/acsphyschemau.4c00044https://doi.org/10.1021/acsphyschemau.4c00044","url":null,"abstract":"Oxidation of indole by nitrate radical (NO3) was previously proposed to form nitroindole, largely responsible for the brown color of indole secondary organic aerosol (SOA). As there are seven known nitroindole isomers, we used chromatographic separation to show that a single nitroindole isomer is produced in the indole + NO3 reaction and definitively assigned it to 3-nitroindole by comparison with chromatograms of nitroindole standards. Mass spectra of aerosolized 3-nitroindole particles were recorded with an aerosol mass spectrometer and directly compared to mass spectra of SOA from smog chamber oxidation of indole by NO3 in order to help identify peaks unique to nitroindole (m/z 162, 132, and 116). Quantum chemical calculations were done to determine the energetics of hypothesized indole + NO3 intermediates and products. The combination of these data suggests a mechanism, wherein a hydrogen atom is first abstracted from the N–H bond in indole, followed by isomerization to a carbon-centered radical in the 3-position and followed by addition of NO2. Alternative mechanisms involving a direct abstraction of a H atom from a C–H bond or a NO3 addition to the ring are predicted to be energetically unfavorable from large barriers for the initial reaction steps.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsphyschemau.4c00044","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142318289","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

Isomeric Identification of the Nitroindole Chromophore in Indole + NO3 Organic Aerosol 吲哚 + NO3 有机气溶胶中硝基吲哚发色团的异构体鉴定

ACS Physical Chemistry Au Pub Date : 2024-07-11 DOI: 10.1021/acsphyschemau.4c00044

Avery B. Dalton, Lisa M. Wingen, Sergey A. Nizkorodov

{"title":"Isomeric Identification of the Nitroindole Chromophore in Indole + NO3 Organic Aerosol","authors":"Avery B. Dalton, Lisa M. Wingen, Sergey A. Nizkorodov","doi":"10.1021/acsphyschemau.4c00044","DOIUrl":"https://doi.org/10.1021/acsphyschemau.4c00044","url":null,"abstract":"Oxidation of indole by nitrate radical (NO3) was previously proposed to form nitroindole, largely responsible for the brown color of indole secondary organic aerosol (SOA). As there are seven known nitroindole isomers, we used chromatographic separation to show that a single nitroindole isomer is produced in the indole + NO3 reaction and definitively assigned it to 3-nitroindole by comparison with chromatograms of nitroindole standards. Mass spectra of aerosolized 3-nitroindole particles were recorded with an aerosol mass spectrometer and directly compared to mass spectra of SOA from smog chamber oxidation of indole by NO3 in order to help identify peaks unique to nitroindole (m/z 162, 132, and 116). Quantum chemical calculations were done to determine the energetics of hypothesized indole + NO3 intermediates and products. The combination of these data suggests a mechanism, wherein a hydrogen atom is first abstracted from the N–H bond in indole, followed by isomerization to a carbon-centered radical in the 3-position and followed by addition of NO2. Alternative mechanisms involving a direct abstraction of a H atom from a C–H bond or a NO3 addition to the ring are predicted to be energetically unfavorable from large barriers for the initial reaction steps.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141614222","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

A Vision for the Future of Neutron Scattering and Muon Spectroscopy in the 2050s 2050 年代中子散射和μ介子能谱学的未来展望

ACS Physical Chemistry Au Pub Date : 2024-07-10 DOI: 10.1021/acsphyschemau.4c00026

Stewart F. Parker, Peter J. Baker, Robert McGreevy

引用次数: 0

A Vision for the Future of Neutron Scattering and Muon Spectroscopy in the 2050s 2050 年代中子散射和μ介子能谱学的未来展望

IF 3.7

ACS Physical Chemistry Au Pub Date : 2024-07-10 DOI: 10.1021/acsphyschemau.4c0002610.1021/acsphyschemau.4c00026

Stewart F. Parker*, Peter J. Baker and Robert McGreevy,

引用次数: 0

Understanding the Vibrational Structure and Ultrafast Dynamics of the Metal Carbonyl Precatalyst [Mn(ppy)(CO)4] 了解金属羰基前催化剂 [Mn(ppy)(CO)4] 的振动结构和超快动力学特性

ACS Physical Chemistry Au Pub Date : 2024-07-09 DOI: 10.1021/acsphyschemau.4c00037

Jonathan B. Eastwood, Barbara Procacci, Sabina Gurung, Jason M. Lynam, Neil T. Hunt

{"title":"Understanding the Vibrational Structure and Ultrafast Dynamics of the Metal Carbonyl Precatalyst [Mn(ppy)(CO)4]","authors":"Jonathan B. Eastwood, Barbara Procacci, Sabina Gurung, Jason M. Lynam, Neil T. Hunt","doi":"10.1021/acsphyschemau.4c00037","DOIUrl":"https://doi.org/10.1021/acsphyschemau.4c00037","url":null,"abstract":"The solution phase structure, vibrational spectroscopy, and ultrafast relaxation dynamics of the precatalyst species [Mn(ppy)(CO)4] (1) in solution have been investigated using ultrafast two-dimensional infrared (2D-IR) spectroscopy. By comparing 2D-IR data with the results of anharmonic density functional theory (DFT) calculations, we establish an excellent agreement between measured and predicted inter-mode couplings of the carbonyl stretching vibrational modes of 1 that relates to the atomic displacements of axial and equatorial ligands in the modes and the nature of the molecular orbitals involved in M–CO bonding. Measurements of IR pump–probe spectra and 2D-IR spectra as a function of waiting time reveal the presence of ultrafast (few ps) intramolecular vibrational energy redistribution between carbonyl stretching modes prior to vibrational relaxation. The vibrational relaxation times of the CO-stretching modes of 1 are found to be relatively solvent-insensitive, suggestive of limited solvent–solute interactions in the ground electronic state. Overall, these data provide a detailed picture of the complex potential energy surface, bonding and vibrational dynamics of 1, establishing a fundamental basis for the next steps in understanding and modulating precatalyst behavior.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141568731","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

Understanding the Vibrational Structure and Ultrafast Dynamics of the Metal Carbonyl Precatalyst [Mn(ppy)(CO)4] 了解金属羰基前催化剂 [Mn(ppy)(CO)4] 的振动结构和超快动力学特性

IF 3.7

ACS Physical Chemistry Au Pub Date : 2024-07-09 DOI: 10.1021/acsphyschemau.4c0003710.1021/acsphyschemau.4c00037

Jonathan B. Eastwood, Barbara Procacci, Sabina Gurung, Jason M. Lynam* and Neil T. Hunt*,

{"title":"Understanding the Vibrational Structure and Ultrafast Dynamics of the Metal Carbonyl Precatalyst [Mn(ppy)(CO)4]","authors":"Jonathan B. Eastwood, Barbara Procacci, Sabina Gurung, Jason M. Lynam* and Neil T. Hunt*, ","doi":"10.1021/acsphyschemau.4c0003710.1021/acsphyschemau.4c00037","DOIUrl":"https://doi.org/10.1021/acsphyschemau.4c00037https://doi.org/10.1021/acsphyschemau.4c00037","url":null,"abstract":"The solution phase structure, vibrational spectroscopy, and ultrafast relaxation dynamics of the precatalyst species [Mn(ppy)(CO)4] (1) in solution have been investigated using ultrafast two-dimensional infrared (2D-IR) spectroscopy. By comparing 2D-IR data with the results of anharmonic density functional theory (DFT) calculations, we establish an excellent agreement between measured and predicted inter-mode couplings of the carbonyl stretching vibrational modes of 1 that relates to the atomic displacements of axial and equatorial ligands in the modes and the nature of the molecular orbitals involved in M–CO bonding. Measurements of IR pump–probe spectra and 2D-IR spectra as a function of waiting time reveal the presence of ultrafast (few ps) intramolecular vibrational energy redistribution between carbonyl stretching modes prior to vibrational relaxation. The vibrational relaxation times of the CO-stretching modes of 1 are found to be relatively solvent-insensitive, suggestive of limited solvent–solute interactions in the ground electronic state. Overall, these data provide a detailed picture of the complex potential energy surface, bonding and vibrational dynamics of 1, establishing a fundamental basis for the next steps in understanding and modulating precatalyst behavior.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":null,"pages":null},"PeriodicalIF":3.7,"publicationDate":"2024-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsphyschemau.4c00037","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142318364","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