Palladium/Platinum/Ruthenium Trimetallic Dendritic Nanozymes Exhibiting Enhanced Peroxidase-like Activity for Signal Amplification of Lateral Flow Immunoassays.

Developing ultrasensitive lateral flow immunoassays (LFIAs) has garnered significant attention in the field of point-of-care testing. In this study, a trimetallic dendritic nanozyme (Pd@Pt-Ru) was synthesized through Ru deposition on a Pd@Pt core and utilized to enhancing the sensitivity of LFIAs. Pd@Pt-Ru exhibited a Km value of 5.23 mM for detecting H2O2, which indicates an H2O2 affinity comparable with that of horseradish peroxidase. The Ru surface layer reduces the activation energy barrier, which increases the maximum reaction rate. As a proof of concept, the proposed Pd@Pt-Ru nanozyme was incorporated into LFIAs (A-Pd@Pt-Ru-LFIAs) for detecting human chorionic gonadotropin (hCG). Compared with conventional gold nanoparticle (AuNP)-LFIAs, A-Pd@Pt-Ru-LFIAs demonstrated 250-fold increased sensitivity, thereby enabling a visible detection limit as low as 0.1 IU/L. True positive and negative rates both reached 100%, which renders the proposed Pd@Pt-Ru nanozyme suitable for detecting hCG in clinical samples.

Performance of Nitrogen-Doped Carbon Nanoparticles Carrying FeNiCu as Bifunctional Electrocatalyst for Rechargeable Zinc-Air Battery.

Catalysts for zinc-air batteries (ZABs) must be stable over long-term charging-discharging cycles and exhibit bifunctional catalytic activity. In this study, by doping nitrogen-doped carbon (NC) materials with three metal atoms (Fe, Ni, and Cu), a single-atom-distributed FeNiCu-NC bifunctional catalyst is prepared. The catalyst includes Fe(Ni-doped)-N4 for the oxygen evolution reaction (OER), Fe(Cu-doped)-N4 for the oxygen reduction reaction (ORR), and the NiCu-NC catalytic structure for the oxygen reduction reaction (ORR) in the nitrogen-doped carbon nanoparticles. This single-atom distribution catalyst structure enhances the bifunctional catalytic activity. If a trimetallic single-atom catalyst is designed, it will surpass the typical bimetallic single-atom catcalyst. FeNiCu-NC exhibits outstanding performance as an electrocatalyst, with a half-wave potential (E1/2) of 0.876 V versus RHE, overpotential (Ej = 10) of 253 mV versus RHE at 10 mA cm-2, and a small potential gap (ΔE = 0.61 V). As the anode in a ZAB, FeNiCu-NC can undergo continuous charge-discharged cycles for 575 h without significant attenuation. This study presents a new method for achieving high-performance, low-cost ZABs via trimetallic single-atom doping.

Modifying the Reactivity of Single Pd Sites in a Trimetallic Sn-Pd-Ag Surface Alloy: Tuning CO Binding Strength.

Improving control over active-site reactivity is a grand challenge in catalysis. Single-atom alloys (SAAs) consisting of a reactive component doped as single atoms into a more inert host metal feature localized and well-defined active sites, but fine tuning their properties is challenging. Here, a framework is developed for tuning single-atom site reactivity by alloying in an additional inert metal, which this work terms an alloy-host SAA. Specifically, this work creates about 5% Pd single-atom sites in a Pd33Ag67(111) single crystal surface, and then identifies Sn based on computational screening as a suitable third metal to introduce. Subsequent experimental studies show that introducing Sn indeed modifies the electronic structure and chemical reactivity (measured by CO desorption energies) of the Pd sites. The modifications to both the electronic structure and the CO adsorption energies are in close agreement with the calculations. These results indicate that the use of an alloy host environment to modify the reactivity of single-atom sites can allow fine-tuning of catalytic performance and boost resistance against strong-binding adsorbates such as CO.

Low Potential CO2 Reduction by Inert Fe(II)-Macrobicyclic Complex: A New Concept of Cavity Assisted CO2 Activation.

The advantage of a pre-organized π-cavity of Fe(II) complex of a newly developed macrobicycle cryptand is explored for CO2 reduction by overcoming the problem of high overpotential associated with the inert nature of the cryptate. Thus, a bipyridine-centered tritopic macrobicycle having a molecular π-cavity capable of forming Fe(II) complex as well as potential for CO2 encapsulation is synthesized. The inert Fe(II)-cryptate shows much lower potential in cyclic voltammetry than the Fe(II)-tris-dimethylbipyridine (Fe-MBP) core. Interestingly, this cryptate shows electrochemical CO2 reduction at a considerably lower potential than the Fe-MBP inert core. Therefore, this study represents that a well-structured π-cavity may generate a new series of molecular catalysts for the CO2 reduction reaction (CO2 RR), even with the inert metal complexes.

Effect of External Electric Field on Nitrogen Activation on a Trimetal Cluster.

Efficient nitrogen (N2) fixation and activation under mild conditions are crucial for modern society. External electric fields (Felectric) can significantly affect N2 activation. In this work, the effect of Felectric on N2 activation by Nb3 clusters supported in a sumanene bowl was studied by density functional theory calculations. Four typical systems at different stages of N-N activation were studied, including two intermediates and two transition states. The impact of Felectric on various properties related to N2 activation was investigated, including the N-N bond length, overlap population density of states (OPDOS), total energy of the system, adsorption energy of N2, decomposition of energy changes, and electron transfer. The sumanene not only functions as a support and protective substrate, but also serves as a donor or acceptor under different Felectric conditions. Negative Felectric is beneficial to N-N bond activation because it promotes electron transfer to the N-N region and improves the d-π* orbital hybridization between metals and N2 in the activation process. Positive Felectric improves d-π* orbital hybridization only when the N-N is nearly dissociated. The microscopic mechanism of Felectric's effects provides insight into N2 activation and theoretical guidance for the design of catalytic reaction conditions for nitrogen reduction reactions (NRR).

Sunlight-mediated removal of endocrine disruptors from wastewater using trimetallic core-shell Ag-TeO2@ZnO nanocomposites.

The current work emphasizes the preparation of trimetallic core-shell Ag-TeO2@ZnO nanocomposites (NCs) by thermo-mechanical method for the efficient photocatalytic degradation of 2,4-Dichlorophenol and ß-naphthol pollutants. FE-SEM shows that Ag and TeO2nanoparticles are deposited on the surface of ZnO nanotubes. The band gap of pristine ZnO NPs and 5 wt% Ag-TeO2@ZnO nanocomposites are found to be 3.16 and 2.96 eV, respectively. The calculated specific surface area (SBET) of pristine ZnO NPs and 5 wt% Ag-TeO2@ZnO nanocomposites are 40.47 and 45.66 m2g-1respectively, confirming that Ag and TeO2nanoparticles contribute to increasing in surface area of pure ZnO. The synthesised nanocomposite showed excellent photocatalytic performance for the degradation of ß -naphthol (95.6%) in 40 min at the concentration of (0.6 mg ml-1) and 2,4-DCP (99.6%) in 180 min (0.4 mg ml-1) under natural sunlight. Cyclic Voltammetry and Electrochemical Impedance Spectroscopy were carried out to study the electrochemical properties. The determination of reactive oxygen species (ROS) confirmed that the degradation of the pollutants by 5 wt% Ag-TeO2@ZnO NCs was due to the formation of superoxide radicals. Electron paramagnetic resonance revealed the presence of sharp signals in pure ZnO nanoparticles at g ∼1.95 and oxygen vacancy peak at g ∼2.01 in 5 wt% Ag-TeO2@ZnO NCs. To study the mechanism behind the degradation of pollutants, Scavenger test using histidine and ascorbic acid (ROS scavengers) was performed. The synthesised nanocomposites are highly stable and showed enhanced efficiency up to three cycles, confirming their reusability as a photocatalyst.

Trimetallic FeCoNi Metal-Organic Framework with Enhanced Peroxidase-like Activity for the Construction of a Colorimetric Sensor for Rapid Detection of Thiophenol in Water Samples.

In recent years, nanozymes have attracted particular interest and attention as catalysts because of their high catalytic efficiency and stability compared with natural enzymes, whereas how to use simple methods to further improve the catalytic activity of nanozymes is still challenging. In this work, we report a trimetallic metal-organic framework (MOF) based on Fe, Co and Ni, which was prepared by replacing partial original Fe nodes of the Fe-MOF with Co and Ni nodes. The obtained FeCoNi-MOF shows both oxidase-like activity and peroxidase-like activity. FeCoNi-MOF can not only oxidize the chromogenic substrate 3,3,5,5-tetramethylbenzidine (TMB) to its blue oxidation product oxTMB directly, but also catalyze the activation of H2O2 to oxidize the TMB. Compared with corresponding monometallic/bimetallic MOFs, the FeCoNi-MOF with equimolar metals hereby prepared exhibited higher peroxidase-like activity, faster colorimetric reaction speed (1.26-2.57 folds), shorter reaction time (20 min) and stronger affinity with TMB (2.50-5.89 folds) and H2O2 (1.73-3.94 folds), owing to the splendid synergistic electron transfer effect between Fe, Co and Ni. Considering its outstanding advantages, a promising FeCoNi-MOF-based sensing platform has been designated for the colorimetric detection of the biomarker H2O2 and environmental pollutant TP, and lower limits of detection (LODs) (1.75 µM for H2O2 and 0.045 µM for TP) and wider linear ranges (6-800 µM for H2O2 and 0.5-80 µM for TP) were obtained. In addition, the newly constructed colorimetric platform for TP has been applied successfully for the determination of TP in real water samples with average recoveries ranging from 94.6% to 112.1%. Finally, the colorimetric sensing platform based on FeCoNi-MOF is converted to a cost-effective paper strip sensor, which renders the detection of TP more rapid and convenient.

In silico and in vitro investigation of the antifungal activity of trimetallic Cu-Zn-magnetic nanoparticles against Fusarium oxysporum with stimulation of the tomato plant's drought stress tolerance response.

Fusarium oxysporum is the fungus responsible for Fusarium wilt. Tomatoes and other plants acquire Fusarium wilt through their root systems. Occasionally, fungicides applied to the soil are used to combat the disease; however, some strains have developed resistance. Carboxymethyl cellulose (CMC) trimetallic magnetic zinc and copper nanoparticles CMC-Cu-Zn-FeMNPs are one of the most promising antifungal agents against a wide range of fungi. One of the most important aspects of using magnetic nanoparticles is their ability to target cells, which confirms the drug's potent fungicidal activity. Using a UV-spectrophotometer, the characterization of synthesized CMC-Cu-Zn-FeMNPs revealed four peaks at226,271, 321 and 335 nm, as well as spherical nanoparticles with a mean size of 5.905 nm and a surface potential of -61.7 mv. In this study, CMC-Cu-Zn-FeMNPs were used to inhibit the growth of F. oxysporum by interfering with the ergosterol production metabolic pathway. Molecular docking experiments demonstrated that the nanoparticles were able to bind to sterol 14-alpha demethylase responsible for inhibiting ergosterol biosynthesis. Real-time PCR analysis showed that the nanoparticles upregulated tomato plants and other assessed parameters under drought stress and downregulated the velvet complex and virulence factors of F. oxysporum on plants. The study results indicate that CMC-Cu-Zn-FeMNPs may be a promising and eco-friendly solution with low potential of accumulation and easy to collected alternative to conventional chemical pesticides that can have negative impacts on the environment and human health. Furthermore, it could provide a sustainable solution for managing Fusarium wilt disease, which can significantly reduce tomato yield and quality.

Preparation of Trimetallic-Organic Framework Film Electrodes via Secondary Growth for Efficient Oxygen Evolution Reaction.

Metal-organic frameworks (MOFs) are promising electrocatalysts for clean energy conversion systems. However, developing MOF-based electrodes with high performance toward oxygen evolution reaction (OER) is still challenging. In this work, a series of MOF film electrodes derived from Ni-btz were prepared by employing the secondary growth strategy under solvothermal conditions. Fe and Co ions were also incorporated into the Ni-btz framework to produce a trimetallic coupling effect to obtain enhanced OER activity. The as-prepared FeCoNi-btz/NF exhibited not only good stability but also excellent OER performance under alkaline conditions. Furthermore, the possible intermediates including metal oxides and metal oxyhydroxides were confirmed by X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM).

Heteronuclear Trimetallic MFe2 and M2 Fe (M=V, Nb, and Ta) Clusters for Dinitrogen Activation.

Catalysts with heteronuclear metal active sites may have high performance in the nitrogen reduction reaction (NRR), and the in-depth understanding of the reaction mechanisms is crucial for the design of related catalysts. In this work, the dissociative adsorption of N2 on heteronuclear trimetallic MFe2 and M2 Fe (M=V, Nb, and Ta) clusters was studied with density functional theory calculations. For each cluster, two reaction paths were studied with N2 initially on M and Fe atoms, respectively. Mayer bond order analysis provides more information on the activation of N-N bonds. M2 Fe is generally more reactive than MFe2 . The coordination mode of N2 on three metal atoms can be end-on: end-on: side-on (EES) for both MFe2 and M2 Fe. In addition, a unique end-on: side-on: side-on (ESS) coordination mode was found for M2 Fe, which leads to a higher degree of N-N bond activation. Nb2 Fe has the highest reactivity towards N2 when both the transfer of N2 and the dissociation of N-N bonds are taken into account, while Ta-containing clusters have a superior ability to activate the N-N bond. These results indicate that it is possible to improve the performance of iron-based catalysts by doping with vanadium group metals.

A new sandwich-type electrochemiluminescence sensor based on HPSNs-NH2@Au NPs and AuPdPt NPs for determination of α(2,3)-sial-Gs.

A novel sandwich-type "on-off" electrochemiluminescence (ECL) biosensor for the determination of α(2,3)-sial-Gs was designed. Specifically, amino-functionalized porous silica nanoparticles (HPSNs-NH2) were first prepared and then decorated with gold nanoparticles (Au NPs) to form HPSNs-NH2@Au NP nanocomposite, which exhibited a strong ability to enhance ECL intensity with K2S2O8 as co-reactant (signal-on) and could immobilize the target-specific binding molecules of maackia amurensis lectin (MAL). Additionally, AuPdPt trimetallic nanoparticles were prepared to serve as a quenched ECL signal indicator (signal-off) with the ability of capturing the target non-specific binding molecules of 3-aminophenylboronic acid (APBA) to form a signal label. The sandwich-type ECL biosensor was constructed based on the structure of MAL-α(2,3)-sial-Gs-APBA and achieved a determination toward α(2,3)-sial-Gs with a wide linear range from 1 fg mL-1 to 10 ng mL-1 and a low detection limit of 0.5 fg mL-1. Furthermore, the proposed ECL biosensor showed satisfactory selectivity, stability, and reproducibility for α(2,3)-sial-Gs determination.

One-pot wet-chemical fabrication of 3D urchin-like core-shell Au@PdCu nanocrystals for electrochemical breast cancer immunoassay.

Carbohydrate antigen 15-3 (CA15-3) is an important biomarker for early diagnosis of breast cancer. Herein, a label-free electrochemical immunosensor was built based on three-dimensional (3D) urchin-like core-shell Au@PdCu nanocrystals (labeled Au@PdCu NCs) for highly sensitive detection of CA15-3, where K3[Fe(CN)6] behaved as an electroactive probe. The Au@PdCu NCs were synthesized by a simple one-pot wet-chemical approach and the morphology, structures, and electrocatalytic property were investigated by several techniques. The Au@PdCu NCs prepared worked as electrode material to anchor more antibodies and as signal magnification material by virtue of its exceptional catalytic property. The developed biosensor exhibited a wide linear detection range from 0.1 to 300 U mL-1 and a low limit of detection (0.011 U mL-1, S/N = 3) for determination of CA15-3 under the optimal conditions. The established biosensing platform exhibits some insights for detecting other tumor biomarkers in clinical assays and early diagnosis.

Applications of trimetallic nanomaterials as Non-Enzymatic glucose sensors.

OBJECTIVE: This article critically reviews recent research on the use of trimetallic nanomaterials for the fabrication of non-enzymatic glucose sensors (NEGS), also known as fourth-generation glucose sensors (FGGS). SIGNIFICANCE: Diabetes is a prevalent chronic disease worldwide, and glucose monitoring is crucial for its management. However, conventional enzymatic glucose sensors suffer from several technological drawbacks, and there is a need to develop new-generation glucose sensors that can overcome these limitations. NEGS, particularly those composed of trimetallic nanocomposites, have demonstrated promising results in terms of improved shelf life, higher sensitivity, and simplicity of operation during glucose measurement. METHODS: In this review, we discuss the different trimetallic nanomaterials developed and used by researchers in recent years for glucose detection, including their mechanisms of action. We also provide a brief discussion of the advantages and disadvantages of FGGS-based trimetallic nanomaterials, as well as the industrial challenges in this area of research. RESULTS: Trimetallic nanomaterials for FGGS have shown excellent reproducibility and high stability, making them suitable for continuous glucose monitoring. The different types of trimetallic nanomaterials have varying sensing properties, and their performance can be tuned by controlling their synthesis parameters. CONCLUSION: Trimetallic nanomaterials are a promising avenue for the development of FGGS, recent research has demonstrated their potential for glucose monitoring. However, there are still some challenges that need to be addressed before their widespread adoption, such as their long-term stability and cost-effectiveness. Further research in this area is needed to overcome these challenges and to develop commercially viable FGGS for diabetes management.

Electrochemical Sensor for Tryptophan Determination Based on Trimetallic-CuZnCo-Nanoparticle-Modified Electrodes.

The superior properties of electrodeposited trimetallic CuZnCo nanoparticles, arising from the synergistic effect of combining the unique features of metallic components, were confirmed using voltametric measurements. The surface morphology and structure of the as-prepared electrocatalysts were determined using scanning electron microscopy, energy-dispersive X-ray, and X-ray photoelectron spectroscopy techniques. Here, the trimetallic CuZnCo nanoparticles were synthesized as a powerful redox probe and highly efficient signal amplifier for the electrochemical oxidation of tryptophan. Differential pulse voltammetry studies showed a linear relationship with a tryptophan concentration of 5-230 µM, and the low detection limit was identified at 1.1 µM with a sensitivity of 0.1831 µA µM-1 cm-2.

Core-Shell Structure Trimetallic Sulfide@N-Doped Carbon Composites as Anodes for Enhanced Lithium-Ion Storage Performance.

The high specific capacity of transition metal sulfides (TMSs) opens up a promising new development direction for lithium-ion batteries with high energy storage. However, the poor conductivity and serious volume expansion during charge and discharge hinder their further development. In this work, trimetallic sulfide Zn-Co-Fe-S@nitrogen-doped carbon (Zn-Co-Fe-S@N-C) polyhedron composite with a core-shell structure is synthesized through a simple self-template method using ZnCoFe-ZIF as precursor, followed by a dopamine surface polymerization process and sulfidation during high-temperature calcination. The obvious space between the internal core and the external shell of the Zn-Co-Fe-S@N-C composites can effectively alleviate the volume expansion and shorten the diffusion path of Li ions during charge and discharge cycles. The nitrogen-doped carbon shell not only significantly improves the electrical conductivity of the material, but also strengthens the structural stability of the material. The synergistic effect between polymetallic sulfides improves the electrochemical reactivity. When used as an anode in lithium-ion batteries (LIBs), the prepared Zn-Co-Fe-S@N-C composite exhibits a high specific capacity retention (966.6 mA h g-1 after 100 cycles at current rate of 100 mA g-1) and good cyclic stability (499.17 mA h g-1 after 120 cycles at current rate of 2000 mA g-1).

Facile Synthesis of Pd and PdPtNi Trimetallic Nanosheets as Enhanced Oxygen Reduction Electrocatalysts.

While bimetallic 2D metallic nanomaterials are widely synthesized and used as electrocatalysts with enhanced performance, trimetallic 2D structures are less commonly reported. In this work, a facile wet chemical method for synthesizing Pd nanosheets and PdPtNi trimetallic alloy nanosheets is developed. Without the introduction of gaseous CO and pressurized equipment, Pd nanosheets with a thickness of ≈2.85 nm and sizes in the range of 1-2 µm can be obtained. The facile synthesis conditions allow for a comprehensive study of the nanosheet growth mechanism. It is found that 2D growth is closely related to the product of solvent decomposition and the additive ligand diethylenetriamine. Further, by depositing Pt and Ni onto the Pd nanosheets, trimetallic nanosheets with tunable compositions can be obtained and applied as oxygen reduction reaction electrocatalysts. Typically, the Pd9 Pt1 Ni1 nanosheets have the highest half-wave potential of 0.928 V (vs reversible hydrogen electrode), which is 34 mV higher than that of commercial Pt/C and 28 mV higher than that of Pd/C, and also have high durability.

A Dual Sensing Platform for Human Exhaled Breath Enabled by Fe-MIL-101-NH2 Metal-Organic Frameworks and its Derived Co/Ni/Fe Trimetallic Oxides.

Limited by the insufficient active sites and the interference from breath humidity, designing reliable gas sensing materials with high activity and moisture resistance remains a challenge to analyze human exhaled breath for the translational application of medical diagnostics. Herein, the dual sensing and cooperative diagnosis is achieved by utilizing metal-organic frameworks (MOFs) and its derivative. The Fe-MIL-101-NH2 serves as the quartz crystal microbalance humidity sensing layer, which exhibits high selectivity and rapid response time (16 s/15 s) to water vapor. Then, the Co2+ and Ni2+ cations are further co-doped into Fe-MIL-101-NH2 host to obtain the derived Co/Ni/Fe trimetallic  oxides (CoNiFe-MOS-n). The chemiresistive CoNiFe-MOS-n sensor displays the high sensitivity (560) and good selectivity to acetone, together with a lower original resistance compared with Fe2 O3 and NiFe2 O4 . Moreover, as a proof-of-concept application, synergistic integration of Fe-MIL-101-NH2 and derived CoNiFe-MOS-n is carried out. The Fe-MIL-101-NH2 is applied as moisture sorbent materials, which realize a sensitivity compensation of CoNiFe-MOS-n sensors for the detection of acetone (biomarker gas of diabetes). The findings provide an insight for effective utilization of MOFs and the derived materials to achieve a trace gas detection in exhaled breath analysis.

High-Efficient Ultrathin PdCuMo Porous Nanosheets with Abundant Defects for Oxygen Reduction Reaction.

To reduce the over-dependence on Pt, Pd-based catalysts have become one of the most effective candidates for oxygen reduction reaction (ORR). In order to further accelerate the ORR kinetics and strengthen the catalytic performance of Pd catalysts, component optimization and morphology design have been adopted. Although great progress has been made, it is still difficult to obtain porous ultrathin nanosheets with excellent performance by a simple method. Here, ultrathin PdCuMo porous nanosheets (PdCuMo NSs) were successfully prepared. This structure possessed a large specific surface area with rich cavities and structural defects, significantly enhancing its ORR performance. In special, the mass activity of PdCuMo NSs was 1.46 A mg-1 at 0.90 V, which was 12.2, 8.6, and 2.7 times as high as that of Pd/C, Pt/C, and PdCuMo nanoparticles (PdCuMo NPs), respectively. In addition, it had an excellent ability to resist CO poisoning and exhibited remarkable long-term stability.

Comparison of Nitrogen Activation on Trinuclear Niobium and Tungsten Sulfide Clusters Nb3 Sn and W3 Sn (n=0-3): A DFT Study.

The reaction of N2 with trinuclear niobium and tungsten sulfide clusters Nb3 Sn and W3 Sn (n=0-3) was systematically studied by density functional theory calculations with TPSS functional and Def2-TZVP basis sets. Dissociations of N-N bonds on these clusters are all thermodynamically allowed but with different reactivity in kinetics. The reactivity of Nb3 Sn is generally higher than that of W3 Sn . In the favorite reaction pathways, the adsorbed N2 changes the adsorption sites from one metal atom to the bridge site of two metal atoms, then on the hollow site of three metal atoms, and at that place, the N-N bond dissociates. As the number of ligand S atoms increases, the reactivity of Nb3 Sn decreases because of the hindering effect of S atoms, while W3 S and W3 S2 have the highest reactivity among four W3 Sn clusters. The Mayer bond order, bond length, vibrational frequency, and electronic charges of the adsorbed N2 are analyzed along the reaction pathways to show the activation process of the N-N bond in reactions. The charge transfer from the clusters to the N2 antibonding orbitals plays an essential role in N-N bond activation, which is more significant in Nb3 Sn than in W3 Sn , leading to the higher reactivity of Nb3 Sn . The reaction mechanisms found in this work may provide important theoretical guidance for the further rational design of related catalytic systems for nitrogen reduction reactions (NRR).

Facile N≡N Bond Cleavage by Anionic Trimetallic Clusters V3-x Tax C4- (x=0-3): A DFT Study.

Activation of N2 on anionic trimetallic V3-x Tax C4- (x=0-3) clusters was theoretically studied employing density functional theory. For all studied clusters, initial adsorption of N2 (end-on) on one of the metal atoms (denoted as Site 1) is transferred to an of end-on: side-on: side-on coordination on three metal atoms, prior to N2 dissociation. The whole reaction is exothermic and has no global energy barriers, indicating that the dissociation of N2 is facile under mild conditions. The reaction process can be divided into two processes: N2 transfer (TRF) and N-N dissociation (DIS). For V-series clusters, which has a V atom on Site 1, the rate-determining step is DIS, while for Ta-series clusters with a Ta on Site 1, TRF may be the rate-determining step or has energy barriers similar to those of DIS. The overall energy barriers for heteronuclear V2 TaC4- and VTa2 C4- clusters are lower than those for homonuclear V3 C4- and Ta3 C4- , showing that the doping effect is beneficial for the activation and dissociation of N2 . In particular, V-Ta2 C4- has low energy barriers in both TRF and DIS, and it has the highest N2 adsorption energy and a high reaction heat release. Therefore, a trimetallic heteronuclear V-series cluster, V-Ta2 C4- , is suggested to have high reactivity to N2 activation, and may serve as a prototype for designing related catalysts at a molecular level.