Analysis Of Electron Density Research Articles

Structural and theoretical study of π-stacking interactions in new complexes based on CuCl2 and 3-sulfonamide-substituted imidazo[2,1-b]thiazoles.

At present, sulfonamides and their metal complexes have received a new impetus for development. Of particular interest is the study of molecular and crystal structures, which takes into account weak non-valent interactions. Despite the low energy of such interactions, in many cases, they act collectively, and the sum of their actions can play a significant role. As a result, the spectrum of medical and biological activity of new metal complexes is expanded. In this regard, the synthesis and study of the molecular and crystal structure of sulfonamides and their metal complexes is of undoubted relevance. In this work, we studied non-valent intra- and intermolecular interactions in ligands of sulfonamide-substituted imidazo[2,1-b]thiazoles and their previously unknown complexes with CuCl2. The performed analysis of the data obtained by X-ray diffraction analysis made it possible to establish the intramolecular π-stacking interaction in imidazothiazole ligands, which is retained in their complexes with CuCl2. Within the framework of QTAIM topological analysis of electron density and DORI analysis, stereoelectronic and topological structures were studied. In the complexes, tetral, chalcogen, and pnycogen new interligand non-valent interactions were established. The energies of all established types of non-valent interactions have been calculated, and their comparative evaluation has been made. X-ray data of new arylsulfonylamino-substituted derivatives of imidazo[2,1-b]thiazoles and their metal complexes with CuCl2 have been studied. To determine the theoretical prerequisites for the occurrence of π-stacking in the molecules under study, the QTAIM method was used in the framework of the DFT/B3LYP/6-311 + G(d) calculation using the GAUSSIAN 09 program. In addition, the DORI electron density region overlap indicator and the Multiwfn program were used to analyze non-valent interactions.

On the Nature of the Partial Covalent Bond between Noble Gas Elements and Noble Metal Atoms

This article provides a discussion on the nature of bonding between noble gases (Ng) and noble metals (M) from a quantum chemical perspective by investigating compounds such as NgMY (Y=CN, O, NO3, SO4, CO3), [NgM-(bipy)]+, NgMCCH, and MCCNgH complexes, where M=Cu, Ag, Au and Ng=Kr-Rn, with some complexes containing the lighter noble gas atoms as well. Despite having very low chemical reactivity, noble gases have been observed to form weak bonds with noble metals such as copper, gold, and silver. In this study, we explore the factors that contribute to this unusual bonding behavior, including the electronic structure of the atoms involved and the geometric configuration of the concerned fragments. We also investigate the metastable nature of the resulting complexes by studying the energetics of their possible dissociation and internal isomerization channels. The noble gas-binding ability of the bare metal cyanides are higher than most of their bromide counterparts, with CuCN and AgCN showing higher affinity than their chloride analogues as well. In contrast, the oxides seem to have lower binding power than their corresponding halides. In the oxide and the bipyridyl complexes, the Ng-binding ability follows the order Au > Cu > Ag. The dissociation energies calculated, considering the zero-point energy correction for possible dissociation channels, increase as we move down the noble gas group. The bond between the noble gases and the noble metals in the complexes are found to have comparable weightage of orbital and electrostatic interactions, suggestive of a partial covalent nature. The same is validated from the topological analysis of electron density.

Charge-Shifted Weak Noncovalent Interactions in the Atmospherically Important OCS Microhydrates.

Stratospheric aerosol, mainly comprising microhydrated carbonyl sulfide (OCS), is among the primary drivers of climate change. In this study, we investigate the effect of microhydration on the structure, energetics, and vibrational properties of the neutral OCS molecule using ab initio calculation, molecular electrostatic potential (MESP), topological analyses of electron density, and natural bond orbital (NBO) analyses. The complexation energy increases with the cluster size, and the first solvation shell of OCS consists of four water molecules that interact with the OCS moiety preferentially through SOCS···OW, OOCS···OW, and COCS···OW type of weak noncovalent interaction instead of the typical OOCS···H-OW and SOCS···H-OW H-bonds. These noncovalent interactions originate due to the electron shift from the water oxygen lone pair to the antibonding orbital of C═S [BD*(C═S)], sometimes via BD*(C═O), which substantially perturbs the bending mode of surrounding water molecules. The present study thus unravels the underlying relationship between the OCS atmospheric hydrolysis and the charge-shifted noncovalent interactions.

Electronic Properties of Functionalized Diamanes for Field-Emission Displays.

Ultrathin diamond films, or diamanes, are promising quasi-2D materials that are characterized by high stiffness, extreme wear resistance, high thermal conductivity, and chemical stability. Surface functionalization of multilayer graphene with different stackings of layers could be an interesting opportunity to induce proper electronic properties into diamanes. Combination of these electronic properties together with extraordinary mechanical ones will lead to their applications as field-emission displays substituting original devices with light-emitting diodes or organic light-emitting diodes. In the present study, we focus on the electronic properties of fluorinated and hydrogenated diamanes with (111), (110), (0001), (101̅0), and (2̅110) crystallographic orientations of surfaces of various thicknesses by using first-principles calculations and Bader analysis of electron density. We see that fluorine induces an occupied surface electronic state, while hydrogen modifies the occupied bulk state and also induces unoccupied surface states. Furthermore, a lower number of layers is necessary for hydrogenated diamanes to achieve the convergence of the work function in comparison with fluorinated diamanes, with the exception of fluorinated (110) and (2̅110) films that achieve rapid convergence and have the same behavior as other hydrogenated surfaces. This induces a modification of the work function with an increase of the number of layers that makes hydrogenated (2̅110) diamanes the most suitable surface for field-emission displays, better than the fluorinated counterparts. In addition, a quasi-quantitative descriptor of surface dipole moment based on the Tantardini-Oganov electronegativity scale is introduced as the average of bond dipole moments between the surface atoms. This new fundamental descriptor is capable of predicting a priori the bond dipole moment and may be considered as a new useful feature for crystal structure prediction based on artificial intelligence.

Structure and stability investigation of oxygen interaction with Fe in bcc-Fe

The precise interaction mechanisms between body-centered cubic Fe and the unavoidable interstitial O atom are critical to understanding oxidation resistance. Even though the Fe–O interaction has been investigated extensively for centuries, the physical evolution processing including the stability, bonding characteristics, and magnetism, remains as one of the most important scientific issues. Here, a four-level (atomic, electronic, orbital, and spin-level) analysis was employed to investigate the precise interactions between Fe and O atoms by multiple complementarity methods (Madelung energy calculation, electronic density analysis, crystal orbital Hamilton population analysis and topology analysis of spin maps). The stability of Fe atoms was enhanced with the O atom at the tetrahedral interstitial site. The bonding strength between Fe and O atoms originates substantially from s orbits. Furthermore, the topology of the minority-spin was changed by the magnetic moment flip of O, and the interaction among Fe atoms were strengthened. A further understanding of the Fe–O mechanism provides a theoretical basis for obtaining excellent physical properties in Fe-based materials.

Giant dielectric properties of Na1/2La1/2Cu3Ti4O12 perovskite ceramic: First-principles and experimental investigations

Na1/2La1/2Cu3Ti4O12 ceramics were successfully fabricated via a sol-gel method. We found that the crystal structure of these sintered ceramics is identical to that of CaCu3Ti4O12, ICSD number 01-075-2188. A small quantity of CuO was observed due to the substitution of Na + at Cu2+ sites of the CaCu3Ti4O12 structure. Additionally, a small number of related Cu phases were discovered at grain junctions in these ceramics. Our Ab initio Molecular Dynamic simulations clearly revealed that oxygen vacancies are created during the sintering process. Additionally, at room temperature, our simulations showed that sites of the oxygen vacancies in the Na1/2La1/2Cu3Ti4O12 lattice are occupied by free oxygen, resulting in a lower oxygen vacancy density. Sintered Na1/2La1/2Cu3Ti4O12 ceramics present excellent dielectric properties, a high dielectric permittivity of 7780–9000 and a rather low dielectric loss tangent (0.041–0.042). From our electron density analysis, it was clearly seen that Cu+ and Ti3+ observed by the XPS measurements originated from the presence of oxygen vacancies in the Na1/2La1/2Cu3Ti4O12 structure. Electrical, DFT, and XPS studies indicated that the internal barrier layer capacitor (IBLC) model is the most appropriate for the colossal dielectric response in these ceramics.

First-principle calculations of stable configurations and electronic structures of pristine and discharged spinel Mg1.31V1.67-xNixO4 (x = 0, 0.13) as cathode materials for magnesium secondary batteries

The stable configurations and electronic structures of spinel Mg1.31V1.67-xNixO4 (x = 0, 0.13) in pristine and discharged samples were determined using first-principles calculations. Structural relaxation, transition state, and projected density of states calculations were performed using density functional theory. Structure relaxation of pristine and discharged Mg1.31V1.67-xNixO4 (x = 0, 0.13) demonstrated that Mg in the 8a site moved to a vacant 16c site during the discharge process. When the Mg insertion was equal to 0.5, the ratio of the structural change from spinel to rock-salt was approximately 0.5. NEB calculations indicated that the energy barrier for Mg diffusion from the 8a site to the 16c site of Mg1.31V1.57Ni0.1O4 was lower than that of Mg1.31V1.67O4. Electron density analysis was used to analyze the covalency between the metals and oxygen, confirming that the covalencies of the V-O and the Mg8asite-O bonds in Mg1.31V1.57Ni0.13O4 were respectively stronger and weaker than that of Mg1.31V1.67O4. Based on the overlap of the d-orbital of vanadium and the p-orbital of oxygen in Mg1.31V1.67-xNixO4 (x = 0, 0.13), the covalency of vanadium and oxygen was constructed from the projected density of states.

Exploring the potential and identifying Withania somnifera alkaloids as novel dihydrofolate reductase (DHFR) inhibitors by the AlteQ method

There is an urgent need to discover and develop novel drugs to combat Mycobacterium tuberculosis, the causative agent of tuberculosis (TB) in humans. Alkaloids have been shown to have wide-ranging therapeutic application and could be ideal candidates for drug development, and research is underway to develop new anti-tubercular drugs from natural sources. In this regard, the current research deals with finding novel lead compounds from the Withania somnifera (WS) plant. Broad health benefits of WS are due to the presence of diverse chemical constituents which include anaferine and anahygrine and which belong to the alkaloid family. In the present study, these two compounds have been theoretically studied to understand their electronic properties using the density functional theory (DFT) at the B3LYP/6-311 + G (d,p) level. HOMO and LUMO properties and molecular electrostatic potential (MEP) surface were calculated. Further, to understand the mechanism of action of these compounds and to identify their putative drug target, molecular docking and dynamics studies were employed against Mycobacterium tuberculosis dihydrofolate reductase (DHFR). It was determined that NADP+ affects stability of the complexes by reducing fluctuations of residues 14–23 and 117–126. It was also found that Ile5 and Gln28 play an important role in complexation. Electron density analysis (using the AlteQ method) of the intermolecular region, analyzing both the anaferin-NADP+ and anahygrin-NADP+ complexes showed that anaferin and anahygrin complexes are more stable in the presence of NADP+. It has been established that in most intermolecular contacts the contribution of the ligand to the electron density is greater than that of NADP+. The present study thus provides an excellent way to analyze the effect of anaferine and anahygrine in essential processes of M. tuberculosis.Communicated by Ramaswamy H. Sarma

Revised Mechanism of C(sp3)-C(sp3) Reductive Elimination from Ni(II) with the Assistance of a Z-Type Metalloligand.

Reductive elimination is a key step in Ni-catalyzed cross-couplings. Compared with processes that proceed from Ni(III) or Ni(IV) intermediates, C(sp3)-C(sp3) reductive eliminations from Ni(II) centers are challenging due to the weak oxidizing ability of Ni(II) species. In this report, we present computational evidence that supports a mechanism in which Zn coordination to the nickel center as a Z-type ligand accelerates reductive elimination. This Zn-assisted pathway is found to be lower in energy compared with direct reductive elimination from a σ-coordinated Ni(II) intermediate, providing new insights into the mechanism of Ni-catalyzed cross-coupling with organozinc nucleophiles. Mayer bond order, Hirshfield charge, Laplacian of the electron density, orbital, and interaction region indicator analyses were conducted to elucidate details of the reductive elimination process and characterize the key intermediates. Theoretical calculations indicate a significant Z-type Ni-Zn interaction that reduces the electron density around the Ni center and accelerates reductive elimination. This mechanistic study of reductive elimination in Ni(0)-catalyzed conjunctive cross-couplings of aryl iodides, organozinc reagents, and alkenes is an important case study of the involvement of Zn-assisted reductive elimination in Ni catalysis. We anticipate that the novel Zn-assisted reductive elimination mode may extend to other cross-coupling processes and explain the unique effectiveness of organozinc nucleophiles in many instances.

Crystal engineering, electron density analysis, andin situvariable temperature studies on co-crystal between nicotinic acid and gallic acid sesquihydrate

The growth and thermal stability of the gallic acid : nicotinic acid cocrystal has been analyzed in terms of electron density analysis and conversion of GA monohydrate into anhydrate through heating the co-crystal.

Grape bunches of novel conjugated chain bonded fullerene oligomers: design of a potential electron trap carbonaceous molecular material.

Developing π electron conjugated groups as covalent bonded bridges between fullerenes in their oligomers is key to optimizing and maximizing functions of the fullerene-based materials. In this work, a series of novel conjugated chain bonded fullerene C60 oligomers (CBFOs) with a well-defined nano-architecture and "grape bunches" shapes are rationally designed and viably constructed based on fullerene-carbenes by means of DFT calculations. The results show that the presently designed CBFOs present a much better electron-accepting ability together with a much lower reorganization energy than the isolated fullerene C60, and characterized as the potential ideal candidate for electron acceptors. The frontier molecular orbital and electron density analysis can well support the results of diabatic electron affinity (EAa) and vertical electron affinity (EAv) calculations. Moreover, these CBFOs exhibit strong absorption in the visible region but no obvious absorption in the ultraviolet region. In addition, the optical properties of the CBFOs and two dimensional structure are also simulated and explored theoretically. We hope that the present study would be helpful for developing covalent-bonded-fullerene based electron trap molecular materials, building blocks of nano-devices and nano-machinery applications.

Revisiting conventional noncovalent interactions towards a complete understanding: from tetrel to pnicogen, chalcogen, and halogen bond.

Typical noncovalent interactions, including tetrel (TtB), pnicogen (PniB), chalcogen (ChalB), and halogen bonds (HalB), were systematically re-investigated by modeling the N⋯Z interactions (Z = Si, P, S, Cl) between NH3 - as a nucleophilic, and SiF4, PF3, SF2, and ClF - as electrophilic components, employing highly reliable ab initio methods. The characteristics of N⋯Z interactions when Z goes from Si to Cl, were examined through their changes in stability, vibrational spectroscopy, electron density, and natural orbital analyses. The binding energies of these complexes at CCSD(T)/CBS indicate that NH3 tends to hold tightly most with ClF (-34.7 kJ mol-1) and SiF4 (-23.7 kJ mol-1) to form N⋯Cl HalB and N⋯Si TtB, respectively. Remarkably, the interaction energies obtained from various approaches imply that the strength of these noncovalent interactions follows the order: N⋯Si TtB > N⋯Cl HalB > N⋯S ChalB > N⋯P PniB, that differs the order of their corresponding complex stability. The conventional N⋯Z noncovalent interactions are characterized by the local vibrational frequencies of 351, 126, 167, and 261 cm-1 for TtB, PniB, ChalB, and HalB, respectively. The SAPT2+(3)dMP2 calculations demonstrate that the primary force controlling their strength retains the electrostatic term. Accompanied by the stronger strength of N⋯Si TtB and N⋯Cl HalB, the AIM and NBO results state that they are partly covalent in nature with amounts of 18.57% and 27.53%, respectively. Among various analysis approaches, the force constant of the local N⋯Z stretching vibration is shown to be most accurate in describing the noncovalent interactions.

Electron delocalization in defect-containing graphene and its influence on tetrel bond formation.

Using the advanced analyses of electron density and fermionic potential, we show how electron delocalization influences the ability of defect-containing graphene to form tetrel bonds. The Cg atoms of a vacancy defect can produce one nonpolar interaction, alongside a peculiar polar Cg⋯Cg bond. The latter stems from the presence of a localized electron pair on a vacancy defect Cg atom and the local depletion of electron localization on another Cg atom. This interaction is an example of intralayer tetrel bond. In the presence of an absorbed molecule of bisphenol A diglycidyl ether (DGEBA), graphene is able to form incipient tetrel Cg⋯O bonds with an ether group oxygen. In contrast to an epoxy group oxygen, the disposition of the ether oxygen often causes the orientation of electron-rich π-domains of graphene carbon on the weakly expressed electrophilic region of the oxygen. In the case of graphene with a point Si defect, the Si atom can form quite strong Si⋯C interactions with the DGEBA aryl carbons. In contrast to other noncovalent bonds, this interaction significantly alters the electron (de)localization on the Si atom and in the aryl ring. The reliability of the obtained results is enhanced by the use of multiple 2D periodic models with defects located at different positions along the DGEBA skeleton.

Sulfur-arene interactions: the S⋯π and S-H⋯π interactions in the dimers of benzofuran⋯sulfur dioxide and benzofuran⋯hydrogen sulfide.

Non-covalent interactions between sulfur centers and aromatic rings play important roles in biological chemistry. We examined here the sulfur-arene interactions between the fused aromatic heterocycle benzofuran and two prototype sulfur divalent triatomics (sulfur dioxide and hydrogen sulfide). The weakly-bound adducts were generated in a supersonic jet expansion and characterized with broadband (chirped-pulsed) time-domain microwave spectroscopy. The rotational spectrum confirmed the detection of a single isomer for both heterodimers, consistent with the computational predictions for the global minima. The benzofuran⋯sulfur dioxide dimer exhibits a stacked structure with sulfur closer to benzofuran, while in benzofuran⋯hydrogen sulfide the two S-H bonds are oriented towards the bicycle. These binding topologies are similar to the corresponding benzene adducts, but offer increased interaction energies. The stabilizing interactions are described as S⋯π or S-H⋯π, respectively, using a combination of density-functional theory calculations (dispersion corrected B3LYP and B2PLYP), natural bond orbital theory, energy decomposition and electronic density analysis methods. The two heterodimers present a larger dispersion component, but nearly balanced by electrostatic contributions.

Investigation of C–F···F–C Interactions Using Experimental and Theoretical Charge Density Analyses

Among the halogens, fluorine plays a crucial role in governing the potency of drugs and pharmaceuticals. In this study, experimental and theoretical charge density analyses have been performed on N-(2,5-difluorophenyl)-3,5-difluoro-N-(3-methoxyphenethyl)benzamide to study the nature of weak intermolecular interactions, especially the F···F interactions, mediated by organic fluorine. The kind of C–F···F–C interactions analyzed in this study are Type I and quasi Type I/Type II. For this, the quantitative and qualitative analyses of electron densities have been performed based on the multipole modeling of high-resolution experimental X-ray diffraction data and theoretical structure factors generated from periodic calculations. The interactions have been analyzed based on the topological properties of electron densities using quantum theory of atoms in molecules (QTAIM). Thus, the nature of organic fluorine has been investigated by studying deformation of electron densities, Laplacian, and topological parameters.

The Presence of Charge Transfer Defect Complexes in Intermediate Band CuAl1−pFepS2

Despite chalcopyrite (CuFeS2) being one of the oldest known copper ores, it exhibits various properties that are still the subject of debate. For example, the relative concentrations of the ionic states of Fe and Cu in CuFeS2 can vary significantly between different studies. The presence of a plasmon-like resonance in the visible absorption spectrum of CuFeS2 nanocrystals has driven a renewed interest in this material over recent years. The successful synthesis of CuAl1−pFepS2 nanocrystals that exhibit a similar optical resonance has recently been demonstrated in the literature. In this study, we use density functional theory to investigate Fe substitution in CuAlS2 and find that the formation energy of neutral [FeCu]2++[CuAl]2− defect complexes is comparable to [FeAl]0 antisites when p≥0.5. Analysis of electron density and density of states reveals that charge transfer within these defect complexes leads to the formation of local Cu2+/Fe2+ ionic states that have previously been associated with the optical resonance in the visible absorption of CuFeS2. Finally, we comment on the nature of the optical resonance in CuAl1−pFepS2 in light of our results and discuss the potential for tuning the optical properties of similar systems.

Na2Mn(CO3)2: A carbonate based prototype cathode material for Na-ion batteries with high rate capability — An ab-initio study

Considering the mounting demand for energy storage systems and the issues associated with the current cathode materials, it is necessary that the search space for novel cathode materials for rechargeable batteries should be widened. In this regard, we have presented the structural, lattice dynamical, electrochemical, and electronic structure studies of a carbonate-based prototype cathode material for Na-ion batteries, using first-principles calculations. The existence of a carbon-containing Mn compound Na2Mn(CO3)2 is predicted using first-principles calculations and the compound is expected to crystallize in trigonal crystal structure with R3̄ space group. The electrochemical analyses reveal that this cathode material could deliver a theoretical capacity of 243mAh/g and a theoretical average voltage of 3.6 V. The desodiation process is modeled via finding the stable crystal structure of intermediate compositions for different Na/vacancy concentrations. The electronic structure and charge density analysis of these intermediate compositions reveal that Mn, O, and a small contribution from C involve in the desodiation process. Even though the involvement of O in the redox is high, we have found that the oxygen evolution during desodiation is not favored thermodynamically, indicating a possible enhancement in the specific capacity. The chemical bonding analyses indicate that the Mn-O bonding interaction is iono-covalent, whereas the C-O bond exhibits a more covalent character with small ionicity. The activation energy of the diffusion barrier for the Na diffusion through the lower energy path in Na2Mn(CO3)2 is estimated to be 0.22 eV using nudged elastic band method. We postulate high ionic conductivity and thereby high rate capability for Na2Mn(CO3)2 as the Na diffusion coefficient is relatively higher compared with that of Li in cathodes used for commercial Li-ion batteries.

Can the Fluxionality in Borospherene Influence the Confinement-Induced Bonding between Two Noble Gas Atoms?

A density functional theory study is performed to determine the stability and bonding in the neon dimer inside the B30N30 fullerene cage, the fluxional B40 cage, and within non-fluxional cages such as B12N12 and C60. The nature of bonding in the Ne2 encapsulated B40 is compared with the that in other cages in an attempt to determine whether any possible alterations are brought about by the dynamical nature of the host cage apart from the associated confinement effects. The bonding analysis includes the natural bond order (NBO), Bader's Atoms-in-Molecules electron density analysis (AIM), and energy decomposition analysis (EDA), revealing the non-covalent nature of the interactions between the Ne atoms and that between the Ne and the cage atoms. The formation of all the Ne2@cage systems is thermochemically unfavourable, the least being that for the B30N30 cage, which can easily be made favourable at lower temperatures. The Ne-Ne distance is lowest in the smallest cage and increases as the cage size increase due to steric relaxation experienced by the dimer. The dynamical picture of the systems is investigated by performing ab initio molecular dynamics simulations using the atom-centred density matrix propagation (ADMP) technique, which shows the nature of the movement of the dimer inside the cages, and by the fact that since it moves as a single entity, a weak bonding force holds them together, apart from their proven kinetic stability.

Study on Molecular Structure Model and Reactivity of Spent Mushroom Substrate: Experiment and Simulation

The infrastructure features of the spent mushroom substrate (SMS) were detected and explored based on experimental data acquired from Fourier Transform Infrared Spectroscopy, Pyrolysis–Gas Chromatography/Mass Spectrometry as well as Thermogravimetric Analysis. Further, molecular simulation methods were combined with diverse testing technologies to build the 2D and associated 3D models from cellulose, hemicellulose, and lignin. Eventually, a rational 3D model was constructed for SMS using geometry optimization calculations and annealing dynamics simulations. According to the Mulliken population analysis and electron density analysis, the π-π conjugation effect of the aromatic ring structures was influenced by the oxygen atoms, thus, resulting in the electron accumulation on these oxygen atoms. At the same time, oxygen exhibited a greater electronic charge density and reactivity in the Furan ring and pyran ring structures in contrast to other atoms. Furthermore, the molecular orbitals for HOMO and LUMO were computed to check the chemical reaction characteristics of the SMS. According to the HOMO–LUMO energy gap, the structure of the polycyclic aromatic hydrocarbons provided reaction sites for the reaction and played a key role in chemical bond breaking.Graphical Abstract

Interaction of imidazolium based ionic liquid electrolytes with carbon nitride electrodes in supercapacitors; a step forward for understanding electrode–electrolyte interaction

Ionic liquids (ILs) are considered as an emerging class of electrolytes finding their applications in energy storage devices due to wide electrochemical windows, nonflammability, low volatility, and high thermal and chemical stability. The interaction of three ionic liquids i.e., 1,3-dimethylimidazolium chloride (MIC), 1,3-disulfonic acid imidazolium nitrate (DIN), 1-Ethyl-3-methylimidazolium tetrafluoroborate (EMI) with C2N surface is evaluated for better understanding electrode–electrolyte interaction in supercapacitors. The interaction of electrolytes on C2N electrode is studied through interaction energy analysis, non-covalent interactions (NCI) analysis and quantum theory of atoms in molecule (QTAIM) analyses. Electronic properties are investigated through natural bond orbital (NBO), frontier molecular orbital (FMOs), density of states and electron density analyses. Interaction energies calculated for the most stable geometry of the studied electrolytes are −13.83 kcal/mol (DIN@C2N), −25.90 kcal/mol (EMI@C2N), and −26.94 kcal/mol (MIC@C2N). NBO analysis reveals that an appreciable amount of charge is transferred from surface to ionic liquids, and these results are further supported by EDD analysis. Moreover, FMO analysis unveils that 2.04 eV decrease in energy gap of MIC@C2N complex. We strongly believe that this study provides a deep insight in better understanding the electrode–electrolyte interactions, which play vital role in various application such as super-capacitors, batteries, and fuel cells.