arXiv - PHYS - Chemical Physics最新文献_第4页

A novel technique based on a cylindrical microwave resonator for high pressure phase equilibrium determination 基于圆柱形微波谐振器的高压相平衡测定新技术

arXiv - PHYS - Chemical Physics Pub Date : 2024-09-12 DOI: arxiv-2409.08144

Rodrigo Susial, Ángel Gómez-Hernández, Daniel Lozano-Martín, Dolores del Campo, M. Carmen Martín, José J. Segovia

{"title":"A novel technique based on a cylindrical microwave resonator for high pressure phase equilibrium determination","authors":"Rodrigo Susial, Ángel Gómez-Hernández, Daniel Lozano-Martín, Dolores del Campo, M. Carmen Martín, José J. Segovia","doi":"arxiv-2409.08144","DOIUrl":"https://doi.org/arxiv-2409.08144","url":null,"abstract":"The development of a novel technique based on a cylindrical microwave\u0000resonator for high pressure phase equilibrium determination is described.\u0000Electric permittivity or dielectric constant is a physical property that\u0000depends on temperature and pressure $epsilon$($p$,$T$). Based on this\u0000property, a measuring technique consisting of a cylindrical resonant cavity\u0000that works in the microwave spectrum has been developed. Equilibrium data of\u0000fluid mixtures are measured at high pressure using a synthetic method, where\u0000phase transition is determined under isothermal conditions due to the change of\u0000the dielectric constant. This technique may be a more accurate alternative to\u0000conventional visual synthetic methods. The technique was validated measuring\u0000pure $CO_{2}$, and phase behaviour was then determined for two binary mixtures\u0000[$CO_{2}$ (0.6) + $CH_{4}$ (0.4)] and [$CO_{2}$ (0.4) + $CH_{4}$ (0.6)],\u0000results for which are presented. These systems are interesting for the study of\u0000biogas-like mixtures. In addition, data were compared with the equation of\u0000state used for natural gas GERG-2008, and also, they were modelled using\u0000Peng-Robinson equation of state and Wong-Sandler mixing rules, which are widely\u0000employed in chemical industries and which give good results.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142190243","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Strong anharmonicity dictates ultralow thermal conductivities of type-I clathrates 强非谐波性决定了 I 型凝块的超低导热率

arXiv - PHYS - Chemical Physics Pub Date : 2024-09-12 DOI: arxiv-2409.08242

Dipti Jasrasaria, Timothy C. Berkelbach

引用次数: 0

Elliptical Silicon Nanowire Covered by the SEI in a 2D Chemo-Mechanical Simulation 二维化学机械模拟中被 SEI 覆盖的椭圆形硅纳米线

arXiv - PHYS - Chemical Physics Pub Date : 2024-09-12 DOI: arxiv-2409.07991

Raphael Schoof, Lukas Köbbing, Arnulf Latz, Birger Horstmann, Willy Dörfler

{"title":"Elliptical Silicon Nanowire Covered by the SEI in a 2D Chemo-Mechanical Simulation","authors":"Raphael Schoof, Lukas Köbbing, Arnulf Latz, Birger Horstmann, Willy Dörfler","doi":"arxiv-2409.07991","DOIUrl":"https://doi.org/arxiv-2409.07991","url":null,"abstract":"Understanding the mechanical interplay between silicon anodes and their\u0000surrounding solid-electrolyte interphase (SEI) is essential to improve the next\u0000generation of lithium-ion batteries. We model and simulate a 2D elliptical\u0000silicon nanowire with SEI via a thermodynamically consistent chemo-mechanical\u0000continuum ansatz using a higher order finite element method in combination with\u0000a variable-step, variable-order time integration scheme. Considering a soft\u0000viscoplastic SEI for three half cycles, we see at the minor half-axis the\u0000largest stress magnitude at the silicon nanowire surface, leading to a\u0000concentration anomaly. This anomaly is caused by the shape of the nanowire\u0000itself and not by the SEI. Also for the tangential stress of the SEI, the\u0000largest stress magnitudes are at this point, which can lead to SEI fracture.\u0000However, for a stiff SEI, the largest stress magnitude inside the nanowire\u0000occurs at the major half-axis, causing a reduced concentration distribution in\u0000this area. The largest tangential stress of the SEI is still at the minor\u0000half-axis. In total, we demonstrate the importance of considering the mechanics\u0000of the anode and SEI in silicon anode simulations and encourage further\u0000numerical and model improvements.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142190247","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Speeds of sound for ($CH_{4}$ + $He$) mixtures from $p$ = (0.5 to 20) MPa at $T$ = (273.16 to 375) K 在 $T$ = (273.16 至 375) K 条件下，p$ = (0.5 至 20) MPa 的 ($CH_{4}$ + $He$) 混合物的声速

arXiv - PHYS - Chemical Physics Pub Date : 2024-09-12 DOI: arxiv-2409.08128

Daniel Lozano-Martín, Andres Rojo, M. Carmen Martín, David Vega-Maza, José Juan Segovia

{"title":"Speeds of sound for ($CH_{4}$ + $He$) mixtures from $p$ = (0.5 to 20) MPa at $T$ = (273.16 to 375) K","authors":"Daniel Lozano-Martín, Andres Rojo, M. Carmen Martín, David Vega-Maza, José Juan Segovia","doi":"arxiv-2409.08128","DOIUrl":"https://doi.org/arxiv-2409.08128","url":null,"abstract":"This work aims to provide accurate and wide-ranging experimental new speed of\u0000sound data $w$($p$,$T$) of two binary ($CH_{4}$ + $He$) mixtures at a nominal\u0000helium content of 5% and 10% at pressures $p$ = (0.5 up to 20) MPa and\u0000temperatures $T$ = (273.16, 300, 325, 350 and 375) K. For this purpose, the\u0000most accurate technique for determining speed of sound in gas phase has been\u0000used: the spherical acoustic resonator. Speed of sound is determined with an\u0000overall relative expanded ($k$ = 2) uncertainty of 230 parts in $10^{6}$ and\u0000compared to reference models for multicomponent natural gas-like mixtures:\u0000AGA8-DC92 and GERG-2008 equations of state. Relative deviations of experimental\u0000data from model estimations are outside the experimental uncertainty limit,\u0000although all points are mostly within the AGA uncertainty of 0.2% and GERG\u0000uncertainty of 0.5% and worsen as the helium content increases. Absolute\u0000average deviations are better than 0.45% for GERG and below 0.14% for AGA\u0000models in (0.95 $CH_{4}$ + 0.05 $He$) mixture and below 0.83% for GERG and\u0000within 0.22% for AGA equations in (0.90 $CH_{4}$ + 0.10 $He$) mixture.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142190246","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Applying Multi-Fidelity Bayesian Optimization in Chemistry: Open Challenges and Major Considerations 在化学中应用多保真贝叶斯优化：公开挑战和主要考虑因素

arXiv - PHYS - Chemical Physics Pub Date : 2024-09-11 DOI: arxiv-2409.07190

Edmund Judge, Mohammed Azzouzi, Austin M. Mroz, Antonio del Rio Chanona, Kim E. Jelfs

引用次数: 0

Water Desalination by Ferroelectric Nanoparticles 利用铁电纳米粒子进行海水淡化

arXiv - PHYS - Chemical Physics Pub Date : 2024-09-11 DOI: arxiv-2409.07318

Sergei V. Kalinin, Eugene A. Eliseev, Anna N. Morozovska

引用次数: 0

Flow is slow at the nanoscale: Revisiting the Green-Kubo relation for friction 在纳米尺度上流动缓慢：重新审视摩擦的格林-久保关系

arXiv - PHYS - Chemical Physics Pub Date : 2024-09-11 DOI: arxiv-2409.07134

Anna T. Bui, Stephen J. Cox

{"title":"Flow is slow at the nanoscale: Revisiting the Green-Kubo relation for friction","authors":"Anna T. Bui, Stephen J. Cox","doi":"arxiv-2409.07134","DOIUrl":"https://doi.org/arxiv-2409.07134","url":null,"abstract":"A central aim of statistical mechanics is to establish connections between a\u0000system's microscopic fluctuations and its macroscopic response to a\u0000perturbation. For non-equilibrium transport properties, this amounts to\u0000establishing Green-Kubo (GK) relationships. In hydrodynamics, relating such GK\u0000expressions for liquid-solid friction to macroscopic slip boundary conditions\u0000has remained a long-standing problem due to two challenges: (i) The GK running\u0000integral of the force autocorrelation function decays to zero rather than\u0000reaching a well-defined plateau value; and (ii) debates persist on whether such\u0000a transport coefficient measures an intrinsic interfacial friction or an\u0000effective friction in the system. Inspired by ideas from the coarse-graining\u0000community, we derive a GK relation for liquid-solid friction where the force\u0000autocorrelation is sampled with a constraint of momentum conservation in the\u0000liquid. Our expression does not suffer from the \"plateau problem\" and\u0000unambiguously measures an effective friction coefficient, in an analogous\u0000manner to Stokes' law. We further establish a link between the derived friction\u0000coefficient and the hydrodynamic slip length, enabling a straightforward\u0000assessment of continuum hydrodynamics across length scales. We find that\u0000continuum hydrodynamics describes the simulation results quantitatively for\u0000confinement length all the way down to 1 nm. Our results also make clear that\u0000water flow under nano-confinement is orders of magnitude slower compared to the\u0000macroscopic case. Our approach amounts to a straightforward modification to the\u0000present standard method of quantifying interfacial friction from molecular\u0000simulations, making possible a sensible comparison between surfaces of vastly\u0000different slippage.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142224809","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Diverse Transient Chiral Dynamics in Evolutionary distinct Photosynthetic Reaction Centers 进化过程中不同光合作用反应中心的多种瞬态手性动力学特征

arXiv - PHYS - Chemical Physics Pub Date : 2024-09-11 DOI: arxiv-2409.06996

Yonglei Yang, Zihui Liu, Fulu Zheng, Panpan Zhang, Hongxing He, Ajay Jha, Hong-Guang Duan

引用次数: 0

Determination of the force transmission error in a single-sinker magnetic suspension densimeter due to the fluid-specific effect and its correction for use with gas mixtures containing oxygen 确定单沉降片磁悬浮密度计因流体特异性效应而产生的力传递误差，并对其在含氧混合气体中的使用进行修正

arXiv - PHYS - Chemical Physics Pub Date : 2024-09-11 DOI: arxiv-2409.07140

Daniel Lozano-Martín, María E. Mondéjar, José J. Segovia, César R. Chamorro

引用次数: 0

Ionization energy: sd transfer error and Perdew-Zunger self-interaction correction energy penalty in 3d atoms 电离能：3d 原子中的 sd 转移误差和 Perdew-Zunger 自相互作用修正能量惩罚

arXiv - PHYS - Chemical Physics Pub Date : 2024-09-11 DOI: arxiv-2409.07438

Rohan Maniar, Priyanka B. Shukla, J. Karl Johnson, Koblar A. Jackson, John P. Perdew

{"title":"Ionization energy: sd transfer error and Perdew-Zunger self-interaction correction energy penalty in 3d atoms","authors":"Rohan Maniar, Priyanka B. Shukla, J. Karl Johnson, Koblar A. Jackson, John P. Perdew","doi":"arxiv-2409.07438","DOIUrl":"https://doi.org/arxiv-2409.07438","url":null,"abstract":"To accurately describe the energetics of transition metal systems, density\u0000functional approximations (DFAs) must provide a balanced description of s- and\u0000d- electrons. One measure of this is the sd transfer error, which has\u0000previously been defined as $E(mathrm{3d}^{n-1} mathrm{4s}^1)\u0000-E(mathrm{3d}^{n-2} mathrm{4s}^2)$. Theoretical concerns have been raised on\u0000the validity of these results owing to the evaluation of excited-state energies\u0000using ground-state DFAs. A more serious concern appears to be strong\u0000correlations in the $mathrm{4s}^2$ configuration. Here we define a\u0000ground-state measure of the sd transfer error, based on the errors of s- and\u0000d-electron second ionization energies of the atoms, that effectively\u0000circumvents the aforementioned problems. We find an improved performance as we\u0000move from LSDA to PBE to r$^2$SCAN for first-row transition metal atoms.\u0000However, we found large (~ 2 eV) ground-state sd transfer errors when applying\u0000a Perdew-Zunger self-interaction correction. This is attributed to an \"energy\u0000penalty\" associated with the noded 3d orbitals. A local scaling of the\u0000self-interaction correction to LSDA results in a cancellation of s- and\u0000d-errors.","PeriodicalId":501304,"journal":{"name":"arXiv - PHYS - Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142190248","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0