Nowadays, density functional theory (DFT)-based high-throughput computational approach is becoming more efficient and, thus, attractive for finding advanced materials for electrochemical applications. In this work, we illustrate how theoretical models, computational methods, and informatics techniques can be put together to form a simple DFT-based throughput computational workflow for predicting physicochemical properties of room-temperature ionic liquids. The developed workflow has been used for screening a set of 48 ionic pairs and for analyzing the gathered data. The predicted relative electrochemical stabilities, ionic charges and dynamic properties of the investigated ionic liquids are discussed in the light of their potential practical applications.
Carbon materials have a range of properties such as high electrical conductivity, high specific surface area, and mechanical flexibility are relevant for electrochemical applications. Carbon materials are utilised in energy conversion-and-storage devices along with electrolytes of complementary properties. In this work, we study the interaction of highly concentrated electrolytes (ionic liquids) at a model carbon surface (circumcoronene) using density functional theory methods. Our results indicate the decisive role of the dispersion interactions that noticeably strengthen the circumcoronene-ion interaction. Also, we focus on the adsorption of halide anions as the electrolytes containing these ions are promising for practical use in supercapacitors and solar cells.
Ionic liquids (IL) are promising electrolytes for electrochemical applications due to their remarkable stability and high charge density. Molecular dynamics simulations are essential for better understanding the complex phenomena occurring at the electrode-IL interface. In this work, we have studied the interface between graphene and 1-ethyl-3-methyl-imidazolium tetrafluoroborate IL, using density functional theory-based molecular dynamics simulations at variable surface charge densities. We have disassembled the electrical double layer poten-1 tial drop into two main components: one involving atomic charges and the other -dipoles.The latter component arises due to the electronic polarisation of the surface and is related to concepts hotly debated in the literature, such as the Thomas-Fermi screening length, effective surface charge plane, and quantum capacitance.
Computational chemistry is a powerful tool for the discovery of novel materials. In particular, it is used to simulate ionic liquids in search of electrolytes for electrochemical applications. Herein, the choice of the computational method is not trivial, as it has to be both efficient and accurate. Density functional theory methods with appropriate corrections for the systematic weaknesses can give precision close to that of the post-Hartree-Fock coupled cluster methods with a fraction of their cost. Thence, we have evaluated the performance of a recently developed nonempirical strongly constrained and appropriately normed (SCAN) density functional on electronic structure calculations of ionic liquid ion pairs. The performance of SCAN and other popular functionals (PBE, M06-L, B2PLYP) among with Grimme's dispersion correction and Boys-Bernardi basis set superposition error correction was compared to DLPNO-CCSD(T)/CBS. We show that SCAN reproduces coupled-cluster results for describing the employed dataset of 48 ion pairs.density functional theory, dispersion correction, ionic liquids, self-interaction error, strongly constrained and appropriately normed 1 | I N TR ODU C TI ON Ionic liquids are promising solvents that have been extensively studied over the last few decades. Their tunable properties make them advantageous candidates for various electrochemical applications. [1,2] The high price of commercially available ionic liquids remains an obstacle for an extensive use of ionic liquids. [3] However, this is also a strong stimulus for the search of advanced ionic liquids. [1] A useful toolkit for studying ionic liquids includes various computer simulation methods. [4] Simulations have been growing in popularity, hand in hand with an exponential increase in the computational capabilities. [5,6] For instance, computational screening allows estimating the properties of many candidates even prior to their synthesis. [7][8][9][10][11] Therefore, it helps to determine, which candidates are the best for a given application. Also, molecular dynamics simulations provide an insight into both structure and dynamics of specific ionic liquids both in bulk and near various interfaces. [5,[12][13][14][15][16] However, they require careful parametrization of the force fields used. [5,12,[17][18][19][20] On the contrary, without parametrization, quantum mechanical calculations allow rapid exploration of the space of ionic liquids, which is vast due to numerous possible anion-cation combinations. [4,21] Fast computational methods are essential for both high-throughput screening and large-size simulations. At the same time, the methods have to be accurate enough to capture all of the physical interactions within the ionic liquids. The density functional theory (DFT) methods offer a good trade-off between speed and accuracy. [4,22,23] The success of DFT depends whether employed exchange-correlation functional can adequately describe the system of interest. [24] In practice, the necessity for faster and scalable methods attracts t...
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