Enhanced Hydrogen Evolution Reaction Activity Research Articles

Surface Termination (-O, -F or -OH) and Metal Doping on the HER Activity of Mo2CTx MXene.

Two-dimensional MXenes have recently garnered significant attention as electrocatalytic materials for hydrogen evolution reaction (HER). However, previous theoretical studies mainly focused on the effect of pure functional groups while neglecting hybrid functional groups that are commonly observed in experiments. Herein, we investigated the hybrid functionalized Mo2CTx MXene (T = -O, -F or -OH) to probe the HER properties. In binary O/F co-functionalization, the presence of F groups would attenuate the H adsorption and lead to the enhanced HER activity than the fully O-terminated Mo2CO2. However, the surface HER activity of ternary O/F/OH functionalized Mo2CTx is not satisfactory owing to the relatively weak H adsorption capacity. To further enhance the catalytic activity, modification was performed by introducing another metal element into its lattice structure. The doped metal (Fe, Co, Ni, Cu) exhibits reduced charge transfer to O compared to Mo atoms, leading to enhanced H adsorption and improved overall activity. The synergistic effect of hybrid functionalization and TM modification provides useful guidance for achieving feasible Mo2CTx candidates with high HER performance, which can be applied to the electrocatalytic applications of other MXenes.

Cost-efficient sunlight-driven thermoelectric electrolysis over Mo-doped Ni5P4 nanosheets for highly efficient alkaline water/seawater splitting

Thermoelectric water spitting to hydrogen systems has great potential in the production of environment-friendly fuel using renewable solar energy in the future. In this work, we prepared porous nanosheet Mo doping Ni5P4 catalysts on nickel foam with efficient hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) performance in alkaline media. Density Functional Theory (DFT) calculations and experimental studies have shown that Mo doping deadeneds the interaction between H and O atomic orbitals of transition state water molecules, effectively weakening the activation energy of H2O dissociation. Therefore, Mo doping is favorable for enhancing HER activity with overpotential at 10 mA cm–2 of 93 mV and Tafel slope of 40.1 mV dec–1 in 1 M KOH. Besides, it exhibits high alkaline OER activity with an ultra-low overpotential of 200 mV at 10 mA cm–2. Moreover, this catalyst only needs 1.537 V in a dual-electrode configuration of the electrolytic cell, which is much lower than the commercial Pt/C-RuO2 couple (1.614 V). In addition, we have developed and constructed a solar thermoelectric generator (TEG) that is capable of floating on water. This TEG has a continuous power output and an exceptionally long lifespan, providing a stable power supply to the synthesized catalyst electrolyzer. It can produce a maximum power output of over 90 mW, meeting the requirement of converting solar radiation heat into usable electricity. As a result, the system achieves productivity of 0.11 mL min–1 H2. This solar thermal energy conversion technology shows the possibility of large-scale industrial production of H2 and provides a new idea for exploring heat source utilization.

Manipulating heterointerface to boost formation and desorption of intermediates for highly efficient alkaline hydrogen evolution

Promoting water dissociation and H intermediate desorption play a pivotal role in achieving highly efficient hydrogen evolution reaction (HER) in alkaline media but remain a great challenge. Herein, we rationally develop a unique W-doped NiSx/Ni heterointerface as a favorable HER electrocatalyst which was directly grown on the Cu nanowire foam substrate (W-NiSx/Ni@Cu) by the electrodeposition strategy. Benefiting from the rational design of the interfaces, the electronic coupling of the W-NiSx/Ni@Cu can be efficiently modulated to lower the HER kinetic barrier. The obtained W-NiSx/Ni@Cu exhibits an enhanced HER activity with a low overpotential of 38 mV at 10 mA cm−2 and a small Tafel value of 27.5 mV dec−1, and high stability during HER catalysis. In addition, in-situ Raman spectra reveal that the Ni2+ active sites preferentially adsorb OH intermediate. The theoretical calculation confirms that the water dissociation is accelerated by the construction of W-NiSx/Ni heterointerface and H intermediate desorption can be also promoted by H spillover from S active sites in W-NiSx to Ni active sites in metal Ni. This work offers a valuable reference for rational designing heterointerface of electrocatalysts and provides an available method to accelerate the HER kinetics for the ampere-level current density under low overpotential.

Thermal Shock Synthesis for Loading Sub-2nm Ru nanoclusters on Titanium Nitride as a Remarkable Electrocatalyst towards Hydrogen Evolution Reaction.

Heterogeneous catalysts embracing metal entities on suitable supports are profound in catalyzing various chemical reactions, and substantial synthetic endeavors in metal-support interaction modulation have been made to enhance catalytic performance. Here, it is reported the loading of sub-2nm Ru nanocrystals (NCs) on titanium nitride support (HTS-Ru-NCs/TiN) via a special Ru-Ti interaction using high temperature shock (HTS) method. Direct dechlorination of the adsorbed RuCl3, ultrafast nucleation process and short coalescence duration at ultrahigh temperatures contribute to the immobilization of Ru NCs on TiN support via producing the Ru-Ti interfacial perimeter. HTS-Ru-NCs/TiN shows remarkable activity towards hydrogen evolution reaction (HER) in alkaline solution, yielding ultralow overpotentials of 16.3 and 86.6mV to achieve 10 and 100mAcm-2, respectively. The alkaline and anion exchange membrane water electrolyzers assembled using HTS-Ru-NCs/TiN yield 1.0Acm-2 at 1.65 and 1.67V, respectively, which validate its applicability in hydrogen production industry. Theoretical simulations reveal the favorable formation of Ru-O and Ti-H bond at the interfacial perimeters between Ru NCs and TiN, which accelerates the prerequisite water dissociation kinetics for the enhanced HER activity. This exemplified work motivates the design of specific interfacial perimeters via the HTS strategy to improve the performance of diverse catalysis. This article is protected by copyright. All rights reserved.

Synergistic engineering of palladium-cobalt nanoalloys on graphite sheet for efficient and sustainable hydrogen evolution reaction

The electrochemical hydrogen evolution reaction (HER)—a carbon-free route for hydrogen (H2) production—is of the utmost importance for H2-economy. Currently, HER performance is mainly restricted by the lack of promising alternatives to Pt-based electrocatalysts. In this study, we developed bimetallic PdCo alloy thin films with outstanding catalytic properties for the HER under acidic conditions. A simple aerosol-assisted chemical vapor deposition technique designed in-house was used to produce bimetallic alloy thin films on graphite sheets. The thin-film morphological patterns were significantly changed by varying the deposition time from 30 to 90 min. The optimized PdCo catalyst deposited for 30 min had a unique nanostructure with numerous active sites and exhibited faster HER kinetics than its analogs and pure Pd. As-prepared PdCo-30 electrode produced current densities of 10 and 1000 mA cm−2 at overpotentials of 41 and 161 mV, respectively, along with a Tafel slope of 42 mV/dec, high conductivity (0.28 Ω), and catalytic stability of ∼24 h in 0.5 M H2SO4. The excellent HER activity of the PdCo alloy was attributed to the synergy between the noble transition metal and the thin nanostructured layer of the bimetallic catalyst, which promoted formation of extensive electroactive sites on the conductive graphite surface. Density functional theory calculations confirmed the experimental findings. The Gibbs free energy (ΔGH*) of the PdCo alloy (−0.43 eV) was significantly lower than that of pure Pd (−0.57 eV), confirming the enhancement in HER activity due to the introduction of Co into the Pd lattice.

In-situ fabrication of self-supported cobalt molybdenum sulphide on carbon paper for bifunctional water electrocatalysis

The fabrication of highly efficient yet stable noble-metal-free bifunctional electrocatalysts that can simultaneously catalyse both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) remains challenging. Herein, we employ the heterostructure coupling strategy, showcasing an aerosol-assisted chemical vapour deposition (AACVD) aided synthetic approach for the in-situ growth of cobalt molybdenum sulphide nanocomposites on carbon paper (CoMoS@CP) as a bifunctional electrocatalyst. The AACVD allows the rational incorporation of Co in the Mo–S binary structure, which modulates the morphology of CoMoS@CP, resulting in enhanced HER activity (ŋ10 = 171 mV in acidic and ŋ10 = 177 mV in alkaline conditions). Furthermore, the CoS2 species in the CoMoS@CP ternary structure extends the OER capability, yielding an ŋ100 of 455 mV in 1 M KOH. Lastly, we found that the synergistic effect of the Co–Mo–S interface elevates the bifunctional performance beyond binary counterparts, achieving a low cell voltage (1.70 V at 10 mA cm−2) in overall water splitting test and outstanding catalytic stability (∼90 % performance retention after 50-/30-h continuous operation at 10 and 100 mA cm−2, respectively). This work has opened up a new methodology for the controllable synthesis of self-supported transition metal-based electrocatalysts for applications in overall water splitting.

Regulation of the d-band center of metal–organic frameworks for energy-saving hydrogen generation coupled with selective glycerol oxidation

The hybrid electrolyzer coupled glycerol oxidation (GOR) with hydrogen evolution reaction (HER) is fascinating to simultaneously generate H2 and high value-added chemicals with low energy input, yet facing a challenge. Herein, Cu-based metal-organic frameworks (Cu-MOFs) are reported as model catalysts for both HER and GOR through doping of atomically dispersed precious and nonprecious metals. Remarkably, the HER activity of Ru-doped Cu-MOF outperformed a Pt/C catalyst, with its Faradaic efficiency for formate formation at 90% at a low potential of 1.40 V. Furthermore, the hybrid electrolyzer only needed 1.36 V to achieve 10 mA cm-2, 340 mV lower than that for splitting pure water. Theoretical calculations demonstrated that electronic interactions between the host and guest (doped) metals shifted downward the d-band centers (εd) of MOFs. This consequently lowered water adsorption and dissociation energy barriers and optimized hydrogen adsorption energy, leading to significantly enhanced HER activities. Meanwhile, the downshift of εd centers reduced energy barriers for rate-limiting step and the formation energy of OH*, synergistically enhancing the activity of MOFs for GOR. These findings offered an effective means for simultaneous productions of hydrogen fuel and high value-added chemicals using one hybrid electrolyzer with low energy input.

Interfacial Design of Ti3C2Tx MXene/Graphene Heterostructures Boosted Ru Nanoclusters with High Activity Toward Hydrogen Evolution Reaction.

The development of a cost-competitive and efficient electrocatalyst is both attractive and challenging for hydrogen production by hydrogen evolution reaction (HER). Herein, a facile glycol reduction method to construct Ru nanoclusters coupled with hierarchical exfoliated-MXene/reduced graphene oxide architectures (Ru-E-MXene/rGA) is reported. The hierarchical structure, formed by the self-assembly of graphene oxides, can effectively prohibit the self-stacking of MXene nanosheets. Meanwhile, the formation of the MXene/rGA interface can strongly trap the Ru3+ ions, resulting in the uniform distribution of Ru nanoclusters within Ru-E-MXene/rGA. The boosted catalytic activity and underlying catalytic mechanism during the HER process are proved by density functional theory. Ru-E-MXene/rGA exhibits overpotentials of 42 and 62mV at 10mAcm-2 in alkaline and acidic electrolytes, respectively. The small Tafel slope and charge transfer resistance (Rct) values elucidate its fast dynamic behavior. The cyclic voltammetry (CV) curves and chronoamperometry test confirm the high stability of Ru-E-MXene/rGA. These results demonstrate that coupling Ru nanoclusters with the MXene/rGA heterostructure represents an efficient strategy for constructing MXene-based catalysts with enhanced HER activity.

Introducing active sites and regulating electron distribution to design Mo and P co-doped Ni for efficient alkaline hydrogen evolution reaction

NiMoP electrocatalysts for hydrogen evolution reaction (HER) are received widespread concern, but the mechanism of Mo/P atoms for improving the HER activity still need to be revealed in details. Herein, we synthesize the Mo/P co-doped Ni (NMP) electrocatalysts, and the alkaline HER performances are tested. The NMP exhibit the excellent activity, durability and stability of material characters. Based on the results of experiments and density functional theory calculations, it is found that the introduced P atoms can regulate the electron redistribution, which can result in enhancing the reaction kinetic, increasing the active sites and charge exchange capacity. Besides, it leads the doped Mo to become the active site in both Volmer and Heyrovsky processes, and Ni bonded to Mo and Ni atoms exhibit the increasing activity. The obtained results display a deeper understanding for the doped metal and non-metallic atoms in enhancing HER activity of Ni, which is of great significant for designing the highly efficient and inexpensive electrocatalysts for producing hydrogen.

Titanium Dioxide and N-Doped Carbon Hybrid Nanofiber Modulated Ru Nanoclusters for High-Efficient Hydrogen Evolution Reaction Electrocatalyst.

The designing and fabricating highly active hydrogen evolution reaction (HER) electrocatalysts that can superior to Pt/C is extremely desirable but challenging. Herein, the fabrication of Ru/TiO2/N-doped carbon (Ru/TiO2/NC) nanofiber is reported as a novel and highly active HER electrocatalyst through electrospinning and subsequent pyrolysis treatment, in which Ru nanoclusters are dispersed into TiO2/NC hybrid nanofiber. As a novel support, experimental and theoretical calculation results reveal that TiO2/NC can more effectively accelerate water dissociation as well as optimize the adsorption strength of *H than TiO2 and NC, thus leading to a significantly enhanced HER activity, which merely requires an overpotential of 18mV to reach 10mAcm-2, outperforming Pt/C in an alkaline solution. The electrolytic cell composed of Ru/TiO2/NC nanofiber and NiFe LDH/NF can generate 500 and 1000mAcm-2 at voltages of 1.631 and 1.753V, respectively. Furthermore, the electrolytic cell also exhibits remarkable durability for at least 100h at 200mAcm-2 with negligible degradation in activity. The present work affords a deep insight into the influence of support on the activity of electrocatalyst and the strategy proposed in this research can also be extended to fabricate various other types of electrocatalysts for diverse electrocatalytic applications.

Structural regulation of amorphous molybdenum sulfide by atomic palladium doping for hydrogen evolution

Molybdenum sulfide materials have long been considered as attractive non-precious-metal electrocatalysts for the hydrogen evolution reaction (HER). However, comparing with the crystalline counterpart, amorphous MoSx has been less investigated previously. We here propose to increase the catalytical activity of a-MoSx by raising the reactant concentration at the catalytic interface via a chemical doping approach. The reconstruction of coordination structure of a-MoSx via Pd doping induces the formation of abundant unsaturated S atoms. Moreover, the reactant friendly catalytic interface is constructed through introducing hydrophilic groups to a-MoSx. The doped a-MoSx catalyst exhibits significantly enhanced HER activity in both acid and alkaline media.

RuSe2 nanoparticles loaded MoSe2 hybrid rods via interface engineering as an efficient electrocatalyst for hydrogen evolution electrocatalysis

Despite being regarded as a favorable substitute for platinum-based catalysts in hydrogen evolution reaction (HER), molybdenum diselenide (MoSe2) exhibits inferior electrocatalytic performance due to its inadequate conductivity and limited active sites. However, employing molecular engineering for modification holds great potential in significantly enhancing its performance, yet it still poses significant challenges. Herein, an interface engineering strategy was adopted to obtain RuSe2 modified MoSe2 composite catalysts (RuSe2/MoSe2). In alkaline media, RuSe2/MoSe2 exhibited a reduced overpotential of 147.8 mV at 10 mA cm−2 comparing with pristine MoSe2 (351.8 mV). Experimental findings and density functional theory (DFT) calculations indicated that increased conductivity, enhanced hydrophily and optimized adsorption free energies of hydrogen contribute to its enhanced HER activity. This work opens up an interface engineering strategy for designing more efficient selenide-based electrocatalysts.

Porous rod-like structured ternary nitride heterocatalyst Co3Mo3N/Ni3Mo3N for efficient and stable hydrogen evolution reaction

Heterostructure electrocatalysts have garnered widespread attention for effectively enhancing electrocatalytic activity. However, less attention has been paid to ternary nitride heterostructure catalysts for the hydrogen evolution reaction (HER), and their synthesis remains challenging. In this study, a Co3Mo3N/Ni3Mo3N heterostructure catalyst on nickel foam (NF) is designed and prepared via high-temperature nitridation of the heterostructured precursor. The resulting 1D/3D hierarchical structure electrode, featuring rich heterointerfaces, provides abundant active sites, enhancing mass transport and charge transfer. Experimental results reveal strong electronic interactions at the heterointerface, while density functional theory (DFT) calculations establish that Co3Mo3N/Ni3Mo3N possesses a lower water dissociation energy barrier and optimized hydrogen adsorption energy. Consequently, it demonstrates excellent HER performance, exhibiting low overpotentials of 36 mV in alkaline and 58 mV in neutral media at 10 mA cm−2. This study presents an innovative approach to designing ternary nitride heterostructure catalysts with enhanced HER activity, applicable to other heterostructure catalysts.

Strain derived from bubbles at monolayer MoS2/hBN interfaces for enhanced hydrogen evolution reaction activity

Strain derived from bubbles at monolayer MoS2/hBN interfaces for enhanced hydrogen evolution reaction activity

Emergence of electrochemical catalytic activity via an electrochemical-probe on defective transition metal dichalcogenide nanosheets

Two-dimensional transition metal dichalcogenides (2D TMDs) have shown exceptional electrochemical catalytic activity for the efficient generation of hydrogen through electrochemical water splitting. In the case of molybdenum disulfide (MoS2), a prominent member of 2D TMDs, the electrochemically active sites primarily reside at the edges, while the basal plane, which constitutes the majority of the MoS2 structure, remains relatively inactive. In this study, we aimed to activate the inert sites of the basal plane with some defective structure for hydrogen evolution reaction (HER) by employing an electrochemical-probe in combination with voltage sweeping. The initiation of HER at these previously inactive sites was visualized and confirmed using scanning electrochemical cell microscopy (SECCM). Our findings reveal that the enhanced HER activity originates from surface defects induced by the probing process.

Boosting the Electrocatalytic Water Splitting Performance Using Hydrophilic Metal-Organic Framework.

In this study, we employed a rapid and efficient microwave method to synthesize Metal-Organic Framework (MOF-303), which was subsequently embedded onto Palladium/Carbon (Pd/C) electrodes. The resulting hybrid material, Pd/C@MOF-303, was thoroughly characterized, and its performance in the Hydrogen Evolution Reaction (HER) was systematically investigated. The Pd/C@MOF-303 composite exhibited remarkable improvements in HER performance compared to the unmodified Pd/C electrode. At a benchmark current density of 10 mA cm-2 , the overpotentials for Pd/C and Pd/C@MOF-303 were measured at 185 mV and 175 mV, respectively. This reduction in overpotential highlights the superior catalytic activity of the Pd/C@MOF-303 hybrid material in facilitating the HER. Furthermore, the Pd/C@MOF-303 electrode demonstrated enhanced HER activity, increased mass activity, and excellent charge transfer rates compared to its unmodified counterpart, Pd/C. The findings underscore the significance of the hydrophilic MOF-303 in tailoring the surface characteristics of electrocatalysts, thereby offering insights into the design principles for advanced materials with superior performance in electrochemical applications.

Enhancing Hydrogen Evolution Reaction Activity of Palladium Catalyst by Immobilization on MXene Nanosheets.

Efficient catalysts with minimal content of catalytically active noble metals are essential for the transition to the clean hydrogen economy. Catalyst supports that can immobilize and stabilize catalytic nanoparticles and facilitate the supply of electrons and reactants to the catalysts are needed. Being hydrophilic and more conductive compared with carbons, MXenes have shown promise as catalyst supports. However, the controlled assembly of their 2D sheets creates a challenge. This study established a lattice engineering approach to regulate the assembly of exfoliated Ti3C2Tx MXene nanosheets with guest cations of various sizes. The enlargement of guest cations led to a decreased interlayer interaction of MXene lamellae and increased surface accessibility, allowing intercalation of Pd nanoparticles. Stabilization of Pd nanoparticles between interlayer-expanded MXene nanosheets improved their electrocatalytic activity. The Pd-immobilized K+-intercalated MXene nanosheets (PdKMX) demonstrated exceptional electrocatalytic performance for the hydrogen evolution reaction with the lowest overpotential of 72 mV (@10 mA cm-2) and the highest turnover frequency of 1.122 s-1 (@ an overpotential of 100 mV), which were superior to those of the state-of-the-art Pd nanoparticle-based electrocatalysts. Weakening of the interlayer interaction during self-assembly with K+ ions led to fewer layers in lamellae and expansion of the MXene in the c direction during Pd anchoring, providing numerous surface-active sites and promoting mass transport. In situ spectroscopic analysis suggests that the effective interfacial electron injection from the Pd nanoparticles strongly immobilized on interlayer-expanded PdKMX may be responsible for the improved electrocatalytic performance.

Efficient electrochemical hydrogen evolution activity of nanostructured Ag3PO4/MoS2 heterogeneous composite catalyst

Hydrogen (H2) generation by electrochemical water splitting is a key technique for sustainable energy applications. Two-dimensional (2D) transition-metal dichalcogenide (MoS2) and silver phosphate (Ag3PO4) possess excellent electrochemical hydrogen evolution reaction (HER) properties when they are combined together as a composite rather than individuals. Reports examining the HER activity by using Ag3PO4, especially, in combination with the 2D layered MoS2 are limited in literature. The weight fraction of MoS2 in Ag3PO4 is optimized for 1, 3, and 5 wt%. The Ag3PO4/1 wt % MoS2 combination exhibits enhanced HER activity with least overpotential of 235 mV among the other samples in the acidic medium. The synergistic effect of optimal nano-scale 2D layered MoS2 structure and Ag3PO4 is essential for creating higher electrochemical active surface area of 217 mF/cm2, and hence this leads to faster reaction kinetics in the HER. This work suggests the advantages of Ag3PO4/1 wt % MoS2 heterogeneous composite catalyst for electrochemical analysis and HER indicating lower resistivity and low Tafel slope value (179 mV/dec) among the prepared catalysts making it a promising candidate for its use in practical energy applications.

Elevating hydrogen evolution performance with plasma-induced sulfur vacancies and heteroatom doping in hollow-structured MnS–CoS catalysts

Transition-metal sulfides doped with various elements show great promise as highly effective catalysts for the hydrogen evolution reaction (HER), potentially serving as alternatives to Pt-based electrocatalysts. Defect engineering has been identified as a key strategy to enhance the HER activity of such catalysts. This study proposes an effective strategy to generate numerous topological/geometric defects on hollow spherical Mn-doped cobalt sulfide (MnS–CoS) via plasma etching. MnS–CoS catalysts with well-defined cavity structures were successfully prepared using a combination of template-assisted and hydrothermal synthesis methods. Under plasma induction, these catalysts exhibited uniformly formed nanocavity structures with a built-in electric field, which uniformly enhanced their topological/geometric defect levels. The plasma-etched MnS–CoS catalyst demonstrated significantly enhanced HER activity, exhibiting an excellent overpotential of 172 mV at a current density of 10 mA·cm⁻2 in alkaline media and a low Tafel slope of 120 mV·dec⁻¹. These improvements can be attributed to the remarkable conductivity of Co and Mn, along with the unique hollow spherical nanostructure of the material, which contained numerous gaps that promoted electron movement and electrolyte penetration, thereby enhancing the overall catalytic performance. The synergistic effects of heteroatom doping and plasma modulation played a crucial role in achieving outstanding catalytic performance toward the HER. Density-functional theory calculations based on a structural model of MnS–CoS-p confirmed that the introduction of defects and heteroatoms reduced hydrogen adsorption: the Gibbs free energy decreased from 0.72 eV for CoS to 0.23 eV for MnS–CoS-p. The excellent HER activity of the MnS–CoS materials stemmed from the abundance of reactive heterostructured interfaces, which optimized the electronic configuration and, thus, accelerated H2O adsorption and dissociation. This study highlights the potential of combining plasma-assisted defect manipulation and transition-metal-element doping to design high-performance catalysts. The findings also offer valuable insights into the development of environment-friendly energy-conversion technologies.

Introducing phosphorus atoms into MoS2 nanosheets through a vapor-phase hydrothermal process for the hydrogen evolution reaction.

Molybdenum disulfide (MoS2)-based electrocatalysts have been considered as promising alternatives to platinum for use in the hydrogen evolution reaction (HER). Developing MoS2 electrocatalysts with more active sites has been recognized as an efficient way to enhance the HER activity. Moreover, phase transition and heteroatom doping show great influence on the HER performance. In this work, we develop a vapor-phase hydrothermal (VPH) approach to introduce phosphorus (P) atoms into a MoS2 nanosheet array on carbon fiber cloth, which presents enhanced HER activity compared with MoS2 without P-doping. The improved performance is due to the synergistic effects of the new active sites formed by the P dopants and the sulfur (S) vacancies in the MoS2 nanosheets generated by the doping of P atoms, which increases the number of active sites. In general, the obtained P-doped MoS2/CFC exhibits a lower onset potential of 80 mV and an overpotential of 162 mV at 10 mA cm-2 than MoS2 without P-doping in 0.5 M H2SO4, accompanied by extremely large cathodic current density and excellent stability. This strategy may open up opportunities for heteroatom doping of electrocatalysts for various applications and provide a new method for material synthesis.