Pub Date : 2026-04-01Epub Date: 2025-11-13DOI: 10.1016/j.chemphys.2025.113027
Masato Kondoh , Saya Suzuki, Taka-aki Ishibashi
We investigated the interaction of an antimicrobial peptide, gramicidin A (gA), with supported lipid bilayers (SLBs) at a CaF2/water interface using total internal reflection-Raman spectroscopy. The gA-addition and premixed experiments were performed, monitoring the CH stretching and amide I regions. In the gA-addition experiment, gA was introduced into the aqueous phase after SLB preparation, and resulting spectral changes were monitored. In the premixed experiment, SLBs were formed from lipid-gA mixtures and spectra were measured. At low peptide concentrations in the premixed experiment, the gA-derived component after subtracting the SLB contribution resembled the changes observed in the gA-addition experiment, confirming that these signals originate from gA interacting with the SLB. At higher peptide concentrations, the spectra changed significantly, suggesting structural alterations of gA due to peptide–peptide interactions. These behaviors were consistent with previously reported gA spectra in vesicles, supporting the validity of SLBs as a model for peptide–lipid interactions.
我们利用全内反射-拉曼光谱研究了抗菌肽gramicidin A （gA）与负载脂质双分子层（slb）在CaF2/水界面上的相互作用。进行了ga添加和预混实验，监测了CH拉伸和酰胺I区。在添加gA的实验中，在制备SLB后，将gA引入水相，并监测其光谱变化。在预混合实验中，脂质- ga混合物形成了slb，并测量了光谱。在低肽浓度预混实验中，减去SLB贡献后的gA衍生成分与添加gA实验中观察到的变化相似，证实了这些信号来自gA与SLB相互作用。在较高的肽浓度下，光谱发生显著变化，表明由于肽-肽相互作用导致gA的结构改变。这些行为与先前报道的囊泡中的gA光谱一致，支持slb作为肽-脂质相互作用模型的有效性。
{"title":"Raman spectra of gramicidin A in a supported lipid bilayer at the CaF2/water interface","authors":"Masato Kondoh , Saya Suzuki, Taka-aki Ishibashi","doi":"10.1016/j.chemphys.2025.113027","DOIUrl":"10.1016/j.chemphys.2025.113027","url":null,"abstract":"<div><div>We investigated the interaction of an antimicrobial peptide, gramicidin A (gA), with supported lipid bilayers (SLBs) at a CaF<sub>2</sub>/water interface using total internal reflection-Raman spectroscopy. The gA-addition and premixed experiments were performed, monitoring the CH stretching and amide I regions. In the gA-addition experiment, gA was introduced into the aqueous phase after SLB preparation, and resulting spectral changes were monitored. In the premixed experiment, SLBs were formed from lipid-gA mixtures and spectra were measured. At low peptide concentrations in the premixed experiment, the gA-derived component after subtracting the SLB contribution resembled the changes observed in the gA-addition experiment, confirming that these signals originate from gA interacting with the SLB. At higher peptide concentrations, the spectra changed significantly, suggesting structural alterations of gA due to peptide–peptide interactions. These behaviors were consistent with previously reported gA spectra in vesicles, supporting the validity of SLBs as a model for peptide–lipid interactions.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"603 ","pages":"Article 113027"},"PeriodicalIF":2.4,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145571118","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-04-01Epub Date: 2025-12-24DOI: 10.1016/j.chemphys.2025.113074
Hossien Hossieni
We propose a new analytical potential function to model proton transfer in the adenine–thymine base pair and develop a non-adiabatic quantum mechanical framework to calculate genetic mutation probabilities. This potential has been used to calculate the probability of mutation in a non-adiabatic process. The results of the new model have been shown to be consistent with the findings of other researchers.
{"title":"Mutation in DNA: A quantum mechanical non-adiabatic model","authors":"Hossien Hossieni","doi":"10.1016/j.chemphys.2025.113074","DOIUrl":"10.1016/j.chemphys.2025.113074","url":null,"abstract":"<div><div>We propose a new analytical potential function to model proton transfer in the adenine–thymine base pair and develop a non-adiabatic quantum mechanical framework to calculate genetic mutation probabilities. This potential has been used to calculate the probability of mutation in a non-adiabatic process. The results of the new model have been shown to be consistent with the findings of other researchers.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"603 ","pages":"Article 113074"},"PeriodicalIF":2.4,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145880078","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-04-01Epub Date: 2025-12-13DOI: 10.1016/j.chemphys.2025.113063
Sajid Ali , Basit Ali , Sani Abdulkarim , Mengtao Sun
The optoelectronic and photocatalytic characteristics of MoS₂, WS₂, and SiS₂ monolayers, as well as MoS₂/SiS₂ and WS₂/SiS₂ van der Waals (vdW) heterostructures, are investigated using first-principles density functional theory (DFT) calculations. Initially, it is verified that, in energy, all monolayers and their vdW heterostructures are structurally stable. SiS₂ has a direct band gap of 2.02 eV, monolayer MoS₂ exhibits a direct band gap of approximately 1.82 eV, while monolayer WS₂ shows a direct band gap of around 1.97 eV. These values differ from their bulk counterparts, which possess indirect band gaps due to interlayer interactions. When applied in photovoltaic and energy-harvesting devices, type-II band alignment has been observed in the MoS₂/SiS₂ and WS₂/SiS₂ vdW heterostructures. Moreover, charge transfer at the interface of these heterostructures provides an intrinsic electric field, which drives electrons and holes in opposite directions, thereby reducing the recombination rate of photogenerated electron–hole pairs. The main prerequisite for optoelectronic and photocatalytic applications in materials is efficient charge-carrier separation within them. Improved optical characteristics of the vdW heterostructures reveal their enhanced absorption in the visible-light region, which offers promise for the development of high-performance photocatalysts and optoelectronic devices.
利用第一性原理密度泛函理论（DFT）计算研究了MoS 2、WS 2和SiS 2单层以及MoS 2 /SiS 2和WS 2 /SiS 2 van der Waals （vdW）异质结构的光电和光催化特性。初步验证了在能量上，所有单层及其vdW异质结构都是结构稳定的。SiS₂的直接带隙为2.02 eV，单层MoS₂的直接带隙约为1.82 eV，单层WS₂的直接带隙约为1.97 eV。这些值不同于它们的体对应值，后者由于层间相互作用而具有间接带隙。当应用于光伏和能量收集器件时，在MoS₂/SiS₂和WS₂/SiS₂vdW异质结构中观察到ii型波段对准。此外，这些异质结构界面处的电荷转移提供了一个本征电场，该电场驱动电子和空穴向相反方向运动，从而降低了光生电子-空穴对的复合速率。光电子和光催化在材料中应用的主要前提是材料内部有效的载流子分离。改进的vdW异质结构的光学特性揭示了其在可见光区的吸收增强，这为高性能光催化剂和光电子器件的发展提供了希望。
{"title":"Structural and optoelectronic properties of XS₂ (X = Mo, W)/SiS₂ van der Waals Heterostructures for advanced energy applications","authors":"Sajid Ali , Basit Ali , Sani Abdulkarim , Mengtao Sun","doi":"10.1016/j.chemphys.2025.113063","DOIUrl":"10.1016/j.chemphys.2025.113063","url":null,"abstract":"<div><div>The optoelectronic and photocatalytic characteristics of MoS₂, WS₂, and SiS₂ monolayers, as well as MoS₂/SiS₂ and WS₂/SiS₂ van der Waals (vdW) heterostructures, are investigated using first-principles density functional theory (DFT) calculations. Initially, it is verified that, in energy, all monolayers and their vdW heterostructures are structurally stable<strong>.</strong> SiS₂ has a direct band gap of 2.02 eV<strong>,</strong> monolayer MoS₂ exhibits a direct band gap of approximately 1.82 eV<strong>,</strong> while monolayer WS₂ shows a direct band gap of around 1.97 eV<strong>.</strong> These values differ from their bulk counterparts, which possess <strong>i</strong>ndirect band gaps due to interlayer interactions. When applied in photovoltaic and energy-harvesting devices, type-II band alignment has been observed in the MoS₂/SiS₂ and WS₂/SiS₂ vdW heterostructures. Moreover, charge transfer at the interface of these heterostructures provides an intrinsic electric field, which drives electrons and holes in opposite directions, thereby reducing the recombination rate of photogenerated electron–hole pairs. The main prerequisite for optoelectronic and photocatalytic applications in materials is efficient charge-carrier separation within them. Improved optical characteristics of the vdW heterostructures reveal their enhanced absorption in the visible-light region, which offers promise for the development of high-performance photocatalysts and optoelectronic devices.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"603 ","pages":"Article 113063"},"PeriodicalIF":2.4,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145786463","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-04-01Epub Date: 2025-11-21DOI: 10.1016/j.chemphys.2025.113035
Navneet Sharma, Kousik Giri
The formation of molecular hydrogen () and its isotopic variants (HD, DH, and D) on a coronene molecule via an Eley-Rideal mechanism is studied using the multiconfiguration time-dependent Hartree method. The calculations are carried out for two- and three-dimensional model systems considering only collinear collisions using a newly developed potential energy surface calculated using the hybrid functional approximation of density functional theory. We report reaction probabilities as a function of collision energy in the range 0–30 meV, relevant to the interstellar medium. The studied reaction is barrierless, leading to a reaction probability close to one, even for low collision energies. We find that the desorbed and its isotopes are vibrationally excited, and the maximum populations at = 3 or 4. The computed vibrational excitation probability values are in good agreement with recent experimental results reported by Latimer et al. (2008) for HD/graphite. The percentage of energy shared by vibration and translation of the product molecule are 42%–62% and 18%–38%, respectively, and 20% of energy is contributed to the surface.
采用多构型时间依赖Hartree方法研究了分子氢（H2）及其同位素变体（HD、DH和D2）在冠烯分子上通过Eley-Rideal机制的形成。利用密度泛函理论的混合泛函近似计算的新发展的势能面，对仅考虑共线碰撞的二维和三维模型系统进行了计算。我们报告了反应概率作为碰撞能量在0-30 meV范围内的函数，与星际介质有关。所研究的反应是无障碍的，即使在低碰撞能量下，反应概率也接近于1。我们发现解吸的H2和它的同位素是振动激发的，在ν = 3或4时最大的居群。计算得到的振动激发概率值与Latimer et al.（2008）最近报道的HD/石墨的实验结果非常吻合。产物分子的振动和平移所共享的能量比例分别为42% ~ 62%和18% ~ 38%，其中20%的能量贡献给了表面。
{"title":"Quantum dynamical study on the formation of molecular hydrogen on a coronene molecule via an Eley-Rideal mechanism","authors":"Navneet Sharma, Kousik Giri","doi":"10.1016/j.chemphys.2025.113035","DOIUrl":"10.1016/j.chemphys.2025.113035","url":null,"abstract":"<div><div>The formation of molecular hydrogen (<span><math><msub><mrow><mi>H</mi></mrow><mrow><mn>2</mn></mrow></msub></math></span>) and its isotopic variants (HD, DH, and D<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>) on a coronene molecule via an Eley-Rideal mechanism is studied using the multiconfiguration time-dependent Hartree method. The calculations are carried out for two- and three-dimensional model systems considering only collinear collisions using a newly developed potential energy surface calculated using the hybrid functional approximation of density functional theory. We report reaction probabilities as a function of collision energy in the range 0–30 meV, relevant to the interstellar medium. The studied reaction is barrierless, leading to a reaction probability close to one, even for low collision energies. We find that the desorbed <span><math><msub><mrow><mi>H</mi></mrow><mrow><mn>2</mn></mrow></msub></math></span> and its isotopes are vibrationally excited, and the maximum populations at <span><math><mi>ν</mi></math></span> = 3 or 4. The computed vibrational excitation probability values are in good agreement with recent experimental results reported by Latimer et al. (2008) for HD/graphite. The percentage of energy shared by vibration and translation of the product molecule are 42%–62% and 18%–38%, respectively, and 20% of energy is contributed to the surface.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"603 ","pages":"Article 113035"},"PeriodicalIF":2.4,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145571119","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-04-01Epub Date: 2025-11-24DOI: 10.1016/j.chemphys.2025.113032
Jianming Ma , Kai Diao , Yiping Yuan , Shunping Shi , Deliang Chen
Based on DFT calculations at the PBE0-D3/def2-TZVP level, this study investigated the lowest energy structures obtained in this study of Ptn+ (n = 3–9) clusters, water molecule adsorption on their surfaces, and the HER mechanism. Water molecules preferentially adsorbed at the top sites of all clusters (adsorption energies: −1.24 to −2.64 eV, exothermic), with Pt₈+ and Pt₉+ exhibiting the highest adsorption energies. For HER, the Pt7+ system required the fewest steps (only 2), while Pt₈+ needed the most (9 steps). Pt3+-Pt7+ showed endothermic behavior (reaction energies: 0.41–1.91 eV), whereas Pt₈+ and Pt9+ were exothermic (−0.47 eV and − 0.71 eV, respectively), with Pt9+ having the most feasible pathway. Except for Pt7+, other systems formed Pt-H-Pt or Pt-O-Pt bonds; Pt3+/Pt4+/Pt7+ stayed stable, others distorted. This study provides a theoretical reference for designing high-efficiency Pt-based catalysts for water splitting.
{"title":"Hydrogen evolution reaction mechanism of Ptn+@H2O (n = 3–9) complexes: A DFT study","authors":"Jianming Ma , Kai Diao , Yiping Yuan , Shunping Shi , Deliang Chen","doi":"10.1016/j.chemphys.2025.113032","DOIUrl":"10.1016/j.chemphys.2025.113032","url":null,"abstract":"<div><div>Based on DFT calculations at the PBE0-D3/def2-TZVP level, this study investigated the lowest energy structures obtained in this study of Pt<sub>n</sub><sup>+</sup> (<em>n</em> = 3–9) clusters, water molecule adsorption on their surfaces, and the HER mechanism. Water molecules preferentially adsorbed at the top sites of all clusters (adsorption energies: −1.24 to −2.64 eV, exothermic), with Pt₈<sup>+</sup> and Pt₉<sup>+</sup> exhibiting the highest adsorption energies. For HER, the Pt<sub>7</sub><sup>+</sup> system required the fewest steps (only 2), while Pt₈<sup>+</sup> needed the most (9 steps). Pt<sub>3</sub><sup>+</sup>-Pt<sub>7</sub><sup>+</sup> showed endothermic behavior (reaction energies: 0.41–1.91 eV), whereas Pt₈<sup>+</sup> and Pt<sub>9</sub><sup>+</sup> were exothermic (−0.47 eV and − 0.71 eV, respectively), with Pt<sub>9</sub><sup>+</sup> having the most feasible pathway. Except for Pt<sub>7</sub><sup>+</sup>, other systems formed Pt-H-Pt or Pt-O-Pt bonds; Pt<sub>3</sub><sup>+</sup>/Pt<sub>4</sub><sup>+</sup>/Pt<sub>7</sub><sup>+</sup> stayed stable, others distorted. This study provides a theoretical reference for designing high-efficiency Pt-based catalysts for water splitting.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"603 ","pages":"Article 113032"},"PeriodicalIF":2.4,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145616296","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-04-01Epub Date: 2025-12-05DOI: 10.1016/j.chemphys.2025.113053
Kaito Sasaki , K.P. Safna Hussan , Rio Kita , Takeru Ito , Yosuke Okamura , Naoki Shinyashiki
Polyvinylpyrrolidone (PVP) is a widely used synthetic polymer known for its versatility, biocompatibility, solubility, and thermal stability, with applications spanning pharmaceuticals, biomedicine, food, cosmetics, and electronics. Despite its broad usage, detailed insights into its dynamic behavior remain limited. This study presents a comprehensive investigation of the structural, dynamic, and spectroscopic properties of bulk PVP (molecular weight of 10,000 g/mol) using a multi-scale approach that combines Density Functional Theory (DFT), thermal analysis with Differential Scanning Calorimetry (DSC) and Thermogravimetric Analysis (TGA), and experimental spectroscopic techniques with Broadband Dielectric Spectroscopy (BDS) and Fourier Transform Infrared (FTIR) spectroscopy. DFT calculations reveal that polymerization significantly enhances reactivity, polarity, solubility, and a reduction in bandgap (from 7.19 to 3.95 eV). FTIR spectra further confirm hydrogen bonding interactions. DSC analysis indicates a glass transition temperature (Tg) of 396 K, while thermal stability extends up to ∼660 K. BDS over a wide frequency (10−2 to 107 Hz) and temperature (178–473 K) range identifies three distinct relaxation processes: α-relaxation associated with cooperative segmental motion related to the glass transition phenomenon, β-relaxation attributed to Johari-Goldstein dynamics, and γ-relaxation linked to localized side-chain motions. The fragility index (m = 46) obtained from the temperature dependence of relaxation time of the α-relaxation classifies PVP as a strong glass former, with excellent structural and thermal resilience. These findings offer fundamental insights into PVP's dynamic behavior and reinforce its potential across diverse high-performance applications.
{"title":"Fundamental insights into bulk polyvinylpyrrolidone (PVP): Combining DFT, molecular dynamics, and spectroscopic techniques","authors":"Kaito Sasaki , K.P. Safna Hussan , Rio Kita , Takeru Ito , Yosuke Okamura , Naoki Shinyashiki","doi":"10.1016/j.chemphys.2025.113053","DOIUrl":"10.1016/j.chemphys.2025.113053","url":null,"abstract":"<div><div>Polyvinylpyrrolidone (PVP) is a widely used synthetic polymer known for its versatility, biocompatibility, solubility, and thermal stability, with applications spanning pharmaceuticals, biomedicine, food, cosmetics, and electronics. Despite its broad usage, detailed insights into its dynamic behavior remain limited. This study presents a comprehensive investigation of the structural, dynamic, and spectroscopic properties of bulk PVP (molecular weight of 10,000 g/mol) using a multi-scale approach that combines Density Functional Theory (DFT), thermal analysis with Differential Scanning Calorimetry (DSC) and Thermogravimetric Analysis (TGA), and experimental spectroscopic techniques with Broadband Dielectric Spectroscopy (BDS) and Fourier Transform Infrared (FTIR) spectroscopy. DFT calculations reveal that polymerization significantly enhances reactivity, polarity, solubility, and a reduction in bandgap (from 7.19 to 3.95 eV). FTIR spectra further confirm hydrogen bonding interactions. DSC analysis indicates a glass transition temperature (<em>T</em><sub><em>g</em></sub>) of 396 K, while thermal stability extends up to ∼660 K. BDS over a wide frequency (10<sup>−2</sup> to 10<sup>7</sup> Hz) and temperature (178–473 K) range identifies three distinct relaxation processes: α-relaxation associated with cooperative segmental motion related to the glass transition phenomenon, β-relaxation attributed to Johari-Goldstein dynamics, and γ-relaxation linked to localized side-chain motions. The fragility index (m = 46) obtained from the temperature dependence of relaxation time of the α-relaxation classifies PVP as a strong glass former, with excellent structural and thermal resilience. These findings offer fundamental insights into PVP's dynamic behavior and reinforce its potential across diverse high-performance applications.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"603 ","pages":"Article 113053"},"PeriodicalIF":2.4,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145733040","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Herein, MoO2/C nanocomposites was synthesized in a single-step reduction process using waste plastic polyethene (C₂H₄)ₙ as a carbon source. The effect of supporting carbon content on the oxygen evolution reaction (OER) activity of MoO2 nanoparticles is investigated. The hydrocarbons present in the polyethene acts as reducing agents during synthesis. The synthesized samples are characterized using X-ray diffraction (XRD), Raman spectroscopy, scanning electron microscope (SEM), transmission electron microscope (TEM) and X-ray photoelectron spectroscopy (XPS). The highly conductive supporting carbon acts like a highway for the charge carries between MoO2 nanoparticles. The amount of carbon is optimized to get highest possible activity from the MoO2 nanoparticles. Furthermore, the sample MoO2/C (C3) shows optimal OER performance with a low overpotential of 1.58 V vs RHE at current density of 10 mA cm−2. Chronoamperometry Stability of 18 h shows that all the samples possess good stability under alkaline medium. The amount of supporting carbon plays a crucial role to achieve optimal OER performance from MoO2 nanoparticles.
本文以废塑料聚乙烯（C₂H₄）为碳源，采用一步还原法合成了MoO2/C纳米复合材料。研究了负载碳含量对MoO2纳米颗粒析氧反应活性的影响。聚乙烯中的碳氢化合物在合成过程中起还原剂的作用。利用x射线衍射（XRD）、拉曼光谱（Raman spectroscopy）、扫描电子显微镜（SEM）、透射电子显微镜（TEM）和x射线光电子能谱（XPS）对合成的样品进行了表征。高导电性的支撑碳就像MoO2纳米颗粒之间的电荷携带的高速公路。优化了碳的用量，使MoO2纳米颗粒的活性尽可能高。此外，样品MoO2/C （C3）在电流密度为10 mA cm−2时表现出最佳的OER性能，过电位低至1.58 V vs RHE。18h的计时安培稳定性表明，样品在碱性介质中具有良好的稳定性。负载碳的数量对MoO2纳米颗粒获得最佳OER性能起着至关重要的作用。
{"title":"Waste plastic upcycling: MoO₂/C nanocomposites supported on Ni foam for efficient oxygen evolution reaction","authors":"Soubhagya Ranjan Panda , Sanjay Upadhyay , Ruby Priya , Abhishek Chandel , O.P. Pandey","doi":"10.1016/j.chemphys.2025.113071","DOIUrl":"10.1016/j.chemphys.2025.113071","url":null,"abstract":"<div><div>Herein, MoO<sub>2</sub>/C nanocomposites was synthesized in a single-step reduction process using waste plastic polyethene (C₂H₄)<strong>ₙ</strong> as a carbon source. The effect of supporting carbon content on the oxygen evolution reaction (OER) activity of MoO<sub>2</sub> nanoparticles is investigated. The hydrocarbons present in the polyethene acts as reducing agents during synthesis. The synthesized samples are characterized using X-ray diffraction (XRD), Raman spectroscopy, scanning electron microscope (SEM), transmission electron microscope (TEM) and X-ray photoelectron spectroscopy (XPS). The highly conductive supporting carbon acts like a highway for the charge carries between MoO<sub>2</sub> nanoparticles. The amount of carbon is optimized to get highest possible activity from the MoO<sub>2</sub> nanoparticles. Furthermore, the sample MoO<sub>2</sub>/C (C3) shows optimal OER performance with a low overpotential of 1.58 V vs RHE at current density of 10 mA cm<sup>−2</sup>. Chronoamperometry Stability of 18 h shows that all the samples possess good stability under alkaline medium. The amount of supporting carbon plays a crucial role to achieve optimal OER performance from MoO<sub>2</sub> nanoparticles.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"603 ","pages":"Article 113071"},"PeriodicalIF":2.4,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145836596","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-04-01Epub Date: 2025-12-16DOI: 10.1016/j.chemphys.2025.113067
Vladimir P. Zhdanov
Herein, the kinetics of Ostwald ripening of supported metal nanoparticles (MNPs) made of two miscible metals is scrutinized theoretically. The whole process is treated as the interplay of two channels including rapid support-mediated redistribution of atoms with smaller sublimation energy and slow redistribution of atoms with larger sublimation energy, so that the growth of the average MNP size is related primarily to the latter channel. The equation derived for this size is similar to that for MNPs made of pure metals and can be easily integrated and employed in applications. The corresponding activation energies and specific surface free energies depend on the alloy composition, and the analysis proposed allows one to describe this effect. In illustrations, it has been done for MNPs made of typical metals used in heterogeneous catalysis by employing the parameters obtained on the basis of the density functional theory.
{"title":"Basics of Ostwald ripening of supported metallic alloy nanoparticles","authors":"Vladimir P. Zhdanov","doi":"10.1016/j.chemphys.2025.113067","DOIUrl":"10.1016/j.chemphys.2025.113067","url":null,"abstract":"<div><div>Herein, the kinetics of Ostwald ripening of supported metal nanoparticles (MNPs) made of two miscible metals is scrutinized theoretically. The whole process is treated as the interplay of two channels including rapid support-mediated redistribution of atoms with smaller sublimation energy and slow redistribution of atoms with larger sublimation energy, so that the growth of the average MNP size is related primarily to the latter channel. The equation derived for this size is similar to that for MNPs made of pure metals and can be easily integrated and employed in applications. The corresponding activation energies and specific surface free energies depend on the alloy composition, and the analysis proposed allows one to describe this effect. In illustrations, it has been done for MNPs made of typical metals used in heterogeneous catalysis by employing the parameters obtained on the basis of the density functional theory.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"603 ","pages":"Article 113067"},"PeriodicalIF":2.4,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145786521","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-04-01Epub Date: 2025-12-16DOI: 10.1016/j.chemphys.2025.113066
Kai Zhang , Guanglu He , Yiquan Wang , Guoliang Chen , Jianjun Fang , Chuan-Kui Wang , Jing Li
Orange-red thermally activated delayed fluorescence (TADF) molecules show great potential for OLEDs. Based on density functional theory (DFT) and the thermal vibration correlation function (TVCF) method, the luminescence mechanisms of the bridged open-ring structure T-DMAC-PPyM and the bridged closed-ring structure P-DMAC-BPyM are investigated in both toluene and the solid state. The fluorescence efficiency (ΦF) of the T-DMAC-PPyM in toluene is slightly higher than that of P-DMAC-BPyM, which is due to the larger radiation rate (kr) and smaller non-radiative decay rate (knr). In contrast, the sharply increased kr of P-DMAC-BPyM in the solid state leads to a much higher ΦF than that of T-DMAC-PPyM. In addition, P-DMAC-BPyM reduces ΔEST in the solid state and increases the spin-orbit coupling (SOC) constant, which is beneficial to improve the reverse intersystem crossing rate (RISC). Studies have shown that T-DMAC-PPyM has better intrinsic fluorescence properties, while P-DMAC-BPyM has better TADF properties in the solid state.
{"title":"Effect of molecular bridging group flexibility on the luminescent properties of Orange-red TADF molecules: A QM/MM study","authors":"Kai Zhang , Guanglu He , Yiquan Wang , Guoliang Chen , Jianjun Fang , Chuan-Kui Wang , Jing Li","doi":"10.1016/j.chemphys.2025.113066","DOIUrl":"10.1016/j.chemphys.2025.113066","url":null,"abstract":"<div><div>Orange-red thermally activated delayed fluorescence (TADF) molecules show great potential for OLEDs. Based on density functional theory (DFT) and the thermal vibration correlation function (TVCF) method, the luminescence mechanisms of the bridged open-ring structure T-DMAC-PPyM and the bridged closed-ring structure P-DMAC-BPyM are investigated in both toluene and the solid state. The fluorescence efficiency (Φ<sub>F</sub>) of the T-DMAC-PPyM in toluene is slightly higher than that of P-DMAC-BPyM, which is due to the larger radiation rate (k<sub>r</sub>) and smaller non-radiative decay rate (k<sub>nr</sub>). In contrast, the sharply increased k<sub>r</sub> of P-DMAC-BPyM in the solid state leads to a much higher Φ<sub>F</sub> than that of T-DMAC-PPyM. In addition, P-DMAC-BPyM reduces ΔE<sub>ST</sub> in the solid state and increases the spin-orbit coupling (SOC) constant, which is beneficial to improve the reverse intersystem crossing rate (RISC). Studies have shown that T-DMAC-PPyM has better intrinsic fluorescence properties, while P-DMAC-BPyM has better TADF properties in the solid state.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"603 ","pages":"Article 113066"},"PeriodicalIF":2.4,"publicationDate":"2026-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145786513","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-03-01Epub Date: 2025-10-28DOI: 10.1016/j.chemphys.2025.113001
Mais Khazaleh, Bilal Aladerah, Abdalla Obeidat
In this study, we employed Density Functional Theory (DFT) combined with high-throughput computational screening to explore the magnetic and structural properties of full Heusler alloys with the general formula X₂YZ, aiming to identify promising candidates for rare-earth-free permanent magnet applications. A total of 360 distinct compounds were generated using 3d transition metals for X and Y, and main group elements for Z. After the initial filtration based on thermodynamic preference for tetragonal symmetry, 41 compounds were retained for further investigation. Among these, three compounds, Co2CrGe, Co2CrSi, and Co2FeGa, exhibited saturation magnetization values greater than 0.5 T. Dynamical stability revealed that Co2CrGe and Co2FeGa are dynamically stable, while Co2CrSi was excluded from further analysis. Magnetocrystalline anisotropy energy (MCA) calculations yielded values of 2.4 MJ/m3 for Co2CrGe and 3.1 MJ/m3 for Co2FeGa, corresponding to high anisotropy fields () of 9.4 and 9.8 MA/m, respectively. Furthermore, Monte Carlo simulations revealed Curie temperatures () of 418 K for Co2CrGe and 654 K for Co2FeGa. These findings underscore the potential of Co2CrGe and Co2FeGa as high-performance, rare-earth-free permanent magnets. Our work demonstrates the power of high-throughput DFT-based screening to accelerate the discovery of novel magnetic materials with targeted functional properties.
{"title":"High-throughput screening of full Heusler alloys (X₂YZ) for advanced permanent magnets: computational insights","authors":"Mais Khazaleh, Bilal Aladerah, Abdalla Obeidat","doi":"10.1016/j.chemphys.2025.113001","DOIUrl":"10.1016/j.chemphys.2025.113001","url":null,"abstract":"<div><div>In this study, we employed Density Functional Theory (DFT) combined with high-throughput computational screening to explore the magnetic and structural properties of full Heusler alloys with the general formula X₂YZ, aiming to identify promising candidates for rare-earth-free permanent magnet applications. A total of 360 distinct compounds were generated using 3d transition metals for X and Y, and main group elements for Z. After the initial filtration based on thermodynamic preference for tetragonal symmetry, 41 compounds were retained for further investigation. Among these, three compounds, Co<sub>2</sub>CrGe, Co<sub>2</sub>CrSi, and Co<sub>2</sub>FeGa, exhibited saturation magnetization values greater than 0.5 T. Dynamical stability revealed that Co<sub>2</sub>CrGe and Co<sub>2</sub>FeGa are dynamically stable, while Co<sub>2</sub>CrSi was excluded from further analysis. Magnetocrystalline anisotropy energy (MCA) calculations yielded values of 2.4 MJ/m<sup>3</sup> for Co<sub>2</sub>CrGe and 3.1 MJ/m<sup>3</sup> for Co<sub>2</sub>FeGa, corresponding to high anisotropy fields (<span><math><msub><mi>H</mi><mi>a</mi></msub></math></span>) of 9.4 and 9.8 MA/m, respectively. Furthermore, Monte Carlo simulations revealed Curie temperatures (<span><math><msub><mi>T</mi><mi>c</mi></msub></math></span>) of 418 K for Co<sub>2</sub>CrGe and 654 K for Co<sub>2</sub>FeGa. These findings underscore the potential of Co<sub>2</sub>CrGe and Co<sub>2</sub>FeGa as high-performance, rare-earth-free permanent magnets. Our work demonstrates the power of high-throughput DFT-based screening to accelerate the discovery of novel magnetic materials with targeted functional properties.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"602 ","pages":"Article 113001"},"PeriodicalIF":2.4,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145425051","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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