Computational and Theoretical Chemistry最新文献

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Theoretical screening of multifunctional single-atom catalysts supported by VS2 monolayer for the electrocatalytic hydrogen evolution, oxygen evolution and oxygen reduction reactions

IF 3 3区化学 Q3 CHEMISTRY, PHYSICAL

Computational and Theoretical Chemistry

Pub Date : 2025-01-23 DOI: 10.1016/j.comptc.2025.115098

Liang-Cai Ma , Pan-Ge Yuan , Yin-Yin Hou , Hao Li , Hai-Juan Wang , Jian-Min Zhang

Exploring highly efficient multifunctional electrocatalysts for the HER, OER, and ORR is of great significance. In this work, transition metal atoms anchored on VS₂ monolayer (TM@VS₂) as single-atom catalysts were systematically investigated for their HER, OER, and ORR performance through first-principles calculations. The results indicate that all TM@VS₂ show high thermal stability and excellent electrical conductivity. Pt@VS₂ and Au@VS₂ are predicted to be the promising HER/OER bifunctional electrocatalysts for overall water-splitting with lower overpotentials of −0.07/0.59 V and − 0.07/0.62 V, respectively, and Ni@VS₂, Pd@VS₂ and Au@VS₂ are potential OER/ORR bifunctional electrocatalysts for metal-air batteries with ultralow overpotentials of 0.26/0.33 V, 0.34/0.28 V and 0.62/0.41 V, respectively. In addition, Au@VS₂ is a promising trifunctional electrocatalyst for the HER/OER/ORR with relatively low overpotentials of −0.07/0.62/0.41 V. The electronic origin of the enhanced HER/OER/ORR activity of TM@VS₂ catalysts can be well understood by the amendatory d-band center model.

{"title":"Theoretical screening of multifunctional single-atom catalysts supported by VS2 monolayer for the electrocatalytic hydrogen evolution, oxygen evolution and oxygen reduction reactions","authors":"Liang-Cai Ma , Pan-Ge Yuan , Yin-Yin Hou , Hao Li , Hai-Juan Wang , Jian-Min Zhang","doi":"10.1016/j.comptc.2025.115098","DOIUrl":"10.1016/j.comptc.2025.115098","url":null,"abstract":"<div><div>Exploring highly efficient multifunctional electrocatalysts for the HER, OER, and ORR is of great significance. In this work, transition metal atoms anchored on VS<sub>2</sub> monolayer (TM@VS<sub>2</sub>) as single-atom catalysts were systematically investigated for their HER, OER, and ORR performance through first-principles calculations. The results indicate that all TM@VS<sub>2</sub> show high thermal stability and excellent electrical conductivity. Pt@VS<sub>2</sub> and Au@VS<sub>2</sub> are predicted to be the promising HER/OER bifunctional electrocatalysts for overall water-splitting with lower overpotentials of −0.07/0.59 V and − 0.07/0.62 V, respectively, and Ni@VS<sub>2</sub>, Pd@VS<sub>2</sub> and Au@VS<sub>2</sub> are potential OER/ORR bifunctional electrocatalysts for metal-air batteries with ultralow overpotentials of 0.26/0.33 V, 0.34/0.28 V and 0.62/0.41 V, respectively. In addition, Au@VS<sub>2</sub> is a promising trifunctional electrocatalyst for the HER/OER/ORR with relatively low overpotentials of −0.07/0.62/0.41 V. The electronic origin of the enhanced HER/OER/ORR activity of TM@VS<sub>2</sub> catalysts can be well understood by the amendatory <em>d</em>-band center model.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1245 ","pages":"Article 115098"},"PeriodicalIF":3.0,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143142893","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}

引用次数: 0

First-principles study of NO2 adsorption on noble metals doped SnS2/SnSe2 heterostructure

IF 3 3区化学 Q3 CHEMISTRY, PHYSICAL

Computational and Theoretical Chemistry

Pub Date : 2025-01-23 DOI: 10.1016/j.comptc.2025.115099

Guo-Xiang Chen , Zi-Mo Xie , Wen-Long Qu , Dou-Dou Wang , Qi Zhang , Jian-Min Zhang

The adsorption behaviors of NO₂ gas molecule on pristine and noble metal (NM) atoms (Pd, Ag, Pt and Au) doped SnS₂/SnSe₂ heterostructure have been studied using the first-principles calculations based on density-functional theory (DFT-D2 method). Pristine SnS₂/SnSe₂ heterostructure exhibits small adsorption energy and low charge transfer, while the NM-doped heterostructures showed chemisorption towards NO₂ gas molecules. The introduction of NM can also enhance the interaction between the NO₂ and substrates. The significant changes in work function (WF) after NO₂ adsorption indicate that Ag-doped and Au-doped SnS₂/SnSe₂ heterostructure are more sensitive to NO₂. In addition, applying electric field and strain can also improve the adsorption behavior of NO₂ in the Ag-doped SnS₂/SnSe₂ heterostructure. Therefore, these results not only provide a fundamental understanding of NM-doped SnS₂/SnSe₂ heterostructure as promising gas sensing materials for NO₂ detection, but also provide theoretical guidance for designing high performance gas sensors based on SnS₂/SnSe₂ heterostructure.

{"title":"First-principles study of NO2 adsorption on noble metals doped SnS2/SnSe2 heterostructure","authors":"Guo-Xiang Chen , Zi-Mo Xie , Wen-Long Qu , Dou-Dou Wang , Qi Zhang , Jian-Min Zhang","doi":"10.1016/j.comptc.2025.115099","DOIUrl":"10.1016/j.comptc.2025.115099","url":null,"abstract":"<div><div>The adsorption behaviors of NO<sub>2</sub> gas molecule on pristine and noble metal (NM) atoms (Pd, Ag, Pt and Au) doped SnS<sub>2</sub>/SnSe<sub>2</sub> heterostructure have been studied using the first-principles calculations based on density-functional theory (DFT-D2 method). Pristine SnS<sub>2</sub>/SnSe<sub>2</sub> heterostructure exhibits small adsorption energy and low charge transfer, while the NM-doped heterostructures showed chemisorption towards NO<sub>2</sub> gas molecules. The introduction of NM can also enhance the interaction between the NO<sub>2</sub> and substrates. The significant changes in work function (WF) after NO<sub>2</sub> adsorption indicate that Ag-doped and Au-doped SnS<sub>2</sub>/SnSe<sub>2</sub> heterostructure are more sensitive to NO<sub>2</sub>. In addition, applying electric field and strain can also improve the adsorption behavior of NO<sub>2</sub> in the Ag-doped SnS<sub>2</sub>/SnSe<sub>2</sub> heterostructure. Therefore, these results not only provide a fundamental understanding of NM-doped SnS<sub>2</sub>/SnSe<sub>2</sub> heterostructure as promising gas sensing materials for NO<sub>2</sub> detection, but also provide theoretical guidance for designing high performance gas sensors based on SnS<sub>2</sub>/SnSe<sub>2</sub> heterostructure.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1245 ","pages":"Article 115099"},"PeriodicalIF":3.0,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143142892","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}

引用次数: 0

Encapsulation effects on the structure and stability of O3, SO2, S2O, and S3 in C60, C70, and C80 fullerenes.

IF 3 3区化学 Q3 CHEMISTRY, PHYSICAL

Computational and Theoretical Chemistry

Pub Date : 2025-01-23 DOI: 10.1016/j.comptc.2025.115096

Vishal Sharma, Vasu Nagpal, Aniruddha Chakraborty

Density functional theory computations were conducted for O₃@C_n, SO₂@C_n, S₂O@C_n, and S₃@C_n (n = 60, 70, and 80) to examine the confinement effects on the structure and relative stability of the open and cyclic forms of O₃, SO₂, S₂O, and S₃. Our study reveals that the energy gap between open and cyclic forms of O₃, SO₂, and S₂O is significantly reduced inside the C₆₀ cage, however, the open form remains energetically more favorable. Conversely, the relative stability of the open and cyclic forms of S₃ changes inside the cages (C₆₀, C₇₀, and C₈₀), with the cyclic form becoming more stable which is less stable in the isolated state. Unlike O₃, OSO (or OOS), and SSO, open structure of S₃ and SOS transform into cyclic inside the C₆₀ cage. The guest species effect on E_gap of host cages and charge transfer between the host cage and guest species are also discussed.

{"title":"Encapsulation effects on the structure and stability of O3, SO2, S2O, and S3 in C60, C70, and C80 fullerenes.","authors":"Vishal Sharma, Vasu Nagpal, Aniruddha Chakraborty","doi":"10.1016/j.comptc.2025.115096","DOIUrl":"10.1016/j.comptc.2025.115096","url":null,"abstract":"<div><div>Density functional theory computations were conducted for O<sub>3</sub>@C<sub>n</sub>, SO<sub>2</sub>@C<sub>n</sub>, S<sub>2</sub>O@C<sub>n</sub>, and S<sub>3</sub>@C<sub>n</sub> (<em>n</em> = 60, 70, and 80) to examine the confinement effects on the structure and relative stability of the open and cyclic forms of O<sub>3</sub>, SO<sub>2</sub>, S<sub>2</sub>O, and S<sub>3</sub>. Our study reveals that the energy gap between open and cyclic forms of O<sub>3</sub>, SO<sub>2</sub>, and S<sub>2</sub>O is significantly reduced inside the C<sub>60</sub> cage, however, the open form remains energetically more favorable. Conversely, the relative stability of the open and cyclic forms of S<sub>3</sub> changes inside the cages (C<sub>60</sub>, C<sub>70</sub>, and C<sub>80</sub>), with the cyclic form becoming more stable which is less stable in the isolated state. Unlike O<sub>3</sub>, OSO (or OOS), and SSO, open structure of S<sub>3</sub> and SOS transform into cyclic inside the C<sub>60</sub> cage. The guest species effect on E<sub>gap</sub> of host cages and charge transfer between the host cage and guest species are also discussed.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1245 ","pages":"Article 115096"},"PeriodicalIF":3.0,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143142897","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}

引用次数: 0

Tuning the optical and photocatalytic properties of hexagonal boron nitride through Fe and co doping: A DFT study

IF 3 3区化学 Q3 CHEMISTRY, PHYSICAL

Computational and Theoretical Chemistry

Pub Date : 2025-01-22 DOI: 10.1016/j.comptc.2025.115095

M. Bouziani , A. Bouziani , H. Zaari , F. Mezzat , R. Hausler

Hexagonal boron nitride (h-BN), a promising two-dimensional material, is known for its wide band gap (∼6 eV) and exceptional thermal and chemical stability. However, its wide band gap limits its photocatalytic applications to the ultraviolet (UV) region. In this study, we explore the effects of Iron (Fe) and Cobalt (Co) on the electronic structure, optical properties, and photocatalytic efficiency of h-BN using Density Functional Theory (DFT). The introduction of Fe and Co into the h-BN lattice is anticipated to reduce the band gap, enhance visible-light absorption, and mitigate electron-hole recombination. Our DFT calculations reveal that the doping process creates impurity states within the band gap, significantly altering the electronic structure and improving the photocatalytic performance of h-BN. The magnetic properties of Fe and Co not only modulate the electronic characteristics but also facilitate the recovery and reuse of the photocatalyst, contributing to the system's sustainability. This work provides valuable insights into the potential of Fe and Co doped h-BN for advanced photocatalytic applications, paving the way for its use in environmental remediation and renewable energy technologies.

{"title":"Tuning the optical and photocatalytic properties of hexagonal boron nitride through Fe and co doping: A DFT study","authors":"M. Bouziani , A. Bouziani , H. Zaari , F. Mezzat , R. Hausler","doi":"10.1016/j.comptc.2025.115095","DOIUrl":"10.1016/j.comptc.2025.115095","url":null,"abstract":"<div><div>Hexagonal boron nitride (h-BN), a promising two-dimensional material, is known for its wide band gap (∼6 eV) and exceptional thermal and chemical stability. However, its wide band gap limits its photocatalytic applications to the ultraviolet (UV) region. In this study, we explore the effects of Iron (Fe) and Cobalt (Co) on the electronic structure, optical properties, and photocatalytic efficiency of h-BN using Density Functional Theory (DFT). The introduction of Fe and Co into the h-BN lattice is anticipated to reduce the band gap, enhance visible-light absorption, and mitigate electron-hole recombination. Our DFT calculations reveal that the doping process creates impurity states within the band gap, significantly altering the electronic structure and improving the photocatalytic performance of h-BN. The magnetic properties of Fe and Co not only modulate the electronic characteristics but also facilitate the recovery and reuse of the photocatalyst, contributing to the system's sustainability. This work provides valuable insights into the potential of Fe and Co doped h-BN for advanced photocatalytic applications, paving the way for its use in environmental remediation and renewable energy technologies.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1245 ","pages":"Article 115095"},"PeriodicalIF":3.0,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143143147","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}

引用次数: 0

Reactive molecular dynamics simulation of the carbendazim degradation induced by reactive oxygen plasma species

IF 3 3区化学 Q3 CHEMISTRY, PHYSICAL

Computational and Theoretical Chemistry

Pub Date : 2025-01-20 DOI: 10.1016/j.comptc.2025.115092

Ruchi Mishra , Akshay Vaid , Alphonsa Joseph

Carbendazim (CBZ), a systemic benzimidazole carbamate fungicide, used in agriculture, forestry, and veterinary practices to combat fungal diseases, is notably classified as a hazardous chemical by the World Health Organization. Cold Atmospheric Plasma (CAP) has demonstrated successful pesticide degradation with notable removal rates, energy efficiency, and eco-friendly attributes. In the present work, we employed RMD simulations to investigate how reactive oxygen species (ROS) induce degradation pathways in CBZ. Our simulations demonstrate that ROS, including O atoms, OH radicals, and O₃ molecules, play a pivotal role in initiating modifications. Typically, the interaction between ROS and pesticides begins with H-abstraction, leading to the disruption and formation of key chemical bonds such as CC, CN, and CO bonds, while facilitating the formation of CC, CO, and CO bonds. Moreover, we examined the dose-dependent effects of ROS on CBZ by incrementally increasing ROS quantities within the simulation environment. As ROS concentration increases, the degree of pesticide damage also increases. The elucidated chemical pathways and statistical data provide insights into the atomic-scale degradation mechanism of CBZ, offering a theoretical foundation for optimizing pesticide degradation strategies in future applications.

{"title":"Reactive molecular dynamics simulation of the carbendazim degradation induced by reactive oxygen plasma species","authors":"Ruchi Mishra , Akshay Vaid , Alphonsa Joseph","doi":"10.1016/j.comptc.2025.115092","DOIUrl":"10.1016/j.comptc.2025.115092","url":null,"abstract":"<div><div>Carbendazim (CBZ), a systemic benzimidazole carbamate fungicide, used in agriculture, forestry, and veterinary practices to combat fungal diseases, is notably classified as a hazardous chemical by the World Health Organization. Cold Atmospheric Plasma (CAP) has demonstrated successful pesticide degradation with notable removal rates, energy efficiency, and eco-friendly attributes. In the present work, we employed RMD simulations to investigate how reactive oxygen species (ROS) induce degradation pathways in CBZ. Our simulations demonstrate that ROS, including O atoms, OH radicals, and O<sub>3</sub> molecules, play a pivotal role in initiating modifications. Typically, the interaction between ROS and pesticides begins with H-abstraction, leading to the disruption and formation of key chemical bonds such as C<img>C, C<img>N, and C<img>O bonds, while facilitating the formation of C<img>C, C<img>O, and C<img>O bonds. Moreover, we examined the dose-dependent effects of ROS on CBZ by incrementally increasing ROS quantities within the simulation environment. As ROS concentration increases, the degree of pesticide damage also increases. The elucidated chemical pathways and statistical data provide insights into the atomic-scale degradation mechanism of CBZ, offering a theoretical foundation for optimizing pesticide degradation strategies in future applications.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1245 ","pages":"Article 115092"},"PeriodicalIF":3.0,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143142891","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}

引用次数: 0

Adsorption and gas-sensing performance of sulfur gases on SnS/GeSe heterojunction

IF 3 3区化学 Q3 CHEMISTRY, PHYSICAL

Computational and Theoretical Chemistry

Pub Date : 2025-01-20 DOI: 10.1016/j.comptc.2025.115079

En-Zhi Liu , Yu-Fang Chu , Wen-Wen Liu , Jian-Ping Liu , Fang Xie , Zhi-Qiang Fan

This article uses first principles calculations to study the electronic transport properties of two-dimensional materials germanium selenide (GeSe), tin sulfide (SnS), and their SnS/GeSe van der Waals heterostructures for adsorbing three sulfur gases. Through total energy calculations, we determined that H₂S and SO₂ tend to adsorb more readily to the vacancies on the surfaces of GeSe, SnS, and the SnS/GeSe heterojunctions, whereas SO₃ shows a stronger preference for adsorbing to the top sites. By analyzing the band structure of sulfur gases after adsorption, we found that H₂S adsorption has no regulatory effect on the electronic structure of monolayers and heterojunctions, but the adsorption of SO₂ and SO₃ can regulate the electronic structure of monolayers and heterojunctions to varying degrees. Among them, the adsorption of SO₂ most significantly modulates the band structure, not only adjusting the position of energy distribution within the band structure but also inducing new energy band. Therefore, we constructed a gas sensing device based on SnS/GeSe heterojunction and focused on studying the electronic transport properties before and after SO₂ adsorption. The device without gas adsorption consistently exhibit very small currents within the bias voltage range of −0.7 V to 0.7 V. However, the adsorption of SO₂ notably enhances the current of the device and displays a negative differential resistance effect in both positive and negative bias region, with a peak-to-valley ratio approaching 300. Therefore, we conclude that SnS/GeSe heterojunction devices can serve as gas sensitive adsorption detection devices for SO₂, which has important physical significance for further understanding the electronic transport mechanism of molecular devices.

{"title":"Adsorption and gas-sensing performance of sulfur gases on SnS/GeSe heterojunction","authors":"En-Zhi Liu , Yu-Fang Chu , Wen-Wen Liu , Jian-Ping Liu , Fang Xie , Zhi-Qiang Fan","doi":"10.1016/j.comptc.2025.115079","DOIUrl":"10.1016/j.comptc.2025.115079","url":null,"abstract":"<div><div>This article uses first principles calculations to study the electronic transport properties of two-dimensional materials germanium selenide (GeSe), tin sulfide (SnS), and their SnS/GeSe van der Waals heterostructures for adsorbing three sulfur gases. Through total energy calculations, we determined that H<sub>2</sub>S and SO<sub>2</sub> tend to adsorb more readily to the vacancies on the surfaces of GeSe, SnS, and the SnS/GeSe heterojunctions, whereas SO<sub>3</sub> shows a stronger preference for adsorbing to the top sites. By analyzing the band structure of sulfur gases after adsorption, we found that H<sub>2</sub>S adsorption has no regulatory effect on the electronic structure of monolayers and heterojunctions, but the adsorption of SO<sub>2</sub> and SO<sub>3</sub> can regulate the electronic structure of monolayers and heterojunctions to varying degrees. Among them, the adsorption of SO<sub>2</sub> most significantly modulates the band structure, not only adjusting the position of energy distribution within the band structure but also inducing new energy band. Therefore, we constructed a gas sensing device based on SnS/GeSe heterojunction and focused on studying the electronic transport properties before and after SO<sub>2</sub> adsorption. The device without gas adsorption consistently exhibit very small currents within the bias voltage range of −0.7 V to 0.7 V. However, the adsorption of SO<sub>2</sub> notably enhances the current of the device and displays a negative differential resistance effect in both positive and negative bias region, with a peak-to-valley ratio approaching 300. Therefore, we conclude that SnS/GeSe heterojunction devices can serve as gas sensitive adsorption detection devices for SO<sub>2</sub>, which has important physical significance for further understanding the electronic transport mechanism of molecular devices.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1245 ","pages":"Article 115079"},"PeriodicalIF":3.0,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143143771","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}

引用次数: 0

Numerical simulation of space charge transport properties of polypropylene laminated paper

IF 3 3区化学 Q3 CHEMISTRY, PHYSICAL

Computational and Theoretical Chemistry

Pub Date : 2025-01-20 DOI: 10.1016/j.comptc.2025.115089

Xi Chen, Minghan Li, Rui Li, Junyi Ma, Tianyan Jiang, Maoqiang Bi

Polypropylene laminated paper (PPLP) serves as an exemplary insulation material for high-temperature superconducting direct current (DC) cables. However, the accumulation of internal space charge can distort the local electric field intensity, leading to material degradation. Currently, the majority of space charge transport analyses for PPLP rely on experimental measurements, with its microscopic processes necessitating further exploration. This paper delves into the interaction and evolution processes among various microscopic particles through numerical simulation. Adopting the bipolar carrier model, we analyze the impacts of temperature, mobility, trap density, and trap energy level on the space charge distribution within PPLP by integrating the interface charge theory and trap theory of multilayer dielectrics. Our findings reveal that as temperature decreases, the space charge injection effect diminishes and stabilizes after reaching a certain threshold. Lower mobility results in charge accumulation at the corresponding electrode, causing electric field distortion and a more pronounced damaging effect, whereas charge accumulation in the middle region is less significant, leading to lesser damage. Furthermore, lower trap levels and densities result in weaker charge accumulation, with charges migrating more towards the opposite electrode, thus exhibiting heteropolar charge accumulation at the electrodes.

{"title":"Numerical simulation of space charge transport properties of polypropylene laminated paper","authors":"Xi Chen, Minghan Li, Rui Li, Junyi Ma, Tianyan Jiang, Maoqiang Bi","doi":"10.1016/j.comptc.2025.115089","DOIUrl":"10.1016/j.comptc.2025.115089","url":null,"abstract":"<div><div>Polypropylene laminated paper (PPLP) serves as an exemplary insulation material for high-temperature superconducting direct current (DC) cables. However, the accumulation of internal space charge can distort the local electric field intensity, leading to material degradation. Currently, the majority of space charge transport analyses for PPLP rely on experimental measurements, with its microscopic processes necessitating further exploration. This paper delves into the interaction and evolution processes among various microscopic particles through numerical simulation. Adopting the bipolar carrier model, we analyze the impacts of temperature, mobility, trap density, and trap energy level on the space charge distribution within PPLP by integrating the interface charge theory and trap theory of multilayer dielectrics. Our findings reveal that as temperature decreases, the space charge injection effect diminishes and stabilizes after reaching a certain threshold. Lower mobility results in charge accumulation at the corresponding electrode, causing electric field distortion and a more pronounced damaging effect, whereas charge accumulation in the middle region is less significant, leading to lesser damage. Furthermore, lower trap levels and densities result in weaker charge accumulation, with charges migrating more towards the opposite electrode, thus exhibiting heteropolar charge accumulation at the electrodes.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1245 ","pages":"Article 115089"},"PeriodicalIF":3.0,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143142888","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}

引用次数: 0

Deciphering the mechanism and selectivities of the reactions of mesitonitrile oxide with 1,5-Dimethyl-6-methylenetricyclo[3.2.1.02,7]oct-3-en-8-one Derivatives: A computational approach

IF 3 3区化学 Q3 CHEMISTRY, PHYSICAL

Computational and Theoretical Chemistry

Pub Date : 2025-01-20 DOI: 10.1016/j.comptc.2025.115093

Anthony Tawiah, Gabriel Amankwah, Benjamin Gyedu Akonor, Evans Adei

Isoxazoline and spirocyclic compounds have been recognized for their notable biological significance in various studies. The preferential selectivities and underlining molecular reaction path for the [3 + 2] cycloaddition reactions of mesitonitrile oxide with 1,5-dimethyl-6-methylenetricyclo[3.2.1.0^2,7]oct-3-en-8-one derivatives have been investigated by employing the hybrid B3LYP/6-311G (d, p) density functional theory. The reaction between mesitonitrile oxide and 1,5,8-trimethyl-6-methylenetricyclo[3.2.1.0^2,7]oct-3-en-8-endo-ol site- and regioselectively proceed by adding across the endocyclic site of the 1,5,8-trimethyl-6-methylenetricyclo[3.2.1.0^2,7]oct-3-en-8-endo-ol. The computed global electron density transfer results predict a low polar process for the mechanism. Analysis from the intrinsic reaction coordinates also confirms the obtained stationary points’ geometries and energies. The global reactivity indices analysis shows that the mesitonitrile oxide behaves as an electrophile in all the reactions. The calculated local reactivity indices align with the energetic trends and the experimentally observed site- and regioselectivity of the [3 + 2] cycloaddition reaction.

{"title":"Deciphering the mechanism and selectivities of the reactions of mesitonitrile oxide with 1,5-Dimethyl-6-methylenetricyclo[3.2.1.02,7]oct-3-en-8-one Derivatives: A computational approach","authors":"Anthony Tawiah, Gabriel Amankwah, Benjamin Gyedu Akonor, Evans Adei","doi":"10.1016/j.comptc.2025.115093","DOIUrl":"10.1016/j.comptc.2025.115093","url":null,"abstract":"<div><div>Isoxazoline and spirocyclic compounds have been recognized for their notable biological significance in various studies. The preferential selectivities and underlining molecular reaction path for the [3 + 2] cycloaddition reactions of mesitonitrile oxide with 1,5-dimethyl-6-methylenetricyclo[3.2.1.0<sup>2,7</sup>]oct-3-en-8-one derivatives have been investigated by employing the hybrid B3LYP/6-311G (d, p) density functional theory. The reaction between mesitonitrile oxide and 1,5,8-trimethyl-6-methylenetricyclo[3.2.1.0<sup>2,7</sup>]oct-3-en-8-<em>endo</em>-ol site- and regioselectively proceed by adding across the endocyclic site of the 1,5,8-trimethyl-6-methylenetricyclo[3.2.1.0<sup>2,7</sup>]oct-3-en-8-<em>endo</em>-ol. The computed global electron density transfer results predict a low polar process for themechanism. Analysis from the intrinsic reaction coordinates also confirms the obtained stationary points’ geometries and energies. The global reactivity indices analysis shows that the mesitonitrile oxide behaves as an electrophile in all the reactions. The calculated local reactivity indices align with the energetic trends and the experimentally observed site- and regioselectivity of the [3 + 2] cycloaddition reaction.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1245 ","pages":"Article 115093"},"PeriodicalIF":3.0,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143142889","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}

引用次数: 0

Caffeine as a stabilizer in Novel Hydroxypropyl-β-cyclodextrin/Axitinib Drug-Delivery Systems: A computational study

IF 3 3区化学 Q3 CHEMISTRY, PHYSICAL

Computational and Theoretical Chemistry

Pub Date : 2025-01-18 DOI: 10.1016/j.comptc.2025.115091

Yeng-Tseng Wang , Tun-Chieh Chen

Age-related macular degeneration (AMD) is a significant global health concern. Axitinib shows high potential for treating wet AMD, but its lipophilic nature makes it difficult to penetrate the cornea. Cyclodextrins (CDs) are promising drug carriers for axitinib due to their hydrophilic outer surface and lipophilic central cavity. However, lipophilic drug/CD complexes may dissociate in water at the same time. Huang et al. found that caffeine molecules can stabilise lipophilic drug/CD complexes, and caffeine-axitinib-hydroxypropyl-β-cyclodextrin (HPβCD) complexes can decrease lipophilic drug/CD complex dissociation. To investigate the interaction mechanisms between the components of caffeine-axitinib-HPβCD complexes, we employed a combination of computational methods, including Ligand Gaussian Accelerated Molecular Dynamics (LiGaMD), 1D potential of mean force (PMF) profiling, ligand binding kinetics analysis based on Kramers’ rate theory, density functional theory (DFT) calculations, and Interaction Region Identifier (IRI) analysis. Our predicted association rate constan k_on rate constants were similar, but k_off rate values decreased when caffeine was added as a stabilizer. The dissociation rate constan k_off values for axitinib-HPβCD, axitinib-HPβCD-caffeine (primary face), axitinib-HPβCD-caffeine (secondary face), and axitinib-HPβCD-caffeine (primary and secondary faces) were 3.000 ± 0.190 s⁻¹, 1.800 ± 0.210 s^−1, 1.700 ± 0.170 s⁻¹, and 0.50 ± 0.001 s⁻¹, respectively. Our IRI analysis results showed that caffeine attaches to the primary and secondary faces of the axitinib-HPβCD complex via van der Waals forces. As a stabilizer, caffeine helps maintain the integrity of the axitinib-HPβCD complex, thereby slowing down the release of axitinib from HPβCD.

{"title":"Caffeine as a stabilizer in Novel Hydroxypropyl-β-cyclodextrin/Axitinib Drug-Delivery Systems: A computational study","authors":"Yeng-Tseng Wang , Tun-Chieh Chen","doi":"10.1016/j.comptc.2025.115091","DOIUrl":"10.1016/j.comptc.2025.115091","url":null,"abstract":"<div><div>Age-related macular degeneration (AMD) is a significant global health concern. Axitinib shows high potential for treating wet AMD, but its lipophilic nature makes it difficult to penetrate the cornea. Cyclodextrins (CDs) are promising drug carriers for axitinib due to their hydrophilic outer surface and lipophilic central cavity. However, lipophilic drug/CD complexes may dissociate in water at the same time. Huang et al. found that caffeine molecules can stabilise lipophilic drug/CD complexes, and caffeine-axitinib-hydroxypropyl-β-cyclodextrin (HPβCD) complexes can decrease lipophilic drug/CD complex dissociation. To investigate the interaction mechanisms between the components of caffeine-axitinib-HPβCD complexes, we employed a combination of computational methods, including Ligand Gaussian Accelerated Molecular Dynamics (LiGaMD), 1D potential of mean force (PMF) profiling, ligand binding kinetics analysis based on Kramers’ rate theory, density functional theory (DFT) calculations, and Interaction Region Identifier (IRI) analysis. Our predicted association rate constan k<sub>on</sub> rate constants were similar, but k<sub>off</sub> rate values decreased when caffeine was added as a stabilizer. The dissociation rate constan k<sub>off</sub> values for axitinib-HPβCD, axitinib-HPβCD-caffeine (primary face), axitinib-HPβCD-caffeine (secondary face), and axitinib-HPβCD-caffeine (primary and secondary faces) were 3.000 ± 0.190 s<sup>−1</sup>, 1.800 ± 0.210 s<sup>−1,</sup> 1.700 ± 0.170 s<sup>−1</sup>, and 0.50 ± 0.001 s<sup>−1</sup>, respectively. Our IRI analysis results showed that caffeine attaches to the primary and secondary faces of the axitinib-HPβCD complex via van der Waals forces. As a stabilizer, caffeine helps maintain the integrity of the axitinib-HPβCD complex, thereby slowing down the release of axitinib from HPβCD.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1245 ","pages":"Article 115091"},"PeriodicalIF":3.0,"publicationDate":"2025-01-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143142894","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}

引用次数: 0

Aluminum clusters graphene supported a DFT-based genetic algorithm study

IF 3 3区化学 Q3 CHEMISTRY, PHYSICAL

Computational and Theoretical Chemistry

Pub Date : 2025-01-18 DOI: 10.1016/j.comptc.2025.115094

Camilo Rodríguez-Quintero , S. Amaya-Roncancio , Mauricio Suárez-Durán , Darwin Augusto Torres-Cerón , Jorge H. Quintero-Orozco

Genetic Algorithm (GA) in conjunction with Density Functional Theory (DFT) was implemented to optimize the geometric configurations of aluminum clusters (Al_n, n = 3–40). GA efficiently explored the configurational space by evolving randomly generated initial structures through selection, crossover, and mutation, yielding energetically metal clusters. Subsequently, DFT was employed to relax these structures, ensuring the precise determination of the most stable geometries. The results showed that the binding energy per aluminum atom increased progressively with cluster size, approaching values close to that of bulk aluminum for large clusters. Notably, clusters with fewer atoms (Al_n, n = 3–9) displayed diverse and irregular geometries, while larger clusters (Al_n, n = 10–40) exhibited defined and stable configurations. Additionally, the obtained aluminum clusters were supported on defected graphene surfaces, undergoing structural rearrangements while maintaining their energetic stability. These results highlight the influence of surface interactions on the minimum energy configurations. This study demonstrates the robust capabilities of the combined GA-DFT approach for predicting structural and energetic properties of metal clusters, offering valuable insights for applications in catalysis and materials science.

{"title":"Aluminum clusters graphene supported a DFT-based genetic algorithm study","authors":"Camilo Rodríguez-Quintero , S. Amaya-Roncancio , Mauricio Suárez-Durán , Darwin Augusto Torres-Cerón , Jorge H. Quintero-Orozco","doi":"10.1016/j.comptc.2025.115094","DOIUrl":"10.1016/j.comptc.2025.115094","url":null,"abstract":"<div><div>Genetic Algorithm (GA) in conjunction with Density Functional Theory (DFT) was implemented to optimize the geometric configurations of aluminum clusters (Al<em><sub>n</sub></em>, <em>n</em> = 3–40). GA efficiently explored the configurational space by evolving randomly generated initial structures through selection, crossover, and mutation, yielding energetically metal clusters. Subsequently, DFT was employed to relax these structures, ensuring the precise determination of the most stable geometries. The results showed that the binding energy per aluminum atom increased progressively with cluster size, approaching values close to that of bulk aluminum for large clusters. Notably, clusters with fewer atoms (Al<em><sub>n</sub></em>, <em>n</em> = 3–9) displayed diverse and irregular geometries, while larger clusters (Al<em><sub>n</sub></em>, <em>n</em> = 10–40) exhibited defined and stable configurations. Additionally, the obtained aluminum clusters were supported on defected graphene surfaces, undergoing structural rearrangements while maintaining their energetic stability. These results highlight the influence of surface interactions on the minimum energy configurations. This study demonstrates the robust capabilities of the combined GA-DFT approach for predicting structural and energetic properties of metal clusters, offering valuable insights for applications in catalysis and materials science.</div></div>","PeriodicalId":284,"journal":{"name":"Computational and Theoretical Chemistry","volume":"1245 ","pages":"Article 115094"},"PeriodicalIF":3.0,"publicationDate":"2025-01-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143142884","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}

引用次数: 0

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