La Site Research Articles

Mechanism and Kinetics of Ethanol–Acetaldehyde Conversion to 1,3-Butadiene over Isolated Lewis Acid La Sites in Silanol Nests in Dealuminated Beta Zeolite

Mechanism and Kinetics of Ethanol–Acetaldehyde Conversion to 1,3-Butadiene over Isolated Lewis Acid La Sites in Silanol Nests in Dealuminated Beta Zeolite

Experimental and computational investigations of biodiesel production from castor oil using Li-doped salmon fish bone-supported lanthanum oxide catalyst in a micro-reactor

Ensuring efficient and sustainable biodiesel production is essential for addressing environmental concerns and meeting global energy demands. This study aims to optimize the transesterification of castor oil through the development of a distinctive Li-doped-salmon fish bone (SFB)-supported La2O3 composite catalyst within a micro-reactor setup. The optimal catalyst (3 % Li/SFB-La) was thoroughly evaluated for its physicochemical features employing a range of characterization techniques, including XRD, XPS, BET, FESEM, TEM, TGA/DSC, and FT-IR. According to density functional theory (DFT) calculations, the function of Li dopants, which have a lower electronegativity (0.98) compared to La (1.1), is to enhance the charge transfer capability of La sites, thereby increasing their reactivity with triglycerides. In the interim, we determined the optimized reaction conditions: a 6:1 methanol/oil molar ratio and a 5 wt % catalyst loading at 338 K. Under these parameters, an impressive 99.38 % conversion was achieved within 1.5 h. Furthermore, the 3 % Li/SFB-La composite catalyst exhibited remarkable stability, retaining its high activity throughout 7 cycles without any significant loss of efficacy. Moreover, the transesterification reaction kinetics were thoroughly investigated, revealing a reaction rate constant of 1.17 h−1 and an activation energy of 14.46 kJ/mol.

Improved microwave dielectric properties of LaZn1/2Ti1/2O3 through Y3+ substitution

LaZn1/2Ti1/2O3 is a double perovskite with promising microwave dielectric properties for applications towards dielectric resonators and antennas. Its dielectric properties can be enhanced through the substitution of suitable ions in either A- or B-sites. In this paper, we report a significant improvement in the quality factor (Q) by substituting Y3+ in the La site with a marginal reduction in dielectric constant (εr). A single phase is confirmed in XRD indicating the formation of La1-xYxZn1/2Ti1/2O3 (0 ≤ x ≤ 0.25) solid solutions. The substitution results in an expansion of lattice along the b direction while there is a contraction in both a and c directions, leading to a reduction in unit cell volume. The dielectric constant, εr, is observed to reduce from 33.4 to 29.6 due to the polarizability of A-site atoms. The temperature coefficient of resonant frequency (τf) increases with an increase in x which does not appear to correlate with reducing tolerance factor (t). This non-conventional behaviour of τf in this perovskite based solid solutions brings bond valence of O site (VO) into picture. VO appears to show competing effect on τf. The non-monotonic behaviour is observed in Q×f with a maximum value of 41,400 GHz at x = 0.15 and a sharp decline for x > 0.15. This observation is correlated with variations in the A-site bond valence (VA) and a long-range ordering (LRO) of B-site ions. LRO is associated with Ag mode at 710 cm−1 in the Raman spectra. The low frequency (< 250 cm−1) Raman modes shift to a higher frequency with the increase in Y3+. Y3+ substitution also induces lattice distortion which is discussed in terms of variations in FWHM and relative intensity of the Raman modes.

Preparation of La-doped NiAl-LDH with boosted electron transfer for the enhanced photocatalytic activity of tetracycline: Performance evaluation, degradation pathway, and mechanism insight

Developing a photocatalysis-based system is an effective strategy for removing antibiotics. Herein, La-doped NiAl-layered double hydroxides (LaNiAl-LDH) photocatalyst was synthesized using a chemical co-precipitation-hydrothermal method. The prepared samples were characterized by various advanced analyses and investigated for the photocatalytic degradation of tetracycline (TC). The crystalline phase and functional groups of the synthesized samples were successfully confirmed by XRD and FTIR analyses. By doping La into NiAl-LDH structure, the band gap was reduced from 3.01 eV to 2.57 eV, indicating higher photocatalytic activity of 1% LaNiAl-LDH. The surface morphology of the synthesized samples shows the formation of nanosheets in the structure of LDH. Under the optimum status ([TC]0 = 10 mg/L, [1% LaNiAl-LDH] = 0.2 g/L, and pH = 6), the photocatalytic activity of 1% LaNiAl-LDH (84.85%) was higher than NiAl-LDH (71.52%) within 90 min reaction. This difference can be attributed to the presence of La sites in 1% LaNiAl-LDH which act as electron-transfer mediators, leading to a significant improvement in the separation of photogenerated charge carriers. The effect of the addition of various scavengers was evaluated. Moreover, using the o-phenylenediamine (OPD), and photoluminescence (PL) analysis, the formation of •OH radicals was supported. The higher charge-transfer efficiency of 1% LaNiAl-LDH was confirmed by photoelectrochemical analysis. Furthermore, the reusability, stability, and degradation pathway of the as-synthesized nanocomposite were systematically examined. This work presents guidance for applying doped LDH-based materials in photocatalysis and promising applications in wastewater remediation.

Regulating active oxygen species and acidity of Ca doped LaMnO3 perovskite catalysts toward efficient n-butylamine oxidation

It is of great significance to design catalysts with high activity, N2 selectivity and stability for nitrogen-containing volatile organic compound (NVOC) catalytic purification. Meanwhile, the role of oxygen species in NVOC catalytic oxidation is still ambiguous. Herein, the oxygen species of La-Mn perovskite catalysts were engineered by doping Ca in La site to elucidate their role in catalytic n-butylamine oxidation. Results demonstrate that La0.9Ca0.1MnO3 exhibits the highest activity owing to its abundant adsorbed oxygen species and high surface area, achieving 100 % n-butylamine conversion (500 ppm; GHSV=60,000 mL g−1h−1) at 200 °C with N2 selectivity of ca. 95 %. More adsorbed oxygen species generated due to Ca doping accelerates the oxidation rate and C-C cleavage of alcohol and acetate intermediates, resulting in higher CO2 yield. Meanwhile, Ca-doping also modifies the acidity of catalysts, which affects the adsorption/desorption process of alkaline substances and yield of nitrogen-containing products. In addition, La0.9Ca0.1MnO3 shows superior stability, high water and SO2 resistance, and acceptable activity for other common NVOCs, demonstrating a promising catalyst for NVOC oxidation even under harsh operation conditions. Furthermore, the toxic effect of pollutant or products during n-butylamine catalytic oxidation on the growth of Chlorella Vulgaris was investigated and results suggest that catalytic oxidation is an environmentally friendly method for NVOC purification. This work sheds light on the relationships among oxygen species, catalyst acidity, and n-butylamine catalytic oxidation, which expand the understanding of rational design of efficient catalyst for NVOC oxidation.

Experimental and Mathematical Investigation of Hydrogen Absorption in LaNi5 and La0.7Ce0.1Ga0.3Ni5 Compounds

In the present study, the hydrogen-absorption properties of the LaNi5 and the La0.7Ce0.1Ga0.3Ni5 compounds were determined and compared. This work is therefore divided into two parts: an experimental part that presents and discusses the kinetics and isotherms of hydrogen absorption in the two compounds at two different temperatures (298 K and 318 K). In addition, the temperature variations inside the hydride bed were determined. In the second section, the experimental isotherms were compared to a numerical model processed using statistical physics. Following that, thanks to the perfect agreement between the experimental data and the proposed model, the stereographic and energetic parameters associated with the hydrogen absorption reaction, such as the number of hydrogen atoms per receptor site (n1, n2), the densities of the sites (Nm1, Nm2), the half-saturation pressures (P1, P2) and the absorption energies (ΔE1, ΔE2) for each receptor site, were calculated. All of these parameters are acquired by making numerical adjustments to the experimental data. Thermodynamic functions, such as internal energy and Gibbs energy, which regulate the absorption process, were then identified using these parameters. For both compounds, all of the aforementioned were compared and discussed in relation to initial temperature and pressure. The results demonstrated that the hydrogen-storage properties in LaNi5 are enhanced by more than 30% of stored mass and kinetics when Ce and Ga are substituted at the La sites.

Mechanism of chromium poisoning on La0.5Sr0.5Co0.25Fe0.75O3 cathode and enhancing chromium tolerance using a novel anion doping strategy

Chromium poisoning the La1-xSrxCoyFe1-yO3(LSCF) cathode for solid oxide fuel cells is a severe issue that can lead to its electrochemical performance degradation. To clarify poisoning mechanism of chromium species and develop a novel anion doping strategy with enhancing chromium tolerance, the adsorption behavior of Cr species on LSCF and F-doping LSCF surface are explored by density functional theory (DFT) calculations. Our results indicate that CrO3 molecule prefers to be adsorbed on the La(Sr)O-terminated surface rather that the Co(Fe)O2-terminated LSCF(001) surface. The adsorption energies of CrO3 molecule are much larger than that of O2 molecules, implies that the CrO3 is more favorable to absorb on the LSCF surface. Bader charge analysis shows the CrO3 molecule behaves as an electron acceptor through an adsorption process. The adsorption of Cr atom is a weak physical adsorption for Sr site and La site and the Cr atom chemisorption is found to occur on hollow site and O site. In addition, F-doping efficiently improves chromium tolerance by weakening the adsorption strength of chromium species that poisons LSCF surface and this may be a feasible strategy to develop cathode for high performance solid oxide fuel cells.

Tailoring Co site reactivity via Sr and Ni doping in LaCoO3 for enhanced water splitting performance

Perovskite oxides (ABO3) featuring rare-earth cations in the A-site and first-row transition-metal cations in the B-site, have emerged as promising catalytic materials for addressing the slow kinetics of the water splitting reaction. In this study, we synthesized La1-xSrxCo1-yNiyO3 using the solution combustion synthesis method and conducted a comprehensive investigation into the structural, surface, and electronic properties of the resulting materials. The strategic doping of Sr in La sites and Ni in Co sites has notably enhanced the kinetics and effectiveness of both the oxygen evolution reaction at the anode and the hydrogen evolution reaction at the cathode, leading to an overall improvement in water splitting efficiency over La1-xSrxCo1-yNiyO3. Detailed mechanistic studies have revealed the crucial role of high covalency and surface oxygen vacancies, tailored through aliovalent doping, in enhancing the catalytic activity of the oxygen evolution reaction in La1-xSrxCo1-yNiyO3. This research serves as a pioneering effort to establish a correlation between electronic and surface properties and to elucidate the mechanistic aspects of water splitting over perovskite materials.

Mesopore-rich La-based metal organic framework derivatives for phosphorus removal from mariculture tailwater

Deep dephosphorization of mariculture tailwater, a typical high-salinity and weakly alkaline wastewater, is difficult but essential for meeting ever-stricter stringent emission standards. Herein, we developed an alkaline-conversion method to prepare lanthanum-based metal organic framework (La–MOF) derivatives for efficient phosphate removal from mariculture tailwater. During the templated alkaline-conversion process, the strong-alkaline regent gradually broke the coordination bonds of La–MOF while maintained its macrostructure, and the La nodes liberated from the framework were then crystallized into La(OH)3. The universality of this conversion method was verified on other La–MOF precursors with different benzoic multicarboxylate ligands. Importantly, numerous mesopores were formed in the derivative interior, increasing the number of exposed active La sites and accessible transfer channels. Therefore, the derivative exhibited superior phosphate-adsorption performance with a high adsorption capacity (Langmuir Q0: 155.7 mg P/g) and a rapid adsorption rate. The obtained La–MOF derivative with stable structure had broad neutral–alkaline pH range adaptability, which was demonstrated satisfactory dephosphorization selectivity and high cyclic performance under different seawater conditions (coexisting anions, cations, H3BO3 and natural organic matter). Finally, the obtained mesopore-rich La–MOF derivative exhibited an excellent deep dephosphorization capacity for actual mariculture tailwaters collected from seven mariculture ponds. The reactive phosphate level was quickly reduced to an ultra-low effluent concentration (<0.05 mg P/L), demonstrating the promising application potential of the La–MOF derivative.

Atomic S, H and C adsorption on MnO(001) surface and the interaction between H and LaCrO3(001) surface: A computational analysis

S poisoning and C deposition are key factors to cause performance degradation of solid oxide fuel cells (SOFC) anodes. The adsorptions of atomic S, H and C on MnO(001) surface and atomic H on LaCrO3(001) surface are systematically investigated using density functional theory (DFT) calculations. The analysis of surface relaxation shows that surface Mn ion slightly moves toward the slab center and surface O ion moves outward on MnO(001) surface. According to the result of adsorption energy, it can be inferred that the MnO weakens the adsorption of atomic S with lower adsorption energies compared to LaCrO3 surface. In addition, the findings show that the preferred site for atomic H adsorption is O site, with the adsorption energy of －1.361 eV, which results in the formation of –OH surface species. Compared to O sites on LaCrO3(001) surface, the atomic H is found to interact weakly with the La and Cr sites. The distances and charges transfer between adsorbate and substrate have also been analyzed. The obtained results are expected to provide some fundamental information for future research on mechanism of S poisoning and C deposition on SOFC anodes.

Enhanced conductivity in Sr doped La3Ni2O7-δ with high-pressure oxygen annealing

The structural, electrical and magnetic properties of a series of La3-xSrxNi2O7-δ polycrystalline samples have been systematically investigated with and without high-pressure oxygen annealing. Without annealing, the introduction of Sr at La site leads to a moderate enhancement of conductivity. The high-pressure oxygen annealing leads to an increase of oxygen content by ∼1.08 %. Consequently, the conductivity of the annealing samples is significantly enhanced comparing to the untreated samples. The La3-xSrxNi2O7-δ samples exhibit metal-like behavior in the whole temperature range with annealing, which is due to the hole doping effect. The present results could contribute to the exploration of possible ambient superconductivity in La3Ni2O7-δ system.

Monodispersed and Organic Amine Modified La(OH)3 Nanocrystals for Superior Advanced Phosphate Removal.

Advanced phosphate removal is critical for alleviating the serious and widespread aquatic eutrophication, strongly depending on the development of superior adsorption materials to overcome low chemical affinity and sluggish mass transfer at low phosphate concentrations. Herein, the first synthesis of monodispersed and organic amine modifiedlanthanum hydroxide nanocrystals (OA-La(OH)3) for advanced phosphate removal by modulating inner Helmholtz plane (IHP), is reported. These OA-La(OH)3 nanocrystals with positively charged surfaces and abundant exposed La sites exhibitspecific affinity toward phosphate, delivering a maximum adsorption capacity of 168mg Pg⁻1 and a wide pH adaptability from 3.0 to 11.0, as well as a robust anti-interference performance, far surpassing those of documented phosphate removal materials. The superior phosphate removal performance of OA-La(OH)3 is attributed to its protonated organic amine in IHP, which enhances the electrostatic attraction around the adsorbent-solution interface. Impressively, OA-La(OH)3 can treat ≈5 000 and ≈3 200 bed volumes of simulated and real phosphate-containing wastewater to below extremely strict standard (0.1mgL⁻1) in a fixed-bed adsorption mode, exhibiting great potential for advanced phosphate removal. This study offers a facile modification strategy to improve phosphate removal performance of nanoscale adsorbents, and sheds light on the structure-reactivity relationship of La-based materials.

Insights in the phase stability and performance enhancement mechanism of La2(Zr1-xCex)2O7 with reduced thermal conductivity

This study proposes a molten salt method-based process for the synthesis of Ce-doped pyrochlore-phase La2(Zr1-xCex)2O7, aiming to develop materials with excellent comprehensive properties, particularly for thermal barrier coatings. The results indicate that by employing the proposed method, the Ce doping level (x) can reach 0.4 for pyrochlore-phase La2(Zr1-xCex)2O7. However, high-temperature testing reveals a reduction in the phase stability of the samples. As the value of x increases, the temperature at which the samples exhibit the fluorite phase gradually decreases. DFT calculations on the crystal formation energy of La2(Zr1-xCex)2O7 confirm that an elevated level of Ce doping leads to an increase in crystal formation energy, indicating a decrease in phase stability. Subsequent thermal conductivity tests on La2(Zr1-xCex)2O7, along with theoretical thermal conductivity fitting, reveal a significantly greater fitting error for Ce doping at the Zr site compared to La site doping with other rare earth elements. Finally, XPS and EPR tests conducted on the samples doped at the Zr and La sites confirm that oxygen vacancies induced by high Ce doping levels play a crucial role in reducting the thermal conductivity of La2(Zr1-xCex)2O7.

Bandgap Energy of Ion‐Doped LaMnO3 Nanoparticles

Based on the s‐d model combined with Green's function technique, the magnetization and the bandgap energy of ion‐doped nanoparticles at La sites are calculated. Due to the change of the valency of Mn ions, from to , as well as the difference between the ionic radii of the doping and host ions, the exchange interaction is modified which allows a tuning of the magnetization and the bandgap energy. For nanoparticles, the bandgap is decreased by Ag and Ba doping, whereas it is increased by K and Sr doping. Macroscopic quantities such as the magnetization and the bandgap energy are directly related to microscopic parameters of the model. The simulations are qualitatively in good agreement with the experimental data.

Heterostructure anion-groups guided design enabling customizable Eu2+ spectrum behavior in borophosphate☆

Definite emission color from rare-earth Eu2+ cannot be guaranteed in distinct hosts because its spectrum behavior is strongly dependent on surrounding microenvironment. Herein, we propose a strategy of heterostructure polyhedron BO3-PO4 substitution that can realize customizable and even predictable Eu2+ emission. Taking Sr3La(PO4)3:Eu2+ blue phosphor as host, we prepared a series of BO3-PO4 substitution-designed Sr3La(PO4)3−x(BO3)x:Eu2+ (SLP3−xBx:Eu2+) phosphors via solid-state reaction. Structural and spectral analyses demonstrate that substitution of PO4 with BO3 unit drives Eu2+ to migrate from original occupied Sr sites to unoccupied six-coordinated La sites, bringing out a brand-new broadband yellow-emitting peak at 530 nm, enabling an efficient spectrum tailoring from initial blue emission at 420 nm to white-light and then yellow. Strikingly, we find that the resultant Eu2+ spectrum behavior in as-prepared SLP3−xBx:Eu2+ and Eu2+-doped other borophosphate phosphors is highly similar (although they have different microenvironments). Such exciting findings indicate that proposed BO3-PO4 substitution-strategy possesses an ability of predicting emission by modulating Eu2+ site-selective occupation. Utilizing SLP3−xBx:Eu2+ (x = 0.1 and 0.4) phosphors, we fabricated optical temperature sensor and white LED prototypes, showcasing remarkable temperature sensitivity of Sr = 1.1%/K and good color rendering index (CRI) of 83. This work may aid the discovery of novel functional materials with specific, desirable physicochemical properties.

Atomic Strain Wave-Featured LaRuIr Nanocrystals: Achieving Simultaneous Enhancement of Catalytic Activity and Stability toward Acidic Water Splitting.

Rare earth microalloying nanocrystals have gotten widespread attention due to their unprecedented performances with customization-defected nanostructures, divided energy bands, and ensembled surface chemistry, regarded as a class of ideal electrocatalysts for oxygen evolution reaction (OER). Herein, a lanthanide microalloying strategy is proposed to fabricate strain wave-featured LaRuIr nanocrystals with oxide skin through a rapid crystal nucleation, using thermally assisted sodium borohydride reduction in aqueous solution at 60°C. The atomic strain waves with alternating compressive and tensile strains, resulting from La-stabilized edge dislocations in form of Cottrell atmospheres. In 0.5m H2SO4, the LaRuIr displays an overpotential of 184mV at 10mA cm-2, running at a steadily cell voltage for 60h at 50mA cm-2, eightfold enhancement of IrO2||Pt/C assemble in PEMWE. The coupled compressive and tensile profiles boost the OER kinetics via faster AEM and LOM pathways. Moreover, the tensile facilitates surface structure stabilization through dynamic refilling of lattice oxygen vacancies by the adsorbed oxyanions on La, Ru, and Ir sites, eventually achieving a long-term stability. This work contributes to developing advanced catalysts with unique strain to realize simultaneous improvement of activity and durability by breaking the so-called seesaw relationship between them during OER for water splitting.

Enhancement of microstructure and electrochemical properties of LLZTO solid state electrolyte by co-doping with Ga and Y

Recently, there has been strong interest in inorganic solid-state electrolytes for all-solid-state batteries, among which the garnet electrolyte LLZO has attracted much attention due to its excellent properties, such as high ionic conductivity and broad electrochemical stability. The aim of our study was to improve the performance of Ta-doped LLZO (LLZTO) by co-doping Ga and Y at the Li and La sites using conventional solid-phase synthesis methods. We thoroughly investigated how Ga and Y affect the microstructure and electrochemical properties of LLZTO. The results show that the relative density of Ga- and Y-doped LLZTO increases significantly up to 94% under the same sintering conditions. This doping resulted in a significant increase in ionic conductivity from 2.0 × 10−4 S·cm−1 to 1.05 × 10−3 S·cm−1 and a decrease in electronic conductivity from 2.16 × 10−7 S·cm−1 to 9.18 × 10−8 S·cm−1. Subsequently, the symmetric cells were assembled and tested, and it was found that the interfaces of the doped solid-state electrolytes were much more stable and that the cycling time was longer. Thus, our study successfully coordinated the co-doping of Ga, Y, and Ta, providing valuable insights for the subsequent production of LLZO materials with higher densities and better performance. This study is a promising step toward the realization of safer all-solid-state batteries with higher energy densities.

Effect of Ca doping on Li ion conductivity of Ge and Ta doped garnet LLZO

The series Li6.55+xGe0.05La3-xCaxZr1.75Ta0.25O12 (x = 0, 0.05, 0.10, 0.15, 0.20) was prepared by conventional solid state reaction method with the sintering temperature of 1050 °C for 7.30 h by substituting Ca at the La site to increase the Li ion conductivity. The synergistic effects of Ca incorporation on Li6.55Ge0.05La3Zr1.75Ta0.25O12 were studied using various structural and electrochemical analyses. X-ray diffraction, scanning electron microscopy, and Impedance analysis were used to determine the crystal structure, morphology, and AC conductivity of the prepared ceramic samples, respectively. The highest conductivity of 9.95 x 10−4 S/cm was obtained for a 0.05 Ca ceramic sample with minimum activation energy of 0.23 eV. The DC polarization measurements confirmed the dominance of ionic conduction in 0.05 Ca ceramic. The results obtained make the 0.05 Ca ceramic sample a promising candidate as solid electrolytes for all solid state Li-ion batteries (ASSLIBs).

Frustrated Lewis Pairs on Zr Single Atoms Supported N‐Doped TiO2‐x Catalysts for Electrochemical Nitrate Reduction To Ammonia

AbstractThe electrochemical reduction of nitrates (NO3RR) for ammonia synthesis at room temperature holds immense potential. One key challenge is the adsorption and activation of NO3−, along with the provision of sufficient active hydrogen to accelerate the hydrogenation process. Here, the study prepares N‐doped TiO2‐x supported by Zr single atoms (Zr‐TiON) with rich oxygen vacancies (Ov), in which unsaturated Zr (Lewis acidic, LA) sites together with oxygen atoms around Ov (Lewis base, LB) form frustrated Lewis acid‐base pairs (FLPs). At −60 mA cm−2, NH3 Faradaic efficiency reaches 94.8%, corresponding to the production rate of 663.15 µmol h−1 mgcat−1. The yield rate is up to 26.16 mmol h−1mgcat−1 at −1 A cm−2 in flowing electrolyzer. Theoretical calculations and in situ spectroscopy analysis reveal that the interaction between LA and LB sites in FLPs plays a crucial role in facilitating adsorption and activation of electron‐rich NO3− and electron‐deficient *H. The presence of enhanced FLPs significantly reduces the energy barrier for H2O dissociation, lowering it to 0.20 eV, which facilitates subsequent hydrogenation reactions. The abundance of *H accelerates hydrogenation process, thereby enhancing the activity of NO3RR. This FLP design offers a promising approach for paving the way for the development of highly efficient NO3RR catalysts.

Experimental and Computational Study of Mg and Ta‐Doped Li7La3Zr2O12 Garnet‐Type Solid Electrolytes for All‐Solid‐State Lithium Batteries

AbstractGarnet‐type Li7La3Zr2O12 electrolytes have garnered significant attention as promising solid‐state electrolyte candidates in all‐solid‐state lithium batteries (ASSLBs). However, its susceptibility to forming Li2CO3 upon atmospheric exposure leads to performance degradation, limiting its application. This study introduces a co‐doping strategy of Mg and Ta to enhance the properties of garnet electrolytes. Pure cubic Mg and Ta‐doped LLZO electrolytes are successfully synthesized using the solid‐state reaction method. Experimental results, coupled with density functional theory (DFT) calculation, reveal that Mg2+ doping occurs primarily at the La site (24c). This substitution, given the substantial disparity in ionic radii between Mg2+ and La3+, effectively narrows the transport bottleneck for Li‐ions, resulting in a decreased ionic conductivity and an increased activation energy. Li6.6La2.8Mg0.2Zr1.4Ta0.6O12 exhibits a relative density of ≈92.6%, demonstrating outstanding performance with a room temperature ionic conductivity of 4.31 × 10−4 S cm−1 and low electronic conductivity of 2.48 × 10−8 S cm−1. Notably, after 4 months of atmospheric exposure, its ionic conductivity decreased to ≈78% of the initial value, attributable to Li2CO3 formation. Furthermore, the material demonstrated exceptional long‐term cycle stability over 1000 h at a current density of 0.1 mA cm−2 at 25 °C, indicating effective suppression of Li dendrite formation.