Pub Date : 2025-02-24DOI: 10.1016/j.commatsci.2025.113772
Ziyi Chen , Yang Yuan , Sihan Liang , Meng Wan , Kai Li , Weiqi Zhou , Yangang Wang , Zongguo Wang
With the rapid development of information technology, there has been an exponential increase in material data. However, challenges such as inconsistencies in data formats and non-standardized storage methods have emerged as primary obstacles for researchers seeking to harness materials science data effectively. To fully exploit material data from diverse sources and achieve the efficient fusion of historical data, this paper introduces a database application framework designed for the automatic collection and analysis of multi-source heterogeneous material data, and two first principles calculations datasets are established. Standardized methods used in this work enable the automatic extraction, storage and analysis of both discrete and database data while also offering an interface for data-driven scientific research. Moreover, this framework used for dataset construction can be deployed in both cloud-based virtual environments and local servers, providing flexibility that not only facilitates data sharing but also ensures data privacy and customized control. The datasets and framework developed in this work offer a robust data foundation and potent tool for researchers engaged in data-driven research.
{"title":"An automatic scientific data collection framework for materials science","authors":"Ziyi Chen , Yang Yuan , Sihan Liang , Meng Wan , Kai Li , Weiqi Zhou , Yangang Wang , Zongguo Wang","doi":"10.1016/j.commatsci.2025.113772","DOIUrl":"10.1016/j.commatsci.2025.113772","url":null,"abstract":"<div><div>With the rapid development of information technology, there has been an exponential increase in material data. However, challenges such as inconsistencies in data formats and non-standardized storage methods have emerged as primary obstacles for researchers seeking to harness materials science data effectively. To fully exploit material data from diverse sources and achieve the efficient fusion of historical data, this paper introduces a database application framework designed for the automatic collection and analysis of multi-source heterogeneous material data, and two first principles calculations datasets are established. Standardized methods used in this work enable the automatic extraction, storage and analysis of both discrete and database data while also offering an interface for data-driven scientific research. Moreover, this framework used for dataset construction can be deployed in both cloud-based virtual environments and local servers, providing flexibility that not only facilitates data sharing but also ensures data privacy and customized control. The datasets and framework developed in this work offer a robust data foundation and potent tool for researchers engaged in data-driven research.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"252 ","pages":"Article 113772"},"PeriodicalIF":3.1,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143474737","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-23DOI: 10.1016/j.commatsci.2025.113775
Can Leng , Xuguang Chen , Jie Liu , Chunye Gong , Bo Yang , Zhuo Tang , Wangdong Yang , Wei-Qing Huang , Yi-Ge Zhou , Mengxia Mo , Kenli Li , Keqin Li
The integration of high-performance computing with machine learning (ML) has established a transformative scientific paradigm that significantly enhances the efficiency of material discovery, particularly in the search for catalysts in alternative energy research. However, significant challenges remain in the utilization of available computational resources to accelerate the screening of catalyst materials. In this study, we implement a high-throughput framework on the new-generation Tianhe supercomputer, featuring the development of a Ping-Fault Recovery algorithm, single-task optimization for Density Functional Theory (DFT) to maximize efficiency, and enhanced task scheduling using a two-level scheduling strategy to ensure efficient utilization of the abundant computational resources of the supercomputer. This framework facilitates the identification of 2,028 candidate surfaces across 868 intermetallics from 2,713,897 unique adsorption sites, achieving a screening speed 193 times faster than traditional methods. Alloys composed of Mo, Nb, and V are used as case studies to provide a detailed elucidation of the process of identifying the most effective catalytic surfaces. The framework achieved the best single-day candidate hit performance on 18,106 nodes, completing in one day what previously took a year. This supercomputer-based framework optimizes the use of computational resources, driving innovation in catalyst material discovery.
{"title":"Fully automated high-throughput computer-based catalytic material screening framework and its application on the new-generation Tianhe supercomputer","authors":"Can Leng , Xuguang Chen , Jie Liu , Chunye Gong , Bo Yang , Zhuo Tang , Wangdong Yang , Wei-Qing Huang , Yi-Ge Zhou , Mengxia Mo , Kenli Li , Keqin Li","doi":"10.1016/j.commatsci.2025.113775","DOIUrl":"10.1016/j.commatsci.2025.113775","url":null,"abstract":"<div><div>The integration of high-performance computing with machine learning (ML) has established a transformative scientific paradigm that significantly enhances the efficiency of material discovery, particularly in the search for catalysts in alternative energy research. However, significant challenges remain in the utilization of available computational resources to accelerate the screening of catalyst materials. In this study, we implement a high-throughput framework on the new-generation Tianhe supercomputer, featuring the development of a Ping-Fault Recovery algorithm, single-task optimization for Density Functional Theory (DFT) to maximize efficiency, and enhanced task scheduling using a two-level scheduling strategy to ensure efficient utilization of the abundant computational resources of the supercomputer. This framework facilitates the identification of 2,028 candidate surfaces across 868 intermetallics from 2,713,897 unique adsorption sites, achieving a screening speed 193 times faster than traditional methods. Alloys composed of Mo, Nb, and V are used as case studies to provide a detailed elucidation of the process of identifying the most effective catalytic surfaces. The framework achieved the best single-day candidate hit performance on 18,106 nodes, completing in one day what previously took a year. This supercomputer-based framework optimizes the use of computational resources, driving innovation in catalyst material discovery.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"252 ","pages":"Article 113775"},"PeriodicalIF":3.1,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471482","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-22DOI: 10.1016/j.commatsci.2025.113780
Christina Schenk, Maciej Haranczyk
Efficient exploration of multicomponent material composition spaces is often limited by time and financial constraints, particularly when mixture and synthesis constraints exist. Traditional methods like Latin hypercube sampling (LHS) struggle with constrained problems especially in high dimensions, while emerging approaches like Bayesian optimization (BO) face challenges in early-stage exploration. This article introduces ConstrAined Sequential laTin hypeRcube sampling methOd (CASTRO), an open-source tool designed to address these challenges. CASTRO is optimized for uniform sampling in constrained small- to moderate-dimensional spaces, with scalability to higher dimensions through future adaptations. CASTRO uses a divide-and-conquer strategy to decompose problems into parallel subproblems, improving efficiency and scalability. It effectively handles equality-mixture constraints, ensuring comprehensive design space coverage and leveraging LHS and LHS with multidimensional uniformity (LHSMDU). It also integrates prior experimental knowledge, making it well-suited for efficient exploration within limited budgets. Validation through two material design case studies, a four-dimensional problem with near-uniform distributions and a nine-dimensional problem with additional synthesis constraints, demonstrates CASTRO’s effectiveness in exploring constrained design spaces for materials science, pharmaceuticals and chemicals. The software and case studies are available on GitHub.
{"title":"A novel constrained sampling method for efficient exploration in materials and chemical mixture design","authors":"Christina Schenk, Maciej Haranczyk","doi":"10.1016/j.commatsci.2025.113780","DOIUrl":"10.1016/j.commatsci.2025.113780","url":null,"abstract":"<div><div>Efficient exploration of multicomponent material composition spaces is often limited by time and financial constraints, particularly when mixture and synthesis constraints exist. Traditional methods like Latin hypercube sampling (LHS) struggle with constrained problems especially in high dimensions, while emerging approaches like Bayesian optimization (BO) face challenges in early-stage exploration. This article introduces ConstrAined Sequential laTin hypeRcube sampling methOd (CASTRO), an open-source tool designed to address these challenges. CASTRO is optimized for uniform sampling in constrained small- to moderate-dimensional spaces, with scalability to higher dimensions through future adaptations. CASTRO uses a divide-and-conquer strategy to decompose problems into parallel subproblems, improving efficiency and scalability. It effectively handles equality-mixture constraints, ensuring comprehensive design space coverage and leveraging LHS and LHS with multidimensional uniformity (LHSMDU). It also integrates prior experimental knowledge, making it well-suited for efficient exploration within limited budgets. Validation through two material design case studies, a four-dimensional problem with near-uniform distributions and a nine-dimensional problem with additional synthesis constraints, demonstrates CASTRO’s effectiveness in exploring constrained design spaces for materials science, pharmaceuticals and chemicals. The software and case studies are available on GitHub.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"252 ","pages":"Article 113780"},"PeriodicalIF":3.1,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463870","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-22DOI: 10.1016/j.commatsci.2025.113784
A. Sakthi Balaji, Akash Ramasamy, K. Janani Sivasankar, Hariharan Rajalakshmi Mohanraj, D. John Thiruvadigal
Motivated by the exceptional thermoelectric performance of 2D buckled GeTe and Sb monolayers, thermoelectric transport characteristics of the stable GeTe/Antimonene (Sb) van der Waals heterostructure (vdWH) are examined by first-principles calculations supplemented by the non-equilibrium Green’s function approach (NEGF). The electronic aspects of these thermoelectric devices are assessed by reviewing the Seebeck coefficient (S) and electrical conductance (Ge) derived from transmission spectra. Simultaneously, the thermal conductance (κph) of the system was computed by analysing the lattice/phonon transmission spectrum. The thermoelectric figure of merit (ZT) for the system is calculated by integrating the electron and phonon transmission spectra across various chemical potentials (μ) and temperatures (T). In this context, the heterostructure featuring a smaller interlayer vdw gap and reduced phonon thermal conductance ultimately exhibits superior thermoelectric performance. The effective phonon scattering at the interface establishes reduced phonon thermal conductance at the heterostructure. At 300 K, low phonon thermal conductance attains 43.23 pW/K and the highest ZT attains 6.97 for heterostructure. Our theoretical research provides an innovative technique and offers valuable theoretical insights into the thermoelectric transport properties of vdW heterostructures device.
{"title":"Low lattice thermal conductance of buckled GeTe/antimonene vdW interface device: A DFT + NEGF study","authors":"A. Sakthi Balaji, Akash Ramasamy, K. Janani Sivasankar, Hariharan Rajalakshmi Mohanraj, D. John Thiruvadigal","doi":"10.1016/j.commatsci.2025.113784","DOIUrl":"10.1016/j.commatsci.2025.113784","url":null,"abstract":"<div><div>Motivated by the exceptional thermoelectric performance of 2D buckled GeTe and Sb monolayers, thermoelectric transport characteristics of the stable GeTe/Antimonene (Sb) van der Waals heterostructure (vdWH) are examined by first-principles calculations supplemented by the non-equilibrium Green’s function approach (NEGF). The electronic aspects of these thermoelectric devices are assessed by reviewing the Seebeck coefficient (S) and electrical conductance (G<sub>e</sub>) derived from transmission spectra. Simultaneously, the thermal conductance (κ<sub>ph</sub>) of the system was computed by analysing the lattice/phonon transmission spectrum. The thermoelectric figure of merit (ZT) for the system is calculated by integrating the electron and phonon transmission spectra across various chemical potentials (μ) and temperatures (T). In this context, the heterostructure featuring a smaller interlayer vdw gap and reduced phonon thermal conductance ultimately exhibits superior thermoelectric performance. The effective phonon scattering at the interface establishes reduced phonon thermal conductance at the heterostructure. At 300 K, low phonon thermal conductance attains 43.23 pW/K and the highest ZT attains 6.97 for heterostructure. Our theoretical research provides an innovative technique and offers valuable theoretical insights into the thermoelectric transport properties of vdW heterostructures device.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"252 ","pages":"Article 113784"},"PeriodicalIF":3.1,"publicationDate":"2025-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143471483","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-21DOI: 10.1016/j.commatsci.2025.113774
Waleed Ftahi , Nusaibah AL-Shaeri , Yuanwei Yang , Sara Ahmed A. , Yongliang Tang , Qingxiang Liu , Yuxiang Ni
ZnO nanostructures have garnered significant attention from researchers and industries due to their outstanding properties as gas-sensing materials. Aluminium (Al) doping, in particular, can further fine-tune or optimize these gas-sensing properties. In this research, we investigate the adsorption of O2 molecules on undoped and Al-doped ZnO nanowires at and doping concentrations using advanced reactive force field (ReaxFF)-based molecular dynamics (MD) simulations. The adsorption process is studied at temperatures of 100 K, 300 K, and 500 K, with 300 O2 molecules in each case, and the influences of these factors on the adsorption type are analyzed through radial distribution function (RDF) analysis. The adsorption behavior of O2 molecules on both undoped and Al-doped ZnO nanowires is compared by calculating system energy, adsorption energy, and the number of adsorbed molecules. The results show that the binding distances between O2 molecules and Zn and Al atoms on the nanowire surfaces are 2.18 Å and 1.78 Å, respectively, as determined from RDF analysis. The O2 adsorption process on undoped and Al-doped ZnO nanowire surfaces occurs in two distinct stages, with higher temperatures leading to an increased number of adsorbed molecules. As Al doping increases, it significantly accelerates O2 adsorption in the initial stage, while pure ZnO shows greater adsorption number in the second stage. Chemisorption dominates the interaction in both undoped and Al-doped ZnO.
{"title":"Investigating the temperature and Al doping effect on the O2 adsorption Process on ZnO nanowire surface: A ReaxFF-MD approach","authors":"Waleed Ftahi , Nusaibah AL-Shaeri , Yuanwei Yang , Sara Ahmed A. , Yongliang Tang , Qingxiang Liu , Yuxiang Ni","doi":"10.1016/j.commatsci.2025.113774","DOIUrl":"10.1016/j.commatsci.2025.113774","url":null,"abstract":"<div><div>ZnO nanostructures have garnered significant attention from researchers and industries due to their outstanding properties as gas-sensing materials. Aluminium (Al) doping, in particular, can further fine-tune or optimize these gas-sensing properties. In this research, we investigate the adsorption of O<sub>2</sub> molecules on undoped and Al-doped ZnO nanowires at <span><math><mrow><mn>5</mn><mtext>%</mtext></mrow></math></span> and <span><math><mrow><mn>10</mn><mtext>%</mtext></mrow></math></span> doping concentrations using advanced reactive force field (ReaxFF)-based molecular dynamics (MD) simulations. The adsorption process is studied at temperatures of 100 K, 300 K, and 500 K, with 300 O<sub>2</sub> molecules in each case, and the influences of these factors on the adsorption type are analyzed through radial distribution function (RDF) analysis. The adsorption behavior of O<sub>2</sub> molecules on both undoped and Al-doped ZnO nanowires is compared by calculating system energy, adsorption energy, and the number of adsorbed molecules. The results show that the binding distances between O<sub>2</sub> molecules and Zn and Al atoms on the nanowire surfaces are 2.18 Å and 1.78 Å, respectively, as determined from RDF analysis. The O<sub>2</sub> adsorption process on undoped and Al-doped ZnO nanowire surfaces occurs in two distinct stages, with higher temperatures leading to an increased number of adsorbed molecules. As Al doping increases, it significantly accelerates O<sub>2</sub> adsorption in the initial stage, while pure ZnO shows greater adsorption number in the second stage. Chemisorption dominates the interaction in both undoped and Al-doped ZnO.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"252 ","pages":"Article 113774"},"PeriodicalIF":3.1,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463868","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-21DOI: 10.1016/j.commatsci.2025.113794
Kuanshu Jiang , Jiangtao Wang , Jiangkai Yuan , Quan Wang
Due to the limitations of graphene processing technology, the as-prepared graphene will inevitably have various defects, which will have remarkable effects on the macroscopic properties of graphene. In this work, graphene resonators based on vacancy defects are investigated. The resonance properties of graphene are demonstrated by molecular dynamics simulations, in which the effects of single and double vacancy defects at different positions and numbers on the resonant frequencies of graphene nanoribbons are unveiled. The results show that the C atoms at the vacancy defect have a much larger movement in the normal direction than in the region of C atoms bound by a complete C–C bond. The resonant frequency is not affected by the location of vacancy defects. As the number of vacancy defects increases, the resonance amplitude value increases monotonically in the normal direction. However, there is no significant difference in the resonance amplitude value when comparing single and double vacancy defects. The resonant frequency decreases monotonically with the increase in the number of vacancy defects, while for the same number of vacancy defects, the resonant frequency is generally smaller for double vacancy defects than for single vacancy defects. The resonant frequency is not sensitive to individual single and double vacancy defects rather than is more affected by a large concentration of vacancy defects, suggesting that extra attention needs to be given to the case of large concentration defects. Our achievement will lay a strong foundation for graphene resonators’ design and performance optimization.
{"title":"Investigating vacancy-defect effects on the vibration characteristics of graphene resonators with molecular dynamics simulation","authors":"Kuanshu Jiang , Jiangtao Wang , Jiangkai Yuan , Quan Wang","doi":"10.1016/j.commatsci.2025.113794","DOIUrl":"10.1016/j.commatsci.2025.113794","url":null,"abstract":"<div><div>Due to the limitations of graphene processing technology, the as-prepared graphene will inevitably have various defects, which will have remarkable effects on the macroscopic properties of graphene. In this work, graphene resonators based on vacancy defects are investigated. The resonance properties of graphene are demonstrated by molecular dynamics simulations, in which the effects of single and double vacancy defects at different positions and numbers on the resonant frequencies of graphene nanoribbons are unveiled. The results show that the C atoms at the vacancy defect have a much larger movement in the normal direction than in the region of C atoms bound by a complete C–C bond. The resonant frequency is not affected by the location of vacancy defects. As the number of vacancy defects increases, the resonance amplitude value increases monotonically in the normal direction. However, there is no significant difference in the resonance amplitude value when comparing single and double vacancy defects. The resonant frequency decreases monotonically with the increase in the number of vacancy defects, while for the same number of vacancy defects, the resonant frequency is generally smaller for double vacancy defects than for single vacancy defects. The resonant frequency is not sensitive to individual single and double vacancy defects rather than is more affected by a large concentration of vacancy defects, suggesting that extra attention needs to be given to the case of large concentration defects. Our achievement will lay a strong foundation for graphene resonators’ design and performance optimization.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"252 ","pages":"Article 113794"},"PeriodicalIF":3.1,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143464019","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-21DOI: 10.1016/j.commatsci.2025.113756
Fiyanshu Kaka, Kalyan Sundar Krishna Chivukula
Addressing the limitations of traditional Li-ion batteries, this study focuses on the crucial transition to All-Solid-State Batteries (ASSBs) by emphasizing the paramount importance of solid electrolyte morphology on battery performance. Utilizing a computational phase-field approach, the study simulates binary solid-electrolyte morphologies and integrates them into ASSBs through a robust process to assess their impact on electrochemical characteristics. The intricate process of transitioning from simulated morphology to Computer-Aided Design geometry is thoroughly explored in the manuscript. Furthermore, upon the successful incorporation of solid-electrolyte morphology, simulations are performed at a constant discharge current density of 5 A.m−2, revealing a significant order of magnitude difference in the discharging times for ASSBs with varying volume fractions, underscoring the pivotal role of solid-electrolyte’s morphology. Additionally, mechanical strength is evaluated across volume fractions ranging from 0.3 to 0.7, showcasing a substantial threefold enhancement under a compressive stress of 10 MPa. Guided by mechano-electrochemical characteristics, an optimal blend ratio for the solid-electrolyte is identified. These findings underscore the crucial role of tailoring solid-electrolyte morphology for optimal ASSB performance, providing valuable guidance for advancing high-performance, safe, and sustainable battery technologies.
{"title":"Combined diffuse and sharp interface approach to unravel morphological dynamics in solid-state Li-ion batteries","authors":"Fiyanshu Kaka, Kalyan Sundar Krishna Chivukula","doi":"10.1016/j.commatsci.2025.113756","DOIUrl":"10.1016/j.commatsci.2025.113756","url":null,"abstract":"<div><div>Addressing the limitations of traditional Li-ion batteries, this study focuses on the crucial transition to All-Solid-State Batteries (ASSBs) by emphasizing the paramount importance of solid electrolyte morphology on battery performance. Utilizing a computational phase-field approach, the study simulates binary solid-electrolyte morphologies and integrates them into ASSBs through a robust process to assess their impact on electrochemical characteristics. The intricate process of transitioning from simulated morphology to Computer-Aided Design geometry is thoroughly explored in the manuscript. Furthermore, upon the successful incorporation of solid-electrolyte morphology, simulations are performed at a constant discharge current density of 5 A.m<sup>−2</sup>, revealing a significant order of magnitude difference in the discharging times for ASSBs with varying volume fractions, underscoring the pivotal role of solid-electrolyte’s morphology. Additionally, mechanical strength is evaluated across volume fractions ranging from 0.3 to 0.7, showcasing a substantial threefold enhancement under a compressive stress of 10 MPa. Guided by mechano-electrochemical characteristics, an optimal blend ratio for the solid-electrolyte is identified. These findings underscore the crucial role of tailoring solid-electrolyte morphology for optimal ASSB performance, providing valuable guidance for advancing high-performance, safe, and sustainable battery technologies.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"252 ","pages":"Article 113756"},"PeriodicalIF":3.1,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463869","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-21DOI: 10.1016/j.commatsci.2025.113791
Fernando A. Soto
This study sheds light on the surface dynamics of a MgTFSI-Cl/DME-based electrolyte solution and a pristine Mg(0001) surface, employing density functional theory (DFT) simulations to characterize the surface area and isosurface of magnesium under varying temperature and salt concentration conditions. A primary focus is understanding how these surface dynamics and factors help us understand the precursor mechanisms and structures leading to dendrite formation in magnesium batteries. The simulations reveal that the combination of high salt concentration and temperature leads to excessive surface areas, deviating from the ideal ‘Goldilocks morphology’, and can cause the isosurface to shift away from the anode’s surface. This displacement can create a concentration gradient conducive to Mg clustering, a precursor to dendrite formation. The simulations provide critical insights into the complex interplay between surface area, isosurface characteristics, and the operational parameters of magnesium anodes. The results underscore the importance of optimizing these factors to mitigate dendrite formation, offering valuable guidance for developing more efficient and safer magnesium-ion batteries (MiBs). This study enhances our understanding of the fundamental processes governing dendrite formation and proposes a novel approach to addressing one of the key challenges in advancing magnesium battery technology.
{"title":"Computational insights into surface dynamics, Mg clustering, and dendrite formation in magnesium batteries","authors":"Fernando A. Soto","doi":"10.1016/j.commatsci.2025.113791","DOIUrl":"10.1016/j.commatsci.2025.113791","url":null,"abstract":"<div><div>This study sheds light on the surface dynamics of a MgTFSI-Cl/DME-based electrolyte solution and a pristine Mg(0001) surface, employing density functional theory (DFT) simulations to characterize the surface area and isosurface of magnesium under varying temperature and salt concentration conditions. A primary focus is understanding how these surface dynamics and factors help us understand the precursor mechanisms and structures leading to dendrite formation in magnesium batteries. The simulations reveal that the combination of high salt concentration and temperature leads to excessive surface areas, deviating from the ideal ‘Goldilocks morphology’, and can cause the isosurface to shift away from the anode’s surface. This displacement can create a concentration gradient conducive to Mg clustering, a precursor to dendrite formation. The simulations provide critical insights into the complex interplay between surface area, isosurface characteristics, and the operational parameters of magnesium anodes. The results underscore the importance of optimizing these factors to mitigate dendrite formation, offering valuable guidance for developing more efficient and safer magnesium-ion batteries (MiBs). This study enhances our understanding of the fundamental processes governing dendrite formation and proposes a novel approach to addressing one of the key challenges in advancing magnesium battery technology.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"252 ","pages":"Article 113791"},"PeriodicalIF":3.1,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143463871","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-20DOI: 10.1016/j.commatsci.2025.113717
Huaijun Sun , Chao Zhang , Jianbo Huang , Xingdu Fan , Weiyi Xia , Ling Tang , Renhai Wang , Kunpeng Cui , Cai-Zhuang Wang
By substitution of rare-earth (R) elements for La and other group 14 elements (X) for Si in the eight most stable La-Si-P ternary phases obtained previously, the stability of the R-X-P ternary compounds are investigated. We show that the formation energies of many such ternary phases are lowered after the substitution, and some stable ternary phases are obtained under the new convex hulls constructed including the newly predicted low-energy phases. Phonon spectra calculations demonstrate the dynamical stability for these lanthanides containing ternary compounds. The Gibbs formation energies as the function of temperature also demonstrate thermodynamic stability for most of the new phases with respect to the nearby competitive crystal phases in the convex hull. The electronic band structures of these ternary phases show metallic properties and indicate spin polarization for the R5XP3 phases. The discoveries of these ternary phases enrich the existing phase diagrams of lanthanide-containing ternary compounds.
{"title":"Prediction of lanthanide-containing ternary compounds","authors":"Huaijun Sun , Chao Zhang , Jianbo Huang , Xingdu Fan , Weiyi Xia , Ling Tang , Renhai Wang , Kunpeng Cui , Cai-Zhuang Wang","doi":"10.1016/j.commatsci.2025.113717","DOIUrl":"10.1016/j.commatsci.2025.113717","url":null,"abstract":"<div><div>By substitution of rare-earth (R) elements for La and other group 14 elements (X) for Si in the eight most stable La-Si-P ternary phases obtained previously, the stability of the R-X-P ternary compounds are investigated. We show that the formation energies of many such ternary phases are lowered after the substitution, and some stable ternary phases are obtained under the new convex hulls constructed including the newly predicted low-energy phases. Phonon spectra calculations demonstrate the dynamical stability for these lanthanides containing ternary compounds. The Gibbs formation energies as the function of temperature also demonstrate thermodynamic stability for most of the new phases with respect to the nearby competitive crystal phases in the convex hull. The electronic band structures of these ternary phases show metallic properties and indicate spin polarization for the R<sub>5</sub>XP<sub>3</sub> phases. The discoveries of these ternary phases enrich the existing phase diagrams of lanthanide-containing ternary compounds.</div></div>","PeriodicalId":10650,"journal":{"name":"Computational Materials Science","volume":"251 ","pages":"Article 113717"},"PeriodicalIF":3.1,"publicationDate":"2025-02-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143444356","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-02-20DOI: 10.1016/j.commatsci.2025.113781
Ryan D. Kerr , Mark R. Gilbert , Samuel T. Murphy
Tungsten is one of the materials of choice for several commercial fusion power plant designs, in particular, for divertor targets and the first wall. In maintenance conditions or during a loss of coolant accident, tungsten is expected to reach temperatures at which it readily volatilises as tungsten trioxide, potentially distributing radioactive material and posing a hazard to personnel. The oxidation of tungsten is reported to show an orientation dependence, however, the mechanism by which it occurs is not fully understood, providing an obstacle to the development of tungsten smart alloys that display reduced oxidation. Using DFT+ simulations, it is shown how key features of the electronic structure of the tungsten–oxygen system change as the tungsten–oxygen ratio evolves. Formation and migration barriers for oxygen in the different tungsten oxides are determined, allowing an assessment of its mobility in the phases observed during the oxidation process. Our results provide a new level of understanding of the sub-stoichiometric Magnéli phases that are observed during the oxidation of tungsten, which are perceived to be composed of WO2- and WO3-like regions.
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