Catalytic Electrode Research Articles

High energy-efficiency decomplexation of metal-complexes by H*-mediated electro-reduction on hydroxyphenyl Co-porphyrin catalysts

Electrochemical reduction of metal-organic complex pollutants has been recognized as an environmental benign method that operates at mild condition. However, the selective reduction of metal complexes and energy consumption in cathodic process are still a big challenge. Herein, we found that hydroxyphenyl Co-porphyrin catalyst (CoTH@NG) realizes the highly selective decomplexation of metal-organic complexes by H* -mediated reduction, and simultaneously the impressive recovery efficiency of metal ions. Density functional theory (DFT) confirms the generation and capturing ability of H* on CoTH@NG, verifying the dominant role of H* -mediated reduction in the selective decomplexation of Cu-EDTA. CoTH@NG realizes the superior energy efficiency for Cu-EDTA removal (279.3 g kWh−1 of EEOCu-EDTA) and Cu recovery (48.6 g kWh−1 of EEOCu), which are remarkably 3.3 × 102 and 9.7 × 102 times higher than traditional carbon cloth electrode. Moreover, the recovered Cu0(s) nanowires on the electrode surface can be efficiently regenerated in HCOOH by a galvanic reaction through the electron channel of CoTH@NG, regenerating catalytic electrode. This is one of the pioneer studies on H* -mediated electro-reduction decomplexation of metal-complexes, metal recovery, and electrode regeneration on CoTH@NG, which providing a technical strategy for developing efficient electrocatalytic system for pollution control.Environmental ImplicationMetal complexes is a dramatic increase in the electroplating and mining industries, and seriously affect both public health and environmental sustainability. Our work reported a new hydroxyphenyl Co-porphyrin catalyst (CoTH@NG) which achieves the selective decomplexation of metal-organic complexes, and simultaneously the recovery of metal ions. CoTH@NG realizes the superior energy efficiency for Cu-EDTA removal (279.3 g kWh−1) and Cu0(s) recovery (48.6 g kWh−1), which are remarkably 3.3 × 102 and 9.7 × 102 times higher than traditional carbon cloth electrode. Moreover, the recovered Cu0(s) can be efficiently regenerated in HCOOH by a galvanic reaction through the electron channel of CoTH@NG, regenerating catalytic electrode.

CrOx Modified Nickel Phosphides Electrocatalyst for Stable Hydrogen Evolution Reaction in Neutral Media

AbstractThe development of efficient and long‐term stable electrodes for hydrogen evolution reaction (HER) in seawater is highly desirable for hydrogen generation but remains challenging. In this work, a highly active CrOx@Ni2P‐Ni5P4/NF electrode is developed and investigated its dynamic reconstruction for HER in neutral electrolytes. The combination of in situ Raman spectra and electrochemical measurements revealed the dynamic surface reconstruction of the catalyst during HER. The CrOx modification not only effectively facilitates water dissociation but also stabilizes the structure post‐reconstruction, enabling rapid and stable hydrogen generation in neutral media. Remarkably, CrOx@Ni2P‐Ni5P4/NF exhibits overpotentials of 109 and 263 mV at current densities of 10 and 100 mA cm−2 in 1 m PBS, respectively. Concurrently, it exhibits stable operation for 500 h in 1 m PBS and 140 h in natural seawater at current densities of 50 and 100 mA cm−2, respectively. The proposed catalytic electrode and the mechanistic insights present a significant stride toward the realization of metal phosphides for direct seawater splitting.

Hydrochar from Pine Needles as a Green Alternative for Catalytic Electrodes in Energy Applications.

Hydrothermal carbonization (HTC) serves as a sustainable method to transform pine needle waste into nitrogen-doped (N-doped) hydrochars. The primary focus is on evaluating these hydrochars as catalytic electrodes for the oxygen reduction reaction (ORR) and carbon dioxide reduction reaction (CO2RR), which are pivotal processes with significant environmental implications. Hydrochars were synthesized by varying the parameters such as nitrogen loading, temperature, and residence time. These materials were then thoroughly characterized using diverse analytical techniques, including elemental analysis, density measurements, BET surface area analysis, and spectroscopies like Raman, FTIR, and XPS, along with optical and scanning electron microscopies. The subsequent electrochemical assessment involved preparing electrocatalytic inks by combining hydrochars with an anion exchange ionomer (AEI) to leverage their synergistic effects. To the best of our knowledge, there are no previous reports on catalytic electrodes that simultaneously incorporate both a hydrochar and AEI. Evaluation metrics such as current densities, onset and half-wave potentials, and Koutecky-Levich and Tafel plots provided insights into their electrocatalytic performances. Notably, hydrochars synthesized at 230 °C exhibited an onset potential of 0.92 V vs. RHE, marking the highest reported value for a hydrochar. They also facilitated the exchange of four electrons at 0.26 V vs. RHE in the ORR. Additionally, the CO2RR yielded valuable C2 products like acetaldehyde and acetate. These findings highlight the remarkable electrocatalytic activity of the optimized hydrochars, which could be attributed, at least in part, to their optimal porosity.

Recycled Cathodes in Rechargeable Aqueous Batteries as Ready-Made Electrodes for Oxygen Evolution Catalysis.

The development of a low-cost and efficient oxygen evolution reaction (OER) electrode is of critical importance for water electrolysis technologies. The general approach to achieving a high-efficiency OER electrode is to regulate catalytic material structures by synthetic control. Here we reported an orthogonal approach to obtaining the OER electrode without intentional design and synthesis, namely, recycling MnO2 cathodes from failed rechargeable aqueous batteries and investigating them as ready-made catalytic electrodes. The recycled MnO2 cathode showed very little Zn2+ storage capacity but surprisingly high OER activity with a low overpotential of 307 mV at 10 mA cm-2 and a small Tafel slope of 77.9 mV dec-1, comparable to the state-of-the-art RuO2 catalyst (310 mV, 86.9 mV dec-1). In situ electrochemical and theoretical studies jointly revealed that the accelerated OER kinetics of the recycled MnO2 electrode was attributed to the enlarged active surface area of MnO2 and optimized electronic structure of Mn sites. This work suggests failed battery cathodes as successful catalysis electrodes for sustainable energy development.

A Highly Reversible Sn‐Air Battery Possessing the Ultra‐Low Charging Potential with the Assistance of Light

AbstractAqueous Sn‐air batteries are attracting a great deal of interest in recent years due to the ultra‐high safety, low cost, dendrite‐free and highly reversible Sn anode. However, the slurry oxygen reduction/evolution reaction (ORR/OER) kinetics on the air cathodes seriously affect the Sn‐air battery performances. Although various advanced catalysts have been developed, the charge overpotentials (~1000 mV) of these Sn‐air batteries are still not satisfactory. Herein, iron oxide (Fe2O3) modified titanium dioxide (TiO2) nanorods with heterogeneous structure are firstly synthesized on Ti mesh (Fe2O3@TiO2/Ti), and the obtained Fe2O3@TiO2/Ti films are further applied as catalytic electrodes for Sn‐air batteries. The core–shell heterogeneous structure of Fe2O3@TiO2/Ti can effectively facilitate the conversion of electrochemical intermediates and separation of photo‐excited electrons and holes to activate oxygen‐related reaction processes. Density functional theory (DFT) and experimental results also confirm that Fe2O3@TiO2/Ti can not only act as the electrocatalysts to improve ORR/OER properties, but also exhibit the superior photo‐catalytic activity to promote charging kinetics. Hence, the Fe2O3@TiO2/Ti‐based Sn‐air batteries show ultra‐low overpotential of ~40 mV, excellent rate capability and good cycling stability under light irradiation. This work will shed light on rational photo‐assisted catalytic cathode design for new‐type metal‐air batteries.

A Highly Reversible Sn-Air Battery Possessing the Ultra-Low Charging Potential with the Assistance of Light.

Aqueous Sn-air batteries are attracting a great deal of interest in recent years due to the ultra-high safety, low cost, dendrite-free and highly reversible Sn anode. However, the slurry oxygen reduction/evolution reaction (ORR/OER) kinetics on the air cathodes seriously affect the Sn-air battery performances. Although various advanced catalysts have been developed, the charge overpotentials (~1000 mV) of these Sn-air batteries are still not satisfactory. Herein, iron oxide (Fe2O3) modified titanium dioxide (TiO2) nanorods with heterogeneous structure are firstly synthesized on Ti mesh (Fe2O3@TiO2/Ti), and the obtained Fe2O3@TiO2/Ti films are further applied as catalytic electrodes for Sn-air batteries. The core-shell heterogeneous structure of Fe2O3@TiO2/Ti can effectively facilitate the conversion of electrochemical intermediates and separation of photo-excited electrons and holes to activate oxygen-related reaction processes. Density functional theory (DFT) and experimental results also confirm that Fe2O3@TiO2/Ti can not only act as the electrocatalysts to improve ORR/OER properties, but also exhibit the superior photo-catalytic activity to promote charging kinetics. Hence, the Fe2O3@TiO2/Ti-based Sn-air batteries show ultra-low overpotential of ~40 mV, excellent rate capability and good cycling stability under light irradiation. This work will shed light on rational photo-assisted catalytic cathode design for new-type metal-air batteries.

Interfacial electronic modulation of NiCo decorated nano-flowered MoS2 on carbonized wood as a remarkable bifunctional electrocatalyst for boosting overall water splitting

The development of a cost-effective and efficient bifunctional electrode for overall water splitting holds significant importance in accelerating the sustainable advancement of hydrogen energy. The present study involved a bifunctional catalytic electrode was prepared by loading NiCo-modified 1T/2H MoS2 onto carbonized wood (NiCo-MoS2-CW) using the hydrothermal and electrodeposition techniques. The XPS analysis revealed that NiCo-modified MoS2 exhibited a weak electron characteristic, which facilitated the ionization of H2O and significantly enhanced the Volmer step. The XPS analysis unveiled that NiCo-modified MoS2 displayed a weak electron characteristic, thereby promoting the ionization of H2O and substantially augmenting the Volmer step. The electrocatalytic performance of the NiCo-MoS2-CW in 1.0 M KOH is remarkably impressive, exhibiting minimal overpotentials of only 64 mV (10 mA cm−2) and 216 mV (50 mA cm−2) for the hydrogen evolution reaction and oxygen evolution reaction, respectively. The NiCo-MoS2-CW || NiCo-MoS2-CW electrolytic cell can achieve a cell voltage of only 1.69 V to achieve a current density of 50 mA cm−2. Overall, this study proposes a potential approach to improve the catalytic efficiency of overall water splitting by modulating the interfacial electronic properties of MoS2.

CoFe hydroxide towards CoP2-FeP4 heterojunction for efficient and long-term stable water oxidation

Electrochemical water splitting stands out as a promising avenue for green hydrogen production, yet its efficiency is fundamentally governed by the oxygen evolution reaction (OER). In this work, we investigated the growth mechanism of CoFe hydroxide formed by in situ self-corrosion of iron foam for the first time and the significant influence of dissolved oxygen in the immersion solution on this process. Based on this, the CoP2-FeP4/IF heterostructure catalytic electrode demonstrates exceptional OER activity in a 1 M KOH electrolyte, with an overpotential of only 253 ± 4 mV (@10 mA cm−2), along with durability exceeding 1000 h. Density functional theory calculations indicate that constructing heterojunction interfaces promotes the redistribution of interface electrons, optimizing the free energy of adsorbed intermediate during the water oxidation process. This research highlights the importance of integrating self-corroding in-situ growth with interface engineering techniques to develop efficient water splitting materials.

Energy Storage Application of CaO/Graphite Nanocomposite Powder Obtained from Waste Eggshells and Used Lithium-Ion Batteries as a Sustainable Development Approach.

The reuse of waste materials has recently become appealing due to pollution and cost reduction factors. Using waste materials can reduce environmental pollution and product costs, thus promoting sustainability. Approximately 95% of calcium carbonate-containing waste eggshells end up in landfills, unused. These eggshells, a form of bio-waste, can be repurposed as catalytic electrode material for various applications, including supercapacitors, after being converted into CaO. Similarly, used waste battery electrode materials pose environmental hazards if not properly recycled. Various types of batteries, particularly lithium-ion batteries, are extensively used worldwide. The recycling of used lithium-ion batteries has become less important considering its low economic benefits. This necessitates finding alternative methods to recover and reuse the graphite rods of spent batteries. Therefore, this study reports the conversion of waste eggshell into calcium oxide by high-temperature calcination and extraction of nanographite from spent batteries for application in energy storage fields. Both CaO and CaO/graphite were characterized for their structural, morphological, and chemical compositions using XRD, SEM, TEM, and XPS techniques. The prepared CaO/graphite nanocomposite material was evaluated for its efficiency in electrochemical supercapacitor applications. CaO and its composite with graphite powder obtained from used lithium-ion batteries demonstrated improved performance compared to CaO alone for energy storage applications. Using these waste materials for electrochemical energy storage and conversion devices results in cheaper, greener, and sustainable processes. This approach not only aids in energy storage but also promotes sustainability through waste management by reducing landfills.

3D transition metal boride monolithic electrode for industrial hectoampere-level current anion exchange membrane water electrolysis

High performance, cost-efficient anion exchange membrane water electrolysis (AEMWE) is of great current interest for industrial-level hydrogen production. However, the lack of active and robust catalytic electrode severely impedes the development of this technology. Herein, a versatile strategy of 3D hierarchical porous monolithic electrode enabling industrial hectoampere-level current AEMWE is successfully explored for the first time. By a facile electroless plating technique coupled with corrosion engineering process, a series of low-cost and highly active 3D transition metal boride (etched-TMB, TM=Ni, Co, NiP, NiMo, CoP, CoMo, CoNi) catalytic electrodes have been prepared. A distinctive hierarchically structured etched-NiPB@MS alloy monolithic electrode exhibits a superior bifunctional hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) catalytic activity and large-current stability, which derive from enhanced intrinsic activity, sufficient electrochemical active sites, mechanical stability as well as efficient gas/liquid transport pathways. An AEMWE electrolyzer with 10×10 cm2 etched-NiPB@MS as both anode and cathode works efficiently at large current of 100 A (1 A cm−2) and reaches a H2 production rate of 41.78 L h−1, verifying its huge potential for industrial hydrogen production. This study paves out a new approach for high-efficient catalytic electrode and industrial-level current AEMWE.

Controlled synthesized of ternary Cu-Co-Ni-S sulfides nanoporous network structure on carbon fiber paper: a superior catalytic electrode for highly-sensitive glucose sensing

BackgroundEfficient monitoring of glucose concentration in the human body necessitates the utilization of electrochemically active sensing materials in nonenzymatic glucose sensors. However, prevailing limitations such as intricate fabrication processes, lower sensitivity, and instability impede their practical application. Herein, ternary Cu-Co-Ni-S sulfides nanoporous network structure was synthesized on carbon fiber paper (CP) by an ultrafast, facile, and controllable technique through on-step cyclic voltammetry, serving as a superior self-supporting catalytic electrode for the high-performance glucose sensor.ResultsThe direct growth of free-standing Cu-Co-Ni-S on the interconnected three-dimensional (3D) network of CP boosted the active site of the composites, improved ion diffusion kinetics, and significantly promoted the electron transfer rate. The multiple oxidation states and synergistic effects among Co, Ni, Cu, and S further promoted glucose electrooxidation. The well-architected Cu-Co-Ni-S/CP presented exceptional electrocatalytic properties for glucose with satisfied linearity of a broad range from 0.3 to 16,000 μM and high sensitivity of 6829 μA mM− 1 cm− 2. Furthermore, the novel sensor demonstrated excellent selectivity and storage stability, which could successfully evaluate the glucose levels in human serum. Notably, the novel Cu-Co-Ni-S/CP showed favorable biocompatibility, proving its potential for in vivo glucose monitoring.ConclusionThe proposed 3D hierarchical morphology self-supported electrode sensor, which demonstrates appealing analysis behavior for glucose electrooxidation, holds great promise for the next generation of high-performance glucose sensors.

Exploring the Use of Fe2.5Ni2.5Sn3 as a Monolithic Catalyst for Oxygen Evolution Reaction Under Alkaline Conditions

Abstract Enabling a hydrogen fuel-based economy is reliant on the discovery of materials that catalyze the electrolysis of water which requires low-cost catalytic electrodes to improve the kinetics of the oxygen evolution reaction. Fe2.5Ni2.5Sn3, was prepared by arc-melting and electrochemical studies were conducted to evaluate its ability to catalyze the oxygen evolution reaction. Potentiodynamic polarization testing revealed that the Fe2.5Ni2.5Sn3 alloy had a Tafel slope of 40 mV/decade and required an overpotential of 326 mV in order to obtain a current density of 10 mA/cm2. X-ray photoelectron spectroscopy studies indicated that the native oxide present on the surface became hydrated upon subjecting it to oxygen evolution studies.

The study of the effects of grain size, orientation and dislocation density on the HER performance of copper catalysts

Utilizing multi-pass friction stir processing with recirculating water cooling, pure copper plates were processed to successfully synthesize catalysts with distinct grain sizes. An exhaustive investigation into their intrinsic structures and properties was conducted. Analyses using X-ray diffraction (XRD) and electron backscatter diffraction (EBSD) revealed that Cu-4.85 exhibits a preferred (111) crystallographic orientation along with a high dislocation density. Transmission electron microscopy (TEM) images clearly identified the types of dislocations present within Cu-4.85. Density functional theory (DFT) calculations further demonstrated that Cu-4.85 displays lower Gibbs free energy at the hollow site on the (111) plane, thereby facilitating the H* adsorption process. Collectively, this study delves into the cooperative influence of grain size, crystal orientation and dislocation density on the electrocatalytic hydrogen evolution (HER) performance. It was found that Cu-4.85 demonstrates exceptional HER activity, characterized by a reduced overpotential and a low Tafel slope. The study elucidates the mechanism of H atom adsorption in Cu-4.85 during the HER process, furnishing theoretical foundations for enhancing HER catalytic performance and offering significant theoretical and experimental insights for the design and fabrication of copper catalytic electrodes.

Electrodeposition of CuxBi1-x-MOF for electrochemical reduction of CO2

Electrochemical reduction of carbon dioxide to hydrocarbon compounds such as formate offers a promising pathway to carbon-neutral future. Bismuth (Bi) has the advantages of low toxicity, good economic returns, and high overpotentials for hydrogen evolution reaction (HER). However, the Faradaic efficiencies and yield rates of Bi-based catalysts still need to be improved before applying to practical applications. In this work, bimetallic metal–organic framework Cux/Bi1-x-BTC was loaded on a copper foam electrode by one-step electrodeposition to form a catalytic electrode. The performance of Cux/Bi1-x-BTC electrodes for reducing carbon dioxide to formic acid was evaluated in H-type electrolytic cells. Electrochemical-prepared Cux/Bi1-x-BTC showed higher reaction rate and Faradaic efficiency (FE), than either Cu-BTC or Bi-BTC in a CO2‒saturated 0.1 M KHCO3 solution. Carbon dioxide was reduced to formic acid on CuxBi1-x-BTC electrtode. The Faradaic efficiency reached 73.4% at −1.5 V (vs. Ag/AgCl) and the conversion rate was 2.68 × 10−4 mol h−1 cm−2.

Synthesis of multifunctional Ti/RuO2-ZnO composite catalytic electrodes for electrochemical oxidation and hydrogen production from toluene-containing wastewater

Developing electrodes that effectively perform indirect oxidation on nondecomposable organic compounds is a key objective in electrochemical oxidation research. This study focuses on fabricating a Ti/RuO2-ZnO electrode through a simple pyrolysis method on a Ti substrate etched with hydrochloric acid. Hydrochloric acid etching played a pivotal role in enhancing coating stability by markedly increasing the Ti substrate's surface area and hydrophilicity. Analyzing the linear sweep voltammetry revealed that the electrode exhibited a low overvoltage of the oxygen evolution reaction, reaching 221 mV at 10 mA cm−2, indicating effective use as an active anode. The electrode's performance was evaluated by removing toluene contained in a 0.1 M NaCl solution at pH 5. The electrochemical reaction generated active chlorine in the solution, oxidizing 98.66 % of toluene over 3 h and concurrently producing 25.62 mL of hydrogen. This study presents a simple and effective synthesis of a RuO2-based active anode, demonstrating its potential application not only in removing toluene from wastewater but also in hydrogen production.

Efficient tuning of the selectivity of Cu-based interface for electrocatalytic CO2 reduction by ligand modification

The development of efficient strategies to tune the CO2RR selectivity of Cu-based catalytic interfaces, especially on specific domains, such as Cu (200) facets with high activity toward competitive hydrogenation evolution reaction (HER), remains a challenging task. In this work, Cu-based catalytic layers with thiocyanate (-SCN), cyanide (-CN), or ethylenediamine (-NH2R) coordination linkages are prepared on Cu nanocolumns arrays (Cu NCAs) with predominant (200) exposed facets. The coordination of these ligands induces more Cu+ species and inhibits the adsorption of H∗ on the Cu (200) facet, leading to enhanced CO2RR performance and substantially suppressing the competitive HER. The faradaic efficiency (FE) of Cu–SCN, Cu–CN, and Cu–NH2R NWAs for producing HCOOH, C2H4, and C1 mixture products (HCOOH and CO) reach to 66.5%, 21.1%, and 57.1%, respectively. In situ spectroscopic studies reveal Cu–SCN, Cu–CN, and Cu–NH2R exhibit more reasonable adsorption energy toward ∗OCHO, ∗CO, and ∗COOH intermediates, promoting the HCOOH, C2H4, and C1 mixture generation, respectively. This study might provide a new perspective for the development of high-performance Cu-based CO2RR catalytic electrodes based on the combination of various commercial free-standing Cu substrates and organic/inorganic ligands.

Comparison of Modifications for Enhancing the Electrooxidation Performance of Porous Ni Foil Catalytic Electrodes Derived from Paper Templates: Cu-Added Alloying and In Situ Growth of Ni-S Nanosheets

Comparison of Modifications for Enhancing the Electrooxidation Performance of Porous Ni Foil Catalytic Electrodes Derived from Paper Templates: Cu-Added Alloying and In Situ Growth of Ni-S Nanosheets

Influence of Nitrogen Position on the Electrocatalytic Performance of B,N-Codoped Carbon Quantum Dots for the Oxygen Reduction Reaction

Nanocomposites containing B,N-codoped carbon quantum dots (CQDs) and an anion exchange ionomer based on poly(2,6-dimethylpolyphenyleneoxide) with trimethylammonium groups on long side chains (PPO-LC) were studied as catalytic electrodes for the oxygen reduction reaction (ORR). The objective was to reveal the impact of graphitic vs pyridinic/pyrrolic nitrogen on the ORR electrocatalysis. The CQDs were prepared by hydrothermal synthesis and analyzed by X-ray photoelectron spectroscpy to ascertain the B and N content and their position. The electrodes were prepared by drop-casting an ink of CQDs and PPO-LC on acid-treated carbon paper support. Characterizations of the electrodes included water contact angle, capacitance measurements, Fourier transform infrared spectra as well as scanning electron microscopy and optical microscopy. The onset and half-wave potentials, limiting current densities, Koutecky-Levich and Tafel plots revealed that the sample with only pyridinic/pyrrolic nitrogen showed the lowest electrocatalytic performance, underlining the importance of graphitic nitrogen for good ORR activity. Four-electron reduction was observed for the samples containing graphitic nitrogen. The onset potential (0.92 V/RHE) was among the best in the literature for carbonaceous materials. Finally, durability tests were performed indicating a good long-time stability of the electrodes; the electrode degradation was analyzed by impedance spectroscopy.

A comparative analysis of square-wave voltammetry and multi-frequency electrochemical Faradaic spectroscopy for kinetic characterisation

A rigorous comparison between square-wave voltammetry (SWV) and the recently proposed multi-frequency electrochemical Faradaic spectroscopy (MEFS) is presented for both a quasireversible electrode reaction of a dissolved redox couple at a planar macroscopic electrode and a catalytic regenerative electrode mechanism (EC′ reaction scheme) by means of numerical simulations. MEFS offers fast kinetic characterisation with a minimal set of experiments, as the system is interrogated with a range of SW frequencies in a single experiment. By changing the mid-potential Em, a critical parameter of MEFS, a broad range of standard rate constants for the heterogeneous interfacial electron transfer is accessible, ranging between 0.006 and 0.12 cm s−1. In the case of the EC′ mechanism, features of the current components in both SWV and MEFS reflect the involvement of the follow-up regenerative chemical reaction (i.e. C′ catalytic step). However, for the kinetic characterisation of the EC′ mechanism, the comparative analysis suggests that SWV should be the main operating technique.

Electrodeposited NiFe‐LDH on the Surface of Ni‐BDC for Electrocatalytic Water Oxidation

AbstractSubstrate surface modification with a functional material can effectively enhance the electrocatalytic performance of an electrode on oxygen evolution reaction (OER). In this work, a functional Ni‐BDC MOF nanosheet layer was in‐situ grown on the surface of nickel foam (NF). Consequently, the NiFe layered double hydroxides (NiFe‐LDH) electrodeposited on the modified layer exhibited an excellent activity and an amazing long‐term stability on electrocatalytic OER. In alkaline electrolyte, the well‐designed NiFe‐LDH/Ni‐BDC/NF drives a current density of 100 mA cm−2 at a small overpotential of 223 mV, with a low Tafel slope of 33.1 mV dec−1 and an outstanding catalytic stability of more than 10 days under continuous electrocatalysis. Such distinguished performances are attributed to the particular hydrophily and electrical conductivity of the Ni‐BDC layer. This work is an important attempt to bring a simple and effective guideline on fabricating a highly efficient catalytic electrode for OER.