Oihana Galparsoro, Raidel Martin Barrios, Paulo Enrique Ibáñez Almaguer, Maykel Marquez Mijares, José David Cremé, Yosvany Silva Solís, Jesus Rubayo-Soneira, Cedric Crespos, P. Larregaray
Molecular dynamics simulations are performed to investigate the influence of isotope substitutions in Eley-Rideal recombination dynamics of hydrogen isotopes from the (100) and (110) surfaces of tungsten. Dissipation to electrons and phonons is taken into account by respectively the Local Density Friction Approximation and the General Langevin Oscillator, effective models which have been intensively used in the recent years. As the coupling to surface phonons and electrons might be altered by the mass combination, the main objective of the paper is to assess the role of dissipation to the surface in the course of abstraction. It has been observed that the mass of the projectile is the main determinant of the competence of the energy dissipation channels.
{"title":"Isotope effects in Eley-Rideal abstraction of Hydrogen from Tungsten surfaces: the role of dissipation.","authors":"Oihana Galparsoro, Raidel Martin Barrios, Paulo Enrique Ibáñez Almaguer, Maykel Marquez Mijares, José David Cremé, Yosvany Silva Solís, Jesus Rubayo-Soneira, Cedric Crespos, P. Larregaray","doi":"10.1039/d4cp04063e","DOIUrl":"https://doi.org/10.1039/d4cp04063e","url":null,"abstract":"Molecular dynamics simulations are performed to investigate the influence of isotope substitutions in Eley-Rideal recombination dynamics of hydrogen isotopes from the (100) and (110) surfaces of tungsten. Dissipation to electrons and phonons is taken into account by respectively the Local Density Friction Approximation and the General Langevin Oscillator, effective models which have been intensively used in the recent years. As the coupling to surface phonons and electrons might be altered by the mass combination, the main objective of the paper is to assess the role of dissipation to the surface in the course of abstraction. It has been observed that the mass of the projectile is the main determinant of the competence of the energy dissipation channels.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"21 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142929098","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}
Yashasvi Naik, Disha Mehta, Hardip R Mahida, Riddhi Desai, Pankaj B. Thakor
The application of 2D material for detecting dissolved gas molecules is essential for identifying faults in oil-immersed transformers. This study investigates the adsorption properties of ZrCl2 monolayer (ML) and pd-doped ZrCl2 ML with six gas molecules (CO, CO2, CH4, C2H2, C2H4, C2H6) in transformer oil using Density Functional Approach. The adsorption behaviour was analysed by calculating and comparing the structures, charge transfer and adsorption energies. Additionally, the chemical interaction and electronic properties of gas molecules on ZrCl2/Pd-ZrCl2 ML are examined through PDOS (Projected Density of States), band structure, recovery time and work function. The pristine ZrCl2 ML has a weak interaction for all six gas molecules, whereas Pd doping on ZrCl2 ML has considerably increased the adsorption strength for C2H4, CO and C2H2 gases. The results presented in this paper offer a theoretical framework for utilizing Pd-ZrCl2 ML in monitoring transformer performance and gas detection.
{"title":"DFT Study of Pd-doped ZrCl2: A Promising Solution for Dissolved Gas Molecules Analysis in Transformer Oil","authors":"Yashasvi Naik, Disha Mehta, Hardip R Mahida, Riddhi Desai, Pankaj B. Thakor","doi":"10.1039/d4cp04151h","DOIUrl":"https://doi.org/10.1039/d4cp04151h","url":null,"abstract":"The application of 2D material for detecting dissolved gas molecules is essential for identifying faults in oil-immersed transformers. This study investigates the adsorption properties of ZrCl2 monolayer (ML) and pd-doped ZrCl2 ML with six gas molecules (CO, CO2, CH4, C2H2, C2H4, C2H6) in transformer oil using Density Functional Approach. The adsorption behaviour was analysed by calculating and comparing the structures, charge transfer and adsorption energies. Additionally, the chemical interaction and electronic properties of gas molecules on ZrCl2/Pd-ZrCl2 ML are examined through PDOS (Projected Density of States), band structure, recovery time and work function. The pristine ZrCl2 ML has a weak interaction for all six gas molecules, whereas Pd doping on ZrCl2 ML has considerably increased the adsorption strength for C2H4, CO and C2H2 gases. The results presented in this paper offer a theoretical framework for utilizing Pd-ZrCl2 ML in monitoring transformer performance and gas detection.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"34 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142917385","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}
Carbonless DNA was designed by replacing all carbon atoms in the standard DNA building blocks with boron and nitrogen, ensuring isoelectronicity. Electronic structure quantum chemistry methods (DFT(ωB97XD)/aug-cc-pVDZ) were employed to study both the individual building blocks and the larger carbon-free DNA fragments. The reliability of the results was validated by comparing selected structures and binding energies using more accurate methods such as MP2, CCSD, and SAPT2+3(CCD)δMP2. Carbonless analogs of DNA components, including cytosine, thymine, guanine, adenine, and deoxyribose, were investigated, showing strong resemblance to the carbon-based versions in terms of spatial structure, polarity, and molecular interaction capabilities. Complementary base pairs of the carbonless analogs exhibited a similar number and length of hydrogen bonds as those found in their carbon-containing counterparts, with binding energies for A-T and G-C analogs remaining comparable. Carbonless DNA fragments containing two and six base pairs were studied, revealing double-helix structures analogous to natural DNA. Structural parameters such as fragment size, hydrogen bond lengths, and rise per base pair were consistent with those observed in unmodified DNA. Docking simulations with a 12 base pair fragment and netropsin as a ligand indicated a slight shift in binding preference for the carbonless DNA through the minor groove, with an approximate 25% increase in binding affinity compared to natural DNA.
{"title":"Carbonless DNA","authors":"Piotr Skurski, Jakub Brzeski","doi":"10.1039/d4cp04410j","DOIUrl":"https://doi.org/10.1039/d4cp04410j","url":null,"abstract":"Carbonless DNA was designed by replacing all carbon atoms in the standard DNA building blocks with boron and nitrogen, ensuring isoelectronicity. Electronic structure quantum chemistry methods (DFT(ωB97XD)/aug-cc-pVDZ) were employed to study both the individual building blocks and the larger carbon-free DNA fragments. The reliability of the results was validated by comparing selected structures and binding energies using more accurate methods such as MP2, CCSD, and SAPT2+3(CCD)δMP2. Carbonless analogs of DNA components, including cytosine, thymine, guanine, adenine, and deoxyribose, were investigated, showing strong resemblance to the carbon-based versions in terms of spatial structure, polarity, and molecular interaction capabilities. Complementary base pairs of the carbonless analogs exhibited a similar number and length of hydrogen bonds as those found in their carbon-containing counterparts, with binding energies for A-T and G-C analogs remaining comparable. Carbonless DNA fragments containing two and six base pairs were studied, revealing double-helix structures analogous to natural DNA. Structural parameters such as fragment size, hydrogen bond lengths, and rise per base pair were consistent with those observed in unmodified DNA. Docking simulations with a 12 base pair fragment and netropsin as a ligand indicated a slight shift in binding preference for the carbonless DNA through the minor groove, with an approximate 25% increase in binding affinity compared to natural DNA.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"34 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142917732","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}
Tarik Ouahrani, Ali Esquembre Kučukalić, Boufatah Reda, Angel Morales-Garcia, Daniel Errandonea
The production of hydrogen (H2 ) fuel through electrocatalysis is emerging as a sustainable alternative to conventional and environmentally harmful energy sources. However, the discovery of cost-effective and efficient materials for this purpose remains a significant challenge. In this study, we explore the potential of the transition-metal-substituted Y2 NS2 MXene as a promising candidate for hydrogen production through the hydrogen evolution reaction (HER). Using density functional theory (DFT) calculations, we first analyzed the Pourbaix diagram, and dissolution potential which showed the stability and resistance to corrosion of the sulfur termination. Later, we address the kinetic limitations of HER on bare Y2 NS2 by introducing single-atom substitutions of Y atoms with 3d transition metals. Nine distinct structures were evaluated, revealing that Fe-substituted Y2 NS2 exhibits the highest HER activity under acidic conditions, as indicated by volcano plot analyses. Further investigation of the bonding characteristics and electronic density of states highlights the crucial role of Fe d -orbitals and the weak interactions at the sulfur-terminated surface in enhancing the HER efficiency. These findings provide insights into the design of advanced, cost-effective materials for HER catalysis, paving the way for their application as efficient electrochemical catalysts across a wide pH range.
{"title":"Untangling the role of single-atom substitution on the improvement of the hydrogen evolution reaction of Y2NS2 MXene in acidic media","authors":"Tarik Ouahrani, Ali Esquembre Kučukalić, Boufatah Reda, Angel Morales-Garcia, Daniel Errandonea","doi":"10.1039/d4cp03333g","DOIUrl":"https://doi.org/10.1039/d4cp03333g","url":null,"abstract":"The production of hydrogen (H2 ) fuel through electrocatalysis is emerging as a sustainable alternative to conventional and environmentally harmful energy sources. However, the discovery of cost-effective and efficient materials for this purpose remains a significant challenge. In this study, we explore the potential of the transition-metal-substituted Y2 NS2 MXene as a promising candidate for hydrogen production through the hydrogen evolution reaction (HER). Using density functional theory (DFT) calculations, we first analyzed the Pourbaix diagram, and dissolution potential which showed the stability and resistance to corrosion of the sulfur termination. Later, we address the kinetic limitations of HER on bare Y2 NS2 by introducing single-atom substitutions of Y atoms with 3d transition metals. Nine distinct structures were evaluated, revealing that Fe-substituted Y2 NS2 exhibits the highest HER activity under acidic conditions, as indicated by volcano plot analyses. Further investigation of the bonding characteristics and electronic density of states highlights the crucial role of Fe d -orbitals and the weak interactions at the sulfur-terminated surface in enhancing the HER efficiency. These findings provide insights into the design of advanced, cost-effective materials for HER catalysis, paving the way for their application as efficient electrochemical catalysts across a wide pH range.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"160 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142917737","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}
Prithwiraj Das, C. V. Anusree, Sonali S. Pradhan, Kanchana Venkatakrishnan
The topological properties of the A15-type compound Ti3Pd reveal a complex landscape of multi-fold fermionic and bosonic states, as uncovered through ab initio calculations within the framework of Density Functional Theory (DFT). The electronic band structure shows multi-fold degenerate crossings at the high-symmetry point R near the Fermi level, which evolves into 4-fold and 8-fold degenerate fermionic states upon the introduction of spin-orbit coupling (SOC). Likewise, the phononic band structure features multi-fold degenerate bosonic crossings at the same R point. Topological analysis, including the calculation of Z2 invariants and surface states, confirms the non-trivial nature of Ti3Pd. Moreover, both fermionic and bosonic quasiparticles exhibit nodal line features, whose topological non-triviality is further substantiated by Berry phase calculation. This research illuminates the intricate topological framework of Ti3Pd, opening avenues for experimental exploration in the field of topological quantum materials.
{"title":"Multi-fold fermionic and bosonic states in topologically non-trivial Ti3Pd","authors":"Prithwiraj Das, C. V. Anusree, Sonali S. Pradhan, Kanchana Venkatakrishnan","doi":"10.1039/d4cp03768e","DOIUrl":"https://doi.org/10.1039/d4cp03768e","url":null,"abstract":"The topological properties of the A15-type compound Ti<small><sub>3</sub></small>Pd reveal a complex landscape of multi-fold fermionic and bosonic states, as uncovered through ab initio calculations within the framework of Density Functional Theory (DFT). The electronic band structure shows multi-fold degenerate crossings at the high-symmetry point R near the Fermi level, which evolves into 4-fold and 8-fold degenerate fermionic states upon the introduction of spin-orbit coupling (SOC). Likewise, the phononic band structure features multi-fold degenerate bosonic crossings at the same R point. Topological analysis, including the calculation of Z2 invariants and surface states, confirms the non-trivial nature of Ti<small><sub>3</sub></small>Pd. Moreover, both fermionic and bosonic quasiparticles exhibit nodal line features, whose topological non-triviality is further substantiated by Berry phase calculation. This research illuminates the intricate topological framework of Ti<small><sub>3</sub></small>Pd, opening avenues for experimental exploration in the field of topological quantum materials.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"6 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142917383","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}
Alexey A. Rulev, Yevgeniya O. Kondratyeva, Lada V. Yashina, Ilia P. Ivanenko, M. Daniil
Growth of lithium whiskers or dendrites is the major obstacle towards safe and stable utilization of lithium metal anodes in rechargeable batteries. In this study, we look deeper into the mechanism of lithium electrodeposition. We found that before lithium whisker or dendrite nucleation occurs, lithium is deposed into the grain boundaries of the metal electrode, which we directly observed on the focused ion beam cross-sections of the lithium electrode, and the structure of grain boundaries near the surface predetermines the capacity for smooth deposition. We then demonstrate that by reducing the metal grain mean size we can extend whisker- and dendrite-free deposition of lithium. With a eutectic Ga-Li alloy containing only 2.5 atomic percent of gallium we observed morphologically stable lithium deposition for 10 hours. The results demonstrate deep interconnections between the metal microstructure and the whisker growth.
{"title":"Whisker-free lithium electrodeposition by tuning electrode microstructure","authors":"Alexey A. Rulev, Yevgeniya O. Kondratyeva, Lada V. Yashina, Ilia P. Ivanenko, M. Daniil","doi":"10.1039/d4cp02638a","DOIUrl":"https://doi.org/10.1039/d4cp02638a","url":null,"abstract":"Growth of lithium whiskers or dendrites is the major obstacle towards safe and stable utilization of lithium metal anodes in rechargeable batteries. In this study, we look deeper into the mechanism of lithium electrodeposition. We found that before lithium whisker or dendrite nucleation occurs, lithium is deposed into the grain boundaries of the metal electrode, which we directly observed on the focused ion beam cross-sections of the lithium electrode, and the structure of grain boundaries near the surface predetermines the capacity for smooth deposition. We then demonstrate that by reducing the metal grain mean size we can extend whisker- and dendrite-free deposition of lithium. With a eutectic Ga-Li alloy containing only 2.5 atomic percent of gallium we observed morphologically stable lithium deposition for 10 hours. The results demonstrate deep interconnections between the metal microstructure and the whisker growth.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"27 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142917382","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}
Two-dimensional (2D) carbon allotropes, together with their binary and ternary counterparts, have attracted substantial research interests due to their peculiar geometries and properties. Among them, grapheneplus, a derivative of penta-graphene, has been proposed to exhibit unusual mechanical and electronic behaviours. In this work, we perform a comprehensive first-principles study on its isoelectronic and isostructural analogue, a grapheneplus-like BCN (gp-BCN) monolayer. It is found that such gp-BCN system exhibits robust structural stability from the energetic, dynamic, thermal, mechanical perspectives. A remarkable anisotropy is observed in its mechanical behaviours, which even presents in-plane auxeticity with a high negative Poisson’s ratio of -0.3. Different from the semimetallic grapheneplus one, the gp-BCN monolayer is a semiconductor with a direct band gap of 3.23 eV. High electron mobilities up to 103 cm2V-1 s-1 appear in the gp-BCN system, which are one to two orders of magnitude greater than the hole mobilities. Furthermore, due to the breaking of inversion symmetry, the gp-BCN monolayer exhibits a spontaneous out-of-plane polarization, yielding prominent out-of-plane piezoelectric responses that are comparable to those of Janus MoSSe, WSSe and H-decorated BN systems. Our study demonstrates that the BCN analogue of graphene-plus possesses promising mechanical, electronic, and piezoelectric properties, rendering it potential applications in nanoelectronics and mechanical nanosensors.
{"title":"Promising mechanical, electronic and piezoelectric properties of grapheneplus-like BCN monolayer: insights from first-principles","authors":"Jinyuan Liu, Yi Ding, Yanli Wang","doi":"10.1039/d4cp04299a","DOIUrl":"https://doi.org/10.1039/d4cp04299a","url":null,"abstract":"Two-dimensional (2D) carbon allotropes, together with their binary and ternary counterparts, have attracted substantial research interests due to their peculiar geometries and properties. Among them, grapheneplus, a derivative of penta-graphene, has been proposed to exhibit unusual mechanical and electronic behaviours. In this work, we perform a comprehensive first-principles study on its isoelectronic and isostructural analogue, a grapheneplus-like BCN (gp-BCN) monolayer. It is found that such gp-BCN system exhibits robust structural stability from the energetic, dynamic, thermal, mechanical perspectives. A remarkable anisotropy is observed in its mechanical behaviours, which even presents in-plane auxeticity with a high negative Poisson’s ratio of -0.3. Different from the semimetallic grapheneplus one, the gp-BCN monolayer is a semiconductor with a direct band gap of 3.23 eV. High electron mobilities up to 10<small><sup>3</sup></small> cm<small><sup>2</sup></small>V<small><sup>-1</sup></small> s<small><sup>-1</sup></small> appear in the gp-BCN system, which are one to two orders of magnitude greater than the hole mobilities. Furthermore, due to the breaking of inversion symmetry, the gp-BCN monolayer exhibits a spontaneous out-of-plane polarization, yielding prominent out-of-plane piezoelectric responses that are comparable to those of Janus MoSSe, WSSe and H-decorated BN systems. Our study demonstrates that the BCN analogue of graphene-plus possesses promising mechanical, electronic, and piezoelectric properties, rendering it potential applications in nanoelectronics and mechanical nanosensors.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"115 3 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142917739","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}
Molecular force field (FF) determines the accuracy of molecular dynamics (MD) and is one of the major bottlenecks that limits the application of MD in molecular design. Recently, artificial intelligence (AI) techniques, such as machine-learning potentials (MLPs), are rapidly reshaping the landscape of MD. Meanwhile, organic molecular systems feature unique characteristics, requiring more careful treatment in both model construction, optimization, and validation. While an accurate and generic organic molecular force field is still missing, significant progress has been made with the facilitation of AI, warranting a promising future. In this review, we overview the various types of AI techniques used in molecular FF development and discuss both the advantages and weaknesses of these methodologies. We show that how AI methods give us unprecedented capabilities in many tasks such as potential fitting, atom typification, and automatic optimization. Meanwhile, it is also worth noting that more efforts are needed to improve the transferability of the model, develop more comprehensive database, and establish more standardized validation procedures. With these discussions, we hope to inspire more efforts to solve the existing problems, eventually leading to the birth of next-generation generic organic FFs.
{"title":"Application of Modern Artificial Intelligence Techniques in the Development of Organic Molecular Force Fields","authors":"Junmin Chen, Qian Gao, Miaofei Huang, Kuang Yu","doi":"10.1039/d4cp02989e","DOIUrl":"https://doi.org/10.1039/d4cp02989e","url":null,"abstract":"Molecular force field (FF) determines the accuracy of molecular dynamics (MD) and is one of the major bottlenecks that limits the application of MD in molecular design. Recently, artificial intelligence (AI) techniques, such as machine-learning potentials (MLPs), are rapidly reshaping the landscape of MD. Meanwhile, organic molecular systems feature unique characteristics, requiring more careful treatment in both model construction, optimization, and validation. While an accurate and generic organic molecular force field is still missing, significant progress has been made with the facilitation of AI, warranting a promising future. In this review, we overview the various types of AI techniques used in molecular FF development and discuss both the advantages and weaknesses of these methodologies. We show that how AI methods give us unprecedented capabilities in many tasks such as potential fitting, atom typification, and automatic optimization. Meanwhile, it is also worth noting that more efforts are needed to improve the transferability of the model, develop more comprehensive database, and establish more standardized validation procedures. With these discussions, we hope to inspire more efforts to solve the existing problems, eventually leading to the birth of next-generation generic organic FFs.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"13 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142917738","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}
The search for new anode materials with high lithium-ion battery (LIB) capacity has attracted considerable attention due to the increasing need for electrical power. Here, we utilized first-principles calculations to develop a honeycomb-structured B2C3N monolayer, which exhibits an ultra-high Li-ion storage capacity of 2,244 mA h g-1 as an anode material for LIBs. Furthermore, the calculations show that the B2C3N monolayer has a comparatively small diffusion barrier of 0.352 eV and a low open-circuit voltage of 0.134 V. The stability of B2C3N has been verified by analyzing phonon dispersion curves, conducting molecular dynamics simulations, and examining elastic constants. We have found an ultra-high capacity and efficient anode material through theoretical design, which provides theoretical reference for responding to the global energy crisis and promoting clean energy transformation.
{"title":"B2C3N monolayer with high theoretical capacity as anode materials for Lithium-ion batteries: A first-principles calculations","authors":"Yutong Zou, Yaqi She, Liuxu Zhao, Ailing Liu, Bo Sun, Yuhong Jiang, Chunlei Kou, Miao Zhang, Yuanye Tian","doi":"10.1039/d4cp03717k","DOIUrl":"https://doi.org/10.1039/d4cp03717k","url":null,"abstract":"The search for new anode materials with high lithium-ion battery (LIB) capacity has attracted considerable attention due to the increasing need for electrical power. Here, we utilized first-principles calculations to develop a honeycomb-structured B2C3N monolayer, which exhibits an ultra-high Li-ion storage capacity of 2,244 mA h g-1 as an anode material for LIBs. Furthermore, the calculations show that the B2C3N monolayer has a comparatively small diffusion barrier of 0.352 eV and a low open-circuit voltage of 0.134 V. The stability of B2C3N has been verified by analyzing phonon dispersion curves, conducting molecular dynamics simulations, and examining elastic constants. We have found an ultra-high capacity and efficient anode material through theoretical design, which provides theoretical reference for responding to the global energy crisis and promoting clean energy transformation.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"4 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142917740","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}
The function of biomolecular systems, including biological macromolecules, often crucially depends on their dynamics. Nuclear Magnetic Resonance (NMR) is one of the most informative methods used to study biomolecules and their internal mobility, with atomic resolution, in near-physiological conditions. NMR relaxation profiles, obtained from the field dependence of the nuclear relaxation rates, in particular, offer the possibility to probe dynamic processes over a wide range of time scales. Relaxation profiles are routinely acquired using field-cycling relaxometers operating at a maximum field of the order of 1 T. These measurements however suffer from a lack of resolution. On the other hand, relaxation rates measured at the high magnetic fields ( > 4 T) of high resolution NMR spectrometers contain poor information on motions on timescales longer than few nanoseconds. The possibility to acquire relaxation profiles extended to low fields but with high resolution, obtained by shuttling the sample back and forth in the stray field of a high-field spectrometer, is expected to dramatically improve the potentialities of NMR relaxometry. Here, we review investigations of relaxometry in a wide range of biomolecular systems, such as proteins, phospholipids, or biological fluids. Although multiple models of motions have been developed to describe the relaxation rates and their field dependence, most experimental investigations rely on the model-free approach. A variety of relaxation profiles of both diamagnetic and paramagnetic biomolecular systems are here reviewed and analysed using point dipole-point dipole interaction models.
{"title":"Field-dependent relaxation profiles of biomolecular systems","authors":"Adam Kubrak, Rajka Pejanovic, Kahinga Kamau, Danuta Kruk, Fabien Ferrage, Giacomo Parigi","doi":"10.1039/d4cp04306e","DOIUrl":"https://doi.org/10.1039/d4cp04306e","url":null,"abstract":"The function of biomolecular systems, including biological macromolecules, often crucially depends on their dynamics. Nuclear Magnetic Resonance (NMR) is one of the most informative methods used to study biomolecules and their internal mobility, with atomic resolution, in near-physiological conditions. NMR relaxation profiles, obtained from the field dependence of the nuclear relaxation rates, in particular, offer the possibility to probe dynamic processes over a wide range of time scales. Relaxation profiles are routinely acquired using field-cycling relaxometers operating at a maximum field of the order of 1 T. These measurements however suffer from a lack of resolution. On the other hand, relaxation rates measured at the high magnetic fields ( > 4 T) of high resolution NMR spectrometers contain poor information on motions on timescales longer than few nanoseconds. The possibility to acquire relaxation profiles extended to low fields but with high resolution, obtained by shuttling the sample back and forth in the stray field of a high-field spectrometer, is expected to dramatically improve the potentialities of NMR relaxometry. Here, we review investigations of relaxometry in a wide range of biomolecular systems, such as proteins, phospholipids, or biological fluids. Although multiple models of motions have been developed to describe the relaxation rates and their field dependence, most experimental investigations rely on the model-free approach. A variety of relaxation profiles of both diamagnetic and paramagnetic biomolecular systems are here reviewed and analysed using point dipole-point dipole interaction models.","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":"34 1","pages":""},"PeriodicalIF":3.3,"publicationDate":"2025-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142917835","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}
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