Spatially Confined Microcells: A Path toward TMD Catalyst Design.

With the ability to maximize the exposure of nearly all active sites to reactions, two-dimensional transition metal dichalcogenide (TMD) has become a fascinating new class of materials for electrocatalysis. Recently, electrochemical microcells have been developed, and their unique spatial-confined capability enables understanding of catalytic behaviors at a single material level, significantly promoting this field. This Review provides an overview of the recent progress in microcell-based TMD electrocatalyst studies.

The practice of reaction window in an electrocatalytic on-chip microcell.

To enhance the efficiency of catalysis, it is crucial to comprehend the behavior of individual nanowires/nanosheets. A developed on-chip microcell facilitates this study by creating a reaction window that exposes the catalyst region of interest. However, this technology's potential application is limited due to frequently-observed variations in data between different cells.

Reducing the Ir-O Coordination Number in Anodic Catalysts based on IrO Nanoparticles towards Enhanced Proton-exchange-membrane Water Electrolysis.

Due to the robust oxidation conditions in strong acid oxygen evolution reaction (OER), developing an OER electrocatalyst with high efficiency remains challenging in polymer electrolyte membrane (PEM) water electrolyzer. Recent theoretical research suggested that reducing the coordination number of Ir-O is feasible to reduce the energy barrier of the rate-determination step, potentially accelerating the OER. Inspired by this, we experimentally verified the Ir-O coordination number's role at model catalysts, then synthesized low-coordinated IrO nanoparticles toward a durable PEM water electrolyzer.

Turning sulfonyl and sulfonimidoyl fluoride electrophiles into sulfur(VI) radicals for alkene ligation.

Sulfonyl and sulfonimidoyl fluorides are versatile substrates in organic synthesis and medicinal chemistry. However, they have been exclusively used as S(VI) electrophiles for defluorinative ligations. Converting sulfonyl and sulfonimidoyl fluorides to S(VI) radicals is challenging and underexplored due to the strong bond dissociation energy of S-F and high reduction potentials, but once achieved would enable dramatically expanded synthetic utility and downstream applications.

High-Pressure Synthesis of Single-Crystalline SnS Nanoribbons.

Two-dimensional tin monosulfide (SnS) is attractive for the development of electronic and optoelectronic devices with anisotropic characteristics. However, its shape-controlled synthesis with an atomic thickness and high quality remains challenging. Here, we show that highly crystalline SnS nanoribbons can be produced via high-pressure (0.

Low-Temperature Potassium Batteries Enabled by Electric and Thermal Field Regulation.

Recharging batteries operate at sub-zero temperature is usually limited by the slow ion diffusion and uneven charge distribution at low temperature. Here, we report a strategy to regulate electric field and thermal field simultaneously, creating a fast and uniform deposition surroundings for potassium ion in potassium metal batteries (PMBs). This regulation is achieved by using a highly ordered 1D nanoarray electrode which provides a dense and flat surface for uniforming the electric field and high thermal conductivity for reducing the temperature fluctuation.

Role of N in Transition-Metal-Nitrides for Anchoring Platinum-Group Metal Atoms toward Single-Atom Catalysis.

Single-atom catalysts (SACs) with a maximum atom utilization efficiency have received growing attention in heterogeneous catalysis. The supporting substrate that provides atomic-dispersed anchoring sites and the local electronic environment in these catalysts is crucial to their activity and stability. Here, inspired by N-doped graphene substrate, the role of N is explored in transition metal nitrides for anchoring single metal atoms toward single-atom catalysis.

Engineering the Morphology and Microenvironment of a Graphene-Supported Co-N-C Single-Atom Electrocatalyst for Enhanced Hydrogen Evolution.

Graphene-supported single-atom catalysts (SACs) are promising alternatives to precious metals for catalyzing the technologically important hydrogen evolution reaction (HER), but their performances are limited by the low intrinsic activity and insufficient mass transport. Herein, a highly HER-active graphene-supported Co-N-C SAC is reported with unique design features in the morphology of the substrate and the microenvironment of the single metal sites: i) the crumpled and scrolled morphology of the graphene substrate circumvents the issues encountered by stacked nanoplatelets, resulting in improved exposure of the electrode/electrolyte interfaces (≈10 times enhancement); ii) the in-plane holes in graphene preferentially orientate the Co atoms at the edge sites with low-coordinated Co-N configuration that exhibits enhanced intrinsic activity (≈2.6 times enhancement compared to the conventional Co-N moiety), as evidenced by detailed experiments and density functional theory calculations.

Programmable patterned MoS film by direct laser writing for health-related signals monitoring.

The two-dimensional (2D) transition metal dichalcogenides (TMDs) are promising flexible electronic materials for strategic flexible information devices. Large-area and high-quality patterned materials were usually required by flexible electronics due to the limitation from the process of manufacturing and integration. However, the synthesis of large-area patterned 2D TMDs with high quality is difficult.

Machine Learning Driven Synthesis of Few-Layered WTe with Geometrical Control.

Reducing the lateral scale of two-dimensional (2D) materials to one-dimensional (1D) has attracted substantial research interest not only to achieve competitive electronic applications but also for the exploration of fundamental physical properties. Controllable synthesis of high-quality 1D nanoribbons (NRs) is thus highly desirable and essential for further study. Here, we report the implementation of supervised machine learning (ML) for the chemical vapor deposition (CVD) synthesis of high-quality quasi-1D few-layered WTe NRs.

Polymorphism of Segmented Grain Boundaries in Two-Dimensional Transition Metal Dichalcogenides.

Grain boundaries (GBs) are vital to crystal materials and their applications. Although GBs in bulk and two-dimensional materials have been extensively studied, the segmented GBs observed in transition metal dichalcogenide monolayers by a sequence of folded segments remain a mystery. We visualize the large-area distribution of the segmented GBs in MoSe monolayers and unravel their structural origin using calculations combined with high-resolution atomic characterizations.

Strain-Modulated Photoelectric Responses from a Flexible α-InSe/3R MoS Heterojunction.

Semiconducting piezoelectric α-InSe and 3R MoS have attracted tremendous attention due to their unique electronic properties. Artificial van der Waals (vdWs) heterostructures constructed with α-InSe and 3R MoS flakes have shown promising applications in optoelectronics and photocatalysis. Here, we present the first flexible α-InSe/3R MoS vdWs p-n heterojunction devices for photodetection from the visible to near infrared region.

Optogenetics inspired transition metal dichalcogenide neuristors for in-memory deep recurrent neural networks.

Shallow feed-forward networks are incapable of addressing complex tasks such as natural language processing that require learning of temporal signals. To address these requirements, we need deep neuromorphic architectures with recurrent connections such as deep recurrent neural networks. However, the training of such networks demand very high precision of weights, excellent conductance linearity and low write-noise- not satisfied by current memristive implementations.

Strain-driven growth of ultra-long two-dimensional nano-channels.

Lateral heterostructures of two-dimensional transition metal dichalcogenides (TMDs) have offered great opportunities in the engineering of monolayer electronics, catalysis and optoelectronics. To explore the full potential of these materials, developing methods to precisely control the spatial scale of the heterostructure region is crucial. Here, we report the synthesis of ultra-long MoS nano-channels with several micrometer length and 2-30 nanometer width within the MoSe monolayers, based on intrinsic grain boundaries (GBs).

Engineering grain boundaries at the 2D limit for the hydrogen evolution reaction.

Atom-thin transition metal dichalcogenides (TMDs) have emerged as fascinating materials and key structures for electrocatalysis. So far, their edges, dopant heteroatoms and defects have been intensively explored as active sites for the hydrogen evolution reaction (HER) to split water. However, grain boundaries (GBs), a key type of defects in TMDs, have been overlooked due to their low density and large structural variations.

Self-gating in semiconductor electrocatalysis.

The semiconductor-electrolyte interface dominates the behaviours of semiconductor electrocatalysis, which has been modelled as a Schottky-analogue junction according to classical electron transfer theories. However, this model cannot be used to explain the extremely high carrier accumulations in ultrathin semiconductor catalysis observed in our work. Inspired by the recently developed ion-controlled electronics, we revisit the semiconductor-electrolyte interface and unravel a universal self-gating phenomenon through microcell-based in situ electronic/electrochemical measurements to clarify the electronic-conduction modulation of semiconductors during the electrocatalytic reaction.

Narrow bandgap oxide nanoparticles coupled with graphene for high performance mid-infrared photodetection.

The pursuit of optoelectronic devices operating in the mid-infrared regime is driven by both fundamental interests and envisioned applications ranging from imaging, sensing to communications. Despite continued achievements in traditional semiconductors, notorious obstacles such as the complicated growth processes and cryogenic operation preclude the usage of infrared detectors. As an alternative path towards high-performance photodetectors, hybrid semiconductor/graphene structures have been intensively explored.

Light-Tunable 1T-TaS Charge-Density-Wave Oscillators.

External stimuli-controlled phase transitions are essential for fundamental physics and design of functional devices. Charge density wave (CDW) is a metastable collective electronic phase featured by the periodic lattice distortion. Much attention has been attracted to study the external control of CDW phases.

Mitochondrial complex I bridges a connection between regulation of carbon flexibility and gastrointestinal commensalism in the human fungal pathogen Candida albicans.

Efficient assimilation of alternative carbon sources in glucose-limited host niches is critical for colonization of Candida albicans, a commensal yeast that frequently causes opportunistic infection in human. C. albicans evolved mechanistically to regulate alternative carbon assimilation for the promotion of fungal growth and commensalism in mammalian hosts.

2D Black Phosphorus/SrTiO3 -Based Programmable Photoconductive Switch.

A novel heterostructure is designed by stacking 2D black phosphorus (BP) on a SrTiO3 substrate. The device demonstrates programmable photoconductive switching under illumination of UV and red light. The light-tunable persistent photoconductivity exhibits a large on/off ratio exceeding 10(5) .

Layer Engineering of 2D Semiconductor Junctions.

A new concept for junction fabrication by connecting multiple regions with varying layer thicknesses, based on the thickness dependence, is demonstrated. This type of junction is only possible in super-thin-layered 2D materials, and exhibits similar characteristics as p-n junctions. Rectification and photovoltaic effects are observed in chemically homogeneous MoSe2 junctions between domains of different thicknesses.

Strain-Induced Electronic Structure Changes in Stacked van der Waals Heterostructures.

Vertically stacked van der Waals heterostructures composed of compositionally different two-dimensional atomic layers give rise to interesting properties due to substantial interactions between the layers. However, these interactions can be easily obscured by the twisting of atomic layers or cross-contamination introduced by transfer processes, rendering their experimental demonstration challenging. Here, we explore the electronic structure and its strain dependence of stacked MoSe2/WSe2 heterostructures directly synthesized by chemical vapor deposition, which unambiguously reveal strong electronic coupling between the atomic layers.

Surface functionalization of two-dimensional metal chalcogenides by Lewis acid-base chemistry.

Precise control of the electronic surface states of two-dimensional (2D) materials could improve their versatility and widen their applicability in electronics and sensing. To this end, chemical surface functionalization has been used to adjust the electronic properties of 2D materials. So far, however, chemical functionalization has relied on lattice defects and physisorption methods that inevitably modify the topological characteristics of the atomic layers.

Defects Engineered Monolayer MoS2 for Improved Hydrogen Evolution Reaction.

MoS2 is a promising and low-cost material for electrochemical hydrogen production due to its high activity and stability during the reaction. However, the efficiency of hydrogen production is limited by the amount of active sites, for example, edges, in MoS2. Here, we demonstrate that oxygen plasma exposure and hydrogen treatment on pristine monolayer MoS2 could introduce more active sites via the formation of defects within the monolayer, leading to a high density of exposed edges and a significant improvement of the hydrogen evolution activity.