NiFe LDH/Ti3C2Tx/nickel foam as a binder-free electrode with enhanced oxygen evolution reaction performance

In this work, NiFe LDH/Ti₃C₂T_x/Nickel foam (NF) was successfully prepared as a binder-free electrode by depositing NiFe layered double hydroxide (LDH) nanosheets on Ti₃C₂T_x/NF substrate through electrodeposition approach. The strong electrostatic interactions between the negatively charged surface of MXene and positively charged NF substrate enabled the direct growth of NiFe LDH nanosheets on Ti₃C₂T_x/NF substrate. As a result, the as-prepared NiFe LDH/Ti₃C₂T_x/NF electrode exhibited an excellent OER performance, fast catalytic reaction kinetics and good chemical stability. Its overpotential reached 200 mV at a current density of 10 mA cm^?2, and the cycling tests suggested a good cycling stability.     

Spatially confined growth of ultrathin NiFe layered double hydroxide nanosheets within carbon nanofibers network for highly efficient water oxidation

The rational design of catalysts with low cost, high efficient and robust stability toward oxygen evolution reaction (OER) is greatly desired but remains a formidable challenge. In this work, a one-pot, spatially confined strategy was reported to fabricate ultrathin NiFe layered double hydroxide (NiFe-LDH) nanosheets interconnected by ultrafine, strong carbon nanofibers (CNFs) network. The as-fabricated NiFe-LDH/CNFs catalyst exhibits enhanced OER catalytic activity in terms of low overpotential of 230 mV to obtain an OER current density of 10 mA cm^?2 and very small Tafel slope of 34 mV dec^?1, outperforming pure NiFe-LDH nanosheets assembly, commercial RuO₂, and most non-noble metal catalysts ever reported. It also delivers an excellent structural and electrocatalytic stability upon the long-term OER operation at a large current of 30 mA cm^?2 for 40 h. Furthermore, the cell assembled by using NiFe-LDH/CNFs and commercial Pt/C as anode (+) and cathode (?) ((+)NiFe-LDH/CNFs||Pt/C(?)) only requires a potential of 1.50 V to deliver the water splitting current of 10 mA cm^?2, 130 mV lower than that of (+)RuO₂||Pt/C(?) couple, demonstrating great potential for applications in cost-efficient water splitting devices.     

Synergistically modulating the electronic structure of Cr-doped FeNi LDH nanoarrays by O-vacancy and coupling of MXene for enhanced oxygen evolution reaction

Water splitting is an environmentally friendly method of hydrogen generation. However, it is severely limited by the slow anodic oxygen evolution reaction (OER). Iron-nickel layered double hydroxides (FeNi LDH) are promising electrocatalysts for OER, but their intrinsically low electrical conductivity and activity limit the practical applications. Herein, chromium-doped FeNi LDH nanoarrays in situ vertically grown on the surface of the Ti₃C₂T_x MXene (Cr-FeNi LDH/MXene) are successfully synthesized. Remarkably, the robust interaction and electrical coupling between Cr–FeNi LDH and MXene, as well as conspicuous charge transfer and the oxygen vacancies optimizing the adsorption free energy of intermediates, equip the nanocomposites with brilliant catalytic activity and stability toward OER. Thus, the optimized Cr–FeNi LDH/MXene shows a considerable boost in the OER, which affords low overpotential (232 mV at 10 mA cm^?2) and excellent durability. This work offers a new path to designing highly efficient and earth-abundant catalysts for water splitting and beyond.     

ZIF67@MoO3 NSs@NF composite electrocatalysts reinforced by chemical bonds and oxygen vacancy for efficient oxygen evolution reaction and overall water-splitting

A kind of composite electrocatalysts with the structure of MoO₃ nanosheets coated by ZIF67 nanocrystals and grown on the nickel foam substrate (ZIF67@MoO₃ NSs@NF) is prepared and mainly used as the electrode for oxygen evolution reaction (OER) and overall water splitting. The excellent electrocatalytic activity of ZIF67@MoO₃ NSs@NF are demonstrated. It can use the overpotential (?) of 178 mV and 386 mV respectively to drive 10 mA cm^?2 and 50 mA cm^?2. It is also observed that the ZIF67@MoO₃ NSs@NF electrode has the highest initial current density (45.7 mA cm^?2) at 1.618 V and can maintain more than 90% of the initial current density after 20,000 s. The ZIF67@MoO₃ NSs@NF electrode also shows the small HER overpotential of 135 mV at 10 mA cm^?2. Furthermore, the voltage of ZIF67@MoO₃ NSs@NF as a bifunctional overall water splitting catalysts is 1.58 V at 10 mA cm^?2, which is superior to another noble metal electric catalyst combination RuO₂/NF(+)//Pt–C/NF(?). And the ZIF67@MoO₃ NSs@NF(+)//ZIF67@MoO₃ NSs@NF(?) combination can maintain more than 90% of the initial current density after 65,000 s at 1.58 V. The main reason is the composite interface of MoO₃ NSs and ZIF67 phases with Co–O bonds, C–O–Mo bonds and oxygen vacancies defects facilitates the increase of the active sites and efficient electron transfer rate.     

Amorphous-crystalline cobalt-molybdenum bimetallic phosphide heterostructured nanosheets as Janus electrocatalyst for efficient water splitting

Efficient and sustainable Janus catalysts toward hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) are highly desirable for future hydrogen production via water electrolysis. Herein we report an active Janus electrocatalyst of amorphous-crystalline cobalt-molybdenum bimetallic phosphide heterostructured nanosheets on nickel foam (CoMoP/CoP/NF) for efficient electrolysis of alkaline water. As-reported CoMoP/CoP/NF consists of amorphous bimetal phosphide nanosheets doped with crystalline CoMoP/CoP heterostructured nanoparticles on NF. It can efficiently catalyze both HER (η = 127 mV@100 mA cm^?2) and OER (η = 308 mV@100 mA cm^?2) in alkaline electrolyte with long-term durability. Serving as anode and cathode of water electrolyzer, CoMoP/CoP/NF generates electrolytic current of 10, 50 and 100 mA cm^?2 at low voltage of 1.50, 1.59, and 1.67 V, respectively.     

Ultrafine Ru nanoparticles derived from few-layered Ti3C2Tx MXene templated MOF for highly efficient alkaline hydrogen evolution

It is meaningful to search high-efficient and inexpensive electrocatalysts for hydrogen evolution reaction (HER) due to the energy crisis and environmental pollution. Here, we report the preparation of ultrafine Ru nanoparticles from a hybrid of ZIF-L(Co) MOF and polydopamine coated few-layered Ti₃C₂T_x MXene (FL-Ti₃C₂T_x). FL-Ti₃C₂T_x is used as a template to grow regular leaf-shaped ZIF-L(Co) nanosheets through the reaction of Co ions anchored on the MXene surface with 2-methylimidazole. The obtained hybrid is then doped with Ru ions through ion exchange between Ru and Co ions, followed by thermal annealing at a temperature of 350 °C in an Ar atmosphere to produce ultrafine Ru nanoparticles. The obtained Ru@ZIF-L(Co)/FL-Ti₃C₂T_x nanocomposite shows outstanding HER performance with a low overpotential of 16.2 mV at a current density of 10 mA cm^?2, a small Tafel slope of 21.0 mV dec^?1 and excellent stability in 1.0 M KOH solution. This work provides a new strategy for the design and synthesis of highly efficient HER catalyst via MOFs with tunable composition and structure.     

Cu2S@NiFe layered double hydroxides nanosheets hollow nanorod arrays self-supported oxygen evolution reaction electrode for efficient anion exchange membrane water electrolyzer

Herein, we prepared highly active self-supported Cu₂S@NiFe layered double hydroxides nanosheets (LDHs) oxygen evolution reaction (OER) electrode (Cu₂S@NiFe LDHs/Cu foam) with three-dimensional (3D) multilayer hollow nanorod arrays structure, which is composed of the outer layer (two-dimensional (2D) NiFe LDHs) and the inner layer (one-dimensional (1D) Cu₂S hollow nanorod arrays). The unique structure of NiFe LDHs and Cu₂S hollow nanorod composites can expose more active sites, and simultaneously promote electrolyte penetration and gas release during the water electrolysis process. Thus, the Cu₂S@NiFe LDHs/Cu foam electrode exhibits a significant OER performance, with the overpotentials of 230 and 286 mV at 50 and 100 mA cm⁻², respectively. Anion exchange membrane water electrolyzer (AEMWE) with the prepared electrode can attain a voltage of 1.56 V at the current density of 0.50 A cm⁻², showing a good performance that is comparable to the-state-of-the-art AEMWE in 1 M KOH. In addition, the AEMWE can be run for 300 h at the current density of 0.50 A cm⁻². The high performance and good stability of AEMWE are attributed to the special structure of the OER electrode, which can prevent the agglomeration of nanosheets and thus expose more active sites at the edge of the nanosheets.     

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.     

Promotion of MXene (Ti3C2Tx) as a robust electrocatalyst for oxygen evolution reaction via active sites of ZIF-67 - In situ mechanism investigations

Developing a robust and highly efficient electrocatalyst for the oxygen evolution reaction (OER) is required, due to its sluggish mechanism and high overpotential. Here, we present the Ti₃C₂T_x and ZIF-67 composites (MXene/ZIF-67) for an efficient OER. The MXene/ZIF-67_1:10 exhibits an overpotential of 366 mV, which is better than MXene (548 mV) and RuO₂ (395 mV). Moreover, it shows improved electrochemical stability at 20 mA·cm^{− 2} with only a 0.2% increase in potential after 5 h, while RuO₂ with an overpotential loss of 3.5%. After an increase in the current density of 10–20 mA cm⁻² the potential increase by 7.4%, while in RuO₂ by 25.3%. To reveal the observed performance, the composite's robustness and explain each component's role. Moreover, a detailed OER mechanism is discussed. It was realized via in situ Raman microscopy and XRD which allowed the revealing of the active species responsible for boosting OER.     

Preparation of NiCo-LDH@NiCoV-LDH interconnected nanosheets as high-performance electrocatalysts for overall water splitting

Alkaline water electrolysis is a promising strategy for the production of hydrogen and oxygen. However, developing high-efficiency non-precious electrocatalysts for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is still a big challenge. Here, we report a nickel foam-based electrode coated with NiCoV-LDH and NiCo-LDH nanosheets (denoted as NiCo-LDH@NiCoV-LDH/NF) by a two-step method for efficient water splitting performance. The NiCo-LDH@NiCoV-LDH/NF with unique nanosheet-on-nanosheet construction can enlarge the electrochemical active specific surface area greatly, and thus accelerate the charge transfer of electrocatalytic reactions. Besides, the doping of vanadium could also improve the OER performance. The electrode only requires a low overpotential for OER (260 mV at 100 mA cm^?2), and HER (80 mV at 10 mA cm^?2) reactions in 1.0 mol/L KOH solution at room temperature. Furthermore, in the two-electrode water splitting test, a current density of 10 mA cm^?2 was achieved at 1.55 V using 1.0 mol/L KOH solution, with excellent durability of 40 h. This work provided a facile method for developing new bifunctional catalysts.     

One-step preparation of Fe-doped Ni3S2/rGO@NF electrode and its superior OER performances

In order to improve the OER performance, Ni₃S₂-based catalysts were directly grown on Ni substrate by simultaneously doping of Fe and compositing with reduced graphene oxide (rGO). Synthesis and loading of Ni₃S₂/rGO were completed during a one-step hydrothermal process, in which Ni foam acted as support and Ni source of Ni₃S₂, as well as the subsequent current collector. It is found that either GO or Fe salt tuned Ni₃S₂ nanosheets into thinner and smaller interconnected nanosheets anchored on rGO, which enhanced the charge transfer resistance and improved the active sites. Hence, as-synthesized Fe-doped Ni₃S₂/rGO composite at 120 °C (Fe-2-Ni₃S₂/rGO@NF-120) exhibited an enhancement on OER performances: An overpotential of 247 mV at 20 mA cm⁻², and a small Tafel slope of 63 mV dec⁻¹, as well as an excellent stability of: 20 h maintaining at 20 mA cm⁻² or 50 mA cm⁻².     

Heterostructured iron-cobalt sulfides nanoclusters entrenched in 3D-nanosheets as high-efficient electrocatalysts for oxygen evolution reaction

Three dimensional (3D) binary Earth-abundant transition metal derived layered nanomaterials are presently considered as the emergent catalysts for the oxygen evolution reaction (OER). In the present study, we demonstrate morphology-controlled bimetallic iron-cobalt (FeCo) nanoclusters (～3.2 nm) embedded in 3D nanosheets (3D-FeCoS NS) on nickel foam (NF) electrode using of single-step electrochemical fabrication approach. The as-developed binder-free 3D-FeCoS NS employ as the potential electrocatalysts for improved OER in 1.0 M KOH. Results display that the 3D-FeCoS NS-B (“B” represents the molar ratio of Fe and Co (1:1)) exhibited an exceptional catalytic OER activity, including a low overpotential (η) (～223 mV @ 10 mA cm^?2), small Tafel slope (～66 mV dec^?1), high mass activity (～208 Ag^?1), high turnover frequency (TOF) (～1.2 s^?1), and long-term stability (over 100 h). More significantly, the 3D-FeCoS NS-B6PtC couple attained the current density of ～10 mA cm^?2 only at the potential of ～1.53 V, comparing positively with the state-of-the-art RuO₂6PtC couple. The abundant active sites of nanoclusters and edges of the sheets, synergy between the heterostructures, and accompanied by the presence of surface sulfides/oxides yield improved the OER activity. This study signifies a novel strategy to establish 3D Earth-abundant transition metal sulfides nanosheets for various electrochemical applications, including energy conversion and storage systems.     

A hierarchical nickel-iron hydroxide nanosheet from the high voltage cathodic polarization for alkaline water splitting

Developing efficient and stable oxygen evolution reaction (OER) electrocatalysts is a promising method to relieve the pressure of noble metals for catalyzing water splitting. Among the prominent candidates, nickel-iron layered double hydroxides (NiFe-LDH) have been found excellent catalytic activity, but their poor conductivity and stability seriously impede their performance. Herein, we report hierarchical NiFe-LDH nanosheets prepared from NiFe-Alloy on nickel mesh (NM) by high voltage cathodic polarization. The resultant NiFe-LDH/NM exhibits a remarkable OER activity and stability, which has a low overpotential of 340 mV at a current density of 10 mA cm^?2, and maintains a current density of 15 mA cm^?2 at a constant voltage of 1.56 V for 50 h if the NiFe-Alloy/NM is used as the cathode. The successful conversion of NiFe-LDH nanosheets originating from NiFe-Alloy nanoparticles would open a new avenue for synthesizing transition metal-based LDH compounds.     

Vertical Nickel–Iron layered double hydroxide nanosheets grown on hills-like nickel framework for efficient water oxidation and splitting

Herein, the vertical thin nickel–iron layered double hydroxide nanosheets grown on the hills-like nickel framework (NiFe LDH/Ni@NF) are employed for the oxygen evolution reaction (OER), securing at the low overpotentials of 197 and 270 mV to obtain the current densities of 20 and 100 mA cm⁻², respectively, with a Tafel slope of 73.34 mV dec⁻¹. The electrodeposited nickel film induces the NiFe LDH nanosheets grow vertically and thinly. As well, the nickel abundant interfaces and inner space makes this catalyst effective for OER. It was further served as the OER electrode in a water splitting system coupled the Pt/C cathode, and a cell voltage was at 1.52 and 1.67 V to achieve the current density of 10 mA cm⁻² and 50 mA cm⁻². In addition, the water electrolyzer can suffer a long time of 24 h at 50 mA cm⁻², showing the feasibility in a practical unbiased alkaline water splitting system.     

Growth of ultrathin nanosheets of nickel iron layered double hydroxide for the oxygen evolution reaction

Because of low cost and abundance, nickel-iron double layered hydroxide (NiFe LDH) is seen as a viable substitute for noble-metal-based electrodes for the oxygen evolution reaction (OER). Herein, we report the growth of NiFe LDH in the form of fine nanosheets in a single step using benzyl alcohol-mediated chemistry. The electrochemical studies clearly suggest that benzyl alcohol is capable of inducing effective chemical interaction between Ni and Fe in the NiFe LDH. The overpotential to produce benchmark 10 mA cm^?2 (η₁₀) for the NiFe LDH electrode is only ～270 mV_RHE, which is much smaller than those of benchmark IrO₂ (η₁₀ = 318 mV_RHE), nickel hydroxide (η₁₀ = 370 mV_RHE) and iron hydroxide (η₁₀ = 410 mV_RHE) for the OER. The difference of the overpotential requirement increases further with increasing current density, indicating faster kinetics of the OER at the catalytic interface of the NiFe LDH. Estimation of Tafel values verifies this notion – the Tafel slopes of NiFe LDH, Ni(OH)₂, and FeOOH are calculated to be 48.6, 55.8, and 59.3 mV dec^?1, respectively. At η = 270 mV, the turnover frequency (TOF) of the NiFe LDH is 0.48 s^?1, which is ～8 and ～11 folds higher than those of Ni(OH)₂ (0.059 s^?1) and FeOOH (0.042 s^?1). In addition to Tafel and TOF, the NiFe LDH electrode has favorable electrochemically active surface area and electrochemical impedance. The electrochemical stability of the NiFe LDH electrode is assessed by conducting potentiostatic measurements at η = 270 mV_RHE (～10 mA cm^?2) and at η = 355 mV_RHE (～30 mA cm^?2) for 24 h of continuous oxygen production.     

Co2P nanoparticles supported on cobalt-embedded N-doped carbon materials as a bifunctional electrocatalyst for rechargeable Zn-air batteries

Reversible oxygen electrodes with high efficiencies for the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) are of great significance for a variety of energy conversion devices, such as fuel cells and metal-air batteries. Herein, Co₂P nanoparticles supported on cobalt-embedded N-doped carbon materials (Co₂P/Co–N–C) have been prepared by pyrolysis of cobalt zeolitic imidazolate framework and phosphating post treatment. The optimal Co₂P/Co–N–C composite shows excellent bifunctional electrocatalytic activities for both OER (the potential of 1.65 V at 10 mA cm^?2) and ORR (half-wave potential of 0.82 V). As a practical demonstration, Co₂P/Co–N–C catalyst is used as an air electrode in liquid Zn-air battery, which displays a large open-circuit voltage of 1.50 V, a high peak-power density of 158 mW cm^?2 and excellent reversibility of over 205 h at 5 mA cm^?2. Moreover, the flexible Zn-air battery with Co₂P/Co–N–C exhibits a high open-circuit voltage of 1.46 V and the good flexibility with different angles. This work provides inspiration to explore new strategies for electrochemical energy conversion and storage.     

Structural engineering of hierarchically hetestructured Mo2C/Co conformally embedded in carbon for efficient water splitting

Developing low-cost and high efficient electrocatalysts for both oxygen and hydrogen evolution reaction in an alkaline electrolyte toward overall water splitting is still a significant challenge. Here, a novel hierarchically heterostructured catalyst composed of ultrasmall Mo₂C and metallic Co nanoparticles confined within a carbon layer is produced by a facile phase separation strategy. During thermal reduction of CoMoO₄ nanosheets in CO ambient, in-situ generated nanoscale Co and ultrafine Mo₂C conformally encapsulated in a conductive carbon layer. In addition, some carbon nanotubes catalyzed by Co nanoparticles vertically grew on its surface, creating 3D interconnected electron channels. More importantly, the integrated C@Mo₂C/Co nanosheets assembled into the hierarchical architecture, providing abundant active surface and retaining the structural integrity. Benefiting from such unique structure, the constructed hierarchical heterostructure shows low overpotentials of 280 mV and 145 mV to reach a current density of 10 mA cm⁻² for OER and HER in an alkaline electrolyte. Furthermore, the symmetrical electrolyzer assembled with catalyst exhibits a small cell voltage of 1.67 V at 10 mA cm⁻² in addition to outstanding durability, demonstrating the great potential as a high efficient bifunctional electrocatalyst for overall water splitting.     

Electroless deposition synthesis of composite catalysts Ni-Fe-P-WO3/NF with superior oxygen evolution performance

The proper construction of high efficiency, low-cost, earth-abundant oxygen evolution reaction (OER) catalyst is essential for hydrogen formation by water splitting. A novel electrocatalyst with highly active OER performance was manufactured by a simple electroless deposition method of Ni-Fe-P-WO₃ on nickel foam (NF). Benefiting from outstanding mass transfer capability of Ni-Fe-P-WO₃/NF heterogeneous structure, abundance of active sites in the amorphous architecture and etc., the Ni-Fe-P-WO₃/NF shows extremely superb electrocatalytic properties compare to noble metal catalyst IrO₂/NF for OER, which needs an overpotential of only 218 mV in 1.0 M KOH solution to achieve the current density of 10 mA cm^?2. It also has remarkable OER activity at high current density that only needs 298 mV to attain 100 mA cm^?2 current density. Moreover, the Ni-Fe-P-WO₃/NF has low Tafel slope of 42 mV dec^?1. This study offers a novel approach to the production of OER multiphase electrocatalysts from oxides and alloys.     

Mo-incorporated three-dimensional hierarchical ternary nickel-cobalt-molybdenum layer double hydroxide for high-efficiency water splitting

Flowers-like 3D hierarchical ternary NiCoMo-layered double hydroxide (NiCoMo-LDH) spheres have been fabricated in substrate-free route via a one-pot hydrothermal method and utilized as efficient electrocatalysts for the OER and HER. The well-structured 3D hierarchical flowers were composed of numerous two-dimensional nanosheets, which inherently possess considerable electrochemical active sites, thereby enhancing catalytic activity. NiMo and CoMo binary LDHs, with similar morphology, were also prepared to illustrate the efficiency of the ternary LDH. The results indicate higher electrocatalytic activity for the ternary LDH as compared to binary LDHs under alkaline conditions. The NiCoMo-LDH required an overpotential as low as 202 and 93 mV to deliver a constant anodic and cathodic current density of 10 mA cm^?2 for the OER and HER, respectively. Furthermore, the NiCoMo-LDH exhibited remarkable HER activity, affording a low overpotential of 198 mV at a current density of ?100 mA cm^?2. Moreover, it could offer a stable current density of 10 mA cm^?2 for overall water splitting at 1.62 V in 1 M KOH with long-term stability for 20 h. The double-layer capacitance (C_dl) value indicated that the NiCoMo-LDH significantly influenced interface conductivity and the electrochemical active surface area. The ternary NiCoMo-LDH electrode yielded low Tafel slope values of 54 and 51 mVdec^?1 for the OER and HER. Owing to the efficient incorporation of Ni, Co, and Mo in a layered structure, synergetic effect, and high electrochemical surface area, the NiCoMo-LDH exhibited remarkable electrocatalytic activity. Such eco-friendly ternary LDHs can be used in rechargeable metal–air batteries for industrial applications.     

CoP-anchored high N-doped carbon@graphene sheet as bifunctional electrocatalyst for efficient overall water splitting

Electrocatalytic water splitting, as an ideal technology in renewable energy applications, suffers from high electrical energy consumption due to the slow kinetics of HER and OER reactions. Therefore, it is urgent to design efficient bifunctional catalysts to improve the reaction kinetics. Herein, a self-supported electrode, anchoring CoP nanoparticles on N-doped carbon/graphene (NC-G) and chemically growing on Ni foam as a whole electrode (denoted as NC-G-CoP/NF) displays promising electrocatalytic performance in 1.0 M KOH electrolyte, with a low overpotentials of 68 mV at 10 mA cm^?2 for HER and 255 mV at 50 mA cm^?2 for OER. This bifunctional electrocatalyst only needs 1.435 V to generate 10 mA cm^?2 for overall water splitting. The outstanding electrocatalytic performance is ascribed to the following factors: i) inherent nature of transition metal phosphides, ii) abundant and high dispersion N active sites in NC-G, iii) strong interaction between the NC-G and CoP nanoparticles, and iv) rapid electron transfer between the catalytic centers and Nickle foam. This provides a new perspective to design efficient electrocatalysts for electrocatalytic water splitting.