arXiv subjects

Anouar Belhboub

Publications and source records attributed to Anouar Belhboub.

4 recordsLinked to original sources

arXiv2026

Reactive Force Field for P/Sn/I System: Atomistic Insight into the Early Stage of Black Phosphorus and Phosphorene Synthesis Process

Black phosphorus and its two dimensional counterpart, phosphorene, are typically synthesized through chemical vapor transport using Sn and I2 additives. Chemical vapor deposition synthesis of phosphorene and allotropes is still yet not well understood. Investigating the atomistic mechanisms underlying phosphorus transport and early stage processes is difficult experimentally. In this study, a reactive force field for the PSnI system was developed and applied using ReaxFF based molecular dynamics to explore the early stage phase of the pre nucleation relevant to BP-phosphorene growth. The force field parameters were trained on a comprehensive quantum mechanical dataset covering bond dissociation, angle and torsion profiles, and tin condensed phase equation of state and cluster formation energies, showing strong agreement in both gas and condensed phases. We demonstrate that iodine and density together control phosphorus recombination. Under low density, atomic phosphorus dominates with minimal clustering. Adding I2 greatly increases P-P recombination, promotes the formation of PxIy motifs, and transient SnxPyIz compounds. Higher density systems favor the formation of larger Px clusters and support the development of ternary SnxPyIz compounds that grow by capturing transported phosphorus. At the highest density, the system produces condensed, Hittorf like phosphorus structures at the edges of SnxPyIz clusters, along with BP-like hexagons stabilized by iodine that may act as nucleation seeds. These results offer an atomistic view of transport and early stage steps in BP synthesis and provide a practical reactive model for studying growth conditions and additive effects in BP phosphorene vapor synthesis.

cond-mat.mes-hall↗

arXiv2021

Mesoscopic simulations of the in situ NMR spectra of porous carbon based supercapacitors: Electronic structure and adsorbent reorganisation effects

In situ NMR spectroscopy is a powerful technique to investigate charge storage mechanisms in carbon-based supercapacitors thanks to its ability to distinguish ionic and molecular species adsorbed in the porous electrodes from those in the bulk electrolyte. The NMR peak corresponding to the adsorbed species shows a clear change of chemical shift as the applied potential difference is varied. This variation in chemical shift is thought to originate from a combination of ion reorganisation in the pores and changes in ring current shifts due to the changes of electronic density in the carbon. While previous Density Functional Theory calculations suggested that the electronic density has a large effect, the relative contributions of these two effects is challenging to untangle. Here, we use mesoscopic simulations to simulate NMR spectra and investigate the relative importance of ion reorganisation and ring currents on the resulting chemical shift. The model is able to predict chemical shifts in good agreement with NMR experiments and indicates that the ring currents are the dominant contribution. A thorough analysis of a specific electrode/electrolyte combination for which detailed NMR experiments have been reported allows us to confirm that local ion reorganisation has a very limited effect but the relative quantities of ions in pores of different sizes, which can change upon charging/discharging, can lead to a significant effect. Our findings suggest that in situ NMR spectra of supercapacitors may provide insights into the electronic structure of carbon materials in the future.

cond-mat.mtrl-sci↗

arXiv2020

Ionic liquids under confinement: From systematic variations of the ion and pore sizes towards an understanding of structure and dynamics in complex porous carbons

We use molecular simulations of an ionic liquid in contact with a range of nanoporous carbons to investigate correlations between ion size, pore size, pore topology and properties of the adsorbed ions. We show that diffusion coefficients increase with the anion size and, surprisingly, with the quantity of adsorbed ions. Both findings are interpreted in terms of confinement: when the in-pore population increases additional ions are located in less confined sites and diffuse faster. Simulations in which the pores are enlarged while keeping the topology constant comfort these observations. The interpretation of properties across structures is more challenging. An interesting point is that smaller pores do not necessarily lead to larger confinement. In this work, the highest degrees of confinements are observed for intermediate pore sizes. We also show a correlation between the quantity of adsorbed ions and the ratio between the maximum pore diameter and the pore limiting diameter.

cond-mat.mtrl-sci↗

arXiv2019

On the development of an original mesoscopic model to predict the capacitive properties of carbon-carbon supercapacitors

We report on the development of an original mesoscopic lattice model to predict structural, dynamical and capacitive properties of carbon-carbon supercapacitors. The model uses input from molecular simulations, such as free energy profiles to describe the ion adsorption, and experiments, such as energy barriers for transitions between lattice sites. The model developed is approximately 10,000 times faster than common molecular simulations. We apply this model to a set of carbon structures with well-defined pore sizes and investigate the solvation effect by doing simulations with neat ionic liquids as well as acetonitrile-based electrolytes. We show that our model is able to predict quantities of adsorbed ions and capacitances in a range compatible with experimental values. We show that there is a strong dependency of the calculated properties on the pore size and on the presence or absence of solvent. In particular, for neat ionic liquids, larger capacitances are obtained for smaller pores, while the opposite trend is observed for organic electrolytes.

cond-mat.mtrl-sci↗