The cobalt-based metal organic frameworks array derived CoFeNi-layered double hydroxides anode and CoP/FeNi2P heterojunction cathode for ampere-level seawater overall splitting.

The seawater electrolysis technology powered by renewable energy is recognized as the promising "green hydrogen" production method to solve serious energy and environmental problems. The lack of low-cost and ampere-level current OER (oxygen evolution reaction) and HER (hydrogen evolution reaction) catalysis limits their industrial application. In this work, a unique tri-metal (Co/Fe/Ni) layered double hydroxide hollow array anode catalyst (CFN-LDH/NF) and the CoP/FeNi2P heterojunction hollow array cathode are successfully prepared via one in-situ growth of Co-MOF on nickel foam (Co-MOF/NF) precursor, which exhibits excellent catalytic performance. The η1000 values of 352 and 392 mV are achieved for CFN-LDH/NF (OER catalyst) in 1.0 M KOH and alkaline seawater solution, respectively. The CFNP/NF with a low overpotential of 281 mV is required to reach 1000 mA cm-2 current density for HER in 1.0 M KOH solution, while the η1000 in alkaline seawater solution is 312 mV. The CFN-LDH/NF||CFNP/NF electrolyzer exhibits excellent long-term durability over 100 h, achieving current density of 500 mA cm-2 at 1.825 V in 1.0 M KOH solution. The construction of hollow tri-metal LDH and phosphides heterostructures may open a new and relatively unexplored path for fabricating high performance seawater splitting catalysis.

Confined Growth of Highly Ordered Metal Atomic Arrays for Seawater Oxidation.

Metal atom catalysts have been among the most important research objects due to their specific physical and chemical properties. However, precise control of the anchoring of metal atoms is still challenging to achieve. Cobalt and iridium atomic arrays formed sequentially ordered stable arrays in graphdiyne (GDY) triangular cavities depending on their intrinsic chemical properties and interactions. The success of this method was attributed to multifunctional integration of GDY, enabling selective growth from one to several atoms and various atomic densities. The bimetallic atom arrays show several advantages resulting from reducibility of acetylene bonds, space limiting effect, incomplete charge transfer between GDY and metal atoms, and sp-C hybridized triple bond skeleton. This well-designed system exhibits unprecedented oxygen evolution reaction (OER) performance with a mass activity of 2.6 A mgcat. -1 at a low overpotential of 300 mV, which is 216.6 times higher than the state-of-the-art IrO2 catalyst, and long-term stability.

Coordination Engineering of Carbon Dots and Mn in Co-Based Phosphides for Highly Efficient Seawater Splitting at Ampere-Level Current Density.

Direct electrolysis of seawater to generate hydrogen is an attractive approach for storing renewable energy. However, direct seawater splitting suffers from low current density and limited operating stability, which severely hinders its industrialization. Herein, a promising strategy is reported to obtain a nano needle-like array catalyst-CDs-Mn-CoxP on nickel foam, in which the Mn─O─C bond tightly binds Mn, Carbon dots (CDs), and CoxP together. The coordination engineering of CDs and Mn not only effectively regulates the electronic structure of CoxP, but also endows the as-prepared catalyst with selectivity and marked long-term stability at ampere-level current density. Low overpotentials of 208 and 447 mV are required to achieve 1000 mA cm-2 for hydrogen evolution reaction (HER) and Oxygen evolution reaction (OER) in simulated seawater, respectively. Cell potentials of 1.78 and 1.86 V are needed to reach 500 and 1000 mA cm-2 in alkaline seawater along with excellent durability for 350 h. DFT studies have verified that the introduction of Mn and CDs effectively shifts the d-band center of Co-3d toward higher energy, thereby strengthening the adsorption of intermediates and enhancing the catalytic activity. This study sheds light on the development of highly effective and stable catalysts for large-scale seawater electrolysis.

Crystalline metal phosphide-coated amorphous iron oxide-hydroxide (FeOOH) with oxygen vacancies as highly active and stable oxygen evolution catalyst in alkaline seawater at high current density.

In this study, we employed a straightforward phosphorylation approach to achieve a dual objective: constructing c-a heterostructures consisting of crystalline Ni12P5 and amorphous FeOOH, while simultaneously enhancing oxygen vacancies. The resulting oxygen evolution reaction (OER) catalyst, Ni12P5/FeOOH/NF, exhibited remarkable performance with current densities of 500 mA cm-2 in both 1 M KOH and 1 M KOH + seawater, requiring low overpotentials of only 288 and 365 mV, respectively. Furthermore, Ni12P5/FeOOH/NF exhibited only a slight increase in overpotential, with increments of 18 mV and 70 mV in 1 M KOH after 15 and 150 h, and 32 mV and 108 mV in 1 M KOH + seawater at 500 mA cm-2 after 15 and 150 h, respectively. This minimal change can be attributed to the stabilized c-a structure, the protective coating of Ni12P5, and superhydrophilic. Through in-situ Raman and ex-situ XPS analysis, we discovered that Ni12P5/FeOOH/NF can undergo a reconfiguration into an oxygen vacancy-rich (Fe/Ni)OOH phase during OER process. The elevated OER activity is mainly due to the contribution of the oxygen vacancy-rich (Fe/Ni)OOH phase from the reconfigure of the Ni12P5/FeOOH/NF. This finding emphasizes the critical role of oxygen vacancies in facilitating the production of OO species and overcoming the limitations associated with OOH formation, ultimately enhancing the kinetics of the OER.

A Dual-Cation Exchange Membrane Electrolyzer for Continuous H2 Production from Seawater.

Direct seawater splitting (DSS) offers an aspirational route toward green hydrogen (H2) production but remains challenging when operating in a practically continuous manner, mainly due to the difficulty in establishing the water supply-consumption balance under the interference from impurity ions. A DSS system is reported for continuous ampere-level H2 production by coupling a dual-cation exchange membrane (CEM) three-compartment architecture with a circulatory electrolyte design. Monovalent-selective CEMs decouple the transmembrane water migration from interferences of Mg2+, Ca2+, and Cl- ions while maintaining ionic neutrality during electrolysis; the self-loop concentrated alkaline electrolyte ensures the constant gradient of water chemical potential, allowing a specific water supply-consumption balance relationship in a seawater-electrolyte-H2 sequence to be built among an expanded current range. Even paired with commercialized Ni foams, this electrolyzer (model size: 2 × 2 cm2) continuously produces H2 from flowing seawater with a rate of 7.5 mL min-1 at an industrially relevant current of 1.0 A over 100 h. More importantly, the energy consumption can be further reduced by coupling more efficient NiMo/NiFe foams (≈6.2 kWh Nm-3 H2 at 1.0 A), demonstrating the potential to further optimize the continuous DSS electrolyzer for practical applications.

Optimized Transition Metal Phosphides for Direct Seawater Electrolysis: Current Trends.

Seawater electrolysis presents a viable route for sustainable large-scale hydrogen production, yet its practical application is hindered by several technical challenges. These include the sluggish kinetics of hydrogen evolution, poor stability, cation deposition at the cathode, electrode corrosion, and competing chloride oxidation at the anode. To overcome these obstacles, the development of innovative electrocatalysts is crucial. Transition metal phosphides (TMPs) have emerged as promising candidates owing to their superior catalytic performance and tunable structural properties. This review provides a comprehensive analysis of recent progress in the structural engineering of TMPs tailored for efficient seawater electrolysis. We delve into the catalytic mechanisms underpinning hydrogen and oxygen evolution reactions in different pH conditions, along with the detrimental side reactions that impede hydrogen production efficiency. Several methods to prepare TMPs are then introduced. Additionally, detailed discussions on structural modifications and interface engineering tactics are presented, showcasing strategies to enhance the activity and durability of TMP electrocatalysts. By analyzing current research findings, our review aims to inform ongoing research endeavors and foster advancements in seawater electrolysis for practical and ecologically sound hydrogen generation.

In-situ construction of cation vacancies in amphoteric-metallic element-doped NiFe-LDH as ultrastable and efficient alkaline hydrogen evolution electrocatalysts at 1000 mA cm-2.

Developing efficient and stable electrocatalysts at affordable costs is very important for large-scale production of green hydrogen. In this study, unique amphoteric metallic element-doped NiFe-LDH nanosheet arrays (NiFeCd-LDH, NiFeZn-LDH and NiFeAl-LDH) using as high-performance bifunctional electrocatalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) were reported, by tuning electronic structure and vacancy engineering. It was found that NiFeCd-LDH possesses the lowest overpotentials of 85 mV and 240 mV (at 10 mA cm-2) for HER and OER, respectively. Density functional theory (DFT) calculations reveal the synergistic effect of Cd vacancies and Cd doping on improving alkaline HER performance, which promote the achievement of excellent catalytic activity and ultrastable hydrogen production at a large current density of 1000 mA cm-2 within 250 h. Besides, the overall water splitting performance of the as-prepared NiFeCd-LDH requires only 1.580 V to achieve a current density of 10 mA cm-2 in alkaline seawater media, underscoring the importance of modifying the electronic properties of LDH for efficient overall water splitting in both alkaline water/seawater environments.

Dopant-Induced Charge Redistribution on the 3D Sponge-like Hierarchical Structure of Quaternary Metal Phosphides Nanosheet Arrays Derived from Metal-Organic Frameworks for Natural Seawater Splitting.

Dopant-induced electron redistribution on transition metal-based materials has long been considered an emerging new electrocatalyst that is expected to replace noble-metal-based electrocatalysts in natural seawater electrolysis; however, their practical applications remain extremely daunting due to their sluggish kinetics in natural seawater. In this work, we developed a facile strategy to synthesize the 3D sponge-like hierarchical structure of Ru-doped NiCoFeP nanosheet arrays derived from metal-organic frameworks with remarkable hydrogen evolution reaction (HER) performance in natural seawater. Based on experimental results and density functional theory calculations, Ru-doping-induced charge redistribution on the surface of metal active sites has been found, which can significantly enhance the HER activity. As a result, the 3D sponge-like hierarchical structure of Ru-NiCoFeP nanosheet arrays achieves low overpotentials of 52, 149, and 216 mV at 10, 100, and 500 mA cm-2 in freshwater alkaline, respectively. Notably, the electrocatalytic activity of the Ru-NiCoFeP electrocatalyst in simulated alkaline seawater and natural alkaline seawater is nearly the same as that in freshwater alkaline. This electrocatalyst exhibits superior catalytic properties with outstanding stability under a high current density of 85 mA cm-2 for more than 100 h in natural seawater, which outperforms state-of-the-art 20% Pt/C at high current density. Our work provides valuable guidelines for developing a low-cost and high-efficiency electrocatalyst for natural seawater splitting.

Manipulating Electron Redistribution in Ni2 P for Enhanced Alkaline Seawater Electrolysis.

Developing bifunctional electrocatalyst for seawater splitting remains a persistent challenge. Herein, an approach is proposed through density functional theory (DFT) preanalysis to manipulate electron redistribution in Ni2 P addressed by cation doping and vacancy engineering. The needle-like Fe-doped Ni2 P with P vacancy (Fe-Ni2 Pv) is successfully synthesized on nickel foam, exhibiting a superior bifunctional hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) catalytic activity for seawater electrolysis in alkaline condition. As a result, bifunctional Fe-Ni2 Pv achieves the industrially required current densities of 1.0 and 3.0 A cm-2 at low voltages of 1.68 and 1.73 V, respectively, for seawater splitting at 60 °C in 6.0 m KOH circumstances. The theoretical calculation and the experimental results collectively reveal the reasons for the enhancement of catalyst activity. Specifically, Fe doping and P vacancies can accelerate the reconstruction of OER active species and optimize the hydrogen adsorption free energy (ΔGH* ) for HER. In addition, the active sites of Fe-Ni2 Pv are identified, where P vacancies greatly improve the electrical conductivity and Ni sites are the dominant OER active centers, meanwhile Fe atoms as active centers for the HER. The study provides a deep insight into the exploration for the enhancement of activity of nickel-based phosphide catalysts and the identification of their real active centers.

Corrosion resistance and earth-abundance FeS-based heterojunction catalyst for seawater splitting at industrial grade density.

The strategic progression toward highly efficient transition metal electrocatalytic electrodes is crucial to achieving efficiency and long-term stability in hydrogen production from authentic seawater sources. This work reports the development of a self-supporting, heterogeneous and corrosion-resistant iron sulfur-based catalytic electrode via a streamlined, one-step process involving sulfide etching and electroless plating on an iron foam substrate (IF). This new electrode, named NiS-FeS@IF, involves a nanostructured NiS-FeS catalytic material that combines in situ, resulting in a thin, ultrathin nanospherical layer on the IF. This construction has low overpotentials of merely 322 mV for the hydrogen evolution reaction (HER) and 563 mV for the oxygen evolution reaction (OER) with a current density of 500 mA cm-2 in alkaline simulated seawater electrolytes. Importantly, the NiS-FeS@IF electrode enduring more than 500 h at an industrial grade high current density of 1 A cm-2 without noteworthy performance deterioration. The unique and uniformly dispersed morphology of NiS-FeS facilitates intensified interfacial electron transfer, optimizes active site exposure and provides efficient channels for the rapid release and mass transfer of gas bubbles. This work introduces a novel approach for the facile preparation of efficient electrode materials.

Amorphous Co-Mo-P film on nickel foam: a superior bifunctional electrocatalyst for alkaline seawater splitting.

Seawater splitting is a compelling avenue to produce abundant hydrogen, which requires high-performance and cost-effective catalysts. Constructing bimetallic transition metal phosphides is a feasible strategy to meet the challenge. Here, an amorphous Co-Mo-P film supported on nickel foam (Co-Mo-P/NF) electrode is developed with bifunctional properties for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in alkaline seawater. Corresponding results indicate that the introduction of Mo can improve the active sites and regulate the intrinsic activity. Such a Co-Mo-P/NF behaves with prominent electrocatalytic activity towards both HER and OER, demanding low overpotentials of 193 and 352 mV at 100 mA cm‒2in alkaline seawater, respectively. Furthermore, the assembled electrolyzer demands a pronounced overall seawater splitting activity with a low cell voltage of 1.76 V to deliver 100 mA cm-2presenting excellent durability without obvious attenuation after 24 h continuous stability test. This work expands the horizon to develop transition metal-phosphorus electrocatalysts with robust and efficient activity for overall seawater splitting.

Ruthenium Oxide Nanoparticles Immobilized on Ti3C2 MXene Nanosheets for Boosting Seawater Electrolysis.

Seawater electrolysis represents a viable alternative for large-scale synthesis of hydrogen (H2), which is recognized as the most promising clean energy source, without relying on scarce fresh water. However, high energy cost and harmful chlorine chemistry in seawater limited its development. Herein, an effective catalyst based on a ruthenium nanoparticle-Ti3C2 MXene composite loaded on nickel foam (RuO2-Ti3C2/NF) with an open, fine, and homogeneous nanostructure was devised and synthesized by electrodeposition for high performance and stable overall seawater splitting. To drive a current density of 100 mA cm-2, the RuO2-Ti3C2/NF electrode required a small overpotential of 85 and 351 mV for HER and OER in 1 M KOH with only a slight increase in 1 M KOH seawater (156 and 378 mV for, respectively, HER and OER). An assembled RuO2-Ti3C2/NF-based two-electrode cell required an overpotential of only 1.84 V to acquire 100 mA cm-2 in 1 M KOH seawater and maintained its activity for over 25 h. This low cell voltage effectively prevented chlorine electrochemical evolution without anode protection. These promising results open up new avenues for the effective conversion of abundant seawater resources to hydrogen fuel.

Mn Doping and P Vacancy Induced Fast Phase Reconstruction of FeP for Enhanced Electrocatalytic Oxygen Evolution Reaction in Alkaline Seawater.

Due to the shortage of pure water resources, seawater electrolysis is a promising strategy to produce green hydrogen energy. To avoid chlorine oxidation reactions (ClOR) and the production of more corrosive hypochlorite, enhancing OER electrocatalyst activity is the key to solving the above problem. Considering that transition metal phosphides (TMPs) are promising OER eletrocatalysts for seawater splitting, a method to regulate the electronic structure of FeP by introducing Mn heteroatoms and phosphorus vacancy on it (Mn-FePV ) is developed. As an OER electrocatalyst in seawater solution, the synthesized Mn-FePV achieves extremely low overpotentials (η500  = 376, η1000  = 395 mV). In addition, the Pt/C||Mn-FePV couple only requires the voltage of 1.81 V to drive the current density of 1000 mA cm-2 for overall seawater splitting. The density functional theory (DFT) calculation shows that Mn-FePV (0.21 e- ) has more charge transfer number compared with FeP (0.17 e- ). In-situ Raman analysis shows that phosphorus vacancy and Mn doping can synergistically regulate the electronic structure of FeP to induce rapid phase reconstruction, further improving the OER performance of Mn-FePV . The new phase species of FeOOH is confirmed to can enhance the adsorption kinetics of OER intermediates.

Engineering P-Fe2O3-CoP nanosheets for overall freshwater and seawater splitting.

Tailoring surface composition and coordinative environment of catalysts in a nano-meter region often influence their chemical performance. It is reported that CoP exhibits a low dissociation ability of H-OH, originating from the poor desorption of intermediate species. Herein, we provide a feasible method to construct P-Fe2O3-CoP nanosheets through a gas-phase phosphorization process. P doping induces the formation of interfacial structure between Fe2O3 and CoP and the generation of defective structures. The resulting P-Fe2O3-CoP nanosheets afford high freshwater/seawater oxidation activity (250/270 mV@10 mA/cm2) in 1 mol/L (M) KOH, which is even lower than commercial RuO2. Compared with CoP||CoP, P-Fe2O3||P-Fe2O3, and Co3O4||Co3O4, the assembled P-Fe2O3-CoP||P-Fe2O3-CoP exhibits the superior water/seawater electrolysis performance with 1.61/1.65 V@10 mA/cm2. The synergistic effect of P doping, defective structure, and heterojunction leads to high water oxidation efficiency and water splitting efficiency.

In situ fabrication of sporoid-like flexible electrodes via Fe-regulated electron density for highly efficient and ultra-stable overall seawater splitting.

Construction of ultra-stable, flexible, efficient and economical catalytic electrodes is of great significance for the seawater electrolysis for hydrogen production. This work is grounded in a one-step mild electroless plating method to construct industrial-grade super-stable overall water splitting (OWS) catalytic electrodes (Fe1-Ni1P@GF) by growing loose and porous spore-like Fe1-Ni1P conductive catalysts in situ on flexible glass fibre (GF) insulating substrates with precise elemental regulation. Cost-effective Fe regulation boosts the electronic conductivity and charge transfer ability to achieve the construction of high intrinsic activity and strong electron density electrodes. Fe1-Ni1P@GF exhibits remarkable catalytic performance in hydrogen and oxygen evolution reaction (HER and OER), providing current densities of 10 mA cm-2 for HER and 100 mA cm-2 for OER at overpotentials of 51 and 216 mV, respectively. Moreover, it achieves 10 mA cm-2 at 1.42 V for OWS, and exhibits stable operation for over 1440 h at 1000 mA cm-2 in quasi-industrial environment of 6.0 M KOH + 0.5 M NaCl, without any performance degradation. This strategy enables the preparation of universally applicable P-based electrodes (ternary, quaternary, etc.) and large-area flexible electrodes (paper or cotton), significantly expands the practicality of the electrodes and demonstrating promising potential for industrial applications.

Dynamically Restructuring Nix Cry O Electrocatalyst for Stable Oxygen Evolution Reaction in Real Seawater.

In the pursuit of long-term stability for oxygen evolution reaction (OER) in seawater, retaining the intrinsic catalytic activity is essential but has remained challenging. Herein, we developed a Nix Cry O electrocatalyst that manifested exceptional OER stability in alkaline condition while improving the activity over time by dynamic self-restructuring. In 1 M KOH, Nix Cry O required overpotentials of only 270 and 320 mV to achieve current densities of 100 and 500 mA cm-2 , respectively, with excellent long-term stability exceeding 475 h at 100 mA cm-2 and 280 h at 500 mA cm-2 . The combination of electrochemical measurements and in situ studies revealed that leaching and redistribution of Cr during the prolonged electrolysis resulted in increased electrochemically active surface area. This eventually enhanced the catalyst porosity and improved OER activity. Nix Cry O was further applied in real seawater from the Red Sea (without purification, 1 M KOH added), envisaging that the dynamically evolving porosity can offset the adverse active site-blocking effect posed by the seawater impurities. Remarkably, Nix Cry O exhibited stable operation for 2000, 275 and 100 h in seawater at 10, 100 and 500 mA cm-2 , respectively. The proposed catalyst and the mechanistic insights represented a step towards realization of non-noble metal-based direct seawater splitting.

Hydrothermal preparation of C3N4 on carbonized wood for photothermal-photocatalytic water splitting to efficiently evolve hydrogen.

Hydrogen generation by photocatalysis is one of the most effective approaches to rationally utilize solar energy. In this work, we designed a biphasic photothermal-photocatalytic system. Spherical g-C3N4 (HCN) was grown on the carbonized wood (CW) by a one-step hydrothermal method. The carbonization layer in carbonized wood/spherical g-C3N4 (CW-HCN) system was able to further enhance the photothermal conversion of water steam production by improving the absorption of solar radiation. In addition, the temperature was increased due to photothermal effect, which was beneficial for H2 evolution reaction. Moreover, the carbonized layer could act as a reservoir for photogenerated electrons on g-C3N4, which could accelerate the charge separation. Benefiting from all above-mentioned merits, the H2 evolution rate of CW-HCN system under simulated sunlight reached 2700.18 µmol/m2/h, which was 42.23 times higher than that of pristine g-C3N4 powder directly dispersed in water. In addition, the CW-HCN system exhibited broad applicability, maintaining the H2 evolution activity of 2013.29 µmol/m2/h with seawater as water resource. This work provided a new strategy for highly efficient H2 evolution.

Sulfide Oxidation on Ladder-Type Heteroarenes to Construct All-Acceptor Copolymers for Visible-Light-Driven Hydrogen Evolution.

Conjugated polymers (CPs) have recently gained increasing attention as photocatalysts for sunlight-driven hydrogen evolution. However, they suffer from insufficient electron output sites and poor solubility in organic solvents, severely limiting their photocatalytic performance and applicability. Herein, solution-processable all-acceptor (A1 -A2 )-type CPs based on sulfide-oxidized ladder-type heteroarene are synthesized. A1 -A2 -type CPs showed upsurging efficiency improvements by two to three orders of magnitude, compared to their donor-acceptor -type CP counterparts. Furthermore, by seawater splitting, PBDTTTSOS exhibited an apparent quantum yield of 18.9% to 14.8% at 500 to 550 nm. More importantly, PBDTTTSOS achieved an excellent hydrogen evolution rate of 35.7 mmol h-1  g-1 and 150.7 mmol h-1  m-2 in the thin-film state, which is among the highest efficiencies in thin film polymer photocatalysts to date. This work provides a novel strategy for designing polymer photocatalysts with high efficiency and broad applicability.

Hierarchically Porous Few-Layer Carbon Nitride and Its High H+ Selectivity for Efficient Photocatalytic Seawater Splitting.

Photocatalysts for seawater splitting are severely restricted because of the presence of multiple types of ions in seawater that cause corrosion and deactivation. As a result, new materials that promote adsorption of H+ and hinder competing adsorption of metal cations should enhance utilization of photogenerated electrons on the catalyst surface for efficient H2 production. One strategy to design advanced photocatalysts involves introduction of hierarchical porous structures that enable fast mass transfer and creation of defect sites that promote selective hydrogen ion adsorption. Herein, we used a facile calcination method to fabricate the macro-mesoporous C3N4 derivative, VN-HCN, that contains multiple nitrogen vacancies. We demonstrated that VN-HCN has enhanced corrosion resistance and elevated photocatalytic H2 production performance in seawater. Experimental results and theoretical calculations reveal that enhanced mass and carrier transfer and selective adsorption of hydrogen ions are key features of VN-HCN that lead to its high seawater splitting activity.

Fabrication of ultra-stable and high-efficient CoP-based electrode toward seawater splitting at industrial-grade current density.

The mild and rapid construction of economical, efficient and ultrastable electrodes for hydrogen production via water splitting at industrial-grade current density remains extremely challenging. Herein, a one-step mild electroless plating method is proposed to deposit cobalt phosphorus (CoP)-based species on robust nickel net (NN, denoted as Co-P@NN). The tight interfacial contact, corrosion-proof self-supporting substrate and synergistic effect of Co-P@Co-O contribute greatly to the rapid electron transport, high intrinsic activity and long-term durability in the alkaline simulated seawater (1.0 M KOH + 0.5 M NaCl). Attractively, Co-P@Co-O also achieves ultrastable catalysis for over 2880 h with negligible activity attenuation under various alkaline extreme conditions (simulated seawater, high-salt environment, domestic sewage and so on). Furthermore, this work successfully constructs a series of ternary elemental doped (Ni, S, B, Fe and so on) CoP-based catalytic electrodes for highly efficient overall seawater splitting (OSWS). This work demonstrates not only an ideal platform for the versatile strategy of mildly obtaining CoP-based electrocatalysts but also the pioneering philosophy of large-scale hydrogen production.