Chemical Physics Letters最新文献

{"title":"Structural entropy of glass-forming liquid","authors":"Rui Qi,&nbsp;Minhua Sun","doi":"10.1016/j.cplett.2024.141685","DOIUrl":"10.1016/j.cplett.2024.141685","url":null,"abstract":"<div><div>Drawing on Shannon entropy, we developed a parameter called “structural entropy,” which is derived uniquely from atomic configurations and serves to measure the evolution of disorder during the glass transition. We applied this parameter to the glass transition in the CuZrAl system. A comparison with configurational entropy suggests that both may fundamentally encapsulate the same physical concept: the system’s level of disorder. This new structural entropy parameter bridges the gap between the macroscopic properties and the microscopic structure of glass, offering insights into the mechanisms underlying the glass transition.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"856 ","pages":"Article 141685"},"PeriodicalIF":2.8,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142433445","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":"Tuning the HOMO-LUMO gap of polycyclic conjugated molecules using benzo-annelation strategy","authors":"Slavko Radenković,&nbsp;Slađana Đorđević,&nbsp;Marijana Nikolendžić","doi":"10.1016/j.cplett.2024.141686","DOIUrl":"10.1016/j.cplett.2024.141686","url":null,"abstract":"<div><div>The effect of benzo-annelations on the HOMO-LUMO energy gaps was examined in a series of benzo-derivatives of anthracene and acridine. It was shown that angular benzo-annelation increases the HOMO-LUMO gap value, while linear benzo-annelation decreases it compared to the non-annelated parent molecules. A simple quantitative model was developed being able to accurately predict the HOMO-LUMO gap values using only the numbers of angularly and linearly annelated benzene rings.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"856 ","pages":"Article 141686"},"PeriodicalIF":2.8,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142445437","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":"First principles insights into the electronic and magnetic properties of SnO2(110) doped with VIII-group transition metal single atom","authors":"Jingzhi Zhao ,&nbsp;Dachang Chen ,&nbsp;Yihang Liu ,&nbsp;Qing Miao ,&nbsp;Song Xiao ,&nbsp;Xiaoxing Zhang ,&nbsp;Beibei Xiao","doi":"10.1016/j.cplett.2024.141677","DOIUrl":"10.1016/j.cplett.2024.141677","url":null,"abstract":"<div><div>Inspired by the unprecedented surface chemical reaction activity of single-atom catalysts (SAC), this research presents a theoretical study on the doping of <span><math><mrow><msub><mrow><mi>S</mi><mi>n</mi><mi>O</mi></mrow><mn>2</mn></msub><mrow><mo>(</mo><mn>110</mn><mo>)</mo></mrow></mrow></math></span> surface with transition metal group VIII atoms (Fe, Co, Ni, Ru, Rh, Pd, Os, Ir, Pt). Using density functional theory (DFT), the formation energy, electronic structure, charge transfer and magnetic moments of the <span><math><mrow><msub><mrow><mi>S</mi><mi>n</mi><mi>O</mi></mrow><mn>2</mn></msub><mrow><mo>(</mo><mn>110</mn><mo>)</mo></mrow></mrow></math></span> system before and after doping were investigated. The formation energies of the different doped systems vary depending on the doping position. The doping of transition metal (TM) atoms can induce produces both charge transfer and magnetic moment. The charge transfer is largest in the Pd-doped system, with + 0.68 e at the position of the penta-coordinated Sn atom (<span><math><mrow><msub><mrow><mi>S</mi><mi>n</mi></mrow><mrow><mn>5</mn><mi>c</mi></mrow></msub></mrow></math></span> position) and + 0.67 e at the position of the hexa-coordinated Sn atom (<span><math><mrow><msub><mrow><mi>S</mi><mi>n</mi></mrow><mrow><mn>6</mn><mi>c</mi></mrow></msub></mrow></math></span> position), while the Co-doped system exhibits the smallest charge transfer of + 0.19 e (<span><math><mrow><msub><mrow><mi>S</mi><mi>n</mi></mrow><mrow><mn>6</mn><mi>c</mi></mrow></msub></mrow></math></span> position). Fe, Co, Ni, Ru and Os atoms introduce magnetic moments, with the Fe-doped system (<span><math><mrow><msub><mrow><mi>S</mi><mi>n</mi></mrow><mrow><mn>5</mn><mi>c</mi></mrow></msub></mrow></math></span> position) having the highest magnetic moments of 2.91 <span><math><mrow><msub><mi>μ</mi><mi>B</mi></msub></mrow></math></span>. In the <span><math><mrow><msub><mrow><mi>S</mi><mi>n</mi><mi>O</mi></mrow><mn>2</mn></msub><mrow><mo>(</mo><mn>110</mn><mo>)</mo></mrow></mrow></math></span> surface system doped with TM atoms, there are varying degrees of orbital overlap between the TM atoms and their surrounding O atoms. This theoretical work provides valuable insights into the physical properties of metal oxide based single-atom catalysts.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"856 ","pages":"Article 141677"},"PeriodicalIF":2.8,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142442827","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":"Transition metal enhanced black phosphorus for early thermal runaway gas detection of lithium-ion batteries: A theoretical study","authors":"Yongxu Yan ,&nbsp;Zhengwei Zhou ,&nbsp;Peng Wu ,&nbsp;Bowen Tang ,&nbsp;Ju Tang ,&nbsp;Xiaoxing Zhang ,&nbsp;Song Xiao","doi":"10.1016/j.cplett.2024.141675","DOIUrl":"10.1016/j.cplett.2024.141675","url":null,"abstract":"<div><div>Lithium-ion batteries have seen widespread use, bringing the issue of thermal runaway into sharp focus. Thermal runaway can be diagnosed by the characteristic gases produced (CO₂, H₂, CO, CH₄, C₂H₄, C₂H₆). Black phosphorus (BP) with corrugated plane was utilized as the base material, enhancing its chemical activity with transition metals (Au, Ag, Pt, Pd). The four transition metal-enhanced BPs can selectively adsorb CO and C₂H₄ with different response characteristics, which can be used to identify CO and C₂H₄. This study provides theoretical guidance for the engineering application of transition metal-enhanced BP in monitoring thermal runaway gases in lithium-ion batteries.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"857 ","pages":"Article 141675"},"PeriodicalIF":2.8,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142445968","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":"Formation of orthorhombic CH3NH3PbI3 perovskite co-doped with ytterbium and gadolinium","authors":"Rina Tanaka ,&nbsp;Atsushi Suzuki ,&nbsp;Takeo Oku ,&nbsp;Tomoharu Tachikawa ,&nbsp;Sakiko Fukunishi","doi":"10.1016/j.cplett.2024.141679","DOIUrl":"10.1016/j.cplett.2024.141679","url":null,"abstract":"<div><div>Orthorhombic CH₃NH₃PbI₃ perovskite crystals were formed by co-doping1.0 at% ytterbium and 0.5 at% gadolinium at lead sites. X-ray diffraction results showed that the perovskite crystals fabricated at 190°C in an atmospheric air provided an orthorhombic structure even at room temperature. Although the highest power conversion efficiency was 1.73 % for the as-prepared device, the efficiency was improved to 11.6 % after 113 days, which could be due to decrease in series resistance caused by (100)-oriented crystal growth during room temperature aging.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"856 ","pages":"Article 141679"},"PeriodicalIF":2.8,"publicationDate":"2024-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142417575","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":"Two-state free-volume model for anomalous dynamics in supercooled water macromolecules undergoing liquid–liquid phase transition","authors":"Peizhao Li ,&nbsp;Haibao Lu ,&nbsp;Tengfei Zheng ,&nbsp;Yong-Qing Fu","doi":"10.1016/j.cplett.2024.141674","DOIUrl":"10.1016/j.cplett.2024.141674","url":null,"abstract":"<div><div>Modelling anomalous dynamics of complex liquid water is a huge challenge due to its various condensed molecular structures and the associated liquid–liquid phase transitions (LLPTs). In this study, we considered, for the first time, the influences of free volume and entropy on LLPTs for both low-density liquid (LDL) and high-density liquid (HDL) waters. Firstly, we proposed a two-state free-volume model and combined with the Adam-Gibbs models to investigate the dynamic equilibria with free diffusion coefficient, viscosity, glass transition temperature and the anomalous dynamics in the two-state water. Free-energy equation was then developed to explore the constitutive relationships of free volume, entropy and anomalously dynamic behaviors. Finally, analytical results of the proposed two-state free-volume model were compared with the experimental data of two-state water reported in literature, and good agreements between them were demonstrated. This study offers a new physical insight into free volume for the anomalous dynamics and LLPTs in the two-state water.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"856 ","pages":"Article 141674"},"PeriodicalIF":2.8,"publicationDate":"2024-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142417568","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":"Large 2π aromatic six-membered Al/In rings stabilized by transition-metal-like heavy alkaline earth metals","authors":"Mingxiao Jin ,&nbsp;Xinde Li ,&nbsp;Peng Jin","doi":"10.1016/j.cplett.2024.141676","DOIUrl":"10.1016/j.cplett.2024.141676","url":null,"abstract":"<div><div>Density functional theory calculations revealed that four half-sandwich Ae(MH)₆ (Ae = Sr or Ba; M = Al or In) complexes all feature large six-membered Al₆/In₆ rings with rare 2π aromaticity. Together with two Ca analogues, these six molecules all exhibit good thermodynamic and kinetic stabilities. Heavy Ca/Sr/Ba atoms can effectively stabilize the two hexagonal rings via both ionic and covalent interactions involving their <em>n</em>s, (<em>n</em> − 1)p and even (<em>n</em> − 1)d orbitals. Our work not only adds new members to the emerging 2π-aromatic ring family, but also demonstrates the critical role of the transition-metal-like behavior of Ca/Sr/Ba in stabilizing novel metalloaromatic ring structures.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"856 ","pages":"Article 141676"},"PeriodicalIF":2.8,"publicationDate":"2024-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142417567","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":"Addition of CuO to form CuO/TiO2 and CuO/ZnO heterojunctions for photocatalytic CO2 conversion to methanol","authors":"Sunil Kumar Sahoo ,&nbsp;Athira P ,&nbsp;Koustuv Ray ,&nbsp;Dharmendra Pandey","doi":"10.1016/j.cplett.2024.141678","DOIUrl":"10.1016/j.cplett.2024.141678","url":null,"abstract":"<div><div>Photocatalytic conversion of carbon dioxide (CO₂) to value-added products is a promising route towards sustainability. In this work, gas phase CO₂ in presence of water vapor and UV irradiation source was converted to methanol using TiO₂, ZnO, CuO/TiO₂ and CuO/ZnO photocatalysts. Characterization by physico-chemical, optical and First-principle based techniques revealed that CuO/TiO₂ possessed increased oxygen vacancy, highest average electron lifetime, transfer rate, injection efficiency and highest separation efficiency. The maximum methanol (∼28 %) yield of CuO/TiO₂ is ascribed due to combined effect of heterojunction formation and increment in surface oxygen vacancies by doping with CuO, acted as electron-trapping cocatalyst.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"856 ","pages":"Article 141678"},"PeriodicalIF":2.8,"publicationDate":"2024-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142417628","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":"Boron nitride graphite intercalated with carbon-boron-nitride fullerenes for enhanced hydrogen storage","authors":"Xuan Peng","doi":"10.1016/j.cplett.2024.141673","DOIUrl":"10.1016/j.cplett.2024.141673","url":null,"abstract":"<div><div>The hydrogen storage of boron nitride graphite intercalated with carbon-boron-nitride fullerenes was investigated using density functional theory and Grand Canonical Monte Carlo simulations. At 77 K and 30 MPa, the optimized structures C₁₄(BN)₂₃-inserted BN graphite material achieved a gravimetric hydrogen adsorption of 6.39 wt% and a volumetric adsorption of 0.07 kg/L, surpassing the U.S. Department of Energy’s targets of 5.5 wt% and 0.04 kg/L, respectively. This improved performance is attributed to the stronger adsorption affinity of BN atoms and the increased lattice constants of the material. These findings offer promising avenues for the development of advanced hydrogen storage materials.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"856 ","pages":"Article 141673"},"PeriodicalIF":2.8,"publicationDate":"2024-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142417574","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":"Small compressive strain tuning of α-TeO2 and β-TeO2 polymorphs: Electronic, linear, and nonlinear optical properties from first-principles calculations","authors":"M. Naveed-Ul-Haq","doi":"10.1016/j.cplett.2024.141669","DOIUrl":"10.1016/j.cplett.2024.141669","url":null,"abstract":"<div><div>This study examines the effects of 2 % compressive strain on the structural, electronic, and optical properties of α-TeO₂ and β-TeO₂ polymorphs. α-TeO₂’s bandgap increases from 3.64 eV to 3.70 eV, while β-TeO₂’s decreases from 3.632 to 3.53 eV. Lattice parameters uniformly reduce in α-TeO₂, but vary dissimilarly in β-TeO₂. PDOS analysis shows O-2<em>p</em> and Te-5<em>p</em> states dominate near the band edges. Optical behavior is anisotropic, with enhanced polarizability and refractive indices under strain. Nonlinear optical properties improve with increased strain, especially the non-linear susceptibility components, which are relevant for second-harmonic generation. Born Effective Charges show increased Te polarization and reduced oxygen polarization, impacting dielectric response.</div></div>","PeriodicalId":273,"journal":{"name":"Chemical Physics Letters","volume":"856 ","pages":"Article 141669"},"PeriodicalIF":2.8,"publicationDate":"2024-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142417573","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}