Physical Chemistry Chemical Physics最新文献

Multi-level chiral edge states in Janus M2XS2Se2 (M = V, Ti; X = W, Mo) monolayers with high Curie temperature and sizable nontrivial topological gaps Janus M2XS2Se2（M = V、Ti；X = W、Mo）单层中的多级手性边缘态，具有高居里温度和可观的非对偶拓扑隙缝

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-22 DOI: 10.1039/d4cp03325f

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

{"title":"Multi-level chiral edge states in Janus M2XS2Se2 (M = V, Ti; X = W, Mo) monolayers with high Curie temperature and sizable nontrivial topological gaps","authors":"Li Deng, Xiang Yin, Yanzhao Wu, Junwei Tong, Gaowu W. Qin, Xianmin Zhang","doi":"10.1039/d4cp03325f","DOIUrl":"https://doi.org/10.1039/d4cp03325f","url":null,"abstract":"Quantum anomalous Hall (QAH) insulators with dissipation-less chiral edge channels provide the ideal platforms for the exploration of topological materials and low-power spintronic devices. However, the ultralow operation temperature and small nontrivial gap are the bottlenecks for QAH insulators towards future applications. Here, a new family of QAH insulators, that is, the Janus M2XS2Se2 (M = V, Ti; X = W, Mo) monolayers are proposed, which are ferromagnets with large perpendicular magnetic anisotropy (PMA) and high Curie temperature above room-temperature. Moreover, the present M2XS2Se2 monolayers hold sizable nontrivial topological gaps, resulting in the 1st chiral edge state with Chern number C=-1. Unexpectedly, there also exists an occupied 2nd chiral edge state below the Fermi level. Although all M2XS2Se2 monolayers remain the characteristic of PMA by applying the biaxial strain, various topological phase transitions are present. V2WS2Se2 monolayer preserves the QAH state regardless of strain, while the V2MoS2Se2 and Ti2WS2Se2 monolayers transform from QAH states to metallic states under the tensile strains. The present M2XS2Se2 monolayers show the competitive advantages among the reported materials for the development of topological electronic devices.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452024","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-field-controlled positioning of magnetic domain wall in Tie-shaped asymmetric nanowire and its application for magnetic field detection 磁场控制铁形非对称纳米线中磁畴壁的定位及其在磁场检测中的应用

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-22 DOI: 10.1039/d4cp01262c

Xiaoxue Yang, Xue-Feng Zhang, Changfeng Li, Huiting Li

引用次数: 0

Experimental and theoretical study of the Sn – O bond formation between atomic tin and molecular oxygen 原子锡和分子氧之间形成 Sn - O 键的实验和理论研究

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-21 DOI: 10.1039/d4cp03687e

Iakov A. Medvedkov, Anatoliy A Nikolayev, Shane Joseph Goettl, Zhenghai Yang, Alexander Mebel, Ralf I. Kaiser

{"title":"Experimental and theoretical study of the Sn – O bond formation between atomic tin and molecular oxygen","authors":"Iakov A. Medvedkov, Anatoliy A Nikolayev, Shane Joseph Goettl, Zhenghai Yang, Alexander Mebel, Ralf I. Kaiser","doi":"10.1039/d4cp03687e","DOIUrl":"https://doi.org/10.1039/d4cp03687e","url":null,"abstract":"The merging of the electronic structure calculations and crossed beam experiments expose the reaction dynamics in the tin (Sn, 3Pj) − molecular oxygen (O2, X3Σg-) system yielding tin monoxide (SnO, X1Σ+) along with ground state atomic oxygen O(3P). The reaction can be initiated on the triplet and singlet surfaces via addition of tin to the oxygen atom leading to linear, bent, and/or triangular reaction intermediates. On both the triplet and singlet surfaces, formation of the tin dioxide structure is required prior to unimolecular decomposition to SnO(X1Σ+) and O(3P). Intersystem crossing (ISC) plays a critical role in the reaction mechanism and extensively interosculates singlet and triplet surfaces. The studied reaction follows a mechanism parallel to that for the gas phase reaction of germanium and silicon with molecular oxygen, however, the presence of the tin atom enhances and expands ISC via the “heavy atom effect”.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452025","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

Modeling Interfacial Electric Fields and the Ethanol Oxidation Reaction at Electrode Surfaces 模拟电极表面的界面电场和乙醇氧化反应

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-21 DOI: 10.1039/d4cp02765e

Yuhan Mei, Fanglin Che, Nathaniel Deskins

{"title":"Modeling Interfacial Electric Fields and the Ethanol Oxidation Reaction at Electrode Surfaces","authors":"Yuhan Mei, Fanglin Che, Nathaniel Deskins","doi":"10.1039/d4cp02765e","DOIUrl":"https://doi.org/10.1039/d4cp02765e","url":null,"abstract":"The electrochemical environment present at surfaces can have a large eﬀect on intended applications. Such environments may occur, for instance, at battery or electrocatalyst surfaces. Solvent, coadsorbates, and electrical ﬁeld eﬀects may strongly inﬂuence surface chemistry. Understanding these phenomena is an on-going area of research, especially in the realm of electrocatalysis. Herein, we modeled key steps in the ethanol oxidation reaction (EOR) over a common EOR catalyst, Rh(111), using density functional theory. We assessed how the presence of electrical ﬁelds may inﬂuence important C-C and C-H bond scission and C-O bond formation reactions with and without coadsorbed water. We found that electric ﬁelds combined with the presence of water can signiﬁcantly aﬀect surface chemistry, including adsorption and reaction energies. Our results show that C-C scission (necessary for the complete oxidation of ethanol) is most likely through CHxCO adsorbates. With no electric ﬁeld or solvent present C-C scission of CHCO has the lowest reaction energy and dominates the oxidation of ethanol. But when applying strong negative ﬁelds (with or without solvent), the C-C scission of CH2 CO and CHCO becomes competitive. The current work provides insights into how electric ﬁelds and water solvent aﬀect EOR, especially when simulated using density functional theory.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452028","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

Sensitivity analysis of aromatic chemistry to gas-phase kinetics in a dark molecular cloud model 暗分子云模型中芳香化学对气相动力学的敏感性分析

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-21 DOI: 10.1039/d4cp03229b

Alex N. Byrne, Ci Xue, Troy Van Voorhis, Brett A. McGuire

{"title":"Sensitivity analysis of aromatic chemistry to gas-phase kinetics in a dark molecular cloud model","authors":"Alex N. Byrne, Ci Xue, Troy Van Voorhis, Brett A. McGuire","doi":"10.1039/d4cp03229b","DOIUrl":"https://doi.org/10.1039/d4cp03229b","url":null,"abstract":"The increasingly large number of complex organic molecules detected in the interstellar medium necessitates robust kinetic models that can be relied upon for investigating the involved chemical processes. Such models require rate coefficients for each of the thousands of reactions; the values of these are often estimated or extrapolated, leading to large uncertainties that are rarely quantified. We have performed a global Monte Carlo and a more local one-at-a-time sensitivity analysis on the gas-phase rate coefficients in a 3-phase dark cloud model. Time-dependent sensitivities have been calculated using four metrics to determine key reactions for the overall network as well as for the cyanonaphthalene molecule in particular, an important interstellar species that is severely under-produced by current models. All four metrics find that reactions involving small, reactive species that initiate hydrocarbon growth have large effects on the overall network. Cyanonaphthalene is most sensitive to a number of these reactions as well as ring-formation of the phenyl cation (C6H5+) and aromatic growth from benzene to naphthalene. Future efforts should prioritize constraining rate coefficients of key reactions and expanding the network surrounding these processes. These results highlight the strength of sensitivity analysis techniques to identify critical processes in complex chemical networks, such as those often used in astrochemical modeling.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452119","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

Hole-states in Li doped NiO: Doping dependence of Zhang-Rice spectral weight 掺锂氧化镍中的空穴态：Zhang-Rice 光谱重量的掺杂依赖性

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-21 DOI: 10.1039/d4cp03373f

Suman Mandal, Krishnakumar S. R. Menon

引用次数: 0

Electrochemical System of Nitrogen-Doped TiO2, Fe-N-C, and Copper Hexacyanoferrate Electrodes for Photo-Assisted Energy Conversion in Acidic Wastewater Treatment 掺氮 TiO2、Fe-N-C 和六氰基铁酸铜电极的电化学系统在酸性废水处理中实现光辅助能量转换

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-21 DOI: 10.1039/d4cp02063d

Bianca Tainá Ferreira, Matheus Martins, Fritz Huguenin

{"title":"Electrochemical System of Nitrogen-Doped TiO2, Fe-N-C, and Copper Hexacyanoferrate Electrodes for Photo-Assisted Energy Conversion in Acidic Wastewater Treatment","authors":"Bianca Tainá Ferreira, Matheus Martins, Fritz Huguenin","doi":"10.1039/d4cp02063d","DOIUrl":"https://doi.org/10.1039/d4cp02063d","url":null,"abstract":"This study aims to investigate the electrochemical behavior of electrodes composed of Nitrogen-Doped TiO2 (TiO2-yNy), iron-nitrogen-carbon (Fe-N-C), and copper hexacyanoferrate (CuHCF) for energy conversion during the neutralization of acidic solutions under visible electromagnetic radiation. The particle size, morphology, and structural properties of these materials were characterized. Time and frequency domain models/methods were employed to determine kinetic parameters and temporal evolution, as well as to propose reaction mechanisms, providing a comprehensive understanding of the processes involved in each half-reaction. In the analysis of the first-order oxygen reduction reaction (ORR) on Fe-N-C electrodes, both direct 4-electron reduction and hydrogen peroxide formation as an intermediate were observed, demonstrating catalytic activity in acidic and dilute saline solutions comparable to those in more concentrated acid solutions. Nitrogen doping of TiO2, which extends the absorption range of electromagnetic radiation to visible light, enabled photoelectrooxidation reactions of water at low potentials, thereby facilitating significant energy conversion/harvesting. CuHCF electrodes demonstrated efficient sodium ion insertion/deinsertion behavior with low practical irreversibility, which is essential for the integration of the half-reactions in the specific full cell designated for energy conversion across different pH values. Under the experimental conditions used, 62.9 kJ per mol of proton produced (or consumed) was obtained. This study provides valuable insights into materials for photo-assisted energy conversion/harvesting in acid wastewater treatment, emphasizing their potential for more efficient and sustainable solutions.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452027","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

Near Equivalence of Polarizability and Bond Flux for Describing Covalent Bond Rearrangements 描述共价键重排的极化性与键通量近乎相等

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-21 DOI: 10.1039/d4cp03337j

Lukas Kim, Teresa Head-Gordon

{"title":"Near Equivalence of Polarizability and Bond Flux for Describing Covalent Bond Rearrangements","authors":"Lukas Kim, Teresa Head-Gordon","doi":"10.1039/d4cp03337j","DOIUrl":"https://doi.org/10.1039/d4cp03337j","url":null,"abstract":"Identification of the breaking point for the chemical bond is essential for our understanding of chemical reactivity. The current consensus is that a point of maximal electron delocalization along the bonding axis separates the different bonding regimes of reactants and products. This maximum transition point has been investigated previously through the total position spread and the bond-parallel components of the static polarizability tensor for describing covalent bond breaking. In this paper, we report that the first-order change of the Wiberg and Mayer bond index with respect to the reaction coordinate, the bond flux, is similarly maximized and is nearly equivalent with the bond breaking points determined by the bond-parallel polarizability. We investigate the similarites and differences between the two bonding metrics for breaking the nitrogen triple bond, twisting around the ethene double bond, and a set of prototypical reactions in the hydrogen combustion reaction network. The Wiberg-Mayer bond flux provides a simpler approach to calculating the point of bond dissociation and formation and can yield greater chemical insight through bond specific information for certain reactions where multiple bond changes are operative.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":null,"pages":null},"PeriodicalIF":3.3,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142452115","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

Machine Learning Accelerating Structure Prediction of PtSnO Nanoclusters under Working Conditions 机器学习加速工作条件下 PtSnO 纳米团簇的结构预测

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-20 DOI: 10.1039/d4cp03769c

Fanke Zeng, Wanglai Cen

引用次数: 0

Extending the Chevrel-type superatoms to nitrogen family 将切弗勒型超原子扩展到氮族

IF 3.3 3区化学

Physical Chemistry Chemical Physics Pub Date : 2024-10-19 DOI: 10.1039/d4cp03580a

Ziyao Yang, Ning Du, Hongshan Chen

引用次数: 0