Gap‐Mode Surface‐Plasmon‐Enhanced Photoluminescence and Photoresponse of MoS2

2D materials hold great potential for designing novel electronic and optoelectronic devices. However, 2D material can only absorb limited incident light. As a representative 2D semiconductor, monolayer MoS₂ can only absorb up to 10% of the incident light in the visible, which is not sufficient to achieve a high optical‐to‐electrical conversion efficiency. To overcome this shortcoming, a “gap‐mode” plasmon‐enhanced monolayer MoS₂ fluorescent emitter and photodetector is designed by squeezing the light‐field into Ag shell‐isolated nanoparticles–Au film gap, where the confined electromagnetic field can interact with monolayer MoS₂. With this gap‐mode plasmon‐enhanced configuration, a 110‐fold enhancement of photoluminescence intensity is achieved, exceeding values reached by other plasmon‐enhanced MoS₂ fluorescent emitters. In addition, a gap‐mode plasmon‐enhanced monolayer MoS₂ photodetector with an 880% enhancement in photocurrent and a responsivity of 287.5 A W^?1 is demonstrated, exceeding previously reported plasmon‐enhanced monolayer MoS₂ photodetectors.     

Unveiling the Interfacial Effects for Enhanced Hydrogen Evolution Reaction on MoS2/WTe2 Hybrid Structures

Using the MoS₂‐WTe₂ heterostructure as a model system combined with electrochemical microreactors and density function theory calculations, it is shown that heterostructured contacts enhance the hydrogen evolution reaction (HER) activity of monolayer MoS₂. Two possible mechanisms are suggested to explain this enhancement: efficient charge injection through large‐area heterojunctions between MoS₂ and WTe₂ and effective screening of mirror charges due to the semimetallic nature of WTe₂. The dielectric screening effect is proven minor, probed by measuring the HER activity of monolayer MoS₂ on various support substrates with dielectric constants ranging from 4 to 300. Thus, the enhanced HER is attributed to the increased charge injection into MoS₂ through large‐area heterojunctions. Based on this understanding, a MoS₂/WTe₂ hybrid catalyst is fabricated with an HER overpotential of ?140 mV at 10 mA cm^?2, a Tafel slope of 40 mV dec^?1, and long stability. These results demonstrate the importance of interfacial design in transition metal dichalcogenide HER catalysts. The microreactor platform presents an unambiguous approach to probe interfacial effects in various electrocatalytic reactions.     

Surface Engineering of MoS2 via Laser‐Induced Exfoliation in Protic Solvents

With excellent performance in the hydrogen evolution reaction (HER), molybdenum disulfide (MoS₂) is considered a promising nonprecious candidate to substitute Pt‐based catalysts. Herein, pulsed laser irradiation in liquid is used to realize one‐step exfoliation of bulk 2H‐MoS₂ to ultrastable few‐layer MoS₂ nanosheets. Such prepared MoS₂ nanosheets are rich in S vacancies and metallic 1T phase, which significantly contribute to the boosted catalytic HER activity. Protic solvents play a pivotal role in the production of S vacancies and 2H‐to‐1T phase transition under laser irradiation. MoS₂ exfoliated in an optimal solvent of formic acid exhibits outstanding HER activity with an overpotential of 180 mV at 10 mA cm^?2 and Tafel slope of 54 mV dec^?1.     

Roll‐to‐Roll Production of Layer‐Controlled Molybdenum Disulfide: A Platform for 2D Semiconductor‐Based Industrial Applications

A facile methodology for the large‐scale production of layer‐controlled MoS₂ layers on an inexpensive substrate involving a simple coating of single source precursor with subsequent roll‐to‐roll‐based thermal decomposition is developed. The resulting 50 cm long MoS₂ layers synthesized on Ni foils possess excellent long‐range uniformity and optimum stoichiometry. Moreover, this methodology is promising because it enables simple control of the number of MoS₂ layers by simply adjusting the concentration of (NH₄)₂MoS₄. Additionally, the capability of the MoS₂ for practical applications in electronic/optoelectronic devices and catalysts for hydrogen evolution reaction is verified. The MoS₂‐based field effect transistors exhibit unipolar n‐channel transistor behavior with electron mobility of 0.6 cm² V^?1 s^?1 and an on‐off ratio of ≈10³. The MoS₂‐based visible‐light photodetectors are fabricated in order to evaluate their photoelectrical properties, obtaining an 100% yield for active devices with significant photocurrents and extracted photoresponsivity of ≈22 mA W^?1. Moreover, the MoS₂ layers on Ni foils exhibit applicable catalytic activity with observed overpotential of ≈165 mV and a Tafel slope of 133 mV dec^?1. Based on these results, it is envisaged that the cost‐effective methodology will trigger actual industrial applications, as well as novel research related to 2D semiconductor‐based multifaceted applications.     

Phosphorus‐Rich Colloidal Cobalt Diphosphide (CoP2) Nanocrystals for Electrochemical and Photoelectrochemical Hydrogen Evolution

Developing earth‐abundant and efficient electrocatalysts for photoelectrochemical water splitting is critical to realizing a high‐performance solar‐to‐hydrogen energy conversion process. Herein, phosphorus‐rich colloidal cobalt diphosphide nanocrystals (CoP₂ NCs) are synthesized via hot injection. The CoP₂ NCs show a Pt‐like hydrogen evolution reaction (HER) electrocatalytic activity in acidic solution with a small overpotential of 39 mV to achieve ?10 mA cm^?2 and a very low Tafel slope of 32 mV dec^?1. Density functional theory (DFT) calculations reveal that the high P content both physically separates Co atoms to prevent H from over binding to multiple Co atoms, while simultaneously stabilizing H adsorbed to single Co atoms. The catalytic performance of the CoP₂ NCs is further demonstrated in a metal–insulator–semiconductor photoelectrochemical device consisting of bottom p‐Si light absorber, atomic layer deposition Al–ZnO passivation layers, and the CoP₂ cocatalyst. The p‐Si/AZO/TiO₂/CoP₂ photocathode shows a photocurrent density of ?16.7 mA cm^?2 at 0 V versus reversible hydrogen electrode (RHE) and an output photovoltage of 0.54 V. The high performance and stability are attributed to the junction between p‐Si and AZO, the corrosion‐resistance of the pinhole‐free TiO₂ protective layer, and the fast HER kinetics of the CoP₂ NCs.     

Highly Robust Non‐Noble Alkaline Hydrogen‐Evolving Electrocatalyst from Se‐Doped Molybdenum Disulfide Particles on Interwoven CoSe2 Nanowire Arrays

Developing efficient non‐noble and earth‐abundant hydrogen‐evolving electrocatalysts is highly desirable for improving the energy efficiency of water splitting in base. Molybdenum disulfide (MoS₂) is a promising candidate, but its catalytic activity is kinetically retarded in alkaline media due to the unfavorable water adsorption and dissociation feature. A heterogeneous electrocatalyst is reported that is constructed by selenium‐doped MoS₂ (Se‐MoS₂) particles on 3D interwoven cobalt diselenide (CoSe₂) nanowire arrays that drives the hydrogen evolution reaction (HER) with fast reaction kinetics in base. The resultant Se‐MoS₂/CoSe₂ hybrid exhibits an outstanding catalytic HER performance with extremely low overpotentials of 30 and 93 mV at 10 and 100 mA cm^–2 in base, respectively, which outperforms most of the inexpensive alkaline HER catalysts, and is among the best alkaline catalytic activity reported so far. Moreover, this hybrid catalyst shows exceptional catalytic performance with very low overpotentials of 84 and 95 mV at 10 mA cm^–2 in acidic and neutral electrolytes, respectively, implying robust pH universality of this hybrid catalyst. This work may provide new inspirations for the development of high‐performance MoS₂‐based HER electrocatalysts in unfavorable basic media for promising catalytic applications.     

Aligned Heterointerface‐Induced 1T‐MoS2 Monolayer with Near‐Ideal Gibbs Free for Stable Hydrogen Evolution Reaction

1T‐phase molybdenum disulfide (1T‐MoS₂) exhibits superior hydrogen evolution reaction (HER) over 2H‐phase MoS₂ (2H‐MoS₂). However, its thermodynamic instability is the main drawback impeding its practical application. In this work, a stable 1T‐MoS₂ monolayer formed at edge‐aligned 2H‐MoS₂ and a reduced graphene oxide heterointerface (EA‐2H/1T/RGO) using a precursor‐in‐solvent synthesis strategy are reported. Theoretical prediction indicates that the edge‐aligned layer stacking can induce heterointerfacial charge transfer, which results in a phase transition of the interfacial monolayer from 2H to 1T that realizes thermodynamic stability based on the adhesion energy between MoS₂ and graphene. As an electrocatalyst for HER, EA‐2H/1T/RGO displays an onset potential of ?103 mV versus RHE, a Tafel slope of 46 mV dec^?1 and 10 h stability in acidic electrolyte. The unexpected activity of EA‐2H/1T/RGO beyond 1T‐MoS₂ is due to an inherent defect caused by the gliding of S atoms during the phase transition from 2H to 1T, leading the Gibbs free energy of hydrogen adsorption (ΔG_H*) to decrease from 0.13 to 0.07 eV, which is closest to the ideal value (0.06 eV) of 2H‐MoS₂. The presented work provides fundamental insights into the impressive electrochemical properties of HER and opens new avenues for phase transitions at 2D/2D hybrid interfaces.     

Cobalt Covalent Doping in MoS2 to Induce Bifunctionality of Overall Water Splitting

The layer‐structured MoS₂ is a typical hydrogen evolution reaction (HER) electrocatalyst but it possesses poor activity for the oxygen evolution reaction (OER). In this work, a cobalt covalent doping approach capable of inducing HER and OER bifunctionality into MoS₂ for efficient overall water splitting is reported. The results demonstrate that covalently doping cobalt into MoS₂ can lead to dramatically enhanced HER activity while simultaneously inducing remarkable OER activity. The catalyst with optimal cobalt doping density can readily achieve HER and OER onset potentials of ?0.02 and 1.45 V (vs reversible hydrogen electrode (RHE)) in 1.0 m KOH. Importantly, it can deliver high current densities of 10, 100, and 200 mA cm^?2 at low HER and OER overpotentials of 48, 132, 165 mV and 260, 350, 390 mV, respectively. The reported catalyst activation approach can be adapted for bifunctionalization of other transition metal dichalcogenides.     

Interface Modulation of MoS2/Metal Oxide Heterostructures for Efficient Hydrogen Evolution Electrocatalysis

Developing efficient earth‐abundant MoS₂ based hydrogen evolution reaction (HER) electrocatalysts is important but challenging due to the sluggish kinetics in alkaline media. Herein, a strategy to fabricate a high‐performance MoS₂ based HER electrocatalyst by modulating interface electronic structure via metal oxides is developed. All the heterostructure catalysts present significant improvement of HER electrocatalytic activities, demonstrating a positive role of metal oxides decoration in promoting the rate‐limited water dissociation step for the HER mechanism in alkaline media. The as‐obtained MoS₂/Ni₂O₃H catalyst exhibits a low overpotential of 84 mV at 10 mA cm^?2 and small charge‐transfer resistance of 1.5 Ω in 1 m KOH solution. The current density (217 mA cm^?2) at the overpotential of 200 mV is about 2 and 24 times higher than that of commercial Pt/C and bare MoS₂, respectively. Additionally, these MoS₂/metal oxides heterostructure catalysts show outstanding long‐term stability under a harsh chronopotentiometry test. Theoretical calculations reveal the varied sensitivity of 3d‐band in different transition oxides, in which Ni‐3d of Ni₂O₃H is evidently activated to achieve fast electron transfer for HER as the electron‐depletion center. Both electronic properties and energetic reaction trends confirm the high electroactivity of MoS₂/Ni₂O₃H in the adsorption and dissociation of H₂O for highly efficient HER in alkaline media.     

Nickel@Nitrogen‐Doped Carbon@MoS2 Nanosheets: An Efficient Electrocatalyst for Hydrogen Evolution Reaction

Developing cheap, abundant, and easily available electrocatalysts to drive the hydrogen evolution reaction (HER) at small overpotentials is an urgent demand of hydrogen production from water splitting. Molybdenum disulfide (MoS₂) based composites have emerged as competitive electrocatalysts for HER in recent years. Herein, nickel@nitrogen‐doped carbon@MoS₂ nanosheets (Ni@NC@MoS₂) hybrid sub‐microspheres are presented as HER catalyst. MoS₂ nanosheets with expanded interlayer spacings are vertically grown on nickel@nitrogen‐doped carbon (Ni@NC) substrate to form Ni@NC@MoS₂ hierarchical sub‐microspheres by a simple hydrothermal process. The formed Ni@NC@MoS₂ composites display excellent electrocatalytic activity for HER with an onset overpotential of 18 mV, a low overpotential of 82 mV at 10 mA cm^?2, a small Tafel slope of 47.5 mV dec^?1, and high durability in 0.5 H₂SO₄ solution. The outstanding HER performance of the Ni@NC@MoS₂ catalyst can be ascribed to the synergistic effect of dense catalytic sites on MoS₂ nanosheets with exposed edges and expanded interlayer spacings, and the rapid electron transfer from Ni@NC substrate to MoS₂ nanosheets. The excellent Ni@NC@MoS₂ electrocatalyst promises potential application in practical hydrogen production, and the strategy reported here can also be extended to grow MoS₂ on other nitrogen‐doped carbon encapsulated metal species for various applications.     

Preparation of High‐Percentage 1T‐Phase Transition Metal Dichalcogenide Nanodots for Electrochemical Hydrogen Evolution

Nanostructured transition metal dichalcogenides (TMDs) are proven to be efficient and robust earth‐abundant electrocatalysts to potentially replace precious platinum‐based catalysts for the hydrogen evolution reaction (HER). However, the catalytic efficiency of reported TMD catalysts is still limited by their low‐density active sites, low conductivity, and/or uncleaned surface. Herein, a general and facile method is reported for high‐yield, large‐scale production of water‐dispersed, ultrasmall‐sized, high‐percentage 1T‐phase, single‐layer TMD nanodots with high‐density active edge sites and clean surface, including MoS₂, WS₂, MoSe₂, Mo_0.5W_0.5S₂, and MoSSe, which exhibit much enhanced electrochemical HER performances as compared to their corresponding nanosheets. Impressively, the obtained MoSSe nanodots achieve a low overpotential of ?140 mV at current density of 10 mA cm^?2, a Tafel slope of 40 mV dec^?1, and excellent long‐term durability. The experimental and theoretical results suggest that the excellent catalytic activity of MoSSe nanodots is attributed to the high‐density active edge sites, high‐percentage metallic 1T phase, alloying effect and basal‐plane Se‐vacancy. This work provides a universal and effective way toward the synthesis of TMD nanostructures with abundant active sites for electrocatalysis, which can also be used for other applications such as batteries, sensors, and bioimaging.     

Superior Hydrogen Evolution Reaction Performance in 2H‐MoS2 to that of 1T Phase

In the hydrogen evolution reaction (HER), energy‐level matching is a prerequisite for excellent electrocatalytic activity. Conventional strategies such as chemical doping and the incorporation of defects underscore the complicated process of controlling the doping species and the defect concentration, which obstructs the understanding of the function of band structure in HER catalysis. Accordingly, 2H‐MoS₂ and 1T‐MoS₂ are used to create electrocatalytic nanodevices to address the function of band structure in HER catalysis. Interestingly, it is found that the 2H‐MoS₂ with modulated Fermi level under the application of a vertical electric field exhibits excellent electrocatalytic activity (as evidenced by an overpotential of 74 mV at 10 mA cm^?2 and a Tafel slope of 99 mV per decade), which is superior to 1T‐MoS₂. This unexpected excellent HER performance is ascribed to the fact that electrons are injected into the conduction band under the condition of back‐gate voltage, which leads to the increased Fermi level of 2H‐MoS₂ and a shorter Debye screen length. Hence, the required energy to drive electrons from the electrocatalyst surface to reactant will decrease, which activates the 2H‐MoS₂ thermodynamically.     

Coupling Interface Constructions of MoS2/Fe5Ni4S8 Heterostructures for Efficient Electrochemical Water Splitting

Water splitting is considered as a pollution‐free and efficient solution to produce hydrogen energy. Low‐cost and efficient electrocatalysts for the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) are needed. Recently, chemical vapor deposition is used as an effective approach to gain high‐quality MoS₂ nanosheets (NSs), which possess excellent performance for water splitting comparable to platinum. Herein, MoS₂ NSs grown vertically on FeNi substrates are obtained with in situ growth of Fe₅Ni₄S₈ (FNS) at the interface during the synthesis of MoS₂. The synthesized MoS₂/FNS/FeNi foam exhibits only 120 mV at 10 mA cm^?2 for HER and exceptionally low overpotential of 204 mV to attain the same current density for OER. Density functional theory calculations further reveal that the constructed coupling interface between MoS₂ and FNS facilitates the absorption of H atoms and OH groups, consequently enhancing the performances of HER and OER. Such impressive performances herald that the unique structure provides an approach for designing advanced electrocatalysts.     

Construction of Defect‐Rich Ni‐Fe‐Doped K0.23MnO2 Cubic Nanoflowers via Etching Prussian Blue Analogue for Efficient Overall Water Splitting

Designing elaborate nanostructures and engineering defects have been promising approaches to fabricate cost‐efficient electrocatalysts toward overall water splitting. In this work, a controllable Prussian‐blue‐analogue‐sacrificed strategy followed by an annealing process to harvest defect‐rich Ni‐Fe‐doped K_0.23MnO₂ cubic nanoflowers (Ni‐Fe‐K_0.23MnO₂ CNFs‐300) as highly active bifunctional catalysts for oxygen and hydrogen evolution reactions (OER and HER) is reported. Benefiting from many merits, including unique morphology, abundant defects, and doping effect, Ni‐Fe‐K_0.23MnO₂ CNFs‐300 shows the best electrocatalytic performances among currently reported Mn oxide‐based electrocatalysts. This catalyst affords low overpotentials of 270 (320) mV at 10 (100) mA cm^?2 for OER with a small Tafel slope of 42.3 mV dec^?1, while requiring overpotentials of 116 and 243 mV to attain 10 and 100 mA cm^?2 for HER respectively. Moreover, Ni‐Fe‐K_0.23MnO₂ CNFs‐300 applied to overall water splitting exhibits a low cell voltage of 1.62 V at 10 mA cm^?2 and excellent durability, even superior to the Pt/C||IrO₂ cell at large current density. Density functional theory calculations further confirm that doping Ni and Fe into the crystal lattice of δ‐MnO₂ can not only reinforce the conductivity but also reduces the adsorption free‐energy barriers on the active sites during OER and HER.     

Metal–Carbon Hybrid Electrocatalysts Derived from Ion‐Exchange Resin Containing Heavy Metals for Efficient Hydrogen Evolution Reaction

Transition metal–carbon hybrids have been proposed as efficient electrocatalysts for hydrogen evolution reaction (HER) in acidic media. Herein, effective HER electrocatalysts based on metal–carbon composites are prepared by controlled pyrolysis of resin containing a variety of heavy metals. For the first time, Cr₂O₃ nanoparticles of 3–6 nm in diameter homogeneously dispersed in the resulting porous carbon framework (Cr–C hybrid) is synthesized as efficient HER electrocatalyst. Electrochemical measurements show that Cr–C hybrids display a high HER activity with an onset potential of ?49 mV (vs reversible hydrogen electrode), a Tafel slope of 90 mV dec^?1, a large catalytic current density of 10 mA cm^?2 at ?123 mV, and the prominent electrochemical durability. X‐ray photoelectron spectroscopic measurements confirm that electron transfer occurs from Cr₂O₃ into carbon, which is consistent with the reported metal@carbon systems. The obtained correlation between metals and HER activities may be exploited as a rational guideline in the design and engineering of HER electrocatalysts.     

Efficient Hydrogen Evolution Reaction Catalysis in Alkaline Media by All‐in‐One MoS2 with Multifunctional Active Sites

MoS₂ becomes an efficient and durable nonprecious‐metal electrocatalyst for the hydrogen evolution reaction (HER) when it contains multifunctional active sites for water splitting derived from 1T‐phase, defects, S vacancies, exposed Mo edges with expanded interlayer spacings. In contrast to previously reported MoS₂‐based catalysts targeting only a single or few of these characteristics, the all‐in‐one MoS₂ catalyst prepared herein features all of the above active site types. During synthesis, the intercalation of in situ generated NH₃ molecules into MoS₂ sheets affords ammoniated MoS₂ (A‐MoS₂) that predominantly comprises 1T‐MoS₂ and exhibits an expanded interlayer spacing. The subsequent reduction of A‐MoS₂ results in the removal of intercalated NH₃ and H₂S to form an all‐in‐one MoS₂ with multifunctional active sites mentioned above (R‐MoS₂) that exhibits electrocatalytic HER performance in alkaline media superior to those of all previously reported MoS₂‐based electrocatalysts. In particular, a hybrid MoS₂/nickel foam catalyst outperforms commercial Pt/C in the practically meaningful high‐current region (>25 mA cm^?2), demonstrating that R‐MoS₂‐based materials can potentially replace Pt catalysts in practical alkaline HER systems.     

Ruthenium Nanoparticles on Cobalt‐Doped 1T′ Phase MoS2 Nanosheets for Overall Water Splitting

2D MoS₂ nanostructures have recently attracted considerable attention because of their outstanding electrocatalytic properties. The synthesis of unique Co–Ru–MoS₂ hybrid nanosheets with excellent catalytic activity toward overall water splitting in alkaline solution is reported. 1T′ phase MoS₂ nanosheets are doped homogeneously with Co atoms and decorated with Ru nanoparticles. The catalytic performance of hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is characterized by low overpotentials of 52 and 308 mV at 10 mA cm^?2 and Tafel slopes of 55 and 50 mV decade^?1 in 1.0 m KOH, respectively. Analysis of X‐ray photoelectron and absorption spectra of the catalysts show that the MoS₂ well retained its metallic 1T′ phase, which guarantees good electrical conductivity during the reaction. The Gibbs free energy calculation for the reaction pathway in alkaline electrolyte confirms that the Ru nanoparticles on the Co‐doped MoS₂ greatly enhance the HER activity. Water adsorption and dissociation take place favorably on the Ru, and the doped Co further catalyzes HER by making the reaction intermediates more favorable. The high OER performance is attributed to the catalytically active RuO₂ nanoparticles that are produced via oxidation of Ru nanoparticles.     

Unique 1D Cd1−xZnxS@O‐MoS2/NiOx Nanohybrids: Highly Efficient Visible‐Light‐Driven Photocatalytic Hydrogen Evolution via Integrated Structural Regulation

Development of noble‐metal‐free photocatalysts for highly efficient sunlight‐driven water splitting is of great interest. Nevertheless, for the photocatalytic H₂ evolution reaction (HER), the integrated regulation study on morphology, electronic band structures, and surface active sites of catalyst is still minimal up to now. Herein, well‐defined 1D Cd_1?xZn_xS@O‐MoS₂/NiO_x hybrid nanostructures with enhanced activity and stability for photocatalytic HER are prepared. Interestingly, the band alignments, exposure of active sites, and interfacial charge separation of Cd_1?xZn_xS@O‐MoS₂/NiO_x are optimized by tuning the Zn‐doping content as well as the growth of defect‐rich O‐MoS₂ layer and NiO_x nanoparticles, which endow the hybrids with excellent HER performances. Specifically, the visible‐light‐driven (>420 nm) HER activity of Cd_1?xZn_xS@O‐MoS₂/NiO_x with 15% Zn‐doping and 0.2 wt% O‐MoS₂ (CZ_0.15S‐0.2M‐NiO_x) in lactic acid solution (66.08 mmol h^?1 g^?1) is about 25 times that of Pt loaded CZ_0.15S, which is further increased to 223.17 mmol h^?1 g^?1 when using Na₂S/Na₂SO₃ as the sacrificial agent. Meanwhile, in Na₂S/Na₂SO₃ solution, the CZ_0.15S‐0.2M‐NiO_x sample demonstrates an apparent quantum yield of 64.1% at 420 nm and a good stability for HER under long‐time illumination. The results presented in this work can be valuable inspirations for the exploitation of advanced materials for energy‐related applications.     

Precursor‐Transformation Strategy Preparation of CuPx Nanodots–Decorated CoP3 Nanowires Hybrid Catalysts for Boosting pH‐Universal Electrocatalytic Hydrogen Evolution

The development of earth‐abundant, low cost, and versatile electrocatalysts for producing hydrogen from water electrolysis is still challenging. Herein, based on high hydrogen evolution reaction (HER) activity of transition metal phosphides, a CoP₃ nanowire decorated with copper phosphides (denoted as CuP_x) nanodots structures synthesized through a simple and easily scalable precursor‐transformation strategy is reported as a highly efficient HER catalyst. By decorating with CuP_x nanodots, the optimized CoP₃ nanowires electrode exhibits excellent catalytic activity and long‐term durability for HER in alkaline conditions, achieving a low overpotential of 49.5 mV at a geometrical catalytic current density of 10 mA cm^?2 with a small Tafel slope of 58.0 mV dec^?1, while also performing quite well in neutral and acidic media. Moreover, its overall performance exceeds most of the reported state‐of‐the‐art catalysts, especially under high current density of 100 mA cm^?2, demonstrating its potential as a promising versatile pH universal electrocatalyst for efficient water electrolysis. These results indicate that the incorporation of earth‐abundant stable element copper can significantly enhance catalytic activity, which widens the application range of copper and provides a new path for design and selection of HER catalysts.     

Hierarchical Nanorods of MoS2/MoP Heterojunction for Efficient Electrocatalytic Hydrogen Evolution Reaction

Hierarchical nanostructures with tailored component and architectures are attractive for energy‐related applications. Here, the delicate design and construction of hierarchical MoS₂/MoP (H‐MoS₂/MoP) nanorods for the hydrogen evolution reaction (HER) are demonstrated. This multiscale design rationally combines the compositional and structural advantages of MoS₂/MoP heterojunction into a hierarchical architecture, which can modulate electronic structure of S, remarkably facilitating the electrocatalytic HER. Benefitting from their unique architecture and electronic structure, the H‐MoS₂/MoP nanorods exhibit excellent performance for HER with ultralow overpotential of 92 mV at current density of 10 mA cm^?2 in 1 m KOH and high stability. This work not only provides an efficient approach to constructing hierarchical heterojunctions, but also a multiscale strategy for all‐round regulation of the electronic structure and hierarchical morphology of nanomaterials for energy‐related applications.