A novel crystal configuration of sandwiched S-Mo-Se structure (Janus SMoSe) at the monolayer limit has been synthesized and carefully characterized in this work. By controlled sulfurization of monolayer MoSe2 the top layer of selenium atoms are substituted by sulfur atoms while the bottom selenium layer remains intact. The peculiar structure of this new material is systematically investigated by Raman, photoluminescence and X-ray photoelectron spectroscopy and confirmed by transmission-electron microscopy and time-of-flight secondary ion mass spectrometry. Density-functional theory calculations are performed to better understand the Raman vibration modes and electronic structures of the Janus SMoSe monolayer, which are found to correlate well with corresponding experimental results. Finally, high basal plane hydrogen evolution reaction (HER) activity is discovered for the Janus monolayer and DFT calculation implies that the activity originates from the synergistic effect of the intrinsic defects and structural strain inherent in the Janus structure.

Janus Monolayer Transition Metal Dichalcogenides

Lithium-ion batteries have had a tremendous impact on several sectors of our society; however, the intrinsic limitations of Li-ion chemistry limits their ability to meet the increasing demands of developing more advanced portable electronics, electric vehicles, and grid-scale energy storage systems. Therefore, battery chemistries beyond Li ions are being intensively investigated and need urgent breakthroughs toward commercial applications, wherein the use of metallic Li is one of the most intuitive choices. Despite several decades of oblivion due to safety concerns regarding the growth of Li dendrites, Li-metal anodes are now poised to be revived because of the advances in investigative tools and globally invested efforts. In this review, we first summarize the existing issues with regard to Li anodes and their underlying reasons and then highlight the recent progress made in the development of high-performance Li anodes. Finally, we propose the persisting challenges and opportunities toward the exploration of practical Li-metal anodes.

Towards practical lithium-metal anodes

Fabricating 2D/2D heterojunction with vacancy is more favorable to the spatial separation and transfer of charge owing to the matching of unique 2D structure and vacancy engineering, but the regulation and observation of interlayer forces and electronic structure is a challenging task for synthesizing heterojunction photocatalyst and studying the photocatalytic hydrogen evolution mechanism Herein, an original 2D/2D ZnIn2S4/g-C3N4 Van der Waals heterojunction with S vacancies (ZIS-S/CN VDW) photocatalyst are firstly engineered The optimized 30ZIS-S/g-C3N4 has the highest H2 evolution rate of 60951 μmol h−1 g−1, which is primarily attributed to the fact that 2D/2D VDW heterojunction possesses larger contact area and strong electronic interaction to stimulate charge kinetics, and the vacancy engineering can enhance light absorption by regulating the electronic band structure and act as effective active sites for capturing electrons This work not only enriches 2D/2D heterojunction photocatalytic system based on g-C3N4, but also provides alternative proposal for engineering 2D/2D heterojunction photocatalyst with satisfactory performance

Synergy between van der waals heterojunction and vacancy in ZnIn2S4/g-C3N4 2D/2D photocatalysts for enhanced photocatalytic hydrogen evolution

Lithium, the lightest and most electronegative metallic element, has long been considered the ultimate choice as a battery anode for mobile, as well as in some stationary applications. The high electronegativity of Li is, however, a double-edged sword—it facilitates a large operating voltage when paired with essentially any cathode, promising a high cell-level energy density. It is also synonymous with a high chemical reactivity and low reduction potential. The interfaces a Li metal anode forms with any other material (liquid or solid) in an electrochemical cell are therefore always mediated by one or more products of its chemical or electrochemical reactions with that material. The physical, crystallographic, mechanical, electrochemical, and transport properties of the resultant new material phases (interphases) regulate all interfacial processes at a Li metal anode, including electrodeposition during battery recharge. This Review takes recent efforts aimed at manipulating the structure, composition, and physical properties of the solid electrolyte interphase (SEI) formed on an Li anode as a point of departure to discuss the structural, electrokinetic, and electrochemical requirements for achieving high anode reversibility. An important conclusion is that while recent reports showing significant advances in the achievement of highly reversible Li anodes, e.g. as measured by the coulombic efficiency (CE), raise prospects for as significant progress towards commercially relevant Li metal batteries, the plateauing of achievable CE values to around 99 ± 0.5% apparent from a comprehensive analysis of the literature is problematic because CE values of at least 99.7%, and preferably >99.9% are required for Li metal cells to live up to the potential for higher energy density batteries offered by the Li metal anode. On this basis, we discuss promising approaches for creating purpose-built interphases on Li, as well as for fabricating advanced Li electrode architectures for regulating Li electrodeposition morphology and crystallinity. Considering the large number of physical and chemical factors involved in achieving fine control of Li electrodeposition, we believe that achievement of the remaining ∼0.5% in anode reversibility will require fresh approaches, perhaps borrowed from other fields. We offer perspectives on both current and new strategies for achieving such Li anodes with the specific aim of engaging established contributors and newcomers to the field in the search for scalable solutions.

Regulating electrodeposition morphology of lithium: towards commercially relevant secondary Li metal batteries

Cocrystal engineering with a noncovalent assembly feature by simple constituent units has inspired great interest and has emerged as an efficient and versatile route to construct functional materials, especially for the fabrication of novel and multifunctional materials, due to the collaborative strategy in the distinct constituent units. Meanwhile, the precise crystal architectures of organic cocrystals, with long-range order as well as free defects, offer the opportunity to unveil the structure-property and charge-transfer-property relationships, which are beneficial to provide some general rules in rational design and choice of functional materials. In this regard, an overview of organic cocrystals in terms of assembly, containing the intermolecular interactions and growth methods, two functionality-related factors including packing structure and charge-transfer nature, and those advanced and novel functionalities, is presented. An outlook of future research directions and challenges for organic cocrystal is also provided.

Cocrystal Engineering: A Collaborative Strategy toward Functional Materials

First-principle study of electronic and optical properties of two-dimensional materials-based heterostructures based on transition metal dichalcogenides and boron phosphide

Recent investigations have revealed that some transition-metal dichalcogenides (TMDs), such as MoS2 and WS2, are excellent candidates for high-efficiency photocatalysts for water splitting. However...

First-Principles Study on Transition-Metal Dichalcogenide/BSe van der Waals Heterostructures: A Promising Water-Splitting Photocatalyst

We performed first-principles calculations of the structural, electronic, and optical properties of heterostructures which consist of transition metal dichalcogenides MX2 (M = Mo, W; X = S) stacked with Mg(OH)2. All the heterostructures are formed by van der Waals forces. The MoS2/Mg(OH)2 and WS2/Mg(OH)2 vdW heterostructures were found to be semiconductors with indirect bandgaps and possess intrinsic type-II band alignment. In particular, a comparison of the band edge positions with the redox potential of water indicates that the heterostructures are potential photocatalysts for water splitting, enabling water reduction on the MX2 layer and water oxidation on the Mg(OH)2 layer. Moreover, the photogenerated charges will be effectively separated in the presence of a large built-in electric field across the interface. In addition, all of the MX2/Mg(OH)2 heterostructures show strong optical absorption in the visible and infrared regions, indicating their promise for application in photocatalytic water splitting.

Transition-metal dichalcogenides/Mg(OH)2 van der Waals heterostructures as promising water-splitting photocatalysts: a first-principles study

https://iopscience.iop.org/article/10.1088/1361-6463/ab71ad/pdf

High-efficiency photocatalyst for water splitting: a Janus MoSSe/XN (X = Ga, Al) van der Waals heterostructure

MoSi2N4 is a recently developed 2D material that exhibits remarkable thermal, mechanical, electronic, and optical properties. We used first principles calculations to study the structural and electronic properties of organic molecule doped MoSi 2N4 monolayers. Effective p-doping was achieved by molecular doping with tetracyanoquinodimethane and tetracyanoethylene, while n-doping was achieved by molecular doping with tetrathiafulvalene. The doping gap of tetrathiafulvalene-doped MoSi2N4 was successfully modulated by the application of an external electric field, which resulted in effective n-doping. Furthermore, molecular doping injects additional carriers into the host, which is beneficial for enhancing the performance of MoSi2N4 in nanoelectronic devices. Our results demonstrate the importance of molecular doping in tuning the electronic properties of MoSi 2N4 and broadening its applications.

Yi Luo

Papers

First-principle study of electronic and optical properties of two-dimensional materials-based heterostructures based on transition metal dichalcogenides and boron phosphide

First-Principles Study on Transition-Metal Dichalcogenide/BSe van der Waals Heterostructures: A Promising Water-Splitting Photocatalyst

Transition-metal dichalcogenides/Mg(OH)2 van der Waals heterostructures as promising water-splitting photocatalysts: a first-principles study

High-efficiency photocatalyst for water splitting: a Janus MoSSe/XN (X = Ga, Al) van der Waals heterostructure

Tuning the electronic properties of MoSi2N4 by molecular doping: A first principles investigation