ACS Physical Chemistry Au最新文献_第3页

IF 3.7

ACS Physical Chemistry Au Pub Date : 2025-07-23

Mohamad Toutounji*,

引用次数: 0

IF 3.7

ACS Physical Chemistry Au Pub Date : 2025-07-23

Sebastian Baumgart*, Axel Groß and Mohsen Sotoudeh*,

引用次数: 0

Evaluation of Structural and Electrochemical Properties of Supercapacitors with Graphene Electrodes and Hydrated Pure or Mixed [bmim]-Based Ionic Liquids via Molecular Dynamics. 基于分子动力学的石墨烯电极和水合纯或混合[bmim]基离子液体超级电容器结构和电化学性能评价

IF 4.3

ACS Physical Chemistry Au Pub Date : 2025-07-15 eCollection Date: 2025-09-24 DOI: 10.1021/acsphyschemau.5c00036

Lucas de S Silva, Guilherme Colherinhas

{"title":"Evaluation of Structural and Electrochemical Properties of Supercapacitors with Graphene Electrodes and Hydrated Pure or Mixed [bmim]-Based Ionic Liquids via Molecular Dynamics.","authors":"Lucas de S Silva, Guilherme Colherinhas","doi":"10.1021/acsphyschemau.5c00036","DOIUrl":"10.1021/acsphyschemau.5c00036","url":null,"abstract":"This study investigates the effect of anion composition on the performance of supercapacitors (SCs) using hydrated ionic liquids and graphene electrodes, focusing on comparing pure and mixed electrolytes. Systems containing [bmim] paired with NO3 -, ClO4 -, and Br- were evaluated to assess their impact on electric double layer (EDL) formation and electrochemical behavior. Molecular dynamics (MD) simulations were performed under varying surface polarization, focusing on interaction energies, species distribution, capacitance, and projected energy density. Capacitance values ranged from 2.30 to 2.55 μF/cm2, while energy densities varied between 5.03 and 5.58 J/g, depending on electrolyte composition. The results show that small, mobile anions like Br- promote more compact EDLs and higher capacitance, even with weak electrode interactions. NO3 - contributes to interfacial organization through hydrogen bonding with water. Mixed anion systems demonstrated competitive performance, with the best results obtained by combining high ion mobility and structural organization. This suggests that hybrid electrolytes are a promising strategy for optimizing energy storage in ionic liquid-based SCs.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 5","pages":"519-532"},"PeriodicalIF":4.3,"publicationDate":"2025-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12464776/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145186930","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

Introducing the Tutorial Manuscript Type at the ACS Au Community Journals 介绍ACS Au社区期刊的教程稿件类型。

IF 4.3

ACS Physical Chemistry Au Pub Date : 2025-07-10 DOI: 10.1021/acsphyschemau.5c00050

Squire J. Booker, Stephanie L. Brock, Xiangdong Li, Géraldine Masson, Sébastien Perrier, Vivek V. Ranade, Raymond E. Schaak, Gemma C. Solomon and Shelley D. Minteer*,

引用次数: 0

Quantum Monte Carlo Approaches to Na Intercalation on Bilayer Graphene. 双层石墨烯上Na嵌入的量子蒙特卡罗方法。

IF 4.3

ACS Physical Chemistry Au Pub Date : 2025-06-25 eCollection Date: 2025-09-24 DOI: 10.1021/acsphyschemau.5c00025

Hyeondeok Shin, Anouar Benali, Christopher S Johnson

{"title":"Quantum Monte Carlo Approaches to Na Intercalation on Bilayer Graphene.","authors":"Hyeondeok Shin, Anouar Benali, Christopher S Johnson","doi":"10.1021/acsphyschemau.5c00025","DOIUrl":"10.1021/acsphyschemau.5c00025","url":null,"abstract":"We have performed Quantum Monte Carlo (QMC) simulations on Na-intercalated bilayer graphene to study the evolution of electronic and optical properties upon Na intercalation into hard carbon layers. The objective was to model the optimal configuration of Na intercalation into a hard carbon matrix containing graphene regions. Our study showed that Na intercalation can be energetically stabilized at large interlayer distances (over 6 Å) in both AA- and AB-stacked bilayer graphene. In the QMC results, we found a significant band gap opening at the equilibrium interlayer distance of Na-intercalated bilayer graphene, while corresponding density functional theory (DFT) results showed no gap. This difference between DFT and QMC results indicates that the gap opening induced by Na intercalation into a hard carbon is underestimated within the DFT framework. In addition, a zigzag configuration of Na atoms was found to be energetically stable at interlayer distances up to 10 Å, leading us to predict the existence of a local minimum of Na intercalation at large interlayer distance. These computation and modeling results can provide guidance on how to synthesize and optimize hard carbon with bilayer graphene regions that permit a zigzag intercalation configuration that will maximize and stabilize sodium hosting.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 5","pages":"478-489"},"PeriodicalIF":4.3,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12464765/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145186982","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

Understanding the Binding and Structures in Model Complexes of Polypeptides and Cofactors. 多肽和辅因子模型配合物的结合和结构研究。

IF 4.3

ACS Physical Chemistry Au Pub Date : 2025-06-17 eCollection Date: 2025-09-24 DOI: 10.1021/acsphyschemau.5c00033

Yinan Li, Kenny K Y Lun, Justin Kai-Chi Lau, Jonathan Martens, Giel Berden, Jos Oomens, Alan C Hopkinson, K W Michael Siu, Ivan K Chu

{"title":"Understanding the Binding and Structures in Model Complexes of Polypeptides and Cofactors.","authors":"Yinan Li, Kenny K Y Lun, Justin Kai-Chi Lau, Jonathan Martens, Giel Berden, Jos Oomens, Alan C Hopkinson, K W Michael Siu, Ivan K Chu","doi":"10.1021/acsphyschemau.5c00033","DOIUrl":"10.1021/acsphyschemau.5c00033","url":null,"abstract":"Competitive binding between metal cofactors and functional groups of polypeptides results in a diversity of structures and chemistries in metalloproteins. Herein, we examined elements of this competitive binding using [metal-(auxiliary ligand)-(peptide)] complexes, where the metal-(auxiliary ligand) combinations are CuII(terpy)2+, CoIII(salen)+, and FeIII(salen)+ and the peptides are either the dipeptide arginine-tyrosine (RY) or the tripeptide arginine-tyrosine-glycine (RYG). Structural diversity was established and substantiated via tandem mass spectrometry, with and without peptide derivatization and substitution. All the complexes dissociated to give high abundances of the peptide radical cations, but the structures of these ions differ depending on the composition of the preceding metal complex. Density functional theory calculations provided insights into different binding modes within the complexes and also provided details of the mechanisms by which different [RY]•+ and [RYG]•+ ions fragment. Infrared multiple-photon dissociation spectroscopy established that [Cu-(terpy)-RYG]2+ is bound through the carboxylate group, but calculations showed that it can convert to the phenolate-bound structure under a low-energy barrier. Despite the variety and apparent complexity in binding, the overall chemistry could be characterized using intrinsic acid-base chemistry and the concept of hard/soft Lewis acids/bases. The resulting complex structures were experimentally probed and were found to be in accordance with predictions. For the complexes, the drive toward energy minimization can take several pathways that involve multiple functional groups, thereby leading to a rich chemistry.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 5","pages":"508-518"},"PeriodicalIF":4.3,"publicationDate":"2025-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12464774/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145186969","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

Liquid-Solid Phase Transitions in Nanoscale Mixtures of Water and Organic Substances by the Data of NMR Spectroscopy. 纳米尺度水与有机物混合物液固相变的核磁共振数据研究。

IF 4.3

ACS Physical Chemistry Au Pub Date : 2025-06-17 eCollection Date: 2025-09-24 DOI: 10.1021/acsphyschemau.5c00029

Tetiana Krupska, Myroslav Lenov, Qiliang Wei, Jinju Zheng, Weiyou Yang, Volodymyr Turov

{"title":"Liquid-Solid Phase Transitions in Nanoscale Mixtures of Water and Organic Substances by the Data of NMR Spectroscopy.","authors":"Tetiana Krupska, Myroslav Lenov, Qiliang Wei, Jinju Zheng, Weiyou Yang, Volodymyr Turov","doi":"10.1021/acsphyschemau.5c00029","DOIUrl":"10.1021/acsphyschemau.5c00029","url":null,"abstract":"The process of water clustering in the interparticle gaps of hydrophilic (A-300) and hydrophobic (AM1) silicas in different media was studied using 1H NMR spectroscopy. It has been established that when equal amounts (100 mg/g) of water and oil are introduced into the interparticle gaps of compacted hydrophilic or hydrophobic silica by grinding under the influence of mechanical load, the water transforms into a nanosized state with cluster radii in the range of 1-50 nm. In air, the main part of water is in a strongly associated state with a network of hydrogen bonds similar to liquid water. Replacing air with a chloroform medium leads to the stabilization of weakly associated forms of water, which are observed in the NMR spectra in the form of one or several signals with chemical shifts δH = 1-2 ppm. A comparison of the intensities of the NMR signals of water and oil allows us to conclude that the oil is partially frozen not only in air, but also in chloroform, which has unlimited solubility in relation to oil. In the medium of acetone, which is capable of dissolving both water and oil, in the interparticle gaps of hydrophobic silica, the formation of several types of clusters of strongly and weakly associated water is observed, existing as spatially separated nanodroplets, slowly (on the NMR time scale) exchanging protons or molecules with each other. It has been shown that the hydrophobic walls of silica particles have such an ordering effect on clusters of water and acetone, oil or TMS located in the interparticle gaps that a significant part of it turns into a solid state at temperatures (up to 287 K), which is several tens of degrees higher than the bulk freezing temperature.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 5","pages":"501-507"},"PeriodicalIF":4.3,"publicationDate":"2025-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12464749/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145187008","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

Ultra-Fast Electrochemical Expansion for Rapid Enhancement of Graphite Paper Electrode 石墨纸电极快速强化的超快速电化学膨胀。

IF 4.3

ACS Physical Chemistry Au Pub Date : 2025-06-12 DOI: 10.1021/acsphyschemau.5c00014

Praeploy Chomkhuntod, Sukanlaya Kornnum, Sirintra Arayawate, Bin Wang and Pawin Iamprasertkun*,

{"title":"Ultra-Fast Electrochemical Expansion for Rapid Enhancement of Graphite Paper Electrode","authors":"Praeploy Chomkhuntod, Sukanlaya Kornnum, Sirintra Arayawate, Bin Wang and Pawin Iamprasertkun*, ","doi":"10.1021/acsphyschemau.5c00014","DOIUrl":"10.1021/acsphyschemau.5c00014","url":null,"abstract":"Graphite paper is widely used in energy storage systems such as batteries and supercapacitors due to its availability, cost, and excellent chemical and thermal stability. However, its hydrophobic surface and dense structure limit electrolytic ion diffusion in aqueous supercapacitors, reducing electrochemical performance. To address these issues, graphite paper was treated with mild acid solution and electrochemically oxidized for varying durations to enhance its properties for high-performance supercapacitors. Acid treatment not only expanded the graphite but also functionalized its surface, making it more hydrophilic, as confirmed by FTIR and contact angle measurements. This modification improved the electrode’s electrochemical performance by facilitating better ion diffusion and insertion, resulting in increased specific capacitance. After 5 min of treatment, the graphite layers enlarged from 35 to 469 μm, resulting in an enhanced specific capacitance of 219 F g–1 at 10 mV s–1 but poor cycling stability with 80% capacitance retention after 500 cycles. In contrast, the 3 min treatment achieved a specific capacitance of 113 F g–1 with excellent cycling stability without significant capacitance fading. These results highlight the importance of optimizing both the structural and chemical properties of graphite for achieving high performance and long cycling stability.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 4","pages":"318–326"},"PeriodicalIF":4.3,"publicationDate":"2025-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12291138/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144733645","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

The Effect of Ceramide Ratio on the Membrane Curvature of Mimetic Models of Matrix Vesicles. 神经酰胺比例对基质囊泡模拟模型膜曲率的影响。

IF 4.3

ACS Physical Chemistry Au Pub Date : 2025-06-09 eCollection Date: 2025-09-24 DOI: 10.1021/acsphyschemau.5c00010

Diane C A Lima, Guilherme Volpe Bossa, Pietro Ciancaglini, Ana P Ramos, Thereza A Soares

{"title":"The Effect of Ceramide Ratio on the Membrane Curvature of Mimetic Models of Matrix Vesicles.","authors":"Diane C A Lima, Guilherme Volpe Bossa, Pietro Ciancaglini, Ana P Ramos, Thereza A Soares","doi":"10.1021/acsphyschemau.5c00010","DOIUrl":"10.1021/acsphyschemau.5c00010","url":null,"abstract":"The lipid composition of membrane systems plays a critical role in regulating their structural dynamics and curvature, particularly in the biological context of matrix vesicles (MVs) formation during bone mineralization. Recent evidence suggests that the lipid composition of MVs, particularly the balance between sphingomyelin (SM) and ceramide (CER), influences their curvature and stability. We report on the impact of SM and CER ratios on membrane curvature through surface pressure-area isotherm measurements and molecular dynamics (MD) simulations at atomistic and coarse-grained levels. Our findings reveal that increasing the CER content up to 25% significantly enhances membrane curvature, as demonstrated by changes in experimental compressibility moduli and lateral pressure profiles. The lateral pressure profiles and spontaneous bending moments calculated from MD simulations of osteoblast-mimetic membrane models suggest a strong propensity for curvature, particularly in asymmetrical bilayers. It also reveals the role of CER-rich domains in the stabilization of membrane curvature, potentially facilitating the budding processes critical for MVs formation in osteoblasts. These findings underscore the critical role of lipid composition in the mechanisms driving MVs biogenesis.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 5","pages":"456-466"},"PeriodicalIF":4.3,"publicationDate":"2025-06-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12464780/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145187010","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

ALX/FPR2 Receptor Activation by Inflammatory (fMLFII) and Pro-resolving (LXA4 and RvD3) Agonists 炎症（fMLFII）和促溶解（LXA4和RvD3）激动剂激活ALX/FPR2受体。

IF 4.3

ACS Physical Chemistry Au Pub Date : 2025-06-06 DOI: 10.1021/acsphyschemau.5c00008

Vinicius S. Nunes*, Charles N. Serhan, Odonírio Abrahão Jr. and Alexandre P. Rogério,

{"title":"ALX/FPR2 Receptor Activation by Inflammatory (fMLFII) and Pro-resolving (LXA4 and RvD3) Agonists","authors":"Vinicius S. Nunes*, Charles N. Serhan, Odonírio Abrahão Jr. and Alexandre P. Rogério, ","doi":"10.1021/acsphyschemau.5c00008","DOIUrl":"10.1021/acsphyschemau.5c00008","url":null,"abstract":"Nine structures of the ALX/FPR2 receptor are currently deposited in the PDB. In seven structures, the receptor is complexed with formylated peptides. In all seven structures, residue D106 is indicated as acting in the ALX/FPR2 receptor activation in addition to residues R201 and R205. Here, we performed docking simulations and long-term molecular dynamics simulations to investigate the ALX/FPR2 receptor activation using two pro-resolution agonists (lipoxin A4 (LXA4) and resolvin D3 (RvD3)) and a formylated peptide pro-inflammatory agonist (fMLFII). We have analyzed the receptor’s activation state, electrostatic interactions, and the binding affinities of the complexes receptor-agonist using the MM/PBSA approach. The results showed that LXA4 and fMLFII kept the receptor in an active state by a higher simulation time when compared to RvD3. Only R201 and R205 were considered key residues in the ALX/FPR2 receptor activation by all agonists. The electrostatic interaction analysis confirmed the importance of these residues in ALX/FPR2 receptor activation. Furthermore, only fMLLII showed interactions with residue D106. The binding free energy calculations indicated that the electrostatic component significantly binds the agonists to the receptor. Overall, the results from this study provide new insights into the ALX/FPR2 receptor activation mechanisms, reinforcing the role of critical residues and interactions in the binding of pro-resolution and inflammatory agonists.","PeriodicalId":29796,"journal":{"name":"ACS Physical Chemistry Au","volume":"5 4","pages":"367–374"},"PeriodicalIF":4.3,"publicationDate":"2025-06-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12291131/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144733636","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