Catalyst For Reaction Research Articles

Ullmann-Type N-, S-, and O-Arylation Using a Well-Defined 7-Azaindole-N-oxide (7-AINO)-Based Copper(II) Catalyst: Scope and Application to Drug Synthesis.

An air-stable, robust, and well-defined copper(II)-7-azaindole-N-oxide-based catalyst [Cu2II(7-AINO)4] (abbreviated as Cu(II)-7-AINO) has been demonstrated as an efficient catalyst for various Ullmann-type coupling reactions. This easily prepared and cost-effective catalyst facilitates the arylation and heteroarylation of diverse N-, S-, and O-nucleophiles, including azoles, aminoazoles, (hetero)arylthiols, and phenols. Notably, they also exhibit substantial compatibility with a wide range of functional groups. Furthermore, the catalyst demonstrates significant selectivity for -NH sites of aminoazoles and -SH sites of aminothiophenols over -NH2 sites in both cases, enhancing its versatility. Exploiting the catalyst's chemo- and regioselective properties, we have successfully demonstrated the applicability of our methodology in synthesizing various drug molecules. Specifically, Epirizole analogue, Nilotinib, and Vortioxetine were successfully synthesized using our protocol.

Investigation of Doping Effects on the Local Electrochemical Activity of Transition Metal Dichalcogenides 2D Materials

AbstractFinding strategies to enhance catalysts’ electrochemical activity is based on controlling the material design. Bidimensional materials (2DM) such as MoS2 are explored as catalysts for the hydrogen evolution reaction (HER). A comprehensive study of the effects of doping 2D materials with transition metals based on theoretical predictions in tandem with experimental investigation correlates the doping type to the changes in the electronic and electrochemical activity. Localized electrochemical maps obtained by scanning electrochemical cell microscopy (SECCM) reveal that Ti‐doping induces a heterogeneous increase in 2H‐MoS2 basal plane electrochemical activity, while Ni‐doping induces a homogeneous decrease. Additionally, Kelvin probe microscopy provides insight into Ti‐doping, showcasing a decline in the 2H‐MoS2 work function, therefore confirming the predictions from density functional theory simulations. In essence, the findings underscore the potential of transition metal coordination on the 2H‐MoS2 surface as an attractive method for locally doping 2D materials with minimal damage to the crystalline lattice, consequently enhancing the electrochemical activity on the material's basal plane.

Novel High-Entropy FeCoNiMoZn-Layered Hydroxide as an Efficient Electrocatalyst for the Oxygen Evolution Reaction

The exploration of catalysts for the oxygen evolution reaction (OER) with high activity and acceptable price is essential for water splitting to hydrogen generation. High-entropy materials (HEMs) have aroused increasing interest in the field of electrocatalysis due to their unusual physicochemical properties. In this work, we reported a novel FeCoNiMoZn-OH high entropy hydroxide (HEH)/nickel foam (NF) synthesized by a facile pulsed electrochemical deposition method at room temperature. The FeCoNiMoZn-OH HEH displays a 3D porous nanosheet morphology and polycrystalline structure, which exhibits extraordinary OER activity in alkaline media, including much lower overpotential (248 mV at 10 mA cm−2) and Tafel slope (30 mV dec−1). Furthermore, FeCoNiMoZn-OH HEH demonstrates excellent OER catalytic stability. The enhanced catalytic performance of the FeCoNiMoZn-OH HEH primarily contributed to the porous morphology and the positive synergistic effect between Mo and Zn. This work provides a novel insight into the design of HEMs in catalytic application.

Post-treatment induced anisotropic growth of MOF-derived surface modified heterogeneous catalyst for efficient oxygen evolution reaction

The advancement of electrocatalysts exhibiting outstanding performance in the oxygen evolution reaction (OER), crucial for hydrogen production, holds immense significance in addressing energy shortages and mitigating environmental pollution. In this study, a novel approach to synthesizing Co-MOF (Metal-Organic Framework) directly immobilized onto a Ni foam substrate through hydrothermal synthesis is presented. In contrast to conventional methods employing powder-based synthesis with binders, our direct attachment method offers a unique and efficient means of creating robust Co-MOF at Ni foam (Co-MOF@NF) hybrid catalysts. Subsequently, a chemical reduction approach utilizing sodium borohydride was employed to introduce surface modification into the Co-MOF structure. The resulting material, sodium borohydride treated Co-MOF@NF (Red. 1 h Co-MOF@NF), exhibited a remarkable enhancement in OER activity compared to the pristine Co-MOF@NF sample. Notably, Red.1 h Co-MOF@NF demonstrated a substantially reduced overpotential of 235 mV to achieve a current density of 10 mA cm⁻2, in contrast to the 300 mV overpotential required by the pristine Co-MOF@NF under the same conditions. Furthermore, the Red.1 h Co-MOF@NF catalyst displayed exceptional stability, sustaining a current density of 50 mA cm⁻2 for over 48 h, highlighting its promising potential for practical applications. The synergistic effects of direct hydrothermal attachment, surface modification, and improved OER performance make this study a significant contribution to the advancement of efficient and stable electrocatalysts for energy conversion applications.

IrO2 Oxygen Evolution Catalysts Prepared by an Optimized Photodeposition Process on TiO2 Substrates.

Preparing high-performance oxygen evolution reaction (OER) catalysts with low precious metal loadings for water electrolysis applications (e.g., for green hydrogen production) is challenging and requires electrically conductive, high-surface-area, and stable support materials. Combining the properties of stable TiO2 with those of active iridium oxide, we synthesized highly active electrodes for OER in acidic media. TiO2 powders (both commercially available Degussa P-25® and hydrothermally prepared in the laboratory from TiOSO4, either as received/prepared or following ammonolysis to be converted to titania black), were decorated with IrO2 by UV photodeposition from Ir(III) aqueous solutions of varied methanol scavenger concentrations. TEM, EDS, FESEM, XPS, and XRD measurements demonstrate that the optimized version of the photodeposition preparation method (i.e., with no added methanol) leads to direct deposition of well-dispersed IrO2 nanoparticles. The electroactive surface area and electrocatalytic performance towards OER of these catalysts have been evaluated by cyclic voltammetry (CV), Linear Sweep Voltammetry (LSV), and Electrochemical Impedance Spectroscopy (EIS) in 0.1 M HClO4 solutions. All TiO2-based catalysts exhibited better mass-specific (as well as intrinsic) OER activity than commercial unsupported IrO2, with the best of them (IrO2 on Degussa P-25® ΤiO2 and laboratory-made TiO2 black) showing 100 mAmgIr-1 at an overpotential of η = 243 mV. Chronoamperometry (CA) experiments also proved good medium-term stability of the optimum IrO2/TiO2 electrodes during OER.

Bimetallic-doped three-dimensional carbon skeleton porous material as efficient catalysts for oxygen reduction reaction

The slowness of the oxygen reduction reaction (ORR) kinetics of the fuel cell cathode has terrifically inhibited its development process. Now it is of considerable importance to research low-cost, multi-defect, high-performance non-noble metal ORR catalysts. Specifically, CuO nanosheets are grown in situ on ZIF-8 to form a composite material (zif-8@CuO), and then undergo a high-temperature carbonization process. Finally, the Zn-Cu codoped composite material Zn-xCu-N/C with a porous structure supported by a three-dimensional carbon skeleton can be obtained. The material has a 3D carbon skeleton support and a rich pore structure, which can expose more active sites. The combination of bimetallic Zn and Cu with carbon materials also increases the overall stability and conductivity of the material, which is beneficial to improvement of catalytic performance. The electrochemical performance test results show that the onset potential and half-wave potential of the Zn-0.1Cu-N/C material are 0.889 V and 0.803 V respectively, with a low Tafel slope of 62 mV dec−1 and excellent long-term stability. After 10000 cycles, the ORR curve only changed 18 mV, while the carbon skeleton can still maintain unchanged.

Construction and catalysis role of a kinetic promoter based on lithium-insertion technology and proton exchange strategy for lithium-sulfur batteries

The high theoretical energy density and specific capacity of lithium-sulfur (Li-S) batteries have garnered considerable attention in the prospective market. However, ongoing research on Li-S batteries appears to have encountered a bottleneck, with unresolved key technical challenges such as the significant shuttle effect and sluggish reaction kinetics. This investigation explores the catalytic efficacy of three catalysts for Li-S batteries and elucidates the correlation between their structure and catalytic impacts. The results suggest that the combined utilization of lithium-insertion technology and a proton exchange approach for δ-MnO2 can optimize its electronic structure, resulting in an optimal catalyst (H/Li inserted δ-MnO2, denoted as HLM) for the sulfur reduction reaction. The replacement of Mn sites in δ-MnO2 with Li atoms can enhance the structural stability of the catalyst, while the introduction of H atoms between transition metal layers contributes to the satisfactory catalytic performance of HLM. Theoretical calculations demonstrate that the bond length of Li2S4 adsorbed by the HLM molecule is elongated, thereby facilitating the dissociation process of Li2S4 and enhancing the reaction kinetics in Li-S batteries. Consequently, the Li-S battery utilizing HLM as a catalyst achieves a high areal specific capacity of 4.2 mAh cm−2 with a sulfur loading of 4.1 mg cm−2 and a low electrolyte/sulfur (E/S) ratio of 8 μL mg−1. This study introduces a methodology for designing effective catalysts that could significantly advance practical developments in Li-S battery technology.

Atomically dispersed Iridium on Mo2C as an efficient and stable alkaline hydrogen oxidation reaction catalyst

Hydroxide exchange membrane fuel cells (HEMFCs) have the advantages of using cost-effective materials, but hindered by the sluggish anodic hydrogen oxidation reaction (HOR) kinetics. Here, we report an atomically dispersed Ir on Mo2C nanoparticles supported on carbon (IrSA-Mo2C/C) as highly active and stable HOR catalysts. The specific exchange current density of IrSA-Mo2C/C is 4.1 mA cm−2ECSA, which is 10 times that of Ir/C. Negligible decay is observed after 30,000-cycle accelerated stability test. Theoretical calculations suggest the high HOR activity is attributed to the unique Mo2C substrate, which makes the Ir sites with optimized H binding and also provides enhanced OH binding sites. By using a low loading (0.05 mgIr cm−2) of IrSA-Mo2C/C as anode, the fabricated HEMFC can deliver a high peak power density of 1.64 W cm−2. This work illustrates that atomically dispersed precious metal on carbides may be a promising strategy for high performance HEMFCs.

Recent Advances in Denitrogenative Organic Transformations of 1,2,3‐Benzotriazin‐4(3H)‐ones

AbstractDenitrogenative organic transformations and related reactions are a class of significant approaches for carrying out unusual C−C/C‐heteroatom (C−O, C−N, C−S) bond‐forming reactions that are usually promoted by Ru, Ir, Pd, Ni, and Cu metal catalysts. In this trait, numerous methods were adopted to synthesize several pharmaceutically valuable N‐ and O‐containing heteroaromatics using 1,2,3‐benzotriazin‐4(3H)‐one as an electrophilic coupling partner. This review involves the recent achievements related to the metal/organo‐catalyzed thermal and visible‐light mediated denitrogenative approaches with 1,2,3‐benzotriazin‐4(3H)‐ones towards the synthesis of imperative N‐heteroaromatic compounds. In addition, metal and oxidant‐free ortho‐functionalization of benzotriazinones by using suitable nucleophilic partners have been discussed. In particular, the most novel methods employing Ni and Pd metal catalysts that have emerged are exhibited. Specific attention has been paid to offering the detailed mechanistic pathway to explain the role of metal catalysts and the mechanism in the absence of metal catalysts in the denitrogenative reactions under a thermal/visible light medium.

Sustainable process intensification: Ultrasonic preparation of MIL-88A for benzoxazole synthesis

This study provides a biodegradable fumaric acid-based MIL-88A metal-organic framework, a cost-effective and non-toxic catalyst, for biologically active benzoxazoles synthesis. Initially, the ultrasonic approach is used for MIL-88A preparation at room temperature, significantly reducing the synthesis time compared to conventional heating protocols. The ultrasonic approach is once again used for the three-component production of benzoxazoles in the presence of MIL-88A catalyst. Subsequently, the benzoxazole reaction is accelerated and yields are also improved. Impressive yields ranging between 84 % and 96 % were obtained within one hour at room temperature for the three-component synthesis of benzoxazoles. Characterization techniques, including FT-IR, TEM, XRD, and SEM-EDS mapping, confirm the successful synthesis of MIL-88A. Moreover, a large-scale reaction for benzoxazole synthesis can be performed with minimal yield loss, indicating its practical application. Notably, fumaric acid, found in many fruits and vegetables, serves as the precursor for catalyst synthesis. Catechol, sourced from various plant sources, is employed for three-component production of benzoxazoles. By integrating sustainable techniques, including ultrasound-assisted synthesis and naturally available substrates, an innovative strategy was developed utilizing a renewable catalyst for an eco-friendly reaction.

Non-precious Electrocatalysts for the Hydrogen Evolution Reaction

The development of non-precious metal-based catalysts for the hydrogen evolution reaction (HER) is a promising research area with the potential to advance water electrolysis and enable the widespread use of hydrogen as a clean energy source. While noble metals like Pt and Pd exhibit excellent HER activity, their limited availability and high cost present significant challenges. Non-precious transition metals such as Fe, Co, and Ni have emerged as alternative catalyst materials due to their natural abundance. However, these metals often encounter obstacles related to their hydrogen adsorption behavior. This commentary highlights the various strategies employed to optimize the electronic structures of non-precious metal-based catalysts to enhance the HER performance. The outlook of non-precious metal-based catalysts is bright, with ongoing and future research activities mainly focusing on improving their properties, integrating these catalysts into commercial water electrolysis systems, and improving the scalability for large-scale hydrogen production. The development of high-performance non-precious metal-based catalysts for HER is crucial to future sustainable and efficient hydrogen production in the transition from fossil fuels to clean energy.

Influence of Oxygen Vacancies in La0.4Sr0.6FeO3-δ Perovskite Oxide Nanoparticles for the Oxygen Evolution Reaction

Oxygen vacancies are important factors to tune the performance of oxide catalysts for the oxygen evolution reaction (OER). However, it remains challenging how to control the concentration of the oxygen vacancies and decouple their effects on OER from other factors. In this work, we use a specific composition/phase La0.4Sr0.6FeO3- d perovskite oxide as an example to tailor the oxygen vacancies of their nanoparticulate using a modified molten salt synthesis and ozone treatment. The OER performance of the resulting La0.4Sr0.6FeO3- d nanoparticles with different degree of oxygen vacancies ranging from 0 to 25% are compared. The OER reactivity increases with increased oxygen vacancies in the materials, but the change is nonlinear. The OER stability, on the other hand, has a bimodal distribution. The activities of fully oxidized sample and the most oxygen-deficient sample degrade slower than the two samples in the middle. The results suggest that it is feasible to design catalysts with oxygen vacancy to be the most OER active and stable. Further investigation into the oxygen vacancy – active site relation would offer guiding principle to design and synthesize high OER performance oxide catalysts.

A new nickel-based δ-isomer Anderson-type polyoxometalates: Synthesis, crystal structure and catalytic activity in 1,2,3-triazoles production

In this study, we present a novel organic hybrid Ni-based δ-isomer of Anderson-type polyoxometalates (POMs), namely, δ-[C6H12Mo6N2NiO24]4− (1), as an efficient catalyst for the cycloaddition reaction between alkynes, halides, and sodium azide. Synthesis of the catalyst was performed using a facile one-pot method followed by characterization using single crystal, powder XRD, SEM, and FT-IR techniques. After optimizing reaction conditions for a model reaction (T = 80 °C, time = 6 h, and solvent = 2 mL H2O), the catalytic activity of this compound was examined for the preparation of diversely substituted 1,2,3-triazoles under ambient atmospheric and additive-free conditions, achieving moderate to good yields. Catalyst 1 could reuse up to four sequential cycles without significant loss in its catalytic activity. Additionally, the true heterogeneity of the catalyst was determined by the hot-filtration test.

High-Entropy La(FeCuMnMgTi)O3 Nanoparticles as Heterogeneous Catalyst for CO2 Electroreduction Reaction.

In this work, La(FeCuMnMgTi)O3 HEO nanoparticles with a perovskite-type structure are synthesized and used in the electrocatalytic CO2 reduction reaction (CO2RR). The catalyst demonstrates high performance as an electrocatalyst for the CO2RR, with a Faradaic efficiency (FE) of 92.5% at a current density of 21.9 mA cm-2 under -0.75 V vs a saturated calomel electrode (SCE). Particularly, an FE above 54% is obtained for methyl isopropyl ketone (C5H10O, MIPK) at a partial current density of 16 mA cm-2, overcoming all previous works. Besides, the as-prepared HEO catalyst displays robust stability in the CO2RR. The excellent catalytic performance of La(FeCuMnMgTi)O3 is ascribed to the synergistic effect between the electronic effects associated with five cations occupying the high-entropy sublattice sites and the oxygen vacancies within the perovskite structure of the HEO. Finally, DFT calculations indicate that Cu plays a vital role in the catalytic activity of the La(FeCuMnMgTi)O3 HEO nanoparticles toward C2+ products.

One-Step Synthesis of High-Efficiency Oxygen Evolution Reaction Catalyst FeSx(Y/MB) with High Temperature Resistance and Strong Alkali

Given the energy crisis and escalating environmental pollution, the imperative for developing clean new energy is evident. Hydrogen has garnered significant attention owing to its clean properties, high energy density, and ease of storage and transportation. This study synthesized four types of catalysts—FeS(DI/MB), FeS(ET/MB), Fe(DI/MB), and Fe(ET/MB)—using two distinct solution systems: DI/MB and ET/MB. The FeS(DI/MB) catalyst, synthesized using the layered solution system (DI/MB), demonstrates a uniformly distributed and dense nanosheet structure, exhibiting excellent resistance to strong bases and superior catalytic properties. The FeS(DI/MB) electrode showed OER overpotentials of 460 mV and 318 mV in 1 M and 6 M, respectively, at current densities of up to 500 mA cm−2. Under industrial electrolysis test conditions, the FeS(DI/MB) electrode required only 262 mV to achieve a current density of 500 mA cm−2, operating in a high-temperature, strong alkaline environment of 6 M at 60 °C. Furthermore, the FeS(DI/MB) electrode exhibited excellent OER catalytic activity and stability, as evidenced by a 60 h stability test These findings provide valuable insights into the preparation of iron nickel sulfide-based catalysts, and further in-depth and comprehensive exploration is anticipated to yield the excellent catalytic performance of these catalysts in the realm of electrolytic water hydrogen production.

A first-principles prediction of the structural, electronic, transport and photocatalytic properties of GaGeX3 (X = S, Se, Te) monolayers.

The discovery of new 2D materials with superior properties motivates scientists to make breakthroughs in various applications. In this study, using calculations based on density functional theory (DFT), we have comprehensively investigated the geometrical characteristics and stability of GaGeX3 monolayers (X = S, Se, or Te), determining their electronic and transport properties, and some essential optical and photocatalytic properties. AIMD simulations show that these materials are highly structurally and thermodynamically stable. Notably, the GaGeSe3 monolayer is a semiconductor with a band gap of 1.9 eV and has a high photon absorption coefficient of up to 1.1 × 105 cm-1 in the visible region. The calculated solar-to-hydrogen conversion efficiency of the GaGeSe3 monolayer is 11.33%, which is relatively high compared to some published 2D materials. Furthermore, the electronic conductivity of the GaGeSe3 monolayer is 790.65 cm2 V-1 s-1. Our findings suggest that the GaGeSe3 monolayer is a new promising catalyst for the solar water-splitting reaction to give hydrogen and a potential new 2D material for electrical devices with high electron mobility.

Tuning Two-Dimensional Phthalocyanine Dual Site Metal-Organic Framework Catalysts for the Oxygen Reduction Reaction.

Metal-organic frameworks (MOFs) offer an interesting opportunity for catalysis, particularly for metal-nitrogen-carbon (M-N-C) motifs by providing an organized porous structural pattern and well-defined active sites for the oxygen reduction reaction (ORR), a key need for hydrogen fuel cells and related sustainable energy technologies. In this work, we leverage electrochemical testing with computational models to study the electronic and structural properties in the MOF systems and their relationship to ORR activity and stability based on dual transitional metal centers. The MOFs consist of two M1 metals with amine nodes coordinated to a single M2 metal with a phthalocyanine linker, where M1/M2 = Co, Ni, or Cu. Co-based metal centers, in particular Ni-Co, demonstrate the highest overall activity of all nine tested MOFs. Computationally, we identify the dominance of Co sites, relative higher importance of the M2 site, and the role of layer M1 interactions on the ORR activity. Selectivity measurements indicate that M1 sites of MOFs, particularly Co, exhibit the lowest (<4%), and Ni demonstrates the highest (>46%) two-electron selectivity, in good agreement with computational studies. Direct in situ stability characterization, measuring dissolved metal ions, and calculations, using an alkaline stability metric, confirm that Co is the most stable metal in the MOF, while Cu exhibits notable instability at the M1. Overall, this study reveals how atomistic coupling of electronic and structural properties affects the ORR performance of dual site MOF catalysts and opens new avenues for the tunable design and future development of these systems for practical electrochemical applications.

A Vacuum Vapor Deposition Strategy to Fe Single-Atom Catalysts with Densely Active Sites for High-Performance Zn-Air Battery.

Iron single-atom catalysts (SACs) have garnered increasing attention as highly efficient catalysts for the oxygen reduction reaction (ORR), yet their performance in practical devices remains suboptimal due to the low density of accessible active sites. Anchoring iron single atoms on 2D support is a promising way to increase the accessible active sites but remains difficult attributing to the high aggregation tendency of iron atoms on the 2D support. Herein, a vacuum vapor deposition strategy is presented to fabricate an iron SAC supported on ultrathin N-doped carbon nanosheets with densely active sites (FeSAs-UNCNS). Experimental analyses confirm that the FeSAs-UNCNS achieves densely accessible active sites (1.11×1020sitesg-1) in the configuration of Fe─N4O. Consequently, the half-wave potential of FeSAs-UNCNS in 0.1m KOH reaches a remarkable value of 0.951V versus RHE. Moreover, when employed as the cathode of various kinds of Zn-air batteries, FeSAs-UNCNS exhibits boosting performances by achieving a maximum power density of 306mWcm-2 and long cycle life (>180h) at room temperature, surpassing both Pt/C and reported SACs. Further investigations reveal that FeSAs-UNCNS facilitates the mass and charge transfer during catalysis and the atomic configuration favors the desorption of *OH kinetically.

Theoretical Study of Single-Atom Catalysts for Hydrogen Evolution Reaction Based on BiTeBr Monolayer.

Developing an inexpensive and efficient catalyst for a hydrogen evolution reaction (HER) is an effective measure to alleviate the energy crisis. Single-atom catalysts (SACs) based on Janus materials demonstrated promising prospects for the HER. Herein, density functional theory calculations were conducted to systematically investigate the performance of SACs based on the BiTeBr monolayer. Among the one hundred and forty models that were constructed, fourteen SACs with potential HER activity were selected. Significantly, the SAC, in which a single Ru atom is anchored on a BiTeBr monolayer with a Bi vacancy (RuS2/VBi-BiTeBr), exhibits excellent HER activity with an ultra-low |ΔGH*| value. A further investigation revealed that RuS2/VBi-BiTeBr tends to react through the Volmer-Heyrovsky mechanism. An electronic structure analysis provided deeper insights into this phenomenon. This is because the Tafel pathway requires overcoming steric hindrance and disrupting stable electron filling states, making it challenging to proceed. This study finally employed constant potential calculations, which approximate experimental situations. The results indicated that the ΔGH* value at pH = 0 is 0.056 eV for RuS2/VBi-BiTeBr, validating the rationality of the traditional Computational Hydrogen Electrode (CHE) method for performance evaluation in this system. This work provides a reference for the research of new HER catalysts.

Accelerating the Screening of Modified MA2Z4 Catalysts for Hydrogen Evolution Reaction by Deep Learning‐Based Local Geometric Analysis

Machine learning (ML) integrated with density functional theory (DFT) calculations have recently been used to accelerate the design and discovery of single‐atom catalysts (SACs) by establishing deep structure–activity relationships. The traditional ML models are always difficult to identify the structural differences among the single‐atom systems with different modification methods, leading to the limitation of the potential application range. Aiming to the structural properties of several typical two‐dimensional MA2Z4‐based single‐atom systems (bare MA2Z4 and metal single‐atom doped/supported MA2Z4), an improved crystal graph convolutional neural network (CGCNN) classification model was employed, instead of the traditional machine learning regression model, to address the challenge of incompatibility in the studied systems. The CGCNN model was optimized using crystal graph representation in which the geometric configuration was divided into active layer, surface layer, and bulk layer (ASB‐GCNN). Through ML and DFT calculations, five potential single‐atom hydrogen evolution reaction (HER) catalysts were screened from chemical space of 600 MA2Z4‐based materials, especially V1/HfSn2N4(S) with high stability and activity (ΔGH* is 0.06 eV). Further projected density of states (pDOS) analysis in combination with the wave function analysis of the SAC‐H bond revealed that the SAC‐dz2 orbital coincided with the H‐s orbital around the energy level of −2.50 eV, and orbital analysis confirmed the formation of σ bonds. This study provides an efficient multistep screening design framework of metal single‐atom catalyst for HER systems with similar two‐dimensional supports but different geometric configurations.