Ni Metal Research Articles

Synthesis of Three Ternary NiPP@PDA@DTA by Bridging Polydopamine and Its Flame Retardancy in Epoxy Resin

Epoxy resin (EP) is an indispensable packaging material for batteries. Excellent thermal and flame-retardant properties of EP can ensure the safety performance of batteries. To solve the low-efficiency flame retardant of EP, nickel phenyl phosphate (NiPP) was synthesized and its surface was modified by polymerization of dopamine (PDA). [3-(hydroxy-phenyl-methylidene) imimine] triazole (DTA) was synthesized using 9,10-dihydro-9-oxygen-10-phosphophene-10-oxide (DOPO), 3-amino-1,2,4-triazole and p-hydroxybenzaldehyde. The hybrid flame retardance NiPP@PDA@DTA was further synthesized by self-assembly between the negative charge on the surface of DTA and the positive charge on the surface of modified NiPP@PDA. Then, NiPP@PDA@DTA was added to EP to prepare EP/NiPP@PDA@DTA composites. The results showed that the incorporation of NiPP@PDA@DTA promoted the residual yield at high temperatures. Furthermore, EP composites showed excellent flame retardancy when NiPP@PDA@DTA was added. The EP/4 wt% NiPP@PDA@DTA composites can reach UL-94 V0 grade with a limit oxygen index (LOI) of 33.7%. While the heat release rate (HRR), total release rate (THR), CO2 production (CO2P) and total smoke release (TSR) of EP/4 wt% NiPP@PDA@DTA composites decreased by 16.9%, 30.8%, 16.9% and 27.7% compared with those of EP. These improvements are mainly due to the excellent catalytic carbonization performance of Ni metal and P compounds. The azazole and phosphaphenanthrene groups have the effects of dilution quenching in the gas phase and cross-linking network blocking, as well as enhanced blowing-out effects.

Selective Electrocatalytic Production of Formic Acid from Plastic Waste Using a Ni Metal Organic Framework Constructed from a Biomass‐Derived Ligand

A novel nickel‐based metal organic framework (MOF) [Ni(FDC)(CH3OH)1.5(H2O)0.5](H2O)0.35 (UOW‐6) utilizing biomass‐derived 2,5‐furan dicarboxylate (FDC) as a ligand is reported as an electrocatalyst for anodic ethylene glycol oxidation with cathodic hydrogen evolution. The MOF structure was analyzed using single crystal X‐ray‐diffraction, TGA and thermodiffractometry, to establish its structure and verify phase purity. The material was dropcast on carbon fiber paper as a catalyst, and by using a three‐electrode system, UOW‐6 requires only 1.47 V to attain a current density of 50 mAcm‐2. During oxidation of the ethylene glycol (EG), UOW‐6 shows unprecedented selectivity towards formic acid with a Faradaic efficiency of 94% and remarkable stability over 20 days. The combination of electrochemical measurements and in situ Raman confirmed in situ formed NiOOH at the surface of UOW‐6 as the catalytically active sites for EG oxidation. This work not only presents a pioneering application of FDC‐based MOFs for polyethylene terephthalate (PET) upcycling but also underscores the potential of electrocatalysis in advancing sustainable plastic valorization strategies.

Nitrogen-doped Porous Carbon Supported Nickel Catalysts for Efficient Hydrodeoxygenation of Lignin-derived Vanillin to 2-methoxy-4-methylphenol in Ethanol

Driven by the urgent global demand for clean energy, the catalytic conversion of renewable lignin biomass has attracted widespread attention. In this work, we proposed a two-step method for synthesizing nickel-supported nitrogen-doped porous carbon catalyst (Ni/NPC) for the in-situ hydrodeoxygenation (HDO) of lignin-derived vanillin (VAN) to 2-methoxy-4-methylphenol (MMP). The process involved co-hydrothermal treatment and pyrolysis of a mixture containing feedstocks and ZnCl2 activator, with simultaneous N doping and pore construction. Under optimal conditions of 0.4MPa N2 at 220 ℃ for 4h, the Ni/NPC achieved 99.13% conversion of VAN and 97.32% yield of MMP using ethanol as a hydrogen donor. The enhanced catalytic activity was attributed to the synergistic effect of Ni metal sites and N doping, and efficient pore activation of ZnCl2. In addition, the Ni/NPC maintained relatively stable activity over four cycles. This cost-effective and simple synthesis method, coupled with the high activity of the catalyst, presents a viable strategy for upgrading lignin derivatives into high-value chemicals in the H2-free HDO process.

Synthesis of Ni-Cu/Mesoporous Silica Catalyst with Variation of TEOS and NH4OH Molar Ratio for Hydrocracking Waste Cooking Oil into Biofuel

Research on the development of sustainable and renewable energy sources has been done and intensified due to the dwindling fossil fuel reserves. Biofuels that are derived from renewable biomass sources offer a promising alternative to traditional fuels. This study focuses on the synthesis and characterization of Ni-Cu/Silica catalysts for the hydrocracking of waste cooking oil into biofuels. Mesoporous silica as supporting material was synthesized with varying TEOS/NH4OH ratios and impregnated with Ni and Cu metals to enhance catalytic activity. The synthesized catalysts were characterized using FTIR, SEM-EDX, and GSA techniques to investigate their structural and textural properties. The catalyst with a TEOS/NH4OH ratio of 1:1 exhibited the highest acidity, surface area, and catalytic activity, resulting in a 71.52% conversion of waste cooking oil into biofuel with a selectivity of 97.69% towards paraffin. These findings demonstrate the potential of Ni-Cu/Silica catalysts for the efficient production of biofuels from waste cooking oil.

Synthesis, Spectral Characterization, Antimicrobial Activity, DFT Calculations, Molecular Docking and ADME Studies of Novel Schiff Base Co(II), Ni(II), Cu(II) and Zn(II) Complexes Derived from 4-nitro-ortho-phenylenediamine.

A condensation reaction was carried out between 4-nitro-ortho-phenylenediamine and 5-bromosalicyaldehyde to synthesize a novel Schiff base ligand 2,2'-[(1E,1'E)-(4-nitro-1,2-phenylene) bis (azaneylylidene) bis (methaneylylidene)] bis (4-bromophenol) [NB] in the current investigation. This was followed by the synthesis of metallic complexes comprising the Co(II), Ni(II), Cu(II) and Zn(II) transition metal ions. A hexadentate environment encircling metal complexes was corroborated by the results of varied spectroscopic methods that were employed to unravel the structure of the ligand and metal complexes. The Tauc's plot and Urbach energy were utilized for quantifying the optical energy band gap to provide insight into optical characteristics. The Coats-Redfern method of thermal analysis was implemented to do the kinetic and thermodynamic calculations. Furthermore, DFT studies were performed to predict geometrical structures and the stability of the compounds. Thorough investigation to evaluate their biological efficacies, docking studies was executed against COVID-19 main protease (PDB-7VAH), Dengue virus NS2B/NS3 protease (PDB-2FOM) and Mycobacterium Tuberculosis (PDB-5AF3). Apart from this, in silico ADMET studies were also accomplished for elucidation of drug likeness characteristics and the results attained disclose the significant proficiency of synthesized compounds. Besides this, antimicrobial studies were assessed with different microbial strains and result validates cobalt and zinc complexes as most potent against the selected bacterial and fungal strains.

Electronic Feature Modification of Ni and Co Free Metal–Organic Framework Nanoparticles by Vanadium Introduction for Water Oxidation

Electronic Feature Modification of Ni and Co Free Metal–Organic Framework Nanoparticles by Vanadium Introduction for Water Oxidation

Catalytic charge synergy on Ni/Sr@rTiO2 system to promote hydrogen evolution for the implementation of green energy technologies

This study demonstrates an effective and sustainable approach for hydrogen production to the practical implementation of green energy technologies. For this purpose, extremely stable catalysts Ni/Sr@rTiO2 have been synthesized and evaluated for hydrogen evolution reactions. Optical and structural characteristics of catalysts have been evaluated via advanced analytical techniques. These techniques include XRD, UV–Vis/DRS, PL, FT-IR, Raman, SEM, AFM and TEM. Surface area and porosity were obtained with BET while, chemical compositions of catalysts were authenticated via EDX, and XPS. All photoreaction was done in 150 mL reactor (Quartz). Hydrogen evolution activities were examined on GC-TCD (Shimadzu-2010/Japan). Results indicate that bare rutile titanium dioxide (rTiO2) and Ni1.5/Sr0.5@rTiO2 have delivered 0.20 mmol g−1h−1 and 35.14 mmol g−1h−1 of hydrogen respectively. Higher activities (i.e. in case of Ni1.5/Sr0.5@rTiO2) were attributed to the rapid charge transfer on active sites i.e. Ni metal centers. It has been predicted that presence of strontium promotes electrons to the conduction bands of rTiO2; hence favor to elevate the electronic pools so that they can progressively involve for water reduction. The results revealed that Ni1.5/Sr0.5@rTiO2 exhibit higher charge separation relative to the bare rTiO2. It has been noted that formation of synergy for the electron quenching and utilization is main cause of higher hydrogen evolution that is due to presence of nickel and strontium. On the basis of results, it has been concluded that catalyst reported herein has potential to replace the expensive and traditional catalysts associated with hydrogen generation technologies.

Ferrocene‐Based Nickel Metal–Organic Framework Nanosheets as Efficient, Long‐Cycle Cathode Catalyst for Li‐CO2 Battery

AbstractLi‐CO2 batteries, as a novel type of secondary battery, show great potential for energy conversion and storage. However, challenges such as large electrode polarization and poor cycling performance, stemming from difficulties in decomposing discharge products, limit their practical application. Here, Ferrocene‐based nickel metal–organic framework (Ni‐Fc) nanosheets structure to act as cathode catalysts, prepared via a one‐pot solvothermal reaction. X‐ray absorption fine structure (XAFS) analysis shows that Ni metal forms abundant catalytic active centers with O coordination of carboxylic acid groups in ferrocene units. The Ni‐Fc‐based battery demonstrates a high discharge capacity of 18636 mAh g−1 and exhibits a cycle life exceeding 2000 h at a current of 200 mA g−1. Density functional theory (DFT) calculations indicate that the stronger interaction of Ni‐Fc with discharge intermediates and enhanced Li adsorption accelerate battery reaction kinetics. This study introduces novel catalyst design concepts aimed at achieving high‐performance CO2 reduction and oxidation, thereby advancing Li‐CO2 batteries toward practical application.

Nickel coated paper electrode constructed by interfacial electrodeposition for biomass upgrading at industrial current density

Substituting the kinetically slow oxygen evolution reaction (OER) with biomass electrooxidation significantly decreases the energy demand of water electrolysis. However, exploring and optimizing efficient electrocatalysts remains a challenge for large−scale production of valuable chemicals and hydrogen. Herein, we have constructed a nickel coated paper electrode (NiCo@Ni/CP) composed of crystalline Ni metal and amorphous NiCo hydroxide nanosheets layers via interfacial electrodeposition on carbon paper (CP) for monosaccharide oxidation reactions (MOR), which achieved a formate yield of 82.4 %. Remarkably, the flow electrolyzer maintained an industrial−grade current density of 1 A cm−2 at 1.70 V with exceptional stability over 100 h, also displaying significant co−generation Faradaic efficiencies of approximately 80.0 % and 97.3 % for formate and hydrogen production, respectively. The superior performance is attributed to the redistribution of electrons at the Ni and amorphous NiCo hydroxide interface, which enhances charge transfer and reactant adsorption by adjusting the d−band center, hence reducing deprotonation and C−C bond cleavage energies of xylose during MOR. This work provides a promising strategy for the design of efficient catalysts for biomass upgrading and the production of hydrogen at high current densities.

Nickel toxicology testing in alternative specimen from farm ruminants in a urban polluted environment

The impact of nickel (Ni) metal toxicity, on public health was assessed analyzing forage samples (Acacia nilotica, Zea mays, Pennisetum glaucum, Capparis decidua and Medicago sativa), soils and blood samples of cow, buffalo and sheep (blood plasma, fecal, and hair) collected from three different agro-ecological zones and analyzed through atomic absorption spectrophotometer. Results showed that nickel values differed in soil samples ranging from 4.49 to 9 to 25 mg/kg, in forages from 3.78 to 9.53 mg/kg and in animal samples from 0.65 to 2.42 mg/kg. Nickel concentration, in soil and forage samples, was below the permitted limits. Soil with the minimum nickel level was found under C. decidua while the maximum concentration was reached under the A. nilotica. Among the animals, nickel was maximum in buffaloes that grazed on the Z. mays fodder. Ni was more accumulated in feces than other body tissues. The sheep and buffaloes showed high vulnerability to Ni pollution due to the highest contamination levels at site II and III. Bioconcentration factor, pollution load index and enrichment factor were found to be higher in buffaloes than cows, respectively. The daily intake and health risk index ranged from 0.0056 to 0.0184 mg/kg/day and 0.186–0.614 mg/kg/day respectively. In short, the results of this study evidenced that Nickel-containing fertilizers should never not be used to grow forage species. Government should to lessen the toxic metal accessibility to animals. Although general values were lower than the admitted limit, nickel can be accumulated and the consume of food containing nickel can increase health risks. General monitoring of soil and vegetation pollution load, as well as the use of other non-conventional water like canal water for forage irrigation could be a sustainable solution to decrease the access of nickel in the food chain.

Enhancement of CO2 adsorption and oxygen transfer properties on γ-Al2O3 support through surface modification with MgO-ZrO2 for coke suppression over Ni catalyst in CO2 reforming of methane

This work focuses on employing commercial γ-Al2O3 for surface modification with MgO-ZrO2 mixed oxide to enhance the potential of CO2 adsorption and oxygen mobility. This enhancement facilitates its application as a support in catalysts for CO2 utilization such as CO2 reforming of methane (CRM). To achieve this perspective, γ-Al2O3 was modified with 10 wt.% of various MgO and ZrO2 contents (MgO:ZrO2= 10:0, 9:1,7:3, 5:5, 3:7, 1:9 and 0:10) using the impregnation method. All samples including unmodified γ-Al2O3 (Al) were characterized. Due to the increase in basicity and oxygen transfer around the surface, the improvement of the CO2 adsorption was observed on γ-Al2O3 modified with 9 wt.% MgO-1 wt.% ZrO2 (9Mg1ZrAl) and 10 wt.% MgO (10MgAl), respectively. An application of these two superior samples as a support of 10 wt.% Ni (10Ni) catalysts for CRM was investigated and compared with an unmodified γ-Al2O3. Characterization results suggest the formation of NiO-MgO solid solution at the surface due to the decrease in metal-support interaction and the increase in metal dispersion. The Ni catalysts with the surface-modified support show higher CO2 activity that raises carbon deposition resistance. The greatest coke prevention was observed on 10Ni/9Mg1ZrAl that lowers the coke deposition by 42 % compared to 10Ni/Al. It indicates that the composition of this modification allowed very low ZrO2 portion to merge with MgO and MgO to form solid solution with NiO. This enables the 10Ni/9Mg1ZrAl catalyst to generate labile oxygens which can be conveyed to the Ni metal sites on the catalyst.

Kinetic modelling of carbothermal reduction of nickel oxide (NiO): Design of Experiments (DOE) approach

ABSTRACT This study presents a mathematical model to evaluate the kinetics of the carbothermal reduction of NiO using graphite. Based on the shrinking core theory, the model was validated against experimental data obtained under both isothermal and non-isothermal conditions. The shrinking core model for isothermal and non-isothermal conditions was created using MATLAB software for the kinetic modelling of the reduction process to determine the extent of reduction and the reaction rate. The kinetics were mathematically modelled from independently measured physical and thermodynamic properties of the reaction system and experimentally measured properties. The carbothermal reduction method was effective in producing Ni metal from NiO and was considered an established basis for evaluating the modelling aspect of the solid–gas system. The experimental investigation of carbothermal reduction was conducted using a statistical design of experiments (DOE), employing a two-level factorial design (23). The experiments were performed for a range of different factors, namely reduction temperature (800-1000°C), reduction time (1-2 h), and the molar ratio of graphite to NiO (0.5-1.5) on the extent of reduction. The extent of reduction increases with increasing reduction temperature, reduction time, and molar ratio of C to NiO. The highest extent of reduction (77.9%) was achieved at a reduction temperature of 1000°C, 2 h of reduction time, and the molar ratio of C to NiO as 1.5. The X-ray diffraction (XRD) studies confirmed the formation of Ni at a lower reduction time, but the intensity of the Ni phase was higher for a longer duration of reduction. SEM-EDS analysis of the reduced products confirmed the formation of Ni in the form of elongated and larger grains, along with traces of residual or unreacted carbon. The predicted extent of reduction is then compared with the experimentally measured results. The kinetic modelling results proved that both isothermal and non-isothermal shrinking core models showed similarity and significant closeness to the experimental data. The deviation between the experimental and model results could be due to the varying geometry and porosity of the reactants and intermediate products.

Searching for the optimum Pt loading in bimetallic PtXNi/SBA-15 catalysts for hydrodeoxygenation

Bimetallic PtXNi5/SBA-15 catalysts with 5 wt% Ni and X = 0.1–2.0 wt% Pt were synthesized and characterized. The XPS characterization of bimetallic catalysts showed the presence of oxide Ni2+, Pt2+ and reduced Pt0 species in the calcined catalysts. After the reduction, metallic Ni0 appeared in addition to the above-mentioned species. The proportions of the reduced Ni and Pt increased with increasing Pt content in the catalysts. The presence of metal species of different oxidation states at the Ni–Pt interface was crucial for their catalytic performance in the hydrodeoxygenation of anisole. The Pt0.5Ni5/SBA-15 catalyst was the most active and selective.Graphical abstract

Detection of Tert-Butylhydroquinone in Edible Oils Using an Electrochemical Sensor Based on a Nickel-Aluminum Layered Double Hydroxide@Carbon Spheres-Derived Carbon Composite.

Phenolic antioxidants such as tert-butylhydroquinone (TBHQ) can prolong the shelf life of edible oils by delaying the oxidation process. The excessive use of TBHQ can damage food quality and public health, so it is necessary to develop an efficient TBHQ detection technique. In this work, nickel-aluminum double hydroxide (NiAl-LDH) was grown on glucose carbon spheres (GC), which formed porous carbon nanomaterials (named NiAl-LDH@GC-800) after pyrolysis at 800 °C. The successful synthesis of the material was verified by scanning electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. The obtained NiAl-LDH@GC-800 was dopped onto a glass carbon electrode to prepare an electrochemical sensor for TBHQ. The synergistic effect of porous carbon and Ni metal reduced from NiAl-LDH by high-temperature calcination accelerated the electron transfer rate and improved the sensitivity of the sensor. The prepared sensor showed a low limit of detection (LOD) of 8.2 nM, a high sensitivity (4.2 A·M-1), and a good linear range (20~300 µM) in detecting TBHQ. The sensor was also successfully used for TBHQ detection in edible oils, including chili oil, peanut oil, and rapeseed oil.

Application of Ni‐Based MOFs Catalyst in Oxidative Coupling Reaction of Benzylamine

AbstractNanoparticles made of porous coordination polymers, known as metal‐organic frameworks (MOFs), are becoming increasingly popular in nanomaterials research, especially in catalytic applications. With their intricate architectures, MOFs make it possible to incorporate metal nodes, encapsulate substrates, and use functional linkers, all of which contribute to synergistic engineering. A Ni‐based metal‐organic framework sample was prepared by the solvothermal method with NiCl2.6H2O as a precursor of Ni metal and terephthalic (H2BDC) acid as a linker. The as‐synthesized NiBDC was verified by X‐ray diffraction (XRD), Fourier‐transform infrared spectroscopy (FT‐IR), scanning electron microscopy (SEM), scanning electron microscopy with energy dispersive X‐ray spectroscopy (SEM‐EDX), transmission electron microscopy (TEM), and N2 adsorption/desorption isotherms. Based on these findings, we applied the as‐synthesized NiBDC to the oxidative coupling reaction of benzylamine. The results revealed that with NiBDC as a heterogeneous catalyst, the oxidative coupling reaction of benzylamine achieved a performance of 92%. Furthermore, the catalyst maintains good stability after four catalytic cycles, with an efficiency of approximately 82%.

Comprehensive extraction of V, Ni and Mo from black shale via selective leaching oxidation process

Black shale is one of the most representative sources of vanadium, nickel and molybdenum in China. Due to the poor endowment of minerals in black shale, V, Ni, Mo and other metals complex co-associated endowment state, extraction is difficult and long-term unused, resulting in a significant waste of resources. In this paper, it is shown that V, Ni and Mo can be obtained from black shale by a stepwise oxidation leaching process. In a first leaching process, V and Ni are effectively leached simultaneously. Mo is left in the residue. The leaching efficiency of V, Ni and Mo was 86.81 %, 89.19 % and 5.80 % respectively under the leaching conditions of 35 wt% H2SO4, 4 wt% CaF2, 1.2:1 liquid to solid ratio (L/kg), 95℃ and 8 h. The residue was then leached twice. The leaching efficiency of molybdenum was 91.10 % under the leaching conditions of 25 wt% H2SO4, 8 wt% NaClO3, 1.5:1 liquid to solid ratio (L/kg), 45℃ and 7 h. V2O5 products have been successfully prepared, the purity of V2O5 reaches 98.34 %. A stepwise oxidation leaching method has been proposed to separate the vanadium, nickel and molybdenum in the leaching process. Vanadium, nickel and molybdenum can be effectively extracted from the black shale by the stepwise oxidation leaching process to maximize the utilization of the resources.

Exploring the efficacy of Re-Ni embedded KIT-6/H-Mor catalysts for renewable energy – A comprehensive experimental and theoretical (DFT) exploration

The global market for n-propyl benzene value is projected to reach $30.47 billion by 2030, with a CAGR of 4.3% from 2023 to 2030. This market analysis identifies diverse applications for propyl benzene, spanning the petroleum industry, industrial chemicals, automotive sector, and more. The research introduces eugenol, a compound derived from lignin, as a model compound for bio-oil to n-propyl benzene (bio-fuel analogs) production. A novel Re-Ni/KIT-6-H-Mordenite catalyst is developed for efficient hydrodeoxygenation of eugenol, showcasing high conversion rates and selectivity under moderate temperatures. Comprehensive characterization techniques and theoretical calculations highlight the synergistic interaction between Re and Ni metals. The catalyst’s reusability and successful application for bio-fuel production under atmospheric conditions further validate its potential. This study pioneers the exploration of Re-Ni bimetallic catalysts for HDO of lignin-derived compounds, offering valuable insights into sustainable bio-fuel development.

Synthesis, characterization, antimicrobial activity of 2-amino-5-picoline and dipicolinic acid of Ni(II) and Cu(II) metal complexes

Synthesis, characterization, antimicrobial activity of 2-amino-5-picoline and dipicolinic acid of Ni(II) and Cu(II) metal complexes

Electronic interaction between d electron-poor and d electron-rich transition metal ions promoted the CO2 capture performance of calcium-based adsorbent

The investigation of intrinsic principles for the more precise design CaO adsorbent with excellent CO2 capture performance by doping metal oxides is of great significance, but has not yet been explored. Herein, we address the critical challenge by systematical evaluation on a series of magnetic bimetallic oxides doped calcium-based adsorbents from the perspective of electronic interaction between d electron-poor and d electron-rich transition metal ions promoting the CO2 capture performance. The Mn, Co, Mo and Ni metal ions with varied d-electron numbers are doped into calcium-based adsorbent, and the results show that the introduction of magnetic bimetallic oxides with d electron-poor and d electron-rich transition metal ions into CaO at the same time can significantly promote the stability of CO2 capture. Taking the (Mn-Co)-codoped samples as an example, the relationship of d electron-poor and d electron-rich transition metal ions synergistic interaction and promoted CO2 adsorption performance is elucidated. The loose flake nanostructures favor the diffusion of CO2 inside the particles, and the uniform distribution of each component effectively ensures the double-exchange interactions. The generation of more oxygen vacancies significantly improves the CO2 affinity for the calcium-based sample. Furthermore, the results of kinetic analysis reveal that the synergistic interaction can reduce the apparent activation energy of carbonation reaction. These insights into the systematical regulation of the double-exchange interaction are expected to provide guidance for the relatively more precise design of the calcium-based adsorbent with high performance of CO2 adsorption.

Ab initio calculations of high-entropy clusters for oxygen reduction and evolution as well as CO2 reduction reactions

This study introduces a design concept for a high-entropy cluster (HEC) comprising of Fe, Co, Ni, Cu, and Rh metals supported on nitrogen-doped graphene. Five different configurations including CoNiCuRh@FeN4, FeNiCuRh@CoN4, FeCoCuRh@NiN4, FeCoNiRh@CuN4, as well as; FeCoNiCu@RhN4 with the mixing entropy change of ΔSmix = 0.14 meV/K were considered. The positive dissociation potential and negative formation energy suggested the electrochemical and thermodynamic stabilities of these materials. According to density functional theory (DFT + U) calculations, the CoNiCuRh@FeN4 catalyst led to the overpotentials of 0.37 VRHE, 0.37 VRHE, and 0.24 VRHE for the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and CO2 reduction reaction (CO2RR) towards CO production, respectively. It was determined that, FeN4 acted as an active site, while CoNiCuRh-HEC behaved as the modulator. Also, FeNiCuRh@CoN4 catalyst led to the CO2RR overpotential of 0.35 VRHE towards CH3OH formation where CoN4 acted as the active site, and FeNiCuRh-HEC species acted as the modulator surpassing the activity of single-atom catalysts (SAC). Moreover, the density of states (DOS) and charge transfer analyses suggested that, the presence of a high-entropy cluster may enhance the charge transfer and stabilize the reaction intermediates, toward selective methanol formation. Therefore, a DFT-based strategy to design a high-entropy cluster was developed through electrochemistry and beyond.