Chemical Physics最新文献

{"title":"Theoretical Systematic investigation as a Strategic Tool for the design of more efficient pure and doped MoS2 catalysts for CO2 Electroreduction","authors":"Viviane S. Vaiss,&nbsp;Luciano T. Costa","doi":"10.1016/j.chemphys.2024.112597","DOIUrl":"10.1016/j.chemphys.2024.112597","url":null,"abstract":"<div><div>The development of efficient technologies that allow the use of CO<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> as a raw material for the synthesis of high value-added products is extremely important. Electrochemical methods are being considered promising. To assist in the planning of more efficient electrocatalysts, this work investigated, through DFT calculations, the structure and properties of pure MoS<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> and doped with various elements. The results obtained indicate that doping with Nb or Ti elements provides a greater reduction in the work function of MoS<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>. The lower the material’s work function, the higher the reaction current density and the better the material’s performance as an electrocatalyst. Furthermore, the formation energies of the COOH<span><math><msup><mrow></mrow><mrow><mo>∗</mo></mrow></msup></math></span> and CHO<span><math><msup><mrow></mrow><mrow><mo>∗</mo></mrow></msup></math></span> intermediates in MoS<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> doped with Nb or Ti are more stable than those of the CO<span><math><msup><mrow></mrow><mrow><mo>∗</mo></mrow></msup></math></span> intermediate. The high stability of the binding energy of the CO* intermediate in relation to other intermediates represents a limitation for the catalytic efficiency.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"591 ","pages":"Article 112597"},"PeriodicalIF":2.0,"publicationDate":"2025-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143164858","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}

{"title":"Molecular Insight into hydrogen storage of H2 + CH4 sII hydrates","authors":"Yiwei Feng ,&nbsp;Yujie Yan ,&nbsp;Hai Xie ,&nbsp;Jinxiang Liu","doi":"10.1016/j.chemphys.2025.112604","DOIUrl":"10.1016/j.chemphys.2025.112604","url":null,"abstract":"<div><div>We performed first-principles calculations and simulations to investigate the hydrogen storage properties of binary hydrates formed by H₂ and CH₄. The results showed that the optimum hydrogen storage capacity ranged from 3.43 wt% to 5.42 wt%, and the high storage capacity could be achieved by tuning cage occupation of CH₄ in 5¹² or 5¹²6⁴ cages. Further, two binary hydrate structures (denoted as <strong>T</strong>1 and <strong>T</strong>2) were chosen to assess the effect of pressure and temperature on the hydrate stability. Simulation results showed that two hydrates were stable at the studied conditions (10–30 MPa, and 260–285 K). At high pressures (more than 20 MPa) <strong>T</strong>1 structure was stable, while at low pressures <strong>T</strong>2 structure was stable. More importantly, H₂ + CH₄ binary hydrates exhibit anomalous stability at about 275 K, which would be helpful for the application of hydrate-based hydrogen storage technology under mild conditions.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"591 ","pages":"Article 112604"},"PeriodicalIF":2.0,"publicationDate":"2025-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143164922","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}

{"title":"Preparation of core–shell structured Cu2O@NH2-MIL-125(Ti) MOF and efficient photocatalytic degradation of methylene blue","authors":"Sakeerali C K ,&nbsp;Sung Min Heo ,&nbsp;Chang Woo Kim","doi":"10.1016/j.chemphys.2025.112602","DOIUrl":"10.1016/j.chemphys.2025.112602","url":null,"abstract":"<div><div>Cu₂O has garnered increased interest due to its ideal band gap and excellent carrier separation efficiency for photo catalysis; nonetheless, charge recombination still causes instability in practical usage. Here we design and fabricate Truncated cube Cu₂O(T C)@NH₂-MIL-125(Ti) core–shell. The main bonds formed between NH₂-MIL-125(Ti) and T C are through the <img>N<img>Cu<img>N<img>, <img>N<img>O<img>Cu<img> bond and the Cu<img>O surface interaction in addition formed. The Truncated cube shape of Cu₂O as a core and NH₂-MIL-125(Ti) shell with limited recombination is seldom researched. The rate constant (K) for the photocatalytic methylene blue degradation of Cu₂O(T C)@NH₂-MIL-125(Ti) was 0.0182 min⁻¹, 3.35 times higher than that of pure TC. The closely spaced band structures and close contact surfaces between T C and NH₂-MIL-125(Ti) should be the origin of the core–shell’s increased photocatalytic activity, as they facilitate the efficient transfer and separation of the photo-generated charge carriers. Cu²⁺ proportion to Cu¹⁺ after core–shell preparation is 45.66 %, which causes more oxygen vacancy and charge imbalances, increasing reactant adsorption and light absorption in the visible spectrum. The stability test towards MB employing T C@NH_2-MIL-125(Ti) core–shell and the photocatalytic scavenger test have also been studied. Moreover, a Type-II heterojunction was produced by photo-generated electron transfer from T C to NH₂-MIL-125(Ti). Such a heterostructure sheds light on Cu₂O-related core–shell materials’ exceptionally effective recombination suppression and improved photocatalytic effectiveness.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"591 ","pages":"Article 112602"},"PeriodicalIF":2.0,"publicationDate":"2025-01-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143164937","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}

{"title":"Exploring modeling techniques for predicting band gaps of Doped-ZnO: A Machine learning approach","authors":"Hajar Lamouadene ,&nbsp;Majid EL Kassaoui ,&nbsp;Mourad El Yadari ,&nbsp;Abdallah El Kenz ,&nbsp;Abdelilah Benyoussef","doi":"10.1016/j.chemphys.2025.112603","DOIUrl":"10.1016/j.chemphys.2025.112603","url":null,"abstract":"<div><div>Machine learning, as one of the promising alternatives for solving complex challenges, has recently received considerable attention. In this study, we apply several well-established machine-learning models for predicting the energy band gap of doped-ZnO as well as novel doping concentrations. This approach significantly expands the possibilities for designing functional materials, offering innovative solutions to meet current energy needs. The results show that the Gaussian Process Regression (GPR) model achieved outstanding performance, with a correlation coefficient (CC) of 98.97%, a root mean square error (RMSE) of 0.0022, and a mean absolute error (MAE) of 0.0020. Comparatively, the Support Vector Machine (SVM) model recorded a CC of 83.70%, an RMSE of 0.0052, and an MAE of 0.0048, while the Random Forest model exhibited a CC of 76.40%, an RMSE of 0.0086, and an MAE of 0.0083. These results underscore the exceptional effectiveness of the GPR model in predicting material properties, while also highlighting the significant contributions of the SVM and Random Forest (RF) methods. This study opens up new research avenues in the fields of materials science and catalysis by exploring the predictive capabilities of different machine learning models for designing functional materials. We emphasize that the selection of the appropriate modeling method is critical for accurately predicting material properties. These results pave the way for future investigations aimed at refining and further comparing the performances of different modeling methods to optimize photocatalytic materials and address the challenges of clean energy.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"591 ","pages":"Article 112603"},"PeriodicalIF":2.0,"publicationDate":"2025-01-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143164859","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}

{"title":"Computational study of the lattice type, band structure, and thermoelectric properties of LiSbX2 (X = S, Se, Te)","authors":"Muhammad Hamid ,&nbsp;Muhammad Faizan ,&nbsp;Tahani A. Alrebdi ,&nbsp;Kausar Shaheen ,&nbsp;Shah Haidar Khan","doi":"10.1016/j.chemphys.2025.112600","DOIUrl":"10.1016/j.chemphys.2025.112600","url":null,"abstract":"<div><div>Chalcogenide materials have garnered significant attention for their excellent performance in optoelectronic and thermoelectric applications. This study explores the band structure and thermoelectric properties of ternary chalcogenides LiSbX₂ (X = S, Se. Te) using density functional theory (DFT). Our analysis reveals that these compounds exhibit negative formation energies and positive phonon frequencies, indicating their stability and a possible easy synthesis. The band structure calculations show that LiSbX₂ (X = S, Se, Te) are indirect bandgap semiconductors with a band gap of 0.96 (LiSbS₂), 0.52 (LiSbSe₂), and 0.13 eV (LiSbTe₂). Notably, these materials exhibit a high Seebeck coefficient, low electronic thermal conductivity, and high electronic conductivity. The maximum figure of merit is 0.61, 0.57, and 0.31 for LiSbS₂, LiSbSe₂, and LiSbTe₂, respectively, at 1000 K. These findings highlight the suitability of these compounds for future thermoelectric applications.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"591 ","pages":"Article 112600"},"PeriodicalIF":2.0,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143164860","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}

{"title":"The charge and spin density of five LaBO3 perovskites (B=Sc, Ti, V, Cr and Co). A Mulliken analysis","authors":"Khaled E. El-Kelany ,&nbsp;Alexander Platonenko ,&nbsp;Julio Sambrano ,&nbsp;Klaus Doll ,&nbsp;Roberto Dovesi","doi":"10.1016/j.chemphys.2024.112594","DOIUrl":"10.1016/j.chemphys.2024.112594","url":null,"abstract":"&lt;div&gt;&lt;div&gt;The charge and spin density distributions of five LaBO&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;3&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt; perovskites (B = Sc, Ti, V, Cr, and Co) have been investigated through the Mulliken population analysis, which yields crucial insights into the net atomic charges Q, magnetic moments &lt;span&gt;&lt;math&gt;&lt;mi&gt;μ&lt;/mi&gt;&lt;/math&gt;&lt;/span&gt;, and bond populations BP. The occupancy of the d shell and of the individual d orbitals of the transition metals B are also discussed. Large differences are observed with respect to the fully ionic representation (or &lt;em&gt;oxidation state&lt;/em&gt;), La&lt;span&gt;&lt;math&gt;&lt;msup&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mo&gt;+&lt;/mo&gt;&lt;mn&gt;3&lt;/mn&gt;&lt;/mrow&gt;&lt;/msup&gt;&lt;/math&gt;&lt;/span&gt;, B&lt;span&gt;&lt;math&gt;&lt;msup&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mo&gt;+&lt;/mo&gt;&lt;mn&gt;3&lt;/mn&gt;&lt;/mrow&gt;&lt;/msup&gt;&lt;/math&gt;&lt;/span&gt; and O&lt;sup&gt;−2&lt;/sup&gt;, which implies that the B atom loses the two 4s electrons and one of the d electrons, so that Sc would be d&lt;span&gt;&lt;math&gt;&lt;msup&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;0&lt;/mn&gt;&lt;/mrow&gt;&lt;/msup&gt;&lt;/math&gt;&lt;/span&gt;, Ti d&lt;span&gt;&lt;math&gt;&lt;msup&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;1&lt;/mn&gt;&lt;/mrow&gt;&lt;/msup&gt;&lt;/math&gt;&lt;/span&gt;, V d&lt;span&gt;&lt;math&gt;&lt;msup&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msup&gt;&lt;/math&gt;&lt;/span&gt; and so on. The results of the quantum mechanical calculations (with an &lt;em&gt;all electron&lt;/em&gt; Gaussian type basis set, hybrid functionals and the CRYSTAL code) show that the d occupancy on B is very close to the one of the isolated neutral atom: Sc=0.91 vs 1.0, Ti=2.02 vs 2.0, V=2.91 vs 3.0, Cr=4.07 vs 4.0, Co 7.07 vs 7.0, in contrast with the fully ionic model. The net atomic charges, Q, on the atom B, are far from the ionic limit: +2.06, +1.92, +2.05, +1.81 and +1.74 from Sc to Co. The B net charges are then close to +2(instead of the formal ionic value of +3), with a maximum difference of −0.3 for Co. This lower atomic charge is compensated by the oxygen charge which is slightly oscillating between −1.48 and −1.62 (instead of −2), whereas the La net charge is around +2.70 (instead of the formal +3 value). The reduced ionicity involves then, rather than the d shell, the partial occupancy of the 4s orbitals and their interaction with the p orbitals of oxygen. At variance with respect to Q, the atomic magnetic moments &lt;span&gt;&lt;math&gt;&lt;mi&gt;μ&lt;/mi&gt;&lt;/math&gt;&lt;/span&gt; are very close to the ideal values: 0.96 vs 1 &lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mo&gt;|&lt;/mo&gt;&lt;mi&gt;e&lt;/mi&gt;&lt;mo&gt;|&lt;/mo&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt; for Ti, 1.90 vs 2 &lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mo&gt;|&lt;/mo&gt;&lt;mi&gt;e&lt;/mi&gt;&lt;mo&gt;|&lt;/mo&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt; for V, 2.88 vs 3 &lt;span&gt;&lt;math&gt;&lt;mrow&gt;&lt;mo&gt;|&lt;/mo&gt;&lt;mi&gt;e&lt;/mi&gt;&lt;mo&gt;|&lt;/mo&gt;&lt;/mrow&gt;&lt;/math&gt;&lt;/span&gt; for Cr (the ground state of the Sc and Co compounds is closed shell, with no spin polarization). The Q and &lt;span&gt;&lt;math&gt;&lt;mi&gt;μ&lt;/mi&gt;&lt;/math&gt;&lt;/span&gt; values of three fluorides (KScF&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;3&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;, KCrF&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;3&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;, KCoF&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;3&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;) are also presented, to evidentiate the large differences between oxides and fluori","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"591 ","pages":"Article 112594"},"PeriodicalIF":2.0,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143164750","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}

{"title":"Structural and vibrational spectral analysis of polymorphs of anhydrous Acyclovir Using terahertz and Raman spectroscopy","authors":"Qiuhui Zhao ,&nbsp;Jiale Zhang ,&nbsp;Yaqi Jing ,&nbsp;Jiadan Xue ,&nbsp;Jianjun Liu ,&nbsp;Jianyuan Qin ,&nbsp;Zhi Hong ,&nbsp;Yong Du","doi":"10.1016/j.chemphys.2024.112584","DOIUrl":"10.1016/j.chemphys.2024.112584","url":null,"abstract":"<div><div>Acyclovir (ACV), a prototypical antiviral drug, exhibits distinct physicochemical properties due to its polymorphism. In this study, two stable anhydrous forms of ACV were prepared at room temperature through high-temperature dehydration and recrystallization from methanol solution, respectively. Our objective was to delve into the differences in internal structure and vibrational modes between these two forms. Terahertz (THz) spectroscopy, combined with Raman spectroscopy, served as the primary characterization techniques. Additionally, gas-phase and multiple solid-state quantum chemical software packages based on density functional theory (DFT) were utilized for simulations to assist in interpreting experimental spectral data, evaluating the accuracy of different simulation methods for spectral prediction, and achieving a more comprehensive and accurate assignment of vibrational modes. These studies not only provide important insights into the THz and Raman spectroscopic characteristics of ACV but also offer novel ideas and methodologies for the spectroscopy study of related drug molecules.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"591 ","pages":"Article 112584"},"PeriodicalIF":2.0,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143164748","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}

{"title":"Effect of quantum interference and doping on thermoelectric performance in GYNR and GYCNNR molecular junctions with PBCF-graphene nanoribbon electrodes","authors":"Xu Tang ,&nbsp;Kai-Bo Zhang ,&nbsp;Shi-Hua Tan ,&nbsp;Xiao-Fang Peng ,&nbsp;Meng-Qiu Long","doi":"10.1016/j.chemphys.2024.112585","DOIUrl":"10.1016/j.chemphys.2024.112585","url":null,"abstract":"<div><div>In carbon-based molecule rings, quantum interference and doping can be employed to enhance the thermoelectric properties by controlling charge transport. Towards this goal, we investigate the thermoelectric performance of GYNR and GYCNNR molecular junctions with PBCF-graphene nanoribbon electrodes by applying the nonequilibrium Green’s function technique and Landauer transport theory. The results reveal that the thermoelectric properties can be greatly enhanced in both GYNR and GYCNNR molecular junctions at positive energies where manifests a constructive quantum interference. While in negative energy region, their thermoelectric performances are very low due to destructive quantum interference. Especially, the nitrogen-atom doped L-GYCNNR-M-PBCFs can obviously suppress phonon transport, resulting in a lower phonon thermal conductance, and effectively tune the electronic properties and seebeck coefficient. Furthermore, the length of carbon chain between GYNR (or GYCNNR) and BCF-graphene nanoribbon electrodes can also significantly regulate the electronic transport properties and thermoelectric performance. As a result, the figure-of-merit will be over 2 in L-GYNR-M-PBCF, and over 5.5 in L-GYCNNR-M-PBCF at room temperature.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"591 ","pages":"Article 112585"},"PeriodicalIF":2.0,"publicationDate":"2025-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143164924","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}

{"title":"Performance analysis of activation functions in molecular property prediction using Message Passing Graph Neural Networks","authors":"Garima Chanana","doi":"10.1016/j.chemphys.2024.112591","DOIUrl":"10.1016/j.chemphys.2024.112591","url":null,"abstract":"<div><div>Deep learning has significantly advanced molecular property prediction, with Message-Passing Graph Neural Networks (MPGNN) standing out as an effective method. This study systematically evaluates the performance of ten activation functions — Sigmoid, Tanh, ReLU, Leaky ReLU, ELU, SELU, Softmax, Swish, Mish, and GeLU — using the MPGNN model on the QM9 dataset. It aims to identify the most suitable activation functions for training neural networks for specific molecular properties. The study examines electronic properties such as HOMO, LUMO, HOMO-LUMO energy gap, dipole moment, and polarizability, as well as thermal properties like zero-point vibrational energy and specific heat capacity. The findings reveal that different activation functions excel for different properties: SELU for HOMO, ELU for LUMO, Sigmoid for the HOMO-LUMO gap, Mish for polarizability, GELU for ZPVE, and Leaky ReLU for dipole moment and specific heat capacity. These insights are vital for optimizing MPGNN design for targeted molecular property prediction.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"591 ","pages":"Article 112591"},"PeriodicalIF":2.0,"publicationDate":"2025-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143164849","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}

{"title":"Influence of vacancy defects on the diffusion of Li adsorbed atoms on arsenene and its role in Li-ion battery","authors":"Hussain Ali,&nbsp;Gul Rahman","doi":"10.1016/j.chemphys.2024.112581","DOIUrl":"10.1016/j.chemphys.2024.112581","url":null,"abstract":"<div><div>First-principles calculations based on density functional theory (DFT) are employed to investigate the influence of vacancy defect on the diffusion of Li adsorbed atoms on arsenene and its role in Li-ion batteries (LIBs). Different adsorption sites are considered for Li at pristine arsenene surface. Li adatom preferably adsorbed on the valley sites, introducing strong binding between lithium atoms and arsenene monolayer which is an important fact for battery application. The diffusion barrier energies of Li ions are calculated using nudged elastic band method. The activation energy barrier of Li-ion is 0.13 eV and show isotropic behavior for different pathways. The open circuit voltage is found to be 0.63 V. The interaction of Li-ions with single vacancy (SV) in arsenene is investigated. The results show that the lithium adatom adsorbed on the vacancy site has a negative adsorption energy of −2.47 eV. During Li migration from vacancy to valley site, the highest diffusion barrier (2.46 eV) is found which suggests that Li could be trapped in the As vacancy. Our findings indicate that low open circuit voltage and low diffusion barrier make arsenene as a good candidate anode material for applications in Li-ion batteries.</div></div>","PeriodicalId":272,"journal":{"name":"Chemical Physics","volume":"591 ","pages":"Article 112581"},"PeriodicalIF":2.0,"publicationDate":"2024-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143164925","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}