Physical Chemistry Chemical Physics最新文献_第10页

pH-dependent reactivity of water at MgO(100) and MgO(111) surfaces†

IF 2.9 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-02-10 DOI: 10.1039/D4CP04223A

Narendra M. Adhikari, Piotr Zarzycki, Zheming Wang and Kevin M. Rosso

{"title":"pH-dependent reactivity of water at MgO(100) and MgO(111) surfaces†","authors":"Narendra M. Adhikari, Piotr Zarzycki, Zheming Wang and Kevin M. Rosso","doi":"10.1039/D4CP04223A","DOIUrl":"10.1039/D4CP04223A","url":null,"abstract":"Facet-dependent surface charging of metal oxides in water dominates the ion transport behavior across the interface, in turn impacting many natural and industrial processes such as adsorption, the formation and stabilization of nanoparticle suspensions, corrosion, and heterogeneous catalysis. Here we investigated the pH-dependent surface chemistry of two low-index MgO single crystal surfaces, namely MgO(100) and MgO(111), using vibrational sum frequency generation (vSFG) spectroscopy. This allowed us to evaluate facet-dependent pH effects on the hydration and hydroxylation at the solid/aqueous interface and point-of-zero charge (PZC) values. The MgO system is complicated by its thermodynamic instability with respect to Mg(OH)2 in water at ambient conditions. For both hydroxylated MgO(100) and MgO(111) surfaces, the PZC is found to be around pH ∼ 12, which compares well with reported values for MgO single crystal and nanoparticle surfaces. However, structure specific differences in the molecular water hydrogen bonding network near the surface are evident at mildly acidic pH. To our knowledge, this is the first account of the PZC values for the MgO(111) single-crystal surface, an electrostatically unstable MgO termination that is prone to reconstruction.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":" 8","pages":" 4343-4354"},"PeriodicalIF":2.9,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375232","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Effect of Doping on Anti-Phase Boundaries and Magnetic Properties of D03 Structure in High Silicon Steel: First-Principles Insights

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-02-10 DOI: 10.1039/d4cp04178j

Meng Sun, Linxian Li, Hongyu Song, Shuai Tang, Qing Peng, Guichang Shen, Tianwei Xie, Fengliang Tan, Zhen-Yu Liu

{"title":"Effect of Doping on Anti-Phase Boundaries and Magnetic Properties of D03 Structure in High Silicon Steel: First-Principles Insights","authors":"Meng Sun, Linxian Li, Hongyu Song, Shuai Tang, Qing Peng, Guichang Shen, Tianwei Xie, Fengliang Tan, Zhen-Yu Liu","doi":"10.1039/d4cp04178j","DOIUrl":"https://doi.org/10.1039/d4cp04178j","url":null,"abstract":"The D03 ordered structure is crucial for the room-temperature plasticity of high silicon steel. The formation of anti-phase boundaries (APBs) due to dislocation movement in the ordered structures hinders subsequent dislocation motion, leading to embrittlement. A low anti-phase boundary energy (γAPB) can facilitate dislocation slip and enhance the plastic deformation capability of the ordered structures. In this study, we calculated γAPB of two types of APBs of D03 (110) <111> by substituting Fe atoms with six transition metals: Ti, V, Cr, Zr, Nb, and Mo. We also evaluated the mechanical constants and magnetic moment of the doped D03 structures. The results show that doping Cr, Nb, and Mo significantly reduces γAPB, positively affecting the plasticity of D03. Charge density analysis indicates that Cr, Nb, and Mo, particularly Cr and Mo, increase charge transfer between atoms across the APBs, enhancing interatomic interactions. Giving a new theoretical explanation for the experimental findings that Cr and Nb can improve the plasticity of high silicon steel. Additionally, alloying elements influence the total magnetic moment of D03 compounds by altering the local environment of Fe atoms closest to Si, interatomic interactions, and the unpaired electrons in the d-band of the compounds.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"9 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375315","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Molecular dynamics simulation on the role of CL5D in accelerating the product dissociation of SIRT6†

IF 2.9 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-02-10 DOI: 10.1039/D4CP03870C

Hao Rao, Ting Yang, Yue Wang, Junwen Fei, Li-Hua Bie and Jun Gao

{"title":"Molecular dynamics simulation on the role of CL5D in accelerating the product dissociation of SIRT6†","authors":"Hao Rao, Ting Yang, Yue Wang, Junwen Fei, Li-Hua Bie and Jun Gao","doi":"10.1039/D4CP03870C","DOIUrl":"10.1039/D4CP03870C","url":null,"abstract":"SIRT6 is a member of the NAD+-dependent histone deacetylase family and is integral to maintaining genome stability and regulating metabolic transcription. SIRT6 transfers acetyl groups from the lysine side chains of protein substrates to the cofactor NAD+, generating nicotinamide, 2′-O-acyl-ADP-ribose (ADPr), and a deacetylated substrate. SIRT6 has been found to be activated by small molecule activators, such as CL5D. However, the process of dissociation of the SIRT6 product and the mechanism of activation by small molecule activators are unknown. In this work, we elucidated these activation mechanisms by performing extensive molecular dynamics simulations. The results of random acceleration molecular dynamics and umbrella sampling demonstrated that the dissociation sequence involves the exit of the deacetylated substrate first, followed by ADPr. The binding of CL5D does not alter the dissociation pathway of the products, but it increases the catalytic activity of SIRT6 by facilitating the dissociation of products within SIRT6. Our results suggest a mechanism of SIRT6 activation, which highlights the importance of product dissociation in enzyme catalysis. This result may help facilitate the development of new SIRT6 activators.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":" 8","pages":" 4298-4306"},"PeriodicalIF":2.9,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375234","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Exploring the physical properties of the new MoX6 (X = Cl or Br) materials

IF 2.9 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-02-10 DOI: 10.1039/D4CP04360J

A. Jabar, N. Maaouni, S. Benyoussef and L. Bahmad

{"title":"Exploring the physical properties of the new MoX6 (X = Cl or Br) materials","authors":"A. Jabar, N. Maaouni, S. Benyoussef and L. Bahmad","doi":"10.1039/D4CP04360J","DOIUrl":"10.1039/D4CP04360J","url":null,"abstract":"In this study, we present a comprehensive investigation of the mechanical, electronic, optical, and thermodynamic properties of MoX6 (X = Cl or Br) using first-principles calculations within the Wien2k framework, which is based on the full-potential linearized augmented plane wave (FPLAPW) method. Our approach incorporates the GGA+SOC+U formalism, crucial for accurately capturing intricate electronic interactions and spin–orbit coupling (SOC) effects, alongside Hubbard U corrections. This rigorous methodology allowed us to thoroughly explore the mechanical robustness, electronic structure, and optical responses of the MoX6 compounds and their thermodynamic behavior under varying conditions. The results reveal the mechanical stability of the MoX6 compounds with significant insights into their electronic structure, characterized by unique band features that underline their potential utility in advanced optoelectronic devices. The optical analysis highlights key absorption properties, which could be harnessed in photonic applications. Furthermore, the thermodynamic properties suggest a strong stability profile, reinforcing their suitability for diverse materials science applications. To our knowledge, this study represents the first detailed examination of MoX6 compounds using this advanced computational framework. These findings provide a foundation for further theoretical and experimental investigations while offering promising avenues for exploring related compounds with analogous structural and electronic characteristics. This work contributes significantly to the broader understanding of transition metal halides and their potential technological applications.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":" 8","pages":" 4383-4397"},"PeriodicalIF":2.9,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375231","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

First-principles study of pristine and transition metal (Fe/Co/Ti)-doped layered MoS2 as anode materials for sodium-ion batteries

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-02-09 DOI: 10.1039/d5cp00286a

Wenlong Xi, Patrick H-L Sit

{"title":"First-principles study of pristine and transition metal (Fe/Co/Ti)-doped layered MoS2 as anode materials for sodium-ion batteries","authors":"Wenlong Xi, Patrick H-L Sit","doi":"10.1039/d5cp00286a","DOIUrl":"https://doi.org/10.1039/d5cp00286a","url":null,"abstract":"In this work, we apply first-principles density functional theory (DFT) calculations to study the intercalation of Na atoms into the pristine and transition metal (TM) doped MoS2 ⁠(MxMo1-xS2) layers. Our results show that TM atom doping enhances the binding of the Na atoms between the MxMo1-xS2⁠ (M: Fe/Co/Ti) layers. Moreover, we find that Na intercalation facilitates the transition from the 2H phase to the 1T phase of the MoS2 in agreement with previous findings. However, Fe and Co doping is found to promote such transition; conversely, Ti doping is found to delay this transition. MxMo1-xS2⁠ have metallic properties, and the doping increases the average open-circuit voltage (OCV) of the 1T and 2H phase MxMo1-xS2. This work provides a new perspective on the phase change mechanism of transition metal dichalcogenide and valuable theoretical insights for the development of doped MoS2 nanomaterials in Na-ion battery applications.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"9 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143371492","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Magnetic quantum phase transition extension in strained P-doped graphene

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-02-07 DOI: 10.1039/d4cp04573d

Natalia Cortés, J. Hernández-Tecorralco, L. Meza-Montes, R. de Coss, Patricio Vargas

{"title":"Magnetic quantum phase transition extension in strained P-doped graphene","authors":"Natalia Cortés, J. Hernández-Tecorralco, L. Meza-Montes, R. de Coss, Patricio Vargas","doi":"10.1039/d4cp04573d","DOIUrl":"https://doi.org/10.1039/d4cp04573d","url":null,"abstract":"We explore quantum-thermodynamic effects in a phosphorous (P)-doped graphene monolayer subjected to biaxial tensile strain. Introducing substitutional P atoms in the graphene lattice generates a tunable spin magnetic moment controlled by the strain control parameter ε. This leads to a magnetic quantum phase transition (MQPT) at zero temperature modulated by ε. The system transitions from a magnetic phase, characterized by an out-of-plane sp3 type hybridization of the P–carbon (P–C) bonds, to a non-magnetic phase when these bonds switch to in-plane sp2 hybridization. Employing a Fermi–Dirac statistical model, we calculate key thermodynamic quantities such as the electronic entropy Se and electronic specific heat Ce. At finite temperatures, we find a MQPT extension characterized by Se and Ce, where both display a distinctive Λ-shape profile as a function of ε. These thermodynamic quantities sharply increase up to ε = 5% in the magnetic regime, followed by a sudden drop at ε = 5.5%, transitioning to a linear dependence on ε in the nonmagnetic regime. This controllable magnetic-to-nonmagnetic switch offers potential applications in electronic nanodevices operating at finite temperatures.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"78 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143258332","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Molecular-level insight into ciprofloxacin adsorption on goethite: I. Approach and non-specific binding†

IF 2.9 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-02-07 DOI: 10.1039/D4CP04027A

Sébastien Le Crom and Jean-François Boily

{"title":"Molecular-level insight into ciprofloxacin adsorption on goethite: I. Approach and non-specific binding†","authors":"Sébastien Le Crom and Jean-François Boily","doi":"10.1039/D4CP04027A","DOIUrl":"10.1039/D4CP04027A","url":null,"abstract":"The fate of the antibiotic ciprofloxacin (CIP) in natural waters can be strongly affected by interactions with nanominerals, such as goethite (GT; α-FeOOH). Using classical molecular dynamics, this study resolved the early stages of CIP adsorption on the four main crystallographic faces of GT nanoparticles, which is otherwise difficult to study experimentally. These early stages are driven by (i) electrostatic attraction, and (ii) the establishment of non-specific bonds between CIP (carboxyl, keto, amine) and GT (surface OH) functional groups. Simulations revealed that the medium-range (<1.5 nm) approach was not influenced by crystallographic orientation, but primarily by local positive charges generated by the interfacial orientation of GT surface OH groups. As a result, the deprotonated CIP− species reached the highest densities and residence times near GT surfaces, followed by the zwitterionic CIP−/+ species, and finally the protonated CIP+ species. Hydrogen bond numbers follow the same trend, and result from interactions between CIP carboxyl and GT surface O(H) groups. However, the protonated CIP+ species formed more hydrogen bonds and the most stable hydrogen bonds with the reactive OH groups of the (100) and (110) faces of GT. Additionally, protonation facilitated access to the (010) face by allowing the carboxyl group to fit into a tightly-bound water layer. By resolving the very first stages of CIP–GT interactions, this study established a foundational understanding of the precursor species which ultimately lead to redox-active Fe-bonded CIP species that can alter antimicrobial resistance in nature. These findings should thus contribute to a deeper understanding of mineral–organic interactions and to antibiotic transport in nature.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":" 8","pages":" 4446-4456"},"PeriodicalIF":2.9,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143258334","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

In-depth electronic behavior of pentagraphene and pentagonal-silicene sheets for DNA nucleic-base detection: implications for genetic biomarker sensing

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-02-07 DOI: 10.1039/d4cp04344h

Arzoo Hassan, Andleeb Mehmood, Umer Younas, Xiaoqing Tian

{"title":"In-depth electronic behavior of pentagraphene and pentagonal-silicene sheets for DNA nucleic-base detection: implications for genetic biomarker sensing","authors":"Arzoo Hassan, Andleeb Mehmood, Umer Younas, Xiaoqing Tian","doi":"10.1039/d4cp04344h","DOIUrl":"https://doi.org/10.1039/d4cp04344h","url":null,"abstract":"Silicon-based chemical sensors are optimal for detecting biological entities, because of their fast biocompatible, non-invasive nature. Going beyond the hexagons in this paper we propose pristine, and metal [Gold (Au) and Tungsten (W)] atoms doped pentagonal silicene (p-Si) and pentagraphene (PG) based single DNA nucleic base sensors. Using first-principles calculations, we present a comparative study of DNA nucleic bases namely Adenine (A), Guanine (G), Cytosine (C), and Thymine (T) adsorbed on pristine and metal-doped PG and p-Si, to determine their potential as nucleic base detectors or other chemical species. The calculated binding affinity on PG and p-Si surface by M062X/6-31G* level of theory and adsorption energies by DFT predicts that PG has higher sensitivity towards DNA nucleic bases compared to p-Si with evident changes in their work function and band structure properties. In the later part, we show that the doping of Au and W has significantly enhanced the sensitivity of PG and p-Si towards the DNA nucleic bases which is also evident in their electronic band structures and PDOS calculations. The significant changes in the electronic properties of PG and p-Si with adsorbed nucleobases make it a promising candidate for rapid sensing, sequencing, and identification of DNA nucleic base elements. This study provides new insights into the physical and chemical interactions between biomolecules and PG/p-Si, highlighting its potential as a template for nanobiological devices. Both Au and W doping enhance the adsorption properties, suggesting that PG and p-Si could be effectively used for biomolecule sensing applications.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"64 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143258337","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Accelerating Structure Prediction of Molecular Crystals using Actively Trained Moment Tensor Potential

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-02-07 DOI: 10.1039/d4cp04578e

Nikita Rybin, Ivan S. Novikov, Alexander V. Shapeev

引用次数: 0

Showcasing physical chemistry research in Australia and New Zealand – a vital nexus of innovation and opportunity

IF 2.9 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-02-07 DOI: 10.1039/D5CP90032H

Sarah L. Masters and Lars Goerigk

引用次数: 0