相关论文: Charge Transfer Kinetics at the Solid-Solid Interf…
We reformulate and extend porous electrode theory for non-ideal active materials, including those capable of phase transformations. Using principles of non-equilibrium thermodynamics, we relate the cell voltage, ionic fluxes, and Faradaic…
Outer sphere electron transfer rates can be calculated from simulation data by sampling the equilibrium statistics of the canonical reaction coordinate -- the vertical energy gap. For these calculations, electron transfer is typically…
The Marcus-Hush-Chidsey (MHC) model is well known in electro-analytical chemistry as a successful microscopic theory of outer-sphere electron transfer at metal electrodes, but it is unfamiliar and rarely used in electrochemical engineering.…
The microscopic theory of chemical reactions is based on transition state theory, where atoms or ions transfer classically over an energy barrier, as electrons maintain their ground state. Electron transfer is fundamentally different and…
Electrodeposition and stripping are fundamental electrochemical processes for metals and have gained importance in rechargeable Li-ion batteries due to lithium metal electrodes. The electrode kinetics associated with lithium metal…
A kinetic model of the electron transfer at the electrode / electrolyte solution interface is developed, implemented in a Monte Carlo framework, and applied to simulate this process in idealised systems consisting of the primitive model of…
Electrochemical kinetics at electrode-electrolyte interfaces limit performance of devices including fuel cells and batteries. While the importance of moving beyond Butler-Volmer kinetics and incorporating the effect of electronic density of…
We couple the Leaky Membrane Model, which describes the diffusion and electromigration of ions in a homogenized porous medium of fixed background charge, with Butler-Volmer reaction kinetics for flat electrodes separated by such a medium in…
Starting from the Boltzmann-Enskog kinetic equations, the charge transport equation for bidisperse granular flows with contact electrification is derived with separate mean velocities, total kinetic energies, charges and charge variances…
Recent theoretical advances, based on a combination of concepts from Thouless' topological theory of adiabatic charge transport and a newly introduced gauge-invariance principle for transport coefficients, have permitted to connect (and…
Porous electrode theory, pioneered by John Newman and collaborators, provides a useful macroscopic description of battery cycling behavior, rooted in microscopic physical models rather than empirical circuit approximations. The theory…
Porous electrodes composed of multiphase active materials are widely used in Li-ion batteries, but their dynamics are poorly understood. Two-phase models are largely empirical, and no models exist for three or more phases. Using a modified…
Molecular conduction operating in dielectric solvent environments are often described using kinetic rates based on Marcus theory of electron transfer at a molecule-metal electrode interface. However, the successive nature of charge transfer…
The rate of electron transfer between a molecular species and a metal, each at a different local temperature, is examined theoretically through implementation of a bithermal (characterized by two temperatures) Marcus formalism. Expressions…
Hybrid interfaces formed by inorganic semiconductors and organic molecules are intriguing materials for opto-electronics. Interfacial charge transfer is primarily responsible for their peculiar electronic structure and optical response.…
Porous electrodes are a vital component of redox flow batteries, fuel cells and electrolyzers. We present a 3D digital twin for a porous electrode by direct numerical solution of the governing Navier-Stokes and Nernst-Planck equations for…
Density Functional Theory (DFT) calculations of electrode material properties in high energy density storage devices like lithium batteries have been standard practice for decades. In contrast, DFT modelling of explicit interfaces in…
Marcus theory is fundamental to describing electron transfer reactions and quantifying their rates, effectively representing the energy surface associated with an electron transfer from the reactant to the product ionic state via parabolas…
Charge transfer is a fundamental process that underlies a multitude of phenomena in chemistry and biology. Recent advances in observing and manipulating charge and heat transport at the nanoscale, and recently developed techniques for…
We investigate the subtle effects of diffuse charge on interfacial kinetics by solving the governing equations for ion transport (Nernst-Planck) with realistic boundary conditions representing reaction kinetics (Butler-Volmer) and…