The Journal of Physical Chemistry B最新文献_第9页

Stimuli-Responsive Peptide Liquid Crystals for Tandem Measurements of Residual Chemical Shift Anisotropy and Residual Dipole Coupling in One Sample 刺激响应肽液晶串联测量样品中残余化学位移各向异性和残余偶极子耦合

IF 2.8 2区化学

The Journal of Physical Chemistry B Pub Date : 2025-04-01 DOI: 10.1021/acs.jpcb.4c0800510.1021/acs.jpcb.4c08005

Jin-Hao He, Yan-Ling Yang, Ai-Qing Zhang and Si-Yong Qin*,

{"title":"Stimuli-Responsive Peptide Liquid Crystals for Tandem Measurements of Residual Chemical Shift Anisotropy and Residual Dipole Coupling in One Sample","authors":"Jin-Hao He, Yan-Ling Yang, Ai-Qing Zhang and Si-Yong Qin*, ","doi":"10.1021/acs.jpcb.4c0800510.1021/acs.jpcb.4c08005","DOIUrl":"https://doi.org/10.1021/acs.jpcb.4c08005https://doi.org/10.1021/acs.jpcb.4c08005","url":null,"abstract":"The combined use of residual chemical shift anisotropy (RCSA) and residual dipolar coupling/residual dipole coupling (RDC) could provide highly complementary information about the structure and relative configuration of unknown organic molecules for their elucidation. However, tandem RCSA and RDC measurements in one sample remain a formidable challenge due to their varied testing requirements. Herein, a stimuli-responsive supramolecular liquid crystal self-assembled from an amphiphilic oligopeptide of C19H39–CONH-VVVVKKK-CONH2 was constructed, which underwent a phasic transformation from anisotropy to isotropy when subjected to a thermal treatment. Both the anisotropic and isotropic phases exhibited good stability, facilitating tandem measurements of 13C-{1H}-RCSA and (13C–1H)-RDC in one sample with no need for special instruments or correction procedures. We expect that the joint use of RCSAs and RDCs will significantly improve data accuracy and utility for structural and configurational determination of small organic molecules and even biomacromolecules.","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":"129 14","pages":"3683–3690 3683–3690"},"PeriodicalIF":2.8,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143809854","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Cluster Structure and Ordering in the Nucleation and Growth of Binary Molecular Mixtures. 二元分子混合物成核和生长中的团簇结构和有序。

IF 2.8 2区化学

The Journal of Physical Chemistry B Pub Date : 2025-03-31 DOI: 10.1021/acs.jpcb.5c00430

Joseph Gregory Z Cabinta, Earl Adrian D R Hans, Roosevelt T Tabag, Johnrob Y Bantang, Ricky B Nellas

{"title":"Cluster Structure and Ordering in the Nucleation and Growth of Binary Molecular Mixtures.","authors":"Joseph Gregory Z Cabinta, Earl Adrian D R Hans, Roosevelt T Tabag, Johnrob Y Bantang, Ricky B Nellas","doi":"10.1021/acs.jpcb.5c00430","DOIUrl":"https://doi.org/10.1021/acs.jpcb.5c00430","url":null,"abstract":"A complete understanding of aerosol formation remains elusive due to the microscopic scale and transient occurrence of nucleation. This process is further complicated by the multicomponent nature of atmospheric nucleating systems in which the properties of conucleating compounds influence the affinity of molecules to cluster. Molecular dynamics simulations were performed to investigate homogeneous vapor-liquid nucleation and growth of six binary mixtures composed of water, n-nonane, 1-butanol, and methanol. Structural analyses were performed to understand the dynamic configurations generated from binary nuclei. Geometric structure analysis revealed that clusters were found to be more spherical with increasing cluster size, while composition analysis revealed that more miscible species had less mole fraction variability from an equimolar composition. Radial density profiling and cluster snapshots revealed structural features that were dependent on the miscibility of the nucleating pairs. Homogeneous mixing was observed in n-nonane/1-butanol and water-methanol due to their miscibility. Meanwhile, systems with partial miscibility (water/1-butanol, water/methanol, 1-butanol/methanol, n-nonane/methanol), exhibited preferential ordering into core-shell structures. In water/n-nonane, simultaneous unary nucleation was observed, leading to lens-on-sphere configuration. Microstructure analysis also revealed internal fragmentation within core-shell motifs of water/1-butanol and 1-butanol/methanol. These findings have serious implications in nucleation theories, which lead to valuable insights for the nucleation of naturally occurring multicomponent systems in the atmosphere.","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":" ","pages":""},"PeriodicalIF":2.8,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143750079","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Cluster Structure and Ordering in the Nucleation and Growth of Binary Molecular Mixtures 二元分子混合物成核和生长中的团簇结构和有序

IF 2.8 2区化学

The Journal of Physical Chemistry B Pub Date : 2025-03-31 DOI: 10.1021/acs.jpcb.5c0043010.1021/acs.jpcb.5c00430

Joseph Gregory Z. Cabinta, Earl Adrian D. R. Hans, Roosevelt T. Tabag Jr., Johnrob Y. Bantang and Ricky B. Nellas*,

{"title":"Cluster Structure and Ordering in the Nucleation and Growth of Binary Molecular Mixtures","authors":"Joseph Gregory Z. Cabinta, Earl Adrian D. R. Hans, Roosevelt T. Tabag Jr., Johnrob Y. Bantang and Ricky B. Nellas*, ","doi":"10.1021/acs.jpcb.5c0043010.1021/acs.jpcb.5c00430","DOIUrl":"https://doi.org/10.1021/acs.jpcb.5c00430https://doi.org/10.1021/acs.jpcb.5c00430","url":null,"abstract":"A complete understanding of aerosol formation remains elusive due to the microscopic scale and transient occurrence of nucleation. This process is further complicated by the multicomponent nature of atmospheric nucleating systems in which the properties of conucleating compounds influence the affinity of molecules to cluster. Molecular dynamics simulations were performed to investigate homogeneous vapor–liquid nucleation and growth of six binary mixtures composed of water, n-nonane, 1-butanol, and methanol. Structural analyses were performed to understand the dynamic configurations generated from binary nuclei. Geometric structure analysis revealed that clusters were found to be more spherical with increasing cluster size, while composition analysis revealed that more miscible species had less mole fraction variability from an equimolar composition. Radial density profiling and cluster snapshots revealed structural features that were dependent on the miscibility of the nucleating pairs. Homogeneous mixing was observed in n-nonane/1-butanol and water–methanol due to their miscibility. Meanwhile, systems with partial miscibility (water/1-butanol, water/methanol, 1-butanol/methanol, n-nonane/methanol), exhibited preferential ordering into core–shell structures. In water/n-nonane, simultaneous unary nucleation was observed, leading to lens-on-sphere configuration. Microstructure analysis also revealed internal fragmentation within core–shell motifs of water/1-butanol and 1-butanol/methanol. These findings have serious implications in nucleation theories, which lead to valuable insights for the nucleation of naturally occurring multicomponent systems in the atmosphere.","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":"129 14","pages":"3670–3682 3670–3682"},"PeriodicalIF":2.8,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806787","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Thermodynamics of Isomers and Solubility Prediction in Multicomponent Sugar Solutions. 多组分糖溶液中异构体的热力学及溶解度预测。

IF 2.8 2区化学

The Journal of Physical Chemistry B Pub Date : 2025-03-31 DOI: 10.1021/acs.jpcb.4c08616

Silvio Trespi, Shina Roshanfekr, Marco Mazzotti

引用次数: 0

Thermodynamics of Isomers and Solubility Prediction in Multicomponent Sugar Solutions 多组分糖溶液中异构体的热力学及溶解度预测

IF 2.8 2区化学

The Journal of Physical Chemistry B Pub Date : 2025-03-31 DOI: 10.1021/acs.jpcb.4c0861610.1021/acs.jpcb.4c08616

Silvio Trespi, Shina Roshanfekr and Marco Mazzotti*,

{"title":"Thermodynamics of Isomers and Solubility Prediction in Multicomponent Sugar Solutions","authors":"Silvio Trespi, Shina Roshanfekr and Marco Mazzotti*, ","doi":"10.1021/acs.jpcb.4c0861610.1021/acs.jpcb.4c08616","DOIUrl":"https://doi.org/10.1021/acs.jpcb.4c08616https://doi.org/10.1021/acs.jpcb.4c08616","url":null,"abstract":"A rigorous thermodynamic modeling framework for a system of isomers in chemical equilibrium is developed and applied to the lactose-water system. Through the knowledge of the water activity and of the liquid phase composition, thermodynamically consistent expressions for the activity coefficients of lactose isomers have been derived and used in the context of solid–liquid equilibria to predict the dependence of the saturation concentration of α-lactose on the dissolved β-lactose concentration. We also developed a comprehensive first-principles model that accurately describes the dissolution dynamics of α-lactose monohydrate. The data support the hypothesis that the sugar activity coefficients are a stronger function of the total sugar content rather than of the sugar solution composition. The activity coefficient expressions have been used to quantitatively predict the effect of glucose, galactose, and sucrose on the solubility of α-lactose monohydrate.","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":"129 14","pages":"3661–3669 3661–3669"},"PeriodicalIF":2.8,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.jpcb.4c08616","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806652","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Aggregation-Induced Excitation-Energy Quenching in Fucoxanthin Chlorophyll a/c-Binding Proteins from the Diatom Phaeodactylum tricornutum 三角藻藻藻黄素叶绿素a/c结合蛋白的聚集诱导激发-能量猝灭

IF 2.8 2区化学

The Journal of Physical Chemistry B Pub Date : 2025-03-29 DOI: 10.1021/acs.jpcb.4c0689410.1021/acs.jpcb.4c06894

Yoshifumi Ueno, Ou-Yang Li, Jian-Ren Shen, Tatsuya Tomo, Seiji Akimoto* and Ryo Nagao*,

{"title":"Aggregation-Induced Excitation-Energy Quenching in Fucoxanthin Chlorophyll a/c-Binding Proteins from the Diatom Phaeodactylum tricornutum","authors":"Yoshifumi Ueno, Ou-Yang Li, Jian-Ren Shen, Tatsuya Tomo, Seiji Akimoto* and Ryo Nagao*, ","doi":"10.1021/acs.jpcb.4c0689410.1021/acs.jpcb.4c06894","DOIUrl":"https://doi.org/10.1021/acs.jpcb.4c06894https://doi.org/10.1021/acs.jpcb.4c06894","url":null,"abstract":"Light-harvesting complexes (LHCs) are vital for photosynthesis, capturing light energy and transferring it to photosystems I and II. In diatoms, fucoxanthin chlorophyll (Chl) a/c-binding proteins (FCPs) function as unique LHCs. In this study, we examined the spectral properties of untreated and aggregated FCP complexes (Untreated-FCP and Aggregated-FCP, respectively) from the diatom Phaeodactylum tricornutum. Fluorescence quantum yields and excitation-energy transfer pathways were evaluated using absolute fluorescence spectroscopy and fluorescence decay-associated (FDA) spectra. Aggregation of FCPs significantly enhanced excitation-energy quenching, with a marked decrease in fluorescence quantum yield from 37.6% in Untreated-FCP to 4.8% in Aggregated-FCP. The FDA spectra of Aggregated-FCP showed prominent fluorescence decays with relatively high amplitudes with time constants of 310 ps and 1.6 ns, reflecting distinct alterations in excitation-energy transfer among Chls upon aggregation. These changes were accompanied by long-wavelength shifts and broadening of the fluorescence-emission spectra, characteristics typically observed in aggregated LHCs in land plants. Our results suggest that the structural rearrangement of pigment molecules, driven by changes in Chl–Chl and Chl–Car interactions, underlies the observed excitation-energy quenching upon aggregation. This study provides key insights into the quenching mechanisms of diatom FCPs, offering broader implications for understanding energy regulation in photosynthetic systems.","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":"129 14","pages":"3553–3558 3553–3558"},"PeriodicalIF":2.8,"publicationDate":"2025-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806678","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Aggregation-Induced Excitation-Energy Quenching in Fucoxanthin Chlorophyll a/c-Binding Proteins from the Diatom Phaeodactylum tricornutum. 三角藻藻藻黄素叶绿素a/c结合蛋白的聚集诱导激发-能量猝灭

IF 2.8 2区化学

The Journal of Physical Chemistry B Pub Date : 2025-03-29 DOI: 10.1021/acs.jpcb.4c06894

Yoshifumi Ueno, Ou-Yang Li, Jian-Ren Shen, Tatsuya Tomo, Seiji Akimoto, Ryo Nagao

{"title":"Aggregation-Induced Excitation-Energy Quenching in Fucoxanthin Chlorophyll a/c-Binding Proteins from the Diatom Phaeodactylum tricornutum.","authors":"Yoshifumi Ueno, Ou-Yang Li, Jian-Ren Shen, Tatsuya Tomo, Seiji Akimoto, Ryo Nagao","doi":"10.1021/acs.jpcb.4c06894","DOIUrl":"https://doi.org/10.1021/acs.jpcb.4c06894","url":null,"abstract":"Light-harvesting complexes (LHCs) are vital for photosynthesis, capturing light energy and transferring it to photosystems I and II. In diatoms, fucoxanthin chlorophyll (Chl) a/c-binding proteins (FCPs) function as unique LHCs. In this study, we examined the spectral properties of untreated and aggregated FCP complexes (Untreated-FCP and Aggregated-FCP, respectively) from the diatom Phaeodactylum tricornutum. Fluorescence quantum yields and excitation-energy transfer pathways were evaluated using absolute fluorescence spectroscopy and fluorescence decay-associated (FDA) spectra. Aggregation of FCPs significantly enhanced excitation-energy quenching, with a marked decrease in fluorescence quantum yield from 37.6% in Untreated-FCP to 4.8% in Aggregated-FCP. The FDA spectra of Aggregated-FCP showed prominent fluorescence decays with relatively high amplitudes with time constants of 310 ps and 1.6 ns, reflecting distinct alterations in excitation-energy transfer among Chls upon aggregation. These changes were accompanied by long-wavelength shifts and broadening of the fluorescence-emission spectra, characteristics typically observed in aggregated LHCs in land plants. Our results suggest that the structural rearrangement of pigment molecules, driven by changes in Chl-Chl and Chl-Car interactions, underlies the observed excitation-energy quenching upon aggregation. This study provides key insights into the quenching mechanisms of diatom FCPs, offering broader implications for understanding energy regulation in photosynthetic systems.","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":" ","pages":""},"PeriodicalIF":2.8,"publicationDate":"2025-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143741761","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Ternary Potassium Single Cation Ionic Liquid Electrolyte for Potassium Secondary Batteries 钾二次电池用三元钾单阳离子离子液体电解质

IF 2.8 2区化学

The Journal of Physical Chemistry B Pub Date : 2025-03-28 DOI: 10.1021/acs.jpcb.4c0810510.1021/acs.jpcb.4c08105

Hiroki Yamamoto*, Keigo Kubota*, Jinkwang Hwang, Kazuhiko Matsumoto and Rika Hagiwara,

{"title":"Ternary Potassium Single Cation Ionic Liquid Electrolyte for Potassium Secondary Batteries","authors":"Hiroki Yamamoto*, Keigo Kubota*, Jinkwang Hwang, Kazuhiko Matsumoto and Rika Hagiwara, ","doi":"10.1021/acs.jpcb.4c0810510.1021/acs.jpcb.4c08105","DOIUrl":"https://doi.org/10.1021/acs.jpcb.4c08105https://doi.org/10.1021/acs.jpcb.4c08105","url":null,"abstract":"Potassium single cation ionic liquids (K-SCILs), which solely contain K+ as the cationic species, realize exceptionally high K+ concentrations and exhibit unique physicochemical and electrochemical properties. However, K-SCILs tend to have high melting points due to the smaller size of K+ than those of bulky organic cations, resulting in high operating temperatures for battery applications. In this study, a K-SCIL with a melting point below that of K metal (64 °C) was developed by evolving a binary system to a ternary one. The resulting K-SCIL, K[FSA]0.33[FTA]0.33[TfO]0.33 (FSA–: bis(fluorosulfonyl)amide, FTA–: (fluorosulfonyl)(trifluoromethanesulfonyl)amide, and TfO–: trifluoromethanesulfonate), has a low melting point of 50 °C with a high K+ concentration of 9.3 mol dm–3 at 55 °C. It allows the safe handling of K metal and exhibits improved solid K metal deposition/dissolution compared to a conventional organic electrolyte. The K-SCIL does not involve the formation of a K+ concentration gradient near the electrode surface, which is demonstrated by the applicability of large currents exceeding a limiting current density assumed by calculation. Furthermore, stable K+ intercalation/deintercalation into/from graphite was successfully demonstrated at 55 °C, highlighting the potential of this K-SCIL for advanced potassium battery applications.","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":"129 14","pages":"3652–3660 3652–3660"},"PeriodicalIF":2.8,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143806738","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Ternary Potassium Single Cation Ionic Liquid Electrolyte for Potassium Secondary Batteries. 钾二次电池用三元钾单阳离子离子液体电解质。

IF 2.8 2区化学

The Journal of Physical Chemistry B Pub Date : 2025-03-28 DOI: 10.1021/acs.jpcb.4c08105

Hiroki Yamamoto, Keigo Kubota, Jinkwang Hwang, Kazuhiko Matsumoto, Rika Hagiwara

{"title":"Ternary Potassium Single Cation Ionic Liquid Electrolyte for Potassium Secondary Batteries.","authors":"Hiroki Yamamoto, Keigo Kubota, Jinkwang Hwang, Kazuhiko Matsumoto, Rika Hagiwara","doi":"10.1021/acs.jpcb.4c08105","DOIUrl":"https://doi.org/10.1021/acs.jpcb.4c08105","url":null,"abstract":"Potassium single cation ionic liquids (K-SCILs), which solely contain K+ as the cationic species, realize exceptionally high K+ concentrations and exhibit unique physicochemical and electrochemical properties. However, K-SCILs tend to have high melting points due to the smaller size of K+ than those of bulky organic cations, resulting in high operating temperatures for battery applications. In this study, a K-SCIL with a melting point below that of K metal (64 °C) was developed by evolving a binary system to a ternary one. The resulting K-SCIL, K[FSA]0.33[FTA]0.33[TfO]0.33 (FSA-: bis(fluorosulfonyl)amide, FTA-: (fluorosulfonyl)(trifluoromethanesulfonyl)amide, and TfO-: trifluoromethanesulfonate), has a low melting point of 50 °C with a high K+ concentration of 9.3 mol dm-3 at 55 °C. It allows the safe handling of K metal and exhibits improved solid K metal deposition/dissolution compared to a conventional organic electrolyte. The K-SCIL does not involve the formation of a K+ concentration gradient near the electrode surface, which is demonstrated by the applicability of large currents exceeding a limiting current density assumed by calculation. Furthermore, stable K+ intercalation/deintercalation into/from graphite was successfully demonstrated at 55 °C, highlighting the potential of this K-SCIL for advanced potassium battery applications.","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":" ","pages":""},"PeriodicalIF":2.8,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143727125","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Structure of Novel Phosphonium-Based Ionic Liquids with S and O Substitutions from Experiments and a Mixed Quantum-Classical Approach. 基于S和O取代的新型磷基离子液体的结构实验和混合量子-经典方法。

IF 2.8 2区化学

The Journal of Physical Chemistry B Pub Date : 2025-03-27 DOI: 10.1021/acs.jpcb.5c00129

Raphael Ogbodo, Gobin Raj Acharya, Ho Martin Yuen, Nicole Zmich, Furong Wang, Hideaki Shirota, Sharon I Lall-Ramnarine, James F Wishart, Andrew J Nieuwkoop, Claudio J Margulis

{"title":"Structure of Novel Phosphonium-Based Ionic Liquids with S and O Substitutions from Experiments and a Mixed Quantum-Classical Approach.","authors":"Raphael Ogbodo, Gobin Raj Acharya, Ho Martin Yuen, Nicole Zmich, Furong Wang, Hideaki Shirota, Sharon I Lall-Ramnarine, James F Wishart, Andrew J Nieuwkoop, Claudio J Margulis","doi":"10.1021/acs.jpcb.5c00129","DOIUrl":"https://doi.org/10.1021/acs.jpcb.5c00129","url":null,"abstract":"This article presents experimental characterization information and synchrotron X-ray scattering measurements on a set of novel O- and S-substituted phosphonium-based ionic liquids (ILs) all coupled with the bis(fluorosulfonyl)imide (FSI-) anion. The ILs include the ethoxyethyltriethylphosphonium (P222(2O2)+) and triethyl[2-(ethylthio)ethyl]phosphonium (P222(2S2)+) cations, and we contrast results on these with those for unsubstituted triethylpentylphosphonium (P2225+). The article also introduces a physics-based protocol that combines classical force field studies on larger simulation boxes with classical and first-principles studies on smaller boxes. The method produces significantly improved S(q) functions in the regime which in prior publications we have associated with inter- and intraionic adjacency correlations. By understanding which shorter-range structural changes improve S(q) in the q-regime of interest, we are also able to pinpoint specific deficiencies in the classical force field model. The approach we take should be quite general and could help study other complex liquids on different length scales.","PeriodicalId":60,"journal":{"name":"The Journal of Physical Chemistry B","volume":" ","pages":""},"PeriodicalIF":2.8,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143727108","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0