Basal Plane Of MoS2 Research Articles

Nuclear irradiation resistance of MoS2-based nanocomposite films: Insights from in situ macroscopic tribometry

In situ performance enhancement of solid lubricating materials are pivotal for the advancement of nuclear facilities. Here, we conducted in situ tribotests against 5.4 MeV Xe20+ ion irradiation for Ti-doped (MoST) and C/Ti co-doped (MoSCT) MoS2 films. The pristine MoST film outperformed MoSCT film but suffered severe degradation owing to irradiation-induced hardening of the amorphized MoS2 phase. Carbon co-doping effectively mitigated the hardening issue through irradiation-induced graphitization of the carbon phase, thereby enhancing the irradiation resistance of MoS2-based films. Both in situ and ex situ irradiation did not adversely affect the shearing-induced re-ordering of MoS2 basal planes, but they inhibit the graphitization and selective release of non-lubricative carbon phase, resulting in an increase in the film wear rate to 7.34 × 10−7 mm3/N·m.

Efficient Hydrogen Evolution Reaction in 2H-MoS2 Basal Planes Enhanced by Surface Electron Accumulation

An innovative strategy has been developed to activate the basal planes in molybdenum disulfide (MoS2) to improve their electrocatalytic activity by controlling surface electron accumulation (SEA) through aging, annealing, and nitrogen-plasma treatments. The optimal hydrogen evolution reaction (HER) performance was obtained on the surface treated with nitrogen-plasma for 120 s. An overpotential of 0.20 V and a Tafel slope of 120 mV dec−1 were achieved for the optimized condition. The angle-resolved photoemission spectroscopy measurement confirmed the HER efficiency enhanced by the SEA conjugated with the sulfur vacancy active sites in the MoS2 basal planes. This study provides new insight into optimizing MoS2 catalysts for energy applications.

Coordination engineering of single-atom ruthenium in 2D MoS2 for enhanced hydrogen evolution.

This study investigates the enhancement of catalytic activity in single-atom catalysts (SACs) through coordination engineering. By introducing non-metallic atoms (X = N, O, or F) into the basal plane of MoS2 via defect engineering and subsequently anchoring hetero-metallic Ru atoms, we created 10 types of non-metal-coordinated Ru SACs (Ru-X-MoS2). Computations indicate that non-metal atom X significantly modifies the electronic structure of Ru, optimizing the hydrogen evolution reaction (HER). Across acidic, neutral, and alkaline electrolytes, Ru-X-MoS2 catalysts exhibit significantly improved HER performance compared with Ru-MoS2, even surpassing commercial Pt/C catalysts. Among these, the Ru-O-MoS2 catalyst, characterized by its asymmetrically coordinated O2-Ru-S1 active sites, demonstrates the most favorable electrocatalytic behavior and exceptional stability across all pH ranges. Consequently, single-atom coordination engineering presents a powerful strategy for enhancing SAC catalytic performance, with promising applications in various fields.

Construction of synergistic active sites on MoS2 basal plane by interfacing with C60 derivative for enhanced photocatalytic hydrogen evolution coupled with biomass alcohol conversion

As a promising alternative to platinum, molybdenum disulfide (MoS2) is widely utilized as catalyst/co-catalyst in hydrogen evolution reaction (HER). However, its inactive basal plane greatly hampers its catalytic activity. Herein, we propose a function-oriented strategy to enhance the catalytic activity of MoS2 by interfacing with fullerene derivatives, specifically indene-C60 bisadduct (ICBA). The ICBA-MoS2 hybrid was then employed as an efficient co-catalyst, in conjunction with CdS, to construct a photocatalyst for solar-driven hydrogen production coupled with the selective oxidation of furfural alcohol (FOL) to furfural (FAL). The optimized 5 % ICBA-MoS2/CdS (5 %-IMC) sample exhibits a remarkable H2 and FAL production rates of 978 and 1160 μmol h−1 g−1, respectively, which was 2.4 times higher than that of the primitive sample without ICBA modified. This prominent catalytic performance can be attributed to the high activity of synergistic active sites in ICBA-MoS2, as well as the speed transportation and separation of the photogenerated charges from CdS to ICBA-MoS2, as evidenced by both experimental and theoretical investigations.

Hydrogen-induced Sulfur Vacancies on the MoS2 Basal Plane Studied by Ambient Pressure XPS and DFT Calculations.

Sulfur vacancy on an MoS2 basal plane plays a crucial role in device performance and catalytic activity; thus, an understanding of the electronic states of sulfur vacancies is still an important issue. We investigate the electronic states on an MoS2 basal plane by ambient-pressure X-ray photoelectron spectroscopy (AP-XPS) and density functional theory calculations while heating the system in hydrogen. The AP-XPS results show a decrease in the intensity ratio of S 2p to Mo 3d, indicating that sulfur vacancies are formed. Furthermore, low-energy components are observed in Mo 3d and S 2p spectra. To understand the changes in the electronic states induced by sulfur vacancy formation at the atomic scale, we calculate the core-level binding energies for the model vacancy surfaces. The calculated shifts for Mo 3d and S 2p with the formation of sulfur vacancy are consistent with the experimentally observed binding energy shifts. Mulliken charge analysis indicates that this is caused by an increase in the electronic density associated with the Mo and S atoms around the sulfur vacancy as compared to the pristine surface. The present investigation provides a guideline for sulfur vacancy engineering.

Visualizing the role of applied voltage in non-metal electrocatalysts.

Understanding how applied voltage drives the electrocatalytic reaction at the nanoscale is a fundamental scientific problem, particularly in non-metallic electrocatalysts, due to their low intrinsic carrier concentration. Herein, using monolayer molybdenum disulfide (MoS2) as a model system of non-metallic catalyst, the potential drops across the basal plane of MoS2 (ΔVsem) and the electric double layer (ΔVedl) are decoupled quantitatively as a function of applied voltage through in-situ surface potential microscopy. We visualize the evolution of the band structure under liquid conditions and clarify the process of EF keeping moving deep into Ec, revealing the formation process of the electrolyte gating effect. Additionally, electron transfer (ET) imaging reveals that the basal plane exhibits high ET activity, consistent with the results of surface potential measurements. The potential-dependent behavior of kf and ns in the ET reaction are further decoupled based on the measurements of ΔVsem and ΔVedl. Comparing the ET and hydrogen evolution reaction imaging results suggests that the low electrocatalytic activity of the basal plane is mainly due to the absence of active sites, rather than its electron transfer ability. This study fills an experimental gap in exploring driving forces for electrocatalysis at the nanoscale and addresses the long-standing issue of the inability to decouple charge transfer from catalytic processes.

Wrapping-Trapping versus Extraction Mechanism of Bactericidal Activity of MoS2 Nanosheets against Staphylococcus aureus Bacterial Membrane.

The promising broad-spectrum antibacterial activity of two-dimensional molybdenum disulfide (2D MoS2) has been widely recognized in the past decade. However, a comprehensive understanding of how the antibacterial pathways opted by the MoS2 nanosheets varies with change in lipid compositions of different bacterial strains is imperative to harness their full antibacterial potential and remains unexplored thus far. Herein, we present an atomistic molecular dynamics (MD) study to investigate the distinct modes of antibacterial action of MoS2 nanosheets against Staphylococcus aureus (S. aureus) under varying conditions. We observed that the freely dispersed nanosheets readily adhered to the bacterial membrane outer surface and opted for an unconventional surface directed "wrapping-trapping" mechanism at physiological temperature (i.e., 310 K). The adsorbed nanosheets mildly influenced the membrane structure by originating a compact packing of the lipid molecules present in its direct contact. Interestingly, these surface adsorbed nanosheets exhibited extensive phospholipid extraction to their surface, thereby inducing transmembrane water passage analogous to the cellular leakage, even at a slight increment of 20 K in the temperature. The strong van der Waals interactions between lipid fatty acyl tails and MoS2 basal planes were primarily responsible for this destructive phospholipid extraction. In addition, the MoS2 nanosheets bound to an imaginary substrate, controlling their vertical alignment, demonstrated a "nano-knives" action by spontaneously piercing inside the membrane core through their sharp corner, subsequently causing localized lipid ordering in their vicinity. The larger nanosheet produced a more profound deteriorating impact in all of the observed mechanisms. Keeping the existing knowledge about the bactericidal activity of 2D MoS2 in view, our study concludes that their antibacterial activity is strongly governed by the lipid composition of the bacterial membrane and can be intensified either by controlling the nanosheet vertical alignment or by moderately warming up the systems.

Electronic sensitization enhanced p-type ammonia gas sensing of zinc doped MoS2/RGO composites.

Zinc (Zn) doping induced synergetic effects of defects engineering and heterojunction in Molybdenum disulphide/Reduced graphene oxide (MoS2/RGO) effectively enhances the p-type Volatile organic compounds (VOC) gas sensing traits and helps in tailoring the over dependence on noble metals for surface sensitization. Through this work, we have successfully prepared Zn doped MoS2 grafted on RGO employing an in-situ hydrothermal method. Optimal doping concentration of Zn dopants in the MoS2 lattice triggered more active sites on the basal plane of MoS2 with the aid of defects promoted by the zinc dopants. Effective intercalation of RGO further boost up the exposed surface area of Zn doped MoS2 for further interaction of ammonia gas molecules. Besides, smaller crystallite size brought out by 5% Zn dopants aids in efficient charge transfer across the heterojunctions that further amplifies the ammonia sensing traits with a peak response of 32.40% along with a response time of 21.3s and recovery time of 44.90s. The as prepared ammonia gas sensor exhibited excellent selectivity and repeatability. The obtained results reveal that transition metal doping into the host lattice proves to be a promising approach for VOC sensing characteristics of p-type gas sensors and gives insight about the importance of dopants and defects for the development of highly efficient gas sensors in the future.

Tiny Ni3S2 boosting MoS2 hydrogen evolution in alkali by enlarging coupling boundaries and stimulating basal plane

The relatively slow reaction kinetics of the hydrogen evolution reaction (HER) by water electrolysis in alkali hinder its large-scale industrial production. To improve the HER activity in alkaline media, a novel Ni3S2/MoS2/CC catalytic electrode was synthesized by a simple two-step hydrothermal method in this work. The modification of MoS2 by Ni3S2 could facilitate the adsorption and dissociation of water, thus accelerating the alkaline HER kinetics. Moreover, the unique morphology of small Ni3S2 nanoparticles grown on MoS2 nanosheets not only increased the interface coupling boundaries, which acted as the most efficient active sites for the Volmer step in alkaline medium, but also sufficiently activated the MoS2 basal plane, thus providing more active sites. Consequently, Ni3S2/MoS2/CC only needed overpotentials of 189.4 and 240 mV to drive current densities of 100 and 300 mA·cm−2, respectively. More importantly, its catalytic performance of Ni3S2/MoS2/CC even exceeded that of Pt/C at a high current density after 261.7 mA·cm−2 in 1.0 M KOH.

Engineering Catalytically Active Sites by Sculpting Artificial Edges on MoS2 Basal Plane for Dinitrogen Reduction at a Low Overpotential.

Engineering catalytically active sites have been a challenge so far and often relies on optimization of synthesis routes, which can at most provide quantitative enhancement of active facets, however, cannot provide control over choosing orientation, geometry and spatial distribution of the active sites. Artificially sculpting catalytically active sites via laser-etching technique can provide a new prospect in this field and offer a new species of nanocatalyst for achieving superior selectivity and attaining maximum yield via absolute control over defining their location and geometry of every active site at a nanoscale precision. In this work, a controlled protocol of artificial surface engineering is shown by focused laser irradiation on pristine MoS2 flakes, which are confirmed as catalytic sites by electrodeposition of AuNPs. The preferential Au deposited catalytic sites are found to be electrochemically active for nitrogen adsorption and its subsequent reduction due to the S-vacancies rather than Mo-vacancy, as advocated by DFT analysis. The catalytic performance of Au-NR/MoS2 shows a high yield rate of ammonia (11.43×10-8 mol s-1 cm-2 ) at a potential as low as -0.1V versus RHE and a notable Faradaic efficiency of 13.79% during the electrochemical nitrogen reduction in 0.1m HCl.

Activation of basal-plane sulfur sites on MoS2 @Ni3S2 nanorods by Zr plasma ion implantation for bifunctional electrocatalysts

Water electrolysis is one of the most promising technologies for sustainable and clean energy production, yet the sluggish kinetics of the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) hampers the commercialization. In this work, Zr-doped MoS2 @Ni3S2 (MSNF) heterogeneous nanorods as bifunctional electrocatalysts were successfully explored to boost the catalytic activity of water electrolysis. The structural characterizations demonstrate the uniform modification of Zr atoms on the basal plane of MoS2 at the heterointerface of MSNF. MSNF implanted with a Zr plasma ion fluence of 5 × 1016 ions-cm−2 (Zr500-MSNF) shows the most remarkable bifunctional electrocatalytic characteristics such as Tafel slope of 60.9 mV dec−1 and overpotential of 98 mV at 10 mA cm−2 for HER, as well as Tafel slope of 78.5 mV dec−1 and overpotential of 275 mV at 20 mA cm−2 for OER. Consistent with the structural and electrocatalytic characterizations, first-principles calculation confirms that the activated S sites in the basal plane of MoS2 upon Zr doping have more empty states in its valence orbital to favor the adsorption of hydrogen and hydroxide, thus contributing to enhanced HER and OER activity. The findings in this work reveal a facile strategy to design high-performance and low-cost bifunctional catalysts based on two-dimensional materials for overall water splitting.

Stable 1T –2H MoS2 heterostructures for efficient electrocatalytic hydrogen evolution

1T-phase molybdenum disulfide (1T MoS2) can efficiently facilitate the charge transfer and provide the active site, exhibiting a better hydrogen evolution reaction (HER) than 2H MoS2. However, its thermodynamic instability becomes a major drawback that hinders its practical application. We report a chemical vapor deposition (CVD) method to grow MoS2 nanosheets with high 1T content (61.5%) by introducing an appropriate amount of antimony oxide. The 1T-2H hybrid structures grown in this mode are thermodynamically stable. 1T phase of the MoS2 produces a unique charge distribution that makes the S atoms at the 1T-2H interface more favorable for H adsorption, thus enhancing the HER activity on the MoS2 basal plane. This study has provided a new idea for the 1T-phase MoS2 preparation for efficient HER.

O-doping induced abundant active-sites in MoS2 nanosheets for propelling polysulfide conversion of Li-S batteries

The oxygen doped MoS2 nanosheets were in-situ grown into the three-dimensional (3D) porous graphene frameworks (O-MoS2/G) through a facile hydrothermal method, and then used to coat the commercial PP separators for Li-S batteries. The relatively low hydrothermal temperature should be a key factor for achieving the O-doped MoS2. The O dopants could expand and disturb interlayer structures of MoS2 to produce abundant active edge sites for adsorption and catalytic conversion of polysulfides. Moreover, the basal planes of MoS2 should be also activated by the O doping and exhibit enhanced chemical adsorption strength towards polysulfides for propelling electrochemical conversion. Owing to the synergistic effects of the 3D porous graphene frameworks and the inlaid O-MoS2 nanosheets, the Li-S cells with high S areal loading cathodes and O-MoS2/G@PP separators exhibit excellent electrochemical performances with a high specific capacity of 1141 mAh g−1 at the 1st cycle at 0.1 C, reversible capacities of 772 mAh g−1 at the 50th cycle at 0.2 C and 583 mAh g−1 at the 100th cycle at 0.5 C. These encouraging results provide that the heteroatom doping should be a promising approach to improve the adsorption and catalytic activity of MoS2 for propelling the polysulfide conversion in Li-S batteries.

Is the doped MoS2 basal plane an efficient hydrogen evolution catalyst? Calculations of voltage-dependent activation energy.

Transition metal dichalcogenides are cheap and earth-abundant candidates for the replacement of precious metals as catalyst materials. Experimental measurements of the hydrogen evolution reaction (HER), for example, have demonstrated significant electrocatalytic activity of MoS2 but there is large variation depending on the preparation method. In order to gain information about the mechanism and active sites for the HER, we have carried out calculations of the reaction and activation energy for HER at the transition metal doped basal plane of MoS2 under electrochemical conditions, i.e. including applied electrode potential and solvent effects. The calculations are based on identifying the relevant saddle points on the energy surface obtained from density functional theory within the generalized gradient approximation, and the information on energetics is used to construct voltage-dependent volcano plots. Doping with 3d-metal atoms as well as Pt is found to enhance hydrogen adsorption onto the basal plane by introducing electronic states within the band gap, and in some cases (Co, Ni, Cu, Pt) significant local symmetry breaking. The Volmer-Heyrovsky mechanism is found to be most likely and the associated energetics show considerable dopant and voltage-dependence. While the binding free energy of hydrogen can be tuned to be seemingly favorable for HER, the calculated activation energy turns out to be significant, at least 0.7 eV at a voltage of -0.5 V vs. SHE, indicating low catalytic activity of the doped basal plane. This suggests that other sites are responsible for the experimental activity, possibly edges or basal plane defects.

Metal-nonmetal atom co-doping engineered transition metal disulfide for highly efficient hydrogen evolution reaction

The development of effective and non-precious electrocatalyts for hydrogen evolution reaction (HER) has attracted massive research interests. Herein, we report a density functional theory (DFT) investigation on the activation and optimization of Molybdenum disulfide (MoS2) monolayer as efficient HER electrocatalysts by cobalt-nonmetal atom (X = B, C, N, P, Se) codoping. Our results show that three CoX-MoS2 (X = C, N, and Se) catalysts display enhanced HER performance with |ΔGH|s in the range of 0.12–0.23 eV. Careful electronic structure analysis manifests that the favorable H adsorption process on the MoS2 basal plane is induced by suitable in-gap states upon codoping. Furthermore, appropriate biaxial strain can help optimize the HER performance of these co-doped systems, e.g, the ΔGHs of CoC@MoS2, CoN@MoS2, and CoSe@MoS2 reaches 0.0 eV, −0.04 eV, and −0.01 eV at 1.86% tensile strain, 5% compressive strain, and 4% compressive strain, respectively. Our work offers a highly promising catalyst for HER and guides the atomic design of more efficient non-noble electrocatalysts.

A novel 0D/2D/2D hetero-layered nitrogen-doped graphene/MoS2 architecture for catalytic hydrogen evolution reaction

• A hybrid of Ni@N-Gr with exfoliated MoS 2 is reasonably designed and synthesized. • Ni@N-Gr/MoS 2 provides a stimulating insight to form non-precious metal doping onto layered 2D/2D hetero-assembly. • The hybrid has high electronic conductivity and rich exposed active sites. • Ni@N-Gr/MoS 2 exhibits superior and durable electrocatalytic performance in acidic medium. Two-dimensional (2D) layered molybdenum disulfide (MoS 2 ) has emerged as a promising Pt-substituting electrocatalyst for the hydrogen evolution reaction (HER) recently. Despite the ever-growing interest in these MoS 2 based-materials, their catalytic performance is still far from satisfactory due to the nature of the inactive basal plane and poor conductivity. This work presents a novel nickel@nitrogen‐doped graphene@MoS 2 (Ni@N-Gr/MoS 2 ) triad heterostructure for catalytic HER. The as-synthesized Ni@N-Gr/MoS 2 assembly exhibits high intrinsic HER activity with a low overpotential of 270 mV at 10 mA cm −2 , an onset overpotential of 60 mV, a small Tafel slope of 56 mV dec −1 , and robust stability in 0.5 M H 2 SO 4 . The notable activity of the Ni@N-Gr/MoS 2 composites is attributed to two main causes (i) presence of further catalytic active sites due to the incorporation of Ni@N-Gr in the basal plane of MoS 2 (ii) improvement of the conductivity due to nitrogen-doped Gr; where a fast electron transfer takes place from Ni@N-Gr core to MoS 2 during HER. Our novel-hybrid strategy is promising as an electrochemical platform in industrial hydrogen production and hence can stimulate further structural realizations to employ other metal species.

Computational screening of nonmetal dopants to active MoS2 basal-plane for hydrogen evolution reaction via structural descriptor

Nonmetal doping is an efficient approach to activate inert MoS2 basal plane, which converts MoS2 into an electrocatalyst for the hydrogen evolution reaction (HER). However, the trial-and-error approach through experimental attempt is still a common practice to search for suitable nonmetal dopants. In this work, we employ density functional theory (DFT) and microkinetic model to assess alkaline HER activity of nonmetal-modified MoS2(001), which show strong variation in the degree of activation by single- or double-dopants across nonmetal element series (B, C, N, P, O, S, Se and Te). To assist the screening of nonmetal dopants to active MoS2 basal plane, a structural descriptor-based prediction model is constructed. It demonstrates that the activation effect of nonmetal dopant is achieved through the adjustment of valence electron occupancy of reaction center, which tunes the adsorption energy of atomic hydrogen and hydroxide radical, and accordingly reaction kinetic for alkaline HER. The structural descriptor-based prediction model reproduce the activity trend among non-metallic doped MoS2 from available experimental references. In addition, we screened out MoS2 modified by BTe and BSe double dopants with lower overpotential than reported nonmetal-modified MoS2 systems. This work gives a deep insight into activation mechanism of nonmetal dopant for MoS2, and provides an efficient screening strategy for future catalyst design of transition metal dichalcogenides.

Enhanced Activities in Alkaline Hydrogen and Oxygen Evolution Reactions on MoS2 Electrocatalysts by In-Plane Sulfur Defects Coupled with Transition Metal Doping.

2D transition metal disulfides (TMDs) are promising and cost-effective alternatives to noble-metal-based catalysts for hydrogen production. Activation of the inert basal plane of TMDs is crucial to improving the catalytic efficiency. Herein, introduction of in-plane sulfur vacancies (Sv ) and 3d transition metal dopants in concert activates the basal planes of MoS2 (M-Sv -MoS2 ) to achieve high activities in the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Acetate introducing mild wet chemical etching removes surface S atoms facilitating subsequent cation exchange between the exposed Mo atoms and targeted metal ions in solution. Density-functional theory calculation demonstrates that the exposed 3d transition metal dopants in MoS2 basal planes serve as multifunctional active centers, which not only reduce ΔGH* but also accelerate water oxidation. As a result, the optimal Ni-Sv -MoS2 and Co-Sv -MoS2 electrocatalysts show excellent stability and alkaline HER and OER characteristics such as low overpotentials of 101 and 190mV at 10mA cm-2 , respectively. The results reveal a strategy to activate the inert MoS2 basal planes by defect and doping co-engineering and the technique can be extended to other types of TMDs for high-efficiency electrocatalysis beyond water splitting.

Defect Mediated Improvements in the Photoelectrochemical Activity of MoS2/SnS2 Ultrathin Sheets on Si Photocathode for Hydrogen Evolution.

Solar-driven water electrolysis to produce hydrogen is one of the clean energy options for the current energy-related challenges. Si as a photocathode exhibits a large overpotential due to the slow hydrogen evolution reaction (HER) kinetics and hence needs to be modified with a cocatalyst layer. MoS2 is a poor HER cocatalyst due to its inert basal plane. Activation of the MoS2 basal plane will facilitate HER kinetics. In this study, we have incorporated SnS2 into MoS2 ultrathin sheets to induce defect formation and phase transformation. MoS2/SnS2 composite ultrathin sheets with a Sn2+ state create a large number of S vacancies on the basal sites. The optimized defect-rich MoS2/SnS2 ultrathin sheets decorated on surface-modified Si micro pyramids as photocathodes show a current density of -23.8 mA/cm2 at 0 V with an onset potential of 0.23 V under acidic conditions, which is higher than that of the pristine MoS2. The incorporation of SnS2 into 2H-MoS2 ultrathin sheets not only induces a phase but also can alter the local atomic arrangement, which in turn is verified by their magnetic response. The diamagnetic SnS2 phase causes a decrease in symmetry and an increase in magnetic anisotropy of the Mo3+ ions.

Stable Liquid-Sulfur Generation on Transition-Metal Dichalcogenides toward Low-Temperature Lithium-Sulfur Batteries.

The electrochemical formation of liquid sulfur at room temperature on the basal plane of MoS2 has attracted much attention due to the high areal capacity and rapid kinetics of lithium-liquid sulfur chemistry. However, the liquid sulfur is converted to the solid phase once it contacts the solid sulfur crystals generated from the edge of MoS2. Thus, stable liquid sulfur cannot be formed on the entire MoS2 surface. Herein, we report entire liquid sulfur generation on hydrogen-annealed MoS2 (H2-MoS2), even under harsh conditions of large overpotentials and low working temperatures. The origins of the solely liquid sulfur formation are revealed to be the weakened interactions between H2-MoS2 and sulfur molecules and the decreased electrical polarization on the edges of the H2-MoS2. Progressive nucleation and droplet-merging growth behaviors are observed during the sulfur formation on H2-MoS2, signifying high areal capacities by releasing active H2-MoS2 surfaces. To demonstrate the universality of this strategy, other transition-metal dichalcogenides (TMDs) annealed in hydrogen also exhibit similar sulfur growth behaviors. Furthermore, the H2 annealing treatment can induce sulfur vacancies on the basal plane and partial oxidation on the edge of TMDs, which facilitates liquid sulfur formation. Finally, liquid sulfur can be generated on H2-MoS2 flakes at an ultralow temperature of -50 °C, which provides a possible development of low-temperature lithium-sulfur batteries. This work demonstrates the potential of a pure liquid sulfur-lithium electrochemical system using functionalized two-dimensional materials.