High-Yield WS2 Synthesis through Sulfurization in Custom-Modified Atmospheric Pressure Chemical Vapor Deposition Reactor, Paving the Way for Selective NH3 Vapor Detection.

Nanostructured transition metal dichalcogenides have garnered significant research interest for physical and chemical sensing applications due to their unique crystal structure and large effective surface area. However, the high-yield synthesis of these materials on different substrates and in nanostructured films remains a challenge that hinders their real-world applications. In this work, we demonstrate the synthesis of two-dimensional (2D) tungsten disulfide (WS2) sheets on a hundred-milligram scale by sulfurization of tungsten trioxide (WO3) powder in an atmospheric pressure chemical vapor deposition reactor. The as-synthesized WS2 powders can be formulated into inks and deposited on a broad range of substrates using techniques like screen or inkjet printing, spin-coating, drop-casting, or airbrushing. Structural, morphological, and chemical composition analysis confirm the successful synthesis of edge-enriched WS2 sheets. The sensing performance of the WS2 films prepared with the synthesized 2D material was evaluated for ammonia (NH3) detection at different operating temperatures. The results reveal exceptional gas sensing responses, with the sensors showing a 100% response toward 5 ppm of NH3 at 150 °C. The sensor detection limit was experimentally verified to be below 1 ppm of NH3 at 150 °C. Selectivity tests demonstrated the high selectivity of the edge-enriched WS2 films toward NH3 in the presence of interfering gases like CO, benzene, H2, and NO2. Furthermore, the sensors displayed remarkable stability against high levels of humidity, with only a slight decrease in response from 100% in dry air to 93% in humid environments. Density functional theory and Bayesian optimization simulations were performed, and the theoretical results agree with the experimental findings, revealing that the interaction between gas molecules and WS2 is primarily based on physisorption.

Sulfurized Two-Dimensional Conductive Metal-Organic Framework as a High-Performance Cathode Material for Rechargeable Mg Batteries.

Rechargeable Mg batteries are a promising energy storage technology to overcome the limitations inherent to Li ion batteries. A critical challenge in advancing Mg batteries is the lack of suitable cathode materials. In this work, we report a cathode design that incorporates S functionality into two-dimensional metal-organic-frameworks (2D-MOFs). This new cathode material enables good Mg2+ storage capacity and outstanding cyclability. It was found that upon the initial Mg2+ insertion and disinsertion, there is an apparent structural transformation that crumbles the layered 2D framework, leading to amorphization. The resulting material serves as the active material to host Mg2+ through reduction and/or oxidation of S and, to a limited extent, O. The reversible nature of S and O redox chemistry was confirmed by spectroscopic characterizations and validated by density functional calculations. Importantly, during the Mg2+ insertion and disinsertion process, the 2D nature of the framework was maintained, which plays a key role in enabling the high reversibility of the MOF cathode.

Iron-Nickel synergistic catalysis growth of (Fe,Ni)9S8/Ni3S2@N,S codoped carbon bridged nanowires enhanced oxygen evolution reaction performance.

Improving the conductivity of the electrocatalyst itself is essential for enhancing its performance. In this work, N, S-rich 6-thioguanine (TG) is selected as the ligand to synthesize a Fe, Ni bimetallic porous coordination polymer (PCP), which is then derived to fabricate N,S codoped carbon (NSC)-coated (Fe,Ni)9S8/Ni3S2 bridged nanowires. The (Fe,Ni)9S8/Ni3S2@NSC bridged nanowires obtained through bimetallic synergistic catalysis and self-sulfurization processes not only introduced additional electrocatalytic active sites but also significantly enhance the overall conductivity of the catalyst due to the interconnected nanowire structure. The resulting (Fe,Ni)9S8/Ni3S2@NSC demonstrates remarkable oxygen evolution reaction (OER) performance, exhibiting an overpotential as low as 252 mV at a current density of 10 mA cm-2. This work proposes a novel strategy for enhancing the overall conductivity of catalysts by growing bridged nanowires, providing valuable insights and inspiration for the design and preparation of advanced transition metal sulfide electrocatalysts.

Influence of Sulfurization Time on Sb2S3 Synthesis Using a New Graphite Box Design.

In recent years, antimony sulfide (Sb2S3) has been investigated as a photovoltaic absorber material due to its suitable absorber coefficient, direct band gap, extinction coefficient, earth-abundant, and environmentally friendly constituents. Therefore, this work proposes Sb2S3 film preparation by an effective two-step process using a new graphite box design and sulfur distribution, which has a high repeatability level and can be scalable. First, an Sb thin film was deposited using the RF-Sputtering technique, and after that, the samples were annealed with elemental sulfur into a graphite box, varying the sulfurization time from 20 to 50 min. The structural, optical, morphological, and chemical characteristics of the resulting thin films were analyzed. Results reveal the method's effectivity and the best properties were obtained for the sample sulfurized during 40 min. This Sb2S3 thin film presents an orthorhombic crystalline structure, elongated grains, a band gap of 1.69 eV, a crystallite size of 15.25 Å, and a nearly stoichiometric composition. In addition, the formation of a p-n junction was achieved by depositing silver back contact on the Glass/FTO/CdS/Sb2S3 structure. Therefore, the graphite box design has been demonstrated to be functional to obtain Sb2S3 by a two-step process.

Unusual Raman Enhancement Effect of Ultrathin Copper Sulfide.

In surface-enhanced Raman spectroscopy (SERS), 2D materials are explored as substrates owing to their chemical stability and reproducibility. However, they exhibit lower enhancement factors (EFs) compared to noble metal-based SERS substrates. This study demonstrates the application of ultrathin covellite copper sulfide (CuS) as a cost-effective SERS substrate with a high EF value of 7.2 × 104 . The CuS substrate is readily synthesized by sulfurizing a Cu thin film at room temperature, exhibiting a Raman signal enhancement comparable to that of an Au noble metal substrate of similar thickness. Furthermore, computational simulations using the density functional theory are employed and time-resolved photoluminescence measurements are performed to investigate the enhancement mechanisms. The results indicate that polar covalent bonds (Cu─S) and strong interlayer interactions in the ultrathin CuS substrate increase the probability of charge transfer between the analyte molecules and the CuS surface, thereby producing enhanced SERS signals. The CuS SERS substrate demonstrates the selective detection of various dye molecules, including rhodamine 6G, methylene blue, and safranine O. Furthermore, the simplicity of CuS synthesis facilitates large-scale production of SERS substrates with high spatial uniformity, exhibiting a signal variation of less than 5% on a 4-inch wafer.

Co4S3 Nanoparticles Confined in an MnS Nanorod-Grafted N, S-Codoped Carbon Polyhedron for Highly Efficient Sodium-Ion Batteries.

Sodium-ion batteries (SIBs) suffer from limited ion diffusion and structural expansion, generating the urgent demand for Na+ accommodable materials with promising architectures. In this work, the rational exploration for Co4S3 nanoparticles confined in an MnS nanorod-grafted N, S-codoped carbon polyhedron (Co-Mn-S@N-S-C) is achieved by the in situ growth of MOF on MnO2 nanorod along with the subsequent carbonization and sulfurization. Benefiting from the distinctive nanostructure, the Co-Mn-S@N-S-C anode delivers excellent structural stability, resulting in prolonged cycling stability with a capacity retention of 90.2% after 1000 cycles at 2 A g-1. Moreover, the reaction storage mechanism is clarified by the in situ X-ray diffraction (XRD) and transmission electron microscopy (TEM) measurements. The results indicate that properly designed electrode materials have huge potential applications for highly efficient energy storage devices.

Ammonium-Amine Co-Activation: Promoting the Sulfurization of Azurite and Its Effect on Xanthate Adsorption.

Enhanced sulfurization has always been the focus of research on the flotation of copper oxide minerals. In this study, combined ammonium-amine salts were innovatively applied to improve the sulfurization of azurite. Flotation tests were carried out to evaluate the promoting effect of ammonium-amine co-activation on the sulfurization-xanthate flotation of azurite, and the microstructure evolution of sulfurized products was investigated to reveal the mechanism underlying this promoting effect. Compared with single ammonium (amine) salt activation, ammonium-amine co-activation improved the floatability of azurite to a greater extent, i.e., the flotation recovery increased by over 4 percentage points. ToF-SIMS, ICP-OES, FESEM-EDS, AFM, XRD, and UV-vis analyses indicated that ammonium-amine co-activation combined the advantages of inorganic ammonium for buffering pH and organic amine for copper ion complexation, thus promoting the growth of sulfurized crystal products (covellite) and enhancing the adhesion stability of sulfurized products on azurite. Therefore, increasing amounts of copper sulfide components were generated under the ammonium-amine-Na2S system, promoting the adsorption of additional xanthate on azurite. This study provides theoretical support for the application of combined ammonium-amine salts for the sulfurization flotation of copper oxide.

Sulfide in engineered methanogenic systems - Friend or foe?

Sulfide ions are regarded to be toxic to microorganisms in engineered methanogenic systems (EMS), where organic substances are anaerobically converted to products such as methane, hydrogen, alcohols, and carboxylic acids. A vast body of research has addressed solutions to mitigate process disturbances associated with high sulfide levels, yet the established paradigm has drawn the attention away from the multifaceted sulfide interactions with minerals, organics, microbial interfaces and their implications for performance of EMS. This brief review brings forward sulfide-derived pathways other than toxicity and with potential significance for anaerobic organic matter degradation. Available evidence on sulfide reactions with organic matter, interventions with key microbial metabolisms, and interspecies electron transfer are critically synthesized as a guidance for comprehending the sulfide effects on EMS apart from the microbial toxicity. The outcomes identify existing knowledge gaps and specify future research needs as a step forward towards realizing the potential of sulfide-derived mechanisms in diversifying and optimizing EMS applications.

Reduction of Friction and Wear for AISI321 Stainless Steel through Surface Modification Using Nanocrystallization.

Through surface nanocrystallization and low-temperature ion sulfurization, the nanocrystalline/FeS thin film with excellent friction-reduction and antiwear properties was fabricated on the surface of AISI321 stainless steel. The nanocrystallization treatment formed the high hardness and active nanocrystalline structure on the surface of AISI321, with the harness increased from 4.6 GPa to 7.56 GPa. Furthermore, the significantly refined nanostructure strongly increased the concentration of S element in comparison with the single-sulfurized layer on the substrate. Tribological tests reveal that both the original AISI321 substrate and the single-sulfurizing-treated samples are subject to severe abrasion. Single nanocrystallization treatment can improve the wear resistance of AISI321, while the compound treatment can obviously improve the comprehensive tribological properties. The compound-modified layer presents excellent tribological properties with the lowest coefficient of friction (COF) of 0.33, which is related to the increased hardness of the substrate and increased thickness, density, and homogeneity of the sulfurized layer. Furthermore, a physical model is developed for the vacuum tribological behavior of the samples after different treatments. This model provides a reference for revealing the tribological mechanism of the compound-modified layer treated using surface nanocrystallization-assisted chemical heat treatment.

Sulfurization alters phenol-formaldehyde resin microplastics redox property and their efficiency in mediating arsenite oxidation.

Microplastics weathering by various types of oxidants in the oxic environment and their interaction with environmental contaminants have drawn numerous scientific attention. However, the environmental fate of microplastics under a reducing environment has been largely unresolved. Herein, the change of physicochemical and redox properties of microplastics during the weathering under a sulfate-reducing environment and the interaction with arsenite were addressed. The sulfurization of phenol-formaldehyde resin microplastics under a sulfate-reducing environment generated smooth and porous particles with the induction of organic S species. Multiple spectroscopic results demonstrated thioether and thiophene groups formed by the substitute removal of O-containing functional groups. Moreover, the sulfurization process induced the reduction of carbonyl groups and oxidation of phenolic hydroxyl groups and resulted in the formation of semiquinone radicals. The O-containing functional groups contributed to microplastics redox property and As(III) oxidation while S-containing functional groups showed no obvious effect. The sulfurized microplastics had lower efficiency in mediating arsenite oxidation than the unsulfurized counterparts due to the decreased electron donating capacity. Producing hydrogen peroxides by electron-donating phenol groups and semiquinone radicals and the direct semiquinone radicals oxidation could mediate arsenite oxidation. The findings of this study help us understand the fate of microplastics in redox fluctuation interfaces.

Structural and Optical Properties of Tungsten Disulfide Nanoscale Films Grown by Sulfurization from W and WO3.

Tungsten disulfide (WS2) was prepared from W metal and WO3 by ion beam sputtering and sulfurization in a different number of layers, including monolayer, bilayer, six-layer, and nine-layer. To obtain better crystallinity, the nine-layer of WS2 was also prepared from W metal and sulfurized in a furnace at different temperatures (800, 850, 900, and 950 °C). X-ray diffraction revealed that WS2 has a 2-H crystal structure and the crystallinity improved with increasing sulfurization temperature, while the crystallinity of WS2 sulfurized from WO3 (WS2-WO3) is better than that sulfurized from W-metal (WS2-W). Raman spectra show that the full-width at half maximum (FWHM) of WS2-WO3 is narrower than that of WS2-W. We demonstrate that high-quality monocrystalline WS2 thin films can be prepared at wafer scale by sulfurization of WO3. The photoluminescence of the WS2 monolayer is strongly enhanced and centered at 1.98 eV. The transmittance of the WS2 monolayer exceeds 80%, and the measured band gap is 1.9 eV, as shown by ultraviolet-visible-infrared spectroscopy.

Temporally probing the thermal phonon and charge transfer induced out-of-plane acoustical displacement of monolayer and bi-layer MoS2/GaN heterojunction.

Acoustical behavior of semiconducting transition metal dichalcogenides determines the heat transfer pathway, and thus plays a crucial role in the electronics and optoelectronics design. In this research, van der Waals heterojunctions (vdWHs) consisting of transferred monolayer and bi-layer MoS2 on GaN substrate were studied. We observed an asymmetric bipolar acoustic strain wave with ∼5 ps duration, which describes the surface of substrate undergoing strong compressive deformation after weak tensile deformation in the out-of-plane direction. We developed a theory to explain the mechanisms responsible for the observed strain waveform in the vdWHs elastic system, and obtained the critical parameters of the carrier dynamics by temporal fitting. Our results not only report a coherent acoustic phonon generated in the vdWHs, which will complement our understanding of the thermal transfer at the 2D/substrate interface, but also provide information about the intrinsic properties in the vdWHs, which would benefit the design of the 2D-based devices in the future.

Nucleation and Growth of Monolayer MoS2 at Multisteps of MoO2 Crystals by Sulfurization.

Two-dimensional (2D) materials and their heterostructures are promising for next-generation optoelectronics, spintronics, valleytronics, and electronics. Despite recent progress in various growth studies of 2D materials, mechanical exfoliation of flakes is still the most common method to obtain high-quality 2D materials because precisely controlling material growth and synthesizing a single domain during the growth process of 2D materials, for the desired shape and quality, is challenging. Here, we report the nucleation and growth behaviors of monolayer MoS2 by sulfurizing a faceted monoclinic MoO2 crystal. The MoS2 layers nucleated at the thickness steps of the MoO2 crystal and grew epitaxially with crystalline correlation to the MoO2 surface. The epitaxially grown MoS2 layer expands outwardly on the SiO2 substrate, resulting in a monolayer single-crystal film, despite multiple nucleations of MoS2 layers on the MoO2 surface owing to several thickness steps. Although the photoluminescence of MoS2 is quenched owing to efficient charge transfer between MoS2 and metallic MoO2, the MoS2 stretched out to the SiO2 substrate shows a high carrier mobility of (15 cm2 V-1 s-1), indicating that a high-quality monolayer MoS2 film can be grown using the MoO2 crystal as a seed and precursor. Our work shows a method to grow high-quality MoS2 using a faceted MoO2 crystal and provides a deeper understanding of the nucleation and growth of 2D materials on a step-like surface.

Comparative Study between Sulfurized MoS2 from Molybdenum and Molybdenum Trioxide Precursors for Thin-Film Device Applications.

Two-dimensional (2D) materials have been studied as an emerging class of nanomaterials owing to their attractive properties in nearly every field of science and technology. Molybdenum disulfide (MoS2) is one of the more promising candidates of these atomically thin 2D materials for its technological potential. The facile synthesis of MoS2 remains a matter of broad interest. In this study, MoS2 was synthesized by chemical vapor deposition sulfurization at various temperatures (550 °C, 650 °C, and 750 °C) of either precursor molybdenum metal (Mo) or molybdenum trioxide (MoO3) deposited on silicon/silicon dioxide (Si/SiO2) via e-beam evaporation. Monolayer, bilayer, and few layers sulfurized samples have been grown and verified by Raman, photoluminescence spectroscopy, XRD, XPS, and AFM. MoO3 sulfurization provided monolayer growth in comparison to Mo sulfurization under the same conditions and precursor thicknesses. Optical microscopy showed the homogeneous nature of grown samples. A main finding of this work is that MoO3 sulfurization produced higher quality MoS2 as compared to those grown by an Mo precursor. Device characteristics based on monolayer MoO3 sulfurized MoS2-x include nonvolatile resistive switching with Ion/Ioff ≈ 104 at a relatively low operating bias of ±1 V. In addition, field-effect transistor characteristics revealed p-type material growth with a carrier mobility ∼ 41 cm2 V-1 s-1, which is in contrast to typically observed n-type characteristics.

A Versatile Sulfur-Assisted Pyrolysis Strategy for High-Atom-Economy Upcycling of Waste Plastics into High-Value Carbon Materials.

With the overconsumption of disposable plastics, there is a considerable emphasis on the recycling of waste plastics to relieve the environmental, economic, and health-related consequences. Here, a sulfur-assisted pyrolysis strategy is demonstrated for versatile upcycling of plastics into high-value carbons with an ultrahigh carbon-atom recovery (up to 85%). During the pyrolysis process, the inexpensive elemental sulfur molecules are covalently bonded with polymer chains, and then thermally stable intermediates are produced via dehydrogenation and crosslinking, thereby inhibiting the decomposition of plastics into volatile small hydrocarbons. In this manner, the carbon products obtained from real-world waste plastics exhibit sulfur-rich skeletons with an enlarged interlayer distance, and demonstrate superior sodium storage performance. It is believed that the present results offer a new solution to alleviate plastic pollution and reduce the carbon footprint of plastic industry.

Vapor-Liquid-Solid Growth of Site-Controlled Monolayer MoS2 Films Via Pressure-Induc ed Supercritical Phase Nucleation.

In this study, a novel pressure-induced supercritical phase nucleation method is proposed to synthesize monolayer MoS2 films, which is promoter free and can avoid contamination of films derived from these heterogeneous promoters in most of the existing techniques. The low-crystallinity and size-controlled MoO2(acac)2 particles are recrystallized on the substrate via the pressure-sensitive solvent capacity of supercritical CO2 and these particles are used as growth sites. The size of single-crystal MoS2 on the substrate is found to be dependent on the wetting area of the pyrolyzed precursor droplets (MoO2) on the surface, and the formation of continuous films with high coverage is mainly controlled by the coalescence of MoO2 droplets. It is enhanced by the increase of the nucleation site density, which can be adjusted by the supersaturation of the supercritical fluid solution. Our findings pave a new way for the controllable growth of MoS2 and other two-dimensional materials and provide sufficient and valuable evidence for vapor-liquid-solid growth.

Chemical processes and sustainability of rice-shrimp farming on saline acid sulfate soils in mekong delta.

In the history of rice-shrimp farming (RSF) in the Mekong Delta, in saline acid sulfate soils (ASS), RSF has proved its sustainability as there is no long-term accumulation of acidity and salinity that adversely affect RSF production. However, the soil processes involved in this phenomenon are not well understood. This study aimed to determine the significant changes in soil and water chemical indicators associated with soil processes during different stages of RSF. Sampling was conducted in six stages to determine the pH and electrical conductivity (EC) of canal and field water, and the pHe, ECe, and sodium-soluble saturated extract (Na-sol) of surface soil (surS) and subsurface soil (subS) in the low-salinity area (LSA) and high salinity area (HSA) of Bac Lieu province. Putative exchange (exch.) Na+ hydrolysis occurs at the beginning of the rainy season when excess salts are leached. This drastically increases the pH of the field water by 0.6 pH units, from 8.2 to 8.8 in stages 1 to 2, respectively. Putative sulfurization has been shown to occur in subS in both LSAs and HSAs, with a significant decrease of 0.5 pH units from stages 4 to 5, leading to a decrease in the Na-sol of subS through exch. Na+ transformation. Simultaneously, with active soil preparation and liming for RSF, chemical processes such as exch. Na+ hydrolysis, sulfurization, and Na+ transformation are the main factors promoting exch. Na+ desorption, which help to reduce the long-term build-up of salinity and acidity that adversely affect RSF production. Although gypsum is considered an effective material in improving saline soils, in Vietnam, gypsum is the liming material of CaSO4; however, it is not commonly used in agriculture because of its high cost. By using CaCO3 or dolomite as a liming material in saline ASS, the dissolution of lime by sulfuric acid can provide a good opportunity for soil improvement and rice growth in RSF.

Enhanced NH3 Sensing Performance of Mo Cluster-MoS2 Nanocomposite Thin Films via the Sulfurization of Mo6 Cluster Iodides Precursor.

The high-performance defect-rich MoS2 dominated by sulfur vacancies as well as Mo-rich environments have been extensively studied in many fields, such as nitrogen reduction reactions, hydrogen evolution reactions, as well as sensing devices for NH3, which are attributed to the under-coordinated Mo atoms playing a significant role as catalytic sites in the defect area. In this study, the Mo cluster-MoS2 composite was creatively synthesized through a one-step sulfurization process via H2/H2S gas flow. The Mo6 cluster iodides (MIs) coated on the fluorine-doped tin oxide (FTO) glass substrate via the electrophoretic deposition method (i.e., MI@FTO) were used as a precursor to form a thin-film nanocomposite. Investigations into the structure, reaction mechanism, and NH3 gas sensing performance were carried out in detail. The results indicated that during the gas flowing, the decomposed Mo6 cluster iodides played the role of template and precursor, forming complicated Mo cluster compounds and eventually producing MoS2. These Mo cluster-MoS2 thin-film nanocomposites were fabricated and applied as gas sensors for the first time. It turns out that after the sulfurization process, the response of MI@FTO for NH3 gas increased three times while showing conversion from p-type to n-type semiconductor, which enhances their possibilities for future device applications.

Molecular evidence for the production of labile, sulfur-bearing dissolved organic matter in the seep sediments of the South China Sea.

Cold seeps with methane-rich fluids leaking out of the seafloor usually support massive biomass of chemosynthetic organisms and associated fauna. A substantial amount of methane is converted to dissolved inorganic carbon by microbial metabolism, and this process also releases dissolved organic matter (DOM) into pore water. Here, pore water samples from "Haima cold seeps" sediments and the non-seep reference sediments in the northern South China Sea were analyzed for optical properties and molecular compositions of pore water DOM. Our results showed that the relative abundance of protein-like DOM, H/Cwa and molecular lability boundary percentage (MLBL%) in the seep sediments were significantly higher than those in the reference sediments, indicating that more labile DOM related to unsaturated aliphatic compounds is produced in the seep sediments. Spearman's correlation of the fluoresce and molecular data suggested that the humic-like components (C1 and C2) mainly constituted the refractory compounds (CRAM, highly unsaturated and aromatics compounds). In contrast, the protein-like component (C3) had high H/C ratios featuring high degree of DOM lability. The amount of S-containing formulas (CHOS and CHONS) was greatly elevated in the seep sediments, likely caused by abiotic and biotic sulfurization of DOM in the sulfidic environment. Although the abiotic sulfurization was proposed to have a stabilizing effect on organic matter, our results implied that the biotic sulfurization in the cold seep sediments would increase DOM lability. Overall, the labile DOM accumulated in the seep sediments is closely linked to methane oxidation, which not only support heterotrophic communities and but also likely have an impact on carbon and sulfur cycling in the sediments and the ocean.

Beyond the Platinum Era─Scalable Preparation and Electrochemical Activation of TaS2 Flakes.

Among 2D materials, transition-metal dichalcogenides (TMDCs) of group 5 metals recently have attracted substantial interest due to their superior electrocatalytic activity toward hydrogen evolution reaction (HER). However, a straightforward and efficient synthesis of the TMDCs which can be easily scaled up is missing. Herein, we report an innovative, simple, and scalable method for tantalum disulfide (TaS2) synthesis, involving CS2 as a sulfurizing agent and Ta2O5 as a metal precursor. The structure of the created TaS2 flakes was analyzed by Raman, XRD, XPS, SEM, and HRTEM techniques. It was demonstrated that a tuning between 1T (metallic) and 3R (semiconductor) TaS2 phases can be accomplished by varying the reaction conditions. The created materials were tested for HER, and the electrocatalytic activity of both phases was significantly enhanced by electrochemical self-activation, up to that comparable with the Pt one. The final values of the Tafel slopes of activated TaS2 were found to be 35 and 43 mV/dec for 3R-TaS2 and 1T-TaS2, respectively, with the corresponding overpotentials of 63 and 109 mV required to reach a current density of 10 mA/cm2. We also investigated the mechanism of flake activation, which can be attributed to the changes in the flake morphology and surface chemistry. Our work provides a scalable and simple synthesis method to produce transition-metal sulfides which could replace the platinum catalyst in water splitting technology.