Hydrogen Adsorption Energy Research Articles

A strongly coupled 1T'-ReSe2@2H-MoSe2 van der Waals heterostructure for efficient electrocatalytic hydrogen evolution at high current densities.

Developing efficient and durable non-noble metal electrocatalysts for high current-density hydrogen evolution reactions (HER) is a pressing requirement for commercial industrial electrolyzers. In this study, a vertical 1T'-ReSe2@2H-MoSe2 van der Waals heterostructure was developed through interface engineering to enhance the advantages of each component and expose numerous active sites. Experimental investigations and density functional theorycalculations demonstrate significant electronic coupling at the interface between 1T'-ReSe2 and 2H-MoSe2, with suitable Gibbs free energy for hydrogen adsorption. The 1T'-ReSe2@2H-MoSe2 heterostructure catalyst achieves high current density HER with low overpotentials of 191 mV to generate up to 800 mA/cm2 in 0.5 M H2SO4, outperforming commercial 5% Pt/C catalysts. Moreover, this catalyst exhibits rapid reaction kinetics and long-term durability, illustrating a successful approach to designing efficient heterostructure electrocatalysts for hydrogen production through interface engineering.

Mo Migration‐Induced Crystalline to Amorphous Conversion and Formation of RuMo/NiMoO4 Heterogeneous Nanoarray for Hydrazine‐Assisted Water Splitting at Large Current Density

AbstractManipulating the atomic structure of the catalyst and tailoring the dissociative water‐hydrogen bonding network at the catalyst‐electrolyte interface is essential for propelling alkaline hydrogen evolution reaction (HER) and hydrazine oxidation reaction (HzOR), but remains a great challenge. Herein, we constructed an advanced a‐RuMo/NiMoO4/NF heterogeneous electrocatalyst with amorphous RuMo alloy nanoclusters anchored to amorphous NiMoO4 skeletons on Ni foam by a heteroatom implantation strategy. Theoretical calculations and in situ Raman tests show that the amorphous and alloying structure of a‐RuMo/NiMoO4/NF not only induces the directional evolution of interfacial H2O, but also lowers the d‐band center (from −0.43 to −2.22 eV) of a‐RuMo/NiMoO4/NF, the Gibbs free energy of hydrogen adsorption (ΔGH*, from −1.29 to −0.06 eV), and the energy barrier of HzOR (ΔGN2(g)=1.50 eV to ΔGN2*=0.47 eV). Profiting from these favorable factors, the a‐RuMo/NiMoO4/NF exhibits excellent electrocatalytic performances, especially at large current densities, with an overpotential of 13 and 129 mV to reach 10 and 1000 mA cm−2 for HER. While for HzOR, it needs only −91 and 276 mV to deliver 10 and 500 mA cm−2, respectively. Further, the constructed a‐RuMo/NiMoO4/NF||a‐RuMo/NiMoO4/NF electrolyzer demands only 7 and 420 mV to afford 10 and 500 mA cm−2.

Regulating oxygen vacancies to optimize the electronic structure and catalytic activity of tungsten oxides for hydrogen evolution reaction

The undesirable intrinsic activity of tungsten oxides derived from poor conductivity and adverse hydrogen absorption energy is insufficient for their practical application. Herein, the tungsten oxides with adjustable oxygen vacancies were synthesized by a facile pyrolysis of ammonium paratungstate hydrate in controllable atmospheres. The structural characterizations confirmed that oxygen vacancies and crystalline phases in tungsten oxides depend on the pyrolysis atmosphere. The electrochemical test indicated a strong dependence between catalytic activity and oxygen vacancies in tungsten oxides. Combining experimental results and density functional theory calculations verified that introducing oxygen vacancies into tungsten oxides effectively modulates the surface electronic structure. The enhanced electronic conductivity by reducing band gap accelerates the electron transfer from catalysts into the reactive species. The optimized hydrogen adsorption energy by electron migration from O into W promotes the activation of reactive species at W sites and the desorption from O sites, thereby accelerating the reaction kinetics.

Controllable morphology of Pd nanostructures: from nanoparticles to nanofoams

Abstract Metallic nanofoams offer enhanced surface area and reduced density compared to their bulk counterparts while keeping intrinsic metallic properties. This combination makes nanofoams ideal for many applications, such as catalysis and battery. However, the synthesis of nanofoams is still challenging. This work introduces a non-complex synthesis method of Pd nanofoams employing a polar lipid structured as a sponge phase in water. The Pd nanostructures were characterized using Scanning Electron Microscopy (SEM), Transmission Electron Microscopy (TEM), X-Ray Diffraction (XRD), N2 adsorption-desorption isotherms, X-Ray Photoelectron Spectroscopy (XPS), and X-Ray Absorption Near Edge Structure (XANES) at Pd K edge techniques. The morphology of the nanostructure, from nanofoam to nanoparticle, is easily controlled by the presence of the polar lipid and the Pd salt used. The Pd nanostructures synthesized are fully oxidized, but the nanofoams reduce quickly (less than 5 minutes) to metallic Pd after H2 exposure at room temperature. The nanostructures were applied for hydrogen storage and Pd nanofoams achieved a remarkable gravimetric capacity of 0.76 wt.% at room temperature and 1 atm H2 pressure. DFT calculation showed that the changes in the morphology of Pd lead to great changes in the adsorption energy of hydrogen, thus allowing the improvement of the material for hydrogen storage applications through the method developed.

Ti-decorated B-doped biphenylene: A hydrogen storage sponge at room temperature

It has always been a difficult problem to design Kubas-type hydrogen storage materials that make hydrogen molecules activate but do not dissociate. Density functional theory calculations confirm that Ti decorated B-doped biphenylene is the first two-dimensional room-temperature hydrogen storage sponge reported so far. The hydrogen adsorption energy of Ti-decorated B-doped biphenylene is in the range of −0.29 ∼ −0.51 eV with hydrogen storage capacity is 6.58–9.13 wt%. What's very interesting and exciting is that the Kubas interaction between Ti sites and H2 can be regulated by changing the electron occupation state of the dx2-y2 orbitals of Ti, and this regulation can be realized through the uniaxial lattice strain in the XOY plane. The average hydrogen adsorption energy of tensile Ti-decorated B-doped biphenylene ranges between −0.34 ∼ −0.66 eV, while −0.22 ∼ −0.48 eV for compressed one. This process makes the reversible hydrogen storage as simple and feasible as a sponge absorbing water. This study provides clear structural for the transformation mechanism to form a folded structure and also provides an important precedent model.

Integrating Pt single atoms and Mo into PtNi/C through Mo doping-displacement synchronisation strategy for enhanced HER at all pH values

This paper proposes a Mo doping-displacement synchronization strategy to integrate Pt SAs and Mo atoms into PtNi/C, synthesizing Pt SAs/Mo-doped PtNi octahedra/carbon support catalyst (Pt SAs/Mo-PtNi/C). In this approach, Mo atoms are doped into PtNi alloy octahedra and displace some Pt atoms, forming Mo-PtNi octahedra. Importantly, the substituted Pt atoms can adhere to carbon substrate, creating Pt SAs. Pt SAs/Mo-PtNi/C exhibits lower overpotentials (38, 59, and 110 mV at 10 mA cm−2) and smaller Tafel slopes (44, 51, and 139 mV dec-1) in acidic, alkaline, and neutral environments. Additionally, the electron pathway of Mo-PtNi → Pt SAs/C has been confirmed, and Pt SAs/Mo-PtNi/C exhibits an optimized hydrogen adsorption energy (ΔGH*=-0.29 eV). Furthermore, catalyzed by Pt SAs/Mo-PtNi/C, the H-O bond length of H2O extends to 1.11 Å and the bond angle reduces to 102.741°, directly confirming that the Pt SAs and doped Mo could facilitate H-O bond breaking. The proposed Mo doping-displacement synchronization strategy not only simplifies the fabrication process of Pt SAs catalyst, but also improves its durability and activity across a wide pH range, thereby potentially advancing hydrogen production technologies.

Sparkling Synergy: Enhancing Hydrogen Evolution with a Mesoporous CoP/FeP Interface.

The reaction kinetics is predominantly determined by the surface and interface engineering of electrocatalysts. Herein, we demonstrate the growth of cobalt monophosphide and iron monophosphide (CoP/FeP) with an effective solid interface. The surface of CoP/FeP is mesoporous, which is obtained by phosphidizing mesoporous CoFe2O4. The CoP/FeP electrode exhibits substantially superior hydrogen evolution reaction (HER) performance compared to CoP and FeP. The overpotentials (η) required to generate 10 mA cm-2 are determined to be around 98 mVRHE (CoP/FeP), 220 mVRHE (FeP), and 265 mVRHE (CoP) in an acidic electrolyte. The exchange current density and Tafel slopes suggest that CoP/FeP has better redox properties and kinetic abilities compared to FeP and CoP. Furthermore, the CoP/FeP electrode exhibits reduced electrochemical impedance and superior surface charge transport characteristics in comparison to both the CoP and FeP electrodes. In addition to having a greater number of catalytically active sites, the turnover frequency of CoP/FeP is approximately 2 and 5 times higher than that of FeP and CoP, respectively. The CoP/FeP electrode maintains a consistent current density of around 25 mA cm-2 for a continuous period of 24 h during the HER, attesting to the excellent durability of the CoP/FeP electrode. In addition, a relationship between differential hydrogen adsorption energy (ΔEH), the corresponding Gibbs free energy change (ΔGH), and the hydrogen coverage on distinct surfaces, namely, CoP, FeP, and CoP/FeP, is established. The calculation findings show that the CoP/FeP surface, which is predominantly exposed with CoP, exhibits the highest catalytic potential for the HER. The estimation of the specific HER activity of the electrodes, normalized to the electrochemically active surface area, corroborates the calculation findings.

Ingenious regulation and activation of sites in the 2H-MoS2 basal planes by oxygen incorporation for enhanced photocatalytic hydrogen evolution of CdS

The 2H phase of MoS2 has the advantages of stable phase structure and tunable preparation approach, while the unfavorable H adsorption ability at the basal plane sites hinders the H2 evolution performance. Here, we developed an effective strategy for the regulation of the basal plane properties of MoS2 via oxygen doping. It is demonstrated that the Gibbs free energy of hydrogen adsorption (ΔGH*) at the sites in the basal plane can be effectively optimized. Using oxygen-doped MoS2 (OMoS) as a cocatalyst, the constructed OMoS/CdS heterojunction photocatalyst shows a stronger built-in electric field and improved photocatalytic H2 production activity. The optimized OMoS/CdS sample with only 0.3 wt% OMoS loading amount achieved an H2 evolution rate of 58.47 mmol g-1h−1 under AM 1.5 light irradiation, which is significantly superior to that of conventional MoS2 modified CdS and even higher than the 1 wt% Pt modified CdS. Our results not only highlighted the significant potential of OMoS as a photocatalyst for hydrogen production, but also proposed a superior to and effective conception for optimizing the H2 evolution activity at the basal plane sites of 2H-MoS2.

Machine learning prediction of hydrogen adsorption energy on platinum nanoclusters: A comparative study of SOAP descriptors

Hydrogen binding energy in metal materials is of high significance in the hydrogen storage as well as the hydrogen evolution reaction of electrocatalysis. In this work, the datasets (more than 9000 data) of hydrogen adsorbed on Pt nanoclusters with different sizes are obtained by first-principles calculations. Data analysis shows that the binding strength of hydrogen with Pt is closely relevant to the local structures of the adsorption sites. The local features of the distance between the platinum and hydrogen and the size of the nanoclusters are supplemented to the Smooth Overlap of Atomic Positions descriptors to fit and predict the adsorption energies of hydrogen on different Pt nano-structures by performing the machine learning method. Gaussian Process Regression (GPR) and Random Forest Regressor (RFR) are used to construct the prediction model of hydrogen binding energies and it is found the R2 of test set is improved from 0.63 to 0.78 with modified descriptors. By applying it into other nanoclusters, the MAE of the prediction model is 0.08 eV, which exhibits high accuracy of the hydrogen adsorption energy. Our model can be easily extended to the prediction of hydrogen adsorption energy of other materials with affordable computational cost and accuracy, which would be helpful for the structural design of high-performance catalysts.

Designing Mo-based transition metal dichalcogenides for sustainable hydrogen production: Anionic substitution and DFT insight

Anionic substitution is an effective approach to optimize the catalytic activity of Mo based transition metal dichalcogenide (TMD)- MoS2 towards hydrogen evolution reaction (HER). By optimizing the S-to-Se ratio, materials with the ideal Gibbs free energy of hydrogen adsorption (ΔGH) values are synthesized (MoS2, MoS1.4Se0.6, MoS1.2Se0.8, MoSSe, MoSe2) and their HER performance is examined in 0.5 M H2SO4 solution. Density functional theory calculations of hydrogen adsorption energy on the surface of the electrocatalysts show that Se substitution facilitates electron transfer between the catalyst surface and the hydrogen donor, thereby lowering the additional potential required for water splitting, making MoS1.2Se0.8 the most favorable HER electrocatalyst with the lowest value of adsorption energy. Further enhancement in the electrocatalytic activity of mixed anion TMDs has been achieved by the incorporation of carbon nanotubes (CNTs). MoS1.2Se0.8-CNT nanocomposite exhibits superior HER performance with an overpotential of 118 mV and a Tafel slope of 63 mV/decade as compared to MoS1.2Se0.8 sample owing to the synergetic effect from CNTs and MoS1.2Se0.8.

Facile synthesis of dual-MOF ultrathin nanosheets supported on layered double hydroxides heterostructure: Electron modulation strategy for enhanced electrocatalytic water splitting

In this study, we achieved electron environment modulation of MOF-based electrocatalyst by creating a dual-functional heterostructure using two-dimensional (2D) MOFs and layered double hydroxides (LDH), to enhance its electrocatalytic performance. Through a self-sacrificial template method, ultrathin hybrid dual-MOF (CoBDC and MIL-100(Fe)) nanosheets were grown on LDH, forming DM@CoFeRu-LDH, a 2D heterostructure benefiting from interference co-growth on the 2D scaffold. The thickness of dual-MOF nanosheets can be controlled by regulating the nucleation and reaction kinetics. Specifically, with a thickness ranging from 1–1.5 nm, it effectively exposes more active sites and accelerate electron and mass transfer. Additionally, electron transfer occurred between the dual-MOF and LDH heterostructures, leveraging synergistic effects from multi-metal centers to achieve an optimal electron structure. DM@CoFeRu-LDH exhibited the lowest energy barrier for the rate-determining step in the oxygen evolution reaction, along with a favorable hydrogen adsorption energy for the hydrogen evolution reaction. As a result, the DM@CoFeRu-LDH demonstrated efficient electrocatalytic activity, requiring only a voltage of 1.50 V to achieve a current density of 10 mA cm−2.

Platinum/Platinum Sulfide on Sulfur-Doped Carbon Nanosheets with Multiple Interfaces toward High Hydrogen Evolution Activity.

Platinum (Pt)-based materials are among the most competitive electrocatalysts for the hydrogen evolution reaction (HER) due to suitable hydrogen adsorption energy. Due to the rarity of Pt, it is desirable to develop cost-effective Pt-based electrocatalysts with low Pt loading. Herein, Pt/PtS electrocatalysts on S-doped carbon nanofilms (PPS/C) have been successfully fabricated through a precursor reduction route with a complex of Pt and 1-dodecanethiol (1-DDT) as the precursor. The PPS/C achieved at 400 °C (PPS/C-400) exhibits excellent HER performances with an ultralow overpotential of 41.3 mV, a low Tafel slope of 43.1 mV dec-1 at a current density of 10 mA cm-2, and a long-term stability of 10 h, superior to many recently reported Pt-based HER electrocatalysts. More importantly, PPS/C-400 shows a high mass-specific activity of 0.362 A mgPt-1 at 30 mV, which is 1.88 times of that of commercial 20% Pt/C (0.193 A mgPt-1). The introduction of sulfur leads to the formation of PtS, which not only reduces the content of Pt but also realizes the interface regulation of Pt/PtS, as well as the doping of carbon. Both regulations make the resulting catalyst have abundant active centers and rapid electron transfer/transport, which is conducive to balancing the adsorption and resolution of intermediate products, and finally achieving great mass-specific activity and stability. The research work may provide ideas for designing effective Pt-based multi-interface electrocatalysts.

Modulated electronic structure of atomic W-doped NiO/Cr2S3 nanotube heterostructure on nickel foam for enhanced overall water splitting

Critical for advancing hydrogen energy industrialization is the need to engineer durable and highly active non-precious electrocatalysts for the hydrogen/oxygen evolution reaction (HER/OER). In this study, we developed a novel approach to construct a vertically grown W-doped NiO/Cr2S3 nanotube heterostructure on nickel foam (referred to as tube W-NiO/Cr2S3/NF). This heterostructure serves as an efficient and bifunctional electrocatalyst for overall water splitting through a combination of electrodeposition and etching processes. Our systematic investigations revealed that W-doping effectively induces modifications in the electronic structure of NiO/Cr2S3, thereby boosting its intrinsic activities. Density functional theory reveals that catalytic activity for HER is influenced by the energy states of active valence dz2 orbitals. After W-doping, the resulting antibonding state orbital's unique property, neither completely empty nor fully filled, leads to an ideal hydrogen adsorption energy. Consequently, tube W-NiO/Cr2S3/NF exhibits significantly enhanced performance for overall water splitting. As a bifunctional electrode, tube W-NiO/Cr2S3/NF demonstrates remarkable activity, achieving a cell voltage of 1.58 V at a current density of 10 mA cm−2 for overall water splitting. Furthermore, it exhibits outstanding stability over 100 h in a 1.0 M KOH solution, outperforming commercial Pt-C and IrO2 counterparts.

Enhanced Photocatalytic Hydrogen Evolution Activity Driven by the Synergy Between Surface Vacancies and Cocatalysts: Surface Reaction Matters.

The incorporation of defects and cocatalysts is known to be effective in improving photocatalytic activity, yet their coupled contribution to the photocatalytic hydrogen evolution process has not been well-explored. In this study, We demonstrate that the incorporation of S vacancies and NiSe can contribute to the improvement of charge separation efficiency via the formation of a strong electric field within the bulk ZnIn2S4 (ZIS) and on its surface. More importantly, We also demonstrate that the synergy of S vacancies and NiSe benefits the overall hydrogen evolution activity by facilitating the H2O adsorption and dissociation process. This is particularly important for hydrogen evolution taking place under alkaline conditions where the proton concentration is low, allowing ZISv-NiSe (containing abundant S vacancies) to outperform ZIS-NiSe under alkaline conditions. In contrast, under acid conditions, since there are already sufficient amounts of protons available for reaction, the hydrogen evolution activity became governed by the hydrogen adsorption/desorption process rather than the H2O dissociation process. This leads to ZIS-NiSe exhibiting higher activity than ZISv-NiSe due to its more favorable hydrogen adsorption energy. The findings thus provide insights into how defect and cocatalyst modification strategies can be tailor-made to improve hydrogen evolution activity under different pH conditions.

Design of hydrogen sensor relying on Pd-MWCNT/WO3 sensing materials for selective and rapid hydrogen detection

In this investigation, hydrogen sensors were designed based on multi-walled carbon nanotubes (MWCNT) and Pd loaded on WO3 nanosheets by means of hydrothermal synthesis and impregnation reduction. First, WO3 with different morphologies were synthesized, including zero dimension (0D) nanoparticles, one dimension (1D) nanowires and two dimension (2D) nanosheets. After testing, the 2D-WO3 material was selected as the substrate material to form final Pd-MWCNT/WO3 composites. Outstandingly, Pd-MWCNT/WO3 sensor exhibited greatest sensitivity with high response value (371.13), fast response/recovery time (1/4 s) to 1000 ppm hydrogen at 175℃, excellent selectivity and reproducibility. Furthermore, the corresponding hydrogen sensing mechanism was proposed combining with DFT calculation of hydrogen adsorption energy. This was the first report on designing a novel ternary Pd-MWCNT/WO3 composites sensor applied to hydrogen detection and the first time to calculate the hydrogen adsorption energy of Pd-MWCNT/WO3.

Hydrogen Adsorption on Solid and Liquid Surfaces of Ga–Sn and Ga–In

AbstractDynamic liquid metal catalysts have remarkable activity and selectivity toward certain reactions, such as carbon dioxide reduction. The surface hydrogen coverage may play a role in this, including controlling competing reactions such as hydrogen evolution. Using a novel method of statistically selecting relevant snapshots from a dynamic liquid metal trajectory, the hydrogen adsorption energy is reported across liquid surfaces of Ga–Sn and Ga–In via density functional theory. A fully dynamic sampling of hydrogen adsorption to the liquid metal is also conducted with ab initio molecular dynamics at temperature. The results indicate that hydrogen only associates weakly with Ga–Sn and Ga–In surfaces, with minimal difference between the two materials. Hydrogen adsorbs only slightly more stably (≈0.1 eV) to the liquid surfaces compared to the solid. A low hydrogen coverage is predicted on the liquid metal of ≈0.03 H Å−2 at potentials of around –1.15 V (vs RHE). However, the mobility of hydrogen on the liquid surface is much greater due to a novel mechanism whereby the dynamic surface rearranges, opening pathways for diffusion. The results suggest that the unique catalytic behavior of these liquid metal materials may be due to changes in adsorbate diffusivity when the metals are melted.

Alkali Metals Activated High Entropy Double Perovskites for Boosted Hydrogen Evolution Reaction.

An efficient and facile water dissociation process plays a crucial role in enhancing the activity of alkaline hydrogen evolution reaction (HER). Considering the intricate influence between interfacial water and intermediates in typical catalytic systems, meticulously engineered catalysts should be developed by modulating electron configurations and optimizing surface chemical bonds. Here, a high-entropy double perovskite (HEDP) electrocatalyst La2(Co1/6Ni1/6Mg1/6Zn1/6Na1/6Li1/6)RuO6, achieving a reduced overpotential of 40.7mV at 10mA cm-2 and maintaining exemplary stability over 82 h in a 1m KOH electrolyte is reported. Advanced spectral characterization and first-principles calculations elucidate the electron transfer from Ru to Co and Ni positions, facilitated by alkali metal-induced super-exchange interaction in high-entropy crystals. This significantly optimizes hydrogen adsorption energy and lowers the water decomposition barrier. Concurrently, the super-exchange interaction enhances orbital hybridization and narrows the bandgap, thus improving catalytic efficiency and adsorption capacity while mitigating hysteresis-driven proton transfer. The high-entropy framework also ensures structural stability and longevity in alkaline environments. The work provides further insights into the formation mechanisms of HEDP and offers guidelines for discovering advanced, efficient hydrogen evolution catalysts through super-exchange interaction.

Modelling the activity trend of the hydrogen oxidation reaction under constant potential conditions.

A microkinetic model is constructed for the electrocatalytic alkaline hydrogen oxidation reaction based on grand canonical density functional theory calculations and linear relationships with the adsorption energies of hydrogen and hydroxide as descriptors. Using this model, the activity trend suitable for efficient catalyst screening has been identified.

Mo Migration-Induced Crystalline to Amorphous Conversion and Formation of RuMo/NiMoO4 Heterogeneous Nanoarray for Hydrazine-Assisted Water Splitting at Large Current Density.

Manipulating the atomic structure of the catalyst and tailoring the dissociative water-hydrogen bonding network at the catalyst-electrolyte interface is essential for propelling alkaline hydrogen evolution reactions (HER) and hydrazine oxidation reaction (HzOR), but remains a great challenge. Herein, we constructed an advanced a-RuMo/NiMoO4/NF heterogeneous electrocatalysts with amorphous RuMo alloy nanoclusters anchored to amorphous NiMoO4 skeletons on Ni foam by a heteroatom implantation strategy. Theoretical calculations and in-situ Raman tests show that the amorphous and alloying structure of a-RuMo/NiMoO4/NF not only induces the directional evolution of interfacial H2O, but also lowers the d-band center (from -0.43 to -2.22 eV) of a-RuMo/NiMoO4/NF, the Gibbs free energy of hydrogen adsorption (ΔGH*, from -1.29 to -0.06 eV), and the energy barrier of HzOR (ΔGN2(g) = 1.50 eV to ΔGN2* = 0.47 eV). Profiting from these favorable factors, the a-RuMo/NiMoO4/NF exhibits excellent electrocatalytic performances, especially at large current densities, with an overpotential of 13 and 129 mV to reach 10 and 1000 mA cm-2 for HER. While for HzOR, it needs only -91 and 276 mV to deliver 10 and 500 mA cm-2, respectively. Further, the constructed a-RuMo/NiMoO4/NF||a-RuMo/NiMoO4/NF electrolyzer demands only 7 and 420 mV to afford 10 and 500 mA cm-2.

Enhanced hydrogen kinetics of Mg–Ni–La alloys via slight Y element additive

Alloying represents an effective approach for addressing challenges related to over stable thermodynamics and slow kinetics in magnesium alloys. The incorporation of Y dopant served to enhance the quantity of grain boundaries and phase boundaries, thereby addressing the issue of high dehydrogenation temperature observed in Mg85–Ni10–La5, which can be decreased to 273.3 °C after the addition of 0.5 wt% Y additive. In addition, the initial hydrogenation rate of Mg85–Ni10–La4.5-Y0.5 reached up to 3.42 wt% H2 at 260 °C and the apparent activation energy for dehydriding was decreased from 115.31 to 86.05 kJ/mol. Theoretical calculations suggested that the hydrogen adsorption energy of Mg85–Ni10–La4.5-Y0.5 was dramatically lower than that of Mg85–Ni10–La5, improving hydrogenation properties. The consistency between theoretical calculations and experimental outcomes provided a valuable reference for the selection of suitable magnesium-based hydrogen storage materials.