The effect of temperature on the kinetics of electrochemical insertion/removal of lithium in graphite is analyzed by kinetic Monte Carlo methods. Different electrochemical techniques are simulated at different temperatures and responses are compared with experimental results. Simulated voltammograms show, similarly to experiment, how the behavior of the system becomes closer to equilibrium as temperature increases. Calculated chronoamperometric profiles show a different qualitative behavior in the current at different temperatures, especially in the Cottrell representation peaks, explained in terms of the relative importance of diffusive versus charge transfer processes at different temperatures. Results at room temperature are in good agreement with experiment, and we further evaluate trends at elevated temperature that have not yet been described in experimental or theoretical works. Exchange current densities for different degrees of lithium intercalation at different temperatures are predicted using potentiostatic simulations, showing an Arrhenius-type relationship. The dependence of the exchange current on electrolyte composition is simulated by investigating the effect of different activation energy barriers at different temperatures. The influence of temperature on diffusion coefficients as a function of lithiation fraction in graphite is simulated and related to Arrhenius plots, explaining the experimentally observed changes in diffusion phenomena with lithium composition and temperature.

A computational model is proposed to study lithium-graphite intercalation compounds in the framework of Monte Carlo simulations in the Gran Canonical Ensemble. The results suggest the existence of fractional stages between stages II and I, which are rarely found in most experimental electrochemical measurements. These fractional stages seem to be part of a more general intercalation mechanism suggested for other intercalation compounds. The thermodynamic information obtained from the simulations for these fractional states at room temperature is discussed in the context of experimental data. In addition, clear evidence was found for the existence of a new stage, supported by recent experimental measurements.

In the present work, we study the adsorption of different monomolecular species on nanoparticles with different sizes and geometries using a grand canonical Monte Carlo method. These species are characterized by repulsive lateral interactions between themselves, as takes place in the case of the adsorption of partially charged atoms or molecules. Nanosize effects are analyzed in terms of adsorption on edge and facet sites. The energy minimization in these systems comes out as a complex conjugation of the repulsive lateral interactions between the adsorbates and the attractive interactions of the adsorbates with the nanoparticle. The phenomenon is analyzed as a function of the occurrence of different ordered structures being formed on the surface of the nanoparticle. We find that layers with different structures may coexist on different facets of the nanoparticle. Finally, a discussion of deposition on flat surfaces and in finite systems is given.

By including a parametric description of the elastic interactions using Monte Carlo simulations, the transition between stages II and I takes place without the presence of fractional stages.