Application Of Density Functional Theory Research Articles

Electronic Structure Determines Geometry: Bond Length Alternating in Cyclo[2n]carbons.

Structure determines the properties. However, whether electronic structure determines geometry or geometry determines electronic structure seems a philosophical question in a chicken and egg situation, which remains unclear. In this work, by applying density functional theory (DFT) and DMRG(4n,4n)-CASSCF methods, theoretical investigation suggested that the dual antiaromaticity in cyclo[2n]carbons with even n should be attributed to the electron correlation effect, instead of decreased geometric symmetry, which actually exists in all cyclo[2n]carbon molecules and does not point out the essence. Such dual antiaromaticity can be conceptualized as electron correlation-stabilized dual antiaromaticity. Results also showed that DFT is reliable for cyclocarbons larger than C14, but we should be careful when applying it to smaller ones. DFT failed to give the correct structure of C6 compared with density matrix renormalization group results.

A new activity model for biotite and its application

A new activity model for biotite is formulated in the system K2O-FeO-MgO-Al2O3-SiO2-H2O-TiO2-O2 (KFMASHTO), which extends that for the KFMASH system by introducing a titanium-biotite and a ferric-biotite end-member (tbio: K(TiMg2)[(O)2(AlSi3)O10] and fbio: K(Fe3+Mg2)[(OH)2(Al2Si2)O10]), as well as a pyrophyllite end-member (pyp: Al2[(OH)2Si4O10]) that accounts for the presence of octahedral excess-Al in natural biotites. Phonon calculations applying density functional theory (DFT) using the software Castep yielded the standard entropies of tbio and fbio as Sotbio = 328.06 J/(mol·K) and Sofbio = 301.69 J/(mol·K), and their heat capacity functions. From experimental phase-equilibrium data, the enthalpy of formation value of tbio was constrained as ΔHf,tbioo\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\Delta {H}_{f,tbio}^{o}$$\\end{document} = −6124.68 ± 3.33 kJ/mol. Natural data were used to derive ΔHf,fbioo\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\Delta {H}_{f,fbio}^{o}$$\\end{document}= −5935.3 ± 6.6 kJ/mol. The single-defect DFT method was applied to parameterize important macroscopic mixing properties (macro-W’s) involving tbio and pyp end-members in the model (fbio was treated ideal). Castep-derived microscopic interaction energies (micro-w’s) are presented herein for KFMASH-biotite. The octahedral same-site (M1) Mg–Al mixing micro-w (wMgAl(M1)), the same-site tetrahedral Si-Al mixing parameter (wSiAl(T1)) and the related cross-site term are: wMgAl(M1) = 82.5 kJ/mol, wSiAl(T1) = 95.6 kJ/mol (two T1-sites) and wMgAlAlSi(M1T1)=\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${w}_{MgAlAlSi(M1T1)}=$$\\end{document} 175.1 kJ/mol. The linear combination of these micro-w’s gives a macroscopic Wphleas = 18.8 kJ/mol, that is not transferable to other mineral groups. Micro w’s for Mg-Fe mixing in biotite (wMgFe(M1), wMgFe(M2),wMgMgFeFe(M1M2)\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${w}_{MgMgFeFe(M1M2)}$$\\end{document}), are all close to ideality. The biotite activity model of this study is thus a first example of next-generation activity models that use DFT- and thus physically based micro-w’s and reassembled macro-W’s for petrological calculations. Test calculations on 5 samples from low- to high-grade metamorphic environments covering metapelite to greywacke bulk-compositions using Perple_X suite of programs illustrate the performance of the new biotite activity model. Computed mineral-chemistries are in all cases in better agreement with measured compositions than resulting from published activity models of biotite.

High-throughput screening of axially bonded dual atom catalysts for enhanced electrocatalytic reactions: The effect of van der Waals interaction

Single- and dual-atom catalysts (SACs and DACs) on single-layer graphene are widely investigated for a wide range of electrochemical reactions. However, the effect of van der Waals interactions on the activity of these catalysts has not been investigated through systematic high-throughput screening. Here we introduce the concept of van der Waals interactions through a double-layer DAC structure which has axial d orbital modification towards enhanced CO2 reduction reaction (CO2RR), hydrogen evolution reaction (HER), oxygen reduction reaction (ORR), and oxygen evolution reaction (OER). We applied density functional theory (DFT) to screen 3d, 4d, and 5d transition metals supported by double-layer nitrogen-doped graphene, denoted as M2N8. We sought catalysts with high thermodynamic and electrochemical stabilities along with low overpotentials for CO2RR, ORR, OER, or HER. We find that HER can take place inside the van der Waals gap of V2N8 and Co2N8 leading to overpotentials of 0.10 and 0.16 V. Moreover, ORR and OER can take place on the surface of Fe2N8 and Ir2N8, respectively, leading to overpotentials of 0.39 and 0.37 V. DFT predicts a CO2RR overpotential of 0.85 V towards CO on the surface of Co2N8 along with the HER overpotential of 0.16 V inside the van der Waals gap of Co2N8 towards the production of syngas (CO+H2). This paper provides fundamental insights into the design of advanced multi-layer catalysts by applying the concept of van der Waals interactions for electrochemistry at room temperature.

DFT study of adsorption and potential detection of carbonyl fluoride on B-doped aluminum nitride nanosheets

Carbonyl fluoride (COF2) is a decomposition product that can be used to find failures in gas-insulated switchgear equipment. In this study, we applied Density Functional Theory (DFT) calculations to examine the suitability of pristine and boron-doped aluminum nitride nanosheets (AlNNS) for COF2 adsorption and sensing applications. Our investigation suggested a dissociative COF2 adsorption on pristine AlNNS, resulting in important adsorption energy (–2.19 eV), the releasing of a fluorine atom from the molecule and formation of new C–N, O–Al and F–Al bonds. Two preferential chemisorption geometries were achieved on the B-doped N-vacancy monolayer (B-vN-AlNNS), with adsorption energies of –1.04 and –3.44 eV. In the first geometry, only an O–B bond was formed, whereas in the another one similar interactions as in COF2/AlNNS took place. Furthermore, we analyzed the evolution of electronic properties in order to evaluate the performance of these nanosheets for COF2 detection purposes. Our results showed significant modifications in both energy gap and work function only after COF2 adsorption on B-vN-AlNNS. Finally, charge transfer analysis revealed electron exchange from the studied surfaces to the gas molecule. These findings suggest that B-doped AlNNS exhibits good performance for COF2 detection, and could encourage further experimental research to develop efficient sensing materials.

Theoretical Investigation of the structure and Raman scattering properties of Hoogsteen- and Watson-Crick-type Adenine-Thymine base pair

Hoogsteen (HG) and Watson-Crick (WC) adenine–thymine (A-T) base pairs are fundamental to gene expression and genomic stability. Our research applied density functional theory (DFT) calculations to analyze these base pairs, demonstrating that linking them with ribose or deoxyribose and their immersion in solvents markedly enhances the distinctions in their optical properties. DFT results reveal that N···HN hydrogen bonds in both HG and WC pairs exhibit characteristics of both ionic and covalent bonds, playing a crucial role in their stability. While WC base pairs demonstrate stronger orbital interactions, they also experience greater repulsion than HG pairs. This repulsion offsets the positive interactions to a degree, making the interaction energy of WC pairs slightly lower than that of HG pairs. Furthermore, the distinct conformations of these base pairs result in different vibrational modes, suggesting Raman spectroscopy as an effective method for distinguishing between WC and HG base pairs.

Acetylcholine and butyrylcholine esterase inhibitory potential of newly synthesized halogenated compounds: In vitro, in silico and MD simulation

Schiff bases have numerous applications especially in the medicinal chemistry. Keeping in view their importance, two new compounds; (E)-2-(((4‑bromo-2-(trifluoromethyl) phenyl)imino)methyl)-4-nitrophenol (1) and (E)-3-((4‑bromo-2-(trifluoromethyl)phenylimino) methyl)pyridin-2-amine (2) have been synthesized. These Schiff bases were characterized with modern spectral tools while precise structures were confirmed through XRD which revealed that compound 1 was monoclinic and compound 2 was orthorhombic. The synthesized compounds were further evaluated theoretically by applying density functional theory approach. Regression coefficient (R2) was utilized to compare the different parameters between DFT and XRD data. Hirshfeld surface study was used to find out the different interactions between the atoms presented in the crystalline molecules. Online free tool was used against AChE and BChE for accomplishment of the molecular modeling study. The molecular dynamics simulation study was also conducted to check the binding mechanism of the most active compound on AChE. On the basis of the docking score and MD simulation, compound 1 depicted more inhibition potential. The in-vitro studies further confirmed that synthesized Schiff bases have potential to cure the Alzheimer disease by inhibiting enzymes related to this disease.

Theoretical insight into the NO* Coverage-Dependent selectivity of Pd and Cu electrocatalysts for nitrate reduction

Nitrate (NO3−) is a concerning contaminant in groundwater that is harmful to human health. Electrocatalytic reduction of NO3− can be achieved with transition metals such as Pd and Cu. In this work, we apply density functional theory (DFT) to discern how the electronic properties of the metal catalyst affect the selectivity of the nitrate reduction mechanism toward either N2 products (e.g., N2 and N2O) or N1 products (e.g., NH3 and NH4+). We find that the greater d-band filling of Cu results in more electron accumulation on the N atom of adsorbed NO*, which drives N–H bond formation favoring the production of HNO* and eventually N1 products (NH3). Conversely, the more delocalized d orbitals of Pd lead to a strong adsorbate–adsorbate coverage effect that lowers key N–N coupling barriers at high NO* coverage favoring selectivity toward N2 products (N2 and N2O). This work elucidates why, at the electronic-structure level, nitrate reduction is highly sensitive to NO* coverage on some metals (such as Pd) and less so on others (such as Cu).

Chalcogen Doping in SnO2: A DFT Investigation of Optical and Electronic Properties for Enhanced Photocatalytic Applications.

Tin dioxide (SnO2) is an important transparent conductive oxide (TCO), highly desirable for its use in various technologies due to its earth abundance and non-toxicity. It is studied for applications such as photocatalysis, energy harvesting, energy storage, LEDs, and photovoltaics as an electron transport layer. Elemental doping has been an established method to tune its band gap, increase conductivity, passivate defects, etc. In this study, we apply density functional theory (DFT) calculations to examine the electronic and optical properties of SnO2 when doped with members of the oxygen family, namely S, Se, and Te. By calculating defect formation energies, we find that S doping is energetically favourable in the oxygen substitutional position, whereas Se and Te prefer the Sn substitutional site. We show that S and Se substitutional doping leads to near gap states and can be an effective way to reduce the band gap, which results in an increased absorbance in the optical part of the spectrum, leading to improved photocatalytic activity, whereas Te doping results in several mid-gap states.

Thermodynamical stability of [CNN and NCN] sequences as indication of most abundant structures in the ISM

Most of the molecules identified in the interstellar medium (ISM) are organic compounds and more than 50 have one isomer or more. Statistically, the most stable isomer of a given chemical formula is the most abundant. This occurrence is verified up to sim 90<!PCT!> of the detected species leading to the so-called minimum energy principle (MEP). Our main objective is to increase the list of the 14 bis-nitrogen species already detected. We focus on ten C$_ x $H$_ y $N$_ z $ isomer families with x=(1,2,3), y=(0,2,4,6,8), z=2. To this end, we look for a reliable and economic way to provide energy scales. We employed standard quantum chemistry methods to determine the relative position of each isomer on the energy scales of each family. We systematically applied density functional theory (DFT) treatments using basis sets of increasing size and quality (6-311++G** and cc-pVQZ). When reasonably feasible, we then performed high-level coupled cluster calculations (CCSD) using the same basis sets to refine relative energies. All 14 bis-nitrogen species already identified in the ISM indeed satisfy the MEP. We determine the relative thermodynamic stability of the isomers with a C$_ x $H$_ y $N$_ $ formula of each of the ten sets (94 compounds altogether), and hightlight those that are potentially detectable. By increasing the number of carbon atoms, we find 15 compounds that are by far the most stable candidates. We confirm that, within the limits of thermodynamics, MEP is an efficient and easily applicable tool for identifying the isomers in a given series that have a greater probability of being detected. Computationally, the combination “B3LYP/cc-pVQZ” provides a suitable compromise for determining energy differences and dipole moments. Clearly, the isomers containing the NCN sequence should be prioritized over those with CNN in future observation campaigns.

Highly selective sensing of toxic NOx gases for environmental monitoring using Ru-doped single walled TiO2 nanotube: A density functional theory study

Applying density functional theory simulations, in this study, we examine the sensing properties of Ru-TNT surface towards NOx molecules such as NO and NO2. The obtained results show that Ru doping creates a large-spin density over the Ru-TNT surface, which hints at an increase in the adsorption energy of NOx molecules. The electronic properties of the Ru-TNT surface are significantly altered after NO and NO2 molecule adsorption, as proven by the larger change in the energy gap values. Moreover, the selectivity study indicates that the Ru-TNT is capable of selectively sensing the NOx molecules in the presence of other gases, e.g., CO2, CO, NH3 and H2O. Using an external positive electric field can resist the strong anchoring of NOx molecules over the Ru-TNT surface, suggesting that material recovery is feasible. Thus, the Ru-TNT structure can be applied as a selective, sensitive, and promising ambient temperature gas sensor for NOx molecules.

Vicinal effect on chlorination of diols

The vicinal effect on chlorination reactions of diols was investigated by computational methods. Applying density functional theory (DFT) combined with polarizable continuum model (PCM) and explicit solvent molecules, we demonstrated the effect of hydration on the leaving and vicinal hydroxyl group in SN2 reactions of selected alcohols. Our results point out to the importance of intermolecular hydrogen bonds as a stabilizing factor in reaction pre-complexes and alcohols with vicinal hydroxyl groups, highlighting the importance of solute-solvent network formation. This indicates the significance of adequately describing the solvent in the study of reaction mechanisms, in special when the interaction with solute molecules and ions are strong. Also, we found a “vinical effect” on the reactivity, in other words, alcohols with vicinal hydroxyl groups exhibit higher activation energies when compared to related monoalcohols. Moreover, 1,3-propanediol and 1,3-butanediol present the highest activation energies.

Thermodynamic and structural characterization of high-entropy garnet electrolytes for all-solid-state battery

This study explores multi-component garnet-based materials as solid electrolytes for all-solid-state lithium batteries. Through a combination of computational and experimental approaches, we investigate the thermodynamic and structural properties of lithium lanthanum zirconium oxide garnets doped with various elements. Applying density functional theory, the influence of dopants on the thermodynamic stability of these garnets was studied. Probable atomic configurations and their impact on materials’ properties were investigated with the focus on understanding the influence of these configurations on structural stability, phase preference, and ionic conductivity. In addition to the computational study, series of cubic-phase garnet compounds were synthesized and their electrochemical performance was evaluated experimentally. Our findings reveal that the stability of cubic phase in doped Li-garnets is primarily governed by enthalpy, with configurational entropy playing a secondary role. Moreover, we establish that the increased number of doping elements significantly enhances the cubic phase’s stability. This in-depth understanding of materials’ properties at atomic level establishes the basis for optimizing high-entropy ceramics, contributing significantly to the advancement of solid-state lithium batteries and other applications requiring innovative material solutions.

Effect of oxygen-containing groups in functionalized graphene on its gas sensing properties

The creation of active material for chemiresistive gas sensors with high selectivity and sensitivity will allow a step towards miniaturization and reduction of power consumption of portable gas sensors. Graphene is a promising platform for the synthesis of two-dimensional active materials with high sensitivity. In this work, applying density functional theory (DFT) calculations, the effect of oxygen-containing functional groups (O, OH, O, COOH) on the adsorption of small gas molecules (NH3, CO2, CO, H2S, NO2, SO2) was rigorously studied. Based on the adsorption energies and partial charges from DFT calculations, the sensitivity and selectivity of graphene with different functionalizations were predicted. It was found that hydroxyl and carboxyl groups demonstrate increased selectivity and sensitivity of gas sensors, and the edge of graphene with hydroxyl groups shows the highest enhancement. Graphene with a carbonyl group was found to undergo irreversible chemisorption of NO2, which can potentially cause active material degradation, limiting the recyclability of gas sensors. Most of the molecules show both donor and acceptor behavior, which highlights the importance of a thorough selection of specific functional group types. The obtained results are useful for the rational design of graphene-based active material with oxygen-containing functional groups for chemiresistive gas sensors.

Computational Insight into the Physical Properties of Bulk MP (M = Li, Na, K) for Energy Applications.

In this study, we applied density functional theory to compute the electronic, optical, and thermal properties of MP (M = Li, Na, K). We find that the materials under consideration are stable, owing to the lack of negative frequencies in the phonon spectra. LiP exhibits an indirect band gap of 1.43 eV. NaP and KP have direct band gaps of 1.67 and 1.76 eV, respectively. The family of these composites shows strong absorption, observed by their very sharp absorption edges and confirmed by their direct transition from the valence to conduction band. They exhibit strong absorption below 4.0 eV in the optical spectra, which could serve in a solar cell device. The thermal calculations show high zT values of 0.74, 0.78, and 0.64 at 300 K for LiP, NaP, and KP, respectively. Thus, our results could be promising for electronic and thermal devices.

Analysis of lattice deformation originated from residual stress on performance of aluminum nitride-based bulk acoustic wave resonators

With the development of MEMS technology to the nanometer scale, the influence of different process conditions on the performance of nano-devices can be calculated through the microscopic changes of materials. During the manufacturing process, the large residual stress from the film stack significantly influences the performance of devices, thereby reducing the wafer yield. Herein, we apply density functional theory to MEMS processes to reveal the intrinsic mechanism of how residual stress affects the performance of aluminum nitride-based bulk acoustic wave (BAW) resonators on an 8-inch high-resistance silicon wafer. The variation rule of physical properties of piezoelectric material aluminum nitride with different residual stresses is calculated via first-principles calculations. Through theory formula derivation, the piezoelectric-coupling constant (Kt2) of the bulk acoustic wave resonator is positively correlated with tensile residual stress, and the resonant frequency (fp, fs) is negatively correlated with tensile residual stress. The measurement results show that the average shifts of Keff2 is 0.12 % within −137 MPa and 183 Mpa residual stress, which is an excellent match with the theory prediction.

A DFTB study on the electronic response of encapsulated DNA nucleobases onto chiral CNTs as a sequencer

Sequencing the DNA nucleobases is essential in the diagnosis and treatment of many diseases related to human genes. In this article, the encapsulation of DNA nucleobases with some of the important synthesized chiral (7, 6), (8, 6), and (10, 8) carbon nanotubes were investigated. The structures were modeled by applying density functional theory based on tight binding method (DFTB) by considering semi-empirical basis sets. Encapsulating DNA nucleobases on the inside of CNTs caused changes in the electronic properties of the selected chiral CNTs. The results confirmed that van der Waals (vdW) interactions, π-orbitals interactions, non-bonded electron pairs, and the presence of high electronegative atoms are the key factors for these changes. The result of electronic parameters showed that among the CNTs, CNT (8, 6) is a suitable choice in sequencing guanine (G) and cytosine (C) DNA nucleobases. However, they are not able to sequence adenine (A) and thymine (T). According to the band gap energy engineering approach and absorption energy, the presence of G and C DNA nucleobases decreased the band gap energy of CNTs. Hence selected CNTs suggested as biosensor substrates for sequencing G and C DNA nucleobases.

Dissolved gases analysis in transformer oil using TM (Pd, Ir, Au) modified MoSSe monolayer: A DFT study

This study applied density functional theory to investigate gas-sensitive devices based on transition metal-doped MoSSe (Pd-MoSSe, Ir-MoSSe, Au-MoSSe), exploring their adsorption and sensing performance towards three characteristic gases (CO, C2H2, C2H4) generated during the use or faults of transformer oil. The results indicate that Pd, Ir, and Au transition metal atoms preferentially anchor to the S surface of the pristine MoSSe monolayer. The doped monolayers exhibit significantly improved sensing characteristics in all aspects, suggesting chemical adsorption of the three characteristic gases. Through the analysis of band structures (BS), adsorption configurations, deformation charge densities (DCD), density of states (DOS), recovery time, and various adsorption parameters, the conclusion is drawn that while TM-MoSSe outperforms the pristine MoSSe monolayer in terms of adsorption and sensing performance, Pd-MoSSe and Au-MoSSe exhibit relatively good recovery times across a broader temperature range, whereas Ir-MoSSe is limited in this aspect. This study provides theoretical guidance for the potential application of transition metal-doped MoSSe monolayers as sensors for gases generated during the thermal runaway of transformer oil.

DFT study of mechanical, optoelectronic, and thermoelectric characteristics of double perovskites Li2CuTiZ6 (Z = Cl, Br, I) for energy harvesting technology

Recent studies have produced stable inorganic perovskites that contain no lead, replacing lead-containing perovskites' risky and unstable properties. The present investigation thoroughly examined the electrical behavior, elastic characteristics, optical features, and transport properties of Li2CuTlZ6 (Z = Cl, Br, I) halides in order to discover potential applications. The Wien2k code was utilized to apply density functional theory (DFT) in order to clarify these physical properties. Using the generalized gradient approximation (PBEsol-GGA), we determined structural parameters through the energy optimization procedure that corresponded with the available data. Additionally, elastic parameters as well as formation energies ranging between -2.33 to -1.39 eV were used to validate cubic durability for the two halides. Moreover, the modified Becke-Johnson (mBJ) potential successfully provided precise direct bandgap values for all halides. According to this study, the shift in anions from Cl to Br is responsible for the reduction in band gap within the infrared spectrum. Our computed optical parameter findings show that Li2CuTlCl6 and Li2CuTlBr6 halides demonstrate excellent optoelectronic efficiency with low reflection, strong optical absorption, and conductivity. The investigation clarifies that the temperature-dependent character of the materials electrical transport properties is due to their very small bandgap. These materials may find use in thermoelectric applications, as evidenced by the almost unity of the obtained figure of merit, which points to their semiconducting behaviour.

Preparation of surface molecularly imprinted polymers with Fe3O4/ZIF-8 as carrier for detection of Dimethoate in cabbage

In this study, molecularly imprinted polymers (MIPs) were prepared for the specific recognition of organophosphorus pesticides and a rapid, efficient and simple method was established for the detection of dimethoate (DIT) in food samples. Fe3O4 magnetic nanoparticles were synthesized by co-precipitation, and Fe3O4/ZIF-8 complexes were prepared by a modified in-situ polymerization method, and then magnetic molecularly imprinted polymers (MMIPs) were prepared and synthetic route was optimized by applying density functional theory (DFT). The morphological characterization showed that the MMIPs were coarse porous spheres with an average particle size of 50 nm. The synthesized materials are highly selective for the organophosphorus pesticide dimethoate with an adsorption capacity of 461.50 mg·g−1 and are effective resistance to matrix effects. A novel method for the determination of DIT in cabbage was developed using the prepared MMIPs in combination with HPLC. The practical results showed that the method can meet the requirements for the determination of DIT in cabbage with recoveries of 85.6–121.1 % and detection limits of 0.033 μg·kg−1.

Optimizing lithium-silver alloy phases for enhanced energy density and electrochemical performance

Lithium (Li) metal batteries though with high energy density are still facing issues like Li dendrite growth, dead Li formation, and thick solid electrolyte interphase (SEI) formation, hindering their long-term stability. Recently, Li-Ag alloys have been reported to potentially address these challenges possibly due to their superior conductivity, lithiophilicity, and mechanical stability. In the pursuit of high-energy-density batteries, Li-Ag alloys typically employ a high Li content phase (γ1). In this study, we applied density functional theory (DFT) calculations to compare the thermodynamic stability, Li adsorption, and Li diffusion of Ag-rich Li-Ag alloy within the γ1 phase (AR-γ1), Ag-poor Li-Ag alloy within the γ1 phase (AP-γ1), and pure Li. AR-γ1 showed better thermodynamic stability and improved Li adsorption and diffusion properties compared to AP-γ1 and pure Li. Electrochemical tests further confirmed the advantages of AR-γ1 in terms of electrode kinetics and cell stability compared to AP-γ1 and pure Li. Our study offers guidance for the selection of the most suitable Li-Ag alloys that can be utilized in high-energy-density lithium batteries.