Superhydrophilic 3D peony flower-like Mo-doped Ni2S3@NiFe LDH heterostructure electrocatalyst for accelerating water splitting

Constructing highly efficient nonprecious electrocatalysts for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is essential to improve the efficiency of overall water splitting, but still remains lots of obstacles. Herein, a novel 3D peony flower-like electrocatalyst was synthesized by employing Mo–Ni₂S₃/NF nanorod arrays as scaffolds to in situ growth ultrathin NiFe LDH nanosheets (Mo-Ni₂S₃@NiFe LDH). As expected, the novel peony flower-like Mo–Ni₂S₃@NiFe LDH displays superior electrocatalytic activity and stability for both OER and HER in alkaline media. Low overpotentials of only 228 mV and 109 mV are required to achieve the current densities of 50 mA cm^?2 and 10 mA cm^?2 for OER and HER, respectively. Additionally, the material remarkably accelerates water splitting with a low voltage of 1.54 V at 10 mA cm^?2, which outperforms most transition metal electrodes. The outstanding electrocatalytic activity benefits from the following these features: 3D peony flower-like structure with rough surface provides more accessible active sites; superhydrophilic surfaces lead to the tight affinity between electrode with electrolyte; metallic Ni substrate and highly conductive Mo–Ni₂S₃ nanorods scaffold together with offer fast electron transfer; the nanorod arrays and porous Ni foam accelerate gas bubble release and ions transmission; the strong interfacial effect between Mo-doped Ni₃S₂ and NiFe LDH shortens transport pathway, which are benefit for electrocatalytic performance enhancement. This work paves a new avenue for construction and fabrication the 3D porous structure to boost the intrinsic catalytic activities for energy conversion and storage applications.     

A highly active composite electrocatalyst Ni–Fe–P–Nb2O5/NF for overall water splitting

This work demonstrates a facile Nb₂O₅-decorated electrocatalyst to prepare cost-effective Ni–Fe–P–Nb₂O₅/NF and compared HER & OER performance in alkaline media. The prepared electrocatalyst presented an outstanding electrocatalytic performance towards hydrogen evolution reaction, which required a quite low overpotential of 39.05 mV at the current density of ?10 mA cm^?2 in 1 M KOH electrolyte. Moreover, the Ni–Fe–P–Nb₂O₅/NF catalyst also has excellent oxygen evolution efficiency, which needs only 322 mV to reach the current density of 50 mA cm^?2. Furthermore, its electrocatalytic performance towards overall water splitting worked as both cathode and anode achieved a quite low potential of 1.56 V (10 mA cm^?2).     

High throughput preparation of Ni–Mo alloy thin films as efficient bifunctional electrocatalysts for water splitting

The synthesis of cost-effective and high-performance electrocatalysts for water splitting is the main challenge in electrochemical hydrogen production. In this study, we adopted a high throughput method to prepare bi-metallic catalysts for oxygen/hydrogen evolution reactions (OER/HER). A series of Ni–Mo alloy electrocatalysts with tunable compositions were prepared by a simple co-sputtering method. Due to the synergistic effect between Ni and Mo, the intrinsic electrocatalytic activity of the Ni–Mo alloy electrocatalysts is improved, resulting in excellent HER and OER performances. The Ni₉₀Mo₁₀ electrocatalyst shows the best HER performance, with an extremely low overpotential of 58 mV at 10 mA cm^?2, while the Ni₄₀Mo₆₀ electrocatalyst shows an overpotential of 258 mV at 10 mA cm^?2 in OER. More significantly, the assembled Ni₄₀Mo₆₀//Ni₉₀Mo₁₀ electrolyzer only needs a cell voltage of 1.57 V to reach 10 mA cm^?2 for overall water splitting.     

Efficient MOF- derived V–Ni3S2 nanosheet arrays for electrocatalytic overall water splitting in alkali

The synergistic achievement of low-cost earth-abundant electrocatalysts and high efficiency to meet renewable energy need is highly desirable yet challenging. Here, we developed a simple Ni foam self -templating route for V-doped Ni₃S₂ nanosheet arrays through in situ formation of metal-organic frameworks (MOFs) combined with subsequent conversion. The as-prepared MOF-V-Ni₃S₂/NF catalyst delivers outstanding electrocatalytic performance in the alkaline solution, which requires low overpotentials of 118.1 mV @10 mA cm^?2 and 268 mV @10 mA cm^?2 for hydrogen evolution reaction and oxygen evolution reaction, respectively. The V-doping and MOF-derived 3D hieratical nanostructure play a vital role in the catalytic process, which provides efficient active sites and large surface areas. Furthermore, an alkaline electrolyzer was assembled with two pieces of MOF-V-Ni₃S₂/NF, which achieves efficient water splitting at 1.58 V @10 mA cm^?2. This strategy opens up new channels to synthesize MOF-based bifunctional electrocatalysts toward overall water spitting.     

Ni3S2-MoSx nanorods grown on Ni foam as high-efficient electrocatalysts for overall water splitting

In order to solve the problem of large overpotential in water electrolysis for hydrogen production, transition metal sulfides are promising bifunctional electrocatalysts for hydrogen evolution reaction/oxygen evolution reaction that can significantly reduce overpotential. In this work, Ni₃S₂ and amorphous MoS_x nanorods directly grown on Ni foam (Ni₃S₂-MoS_x/NF) were prepared via one-step solvothermal process, which were used as a high-efficient electrocatalyst for overall water splitting. The Ni₃S₂-MoS_x/NF composite exhibits very low overpotentials of 65 and 312 mV to reach 10 mA cm⁻² and 50 mA cm⁻² in 1.0 M KOH for HER and OER, respectively. Besides, it exhibits a low Tafel slope (81 mV dec⁻¹ for HER, 103 mV dec⁻¹ for OER), high exchange current density (1.51 mA cm⁻² for HER, 0.26 mA cm⁻² for OER), and remarkable long-term cycle stability. This work provides new perspective for further the development of highly effective non-noble-metal materials in the energy field.     

Ni3S2@Co(OH)2 heterostructures grown on Ni foam as an efficient electrocatalyst for water oxidation

It is of high significance to design robust, low-cost and stable electrocatalysts for the oxygen evolution reaction (OER) under alkaline medium. In this communication, we present the exploitation of Ni₃S₂@Co(OH)₂ which directly grown on nickel foam (Ni₃S₂@Co(OH)₂/NF) as a robust and stable electrocatalyst for OER. Such Ni₃S₂@Co(OH)₂/NF-5h demanding overpotential of only 290 mV is less than that of Ni₃S₂@Co(OH)₂/NF-10h (310 mV), Ni₃S₂@Co(OH)₂/NF-2h (320 mV) and Ni₃S₂/NF(350 mV), respectively, to drive a geometrical catalytic current density of 35 mA cm⁻², which is also better than that of noble metal catalyst IrO₂/NF (320 mV). In addition, the Ni₃S₂@Co(OH)₂/NF-5h presents a superior long-term electrocatalytic stability, keeping its activity at 26 mA cm⁻² for 40 h.     

Electrodeposition of NiS/Ni2P nanoparticles embedded in amorphous Ni(OH)2 nanosheets as an efficient and durable dual-functional electrocatalyst for overall water splitting

To develop earth-abundant and cost-effective catalysts for overall water splitting is still a major challenge. Herein, a unique “raisins-on-bread” Ni–S–P electrocatalyst with NiS and Ni₂P nanoparticles embedded in amorphous Ni(OH)₂ nanosheets is fabricated on Ni foam by a facile and controllable electrodeposition approach. It only requires an overpotential of 120 mV for HER and 219 mV for OER to reach the current density of 10 mA cm⁻² in 1 M KOH solution. Employed as the anode and cathode, it demonstrates extraordinary electrocatalytic overall water splitting activity (cell voltage of only 1.58 V @ 10 mA cm⁻²) and ultra-stability (160 h @ 10 mA cm⁻² or 120 h @50 mA cm⁻²) in alkaline media. The synergetic electronic interactions, enhanced mass and charge transfers at the heterointerfaces facilitate HER and OER processes. Combined with a silicon PV cell, this Ni–S–P bifunctional catalyst also exhibits highly efficient solar-driven water splitting with a solar-to-hydrogen conversion efficiency of 12.5%.     

Accelerate the alkaline hydrogen evolution reaction of the heterostructural Ni2P@Ni(OH)2/NF by dispersing a trifle of Ru on the surface

Electrocatalytic water splitting for hydrogen production plays a vital role in the development of new energy field, but there is still a lack of low-content precious metal or cost-effective non-noble metal catalysts for the hydrogen evolution reaction (HER). Therefore, how to develop the catalysts with a smaller amount of precious metal to achieve higher performance is still a major challenge. Herein, we have fabricated Ru–Ni₂P@Ni(OH)₂/NF-2 heterostructure by phosphating Ni(OH)₂/NF and then anchoring Ru on the surface through wet chemical strategy. Benefiting from its optimal ΔG_H1 and synergistic effect, this Ru–Ni₂P@Ni(OH)₂/NF-2 catalyst shows superior electrocatalytic HER kinetics in alkaline electrolyte. A small overpotential of 31 mV is needed for this electrocatalyst to obtain the current densities of 10 mA cm^?2 with remarkable durability over 24 h. This work provides a new strategy for the preparation of effective HER electrocatalyst with a low precious metal content.     

A novel efficient dual-functional electrocatalyst for overall water splitting based on Ni0.85Se/RGO/CNTs nanocomposite synthesized via different nickel precursors

Synthesizing efficient and affordable electrocatalysts for the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) remains a crucial problem on the way to practical applications for producing clean H₂ fuel. Herein, high-efficiency and stable transition metal based electrocatalysts Ni_0.85Se-1, Ni_0.85Se-2 and Ni_0.85Se-3 materials with different morphological characteristics were derived via a one-step hydrothermal route using the Ni(OH)₂ and metal-organic framework (Ni-BDC and Ni-BTC) as precursors, respectively. The results showed that Ni_0.85Se-2 exhibited excellent electrocatalytic activity. Subsequently, introducing carbon nanomaterials (RGO and CNTs) to form Ni_0.85Se/RGO/CNTs nanocomposite material further improves the catalytic activity owing to high conductivity. The resulting Ni_0.85Se/RGO/CNTs nanocomposites electrocatalyst showed a low overpotential of 232 mV and 165 mV and a low Tafel slope of 64 mV dec^?1 and 98 mV dec^?1 when the current density was 10 mA cm^?2 for OER and HER, respectively. In addition, the Ni_0.85Se/RGO/CNTs nanocomposites were used as an anode and cathode of the water electrolysis device and the overall water splitting performance was investigated. The results show just a voltage of 1.59 V was required when the current density was 10 mA cm^?2 and good overall water splitting stability for 20 h. The outstanding electrocatalytic performance of Ni_0.85Se/RGO/CNTs is mostly due to its noticeable porous structure, the high conductivity and the large surface area that came from RGO and CNTs.     

Autogenous growth of highly active bifunctional Ni–Fe2B nanosheet arrays toward efficient overall water splitting

Developing an effective and low-cost bifunctional electrocatalyst for both OER and HER to achieve overall water splitting is remaining a challenge to meet the needs of sustainable development. Herein, an electroless plating method was employed to autogenous growth of ultrathin Ni–Fe₂B nanosheet arrays on nickel foam (NF), in which the whole liquid phase reduction reaction took no more than 20 min and did not require any other treatments such as calcination. In 1.0 M KOH electrolyte, the resulted Ni–Fe₂B ultrathin nanosheet displayed a low overpotential of 250 mV for OER and 115 mV for HER to deliver a current density of 10 mA cm^?2, and both OER and HER activities remained stable after 26 h stability testing. Further, the couple electrodes composed of Ni–Fe₂B could afford a current density of 10 mA cm^?2 towards overall water splitting at a cell voltage of 1.64 V in 1.0 M KOH and along with excellent stability for 26 h. The outstanding electrocatalytic activities can be attributed to the synergistic effect of electron-coupling across Ni and Fe atoms and active sites exposed by large surface area. The effective combination of low cost and high electrocatalytic activity brings about a promising prospect for Ni–Fe₂B nanosheet arrays in the field of overall water splitting.     

Facile construction of heterostructural Ni3(NO3)2(OH)4/CeO2 bifunctional catalysts for boosted overall water splitting

Interface engineering has aroused vitally widespread concern since it could be an effective strategy for exploring high-performance and low-cost water oxidation electrocatalysts. Herein, we report a hetero-structured Ni₃(NO₃)₂(OH)₄/CeO₂/NF (NNO/CeO₂/NF) electrode, exhibiting superior performance owning to the NO₃^? anion substitution for the OH^? in nickel hydroxide to form Ni₃(NO₃)₂(OH)₄, together with its interface synergy with ceria. In alkaline solution, the NNO/CeO₂/NF electrocatalyst could catalyze the OER with an overpotential of 330 mV to approach 50 mA cm^?2. Also, it needs only an overpotential of 120 mV to reach 10 mA cm^?2 for HER. Additionally, when a standard two-electrode water electrolyzer is fabricated by employing NNO/CeO₂/NF as both the cathode and anode, it can generate 10 mA cm^?2 at 1.64 V and operate steadily without performance degradation after 25 h. This research provides a novel perspective for reasonable design of advanced catalytic materials with improvements in the field of electrocatalysis.     

Ni activated Mo2C nanoparticles supported on stereotaxically-constructed graphene for efficient overall water splitting

Exploring cost-effective, high-efficiency and stable electrocatalysts for overall water splitting is greatly desirable and challenging for sustainable energy. Herein, a novel designed Ni activated molybdenum carbide nanoparticle loaded on stereotaxically-constructed graphene (SCG) using two steps facile strategy (hydrothermal and carbonization) as a bifunctional electrocatalyst for overall water splitting. The optimized Ni/Mo₂C(1:20)-SCG composites exhibit excellent performance with a low overpotential of 150 mV and 330 mV for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively to obtain a current density of 10 mA cm^?2 in 1.0 M KOH solution. In addition, when the optimized Ni/Mo₂C(1:20)-SCG composite is used as a bifunctional electrode for overall water splitting, the electrochemical cell required a low cell voltage of 1.68 V at a current density of 10 mA cm^?2 and long-term stability of 24 h. More significantly, the synergetic effects between Ni-activated Mo₂C nanoparticles and SCG are regarded as a significant contributor to accelerate charge transfer and promote electrocatalytic performance in hybrid electrocatalysts. Our works introduce a novel approach to design advanced bifunctional electrodes for overall water splitting.     

Cu2S/Ni3S2 ultrathin nanosheets on Ni foam as a highly efficient electrocatalyst for oxygen evolution reaction

It is an inevitable choice to find efficient and economically-friendly electrocatalysts to reduce the high overpotential of oxygen evolution reaction (OER), which is the key to improve the energy conversion efficiency of water splitting. Herein, we synthesized Cu₂S/Ni₃S₂ catalysts on nickel foam (NF) with different molar ratios of Ni/Cu by a simple two-step hydrothermal method. Cu₂S/Ni₃S₂-0.5@NF (CS/NS-0.5@NF) effectively reduces the overpotential of OER, displaying small overpotentials (237 mV@100 mA cm^?2 and 280 mV@500 mA cm^?2) in an alkaline solution, along with a low Tafel slope of 44 mV dec^?1. CS/NS-0.5@NF also presents an excellent durability at a relatively high current density of 100 mA cm^?2 for 100 h. The excellent performance is benefited by the prominent structural advantages and desirable compositions. The nanosheet has a high electrochemical active surface area and the porous structure is conducive to electrolyte penetration and product release. This work provides an economically-friendly Cu-based sulfide catalyst for effective electrosynthesis of OER.     

In-situ growth of Fe–Co Prussian-blue-analog nanocages on Ni(OH)2/NF and the derivative electrocatalysts with hierarchical cage-on-sheet architectures for efficient water splitting

To design an efficient and cost-effective electrocatalyst based on Prussian blue and its analogs are a promising choice to realize energy transformation and storage via water-splitting. Herein, a facile and practical method is developed to in-situ grow Fe–Co Prussian-blue-analog (PBA) nanocages with an open hole in each face center on Ni(OH)₂/NF substrate to form the hierarchical cage-on-plate structure. Furthermore, the Fe–Co PBA nanocages attached to Ni(OH)₂/NF plates are hydrogenated and nitrogenized into FeCoNi/NF and FeCoNiN/NF electrodes, respectively. As-prepared electrodes successfully retain the 3D hierarchical micro-nano structures of Fe–Co PBA@Ni(OH)₂/NF precursor and can be used as a bifunctional water-splitting catalyst for overall water splitting. Compared to FeCoNi/NF, FeCoNiN/NF shows more efficiency and durability in the electrolytic water splitting tests in alkaline media. For the FeCoNiN/NF electrocatalyst, ultralow overpotentials for hydrogen evolution reaction (HER) are only 56 and 290 mV at current densities of 10 and 500 mA cm^?2. Meanwhile, overpotentials for oxygen evolution reaction (OER) are 267 and 374 mV at current densities of 50 and 500 mA cm^?2. The FeCoNiN/NF electrode can act both the cathode and the anode for overall water splitting, this electrolyzer only requires a cell voltage of 1.492 V to afford a current density of 10 mA cm^?2. This electrolyzer can stably deliver a viable high current density of 625 mA cm^?2 for 40 h to meet the condition of industrial application.     

Facile one-pot synthesis of binder-free nano/micro structured dendritic cobalt activated nickel sulfide: a highly efficient electrocatalyst for oxygen evolution reaction

Reasonable design and preparation of non-noble metal electrocatalysts with predominant catalytic activity and long-term stability for oxygen evolution reaction (OER) are essential for electrocatalytic water splitting. Ni foam (NF) is highlighted for its 3D porous structure, impressive conductivity and large specific surface area. Herein, nano/micro structured dendritic cobalt activated nickel sulfide grown on 3D porous NF (Co–Ni₃S₂/NF) has been successfully synthesized by one-step hydrothermal method. Due to the ingenious incorporation of Co, Co–Ni₃S₂/NF electrode shows auspicious electrocatalytic performance for OER compared with Ni₃S₂/NF electrode. As a result, Co–Ni₃S₂/NF needs overpotential of only 274 and 459 mV at current density of 10 and 50 mA cm⁻², respectively, while Ni₃S₂/NF requires overpotential of 344 and 511 mV. At potential of 2.0 V (vs. RHE), Co–Ni₃S₂/NF displays current density of 191 mA cm⁻², while Ni₃S₂/NF just attains current density of only 135 mA cm⁻². Moreover, Co–Ni₃S₂/NF demonstrates excellent stability for uninterrupted OER in alkaline electrolyte. The strategy of designing and preparing cobalt activated nickel sulfide grown on NF renders a magnificent prospect for the development of metal-sulfide-based oxygen evolution catalysts with excellent electrocatalytic performances.     

Vermicular Ni3S2–Ni(OH)2 heterostructure supported on nickel foam as efficient electrocatalyst for hydrogen evolution reaction in alkaline solution

Alkaline solution is considered to be more suitable for industrial application of hydrogen production by water electrolysis. However, most of the low-cost electrocatalyts such as Ni₃S₂ has poor ability to dissociate HO–H, resulting in unsatisfied hydrogen evolution performance in alkaline media. In this paper, a novel vermicular structure of Ni₃S₂–Ni(OH)₂ hybrid have been successfully prepared on nickel foam substrate (v-Ni₃S₂–Ni(OH)₂/NF) through a facile two-step containing hydrothermal and electrodeposition processes. The heterostructure consists of rod-like Ni₃S₂ and Ni(OH)₂ nanosheets, in which Ni(OH)₂ is coated on the surface of Ni₃S₂. This structure not only constructs a fast electron transfer channel but also possesses rich heterointerface, thus accelerating the Volmer step and allowing more active sites of Ni₃S₂ to functioning well. As a result, v-Ni₃S₂–Ni(OH)₂/NF exhibited excellent electrocatalytic activity toward HER in 1.0 M KOH solution. It only needs 78 mV and 137 mV to drive current density of 10 mA cm⁻² and 100 mA cm⁻². Moreover, the catalytic stability of this electrocatalyst in alkaline solution is also satisfactory.     

Hairy sphere-like Ni9S8/CuS/Cu2O composites grown on nickel foam as bifunctional electrocatalysts for hydrogen evolution and urea electrooxidation

The urea solution electrolysis has become more attractive than water splitting, because it not only produces clean H₂ via the cathodic hydrogen evolution reaction (HER) with lower cell voltage, but also treats sewage containing urea through anodic urea oxidation reaction (UOR). However, lack of efficient electrocatalysts for HER and UOR has limited its development. Herein, hairy sphere -like Ni₉S₈/CuS/Cu₂O composites were synthesized on nickel foam (NF) in situ by a two-step hydrothermal method. The Ni₉S₈/CuS/Cu₂O/NF exhibited good electrocatalytic activity for both HER (?0.146 V vs. RHE to achieve 10 mA cm^?2) and UOR (1.357 V vs. RHE to achieve 10 mA cm^?2). Based on the bifunctional properties of Ni₉S₈/CuS/Cu₂O/NF, a dual-electrode urea solution electrolytic cell was constructed, which only needed a low voltage of 1.47 V to reach a current density of 10 mA cm^?2, and displayed a good stability during a 20-h test. In addition, the reason for the good catalytic activity of Ni₉S₈/CuS/Cu₂O/NF was analyzed and the UOR mechanism was discussed in detail. Our research shows that Ni₉S₈/CuS/Cu₂O/NF is a very promising low-cost dual-function electrocatalyst, which can be used for high-efficiency electrolysis of urea solution to produce hydrogen and treat wastewater.     

Adjusting electronic structure coupling of Fe–Ni2P (NiFeP-MOF) multilevel structure for ultra-activity and durable catalytic water oxidation

Efficient electrocatalyst for alkaline oxygen evolution reaction is the critical core to the wide application of metal-air energy storage and water electrolysis hydrogen energy. Therefore, appropriate design of highly active and stable non-noble metal oxygen evolution electrocatalyst with good electronic structure and multilevel structure is both a goal and a challenge. Here, we report a Fe–Ni₂P electrocatalyst (NiFeP-MOF) with multilevel structure, which was obtained by anion exchange on the basis of Fe–Ni(OH)₂ (NiFe-MOF) grown on nickel foam in situ by solvothermal method. As expected, Fe substitution regulates the Ni oxidation state in the NiFeP-MOF and realizes electronic structure coupling, showing a highly active and stable oxygen evolution reaction (OER) in alkaline electrolyte solution. Specifically, the NiFeP-MOF demonstrates an ultralow overpotentials (232 mV, 10 mA cm^?2; 267 mV 100 mA cm^?2), respectively, an extremely small Tafel slope (34 mV dec^?1). Separately, the electrocatalyst shows an excellent cycle stability at 10 mA cm^?2 for 12 h (43,200 s). More importantly, this work come up with an available policy for the preparation of excellent alkaline hydrolysis electrolysis catalysts and air cathodes with excellent performance.     

Construction of NiCo2S4/Ni3S2 nanoarrays on Ni foam substrate as an enhanced electrode for hydrogen evolution reaction and supercapacitors

Developing a multifunctional and sustainable electrode material for hydrogen evolution reaction and supercapacitors is a highly feasible avenue for producing the high energy density and renewable energies. In our study, nanostructured NiCo₂S₄/Ni₃S₂/NF nanoarrays are rational developed in experiments via a simple hydrothermal reaction. Ascribed to the 3D nanostructured NiCo₂S₄/Ni₃S₂ with numerous exposure active sites and large contact areas for the electrolyte, the binder-free feature of NiCo₂S₄/Ni₃S₂/NF facilitates a low charge transfer resistance, as well as the synergetic effect of NiCo₂S₄ and Ni₃S₂. The obtained electrocatalyst showed ultrahigh electrocatalytic activity with an overpotential of 111 mV at 10 mA cm⁻² and a Tafel slope of 57 mV dec⁻¹. In addition, the electrode showed an area specific capacity of 6.13 F cm⁻² at 10 mA cm⁻² and superior rate capability (2.72 F cm⁻² at 80 mA cm⁻²), accompanied by excellent cycling stability. This results presented in our work can provide an effective strategy for rational design of other hybrid materials with excellent electrochemical performance in the application of electrocatalysis and supercapacitors.     

Heterogeneous layered multiple transition metal composite electrocatalysts with controlled composition for hydrogen production

The exploration of highly efficient and low-cost bifunctional electrocatalyst is essential for overall water splitting, especially for industrial application under alkaline conditions. Herein, we propose a controllable structural engineering strategy of constructing heterogeneous layered electrocatalyst with wetting surface for hydrogen evolution reaction and oxygen evolution reaction. Heterogeneous layered NiFe LDH (layered double hydroxide)/CoFeP/NF (Ni foam) with superhydrophilic surfaces is successfully fabricated by successive electrodeposition, phosphorization and solvothermal method. The NiFe LDH/CoFeP/NF for hydrogen evolution achieves a low overpotential of 198 mV at 50 mA cm^?2 in 1.0 M KOH. An overpotential of 269 mV is required at 50 mA cm^?2 for oxygen evolution. Meanwhile, the practical utilization of NiFe LDH/CoFeP/NF as bifunctional electrocatalysts for overall water splitting yields 1.73 V at 50 mA cm^?2 in the two-electrode cell. Moreover, NiFe LDH/CoFeP/NF can retain over 50 h without an obvious degradation at 10 mA cm^?2. The satisfactory operating stability and high activity of NiFe LDH/CoFeP/NF in alkaline solution can be attributed to the heterogeneous layered structure and excellent hydrophilic surface. The study provides a strategy to engineering heterogeneous layered structures with wetting surface for excellent electrocatalytic activities toward overall water splitting.