Universal Platform for Robust Dual-Atom Doped 2D Catalysts with Superior Hydrogen Evolution in Wide pH Media.

Layered 2D transition metal dichalcogenides (TMDs) have been suggested as efficient substitutes for Pt-group metal electrocatalysts in the hydrogen evolution reaction (HER). However, poor catalytic activities in neutral and alkaline electrolytes considerably hinder their practical applications. Furthermore, the weak adhesion between TMDs and electrodes often impedes long-term durability and thus requires a binder. Here, a universal platform is reported for robust dual-atom doped 2D electrocatalysts with superior HER performance over a wide pH range media. V:Co-ReS2 on a wafer scale is directly grown on oxidized Ti foil by a liquid-phase precursor-assisted approach and subsequently used as highly efficient electrocatalysts. The catalytic performance surpasses that of Pt group metals in a high current regime (≥ 100 mA cm-2 ) at pH ≥ 7, with a high durability of more than 70 h in all media at 200 mA cm-2 . First-principles calculations reveal that V:Co dual doping in ReS2 significantly reduces the water dissociation barrier and simultaneously enables the material to achieve the thermoneutral Gibbs free energy for hydrogen adsorption.

Unraveling the surface self-reconstruction of Fe-doped Ni-thiophosphate for efficient oxygen evolution reaction.

Surface self-reconstruction of oxygen evolution reaction (OER) electrocatalysts generally occurs during the electrochemical activation process. Herein, we study the surface self-reconstruction of a 2D layered Fe-doped Ni-thiophosphate (NixFe1-xPS3) nanosheet. The role of Fe in the surface self-reconstruction of NiPS3 during the OER is investigated by using an in situ Raman analysis. Formation of amorphous metal/non-metal oxide layers on the surface of NixFe1-xPS3 can efficiently act as the ultimate catalytic center for the OER.

Internal Thermal Stress-Driven Phase Transformation in Van der Waals Layered Materials.

High pressure or strain is an effective strategy for generating phase transformations in van der Waals (vdW) layered materials without introducing defects, but this approach remains difficult to perform consistently. We present a scalable and facile method for achieving phase transformation in vdW materials, wherein solid vdW materials are subject to internal thermal stress within a molten metal mantle as it undergoes cooling. This internal thermal stress is principally the product of differential thermal expansion between mantle and core and can be tuned by the mantle material and temperature conditions. We validated this approach by achieving phase transformation of red phosphorus to black phosphorus, and metallic 1T'- to semiconducting 2H-MoTe2 crystals. We further demonstrate quantum electronic phase transformation of suppressed charge density wave in TiSe2 by means of electron-phonon coupling using the same system.

Atomic and structural modifications of two-dimensional transition metal dichalcogenides for various advanced applications.

Two-dimensional (2D) transition metal dichalcogenides (TMDs) and their heterostructures have attracted significant interest in both academia and industry because of their unusual physical and chemical properties. They offer numerous applications, such as electronic, optoelectronic, and spintronic devices, in addition to energy storage and conversion. Atomic and structural modifications of van der Waals layered materials are required to achieve unique and versatile properties for advanced applications. This review presents a discussion on the atomic-scale and structural modifications of 2D TMDs and their heterostructures via post-treatment. Atomic-scale modifications such as vacancy generation, substitutional doping, functionalization and repair of 2D TMDs and structural modifications including phase transitions and construction of heterostructures are discussed. Such modifications on the physical and chemical properties of 2D TMDs enable the development of various advanced applications including electronic and optoelectronic devices, sensing, catalysis, nanogenerators, and memory and neuromorphic devices. Finally, the challenges and prospects of various post-treatment techniques and related future advanced applications are addressed.

Interface Trap Suppression and Electron Doping in Van der Waals Materials Using Cross-Linked Poly(vinylpyrrolidone).

The instability of van der Waals (vdW) materials leads to spontaneous morphological and chemical transformations in the air. Although the passivation of vdW materials with other resistive materials is often used to solve stability issues, this passivation layer can block carrier injection and thus interfere with charge transfer doping. In this study, a facile method is proposed for n-doping and mediation of Se vacancies in tungsten diselenide (WSe2) by poly(vinylpyrrolidone) (PVP) coating. The major carrier type of the PVP-coated WSe2-based field-effect transistor (FET) was converted from hole (p-type) to electron (n-type). Furthermore, the vacancy-induced interface trap density was reduced by approximately 500 times. This study provides a practical doping and passivation method for the van der Waals materials, as well as a comprehensive understanding of the chemical reaction and electronic transport in these materials.

Epitaxial Single-Crystal Growth of Transition Metal Dichalcogenide Monolayers via the Atomic Sawtooth Au Surface.

Growth of 2D van der Waals layered single-crystal (SC) films is highly desired not only to manifest the intrinsic physical and chemical properties of materials, but also to enable the development of unprecedented devices for industrial applications. While wafer-scale SC hexagonal boron nitride film has been successfully grown, an ideal growth platform for diatomic transition metal dichalcogenide (TMdC) films has not been established to date. Here, the SC growth of TMdC monolayers on a centimeter scale via the atomic sawtooth gold surface as a universal growth template is reported. The atomic tooth-gullet surface is constructed by the one-step solidification of liquid gold, evidenced by transmission electron microscopy. The anisotropic adsorption energy of the TMdC cluster, confirmed by density-functional calculations, prevails at the periodic atomic-step edge to yield unidirectional epitaxial growth of triangular TMdC grains, eventually forming the SC film, regardless of the Miller indices. Growth using the atomic sawtooth gold surface as a universal growth template is demonstrated for several TMdC monolayer films, including WS2 , WSe2 , MoS2 , the MoSe2 /WSe2 heterostructure, and W1- x Mox S2 alloys. This strategy provides a general avenue for the SC growth of diatomic van der Waals heterostructures on a wafer scale, to further facilitate the applications of TMdCs in post-silicon technology.