Pub Date : 2024-10-16DOI: 10.1016/j.cplett.2024.141691
Shuang Ni , Xiao-Ming Song , Guo-Ce An , Tai-Xing Chi , Xin-Xin Li , Xin Zhou , Yi-Zhen Tang , Feng-Yang Bai , Ke Zhang , Zhen Zhao
The role of substituent group in organosulfate/organosulfonate (methanesulfonic acid, methyl hydrogen sulfate and hydroxymethanesulfonic acid) and amides (formamide, acetamide, methylformamidne, and urea) on structure, thermodynamics, intermolecular forces, atmospheric influence and optical properties was studied theoretically. The results show that the substituents can not promote the clustering of rganosulfate/organosulfonate, and can promote the clustering of amides. Additionally, the substituents can improve the optical properties of amide, organosulfate/organosulfonate. Low temperature, high pressure and high altitude contribute to the formation of clusters, and temperature is the dominate factor. Additionally, organic acid promotes the clustering with organosulfate/organosulfonate and amide, and enhances Rayleigh scattering properties, further strengthens the extinction properties of aerosols to affect atmospheric visibility.
{"title":"Role of substituent on organosulfate/organosulfonate and amide molecules in the initial stage of atmospheric new particle formation","authors":"Shuang Ni , Xiao-Ming Song , Guo-Ce An , Tai-Xing Chi , Xin-Xin Li , Xin Zhou , Yi-Zhen Tang , Feng-Yang Bai , Ke Zhang , Zhen Zhao","doi":"10.1016/j.cplett.2024.141691","DOIUrl":"10.1016/j.cplett.2024.141691","url":null,"abstract":"<div><div>The role of substituent group in organosulfate/organosulfonate (methanesulfonic acid, methyl hydrogen sulfate and hydroxymethanesulfonic acid) and amides (formamide, acetamide, methylformamidne, and urea) on structure, thermodynamics, intermolecular forces, atmospheric influence and optical properties was studied theoretically. The results show that the substituents can not promote the clustering of rganosulfate/organosulfonate, and can promote the clustering of amides. Additionally, the substituents can improve the optical properties of amide, organosulfate/organosulfonate. Low temperature, high pressure and high altitude contribute to the formation of clusters, and temperature is the dominate factor. Additionally, organic acid promotes the clustering with organosulfate/organosulfonate and amide, and enhances Rayleigh scattering properties, further strengthens the extinction properties of aerosols to affect atmospheric visibility.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"857 ","pages":"Article 141691"},"PeriodicalIF":2.8,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142530460","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 : 2024-10-16DOI: 10.1016/j.cplett.2024.141690
Kamal Ziadi
Herein, we employ deperturbed second-order vibrational perturbation theory (DVPT2) and generalized VPT2 (GVPT2) methodologies to predict and analyze two distinct spectral regions in the infrared, VCD, and Raman spectra of α-thujone and S-camphor. The first spectral region spans from 3200 to 2900 cm−1, while the second region extends from 1800 to 500 cm−1. We aim to introduce and validate a program for the simultaneous analysis of vibrational spectra intensity in medium-sized molecules using GVPT2 and DVPT2. Furthermore, employing a graphical presentation (heat map) to illustrate the important contribution of cubic force constant and χ-matrix to anharmonicity.
{"title":"Use of deperturbed and generalized second-order vibrational perturbation theories to study vibrational spectra intensity and the role of cubic force constant and total anharmonic matrix contributions to anharmonicity: α-thujone and S-camphor","authors":"Kamal Ziadi","doi":"10.1016/j.cplett.2024.141690","DOIUrl":"10.1016/j.cplett.2024.141690","url":null,"abstract":"<div><div>Herein, we employ deperturbed second-order vibrational perturbation theory (DVPT2) and generalized VPT2 (GVPT2) methodologies to predict and analyze two distinct spectral regions in the infrared, VCD, and Raman spectra of α-thujone and S-camphor. The first spectral region spans from 3200 to 2900 cm<sup>−1</sup>, while the second region extends from 1800 to 500 cm<sup>−1</sup>. We aim to introduce and validate a program for the simultaneous analysis of vibrational spectra intensity in medium-sized molecules using GVPT2 and DVPT2. Furthermore, employing a graphical presentation (heat map) to illustrate the important contribution of cubic force constant and χ-matrix to anharmonicity.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"857 ","pages":"Article 141690"},"PeriodicalIF":2.8,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142530486","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 : 2024-10-15DOI: 10.1016/j.cplett.2024.141687
Peter L. Rodríguez-Kessler , Alvaro Muñoz-Castro
The formation of persistent molecular units for further materials requires acquiring insights into the rich versatility of available species. The Nb11O15− cluster exhibits a sizable frontier orbital gap with particular stability. Its electronic structure denotes a partially filled 1F superatomic shell, not fulfilling the 2(N + 1)2 Hirsh rule for spherical aromatic species. Our results unravel a spherical antiaromatic behavior, which is scarce in literature. Furthermore, to gain a fundamental understanding of the accounted results, both diamagnetic and paramagnetic contributions to the overall magnetic behavior are discussed. Thus, Nb11O15− is an interesting oxo-bridged cluster, featuring spherical antiaromaticity as a stable cluster unit.
{"title":"Nb11O15−. As a persistent spherical antiaromatic cluster","authors":"Peter L. Rodríguez-Kessler , Alvaro Muñoz-Castro","doi":"10.1016/j.cplett.2024.141687","DOIUrl":"10.1016/j.cplett.2024.141687","url":null,"abstract":"<div><div>The formation of persistent molecular units for further materials requires acquiring insights into the rich versatility of available species. The Nb<sub>11</sub>O<sub>15</sub><sup>−</sup> cluster exhibits a sizable frontier orbital gap with particular stability. Its electronic structure denotes a partially filled 1F superatomic shell, not fulfilling the 2(<em>N</em> + 1)<sup>2</sup> Hirsh rule for spherical aromatic species. Our results unravel a spherical antiaromatic behavior, which is scarce in literature. Furthermore, to gain a fundamental understanding of the accounted results, both diamagnetic and paramagnetic contributions to the overall magnetic behavior are discussed. Thus, Nb<sub>11</sub>O<sub>15</sub><sup>−</sup> is an interesting <em>oxo</em>-bridged cluster, featuring spherical antiaromaticity as a stable cluster unit.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"857 ","pages":"Article 141687"},"PeriodicalIF":2.8,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142530464","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 : 2024-10-15DOI: 10.1016/j.cplett.2024.141689
Shiyu Xing , Xuying Wang , Tao Wang , Yan Yan , Yong Sun , Peifang Li
In the article, the first-principles and particle swarm optimization methods are used to predict the high-pressure structure of ClF3 with the space groups P1 (phase I), P21/c (phase II), P (phase III), and Imma (phase IV). Shows transition sequence. Calculates phonons and elastic constants. Finds ClF3 becomes metallic at 297 GPa. Phases II and IV meet stability criteria. All but phase I are dynamically stable.
文章采用第一性原理和粒子群优化方法预测了 ClF3 的高压结构，其空间群分别为 P1（Ⅰ相）、P21/c（Ⅱ相）、P 1¯（Ⅲ相）和 Imma（Ⅳ相）。显示过渡序列。计算声子和弹性常数。发现 ClF3 在 297 GPa 时变成金属。相 II 和相 IV 符合稳定性标准。除第一相外，其他各相都具有动态稳定性。
{"title":"The crystal structure and characteristics of chlorine trifluoride under high-pressure","authors":"Shiyu Xing , Xuying Wang , Tao Wang , Yan Yan , Yong Sun , Peifang Li","doi":"10.1016/j.cplett.2024.141689","DOIUrl":"10.1016/j.cplett.2024.141689","url":null,"abstract":"<div><div>In the article, the first-principles and particle swarm optimization methods are used to predict the high-pressure structure of ClF<sub>3</sub> with the space groups <em>P</em>1 (phase I), <em>P</em>2<sub>1</sub>/<em>c</em> (phase II), <em>P</em> <span><math><mover><mrow><mn>1</mn></mrow><mrow><mo>¯</mo></mrow></mover></math></span> (phase III), and <em>Imma</em> (phase IV). Shows transition sequence. Calculates phonons and elastic constants. Finds ClF<sub>3</sub> becomes metallic at 297 GPa. Phases II and IV meet stability criteria. All but phase I are dynamically stable.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"857 ","pages":"Article 141689"},"PeriodicalIF":2.8,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142530463","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 : 2024-10-15DOI: 10.1016/j.cplett.2024.141688
Sunwoo Kang , Taekyung Kim
Density functional theory (DFT) and time-dependent DFT (TDDFT) calculations were performed to understand the effect of the external electric field (EEF) on the reorganization (λ) and the lowest triplet excited-state (T1) energies of high T1 blue host materials. Depending on the direction and the strength of the external electric field (EEF), the positive and negative changes of hole and electron λ(h and λ e) values were found in these materials. More importantly, λ e seems to be more sensitive than λ h values under the EEF. It is also noticed that the calculated T1 energies are meaningfully changed in the application of EEFx and EEFy. In contrast, the effect of EEFz on the T1 energies can be negligible. From the results of theoretical investigation, the obvious evidence related to the influence of EEF on the charge transport and excited-state properties of high T1 blue host materials were obtained. In the present work, we expect that our theoretical study will provide new insight into understanding the influence of EEF as a key player in manipulating essential properties of the high T1 blue host material during the electrical operation.
{"title":"Unveiling the role of external electric field on the charge transport and excited-state properties of high T1 host for blue OLED devices","authors":"Sunwoo Kang , Taekyung Kim","doi":"10.1016/j.cplett.2024.141688","DOIUrl":"10.1016/j.cplett.2024.141688","url":null,"abstract":"<div><div>Density functional theory (DFT) and time-dependent DFT (TDDFT) calculations were performed to understand the effect of the external electric field (EEF) on the reorganization (<em>λ</em>) and the lowest triplet excited-state (T<sub>1</sub>) energies of high T<sub>1</sub> blue host materials. Depending on the direction and the strength of the external electric field (EEF), the positive and negative changes of hole and electron <em>λ(<sub>h</sub></em> and <em>λ <sub>e</sub></em>) values were found in these materials. More importantly, <em>λ <sub>e</sub></em> seems to be more sensitive than <em>λ <sub>h</sub></em> values under the EEF. It is also noticed that the calculated T<sub>1</sub> energies are meaningfully changed in the application of EEF<sub>x</sub> and EEF<sub>y</sub>. In contrast, the effect of EEF<sub>z</sub> on the T<sub>1</sub> energies can be negligible. From the results of theoretical investigation, the obvious evidence related to the influence of EEF on the charge transport and excited-state properties of high T<sub>1</sub> blue host materials were obtained. In the present work, we expect that our theoretical study will provide new insight into understanding the influence of EEF as a key player in manipulating essential properties of the high T<sub>1</sub> blue host material during the electrical operation.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"856 ","pages":"Article 141688"},"PeriodicalIF":2.8,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142445344","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 : 2024-10-11DOI: 10.1016/j.cplett.2024.141683
You-Qian Ma , Hang Zhang , Yan Zhang , Ning Zhao , Ling-Ling Lu , Dong Liu , Guang-Yue Li
TDDFT has been used to confirm the cysteine-sensing mechanism of a reported fluorescent probe (Talanta, 2020, 220, 12136). Frontier molecular orbital analysis showed that the probe underwent a PET process from quinazolinone to acryloyl, which made the fluorescence quenched together with nonplanar structure. Cysteine removed the acryloyl moiety and inhibited the PET process. The planar geometry of the probe-cysteine product enlarged the conjugated system and enhanced the green fluorescence of the fluorophore. Moreover, the charge redistribution also led to the excited-state proton transfer process, ultimately enhanced the fluorescence intensity and a notable Stocks shift.
TDDFT 被用于证实一种已报道的荧光探针的半胱氨酸感应机制（Talanta，2020，220，12136）。前沿分子轨道分析表明，该探针经历了从喹唑啉酮到丙烯酰基的 PET 过程，这使得荧光淬灭，同时出现了非平面结构。半胱氨酸去除了丙烯酰基，抑制了 PET 过程。探针-半胱氨酸产物的平面几何结构扩大了共轭体系，增强了荧光团的绿色荧光。此外，电荷的重新分配也导致了激发态质子转移过程，最终增强了荧光强度并发生了显著的斯托克斯位移。
{"title":"TDDFT elucidating the PET-Inhibition Mediated fluorescence enhancement in a Cysteine probe","authors":"You-Qian Ma , Hang Zhang , Yan Zhang , Ning Zhao , Ling-Ling Lu , Dong Liu , Guang-Yue Li","doi":"10.1016/j.cplett.2024.141683","DOIUrl":"10.1016/j.cplett.2024.141683","url":null,"abstract":"<div><div>TDDFT has been used to confirm the cysteine-sensing mechanism of a reported fluorescent probe (Talanta, 2020, 220, 12136). Frontier molecular orbital analysis showed that the probe underwent a PET process from quinazolinone to acryloyl, which made the fluorescence quenched together with nonplanar structure. Cysteine removed the acryloyl moiety and inhibited the PET process. The planar geometry of the probe-cysteine product enlarged the conjugated system and enhanced the green fluorescence of the fluorophore. Moreover, the charge redistribution also led to the excited-state proton transfer process, ultimately enhanced the fluorescence intensity and a notable Stocks shift.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"856 ","pages":"Article 141683"},"PeriodicalIF":2.8,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142442843","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 : 2024-10-11DOI: 10.1016/j.cplett.2024.141681
Ali Ait Baha , Nabil Khossossi , Omar Lakbita , Younes Brahmi , Yassine El Mernissi , Taoufyq Aziz , Abdeljalil Benlhachemi , Bahcine Bakiz , Hicham Abou Oualid
The present study highlights the efficiency of Ag3PO4 photocatalyst with a band gap of 2.25 eV, synthesized by a green and one-pot simple mechanochemical method, towards photodegradation of orange G under visible irradiation. The phase structure, morphology, and optical properties of mechano-synthesized Ag3PO4 were investigated using X-ray diffraction, Scanning Electron Microscopy, Thermogravimetric Analysis, Fourier Transform Infrared, the Brunauer-Emmet-Teller surface area, and UV–vis diffuse reflectance spectroscopy. DFT calculations were also conducted for band gap energy prediction. The photocatalytic activity of the sample was evaluated using a central composite design for surface response methodology (CCD-RSM) to determine the optimal conditions for Orange G (OG) removal. The photocatalytic activity of Ag3PO4 was approximately 93 % within 20 min of reaction under irradiation for 24.6 mg/L and 11 mg/L of Ag3PO4 and Orange G, respectively. Trapping experiments confirmed that peroxides and hydroxyl radicals are the dominant active species in the photodegradation process.
本研究采用绿色、一锅简单的机械化学方法合成了带隙为 2.25 eV 的 Ag3PO4 光催化剂，在可见光照射下对橙 G 进行光降解。利用 X 射线衍射、扫描电子显微镜、热重分析、傅里叶变换红外、布鲁诺-艾美特-泰勒比表面积和紫外-可见漫反射光谱研究了机械合成 Ag3PO4 的相结构、形貌和光学性质。此外，还进行了带隙能预测的 DFT 计算。采用表面响应方法的中心复合设计（CCD-RSM）对样品的光催化活性进行了评估，以确定去除橙 G（OG）的最佳条件。在 24.6 mg/L 和 11 mg/L 的 Ag3PO4 和 Orange G 的照射下，Ag3PO4 在 20 分钟内的光催化活性约为 93%。捕集实验证实，过氧化物和羟基自由基是光降解过程中的主要活性物种。
{"title":"Enhanced band gap energy of one-pot mechano-synthesized Ag3PO4 for Orange G photodegradation under visible light irradiation: An in-depth experimental and DFT studies","authors":"Ali Ait Baha , Nabil Khossossi , Omar Lakbita , Younes Brahmi , Yassine El Mernissi , Taoufyq Aziz , Abdeljalil Benlhachemi , Bahcine Bakiz , Hicham Abou Oualid","doi":"10.1016/j.cplett.2024.141681","DOIUrl":"10.1016/j.cplett.2024.141681","url":null,"abstract":"<div><div>The present study highlights the efficiency of Ag<sub>3</sub>PO<sub>4</sub> photocatalyst with a band gap of 2.25 eV, synthesized by a green and one-pot simple mechanochemical method, towards photodegradation of orange G under visible irradiation. The phase structure, morphology, and optical properties of mechano-synthesized Ag<sub>3</sub>PO<sub>4</sub> were investigated using X-ray diffraction, Scanning Electron Microscopy, Thermogravimetric Analysis, Fourier Transform Infrared, the Brunauer-Emmet-Teller surface area, and UV–vis diffuse reflectance spectroscopy. DFT calculations were also conducted for band gap energy prediction. The photocatalytic activity of the sample was evaluated using a central composite design for surface response methodology (CCD-RSM) to determine the optimal conditions for Orange G (OG) removal. The photocatalytic activity of Ag<sub>3</sub>PO<sub>4</sub> was approximately 93 % within 20 min of reaction under irradiation for 24.6 mg/L and 11 mg/L of Ag<sub>3</sub>PO<sub>4</sub> and Orange G, respectively. Trapping experiments confirmed that peroxides and hydroxyl radicals are the dominant active species in the photodegradation process.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"856 ","pages":"Article 141681"},"PeriodicalIF":2.8,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142445345","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 : 2024-10-11DOI: 10.1016/j.cplett.2024.141682
Albert Akeno Nyaaba, Yao Peng, Ziliang Kang, Hina Naz, Subramanian Premlatha, Zhenyuan Ji, Stennard Leetroy George, Guoxing Zhu
The use of hydrogen as an intermediator to convert and store electrochemical energy has been a subject of significant interest and focus. Unfortunately, the slow alkaline hydrogen oxidation reaction (HOR) is a barrier to further development of hydrogen–oxygen fuel cells. Ruthenium (Ru) has recently been investigated as a possible replacement for platinum (Pt) catalyst in the HOR because of the similar hydrogen binding energy (HBE) to Pt. Herein, Ru species was loaded on Ni3N@Mo2C support, which was used as an electrocatalyst for HOR. The catalyst presents an exchange current density and kinetic current densities of 3.05 and 4.76 mA cmdisk−2 that are 2 and 1.4 times greater than that of commercial Pt/C, respectively. The findings indicate that the Ni3N@Mo2C support reduces the hydrogen binding energy on Ru sites. This improves the Volmer step for HOR and increases the catalytic activity. This study thus provides some guidance in the designing of HOR catalysts for efficient hydrogen energy conversion.
使用氢气作为中间体来转换和储存电化学能量一直是人们非常感兴趣和关注的话题。遗憾的是，缓慢的碱性氢氧化反应（HOR）阻碍了氢氧燃料电池的进一步发展。由于钌（Ru）与铂（Pt）具有相似的氢结合能（HBE），最近有人将其作为氢氧化反应中铂（Pt）催化剂的替代品进行了研究。该催化剂的交换电流密度和动力学电流密度分别为 3.05 和 4.76 mA cmdisk-2，分别是商用 Pt/C 的 2 倍和 1.4 倍。研究结果表明，Ni3N@Mo2C 支持降低了 Ru 位点上的氢结合能。这改善了 HOR 的 Volmer 步骤，提高了催化活性。因此，这项研究为设计高效氢能转化的 HOR 催化剂提供了一些指导。
{"title":"Enhancing hydrogen oxidation by Modulating Ru species on Ni3N@Mo2C through a Support-Induced Strategy","authors":"Albert Akeno Nyaaba, Yao Peng, Ziliang Kang, Hina Naz, Subramanian Premlatha, Zhenyuan Ji, Stennard Leetroy George, Guoxing Zhu","doi":"10.1016/j.cplett.2024.141682","DOIUrl":"10.1016/j.cplett.2024.141682","url":null,"abstract":"<div><div>The use of hydrogen as an intermediator to convert and store electrochemical energy has been a subject of significant interest and focus. Unfortunately, the slow alkaline hydrogen oxidation reaction (HOR) is a barrier to further development of hydrogen–oxygen fuel cells. Ruthenium (Ru) has recently been investigated as a possible replacement for platinum (Pt) catalyst in the HOR because of the similar hydrogen binding energy (HBE) to Pt. Herein, Ru species was loaded on Ni<sub>3</sub>N@Mo<sub>2</sub>C support, which was used as an electrocatalyst for HOR. The catalyst presents an exchange current density and kinetic current densities of 3.05 and 4.76 mA cm<sub>disk</sub><sup>−2</sup> that are 2 and 1.4 times greater than that of commercial Pt/C, respectively. The findings indicate that the Ni<sub>3</sub>N@Mo<sub>2</sub>C support reduces the hydrogen binding energy on Ru sites. This improves the Volmer step for HOR and increases the catalytic activity. This study thus provides some guidance in the designing of HOR catalysts for efficient hydrogen energy conversion.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"856 ","pages":"Article 141682"},"PeriodicalIF":2.8,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142442844","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 : 2024-10-11DOI: 10.1016/j.cplett.2024.141680
Ken Sasaki , Yuuki Ishiwatari , Kazuki Ueno , Tomoya Kojima , Taisuke Banno , Noriyoshi Arai
This study employed dissipative particle dynamics (DPD) simulations to investigate the self-propelled motion of oil droplets in water–oil–surfactant systems. It is the first attempt to replicate self-propulsion models of oil droplets at the molecular level, contrasting previous simulations focused on Brownian motion and hydrodynamic behaviour of colloidal particles. The DPD model reproduced droplet propulsion and visualised internal Marangoni flow, showing that larger droplet radii and greater interfacial tension differences increase propulsion speeds. Additionally, surfactants with stronger oil–oil repulsion enhanced propulsion speed, suggesting that surfactant-induced local structures are crucial for the self-propulsion mechanism.
{"title":"Molecular modelling of active oil droplet propulsion: Insights from dissipative particle dynamics simulation","authors":"Ken Sasaki , Yuuki Ishiwatari , Kazuki Ueno , Tomoya Kojima , Taisuke Banno , Noriyoshi Arai","doi":"10.1016/j.cplett.2024.141680","DOIUrl":"10.1016/j.cplett.2024.141680","url":null,"abstract":"<div><div>This study employed dissipative particle dynamics (DPD) simulations to investigate the self-propelled motion of oil droplets in water–oil–surfactant systems. It is the first attempt to replicate self-propulsion models of oil droplets at the molecular level, contrasting previous simulations focused on Brownian motion and hydrodynamic behaviour of colloidal particles. The DPD model reproduced droplet propulsion and visualised internal Marangoni flow, showing that larger droplet radii and greater interfacial tension differences increase propulsion speeds. Additionally, surfactants with stronger oil–oil repulsion enhanced propulsion speed, suggesting that surfactant-induced local structures are crucial for the self-propulsion mechanism.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"857 ","pages":"Article 141680"},"PeriodicalIF":2.8,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142530462","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-10-11DOI: 10.1016/j.cplett.2024.141685
Rui Qi, Minhua Sun
Drawing on Shannon entropy, we developed a parameter called “structural entropy,” which is derived uniquely from atomic configurations and serves to measure the evolution of disorder during the glass transition. We applied this parameter to the glass transition in the CuZrAl system. A comparison with configurational entropy suggests that both may fundamentally encapsulate the same physical concept: the system’s level of disorder. This new structural entropy parameter bridges the gap between the macroscopic properties and the microscopic structure of glass, offering insights into the mechanisms underlying the glass transition.
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