Physical Chemistry Chemical Physics最新文献_第5页

Planar Fe2B Monolayer with Room Temperature Antiferromagnetism 具有室温反铁磁性的平面Fe2B单层

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-04-25 DOI: 10.1039/d5cp01417d

Wanting Han, Xu Yan, Ying Liu, Han Fu, Mingyang Sun, Xinrong Li, Dan Dan Wang, Lihua Yang, Xin Qu

{"title":"Planar Fe2B Monolayer with Room Temperature Antiferromagnetism","authors":"Wanting Han, Xu Yan, Ying Liu, Han Fu, Mingyang Sun, Xinrong Li, Dan Dan Wang, Lihua Yang, Xin Qu","doi":"10.1039/d5cp01417d","DOIUrl":"https://doi.org/10.1039/d5cp01417d","url":null,"abstract":"The design of two-dimensional materials with antiferromagnetic properties above room temperature is crucial for the preparation of next-generation nano-scale spintronic devices. Based on first-principles calculation combined swarm-intelligence structural prediction methods, we propose a novel planar Fe2B monolayer material. In this structure, Fe atoms form a graphene-like honeycomb pattern sublattice, with B atoms occupying the centers of Fe6 hexagons in a hexagonal lattice. The Fe2B monolayer is predicted to be kinetically, thermally, thermodynamically, and mechanically stable. Notably, it exhibits strong intrinsic antiferromagnetism arising from both superexchange and direct exchange interactions between Fe atoms. Monte Carlo simulations estimate a high Néel temperature of 608 K, indicating robust magnetic order well above room temperature. Interestingly, its above room-temperature antiferromagnetism and easy axis of magnetization can be well preserved under biaxial strains from -5% to +5%. The Fe2B monolayer provides a promising candidate material for high-performance, strain-tolerant spintronic devices and offers valuable guidance for the research of nanoscale magnetic materials.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"15 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872668","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

Mixed Functionalization as a Pathway to Induce Superconductivity in MXenes: Vanadium and Niobium Carbide 混合功能化作为诱导MXenes：钒和铌碳化物超导的途径

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-04-25 DOI: 10.1039/d5cp00774g

Prarena Jamwal, Rajeev Ahuja, Rakesh Kumar

{"title":"Mixed Functionalization as a Pathway to Induce Superconductivity in MXenes: Vanadium and Niobium Carbide","authors":"Prarena Jamwal, Rajeev Ahuja, Rakesh Kumar","doi":"10.1039/d5cp00774g","DOIUrl":"https://doi.org/10.1039/d5cp00774g","url":null,"abstract":"The functionalization versatility of MXenes distinguishes them from other two-dimensional materials, enabling the design of numerous new materials with unique properties. By leveraging surface chemistry, functionalization allows for the manipulation of critical parameters such as the density of states and electron-phonon coupling, providing an excellent platform for exploring two-dimensional superconductivity. In this study, we investigate the impact of functionalization on Vanadium Carbide (V2C) MXene, which is intrinsically non-superconducting, by considering three different cases: (i) hydrogen adatoms, (ii) fluorine adatoms, and (iii) mixed functionalization with hydrogen and fluorine adatoms. We confirm the mechanical and dynamical stability of functionalized V2C using Born's stability criteria and phonon dispersion analyses. In all three cases, superconductivity emerges due to the presence of functional groups, which influence the electron-phonon interaction and electronic structure, leading to an enhanced electron-phonon coupling constant. The highest superconducting transition temperature is observed for mixed-functionalized V2C, attributed to the softening of the ZA phonon mode along with high-energy phonon modes induced by hydrogen. To further explore the potential of mixed functionalization in inducing superconductivity, we extend our approach to another non-superconducting MXene, Nb2C. The mixed-functionalized Nb2C exhibits a superconducting transition temperature of 9.2 K, which surpasses the reported values for Nb2CH2, Nb2CS2, and Nb2CBr2. These findings underscore the effectiveness of mixed functionalization in enabling superconductivity in MXenes, paving the way for future theoretical and experimental investigations.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"70 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143876018","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

Irregularly mechanical and thermal response of the N-H modes in the FOX-7 energetic material FOX-7高能材料中N-H模式的不规则机械和热响应

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-04-25 DOI: 10.1039/d5cp01236h

Jushan Wang, Zhaoyang Zheng, Yangyang Zeng, Zanhao Wang, Guoyang Yu, Qi-Long Yan, Huashan Li, Yanqiang Yang, Biao Wang

{"title":"Irregularly mechanical and thermal response of the N-H modes in the FOX-7 energetic material","authors":"Jushan Wang, Zhaoyang Zheng, Yangyang Zeng, Zanhao Wang, Guoyang Yu, Qi-Long Yan, Huashan Li, Yanqiang Yang, Biao Wang","doi":"10.1039/d5cp01236h","DOIUrl":"https://doi.org/10.1039/d5cp01236h","url":null,"abstract":"With the aid of Raman spectroscopy and density functional theory (DFT) calculations, we investigated the bonding dynamics of FOX-7 under mechanical and thermal perturbations. Results revealed that mechanical compression shortens and stiffens the O···H nonbonds while simultaneously lengthening and softening the H-N covalent bonds, up to critical pressures PC of 4.5 GPa, being in line with the O···H-O of ice transiting from the VII/VIII to phase X at 60 GPa. Conversely, thermal heating impacts both O···H nonbonds and H-N covalent bonds at distinct rates. The stretching and wagging vibrational modes of the H-N bonds soften within a specific pressure range, attributable to O···H-N hydrogen bonds. Additionally, FOX-7 undergoes multiple phase transitions under high pressure, including a continuous α to α' phase transition (second-order or higher-order) and a discontinuous α' to ε transition (first-order). These findings provide new insight into the bonding dynamics of FOX-7, which is in line with O···H-O bond for water and ice, showing the essentiality of inter- and intramolecular coupling interaction.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"4 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872694","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

Electrochemical-mechanical model of space charge zone at interface 界面空间电荷区的电化学-机械模型

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-04-25 DOI: 10.1039/d5cp00467e

Fuqian Yang, Erwin Hüger

{"title":"Electrochemical-mechanical model of space charge zone at interface","authors":"Fuqian Yang, Erwin Hüger","doi":"10.1039/d5cp00467e","DOIUrl":"https://doi.org/10.1039/d5cp00467e","url":null,"abstract":"The interface between solid electrolyte and electrode plays an important role in determining the physical processes controlling electrochemical performance of metal-ion batteries. In this work, we develop an electrochemical-mechanical model for the determination of net charge density, stress and electric fields in solid electrolyte, which is in contact with electrode, under the framework of thermodynamics and linear elasticity. The mobile species are cations, which occupy interstitial sites through the formation of Frenkel defects. Analytical solutions of net charge density, stress and electric fields are obtained for the linear, coupling model, which is simplified from the nonlinear, coupling system under small stress and electric fields. For a solid electrolyte sandwiched between two parallel electrodes, the numerical results predict that there exists accumulation/adsorption of a layer of charges (interstitial ions) to electrode, i.e., the presence of space charge zone, whose size is dependent on electric potential and elastic constants of the solid electrolyte. Such behavior is similar to the Stern layer for liquid electrolyte and allows for the storage of energy in a capacitive form, similar to electrical double layer. The ratio of the nominal size of space charge zone to the thickness of solid electrolyte is a decreasing function of the thickness of the solid electrolyte. The nonlinear and coupling system developed in this work lays a foundation to analyze the interface behavior of heterogeneous structures and the effects of space charge zone on the energy storage of multilayer structures. The approach developed in this work can be extended to investigate the multi-field coupling problems in solid oxide fuel cells, mixed halide quantum dots and transducers. Keyworks: Interface; Space charge zone; Gibbs free energy; Strain energy; Electric field.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"4 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143876022","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

Multi-scale Modeling and Experimental Investigation of Oxidation Behavior in Platinum Nanoparticles 铂纳米颗粒氧化行为的多尺度模拟与实验研究

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-04-24 DOI: 10.1039/d5cp00134j

Tom Demeyere, Husn Islam, Tom Ellaby, Misbah Sarwar, David Thompsett, Chris-Kriton Skylaris

{"title":"Multi-scale Modeling and Experimental Investigation of Oxidation Behavior in Platinum Nanoparticles","authors":"Tom Demeyere, Husn Islam, Tom Ellaby, Misbah Sarwar, David Thompsett, Chris-Kriton Skylaris","doi":"10.1039/d5cp00134j","DOIUrl":"https://doi.org/10.1039/d5cp00134j","url":null,"abstract":"Understanding the impact of oxidation on the reactivity and performance of Pt nanoparticles (NPs) is crucial for developing durable and efficient catalysts. In this study, we investigate the oxidation process of a realistic Pt NP using a multistep approach combining computational methods (ReaxFF, MACE-MP-0, and DFT) with experimental techniques (XRD, TEM, and EXAFS). Our workflow aims to measure oxidation extent, compare different computational models, analyze electronic structure changes, and provide guidance for selecting appropriate computational models in catalytic atomistic studies. We perform Hybrid MD-MC simulations using ReaxFF which reveal significant oxidation with oxygen penetrating deep into the core at high oxygen partial pressure, with the formation of detached small cluster oxide Pt6O8 species. We investigate the plausibility of these configurations and possible degradation mechanism by carrying out XRD, TEM, and EXAFS measurements on samples of various average particle sizes. Experimental measurements show partial agreement with our simulations in terms of coordination numbers, bond distances, oxygen fractional occupancy and onset/place-exchange potentials. Despite these agreements, we find poor matches between the binding energies calculated by ReaxFF and DFT, casting doubt on the predictive power of ReaxFF and the existence of Pt6O8 species. In contrast, the universal MACE-MP-0 model shows significant improvement in the prediction of energetics. Comparing these force fields with DFT calculations on oxidized and non-idealized systems is essential for understanding the limitations of such models in predicting catalytically relevant properties at high potentials and was previously unexplored in the literature. Our study provides a foundation for understanding the complex interplay between nanoparticle structure, oxidation state, and catalytic performance, aiming to guide the rational design of advanced catalytic materials through atomistic modeling.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"91 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866577","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

Investigating the Effectiveness of an Imidazopyridine-Based Compound as an Anti-corrosive Additive for Mild Steel in Molar Hydrochloric Solutions: A Mutual Multi-Facet Experimental and Computational Approach 咪唑吡啶基化合物在盐酸溶液中作为低碳钢防腐添加剂的有效性研究：一种相互的多方面实验和计算方法

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-04-24 DOI: 10.1039/d5cp00711a

Noureddine IDLAHOUSSAINE, Brahim El Ibrahimi, Abdelaziz AIT ADDI, Walid DAOUDI, Rachid IDOUHLI, Mohammed LASRI, Murat YILMAZ, Mahmoud EL OUARDI, El aatiaoui Abdelmalik, Abdesselam ABOUELFIDA

{"title":"Investigating the Effectiveness of an Imidazopyridine-Based Compound as an Anti-corrosive Additive for Mild Steel in Molar Hydrochloric Solutions: A Mutual Multi-Facet Experimental and Computational Approach","authors":"Noureddine IDLAHOUSSAINE, Brahim El Ibrahimi, Abdelaziz AIT ADDI, Walid DAOUDI, Rachid IDOUHLI, Mohammed LASRI, Murat YILMAZ, Mahmoud EL OUARDI, El aatiaoui Abdelmalik, Abdesselam ABOUELFIDA","doi":"10.1039/d5cp00711a","DOIUrl":"https://doi.org/10.1039/d5cp00711a","url":null,"abstract":"The use of effective, environmentally friendly inhibitors is a promising strategy to mitigate metallic corrosion. This work involved the development of a newly developed imidazopyridine-based compound (i.e., MPPIP) and an assessment of its effectiveness as an anti-corrosive entity for the mild steel metal (MS) in 1.00M hydrochloric medium. The compound’s performance was evaluated using potentiodynamic polarization (PDP) and electrochemical impedance spectroscopy (EIS), which demonstrated that MPPIP achieves 98% inhibition efficiency with 10⁻³ M concentration at the room temperature. The electrochemical analysis confirmed that MPPIP acts as a mixed-type inhibitor, reducing both anodic and cathodic reactions. Thermodynamic analyses revealed that MPPIP adsorption follows the Langmuir’s isotherm, involving a combination of physisorption and chemisorption mechanisms. Additional validation was performed using UV-Vis. spectroscopy, scanning electron microscopy (SEM), and energy-dispersive X-ray spectroscopy (EDX), which revealed a uniform protective film on the steel surface, preventing metal dissolution. Computational approaches, including density functional theory (DFT) and Monte Carlo simulations, highlighted the molecule’s high electron-donating ability and strong adsorption energy, confirming its strong interaction with the metal surface. These findings demonstrate that MPPIP is a promising and efficient corrosion inhibitor for mild steel in acidic environments with an inexpensive and easily synthesized route characteristics.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"53 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866575","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

Novel mixed topological state in monolayer MnSbO3 单层MnSbO3的新型混合拓扑态

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-04-24 DOI: 10.1039/d5cp00782h

Yanzhao Wu, Li Deng, Junwei Tong, Xiang Yin, Gaowu W. Qin, Xianmin Zhang

引用次数: 0

Strain trailing band engineering and phonon transport of high ZT ZrCoBi Half-Heusler alloy: A Mechanistic understanding from the first principles 高ZT ZrCoBi半heusler合金的应变拖带工程和声子输运：从第一性原理的机理理解

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-04-24 DOI: 10.1039/d5cp01052g

S. Mahakal, Avijit Jana, Subrata Jana, Prasanjit Samal

引用次数: 0

Improving the fluorescence brightness of NIR-II fluorophore via intramolecular covalent bond locking: A theoretical perspective 通过分子内共价键锁定提高NIR-II荧光团的荧光亮度：一个理论视角

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-04-24 DOI: 10.1039/d5cp00772k

Lingling Dong, Yuying Du, Meina Zhang, Jiancai Leng, Wei Hu, Yujin Zhang

{"title":"Improving the fluorescence brightness of NIR-II fluorophore via intramolecular covalent bond locking: A theoretical perspective","authors":"Lingling Dong, Yuying Du, Meina Zhang, Jiancai Leng, Wei Hu, Yujin Zhang","doi":"10.1039/d5cp00772k","DOIUrl":"https://doi.org/10.1039/d5cp00772k","url":null,"abstract":"Fluorescence imaging in the second near-infrared (NIR-II) region, characterized by deep tissue penetration and high spatial resolution, has emerged as a promising modality for biomedical applications. However, the majority of NIR-II fluorophores suffer from insufficient brightness primarily attributed to the limited fluorescence quantum yields. Herein, the mechanism of fluorescence brightness enhancement through intramolecular covalent bond locking strategy for donor-acceptor-donor NIR-II fluorophores is investigated. Compared with the unlocked TQ-1, fusing phenyl rings on the acceptor moiety induces bathochromic shifts in both the photoabsorption and photoemission spectra, while the modification to the donor unit results in hypsochromic effect. Notably, incorporating intramolecular covalent bond within the acceptor segment facilitates structural relaxation during the electronic transitions, which is mainly responsible for the reduction on luminescent efficiency. In contrast, by locking the terminal phenyl groups of the fluorophore, the adiabatic excitation energy is enlarged and the electron–vibration coupling as well as nonadiabatic electronic coupling is decreased, resulting in a significantly reduction on the nonradiative decay rate. Consequently, TQ-4 achieves optimal fluorescence quantum yield and brightness in the premise of NIR-II emission, demonstrating its potential as a high-performance NIR-II chromophore. This work highlights the feasibility of constructing efficient NIR-II fluorophores via intramolecular covalent bond locking, providing rational design principles for developing novel NIR-II fluorophores toward biomedical applications.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"37 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866951","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

The two-dimensional n/p type carriers at the interface of LaAlO3/KTaO3 heterostructures LaAlO3/KTaO3 异质结构界面上的二维 n/p 型载流子

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2025-04-24 DOI: 10.1039/d5cp00734h

Yirong Geng, Zuhui Hu, Chang Liu, Ruiling Gao, Hui Zhang, Le Fang, Wei Ren

{"title":"The two-dimensional n/p type carriers at the interface of LaAlO3/KTaO3 heterostructures","authors":"Yirong Geng, Zuhui Hu, Chang Liu, Ruiling Gao, Hui Zhang, Le Fang, Wei Ren","doi":"10.1039/d5cp00734h","DOIUrl":"https://doi.org/10.1039/d5cp00734h","url":null,"abstract":"This study employs first-principles calculations to investigate the behavior of two-dimensional carriers at the interfaces and surfaces of polar/polar LaAlO3/KTaO3 (LAO/KTO) heterostructures. Unlike the traditional LaAlO3/SrTiO3 (LAO/STO) polar/nonpolar heterostructures with LaAlO3 unit-cell thickness-dependent critical conductive behavior, the LaAlO3/KTaO3 heterostructures are demonstrated to have intrinsic two-dimensional carriers with carrier concentrations reaching up to 1014 cm-2, significantly higher than those observed in LaAlO3/SrTiO3 systems. Furthermore, in contrast to traditional sandwich heterostructure models, the single-interface LaAlO3/KTaO3 heterostructures exhibit no bandgap dependence on the LaAlO3 thickness. These phenomena arise from the bipolar characteristics of the LaAlO3/KTaO3 system, and it can introduce increased carrier density and reduce symmetry within the single-interface polar heterostructure. Simulation results also show that applying in-plane strain can suppress and even reverse the n/p-type of two-dimensional carriers at the interfaces. Additionally, the presence of oxygen vacancies enhances carrier accumulation by redistributing the internal polarization field of the heterostructures. Overall, this research offers a comprehensive elucidation of the behaviors and formation mechanisms for n/p-type two-dimensional carriers in polar/polar LaAlO3/KTaO3 heterostructures and provides potential strategies for manipulating these two-dimensional carriers in relevant materials and devices","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"42 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143866573","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