Peel-and-Stick Integration of Atomically Thin Nonlayered PtS Semiconductors for Multidimensionally Stretchable Electronic Devices.

Various near-atom-thickness two-dimensional (2D) van der Waals (vdW) crystals with unparalleled electromechanical properties have been explored for transformative devices. Currently, the availability of 2D vdW crystals is rather limited in nature as they are only obtained from certain mother crystals with intrinsically possessed layered crystallinity and anisotropic molecular bonding. Recent efforts to transform conventionally non-vdW three-dimensional (3D) crystals into ultrathin 2D-like structures have seen rapid developments to explore device building blocks of unique form factors. Herein, we explore a "peel-and-stick" approach, where a nonlayered 3D platinum sulfide (PtS) crystal, traditionally known as a cooperate mineral material, is transformed into a freestanding 2D-like membrane for electromechanical applications. The ultrathin (∼10 nm) 3D PtS films grown on large-area (>cm2) silicon dioxide/silicon (SiO2/Si) wafers are precisely "peeled" inside water retaining desired geometries via a capillary-force-driven surface wettability control. Subsequently, they are "sticked" on strain-engineered patterned substrates presenting prominent semiconducting properties, i.e., p-type transport with an optical band gap of ∼1.24 eV. A variety of mechanically deformable strain-invariant electronic devices have been demonstrated by this peel-and-stick method, including biaxially stretchable photodetectors and respiratory sensing face masks. This study offers new opportunities of 2D-like nonlayered semiconducting crystals for emerging mechanically reconfigurable and stretchable device technologies.

Crack-Bridging Property Evaluation of Synthetic Polymerized Rubber Gel (SPRG) through Yield Stress Parameter Identification.

Yield stress parameter derivation was conducted by stress-strain curve analysis on four types of grout injection leakage repair materials (GILRM); acrylic, epoxy, urethane and SPRG grouts. Comparative stress-strain curve analysis results showed that while the yield stress point was clearly distinguishable, the strain ratio of SPRG reached up to 664% (13 mm) before material cohesive failure. A secondary experimental result comprised of three different common component ratios of SPRG was conducted to derive and propose an averaged yield stress curve graph, and the results of the yield stress point (180% strain ratio) were set as the basis for repeated stress-strain curve analysis of SPRGs of up to 15 mm displacement conditions. Results showed that SPRG yield stress point remained constant despite repeated cohesive failure, and the modulus of toughness was calculated to be on average 53.1, 180.7, and 271.4 N/mm2, respectively, for the SPRG types. The experimental results of this study demonstrated that it is possible to determine the property limits of conventional GILRM (acrylic, epoxy and urethane grout injection materials) based on yield stress. The study concludes with a proposal on potential application of GILRM toughness by finite element analysis method whereby strain of the material can be derived by hydrostatic pressure. Comparative analysis showed that the toughness of SPRG materials tested in this study are all able to withstand hydrostatic pressure range common to underground structures (0.2 N/mm2). It is expected that the evaluation method and model proposed in this study will be beneficial in assessing other GILRM materials based on their toughness values.

Strain Concentration Ratio Analysis of Different Waterproofing Materials during Concrete Crack Movement.

When a crack occurs under an installed waterproofing material and moves due to environmental effects (freeze-thaw, settlement, vibration, dead load, etc.), waterproofing materials without adequate elongation or tensile strength properties may break and tear. To enable the selection of materials with proper response against the strain that occur during crack movement, this study proposes and demonstrates a new evaluation method for determining and comparing strain concentration of waterproofing materials under the effect of concrete crack movement. For the proposed testing method and demonstration, three common types of waterproofing material types were selected for testing, poly-urethane coating (PUC), self-adhesive asphalt sheet (SAS) and composite asphalt sheet (CAS). Respective materials are installed with strain gauges and applied onto a specimen with a separated joint that undergoes concrete crack movement simulation. Each specimen types are subject to repeated movement cycles, whereby strain occurring directly above the moving joint is measured and compared with the strain occurring at the localized sections (comparison ratio which is hereafter referred to as strain concentration ratio). Specimens are tested under four separate movement length conditions, 1.5 mm, 3.0 mm, 4.5 mm and 6.0 mm, and the results are compared accordingly. Experimental results show that materials with strain concentration ratio from highest to lowest are as follows: PUC, SAS and CAS.

Mechanically rollable photodetectors enabled by centimetre-scale 2D MoS2 layer/TOCN composites.

Two-dimensional (2D) molybdenum disulfide (MoS2) layers are suitable for visible-to-near infrared photodetection owing to their tunable optical bandgaps. Also, their superior mechanical deformability enabled by an extremely small thickness and van der Waals (vdW) assembly allows them to be structured into unconventional physical forms, unattainable with any other materials. Herein, we demonstrate a new type of 2D MoS2 layer-based rollable photodetector that can be mechanically reconfigured while maintaining excellent geometry-invariant photo-responsiveness. Large-area (>a few cm2) 2D MoS2 layers grown by chemical vapor deposition (CVD) were integrated on transparent and flexible substrates composed of 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO)-oxidized cellulose nanofibers (TOCNs) by a direct solution casting method. These composite materials in three-dimensionally rollable forms exhibited a large set of intriguing photo-responsiveness, well preserving intrinsic opto-electrical characteristics of the integrated 2D MoS2 layers; i.e., light intensity-dependent photocurrents insensitive to illumination angles as well as highly tunable photocurrents varying with the rolling number of 2D MoS2 layers, which were impossible to achieve with conventional photodetectors. This study provides a new design principle for converting 2D materials to three-dimensional (3D) objects of tailored functionalities and structures, significantly broadening their potential and versatility in futuristic devices.

Direct recovery of spilled oil using hierarchically porous oil scoop with capillary-induced anti-oil-fouling.

The pitcher plant has evolved its hierarchically grooved peristome to enhance a water-based slippery system for capturing insects with oil-covered footpads. Based on this, we proposed a hierarchically porous oil scoop (HPOS) with capillary-induced oil peel-off ability for repeatable spilled oil recovery. As the HPOS scoops oil-water mixture, water passes through the hole while the oil is confined within a curved geometry. The filter in HPOS has three levels of porous structures; (1) 3D-printed mesh structure with sub-millimeter scale hole to filter out oil from an oil-water mixture, (2) internal micropore in fibers enhancing capillarity and water transport, (3) O2 plasma-induced high-aspect-ratio nanopillar structures imposing anti-oil-fouling property with capillary-induced oil peeling. As the oil-contaminated HPOS makes contact with water, water meniscus rises and peels off the oil immediately at the air-water interface. The oil-peel-off ability of the HPOS would prevent pores from clogging by oils for reuse. The study demonstrated that the HPOS recovers highly viscous oil (up to 5000 mm2·s-1) with a high recovery rate (>95%), leaving the filtered water with low oil content (<10 ppm), which satisfies the discharge criterion of 15 ppm.

Metallophobic Coatings to Enable Shape Reconfigurable Liquid Metal Inside 3D Printed Plastics.

Liquid metals adhere to most surfaces despite their high surface tension due to the presence of a native gallium oxide layer. The ability to change the shape of functional fluids within a three-dimensional (3D) printed part with respect to time is a type of four-dimensional printing, yet surface adhesion limits the ability to pump liquid metals in and out of cavities and channels without leaving residue. Rough surfaces prevent adhesion, but most methods to roughen surfaces are difficult or impossible to apply on the interior of parts. Here, we show that silica particles suspended in an appropriate solvent can be injected inside cavities to coat the walls. This technique creates a transparent, nanoscopically rough (10-100 nm scale) coating that prevents adhesion of liquid metals on various 3D printed plastics and commercial polymers. Liquid metals roll and even bounce off treated surfaces (the latter occurs even when dropped from heights as high as 70 cm). Moreover, the coating can be removed locally by laser ablation to create selective wetting regions for metal patterning on the exterior of plastics. To demonstrate the utility of the coating, liquid metals were dynamically actuated inside a 3D printed channel or chamber without pinning the oxide, thereby demonstrating electrical circuits that can be reconfigured repeatably.

Two-Dimensional Near-Atom-Thickness Materials for Emerging Neuromorphic Devices and Applications.

Two-dimensional (2D) layered materials and their heterostructures have recently been recognized as promising building blocks for futuristic brain-like neuromorphic computing devices. They exhibit unique properties such as near-atomic thickness, dangling-bond-free surfaces, high mechanical robustness, and electrical/optical tunability. Such attributes unattainable with traditional electronic materials are particularly promising for high-performance artificial neurons and synapses, enabling energy-efficient operation, high integration density, and excellent scalability. In this review, diverse 2D materials explored for neuromorphic applications, including graphene, transition metal dichalcogenides, hexagonal boron nitride, and black phosphorous, are comprehensively overviewed. Their promise for neuromorphic applications are fully discussed in terms of material property suitability and device operation principles. Furthermore, up-to-date demonstrations of neuromorphic devices based on 2D materials or their heterostructures are presented. Lastly, the challenges associated with the successful implementation of 2D materials into large-scale devices and their material quality control will be outlined along with the future prospect of these emergent materials.

Vertically Aligned 2D MoS2 Layers with Strain-Engineered Serpentine Patterns for High-Performance Stretchable Gas Sensors: Experimental and Theoretical Demonstration.

Two-dimensional (2D) molybdenum disulfide (MoS2) with vertically aligned (VA) layers exhibits significantly enriched surface-exposed edge sites with an abundance of dangling bonds owing to its intrinsic crystallographic anisotropy. Such structural variation renders the material with exceptionally high chemical reactivity and chemisorption ability, making it particularly attractive for high-performance electrochemical sensing. This superior property can be further promoted as far as it is integrated on mechanically stretchable substrates well retaining its surface-exposed defective edges, projecting opportunities for a wide range of applications utilizing its structural uniqueness and mechanical flexibility. In this work, we explored VA-2D MoS2 layers configured in laterally stretchable forms for multifunctional nitrogen dioxide (NO2) gas sensors. Large-area (>cm2) VA-2D MoS2 layers grown by a chemical vapor deposition (CVD) method were directly integrated onto a variety of flexible substrates with serpentine patterns judiciously designed to accommodate a large degree of tensile strain. These uniquely structured VA-2D MoS2 layers were demonstrated to be highly sensitive to NO2 gas of controlled concentration preserving their intrinsic structural and chemical integrity, e.g., significant current response ratios of ∼160-380% upon the introduction of NO2 at a level of 5-30 ppm. Remarkably, they exhibited such a high sensitivity even under lateral stretching up to 40% strain, significantly outperforming previously reported 2D MoS2 layer-based NO2 gas sensors of any structural forms. Underlying principles for the experimentally observed superiority were theoretically unveiled by density functional theory (DFT) calculation and finite element method (FEM) analysis. The intrinsic high sensitivity and large stretchability of VA-2D MoS2 layers confirmed in this study are believed to be applicable in sensing diverse gas species, greatly broadening their versatility in stretchable and wearable technologies.

Joint- or Crack-Opening Resistance Evaluation of Waterproofing Material and System for Structural Sustainability in Railroad Bridge Deck.

A joint- or crack-opening resistance evaluation method for the selection of optimal waterproofing material for a railroad bridge deck is proposed. The joint opening range (mm) for the evaluation, and a typical load case of a high-speed double-track railroad bridge structure deck, is analyzed through the finite element method (FEM) and the results of analysis are used to calculate the minimum opening range. The evaluation method is then demonstrated with 4 commonly used waterproofing types of cementitious membrane system: a polyurethane coating system, self-adhesive asphalt sheet system and synthetic polymerized rubber gel composite asphalt sheet system. Five specimens of each type are subjected to continuous joint opening under 4 different joint width range conditions (1.5, 3.0, 4.5, and 6.0 mm), and the joint-opening resistance performance is compared. The proposal for the evaluation criteria and the specimen test results demonstrate how the evaluation method is pertinent for future selection of waterproofing membranes for the sustainability of high-speed railroad bridge deck structures.

An Implantable Ionic Wireless Power Transfer System Facilitating Electrosynthesis.

A number of implantable biomedical devices have been developed, and wireless power transfer (WPT) systems are emerging as a way to provide power to these devices without requiring a hardwired connection. Most of the WPT has been based on conventional conductive materials, such as metals, which tend to be less biocompatible and stiff. Herein, we describe a development of an ionic wireless power transfer (IWPT) system using hydrogel receivers that are soft and biocompatible. Although the hydrogel receiver has a lower conductivity than metal (ρgel/ρmetal ∼ 10-7), a capacitive coupling between receiver and transmitter enables the IWPT to deliver 4 mA of current at its resonance frequency. The capacitive coupling through the dielectric and the electrolyte was analyzed including a parasitic effect, and the IWPT was applied to implantable devices to transfer power via the skin. The IWPT system was further developed to facilitate electrosynthesis. Generation of nicotinamide adenine dinucleotide phosphate, a reducing agent in metabolism, was demonstrated by IWPT to show its potential for electrosynthesis.

Wafer-Scale Two-Dimensional MoS2 Layers Integrated on Cellulose Substrates Toward Environmentally Friendly Transient Electronic Devices.

We explored the feasibility of wafer-scale two-dimensional (2D) molybdenum disulfide (MoS2) layers toward futuristic environmentally friendly electronics that adopt biodegradable substrates. Large-area (> a few cm2) 2D MoS2 layers grown on silicon dioxide/silicon (SiO2/Si) wafers were delaminated and integrated onto a variety of cellulose-based substrates of various components and shapes in a controlled manner; examples of the substrates include planar papers, cylindrical natural rubbers, and 2,2,6,6-tetramethylpiperidine-1-oxyl-oxidized cellulose nanofibers. The integrated 2D layers were confirmed to well preserve their intrinsic structural and chemical integrity even on such exotic substrates. Proof-of-concept devices employing large-area 2D MoS2 layers/cellulose substrates were demonstrated for a variety of applications, including photodetectors, pressure sensors, and field-effect transistors. Furthermore, we demonstrated the complete "dissolution" of the integrated 2D MoS2 layers in a buffer solution composed of baking soda and deionized water, confirming their environmentally friendly transient characteristics. Moreover, the approaches to delaminate and integrate them do not demand any chemicals except for water, and their original substrates can be recycled for subsequent growths, ensuring excellent chemical benignity and process sustainability.

Wafer-scale 2D PtTe2 layers for high-efficiency mechanically flexible electro-thermal smart window applications.

Two-dimensional (2D) transition metal dichalcogenide (TMD) layers have gained increasing attention for a variety of emerging electrical, thermal, and optical applications. Recently developed metallic 2D TMD layers have been projected to exhibit unique attributes unattainable in their semiconducting counterparts; e.g., much higher electrical and thermal conductivities coupled with mechanical flexibility. In this work, we explored 2D platinum ditelluride (2D PtTe2) layers - a relatively new class of metallic 2D TMDs - by studying their previously unexplored electro-thermal properties for unconventional window applications. We prepared wafer-scale 2D PtTe2 layer-coated optically transparent and mechanically flexible willow glasses via a thermally-assisted tellurization of Pt films at a low temperature of 400 °C. The 2D PtTe2 layer-coated windows exhibited a thickness-dependent optical transparency and electrical conductivity of >106 S m-1 - higher than most of the previously explored 2D TMDs. Upon the application of electrical bias, these windows displayed a significant increase in temperature driven by Joule heating as confirmed by the infrared (IR) imaging characterization. Such superior electro-thermal conversion efficiencies inherent to 2D PtTe2 layers were utilized to demonstrate various applications, including thermochromic displays and electrically-driven defogging windows accompanying mechanical flexibility. Comparisons of these performances confirm the superiority of the wafer-scale 2D PtTe2 layers over other nanomaterials explored for such applications.

Automated Assembly of Wafer-Scale 2D TMD Heterostructures of Arbitrary Layer Orientation and Stacking Sequence Using Water Dissoluble Salt Substrates.

We report a novel strategy to assemble wafer-scale two-dimensional (2D) transition metal dichalcogenide (TMD) layers of well-defined components and orientations. We directly grew a variety of 2D TMD layers on "water-dissoluble" single-crystalline salt wafers and precisely delaminated them inside water in a chemically benign manner. This manufacturing strategy enables the automated integration of vertically aligned 2D TMD layers as well as 2D/2D heterolayers of arbitrary stacking orders on exotic substrates insensitive to their kind and shape. Furthermore, the original salt wafers can be recycled for additional growths, confirming high process sustainability and scalability. The generality and versatility of this approach have been demonstrated by developing proof-of-concept "all 2D" devices for diverse yet unconventional applications. This study is believed to shed a light on leveraging opportunities of 2D TMD layers toward achieving large-area mechanically reconfigurable devices of various form factors at the industrially demanded scale.

Thickness-Independent Semiconducting-to-Metallic Conversion in Wafer-Scale Two-Dimensional PtSe2 Layers by Plasma-Driven Chalcogen Defect Engineering.

Platinum diselenide (PtSe2) is an emerging class of two-dimensional (2D) transition-metal dichalcogenide (TMD) crystals recently gaining substantial interest, owing to its extraordinary properties absent in conventional 2D TMD layers. Most interestingly, it exhibits a thickness-dependent semiconducting-to-metallic transition, i.e., thick 2D PtSe2 layers, which are intrinsically metallic, become semiconducting with their thickness reduced below a certain point. Realizing both semiconducting and metallic phases within identical 2D PtSe2 layers in a spatially well-controlled manner offers unprecedented opportunities toward atomically thin tailored electronic junctions, unattainable with conventional materials. In this study, beyond this thickness-dependent intrinsic semiconducting-to-metallic transition of 2D PtSe2 layers, we demonstrate that controlled plasma irradiation can "externally" achieve such tunable carrier transports. We grew wafer-scale very thin (a few nm) 2D PtSe2 layers by a chemical vapor deposition (CVD) method and confirmed their intrinsic semiconducting properties. We then irradiated the material with argon (Ar) plasma, which was intended to make it more semiconducting by thickness reduction. Surprisingly, we discovered a reversed transition of semiconducting to metallic, which is opposite to the prediction concerning their intrinsic thickness-dependent carrier transports. Through extensive structural and chemical characterization, we identified that the plasma irradiation introduces a large concentration of near-atomic defects and selenium (Se) vacancies in initially stoichiometric 2D PtSe2 layers. Furthermore, we performed density functional theory (DFT) calculations and clarified that the band-gap energy of such defective 2D PtSe2 layers gradually decreases with increasing defect concentration and dimensions, accompanying a large number of midgap energy states. This corroborative experimental and theoretical study decisively verifies the fundamental mechanism for this externally controlled semiconducting-to-metallic transition in large-area CVD-grown 2D PtSe2 layers, greatly broadening their versatility for futuristic electronics.

Wafer-Scale Growth of 2D PtTe2 with Layer Orientation Tunable High Electrical Conductivity and Superior Hydrophobicity.

Platinum ditelluride (PtTe2) is an emerging semimetallic two-dimensional (2D) transition-metal dichalcogenide (TMDC) crystal with intriguing band structures and unusual topological properties. Despite much devoted efforts, scalable and controllable synthesis of large-area 2D PtTe2 with well-defined layer orientation has not been established, leaving its projected structure-property relationship largely unclarified. Herein, we report a scalable low-temperature growth of 2D PtTe2 layers on an area greater than a few square centimeters by reacting Pt thin films of controlled thickness with vaporized tellurium at 400 °C. We systematically investigated their thickness-dependent 2D layer orientation as well as its correlated electrical conductivity and surface property. We unveil that 2D PtTe2 layers undergo three distinct growth mode transitions, i.e., horizontally aligned holey layers, continuous layer-by-layer lateral growth, and horizontal-to-vertical layer transition. This growth transition is a consequence of competing thermodynamic and kinetic factors dictated by accumulating internal strain, analogous to the transition of Frank-van der Merwe (FM) to Stranski-Krastanov (SK) growth in epitaxial thin-film models. The exclusive role of the strain on dictating 2D layer orientation has been quantitatively verified by the transmission electron microscopy (TEM) strain mapping analysis. These centimeter-scale 2D PtTe2 layers exhibit layer orientation tunable metallic transports yielding the highest value of ∼1.7 × 106 S/m at a certain critical thickness, supported by a combined verification of density functional theory (DFT) and electrical measurements. Moreover, they show intrinsically high hydrophobicity manifested by the water contact angle (WCA) value up to ∼117°, which is the highest among all reported 2D TMDCs of comparable dimensions and geometries. Accordingly, this study confirms the high material quality of these emerging large-area 2D PtTe2 layers, projecting vast opportunities employing their tunable layer morphology and semimetallic properties from investigations of novel quantum phenomena to applications in electrocatalysis.

Evaluation Method of Relative Humidity Changes in Below-Grade Concrete Structure Space Depending on Different Waterproofing Material and Installation Method.

An evaluation method for assessing the difference in the relative humidity (RH) control performance of waterproofing material is proposed. For a demonstration of this evaluation method, two waterproofing materials (urethane coating and cementitious waterproofing material) installed with different methods (positive and negative side of concrete structure respectively) are exposed to temperature conditions representing three seasonal conditions: Summer (40 °C), spring/autumn (20 °C) and winter (4 °C). Condensation level changes on the inner side of the waterproofing material installed specimen is measured, and for derive criteria for comparison, three parameters based on the average RH, intercept RH (derived from a linear regression analysis of RH measurement), and maximum relative humidity are derived for each different waterproofing material installed specimen. Based on quality specification for underground concrete structures, the demonstration evaluation establishes provisional standard criteria of below 70% RH, and all three parameters are evaluated to determine whether the tested waterproofing material/method complies to the performance requirement. Additional analysis through linear regression and cumulative probability density graphs are derived to evaluate the RH consistency and range parameters. The evaluation regime demonstrates a quantitative RH analysis method and apparatus, and a newly designed evaluation criteria is used to compare the RH control performance of positive-side installed urethane waterproofing materials and negative-side installed cementitious waterproofing material.

Single-step plasma-induced hierarchical structures for tunable water adhesion.

Smart surfaces in nature have been extensively studied to identify their hierarchical structures in micro-/nanoscale to elucidate their superhydrophobicity with varying water adhesion. However, mimicking hybrid features in multiscale requires complex, multi-step processes. Here, we proposed a one-step process for the fabrication of hierarchical structures composed in micro-/nanoscales for superhydrophobic surfaces with tunable water adhesion. Hierarchical patterns were fabricated using a plasma-based selective etching process assisted by a dual scale etching mask. As the metallic mesh is placed above the substrate, it serves the role of dual scale etching masks on the substrate: microscale masks to form the micro-wall network and nanoscale masks to form high-aspect-ratio nanostructures. The micro-walls and nanostructures can be selectively hybridized by adjusting the gap distance between the mesh and the target surface: single nanostructures on a large area for a larger gap distance and hybrid/hierarchical structures with nanostructures nested on micro-walls for a shorter gap distance. The hierarchically nanostructured surface shows superhydrophobicity with low water adhesion, while the hybrid structured surface becomes become superhydrophobic with high adhesion. These water adhesion tunable surfaces were explored for water transport and evaporation. Additionally, we demonstrated a robust superhydrophobic surface with anti-reflectance over a large area.

Multiple air-bubble enhanced oil rupture on nanostructured cellulose fabric for easy-oil cleaning fouled in a dry state.

Nanostructured cellulose fabric with an air-bubble-enhanced anti-oil fouling property is introduced for quick oil-cleaning by water even with the surface fouled by oil before water contact under a dry state. It is very challenging to recover the super-hydrophilicity because once the surface is oil-fouled, it is hard to be re-wetted by water. Anti-oil-fouling under a dry state was realized through two main features of the nanostructured, porous fabric: a low solid fraction with high-aspect-ratio nanostructures significantly increasing the retracting forces, and trapped multiscale air bubbles increasing the buoyancy and backpressure for an oil-layer rupture. The nanostructures were formed on cellulose-based rayon microfibers through selective etching with oxygen plasma, forming a nanoscale open-pore structure. Viscous crude oil fouled on a fabric under a dry state was cleaned by immersion into water owing to a higher water affinity of the rayon material and low solid fraction of the high-aspect-ratio nanostructures. Air bubbles trapped in dry porous fibers and nanostructures promote oil detachment from the fouled sites. The macroscale bubbles add buoyancy on top of the oil droplets, enhancing the oil receding at the oil-water-solid interface, whereas the relatively smaller microscale bubbles induce a backpressure underneath the oil droplets. The oil-proofing fabric was used for protecting underwater conductive sensors, allowing a robot fish to swim freely in oily water.

Experimental Realization of Few Layer Two-Dimensional MoS2 Membranes of Near Atomic Thickness for High Efficiency Water Desalination.

A globally imminent shortage of freshwater has been demanding viable strategies for improving desalination efficiencies with the adoption of cost- and energy-efficient membrane materials. The recently explored 2D transition metal dichalcogenides (2D TMDs) of near atomic thickness have been envisioned to offer notable advantages as high-efficiency membranes owing to their structural uniqueness; that is, extremely small thickness and intrinsic atomic porosity. Despite theoretically projected advantages, experimental realization of near atom-thickness 2D TMD-based membranes and their desalination efficiency assessments have remained largely unexplored mainly due to the technical difficulty associated with their seamless large-scale integration. Herein, we report the experimental demonstration of high-efficiency water desalination membranes based on few-layer 2D molybdenum disulfide (MoS2) of only ∼7 nm thickness. Chemical vapor deposition (CVD)-grown centimeter-scale 2D MoS2 layers were integrated onto porous polymeric supports with well-preserved structural integrity enabled by a water-assisted 2D layer transfer method. These 2D MoS2 membranes of near atomic thickness exhibit an excellent combination of high water permeability (>322 L m-2 h-1 bar-1) and high ionic sieving capability (>99%) for various seawater salts including Na+, K+, Ca2+, and Mg2+ with a range of concentrations. Moreover, they present near 100% salt ion rejection rates for actual seawater obtained from the Atlantic coast, significantly outperforming the previously developed 2D MoS2 layer membranes of micrometer thickness as well as conventional reverse osmosis (RO) membranes. Underlying principles behind such remarkably excellent desalination performances are attributed to the intrinsic atomic vacancies inherent to the CVD-grown 2D MoS2 layers as verified by aberration-corrected electron microscopy characterization.

Multifunctional Two-Dimensional PtSe2-Layer Kirigami Conductors with 2000% Stretchability and Metallic-to-Semiconducting Tunability.

Two-dimensional transition-metal dichalcogenide (2D TMD) layers are highly attractive for emerging stretchable and foldable electronics owing to their extremely small thickness coupled with extraordinary electrical and optical properties. Although intrinsically large strain limits are projected in them (i.e., several times greater than silicon), integrating 2D TMDs in their pristine forms does not realize superior mechanical tolerance greatly demanded in high-end stretchable and foldable devices of unconventional form factors. In this article, we report a versatile and rational strategy to convert 2D TMDs of limited mechanical tolerance to tailored 3D structures with extremely large mechanical stretchability accompanying well-preserved electrical integrity and modulated transport properties. We employed a concept of strain engineering inspired by an ancient paper-cutting art, known as kirigami patterning, and developed 2D TMD-based kirigami electrical conductors. Specifically, we directly integrated 2D platinum diselenide (2D PtSe2) layers of controlled carrier transport characteristics on mechanically flexible polyimide (PI) substrates by taking advantage of their low synthesis temperature. The metallic 2D PtSe2/PI kirigami patterns of optimized dimensions exhibit an extremely large stretchability of ∼2000% without compromising their intrinsic electrical conductance. They also present strain-tunable and reversible photoresponsiveness when interfaced with semiconducting carbon nanotubes (CNTs), benefiting from the formation of 2D PtSe2/CNT Schottky junctions. Moreover, kirigami field-effect transistors (FETs) employing semiconducting 2D PtSe2 layers exhibit tunable gate responses coupled with mechanical stretching upon electrolyte gating. The exclusive role of the kirigami pattern parameters in the resulting mechanoelectrical responses was also verified by a finite-element modeling (FEM) simulation. These multifunctional 2D materials in unconventional yet tailored 3D forms are believed to offer vast opportunities for emerging electronics and optoelectronics.