Performance Of MoS2 Research Articles

Oxophilic Tm‐Sites in MoS2 Trigger Thermodynamic Spontaneous Water Dissociation for Enhanced Hydrogen Evolution

Abstract2D MoS2 is acknowledged as a potential alternative to Pt‐based catalysts for hydrogen evolution reaction (HER) due to its suitable *H adsorption energy. However, the weak water adsorption capacity of MoS2 in an alkaline solution limits its performance improvement toward HER. Herein, a novel rare‐earth Tm single atoms decorated MoS2 (Tm SAs‐MoS2) catalyst is proposed, and the key role of Tm SAs on the enhanced HER performance of MoS2 is identified. It is verified that the Tm‐site in MoS2 contributes to the asymmetric [Mo‐S‐Tm] unit site, which serves as the electron donor to disturb the electronic state and accelerate electron accumulation at surrounding Mo‐S site. The obtained Tm SAs‐MoS2 exhibits significantly improved HER activity with a low overpotential of 80 mV at 10 mA cm−2, robust stability and good selectivity in alkaline solution compared with pure MoS2 and most MoS2‐based catalysts. In situ Raman and theoretical calculations prove that the oxophilic Tm in [Mo‐S‐Tm] unit sites significantly improves the migration and thermodynamic spontaneous dissociation of interfacial H2O molecules during HER by the Tm‐4f‐OH orbital overlap. Such [Tm‐S‐Mo] unit site allows the optimal G*H location of Tm SAs‐MoS2, which in turn reaches the apex of the theoretical HER volcano plot. This work is expected to open up new avenues for the design of novel alkaline HER catalysts and provide a valuable understanding of rare earth enhanced mechanisms.

Activating and optimizing the In-Plane interface of 1 T/2H MoS2 for efficient hydrogen evolution reaction

Implanting the octahedral phase (1 T) into the hexagonal phase (2H) of the molybdenum disulfide (MoS2) matrix is considered one of the effective methods to enhance hydrogen evolution reaction (HER) performances of MoS2. In this paper, hybrid 1 T/2H MoS2 nanosheets array was successfully grown on conductive carbon cloth (1 T/2H MoS2/CC) via facile hydrothermal method and the 1 T phase content in 1 T/2H MoS2 is regulated to gradually increase from 0 % to 80 %. 1 T/2H MoS2/CC with 75 % 1 T phase content exhibits optimal HER performances. The DFT calculation results show that S atoms in 1 T/2H MoS2 interface exhibit the lowest hydrogen adsorption Gibbs free energies (ΔGH*) compared with other sites. The improvement of HER performances are primarily attributed to activating the in-plane interface regions of the hybrid 1 T/2H MoS2 nanosheets. Furthermore, the relationship between 1 T MoS2 content in 1 T/2H MoS2 and catalytic activity was simulated by a mathematical model, which shows that the catalytic activity presents a trend of increasing and then decreasing with the increase of 1 T phase content.

Unlocking the Ultrahigh‐Current‐Density Hydrogen Evolution on 2H‐MoS2 via Simultaneous Structural Control across Seven Orders of Magnitude

AbstractMembers of transition metal dichalcogenides, particularly molybdenum disulfide, have been recognized as promising efficient and durable earth‐abundant catalysts for the hydrogen evolution reaction (HER). Despite the recent significant progress, the HER performance of MoS2 is still far from satisfactory, especially at high current densities. Here, a simultaneous multilevel structural control strategy is reported to cooperatively boost hydrogen evolution on 2H‐MoS2, unlocking its potential for practical hydrogen evolution at ampere‐level current densities. By confining the epitaxial growth of few‐layered, curved MoS2 nanosheets within a tubular mesoporous graphitic framework, one can achieve deliberate structural control of MoS2 across seven orders of magnitude on the length scale. The resulting MoS2@C supertubes, benefiting from their unique structural features across atomic‐to‐microscopic scales, are characterized by abundant edge sites and sulfur vacancies, facilitated charge and mass transport, and rapid gas bubble removal. As a consequence, such MoS2@C supertubes exhibit exceptional high‐current‐density HER activity surpassing previously reported 2H‐MoS2 catalysts and even commercial Pt/C catalysts. This work demonstrates the validity of multilevel structural engineering of 2H‐MoS2 by confinement growth, opening a viable route of developing low‐cost catalysts toward practical hydrogen evolution.

The electronic properties and water desalination performance of a photocatalytic TiO2/MoS2 nanocomposites bilayer membrane: a molecular dynamic simulation.

Due to the rapid depletion of water resources, more interest is paid for the efficient desalination process in recent years. MoS2 membrane aroused attention due to its high mechanical stability and electronic properties, which can sustain extra-large strains. In this study, the electronic properties and water desalination performance of TiO2/MoS2-hexagonal, and TiO2/MoS2-rhombohedral nanocomposites bilayer membranes were studied and simulated for the first time. The effect of TiO2 in the performance of MoS2 was observed in water desalination under the defined applied pressure ranging from 50 to 250MPa with a 6.4Å pore diameter. The membrane structure is created and optimized. The energy minimized for TiO2 from - 19,596.4282kcal/mol for the initial structure to - 19,605.1611kcal/mol for the final structure. For TiO2/MoS2-hexagonal, the energy minimized from - 4955.54271eV) to - 4955.62091eV and TiO2/MoS2-rhombohedral from - 6042.26925eV to - 6046.91835eV. A molecular dynamic (MD) simulation was performed using Material Studio 2019 to study the electronic properties under 0-1eV electric field using the CASTEP code. The results showed a better photocatalytic performance under the external electric field. The effect of external electric field significantly intensifies absorption in the visible range and achieved a high photocatalytic activity on TiO2/MoS2. TiO2, TiO2/MoS2-hexagonal and TiO2/MoS2-rhombohedral nanocomposites bilayer membranes are simulated and evaluated for the water desalination using ReaxFF software. Both MoS2 phases with TiO2 have achieved a high salt rejection up to 97% (P-value = 0.0036, R2 = 0.958), while TiO2/MoS2-rhombohedral achieved the highest permeability (6.0*10-8mmgcm-2s-1bar-1) (P-value = 0.000296, R2 = 0.972) under 250MPa applied pressure.

Modulating the Electronic Properties of MoS2 Nanosheets for Electrochemical Hydrogen Production: A Review

Benefiting from the low cost and excellent stability, transition metal dichalcogenides (TMDs) have been widely applied in electrocatalysis for hydrogen evolution. As a member of TMDs, molybdenum disulfide (MoS2) nanosheets exhibited excellence because of their S-edges with near optimal hydrogen adsorption free energy. However, the performance of MoS2 is affected by the inert basal surface and poor electron transfer ability. Various strategies have been reported. In this review, we systematically summarize the recent progress in regulating electronic structures of MoS2 for electrochemical hydrogen production and focus on the relationship between the intrinsic electronic structure and its electrocatalytic activity. We close this review with the challenges and outlook on MoS2 nanosheets as efficient and low-cost electrocatalysts, thereby providing helpful guidance for feasible design of efficient MoS2-based electrocatalysts for hydrogen production.

Catkin-derived mesoporous carbon-supported molybdenum disulfide and nickel hydroxyl oxide hybrid as a bifunctional electrocatalyst for driving overall water splitting

In this work, a two-dimensional heterostructure of molybdenum disulfide (MoS2) and nickelhydroxyloxide (NiOOH) nanosheets supported on catkin-derived mesoporous carbon (C-MC) was constructed and exploited as an efficient electrocatalyst for overall water splitting. The C-MC nanostructure was prepared by pyrolyzing biomass material of catkin at 600 °C in N2 atmosphere. The C-MC network exhibited hollow nanotube structure and had a large specific surface area, comprising trace nitrogen and a large amount of oxygen vacancies. It further served as the support for the growth of NiOOH nanosheets (NiOOH@C-MC), which was combined with MoS2 nanosheets by in situ growth, yielding a multicomponent electrocatalyst (MoS2@NiOOH@C-MC). By integrating the superior hydrogen evolution reaction (HER) performance of MoS2, oxygen evolution reaction (OER) performance of NiOOH, and the fast electron transfer capability of C-MC, the prepared MoS2@NiOOH@C-MC illustrated a low potential of − 250 mV for HER and 1.51 V for OER at the current density of 10 mV cm−2. Consequently, when applied as the working electrode for driving overall water splitting in a two-electrode system, the bifunctional MoS2@NiOOH@C-MC electrocatalyst displayed a low cell voltage of 1.62 V at the current density of 10 mA cm−2. The present work provides a new strategy that uses biomass material for developing bifunctional electrocatalyst for overall water splitting.

Effect of Modulation Periods on the Mechanical and Tribological Performance of MoS2–TiL/MoS2–TiH Multilayer Coatings

MoS2–Ti coating is a widely used solid lubricant owing to its low friction coefficient. The mechanical and tribological performance of the coating can be further improved via introducing a multilayer structure, which is closely related to the modulation period and significantly affects the properties of the coating. Herein, the effect of two different modulation periods on the mechanical and tribological performance of the MoS2–TiL/MoS2–TiH multilayer coatings (where L and H represent low and high-powered sputtering of the titanium target) was studied. The performance of the coatings was found to depend on modulation periods of single layer thickness and thickness ratio, respectively. When the thickness ratio of MoS2–TiL layer to MoS2–TiH layer was fixed with different number of layers, the adverse effects of the interface outweighed the beneficial effect; thus, the mechanical and tribological performance of the multilayer coatings were improved with an increase in the single layer thickness. When the effect of the multilayer interfaces on the studied coatings was similar with the same number of layers, the MoS2–TiH layer had more impact on the hardness of the MoS2–TiL/MoS2–TiH multilayer coatings, whereas the MoS2–TiL layer substantially affected the adhesion properties, friction behavior and wear resistance. This study can provide a way to regulate coatings with different performance requirements via building different multilayer microstructures.

Tuning the Intrinsic Activity and Electrochemical Surface Area of MoS2 via Tiny Zn Doping: Toward an Efficient Hydrogen Evolution Reaction (HER) Catalyst.

Molybdenum sulfide (MoS2 ) is considered as an alternative material for commercial platinum catalysts for electrocatalytic hydrogen evolution reaction (HER). Improving the apparent HER activity of MoS2 to a level comparable to that of Pt is an essential premise for the commercial use of MoS2 . In this work, a Zn-doping strategy is proposed to enhance the HER performance of MoS2 . It is shown that tiny Zn doping into MoS2 leads to the enhancement of the electrochemical surface area, increases in proportion of HER active 1T phase in the material and formation of catalytic sites of higher intrinsic activity. These benefits result in a high-performance HER electrocatalyst with a low overpotential of 190 mV(@10 mA cm-2 ) and a low Tafel slope of 58 mV dec-1 . The origin for the excellent electrochemical performance of the doped MoS2 is rationalized with both experimental and theoretical investigations.

Effects of nitrogen-doping structural changes of spherical hollow graphene on the growth of MoS2+x nanosheets and the enhanced hydrogen evolution reaction

MoS2, a two-dimensional (2D) layered structural transition metal dichalcogenide (TMDs), has been widely investigated towards hydrogen evolution reaction (HER) in previous few years. Except for the inert basal plane sites of the MoS2 itself, its inherent low conductivity also hinders the electron transfer process, which adversely affects its efficiency towards HER. Therefore, how to expose more edge active sites and at the same time improve the conductivity of MoS2, either intrinsically or with the help of high conductive substrates, is a key means to improve the HER performance of MoS2. Herein, the polystyrene (PS) nanospheres are used not only as an intercalation agent of graphene carbon sheets, but also as a spherical template for the preparation of 3D spherical hollow graphene. Different nitrogen precursors and nitrogen doping methods are used to prepare the 3D spherical hollow graphene substrate materials with different nitrogen-doping structures, such as amine N, pyrrolic N, pyridinic N or quaternary N. The investigation results show that the structure of doped nitrogen atom has a great influence on the loading of molybdenum disulfide. Among them, amine N was the most favorable for the loading of molybdenum disulfide, followed by pyrrole N, quaternary N and pyridine N. Moreover, the structure of doped N active sites synthesized by different preparation methods can also affect the uniform distribution of molybdenum disulfide on 3D spherical hollow graphene and the corresponding HER performance. The results show that, using ammonia as nitrogen source and PS microspheres as template, the prepared molybdenum disulfide loaded 3D spherical hollow graphene electrode material has the best HER performance, which should be attributed to the uniform distribution of the molybdenum disulfide and its close combination with the substrate, as well as the 3D spherical hollow structure. Moreover, the amorphous structure of molybdenum disulfide formed in the hydrothermal process can also improve the activity of HER.

Photoelectrochemical performance of P@MoS2 for hydrogen evolution reaction

Hydrogen production through water splitting could be a splendid technique as an alternative to fossil fuel derived methods. Recently, molybdenum disulfide (MoS2) has gained great attention for electrocatalytic HER. Nevertheless, the catalytic activity of MoS2 was limited by poor active sites with higher intrinsic activity. The present work correlates the enhancement on the performance of MoS2 was done by doping with phosphorus that contribute for the higher activity of hydrogen evolution reaction (HER). During light irradiation, the phosphorus doped MoS2 (P@MoS2) possessed lowest overpotential (134 mV) and smallest Tafel slope (86 mV/dec) in contrast to bulk MoS2 thereby propitious for HER activities. Thus, the highly effective P@MoS2 nanocomposite could be a remarkable candidate that reassuring the growth of hydrogen production regimes.

One-step construction of sulfide heterostructures with P doping for efficient hydrogen evolution

Molybdenum disulfide (MoS2) exhibits the modest properties toward hydrogen evolution due to its poor electrical conductivity and a limited number of active sites. To make up for the defects in MoS2, we built hierarchical P-doped MoS2/NiS2@carbon hollow nanospheres (P–MoS/NiS@CHNS) electrocatalyst via one-step hydrothermal method owning to the priority of the reaction between Ni2+ and H2S. Motivated by high-efficient electron transfer at the interface of heterostructure and the activation of MoS2 by P dopant, P–MoS/NiS@CHNS exhibits optimal Gibbs free energies (ΔGH∗) and superior HER performance with low overpotential (ƞ10) of 110 ​mV ​at 10 ​mA ​cm−2 and small Tafel slope of 61 ​mV dec−1. The focus of this work is to optimize the HER performance of MoS2 through P-doping and heterostructure construction, which can further provide a reference for the design of MoS2 based catalysts.

First-principles study of sulfur vacancy concentration effect on the electronic structures and hydrogen evolution reaction of MoS2

Defect engineering has been widely used in experiments to modulate the electrocatalytic properties of molybdenum disulfide (MoS2). However, the effect of vacancy concentration on the vacancy distribution, electronic properties, and hydrogen evolution reaction (HER) activity remains elusive. Herein, we perform density functional theory (DFT) studies to investigate defective MoS2 with different numbers of sulfur vacancies. In the case of low S-vacancy concentration, the vacancies prefer to agglomerate rather than being dispersed, while at the higher-vacancy concentration, the combination of local point defect and clustered vacancy chain is preferred. The coupling between S-vacancies leads to decreased band gap and increased Mo–H adsorption strength with increasing vacancy concentration. The optimal HER activity is identified to occur below vacancy concentration of 12.50%. Our work provides an atomic-level understanding about the role of S-vacancies in the HER performance of MoS2, and offers useful guidelines for the design of defective MoS2 and other TMDs electrocatalysts.

Ni–Mo–S Ternary Chalcogenide Thin Film for Enhanced Hydrogen Evolution Reaction

Transition metal dichalcogenides (TMDs) hold a great promise to replace Pt-based catalysts for hydrogen evolution reaction (HER). Among those, MoS2 has been the center of attention. In this work, we investigate the effect of Ni addition on the catalytic activity of MoS2 thin film in HER. Ni–Mo–S ternary chalcogenide thin films with varying Ni concentrations were fabricated by a two-step process: co-sputtering of Ni-Mo alloy films and thermal sulfurization. The HER performance of MoS2 (620 mV overpotential and 138 mV dec−1 Tafel slope) is surpassed by the resulting ternary chalcogenides, among which the Ni–Mo–S film at 50 at.% Ni concentration exhibits the highest catalytic activity with an overpotential of 400 mV at 10 mA cm−2 and Tafel slope of 81 mV dec−1. The Ni addition promotes HER kinetics by altering the morphology and electronic structure of MoS2 thin film, leading to improved H+ ion adsorption, reduced charge transfer resistance and increased electrochemical surface area. This study provides a method for the controllable fabrication of ternary chalcogenide thin films and paves the way for the exploration of new combinations of ternary TMDs.

Boosting magnesium storage in MoS2via a 1T phase introduction and interlayer expansion strategy: theoretical prediction and experimental verification

The Mg-storage performance of MoS2 is enhanced by 1T phase introduction and interlayer-expansion.

Fabrication of MoS2/ZnO Hybrid Nanostructures for Enhancing Photodetection

In this article, the effect of MoS <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> and ZnO blend ratio on the performance of MoS <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> :ZnO hybrid photodiodes is investigated. The UV and visible performance parameters for five different devices consisting of semiconducting layers like MoS <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> , ZnO, MoS <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> :ZnO (1:1), MoS <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> :ZnO (1:2), and MoS <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> :ZnO (2:1) each are analyzed. The device MoS2:ZnO (1:2) shows the best performance in the UV region with a responsivity of 17.04 A/W, detectivity of 6.84 × 10 <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">13</sup> Jones and external quantum efficiency (EQE) of 6604% at 320nm, -1 V bias. On the other hand, the device MoS <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> :ZnO (2:1) gives the best performance in the visible region with a responsivity of 2.27 A/W, detectivity of 0.60 × 1013 Jones, and EQE of 533% at 529nm, -1 V.

Growth of Multiorientated Polycrystalline MoS2 Using Plasma-Enhanced Chemical Vapor Deposition for Efficient Hydrogen Evolution Reactions.

Molybdenum disulfide (MoS2) has attracted considerable attention as a promising electrocatalyst for the hydrogen evolution reaction (HER). However, the catalytic HER performance of MoS2 is significantly limited by the few active sites and low electrical conductivity. In this study, the growth of multiorientated polycrystalline MoS2 using plasma-enhanced chemical vapor deposition (PECVD) for the HER is achieved. The MoS2 is synthesized by sulfurizing a sputtered pillar-shaped Mo film. The relatively low growth temperature during the PECVD process results in multiorientated MoS2 with an expanded interlayer spacing of ~0.75 nm, which provides abundant active sites, a reduced Gibbs free energy of H adsorption, and enhanced intralayer conductivity. In HER applications, the PECVD-grown MoS2 exhibits an overpotential value of 0.45 V, a Tafel slope of 76 mV dec−1, and excellent stability in strong acidic media for 10 h. The high HER performance achieved in this study indicates that two-dimensional MoS2 has potential as an electrocatalyst for next-generation energy technologies.

Positive and Negative Effects of Dopants toward Electrocatalytic Activity of MoS2 and WS2: Experiments and Theory.

Two-dimensional transition-metal dichalcogenides (TMDs) are lately in the scope within the scientific community owing to their exploitation as affordable catalysts for next-generation energy devices. Undoubtedly, only precise tailoring and control over the catalytic properties can ensure high efficiency and successful implementation of such devices in day-to-day practical utilization. However, contrary to theoretical predictions, systematic experimental work dealing with the doped materials and their impact to electrocatalysis are relatively underrated despite the considerable effect that it could bring into this field. Herein, we investigate the effect of four different dopants (i.e., Ti, V, Mn, and Fe) incorporated to both layered MoS2 and WS2 as solid-state solution toward their electrocatalytic performance through their evaluation as catalysts for oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER). Our results pointed out that doping by Mn and Fe can enhance the electrocatalytic performance toward ORR, whereas doping by Ti and V revealed poor electrocatalytic effects (inhibition) compared to both undoped MoS2 and WS2. Surprisingly, none of the dopants contributed to the improvement of either MoS2 or WS2 toward HER activity. Therefore, in addition to the experimental data, density functional theory calculations were performed to further investigate the role of the dopants in the performance of MoS2 toward HER. According to these calculations, all dopants preferably occupied the edges of the crystal structure and thus could affect the electrocatalytic properties of the initial material. However, the observed ΔG values for hydrogen adsorption revealed that MoS2 is the best catalyst with a subsequent trend for doped materials following the less negative binding energies V < Ti < Mn < Fe, which was in good agreement with experimentally obtained overpotentials of the respective samples. This study thus elucidates the reasons for negative effects of doping in TMDs. This study brings an insight that not all dopants are beneficial and not all reactions are affected in the same way by dopants in TMDs.

Strong interfacial interaction significantly improving hydrogen evolution reaction performances of MoS2/Ti4O7 composite catalysts

A catalytic non-carbon composite composed of molybdenum disulfide (MoS2) and conducting Magnéli phase Ti4O7 is firstly synthesized by a facile hydrothermal method. The MoS2/Ti4O7 composite catalyst shows significantly improved hydrogen evolution reaction (HER) activity in 0.5 M H2SO4 especially at high overpotentials mainly due to the fast electron transfer ability caused by the newly formed interfacial S–O–Ti bonds and the enhanced electrochemical surface area. Tafel slope of the optimized MoS2/Ti4O7 catalyst is as low as 48 mV · dec−1. It also presents an impressive stability with smaller activity degradation (5 mV potential shift at 10 mA cm−2) after 1000 cycles of cyclic voltammetry (CV) scanning. This is the first exploration on HER performances of MoS2 and conductive metal oxide composite electrocatalysts, shedding light on the research of non-noble metal (sulphide)-metal oxide interface in energy catalysis significantly crucial for the development of cost-effective and stable HER electrocatalysts and even other electrocatalytic materials.

Three-dimensionally hierarchical MoS2/graphene architecture for high-performance hydrogen evolution reaction

Molybdenum disulfide (MoS2) has been considered as a potential alternative to precious metal catalysts for the hydrogen evolution reaction (HER). However, the performance of MoS2 is still limited due to the poor electron conductivity, scarce active sites and low structural stability. A multiscale design of MoS2 in the structure and atomic composition is needed but still a great challenge. Herein, we report a well-organized three-dimensionally (3D) mesoporous hybrid structure of Co-doped MoS2 and graphene for highly efficient electrocatalytic HER. The mesoporous morphology ensures the well-dispersion of MoS2 layers and exposure of abundant edge sites. Doping of Co atoms into the MoS2 lattice improves the intrinsic HER activity of in-plane sulfur sites. The highly conductive and robust graphene network enhances the conduction of electrons and simultaneously improves the stability of the hybrid structure. The catalyst achieves a current density of 10 mA cm−2 at an overpotential of 143 mV versus the reversible hydrogen electrode (RHE) which is 200 mV lower compared with pure 2D MoS2, and maintains the activity for over 5000 cyclic voltammetry sweeps. This work provides a promising strategy for efficiently enhancing both the activity and stability of MoS2-based catalyst for HER.

P doped MoS2 nanoplates embedded in nitrogen doped carbon nanofibers as an efficient catalyst for hydrogen evolution reaction

Two-dimensional (2D) molybdenum sulfide (MoS2) is considered as a promising catalyst for hydrogen evolution reaction (HER), originated from its abundant hydrogen evolution active sites. However, the HER performance of MoS2 is currently hindered by the limited exposed density of the active sites and low conductivity. Herein, we report a facile and scalable electrospinning technique to fabricate 2D MoS2 nanoplates doped with phosphorus within one-dimensional nitrogen doped-carbon nanofibers (NCNFs-MoS2|P) as a highly efficient HER catalyst. The space-confined growth with the presence of NCNFs avoided the stacking and aggregation of the MoS2 nanoplates, resulting in more exposed edge sites. The introduction of phosphorus atoms further activated the surface of MoS2 and enhanced the electron transfer. The overpotential of NCNFs-MoS2|P reached 98 mV at 10 mA cm−2, exhibiting excellent HER catalytic activity. Besides, almost no decay was observed after the stability test (5000 cycles or 20 h). The density functional calculations (DFT) elucidated that the incorporation of phosphorus atoms significantly improved the electrical conductivity and decreased the H adsorption energy barrier on MoS2, leading to a high catalytic performance of NCNFs-MoS2|P.