Electrocatalytic Oxygen Evolution Reaction Research Articles

Oxygen evolution reaction activity of carbon aerogel supported Pd–Ni–Al catalysts synthesized by microwave irradiation method

The oxygen evolution reaction (OER) is a critical step for oxygen production during the electrochemical splitting of water. Effective OER catalysts support the development of clean energy technologies by increasing the energy efficiency of these processes. In this study, carbon aerogel (CA) was first synthesized as a catalyst support material using sol-gel, supercritical drying, and pyrolysis process. Then, mono-metallic (Pd/CA, Al/CA), bi-metallic (Pd–Al/CA, Pd–Ni/CA), and tri-metallic (Pd–Ni–Al/CA) catalysts were synthesized by microwave irradiation method. Inductively coupled plasma-mass spectrometry (ICP-MS), X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), Raman spectroscopy have been made to examine the structural properties of the synthesized catalysts. Electrochemical analysis was carried out through cyclic voltammetry (CV), chronoamperometry, and electrochemical impedance spectroscopy (EIS) in alkaline media (1 M KOH: Methanol) to examine the effect of metal loading of CA support material towards OER performance. All the compositions showed excellent activity toward OER, among all Pd–Ni/CA catalysts showed the highest activity. The OER peak current increased remarkably up to 48 mA cm−2 with methanol addition, which signifies the substantial application of carbon aerogel supported-Pd-Ni-Al catalysts in direct methanol fuel cells (DMFCs). Pd–Ni/CA display high OER performance with maximum diffusion coefficient, Do (6.6 × 10−8 cm2 s−1) and heterogeneous rate constant, ko (4.706 × 10−4 cm s−1), and smaller value of Tafel slope (128 mV dec−1). Electrochemical studies predicted that all the prepared carbon aerogel supported-Pd-Ni-Al catalysts can be used as efficient catalysts for OER and other related electrocatalysis applications.

Toward Realistic Models of the Electrocatalytic Oxygen Evolution Reaction.

The electrocatalytic oxygen evolution reaction (OER) supplies the protons and electrons needed to transform renewable electricity into chemicals and fuels. However, the OER is kinetically sluggish; it operates at significant rates only when the applied potential far exceeds the reversible voltage. The origin of this overpotential is hidden in a complex mechanism involving multiple electron transfers and chemical bond making/breaking steps. Our desire to improve catalytic performance has then made mechanistic studies of the OER an area of major scientific inquiry, though the complexity of the reaction has made understanding difficult. While historically, mechanistic studies have relied solely on experiment and phenomenological models, over the past twenty years ab initio simulation has been playing an increasingly important role in developing our understanding of the electrocatalytic OER and its reaction mechanisms. In this Review we cover advances in our mechanistic understanding of the OER, organized by increasing complexity in the way through which the OER is modeled. We begin with phenomenological models built using experimental data before reviewing early efforts to incorporate ab initio methods into mechanistic studies. We go on to cover how the assumptions in these early ab initio simulations─no electric field, electrolyte, or explicit kinetics─have been relaxed. Through comparison with experimental literature, we explore the veracity of these different assumptions. We summarize by discussing the most critical open challenges in developing models to understand the mechanisms of the OER.

Ir-Doped Core-Shell Hollow Heterogeneous Nanospindles for Electrocatalytic Oxygen Evolution Reaction.

By utilizing Metal-organic framework (MOF) materials as a base, constructing electrocatalysts with heterogeneous structures offers advantages for catalyzing water splitting. In this study, a hollow heterogeneous nanocatalyst, Ir-MIL-88A@NiFe-LDHs, was prepared by growing a layered double hydroxides (LDHs) shell on MIL-88A substrate. The catalyst shows excellent oxygen evolution reaction (OER) performance in a 1.0 M KOH solution, requiring only 217 mV overpotential to achieve a current density of 10 mA cm-2 with a Tafel slope of 62.18 mV dec-1, indicating significant electrocatalytic performance and reaction kinetics characteristics. Furthermore, long-term OER testing also demonstrates the catalyst's outstanding stability. Emphasizing the interfacial interaction between MOF and LDHs, as well as the synergistic effect among Ni, Fe, and Ir elements, the study highlights how these factors collaboratively control the local electronic structure of the hollow Ir-MIL-88A@NiFe-LDHs, resulting in an efficient MOF-derived electrocatalyst.

An efficient and robust noble-metal-free self-standing bifunctional water electrolysis catalyst: Co3S4@Ex.NiFe-LDH for alkaline water electrolysis

Electrolysis of water integrated with the renewable energy as input source can contribute significantly in the production of green hydrogen, a clean and versatile energy carrier. In water electrolyzer, the hydrogen evolution reaction (HER) at the cathode must act synchronously with the oxygen evolution reaction (OER) at the anode to effectively accomplish total water-splitting. The performance of an electrolyzer is often limited by the low performance of anode and it is important to develop an electrocatalyst which can efficiently perform both HER and OER. Ni and Fe based layered-double-hydroxides (LDHs) have gained a lot of interest owing to their outstanding OER electrocatalytic activity, however they are known to have poor HER performance. To enhance the overall water splitting efficiency of the LDHs, we present a simple approach of preparing a heterojunction of LDH with cobalt sulphide. The bifunctional electroactivity of the designed electrocatalyst Co3S4@Ex.NiFe-LDH, worked efficiently in both HER and OER electrocatalysis. Chalcogenides known for HER, not only improves the HER performance of the composites but also found to reduce the charge transfer resistance. Obtained results showed that when it comes to the OER performance, the recommended catalyst shadows the state of art catalyst RuO2. Additionally, the catalyst has outstanding activity and stability, achieving a current density of around −120 mA/cm2 over a six-day period. The electrolyzer composed of both anode and cathode designated as Co3S4@Ex.NiFe-LDH||Co3S4@Ex.NiFe-LDH only needs a low voltage input of 1.49 V to achieve a total water splitting reaction at required current density of 10 mA/cm2, showing efficacy at the low voltage input. Experimental observations showed Co3S4@Ex.NiFe-LDH performs better than Pt/C–RuO2 in alkaline water electrolysis. The electrolyzer can continuously produce hydrogen at 50 mA/cm2 for more than a week period; indicating its potential for long-term application.

Fabrication of Fe-Zr, Co-Zr, and Ni-Zr Catalysts to Boost CNTs Synthesis from Plastic Wastes and the Electrocatalytic Oxygen Evolution Reaction.

The efficient conversion of plastic wastes to high-value carbon materials like carbon nanotubes (CNTs) is one important issue about the rational recycling, reduction, and reuse of solid wastes. Herein, Fe-, Co-, and Ni-Zr catalysts were prepared and used for CNTs synthesis from polyethylene (PE) waste via a two-stage reaction system. At the same time, the effects of the PE/catalyst ratio and reaction temperature on CNTs synthesis have been studied. Compared with Co-Zr and Ni-Zr, Fe-Zr exhibited the best activity in CNTs synthesis from PE, and it achieved the highest CNTs yield of 806.3 mg/g (per gram of Fe-Zr) at 800 °C with a PE/catalyst ratio of 4. Furthermore, the obtained Fe-Zr/CNTs composite exhibited a low overpotential of 267 mV for the electrocatalytic oxygen evolution reaction (OER) at 20 mA/cm2 in 1 M KOH electrolyte solution, which was 21 mV lower than commercial RuO2 (288 mV) and 50 mV lower than Fe-Zr (317 mV). It was deduced that the in situ growth of CNTs reduced the charge transfer resistance and improved the electron transport efficiency of the Fe-Zr/CNTs composite, leading to superior activity in the electrocatalytic OER. This work provided detailed information for the preparation of the metal/CNTs composite from plastic wastes, which contributed positively to alleviate the environment and energy crisis.

Three-dimensional pine-tree-like bimetallic sulfide with maximally exposed active sites by secondary structural restructuring for efficient electrocatalytic OER

Developing efficient, low-cost and bifunctional catalysts with predominant durability for the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) is an extraordinary challenge in the preparation of green hydrogen energy by electrochemical water splitting. Three-dimensional (3D) transition metal compounds have become a research hotspot as OER electrocatalysts, which can replace noble metal oxides such as RuO2 and IrO2 to reduce application costs. Herein, we synthesized a novel three-dimensional pine-tree-like bimetallic sulfide arrays on nickel foam (FeCoS/NF) using various optimization strategies such as morphology optimization, in situ growth and introduction of heterogeneous structures. The as-synthesized FeCoS/NF electrocatalyst only requires relatively low overpotential of 156 mV to achieve a current density of 20 mA cm−2 for OER, with a Tafel slope of only 37 mV dec−1. It also has a small charge transfer resistance, an electrochemical surface area and good electrochemical stability in alkaline electrolytes. The excellent performance of FeCoS/NF can be attributed to the synergistic effect and amorphous phase of FeCoS as well as the well-defined pine-tree-like array architecture with a large surface area, abundant active sites, and sufficient gas and electrolyte diffusion channels.

Lanthanum‐Nickel‐Based Mixed‐Oxide‐Coated Nickel Electrodes for the OER Electrocatalysis

ABSTRACTThe anodic oxygen evolution reaction (OER) remains a bottleneck for electrocatalytic water splitting due to its sluggish kinetics and, thus, high overpotentials. This limits water electrolysis as a key technology for the generation of hydrogen as a sustainable alternative to fossil fuels. For alkaline water splitting, perovskite phases (ABO3) with earth‐abundant first‐row transition‐metals have emerged as a promising material class for OER electrocatalysts. Among these, LaNiO3 has been found to exhibit high intrinsic OER activity. To increase catalyst utilization, a high surface area of the catalyst is desirable and can be achieved by impregnation of porous templates. In this work, La–Ni‐based oxides were prepared via impregnation of activated carbon and subsequent heating, combining precursor calcination and template removal into one step. The phase structure of the samples is analyzed via powder X‐ray diffractometry, and the morphology is determined by scanning electron microscopy. The synergistic effect of B‐site mixing iron as well as A‐site mixing strontium into LaNiO3 is studied and found to increase its OER activity, confirming the activity‐enhancing effect of Fe in Ni‐based OER electrocatalysts. To allow for facile technical application of the catalysts, the electrodes are prepared by coating a perovskite ink onto Ni‐metal as industrially relevant substrates, followed by calcination.

Lanthanum‐Nickel‐Based Mixed‐Oxide‐Coated Nickel Electrodes for the OER Electrocatalysis

ABSTRACTThe anodic oxygen evolution reaction (OER) remains a bottleneck for electrocatalytic water splitting due to its sluggish kinetics and, thus, high overpotentials. This limits water electrolysis as a key technology for the generation of hydrogen as a sustainable alternative to fossil fuels. For alkaline water splitting, perovskite phases (ABO3) with earth‐abundant first‐row transition‐metals have emerged as a promising material class for OER electrocatalysts. Among these, LaNiO3 has been found to exhibit high intrinsic OER activity. To increase catalyst utilization, a high surface area of the catalyst is desirable and can be achieved by impregnation of porous templates. In this work, La–Ni‐based oxides were prepared via impregnation of activated carbon and subsequent heating, combining precursor calcination and template removal into one step. The phase structure of the samples is analyzed via powder X‐ray diffractometry, and the morphology is determined by scanning electron microscopy. The synergistic effect of B‐site mixing iron as well as A‐site mixing strontium into LaNiO3 is studied and found to increase its OER activity, confirming the activity‐enhancing effect of Fe in Ni‐based OER electrocatalysts. To allow for facile technical application of the catalysts, the electrodes are prepared by coating a perovskite ink onto Ni‐metal as industrially relevant substrates, followed by calcination.

Atomic-Layer IrOx Enabling Ligand Effect Boosts Water Oxidation Electrocatalysis.

An in situ formed IrOx (x ≤ 2) layer driven by anodic bias serves as the essential active site of Ir-based materials for oxygen evolution reaction (OER) electrocatalysis. Once being confined to atomic thickness, such an IrOx layer possesses both a favorable ligand effect and maximized active Ir sites with a lower O-coordination number. However, limited by a poor understanding of surface reconstruction dynamics, obtaining atomic layers of IrOx remains experimentally challenging. Herein, we report an idea of material design using intermetallic IrVMn nanoparticles to induce in situ formation of an ultrathin IrOx layer (O-IrVMn/IrOx) to enable the ligand effect for achieving superior OER electrocatalysis. Theoretical calculations predict that a strong electronic interaction originating from an orderly atomic arrangement can effectively hamper the excessive leaching of transition metals, minimizing vacancies for oxygen coordination. Linear X-ray absorption near edge spectra analysis, extended X-ray absorption fine structure fitting outcomes, and X-ray photoelectron spectroscopy collectively confirm that Ir is present in lower oxidation states in O-IrVMn/IrOx due to the presence of unsaturated O-coordination. Consequently, the O-IrVMn/IrOx delivers excellent acidic OER performances with an overpotential of only 279 mV at 10 mA cm-2 and a high mass activity of 2.3 A mg-1 at 1.53 V (vs RHE), exceeding most Ir-based catalysts reported. Moreover, O-IrVMn/IrOx also showed excellent catalytic stability with only 0.05 at. % Ir dissolution under electrochemical oxidation, much lower than that of disordered D-IrVMn/IrOx (0.20 at. %). Density functional theory calculations unravel that the intensified ligand effect optimizes the adsorption energies of multiple intermediates involved in the OER and stabilizes the as-formed catalytic IrOx layer.

Mesoporous graphene-supported nanostructured nickel telluride for efficient electrocatalytic oxygen evolution reaction

The electrocatalytic oxygen evolution reaction (OER) imposes significant constraints on the operational overpotential of electrochemical energy devices, such as water electrolyzers, metal-air batteries, and fuel cells. However, the sluggish kinetics of OER reactions hinder these applications, which has prompted efforts to design more effective electrocatalysts. In this study, we have synthesized NiTe via in-situ growth into mesoporous graphene (MG), with varying nominal weight percentages (5- wt%, 10- wt%, and 15- wt%) of NiTe. The resulting NiTe/MG nanohybrids displayed hexagonally structured NiTe nanoparticles with a predominant (101) surface that promotes the OER kinetics. The wrinkled 3D mesoporous graphene scaffold facilitated the attachment and dispersion of NiTe particles of nanoscale on its surface, preventing their agglomeration. The porous characteristics of the MG significantly increased the high surface area of the NiTe/MG nanohybrids (583–671 m2 g−1), promoting enhanced accessibility of active sites and mass transport beneficial for the OER. Moreover, the altered electronic structure of the NiTe in the MG nanohybrid indicates enhancing O2 desorption during the OER. The optimized composition of the 10 wt% NiTe-loaded MG nanohybrid electrocatalyst demonstrates superior OER activity compared to other nanohybrids. It exhibits a small overpotential of 250 mV at 10 mA cm−2, a low Tafel slope of 63 mV dec−1 and maintained stability in 1 M KOH (pH = 14) as the electrolyte for a prolonged period. This enhanced OER activity is ascribed to the synergistic effect of MG’s high conductivity and the improved intrinsic activity of NiTe within the nanohybrid structure.

Surface reconstruction and entropy engineering of Ni(OH)2 nanosheets for enhanced electrocatalytic performances of oxygen evolution reaction in alkaline seawater

Hydrogen production via electrochemical splitting of seawater is highly desirable but still facing great challenges. Herein, we report the facile preparation of medium-entropy oxyhydroxides on Ni(OH)2 nanosheets via surface reconstruction and entropy engineering strategies, achieving enhanced electrocatalytic activity and stability for oxygen evolution reaction (OER) in alkaline seawater. The electrochemical oxidation is conducted on Ni(OH)2 nanosheets to create abundant reactive oxygen (reactive-O) atoms on the reconstructed surface, thus forming a reactive-O enriched surface on Ni(OH)2 (NiOx/Ni(OH)2). Additionally, cations are incorporated onto the reconstructed surface of NiOx/Ni(OH)2 via an electrodeposition method, forming the medium-entropy oxyhydroxides on Ni(OH)2 nanosheets ((FeCoCrNi)Ox/Ni(OH)2). Benefiting from the composition and structure advantages, the resulting (FeCoCrNi)Ox/Ni(OH)2@NF demonstrates obviously enhanced performances for OER electrocatalysis, with an overpotential of 239 mV at the current density of 10 mA cm−2 and a low Tafel slope of 24.66 mV dec−1 in 1.0 M KOH + 0.5 M NaCl solution. Furthermore, it exhibits exceptional durability for OER electrocatalysis in alkaline seawater, maintaining over 90.7 % of the OER current density after 100 h.

Biogenic Bovine Serum Albumin/Zn3(PO4)2/Cr2O3 hybrid electrocatalyst for improved oxygen evolution reaction

The fabrication of nanostructured protein-inorganic hybrid materials is crucial for the development of advanced multifunctional materials. Protein-inorganic mesoporous composites are gaining attention due to their remarkable properties, including large surface areas and active surface functional groups. We have successfully synthesized mesoporous BSA/Zn3(PO4)2/Cr2O3 catalysts to improve the kinetics of the oxygen evolution reaction (OER) in electrocatalytic water splitting for sustainable energy generation. This approach utilizes BSA in the synthesis process and is environmentally friendly. By adjusting the BSA quantity, we could control the yield of BSA/Zn3(PO4)2/Cr2O3 mesoporous. We employed various techniques, including FE-SEM, XRD, and FTIR, to analyze the morphology and structural characteristics of the biogenic BSA/Zn3(PO4)2/Cr2O3 electrocatalyst. Our comprehensive evaluation of the electrocatalytic OER activity of the BSA/Zn3(PO4)2/Cr2O3 hybrid structure demonstrated its remarkable performance. The biologically synthesized catalyst exhibited exceptional OER efficiency, maintaining a high current density of 10 mA cm−2 at very low overpotentials (only 216 mV) under alkaline conditions. The elongated peptide backbone of BSA significantly facilitated ion and electron transport, contributing to improved OER activity. The synergistic interaction between various amino acids from BSA and the metal ions within Zn3(PO4)2/Cr2O3 can be attributed to this enhancement, highlighting the potential of this hybrid structure in electrocatalytic OER applications.

Effects of Ir‐Incorporation and Nanostructuring in β‐MnO2 for an Enhanced Electrocatalytic Oxygen Evolution Reaction

Effects of Ir‐Incorporation and Nanostructuring in β‐MnO2 for an Enhanced Electrocatalytic Oxygen Evolution Reaction

Ultrathin high-entropy layered double hydroxide electrocatalysts for enhancing oxygen evolution reaction

At the heart of the oxygen evolution reaction (OER), the properties of electrocatalysts play a crucial role in determining reaction efficiency. This underscores the need to design and develop highly effective OER electrocatalysts. The unique layer structure and electronic properties make layer double hydroxide (LDH) a promising candidate for driving OER electrocatalysis. Furthermore, high-entropy materials (HEMs) exhibit core effects such as high entropy, lattice distortion, sluggish diffusion, and cocktail effect, which can enhance active sites and optimize binding energy with intermediates. Combining the advantages of these two material categories, we propose the synthesis of high-entropy layered double hydroxides (HE-LDHs) through a straightforward MOF-mediated synthesis method to showcase exceptional electrocatalytic OER performance. Detailed mechanistic studies have shown that its outstanding performance stems from its ultrathin structure and the inherent activity of a high-entropy material that promotes charge transfer, mass transport, and the evolution of reaction intermediates.

ZIF‐67 Derived Co‐LDH Nanocubes for Oxygen Evolution Reaction

AbstractTo address the substantial energy needs of the quickly evolving modern civilization, efforts are still needed to provide sustainable renewable energy sources. The electrocatalytic Oxygen evolution reaction (OER) is one of the essential technologies used in the various hydrogen production techniques. ZIF‐67 nanocubes (ZIF‐67 NCs) were synthesized in an aqueous solution and used as sacrificial templates. Cobalt nitrate hexahydrate was added under water bath conditions, resulting in the evolution of numerous small layered layers of cobalt hydroxide. This ultimately led to the formation of multilayered, three‐dimensionally crosslinked Co‐LDH with a porous networked cubic morphology. Hydrolysis of Co2+ at different concentrations produces different degrees of weak acidic environments, and the loose LDH on the cubic structure of the best catalyst, Co‐LDH‐1, exposes more active cobalt sites for the OER, which results in a high electrochemically active surface area, with an overpotential of 354 mV and a Tafel slope of 79.06 mV dec−1 at a current density of 10 mA cm−2, and good stability and low activation under alkaline condition also has good stability and low activation energy. It provides us an easy and practical plan for logically creating ZIF‐derived hydroxide materials, leading to the development of affordable and effective electrocatalysts.

Recent Developments in Nickel-Based Layered Double Hydroxides for Photo(-/)electrocatalytic Water Oxidation.

Layered double hydroxides (LDHs), especially those containing nickel (Ni), are increasingly recognized for their potential in photo(-/)electrocatalytic water oxidation due to the abundant availability of Ni, their corrosion resistance, and their minimal toxicity. This review provides a comprehensive examination of Ni-based LDHs in electrocatalytic (EC), photocatalytic (PC), and photoelectrocatalytic (PEC) water oxidation processes. The review delves into the operational principles, highlighting similarities and distinctions as well as the benefits and limitations associated with each method of water oxidation. It includes a detailed discussion on the synthesis of monolayer, ultrathin, and bulk Ni-based LDHs, focusing on the merits and drawbacks inherent to each synthesis approach. Regarding the EC oxygen evolution reaction (OER), strategies to improve catalytic performance and insights into the structural evolution of Ni-based LDHs during the electrocatalytic process are summarized. Furthermore, the review extensively covers the advancements in Ni-based LDHs for PEC OER, including an analysis of semiconductors paired with Ni-based LDHs to form photoanodes, with a focus on their enhanced activity, stability, and underlying mechanisms facilitated by LDHs. The review concludes by addressing the challenges and prospects in the development of innovative Ni-based LDH catalysts for practical applications. The comprehensive insights provided in this paper will not only stimulate further research but also engage the scientific community, thus driving the field of photo(-/)electrocatalytic water oxidation forward.

Ceria-Optimized Oxygen-Species Exchange in Hierarchical Bimetallic Hydroxide for Electrocatalytic Water Oxidation.

The utilization of rare earth elements to regulate the interaction between catalysts and oxygen-containing species holds promising prospects in the field of oxygen electrocatalysis. Through structural engineering and adsorption regulation, it is possible to achieve high-performance catalytic sites with a broken activity-stability tradeoff. Herein, we fabricate a hierarchical CeO2/NiCo hydroxide for electrocatalytic oxygen evolution reaction (OER). This material exhibits superior overpotentials and enhanced stability. Multiple potential-dependent experiments reveal that CeO2 promotes oxygen-species exchange, especially OH- ions, between catalyst and environment, thereby optimizing the redox transformation of hydroxide and the adsorption of oxygen-containing intermediates during OER. This is attributed to the reduction in the adsorption energy barrier of Ni to *OH facilitated by CeO2, particularly the near-interfacial Ni sites. The less-damaging adsorbate evolution mechanism and the CeO2 hierarchical shell significantly enhance the structural robustness, leading to exceptional stability. Additionally, the observed "self-healing" phenomenon provides further substantiation for the accelerated oxygen exchange. This work provides a neat strategy for the synthesis of ceria-based complex hollow electrocatalysts, as well as an in-depth insight into the co-catalytic role of CeO2 in terms of oxygen transfer. This article is protected by copyright. All rights reserved.

Controllable Phase Separation Engineering of Iron-Cobalt Alloy Heterojunction for Efficient Water Oxidation.

The tailor-made transition metal alloy-based heterojunctions hold a promising prospect for the electrocatalytic oxygen evolution reaction (OER). Herein, a series of iron-cobalt bimetallic alloy heterojunctions are purposely designed and constructed via a newly developed controllable phase separation engineering strategy. The results show that the phase separation process and alloy component distribution rely on the metal molar ratio (Fe/Co), indicative of the metal content dependent behavior. Theoretical calculations demonstrate that the electronic structure and charge distribution of iron-cobalt bimetallic alloy can be modulated and optimized, thus leading to the formation of an electron-rich interface layer, which likely tunes the d-band center and reduces the adsorption energy barrier toward electrocatalytic intermediates. As a result, the Fe0.25Co0.75/Co heterojunction exhibits superior OER activity with a low overpotential of 185 mV at 10 mA cm-2. Moreover, it can reach industrial-level current densities and excellent durability in high-temperature and high-concentration electrolyte (30 wt % KOH), exhibiting enormous potential for industrial applications.

Research progress on electronic and active site engineering of cobalt‐based electrocatalysts for oxygen evolution reaction

AbstractElectrocatalytic water splitting has been identified as a potential candidate for producing clean hydrogen energy with zero carbon emission. However, the sluggish kinetics of oxygen evolution reaction on the anode side of the water‐splitting device significantly hinders its practical applications. Generally, the efficiency of oxygen evolution processes depends greatly on the availability of cost‐effective catalysts with high activity and selectivity. In recent years, extensive theoretical and experimental studies have demonstrated that cobalt (Co)‐based nanomaterials, especially low‐dimensional Co‐based nanomaterials with a huge specific surface area and abundant unsaturated active sites, have emerged as versatile electrocatalysts for oxygen evolution reactions, and thus, great progress has been made in the rational design and synthesis of Co‐based nanomaterials for electrocatalytic oxygen evolution reactions. Considering the remarkable progress in this area, in this timely review, we highlight the most recent developments in Co‐based nanomaterials relating to their dimensional control, defect regulation (conductivity), electronic structure regulation, and so forth. Furthermore, a brief conclusion about recent progress achieved in oxygen evolution on Co‐based nanomaterials, as well as an outlook on future research challenges, is given.

Accurately Modulating Binuclear Metal Nodes of Metal-Organic Frameworks for Oxygen Evolution.

The accurate manipulation of the species and locations of catalytic centers is crucial for regulating the catalytic activity of catalysts, which is essential for their efficient design and development. Metal-organic frameworks (MOFs) with coordinated metal sites are ideal materials for investigating the origin of catalytic activity. In this study, we present a Ni2-MOF featuring novel Ni-based binuclear nodes with open metal sites (OMSs) and saturated metal sites (SMSs). The nickel was replaced by iron to obtain Ni1Fe1-MOF. In the electrocatalytic oxygen evolution reaction, Ni1Fe1-MOF exhibited an overpotential and Tafel slope of 370 mV@10 mA cm-2 and 87.06 mV dec-1, respectively, which were higher than those of Ni2-MOF (283 mV@10 mA cm-2 and 39.59 mV dec-1, respectively), demonstrating the superior performance of Ni1Fe1-MOF. Furthermore, theoretical calculations revealed that iron as an SMS may effectively regulate the electronic structure of the nickel catalytic center to reduce the free energy barrier ΔG*OH of the rate-determining step.