Machine‐learned force fields (MLFFs) promise to offer a computationally efficient alternative to ab initio simulations for complex molecular systems. However, ensuring their generalizability beyond training data is crucial for their wide application in studying solid materials. This work investigates the ability of a graph neural network (GNN)‐based MLFF, trained on Lennard–Jones Argon, to describe solid‐state phenomena not explicitly included during training. The MLFF's performance is assessed in predicting phonon density of states (PDOS) for a perfect face‐centered cubic (FCC) crystal structure at both zero and finite temperatures. Additionally, vacancy migration rates and energy barriers are evaluated in an imperfect crystal using direct molecular dynamics (MD) simulations and the string method. Notably, vacancy configurations are absent from the training data. These results demonstrate the MLFF's capability to capture essential solid‐state properties with good agreement to reference data, even for unseen configurations. Data engineering strategies are further discussed to enhance the generalizability of MLFFs. The proposed set of benchmark tests and workflow for evaluating MLFF performance in describing perfect and imperfect crystals pave the way for reliable application of MLFFs in studying complex solid‐state materials.
{"title":"Generalizability of Graph Neural Network Force Fields for Predicting Solid‐State Properties","authors":"Shaswat Mohanty, Yifan Wang, Wei Cai","doi":"10.1002/adts.202401058","DOIUrl":"https://doi.org/10.1002/adts.202401058","url":null,"abstract":"Machine‐learned force fields (MLFFs) promise to offer a computationally efficient alternative to ab initio simulations for complex molecular systems. However, ensuring their generalizability beyond training data is crucial for their wide application in studying solid materials. This work investigates the ability of a graph neural network (GNN)‐based MLFF, trained on Lennard–Jones Argon, to describe solid‐state phenomena not explicitly included during training. The MLFF's performance is assessed in predicting phonon density of states (PDOS) for a perfect face‐centered cubic (FCC) crystal structure at both zero and finite temperatures. Additionally, vacancy migration rates and energy barriers are evaluated in an imperfect crystal using direct molecular dynamics (MD) simulations and the string method. Notably, vacancy configurations are absent from the training data. These results demonstrate the MLFF's capability to capture essential solid‐state properties with good agreement to reference data, even for unseen configurations. Data engineering strategies are further discussed to enhance the generalizability of MLFFs. The proposed set of benchmark tests and workflow for evaluating MLFF performance in describing perfect and imperfect crystals pave the way for reliable application of MLFFs in studying complex solid‐state materials.","PeriodicalId":7219,"journal":{"name":"Advanced Theory and Simulations","volume":"81 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142917017","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Noy Midler, Ekaterina Kuznetsova, Shahar Shalom, Dilorom Begmatova, Dekel Rosenfeld
Hyperthermia therapy involves the controlled elevation of tissue temperature. It holds promise as a therapeutic modality for various medical applications, including tissue ablation and the activation of thermosensitive cellular mechanisms. This study leverages finite element modeling (FEM) of nanomaterial-mediated hyperthermia to optimize the geometry of the heat source within the tissue, with the goal of maximizing temperature distribution in solid and hollow organs, tailored for activation of heat-sensitive ion channels while aspiring to minimize tissue damage or ablation. The models consider physiological factors, such as surrounding fat tissues, vascularization, and fluids, and are developed to match rodent experiments with a scale-up to human scale organs. The two examined heat source configurations are direct injection of droplets of magnetic nanoparticles versus attached heat-generating magnetic transducers. The externally attached heat sources prove more effective at achieving therapeutic temperatures with minimal invasiveness, particularly in hollow organs. Furthermore, the simulations demonstrate the importance of heat source volume and density for uniform temperature distribution and reduced tissue damage. Human-scale models demonstrate the heat source and stimulation duration required for hyperthermia in organs. The suggested model is verified experimentally to match electrogenic cell modulation via heat-sensitive receptors, paving the way for more precise and safer treatments.
{"title":"In Silico Study on the Geometry of Thermal Transducers in Magnetothermal Stimulation","authors":"Noy Midler, Ekaterina Kuznetsova, Shahar Shalom, Dilorom Begmatova, Dekel Rosenfeld","doi":"10.1002/adts.202401071","DOIUrl":"https://doi.org/10.1002/adts.202401071","url":null,"abstract":"Hyperthermia therapy involves the controlled elevation of tissue temperature. It holds promise as a therapeutic modality for various medical applications, including tissue ablation and the activation of thermosensitive cellular mechanisms. This study leverages finite element modeling (FEM) of nanomaterial-mediated hyperthermia to optimize the geometry of the heat source within the tissue, with the goal of maximizing temperature distribution in solid and hollow organs, tailored for activation of heat-sensitive ion channels while aspiring to minimize tissue damage or ablation. The models consider physiological factors, such as surrounding fat tissues, vascularization, and fluids, and are developed to match rodent experiments with a scale-up to human scale organs. The two examined heat source configurations are direct injection of droplets of magnetic nanoparticles versus attached heat-generating magnetic transducers. The externally attached heat sources prove more effective at achieving therapeutic temperatures with minimal invasiveness, particularly in hollow organs. Furthermore, the simulations demonstrate the importance of heat source volume and density for uniform temperature distribution and reduced tissue damage. Human-scale models demonstrate the heat source and stimulation duration required for hyperthermia in organs. The suggested model is verified experimentally to match electrogenic cell modulation via heat-sensitive receptors, paving the way for more precise and safer treatments.","PeriodicalId":7219,"journal":{"name":"Advanced Theory and Simulations","volume":"35 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2024-12-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142905402","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ning Yang, Li‐yang Su, Wei‐teng Li, Xiu‐ming Li, Li‐yuan Wang, Yu‐chun Mei, Bing‐jun Sun
To clarify the supporting effect and influencing factors of energy‐absorbing rockbolts in soft rock roadways with large deformation, by considering four factors including rock deformation, plastic zone, rockbolt force, and stress of the surrounding rock, comparative analysis of no‐rockbolt, conventional rockbolt, and energy‐absorbing rockbolt schemes is conducted. The effect of the energy‐absorbing rockbolt is analyzed based on a self‐developed numerical simulation program, and a study is conducted on the influence of five factors such as the energy‐absorption starting axial force, ultimate yielding distance on the supporting effect. The results show that: 1) Compared to conventional rockbolts, the energy‐absorbing rockbolts maintain a intact support system and continuously providing support resistance within 75 d of calculation. 2) Energy‐absorbing rockbolts significantly increase the maximum and minimum principal stresses of the roadway. The increase in maximum principal stress significantly enhances the range of the bearing arch in the surrounding rock. Energy‐absorbing rockbolts have a high capacity to compensate for radial stresses unloaded. 3) The greater the energy‐absorption starting axial force, the more significant the compensation effect of the rockbolts on the radial stress. Appropriately increasing the ultimate yielding distance and rockbolt length can effectively prevent rockbolt failure and control the area of plastic zone.
{"title":"Supporting Effect and Influence Law of Energy‐Absorbing Rockbolts in Soft Rock Roadway with Large Deformation","authors":"Ning Yang, Li‐yang Su, Wei‐teng Li, Xiu‐ming Li, Li‐yuan Wang, Yu‐chun Mei, Bing‐jun Sun","doi":"10.1002/adts.202400832","DOIUrl":"https://doi.org/10.1002/adts.202400832","url":null,"abstract":"To clarify the supporting effect and influencing factors of energy‐absorbing rockbolts in soft rock roadways with large deformation, by considering four factors including rock deformation, plastic zone, rockbolt force, and stress of the surrounding rock, comparative analysis of no‐rockbolt, conventional rockbolt, and energy‐absorbing rockbolt schemes is conducted. The effect of the energy‐absorbing rockbolt is analyzed based on a self‐developed numerical simulation program, and a study is conducted on the influence of five factors such as the energy‐absorption starting axial force, ultimate yielding distance on the supporting effect. The results show that: 1) Compared to conventional rockbolts, the energy‐absorbing rockbolts maintain a intact support system and continuously providing support resistance within 75 d of calculation. 2) Energy‐absorbing rockbolts significantly increase the maximum and minimum principal stresses of the roadway. The increase in maximum principal stress significantly enhances the range of the bearing arch in the surrounding rock. Energy‐absorbing rockbolts have a high capacity to compensate for radial stresses unloaded. 3) The greater the energy‐absorption starting axial force, the more significant the compensation effect of the rockbolts on the radial stress. Appropriately increasing the ultimate yielding distance and rockbolt length can effectively prevent rockbolt failure and control the area of plastic zone.","PeriodicalId":7219,"journal":{"name":"Advanced Theory and Simulations","volume":"328 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2024-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142901809","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Maryam Babaei, Vahid Ahmadi, Seyed Mojtaba Pakzad Moghadam
The development of halide double perovskites has received a lot of interest from many researchers due to solving the problem of poor stability and toxicity of lead‐based perovskites, which hinders the commercialization of perovskite solar cells. Therefore, in this work, the adsorption of water molecules, stability, optical, and electronic properties of double perovskites Cs2AgInX6 (X = Br, Cl) are investigated using Density Functional Theory (DFT) calculations. Theoretical analysis shows that these double perovskites are thermodynamically stable. The diffusion coefficient of water in layers of Cs2AgInBr6 and Cs2AgInCl6 is much lower than that of MAPbI3 according to means square displacement analysis, and also based on values of adsorption energy, the hydrophilicity of the proposed structure is lower than that of PbI2‐terminated and MAI‐terminated surfaces. These materials demonstrate better ductility and mechanical stability than their corresponding 3D perovskites. For Cs2AgInBr6 and Cs2AgInCl6, direct bandgap values are 1.49 and 3.14 eV, respectively, using hybrid Perdew‐Berke‐Ernzerhof + spin‐orbit‐coupling(PBE0+SOC) functional. Calculations of key solar cell parameters predict that Cs2AgInBr6 may achieve efficiencies competitive with MAPbI3 due to its high short‐circuit current, making it a promising stable, non‐toxic perovskite absorber material. This work provides fundamental insights that can guide further research on double perovskites for lead‐free, moisture‐resistant perovskite solar technologies.
{"title":"Water Molecules Adsorption, Stability, and Optoelectronic Characteristics of Pb‐Free Hybrid Double Perovskites Cs2AgInX6 (X = Br, Cl) for Solar Cells Application: A DFT Analysis","authors":"Maryam Babaei, Vahid Ahmadi, Seyed Mojtaba Pakzad Moghadam","doi":"10.1002/adts.202401024","DOIUrl":"https://doi.org/10.1002/adts.202401024","url":null,"abstract":"The development of halide double perovskites has received a lot of interest from many researchers due to solving the problem of poor stability and toxicity of lead‐based perovskites, which hinders the commercialization of perovskite solar cells. Therefore, in this work, the adsorption of water molecules, stability, optical, and electronic properties of double perovskites Cs<jats:sub>2</jats:sub>AgInX<jats:sub>6</jats:sub> (X = Br, Cl) are investigated using Density Functional Theory (DFT) calculations. Theoretical analysis shows that these double perovskites are thermodynamically stable. The diffusion coefficient of water in layers of Cs<jats:sub>2</jats:sub>AgInBr<jats:sub>6</jats:sub> and Cs<jats:sub>2</jats:sub>AgInCl<jats:sub>6</jats:sub> is much lower than that of MAPbI<jats:sub>3</jats:sub> according to means square displacement analysis, and also based on values of adsorption energy, the hydrophilicity of the proposed structure is lower than that of PbI<jats:sub>2</jats:sub>‐terminated and MAI‐terminated surfaces. These materials demonstrate better ductility and mechanical stability than their corresponding 3D perovskites. For Cs<jats:sub>2</jats:sub>AgInBr<jats:sub>6</jats:sub> and Cs<jats:sub>2</jats:sub>AgInCl<jats:sub>6</jats:sub>, direct bandgap values are 1.49 and 3.14 eV, respectively, using hybrid Perdew‐Berke‐Ernzerhof + spin‐orbit‐coupling(PBE0+SOC) functional. Calculations of key solar cell parameters predict that Cs<jats:sub>2</jats:sub>AgInBr<jats:sub>6</jats:sub> may achieve efficiencies competitive with MAPbI<jats:sub>3</jats:sub> due to its high short‐circuit current, making it a promising stable, non‐toxic perovskite absorber material. This work provides fundamental insights that can guide further research on double perovskites for lead‐free, moisture‐resistant perovskite solar technologies.","PeriodicalId":7219,"journal":{"name":"Advanced Theory and Simulations","volume":"31 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2024-12-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142887801","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
In this analytical study, four‐layer MoS2‐based renewable energy photovoltaic cell has been first introduced using SCAPS‐1d. Proposed cell has FTO as window layer, ZnSe as electron transport layer (ETL), MoS2 as absorber layer, and an exclusive Zn3P2 hole transport layer (HTL) with least lattice mismatch of about 1.8%. To explore highest performance through proposed novel solar cell configuration, simulation studies have been done on best possible optimized physical and electrical parameters. Simulated power conversion efficiency, short circuit current, open circuit voltage, and fill factor are 32.55%, 37.75 mA/cm2, 1038.4 mV, and 83.01% respectively. Further to investigate defect states between band levels, admittance, and impedance spectroscopic analysis has been done with an equivalent electrical circuit model obtained from EIS module. Present studies help to identify the carrier accumulation behavior at various least‐lattice mismatched interfaces and in bulk of four‐layer solar device. For this analysis, proposed renewable solar device is simulated for characteristics such as capacitance‐voltage (C‐V), capacitance‐frequency (C‐F), conductance‐voltage (G‐V), and conductance‐frequency (G‐F) under different suitable and practical physical conditions. In this technique, AC signal is applied to the solutions obtained from the semiconductor and continuity equations in SCAPS‐1d. Further, we have done an in‐depth analysis through these measurements.
{"title":"Comprehensive Spectroscopic Investigation of MoS2‐Solar Cells with Exclusive Zn3P2 as HTL Having Least Lattice Mismatches for 32.55% PCE","authors":"Atish Kumar Sharma, Ankita Srivastava, Prakash Kumar Jha, Keyur Sangani, Nitesh K. Chourasia, Ritesh Kumar Chourasia","doi":"10.1002/adts.202401237","DOIUrl":"https://doi.org/10.1002/adts.202401237","url":null,"abstract":"In this analytical study, four‐layer MoS<jats:sub>2</jats:sub>‐based renewable energy photovoltaic cell has been first introduced using SCAPS‐1d. Proposed cell has FTO as window layer, ZnSe as electron transport layer (ETL), MoS<jats:sub>2</jats:sub> as absorber layer, and an exclusive Zn<jats:sub>3</jats:sub>P<jats:sub>2</jats:sub> hole transport layer (HTL) with least lattice mismatch of about 1.8%. To explore highest performance through proposed novel solar cell configuration, simulation studies have been done on best possible optimized physical and electrical parameters. Simulated power conversion efficiency, short circuit current, open circuit voltage, and fill factor are 32.55%, 37.75 mA/cm<jats:sup>2</jats:sup>, 1038.4 mV, and 83.01% respectively. Further to investigate defect states between band levels, admittance, and impedance spectroscopic analysis has been done with an equivalent electrical circuit model obtained from EIS module. Present studies help to identify the carrier accumulation behavior at various least‐lattice mismatched interfaces and in bulk of four‐layer solar device. For this analysis, proposed renewable solar device is simulated for characteristics such as capacitance‐voltage (C‐V), capacitance‐frequency (C‐F), conductance‐voltage (G‐V), and conductance‐frequency (G‐F) under different suitable and practical physical conditions. In this technique, AC signal is applied to the solutions obtained from the semiconductor and continuity equations in SCAPS‐1d. Further, we have done an in‐depth analysis through these measurements.","PeriodicalId":7219,"journal":{"name":"Advanced Theory and Simulations","volume":"14 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2024-12-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142887800","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Effective antiviral drug delivery systems, such as for 4′-Fluorouridine (4′-FlU), are crucial for addressing viral infections like COVID-19. This study used ab-initio analysis to examine interactions between 4′-FlU and graphene oxide (GO)-based carriers, with and without polyethylene glycol (PEG) functionalization, across various physiological conditions. Non-PEGylated GO showed strong gas-phase binding (−103.36 kcal mol−1), supporting systemic stability, while PEGylation reduced aqueous-phase binding (−33.72 kcal mol−1), enhancing biocompatibility and circulation. Adsorption energies were significant in acidic and alkaline environments, with PEGylation intensifying alkaline interactions (−118.42 kcal mol−1). Charge transfer dynamics, influenced by pH and PEGylation, revealed enhanced stability under acidic conditions, suitable for tumor microenvironments. Hydrogen bonding stabilized GO-drug complexes, ensuring prolonged release. PEGylated GO excelled in acidic environments, especially for tumor delivery, as confirmed by miscibility studies and controlled release kinetics. Thermodynamic and quantum chemical analyses highlighted environmental factors and PEGylation in optimizing stability and reactivity. GO/PEG-4′-FlU is ideal for localized drug delivery in acidic tumors, while GO/4′-FlU supports systemic delivery requiring broader dispersion. This research lays the groundwork for nanotechnology-based antiviral strategies and the design of adaptable drug delivery systems for both systemic and localized applications.
{"title":"Pegylated Graphene Oxide For 4′-Fluorouridine Delivery: An Ab Initio Approach to Antiviral Therapy","authors":"Oluwasegun Chijioke Adekoya, Gbolahan Joseph Adekoya, Wanjun Liu, Emmanuel Rotimi Sadiku, Yskandar Hamam","doi":"10.1002/adts.202401145","DOIUrl":"https://doi.org/10.1002/adts.202401145","url":null,"abstract":"Effective antiviral drug delivery systems, such as for 4′-Fluorouridine (4′-FlU), are crucial for addressing viral infections like COVID-19. This study used ab-initio analysis to examine interactions between 4′-FlU and graphene oxide (GO)-based carriers, with and without polyethylene glycol (PEG) functionalization, across various physiological conditions. Non-PEGylated GO showed strong gas-phase binding (−103.36 kcal mol<sup>−1</sup>), supporting systemic stability, while PEGylation reduced aqueous-phase binding (−33.72 kcal mol<sup>−1</sup>), enhancing biocompatibility and circulation. Adsorption energies were significant in acidic and alkaline environments, with PEGylation intensifying alkaline interactions (−118.42 kcal mol<sup>−1</sup>). Charge transfer dynamics, influenced by pH and PEGylation, revealed enhanced stability under acidic conditions, suitable for tumor microenvironments. Hydrogen bonding stabilized GO-drug complexes, ensuring prolonged release. PEGylated GO excelled in acidic environments, especially for tumor delivery, as confirmed by miscibility studies and controlled release kinetics. Thermodynamic and quantum chemical analyses highlighted environmental factors and PEGylation in optimizing stability and reactivity. GO/PEG-4′-FlU is ideal for localized drug delivery in acidic tumors, while GO/4′-FlU supports systemic delivery requiring broader dispersion. This research lays the groundwork for nanotechnology-based antiviral strategies and the design of adaptable drug delivery systems for both systemic and localized applications.","PeriodicalId":7219,"journal":{"name":"Advanced Theory and Simulations","volume":"2 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2024-12-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142887237","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The air pollution and the rising emission of dangerous gases into the atmosphere are recently worrisome. In order to protect the humans and animals life's, it is crucial to monitor these harmful gases. Gases like HCHO, N2, NH3, CO2, CH4, CO, and SO2 are dangerous for human health. As a result, gas sensors have been attracted significant interest as a means to effectively detect and adsorb these pollutants. In this study, the adsorption behavior of several common gas molecules on SiB monolayers has been investigated using density functional theory (DFT). The study focuses on examining the most stable configurations, adsorption energies, charge transfer, and electronic properties of selected gas molecules on the SiB surface. The gas adsorption behavior on SiB monolayers has been considered for use in work function type gas sensors and conductometric sensor devices. The work function of the SiB layer is found to vary between 4.06% and 27% after exposure to the selected gas molecules, indicating its high sensitivity to these gases. The current–voltage (I–V) characteristics exhibit distinct responses for different gas adsorptions on the SiB surface, particularly for HCHO, CO, and CO2 gas molecules. Furthermore, the high sensitivity of SiB to gas adsorption open up possibilities for the improvement of gas sensing devices for monitoring and detecting harmful gases in various environments
{"title":"SiB Monolayers-Based Gas Sensor: Work Function and Conductometric Type Gas Sensors","authors":"Mahnaz Mohammadi, Esmaeil Pakizeh","doi":"10.1002/adts.202401127","DOIUrl":"https://doi.org/10.1002/adts.202401127","url":null,"abstract":"The air pollution and the rising emission of dangerous gases into the atmosphere are recently worrisome. In order to protect the humans and animals life's, it is crucial to monitor these harmful gases. Gases like HCHO, N<sub>2</sub>, NH<sub>3</sub>, CO<sub>2</sub>, CH<sub>4</sub>, CO, and SO<sub>2</sub> are dangerous for human health. As a result, gas sensors have been attracted significant interest as a means to effectively detect and adsorb these pollutants. In this study, the adsorption behavior of several common gas molecules on SiB monolayers has been investigated using density functional theory (DFT). The study focuses on examining the most stable configurations, adsorption energies, charge transfer, and electronic properties of selected gas molecules on the SiB surface. The gas adsorption behavior on SiB monolayers has been considered for use in work function type gas sensors and conductometric sensor devices. The work function of the SiB layer is found to vary between 4.06% and 27% after exposure to the selected gas molecules, indicating its high sensitivity to these gases. The current–voltage (<i>I</i>–<i>V</i>) characteristics exhibit distinct responses for different gas adsorptions on the SiB surface, particularly for HCHO, CO, and CO<sub>2</sub> gas molecules. Furthermore, the high sensitivity of SiB to gas adsorption open up possibilities for the improvement of gas sensing devices for monitoring and detecting harmful gases in various environments","PeriodicalId":7219,"journal":{"name":"Advanced Theory and Simulations","volume":"18 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2024-12-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142887236","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
This work explores the copolymerization of propylene and 1-decene using homogeneous metallocene catalysts to optimize polyolefin functionalization. A detailed mathematical model is developed with experimental validation employing the method of moments and probability generating functions to predict average molecular properties, the molecular weight distribution, the copolymer composition distribution, and the joint molecular weight distribution-copolymer composition distribution. To efficiently handle computational resources, the model code is parallelized. This comprehensive model allows for explaining in detail the copolymer's microstructure under various semibatch reactor conditions. Moreover, the model is a powerful tool for selecting reaction conditions to synthesize materials with desired properties.
{"title":"Predicting Polyolefin Microstructure: A Parallelized Multidimensional Model for Metallocene-Catalyzed Copolymerization of Propylene and 1-Decene","authors":"Franco Herrero, Adriana Brandolin, Claudia Sarmoria, Mariano Asteasuain","doi":"10.1002/adts.202401072","DOIUrl":"https://doi.org/10.1002/adts.202401072","url":null,"abstract":"This work explores the copolymerization of propylene and 1-decene using homogeneous metallocene catalysts to optimize polyolefin functionalization. A detailed mathematical model is developed with experimental validation employing the method of moments and probability generating functions to predict average molecular properties, the molecular weight distribution, the copolymer composition distribution, and the joint molecular weight distribution-copolymer composition distribution. To efficiently handle computational resources, the model code is parallelized. This comprehensive model allows for explaining in detail the copolymer's microstructure under various semibatch reactor conditions. Moreover, the model is a powerful tool for selecting reaction conditions to synthesize materials with desired properties.","PeriodicalId":7219,"journal":{"name":"Advanced Theory and Simulations","volume":"41 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2024-12-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142884770","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Stéphane B. Olou'ou Guifo, Jonathan E. Mueller, Torsten Markus
To investigate the influence of the local environment on Li-ion diffusivity in layered lithium nickel oxide (LixNiO2) cathodes, a bottom-up, multiscale-modeling approach is applied, utilizing density functional theory (DFT) with corrected Coulomb and van der Waals interactions to describe the energy-structure relationship of LixNiO2 (x = 0 – 1) in good agreement with previous experiments. The UNiversal CLuster Expansion (UNCLE) is employed to construct high-probability Li–vacancy configurations and the Nudged Elastic Band (NEB) method to compute energy barriers for representative Li diffusion mechanisms. By fitting a cluster expansion model to these barriers, diffusion barriers are determined for all possible Li–vacancy configurations within a nearest-neighbor approximation. Based on this description, Li-concentration-dependent diffusion coefficients are predicted for the entire Li-concentration range. For the LixNiO2 crystal lattice, the computed Li chemical diffusivities well lie within experimental ranges, namely 10 – 10 cm2 s−1, at room temperature with activation energies around 37.9 kJ mol−1. The maximum diffusivity of 4.23 × 10 cm2 s−1 is identified at x = 0.63. The new analytical, self-consistent approach here relies on configurational samplings of individual atomistic mechanisms and can be applied to investigate diffusion properties in further dilute and concentrated alloy systems more efficiently than common numerical procedures.
{"title":"Statistical, Bottom-Up Model for Chemical Diffusion Based on Atomic Vacancy Sublattice Configurations in Layered Lithium Nickel Oxide Cathode Materials","authors":"Stéphane B. Olou'ou Guifo, Jonathan E. Mueller, Torsten Markus","doi":"10.1002/adts.202400917","DOIUrl":"https://doi.org/10.1002/adts.202400917","url":null,"abstract":"To investigate the influence of the local environment on Li-ion diffusivity in layered lithium nickel oxide (Li<sub><i>x</i></sub>NiO<sub>2</sub>) cathodes, a bottom-up, multiscale-modeling approach is applied, utilizing density functional theory (DFT) with corrected Coulomb and van der Waals interactions to describe the energy-structure relationship of Li<sub><i>x</i></sub>NiO<sub>2</sub> (<i>x</i> = 0 – 1) in good agreement with previous experiments. The UNiversal CLuster Expansion (UNCLE) is employed to construct high-probability Li–vacancy configurations and the Nudged Elastic Band (NEB) method to compute energy barriers for representative Li diffusion mechanisms. By fitting a cluster expansion model to these barriers, diffusion barriers are determined for all possible Li–vacancy configurations within a nearest-neighbor approximation. Based on this description, Li-concentration-dependent diffusion coefficients are predicted for the entire Li-concentration range. For the Li<sub><i>x</i></sub>NiO<sub>2</sub> crystal lattice, the computed Li chemical diffusivities well lie within experimental ranges, namely 10 – 10 cm<sup>2</sup> s<sup>−1</sup>, at room temperature with activation energies around 37.9 kJ mol<sup>−1</sup>. The maximum diffusivity of 4.23 × 10 cm<sup>2</sup> s<sup>−1</sup> is identified at <i>x</i> = 0.63. The new analytical, self-consistent approach here relies on configurational samplings of individual atomistic mechanisms and can be applied to investigate diffusion properties in further dilute and concentrated alloy systems more efficiently than common numerical procedures.","PeriodicalId":7219,"journal":{"name":"Advanced Theory and Simulations","volume":"122 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2024-12-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142874383","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
MoS2/WS2 in-plane heterojunction is constructed using density functional theory (DFT), and its adsorption properties for different gas molecules (CO, CO2, NO2, H2S, SO2, and SO3) are analyzed. Results indicate that the heterojunction exhibits excellent selection toward S-series gas molecules (H2S, SO2, and SO3), particularly SO3. The adsorption energy is determined to be −3.67 eV. Then, the adsorption properties of the heterojunction are further improved by noble metal (Ag, Au, and Pt) modification. Noble metal atoms alter the surface potential energy of the heterojunction, resulting in stronger adsorption activity. For instance, the binding energies of noble metals in the Ag-MoS2/WS2, Au-MoS2/WS2, and Pt-MoS2/WS2 systems are −1.03, −1.04, and −2.76 eV, respectively. Additionally, there has been a significant alteration in their bandgaps. Notably, the bandgap of Pt-MoS2/WS2 has decreased to 1.42 eV (24.16%), which is the most pronounced change. Then, the charge density difference and density of states of noble metal-modified MoS2/WS2 heterojunction adsorbed SO3 are analyzed. The results demonstrate that the adsorption capacity of a noble metal-modified system for SO3 is enhanced. Finally, raising the temperature can accelerate gas molecule desorption from the system. Combining all calculation results, Ag-MoS2/WS2 in-plane heterojunction can be used as a candidate gas-sensitive material for detecting SO3 at room temperature (300 K). The Pt-MoS2/WS2 in-plane heterojunction is demonstrated to possess effective adsorbent properties for trapping SO3 gas molecules at room temperature. This provides a new idea and theoretical basis for gas sensor development.
{"title":"Enhanced Adsorption Properties of Noble Metal Modified MoS2/WS2 Heterojunctions","authors":"Kewei Gao, Haixia Chen, Jijun Ding, Mingya Yang, Haiwei Fu, Jianhong Peng","doi":"10.1002/adts.202400949","DOIUrl":"https://doi.org/10.1002/adts.202400949","url":null,"abstract":"MoS<sub>2</sub>/WS<sub>2</sub> in-plane heterojunction is constructed using density functional theory (DFT), and its adsorption properties for different gas molecules (CO, CO<sub>2</sub>, NO<sub>2</sub>, H<sub>2</sub>S, SO<sub>2</sub>, and SO<sub>3</sub>) are analyzed. Results indicate that the heterojunction exhibits excellent selection toward S-series gas molecules (H<sub>2</sub>S, SO<sub>2</sub>, and SO<sub>3</sub>), particularly SO<sub>3</sub>. The adsorption energy is determined to be −3.67 eV. Then, the adsorption properties of the heterojunction are further improved by noble metal (Ag, Au, and Pt) modification. Noble metal atoms alter the surface potential energy of the heterojunction, resulting in stronger adsorption activity. For instance, the binding energies of noble metals in the Ag-MoS<sub>2</sub>/WS<sub>2</sub>, Au-MoS<sub>2</sub>/WS<sub>2</sub>, and Pt-MoS<sub>2</sub>/WS<sub>2</sub> systems are −1.03, −1.04, and −2.76 eV, respectively. Additionally, there has been a significant alteration in their bandgaps. Notably, the bandgap of Pt-MoS<sub>2</sub>/WS<sub>2</sub> has decreased to 1.42 eV (24.16%), which is the most pronounced change. Then, the charge density difference and density of states of noble metal-modified MoS<sub>2</sub>/WS<sub>2</sub> heterojunction adsorbed SO<sub>3</sub> are analyzed. The results demonstrate that the adsorption capacity of a noble metal-modified system for SO<sub>3</sub> is enhanced. Finally, raising the temperature can accelerate gas molecule desorption from the system. Combining all calculation results, Ag-MoS<sub>2</sub>/WS<sub>2</sub> in-plane heterojunction can be used as a candidate gas-sensitive material for detecting SO<sub>3</sub> at room temperature (300 K). The Pt-MoS<sub>2</sub>/WS<sub>2</sub> in-plane heterojunction is demonstrated to possess effective adsorbent properties for trapping SO<sub>3</sub> gas molecules at room temperature. This provides a new idea and theoretical basis for gas sensor development.","PeriodicalId":7219,"journal":{"name":"Advanced Theory and Simulations","volume":"52 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142857553","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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