Toward Scalable Electrochemical Exfoliation of Molybdenum Disulfide Powder through an Accessible Electrode Design.

Cathodic electrochemical intercalation/exfoliation of transition metal dichalcogenides (TMDs) with bulky tetraalkylammonium-based cations is gaining popularity as it avoids the semiconducting (2H) to metallic (1T) phase transformation in TMDs like molybdenum disulfide (MoS2) and, generally, produces sheets with a larger aspect ratio - important for achieving conformal sheet-to-sheet contact in optoelectronic devices. Large single crystals are typically used as the precursor, but these are expensive, often inaccessible, and result in limited quantities of material. In this paper, a 3D-printable electrochemical cell capable of intercalating gram-scale quantities of commercially available TMD powders is presented. By incorporating a reference electrode in the cell and physically restraining the powder with a spring-loaded mechanism, the system can probe the intercalation electrochemistry, for example, determining the onset of intercalation to be near -2.5 V versus the ferrocene redox couple. While the extent of intercalation depends on precursor quantity and reaction time, a high yield of exfoliated product can be obtained exhibiting average aspect ratios as high as 49 ± 44 similar to values obtained by crystal intercalation. The intercalation and exfoliation of a wide variety of pelletized commercial powders including molybdenum diselenide (MoSe2), tungsten diselenide (WSe2), tungsten disulfide (WS2), and graphitic carbon nitride (gCN) are also demonstrated.

Lamellar Ti3C2 MXene composite decorated with platinum-doped MoS2 nanosheets as electrochemical sensing functional platform for highly sensitive analysis of organophosphorus pesticides.

Precisely detecting organophosphorus pesticides (OPs) is paramount in upholding human safety and environmental preservation, especially in food safety. Herein, an electrochemical acetylcholinesterase (AChE) sensing platform entrapped in chitosan (Chit) on the glassy carbon electrodes (GCEs) decorated with Pt/MoS2/Ti3C2 MXene (Pt/MoS2/TM) was constructed for the detection of chlorpyrifos. It is worth noting that Pt/MoS2/TM possesses good biocompatibility, remarkable electrical conductivity, environmental stability and large specific surface area. Besides, the heterostructure formed by the composite of TM and MoS2 improves the conductivity and maintains the original structure, which is conducive to improving the electrochemical property. The coordination effect between the individual components enables the even distribution of functional components and enhances the electrochemical performance of the biosensor (AChE-Chit/Pt/MoS2/TM). Under optimal efficiency and sensitivity, the AChE-Chit/Pt/MoS2/TM/GCE sensing platform exerts comparable analytical performance and a wide concentration range of chlorpyrifos from 10-12 to 10-6 M as well as a low limit of detection (4.71 × 10-13 M). Furthermore, the biosensor is utilized to detect OPs concerning three kinds of fruits and vegetables with good feasibility and recoveries (94.81% to 104.0%). This work would provide a new scheme to develop high-sensitivity sensors based on the two-dimensional nanosheet/laminar hybrid structure for practical applications in environmental monitoring and agricultural product detection.

Real-Time Observation for MoS2 Growth Kinetics and Mechanism Promoted by the Na Droplet.

While the molten salt-catalyzed chemical vapor deposition (CVD) technique is recognized for its effectiveness in producing large-area transition metal chalcogenides, understanding their growth mechanisms involving alkali metals remains a challenge. Here, we investigate the kinetics and mechanism of sodium-catalyzed molybdenum disulfide (MoS2) growth and etching through image analysis conducted using an integrated CVD microscope. Sodium droplets, agglomerated via the thermal decomposition of the sodium cholate dispersant, catalyze the precipitation of supersaturated MoS2 laminates and induce growth despite fragmentation during this process. Triangular MoS2 crystals display a distinct self-exhausting exponential behavior and slow growth of thermodynamically favorable crystallographic faces, exhibiting a sulfur-dominant pressure. The growth and etching processes are facilitated by the scooting of sodium droplets along grain edges, displaying comparable rates. Leveraging these kinetics makes it possible to engineer atypical MoS2 shapes. This combined microscope not only enhances the understanding of growth mechanisms but also contributes to the facile development of next-generation nanomaterials.

Substrate-induced strain in molybdenum disulfide grown by aerosol-assisted chemical vapor deposition.

Transition metal dichalcogenides have been extensively studied in recent years because of their fascinating optical, electrical, and catalytic properties. However, low-cost, scalable production remains a challenge. Aerosol-assisted chemical vapor deposition (AACVD) provides a new method for scalable thin film growth. In this study, we demonstrate the growth of molybdenum disulfide (MoS2) thin films using AACVD method. This method proves its suitability for low-temperature growth of MoS2thin films on various substrates, such as glass, silicon dioxide, quartz, silicon, hexagonal boron nitride, and highly ordered pyrolytic graphite. The as-grown MoS2shows evidence of substrate-induced strain. The type of strain and the morphology of the as-grown MoS2highly depend on the growth substrate's surface roughness, crystallinity, and chemical reactivity. Moreover, the as-grown MoS2shows the presence of both direct and indirect band gaps, suitable for exploitation in future electronics and optoelectronics.

Bottom-up Synthesis of Highly Chiral 1T Molybdenum Disulfide Nanosheets.

Chirality in inorganic nanostructures has recently stimulated the attention of many researchers, both to unravel fundamental questions on the origin of chirality in inorganic and hybrid materials, as well as to introduce novel promising properties that are originated by the symmetry breaking. MoS2 is one of the most investigated among the large family of layered transition metal dichalcogenides. In particular, the metastable metallic 1T-MoS2 phase is of large interest for potential applications. However, due to thermodynamic reasons, the synthesis of 1T-MoS2 phase is quite challenging. Herein, we present the first synthesis of chiral 1T-MoS2 phase which shows remarkably high chiroptical activity with a g-factor up to 0.01. Chiral 1T-MoS2 was produced using tartaric acid as a chiral ligand to induce symmetry breaking during the material's growth under hydrothermal conditions, leading to the formation of distorted hierarchical nanosheet assemblies exhibiting chiral morphology. Thorough optimization of the synthetic conditions was carried out to maximize chiroptical activity, which is strongly related to the nanostructures' morphology. Finally, the formation mechanism of the chiral 1T-MoS2 nanosheet assemblies was investigated, focusing on the role of molecular intermediates in the growth of the nanosheets and the transfer of chirality.

Crystalline Phase Regulates Microbial Methylation Potential of Mercury Bound to MoS2 Nanosheets: Implications for Safe Design of Mercury Removal Materials.

Transition-metal dichalcogenides (TMDs) have shown great promise as selective and high-capacity sorbents for Hg(II) removal from water. Yet, their design should consider safe disposal of spent materials, particularly the subsequent formation of methylmercury (MeHg), a highly potent and bioaccumulative neurotoxin. Here, we show that microbial methylation of mercury bound to MoS2 nanosheets (a representative TMD material) is significant under anoxic conditions commonly encountered in landfills. Notably, the methylation potential is highly dependent on the phase compositions of MoS2. MeHg production was higher for 1T MoS2, as mercury bound to this phase primarily exists as surface complexes that are available for ligand exchange. In comparison, mercury on 2H MoS2 occurs largely in the form of precipitates, particularly monovalent mercury minerals (e.g., Hg2MoO4 and Hg2SO4) that are minimally bioavailable. Thus, even though 1T MoS2 is more effective in Hg(II) removal from aqueous solution due to its higher adsorption affinity and reductive ability, it poses a higher risk of MeHg formation after landfill disposal. These findings highlight the critical role of nanoscale surfaces in enriching heavy metals and subsequently regulating their bioavailability and risks and shed light on the safe design of heavy metal sorbent materials through surface structural modulation.

The Impact of Microwave Annealing on MoS2 Devices Assisted by Neural Network-Based Big Data Analysis.

Microwave annealing, an emerging annealing method known for its efficiency and low thermal budget, has established a foundational research base in the annealing of molybdenum disulfide (MoS2) devices. Typically, to obtain high-quality MoS2 devices, mechanical exfoliation is commonly employed. This method's challenge lies in achieving uniform film thickness, which limits the use of extensive data for studying the effects of microwave annealing on the MoS2 devices. In this experiment, we utilized a neural network approach based on the HSV (hue, saturation, value) color space to assist in distinguishing film thickness for the fabrication of numerous MoS2 devices with enhanced uniformity and consistency. This method allowed us to precisely assess the impact of microwave annealing on device performance. We discovered a relationship between the device's electrical performance and the annealing power. By analyzing the statistical data of these electrical parameters, we identified the optimal annealing power for MoS2 devices as 700 W, providing insights and guidance for the microwave annealing process of two-dimensional materials.

Flexible Resistive Gas Sensor Based on Molybdenum Disulfide-Modified Polypyrrole for Trace NO2 Detection.

High sensitivity and selectivity and short response and recovery times are important for practical conductive polymer gas sensors. However, poor stability, poor selectivity, and long response times significantly limit the applicability of single-phase conducting polymers, such as polypyrrole (PPy). In this study, PPy/MoS2 composite films were prepared via chemical polymerization and mechanical blending, and flexible thin-film resistive NO2 sensors consisting of copper heating, fluorene polyester insulating, and PPy/MoS2 sensing layers with a silver fork finger electrode were fabricated on a flexible polyimide substrate using a flexible electronic printer. The PPy/MoS2 composite films were characterized using X-ray diffraction, Fourier-transform infrared spectroscopy, and field-emission scanning electron microscopy. A home-built gas sensing test platform was built to determine the resistance changes in the composite thin-film sensor with temperature and gas concentration. The PPy/MoS2 sensor exhibited better sensitivity, selectivity, and stability than a pure PPy sensor. Its response to 50 ppm NO2 was 38% at 150 °C, i.e., 26% higher than that of the pure PPy sensor, and its selectivity and stability were also higher. The greater sensitivity was attributed to p-n heterojunction formation after MoS2 doping and more gas adsorption sites. Thus, PPy/MoS2 composite film sensors have good application prospects.

Employing a magnetic chitosan/molybdenum disulfide nanocomposite for efficiently removing polycyclic aromatic hydrocarbons from milk samples.

This study aimed to develop a highly efficient nanocomposite composed of magnetic chitosan/molybdenum disulfide (CS/MoS2/Fe3O4) for the removal of three polycyclic aromatic hydrocarbons (PAHs)-pyrene, anthracene, and phenanthrene. Novelty was introduced through the innovative synthesis procedure and the utilization of magnetic properties for enhanced adsorption capabilities. Additionally, the greenness of chitosan as a sorbent component was emphasized, highlighting its biodegradability and low environmental impact compared to traditional sorbents. Factors influencing PAH adsorption, such as nanocomposite dosage, initial PAH concentration, pH, and contact time, were systematically investigated and optimized. The results revealed that optimal removal efficiencies were attained at an initial PAH concentration of 150 mg/L, a sorbent dose of 0.045 g, pH 6.0, and a contact time of 150 min. The pseudo-second-order kinetic model exhibited superior fitting to the experimental data, indicating an equilibrium time of approximately 150 min. Moreover, the equilibrium adsorption process followed the Freundlich isotherm model, with kf and n values exceeding 7.91 mg/g and 1.20, respectively. Remarkably, the maximum absorption capacities for phenanthrene, anthracene, and pyrene on the sorbent were determined as 217 mg/g, 204 mg/g, and 222 mg/g, respectively. These findings underscore the significant potential of the CS/MoS2/Fe3O4 nanocomposite for efficiently removing PAHs from milk and other dairy products, thereby contributing to improved food safety and public health.

Janus and Amphiphilic MoS2 2D Sheets for Surface-Directed Orientational Assemblies toward Ex Vivo Dual Substrate Release.

The two-dimensional (2-D) Janus and amphiphilic molybdenum disulfide (MoS2) nanosheet with opposite optical activities on each side (amphichiral) is synthesized by modifying sandwich-like bulk MoS2 with tannic acid and cholesterol through biphasic emulsion method. This new type of amphichiral Janus MoS2 nanosheet consists of a hydrophilic and positive optical activity tannic acid side as well as a hydrophobic and negative optical activity cholesterol side thereby characterized by circular dichroism. Surface-directed orientational differentiation assemblies are performed for the as-synthesized 2D material and are characterized by contact angle, infrared spectroscopy, X-ray photoelectron, and circular dichroism spectroscopies. The amphiphilic nature of the materials is demonstrated by the pre-organization of the nanosheets on either hydrophobic or hydrophilic surfaces, providing unprecedented properties of circular dichroism signal enhancement and wettability. Selective detachment of the surface organic groups (cholesterol and tannic acid fragments) is realized by matrix-assisted laser desorption/ionisation - time-of-flight (MALDI-TOF) mass spectrometry, and the dual substrate release in tissue is detected by ex vivo mass spectrometry imaging.

Electrochemical Determination of Uric Acid Using a Nanocomposite Electrode with Molybdenum Disulfide/Multiwalled Carbon Nanotubes (MoS2@MWCNT).

This paper presents an application for a molybdenum disulfide nanomaterial with multiwalled carbon nanotubes (MoS2@MWCNT/E) in a modified electrode substrate for the detection of uric acid (UA). The modified electrode generates a substantial three-fold increase in the anodic peak current for UA compared to the unmodified MWCNT electrode (MWCNT/E). The MoS2@MWCNT/E surface was characterized by cyclic voltammetry (CV), scanning electron microscopy (SEM), energy-dispersive spectroscopy (EDS) and electrochemical impedance spectroscopy (EIS). The achieved detection limit stood at 0.04 µmol/L, with a relative standard deviation (RSD) of 2.0% (n = 10). The method's accuracy, assessed through relative error and percent recovery, was validated using a urine standard solution spiked with known quantities of UA.

Chiral MoS2@BC fibrous membranes selectively promote peripheral nerve regeneration.

BACKGROUND: Molybdenum disulfide (MoS2) has excellent physical and chemical properties. Further, chiral MoS2 (CMS) exhibits excellent chiroptical and enantioselective effects, and the enantioselective properties of CMS have been studied for the treatment of neurodegenerative diseases. Intriguingly, left- and right-handed materials have different effects on promoting the differentiation of neural stem cells into neurons. However, the effect of the enantioselectivity of chiral materials on peripheral nerve regeneration remains unclear. METHODS: In this study, CMS@bacterial cellulose (BC) scaffolds were fabricated using a hydrothermal approach. The CMS@BC films synthesized with L-2-amino-3-phenyl-1-propanol was defined as L-CMS. The CMS@BC films synthesized with D-2-amino-3-phenyl-1-propanol was defined as D-CMS. The biocompatibility of CMS@BC scaffolds and their effect on Schwann cells (SCs) were validated by cellular experiments. In addition, these scaffolds were implanted in rat sciatic nerve defect sites for three months. RESULTS: These chiral scaffolds displayed high hydrophilicity, good mechanical properties, and low cytotoxicity. Further, we found that the L-CMS scaffolds were superior to the D-CMS scaffolds in promoting SCs proliferation. After three months, the scaffolds showed good biocompatibility in vivo, and the nerve conducting velocities of the L-CMS and D-CMS scaffolds were 51.2 m/s and 26.8 m/s, respectively. The L-CMS scaffolds showed a better regenerative effect than the D-CMS scaffolds. Similarly, the sciatic nerve function index and effects on the motor and electrophysiological functions were higher for the L-CMS scaffolds than the D-CMS scaffolds. Finally, the axon diameter and myelin sheath thickness of the regenerated nerves were improved in the L-CMS group. CONCLUSION: We found that the CMS@BC can promote peripheral nerve regeneration, and in general, the L-CMS group exhibited superior repair performance. Overall, the findings of this study reveal that CMS@BC can be used as a chiral nanomaterial nerve scaffold for peripheral nerve repair.

Optimizing graphene content in scaffolds for evenly distributed crumpled MoS2paper wads as anodes for high-performance Li-ion batteries.

Lithium-ion batteries (LIBs) have revolutionized portable electronics, yet their conventional graphite anodes face capacity limitations. Integrating graphene and 3D molybdenum disulfide (MoS2) offers a promising solution. Ensuring a uniform distribution of 3D MoS2nanostructures within a graphene matrix is crucial for optimizing battery performance and preventing issues like agglomeration and capacity degradation. This study focuses on synthesizing a uniformly distributed paper wad structure by optimizing a composite of reduced graphene oxide RGO@MoS2through structural and morphological analyses. Three composites with varying graphene content were synthesized, revealing that the optimized sample containing 30 mg RGO demonstrates beneficial synergy between MoS2and RGO. The interconnected RGO network enhances reactivity and conductivity, addressing MoS2aggregation. Experimental results exhibit an initially superior capacity of 911 mAh g-1, retained at 851 mAh g-1even after 100 cycles at 0.1 A g-1current density, showcasing improved rate efficiency and long-term stability. This research underscores the pivotal role of graphene content in customizing RGO@MoS2composites for enhanced LIB performance.

Synthesis and Electrocatalytic Performance Study of Sulfur Quantum Dots Modified MoS2.

The electrolysis of water for hydrogen production is currently receiving significant attention due to its advantageous features such as non-toxicity, safety, and environmental friendliness. This is especially crucial considering the urgent need for clean energy. However, the current method of electrolyzing water to produce hydrogen largely relies on expensive metal catalysts, significantly increasing the costs associated with its development. Molybdenum disulfide (MoS2) is considered the most promising alternative to platinum for electrocatalyzing the hydrogen evolution reaction (HER) due to its outstanding catalytic efficiency and robust stability. However, the practical application of this material is hindered by its low conductivity and limited exposure of active sites. MoS2/SQDs composite materials were synthesized using a hydrothermal technique to deposit SQDs onto MoS2. These composite materials were subsequently employed as catalysts for the HER. Research findings indicate that incorporating SQDs can enhance electron transfer rates and increase the active surface area of MoS2, which is crucial for achieving outstanding catalytic performance in the HER. The MoS2/SQDs electrocatalyst exhibits outstanding performance in the HER when tested in a 0.5 M H2SO4 solution. It achieves a remarkably low overpotential of 204 mV and a Tafel slope of 65.82 mV dec-1 at a current density of 10 mA cm-2. Moreover, during continuous operation for 24 h, the initial current density experiences only a 17% reduction, indicating high stability. This study aims to develop an efficient and cost-effective electrocatalyst for water electrolysis. Additionally, it proposes a novel design strategy that uses SQDs as co-catalysts to enhance charge transfer in nanocomposites.

Molybdenum disulfide nanosheets based non-oxygen-dependent and heat-initiated free radical nanogenerator with antimicrobial peptides for antimicrobial, biofilm ablation and wound healing.

Chronic refractory wounds caused by multidrug-resistant (MDR) bacterial and biofilm infections are a substantial threat to human health, which presents a persistent challenge in managing clinical wound care. We here synthesized a composite nanosheet AIPH/AMP/MoS2, which can potentially be used for combined therapy because of the photothermal effect induced by MoS2, its ability to deliver antimicrobial peptides, and its ability to generate alkyl free radicals independent of oxygen. The synthesized nanosheets exhibited 61 % near-infrared (NIR) photothermal conversion efficiency, marked photothermal stability and free radical generating ability. The minimal inhibitory concentrations (MICs) of the composite nanosheets against MDR Escherichia coli (MDR E. coli) and MDR Staphylococcus aureus (MDR S. aureus) were approximately 38 µg/mL and 30 µg/mL, respectively. The composite nanosheets (150 µg/mL) effectively ablated >85 % of the bacterial biofilm under 808-nm NIR irradiation for 6 min. In the wound model experiment, approximately 90 % of the wound healed after the 4-day treatment with the composite nanosheets. The hemolysis experiment, mouse embryonic fibroblast (MEFs) cytotoxicity experiment, and mouse wound healing experiment all unveiled the excellent biocompatibility of the composite nanosheets. According to the transcriptome analysis, the composite nanosheets primarily exerted a synergistic therapeutic effect by disrupting the cellular membrane function of S. aureus and inhibiting quorum sensing mediated by the two-component system. Thus, the synthesized composite nanosheets exhibit remarkable antibacterial and biofilm ablation properties and therefore can be used to improve wound healing in chronic biofilm infections.

Study of the Rolling Effect on MoS2-Carbon Fiber Density and Its Consequences for the Functionality of Li-Ion Batteries.

In this study, an electrode slurry composed of molybdenum disulfide (MoS2) and vapor-grown carbon fiber (VGCF) prepared through a solid-phase synthesis method was blade-coated onto copper foil to form a thick film as the anode for lithium-ion batteries. In previously reported work, MoS2-based lithium-ion batteries have experienced gradual deformation, fracture, and pulverization of electrode materials during the charge and discharge cycling process. This leads to an unstable electrode structure and rapid decline in battery capacity. Furthermore, MoS2 nanosheets tend to aggregate over charge and discharge cycles, which diminishes the surface activity of the material and results in poor electrochemical performance. In this study, we altered the density of the MoS2-carbon fiber/Cu foil anode electrode by rolling. Three different densities of electrode sheets were obtained through varying rolling repetitions. Our study shows the best electrochemical performance was achieved at a material density of 2.2 g/cm3, maintaining a capacity of 427 mAh/g even after 80 cycles.

Molybdenum Disulfide-Assisted Spontaneous Formation of Multistacked Gold Nanoparticles for Deep Learning-Integrated Surface-Enhanced Raman Scattering.

Several fabrication methods have been developed for label-free detection in various fields. However, fabricating high-density and highly ordered nanoscale architectures by using soluble processes remains a challenge. Herein, we report a biosensing platform that integrates deep learning with surface-enhanced Raman scattering (SERS), featuring large-area, close-packed three-dimensional (3D) architectures of molybdenum disulfide (MoS2)-assisted gold nanoparticles (AuNPs) for the on-site screening of coronavirus disease (COVID-19) using human tears. Some AuNPs are spontaneously synthesized without a reducing agent because the electrons induced on the semiconductor surface reduce gold ions when the Fermi level of MoS2 and the gold electrolyte reach equilibrium. With the addition of polyvinylpyrrolidone, a two-dimensional large-area MoS2 layer assisted in the formation of close-packed 3D multistacked AuNP structures, resembling electroless plating. This platform, with a convolutional neural network-based deep learning model, achieved outstanding SERS performance at subterascale levels despite the microlevel irradiation power and millisecond-level acquisition time and accurately assessed susceptibility to COVID-19. These results suggest that our platform has the potential for rapid, low-damage, and high-throughput label-free detection of exceedingly low analyte concentrations.

Ball-milled MoS2 with graphene shows enhanced catalytic activity for hydrogen evolution reaction.

The hydrogen evolution reaction (HER) is an important phenomenon in water splitting. Consequently, the development of an active, earth-abundant, and inexpensive HER catalyst is highly desired. MoS2 has drawn considerable interest as an HER catalyst because it is composed of non-precious metal and exhibits high catalytic activity in the nanosheet form. In this study, size-controlled MoS2 particles were synthesized by ball milling. The as-prepared samples exhibited significantly enhanced electrochemical and catalytic properties compared to those of pristine bulk MoS2. Furthermore, the HER activity improved further upon the introduction of graphene into the as-prepared ball-milled samples. In particular, the MoS2 sample ball-milled for 12 h mixed with graphene exhibited optimal performance, showing an overpotential (160 mV at 10 mA cm-2) that was ~ 335 mV lower than that of pristine bulk MoS2. The superior catalytic activity was ascribed to the exposed edge sites, sulfur vacancies, and 1T phase of MoS2, as well as the noteworthy fortifying effect of the electronically conductive flexible material, graphene. The results provide a promising strategy for its application as an efficient and stable HER catalyst.

Li et al. reported MoS₂-based electrocatalysts for the hydrogen evolution reaction. The superior catalytic activity was ascribed to exposed edge sites, sulfur vacancies, 1T phase, and the effect of graphene.

Optimizing Amorphous Molybdenum Sulfide Thin Film Electrocatalysts: Trade-Off between Specific Activity and Microscopic Porosity.

Amorphous molybdenum sulfide (a-MoSx) is a promising candidate to replace noble metals as electrocatalysts for the hydrogen evolution reaction (HER) in electrochemical water splitting. So far, understanding of the activity of a-MoSx in relation to its physical (e.g., porosity) and chemical (e.g., Mo/S bonding environments) properties has mostly been derived from bulk electrochemical measurements, which provide limited information about electrode materials that possess microscopic structural heterogeneities. To overcome this limitation, herein, scanning electrochemical cell microscopy (SECCM) has been deployed to characterize the microscopic electrochemical activity of a-MoSx thin films (ca. 200 nm thickness), which possess a significant three-dimensional structure (i.e., intrinsic porosity) when produced by electrodeposition. A novel two-step SECCM protocol is designed to quantitatively determine spatially resolved electrochemical activity and electrochemical surface area (ECSA) within a single, high-throughput measurement. It is shown for the first time that although the highest surface area (e.g., most porous) regions of the a-MoSx film possess the highest total activity (measured by the electrochemical current), they do not possess the highest specific activity (measured by the ECSA-normalized current density). Instead, the areas of highest specific activity are localized at/around circular structures, coined "pockmarks", which are tens to hundreds of micrometers in size and ubiquitous to a-MoSx films produced by electrodeposition. By coupling this technique with structural and elemental composition analysis techniques (scanning electron microscopy, energy-dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy) and correlating ECSA with activity and specific activity across SECCM scans, this work furthers the understanding of structure-activity relations in a-MoSx and highlights the importance of local measurements for the systematic and rational design of thin film catalyst materials.

Stabilizing and Activating Active Sites: 1T-MoS2 Supported Pd Single Atoms for Efficient Hydrogen Evolution Reaction.

Metallic 1T-MoS2 with high intrinsic electronic conductivity performs Pt-like catalytic activity for hydrogen evolution reaction (HER). However, obtaining pure 1T-MoS2 is challenging due to its high formation energy and metastable properties. Herein, an in situ SO4 2--anchoring strategy is reported to synthesize a thin layer of 1T-MoS2 loaded on commercial carbon. Single Pd atoms, constituting a substantial loading of 7.2 wt%, are then immobilized on the 1T-phase MoS2 via Pd─S bonds to modulate the electronic structure and ensure a stable active phase. The resulting Pd1/1T-MoS2/C catalyst exhibits superior HER performance, featuring a low overpotential of 53 mV at the current density of 10 mA cm-2, a small Tafel slope of 37 mV dec-1, and minimal charge transfer resistance in alkaline electrolyte. Moreover, the catalyst also demonstrates efficacy in acid and neutral electrolytes. Atomic structural characterization and theoretical calculations reveal that the high activity of Pd1/1T-MoS2/C is attributed to the near-zero hydrogen adsorption energy of the activated sulfur sites on the two adjacent shells of atomic Pd.