Ab Initio Dynamics of Graphene and Graphyne Electrodes in Vacuum and in the Presence of Electrolytes

Abstract

Graphene and graphyne electrodes are both relevant for electrochemical energy storage applications due to their unique physical, chemical, and electronic properties. Graphyne has been considered even more attractive than graphene due to its larger specific surface area, greater electronic mobility, and intrinsic band gap. The analyses presented here reveal relevant features of graphyne in an interaction with an electrolyte that can be useful for practical applications. Although there is already a considerable volume of work on graphyne, the analysis of its properties taking into account the dynamics of its network and the interaction with the condensed medium has not yet been presented. In this work, ab initio molecular dynamics simulations were performed to study the energetic, structural, spectroscopic, and electronic properties of graphene and graphyne electrodes in vacuum and in the presence of an electrolyte (EMIM-BF4). A detailed analysis of the electrode–electrolyte interaction is reported for both systems. Structural features are presented in terms of both radial and spatial distribution functions and angular orientation distributions. Power spectral analyses and molecular orbital maps provided important insights into the intermolecular interactions in graphene and graphyne systems, describing the main differences as well as revealing similarities between them.

Evaluating quantum entanglement generation in two‐dimensional graphene systems through lithium ion interactions: A DFT‐based study

“…Since then, graphene has been the subject of studies in various fields, including electronics, energy, materials physics, semiconductors, and applied medicine. [7][8][9][10][11][12][13][14] In addition to these areas of knowledge, the field of quantum mechanics has emerged, particularly concerning quantum information and quantum computing, highlighting the concept of quantum entanglement. 15 Indeed, the study of entanglement has attracted the interest of researchers due to its promising applications, such as, in quantum computing, 16,17 quantum teleportation, 18 quantum sensors, 19 quantum communication 20 and so forth.…”

“…Graphene was first isolated in 2004 6 using a technique known as “mechanical exfoliation”, which involves the successive removal of thinner layers from graphite until a single layer of carbon atoms is obtained. Since then, graphene has been the subject of studies in various fields, including electronics, energy, materials physics, semiconductors, and applied medicine 7–14 . In addition to these areas of knowledge, the field of quantum mechanics has emerged, particularly concerning quantum information and quantum computing, highlighting the concept of quantum entanglement 15 .…”

Structure and Dynamics of Aqueous 2-Aminothiazole/NaCl Electrolytes at Electrified Interfaces

“…In method development, the coupling of accurate atomistic models, including DFT, and spatially continuous processes, such as the electric fields modeled by finite-element (FE) approaches, is a key for cost-efficient multiscale modeling of electrolytes and the EDL, as well as the implementation of FE real-space basis sets in DFT programs. − In energy storage research, however, many theoretical studies applying DFT or classical molecular dynamics (MD) focus on the OHP primarily to investigate the interfacial nanostructure of electrolytes and their ionic transport dynamics near electrodes at the atomic level. Here, interface models are utilized and often replacing the metallic electrode by graphene sheets to introduce simple charged surfaces up to ±1.5 e/nm 2 and model the localized restructuring of the electrolyte in the EDL. − The fluctuating electrode potentials of an electrified interface are simulated with a constant-potential model (CPM), which is most accurate when combined with a grand canonical (GC) treatment of ions. − A computationally more efficient alternative is the constant-charge model (CCM). , …”