Large Lateral Size Research Articles

Wafer-Sized CsPbBr3/CsPbCl3 Heterojunction: Breaking the Trade-Off between Sensitivity and Dark Current for Efficient X-ray Detector.

Polycrystalline lead halide perovskite finds promising use in fabricating X-ray detectors with a large lateral size, adjustable thickness, and diverse synthesis processes. However, a large dark current hinders its development for weak signal detection. Herein, we propose a multistep pressing strategy for manufacturing a CsPbBr3/CsPbCl3 heterojunction wafer for a reduced dark current X-ray detector, and the device keeps a high sensitivity value after the insertion of a barrier by heterojunction; thus, the trade-off between sensitivity and dark current can be broken. The X-ray detector with a metal-semiconductor-metal structure yields a sensitivity of 6.32 × 104 μC Gyair-1 cm-2 at a bias of 12 V, a 1/f noise of 1.02 × 10-13 A/Hz-1/2, and a detection limit of 66.58 nGy s-1. These performance parameters are considerably better than those of a similar X-ray detector based on the single-structure wafer. The improved device performance of the heterostructure X-ray detector is ascribed to the suppressed carrier recombination, enhanced carrier transportation of the heterojunction, and strong X-ray attenuation of the CsPbCl3 layer. The pixel array device is further used in imaging applications. Hence, this study provides an efficient strategy for fabricating heterostructure polycrystalline lead halide perovskite wafers for use in high-performance wafer-based X-ray detectors.

Fabrication of Self-Assembled Graphene Oxide Film and Its Application in Aqueous Zinc Metal Batteries.

Fabrication of well-dispersed thin graphene oxide (GO) films (GOFs) has always been a challenge. Herein, a quick preparation method for GOFs was developed using our homemade GO with a large lateral size. The film can be prepared in less than 2 h via a metal framework-induced self-assembly process. The thickness of the films can be as thin as ∼15.5 μm, which will be thinner with compression. When it is used as a flexible modification layer on the Zn metal for aqueous Zn-ion batteries, Zn can grow along the [010] direction in plane and stack orderly along the [002] direction even on the Cu substrate with GOF through epitaxial plating owing to negligible lattice mismatch between the (002) plane of Zn and the hexagonal ring [also (002) plane for graphite] of GO. Meanwhile, the rich O groups on the GO film can provide abundant zincophilic points and promote uniform distribution of Zn2+ around the anode. Finally, dendrite-free and dense Zn stripping/plating can be achieved and well remained. The GOF@Zn symmetric cell reveals long cyclic stability of 1300 h at 1 mA cm-2 and 1 mA h cm-2. It still can remain at 350 h even at a very high current density of 10 mA cm-2 accompanied by a high areal capacity of 10 mA h cm-2. With the same plating amount of 5 mA h cm-2, the thickness of the plated Zn is only ∼10 μm with GOF modification, very close to the theoretical value of 8.54 μm, much thinner than that without GOF (∼18 μm), indicating very dense deposition. Full cells assembled with the GOF@Zn anode and the MnO2 cathode exhibit a capacity retention rate of 71% over 1000 cycles at 0.7 A g-1, showing much better cycling performance than that using bare Zn.

Dimethyl sulfoxide dispersion of aramid nanofibers: An excellent medium for exfoliating high-quality boron nitride nanosheets towards heat spreading films with high thermal conductivity

Herein, we used dimethyl sulfoxide (DMSO) dispersion of aramid nanofibers (ANFs) as medium to exfoliate boron nitride nanosheets (BNNSs) from their bulk materials via a ball-milling route. The obtained BNNSs displayed large lateral sizes and were very clean without any contaminants. When milling under a high energy condition, many small-area nanosheets were appeared but the sample produced with high ANF concentration could still contain more large-size BNNSs. It was concluded that the DMSO is a good exfoliating medium for BNNSs due to the suitable viscosity, molecular weight, and polarity, while the introduction of ANFs can further improve the exfoliated sizes of BNNSs because of the buffering to impacting forces of milling balls. The ANF/BNNS composite exfoliated under high energy ball-milling and high ANF concentration gained the highest in-plane thermal conductivity of 27.23 W m−1 K−1 since the densified microstructure and the high dispersity, large lateral size, and high horizontal orientation of BNNSs.

Machine learning method for roughness prediction

This work aims to employ machine-learning models, specifically neural networks, to predict the time evolution of the global surface roughness in a lattice model that represents a film growing on a d-dimensional substrate. We analyze the well-known ballistic deposition (BD) model for d=1, 2 since it presents strong corrections to the scaling, making it difficult to observe directly, via effective scaling exponents, its correspondence with the Kardar-Parisi-Zhang (KPZ) universality class. As an alternative to overcome this difficulty, we first intend to learn the time evolution of the global roughness for substrate sizes that are computationally viable to simulate. To test the learning, we apply two different methodologies for d = 1: the first one learns the Family-Vicsek scaling relation, and by doing the reverse transformation, we get the global roughness as a function of the time, and the second one learns the kinetic roughening directly from the time series data. For growth in d = 2 where applications arise and no exact KPZ scaling exponents are known, we apply the second methodology. However, we employ a more resilient learning model tailored for time series problems. Hence, the time required to generate the same amount of data, showing the evolution of global roughness, is reduced dramatically. Importantly, machine learning techniques capture the scaling corrections of the BD model, predicting an effective global roughness exponent, α, calculated from the learned data extracted from very large lateral sizes and times that cannot be simulated using lattice models. Our prediction is consistent with accurate estimates of the KPZ roughness exponent reported in the literature for d = 2.

Transition metal catalysts coordinated with electrochemistry for preparation of graphene

It is still crucial to produce mass high-quality graphene through simple and low-cost methods for its wide applications. Herein, a simple and fast method by combining inexpensive transition metal catalysts with electrochemistry to exfoliate natural flake graphite is reported. The electrode is prepared in a sandwich structure, where the titanium mesh will enwrap the nickel net coated with graphite powder. This method can quickly achieve the large-scale preparation of graphene within 15 min. The quality of graphene with large lateral size and few layers has been characterized by XRD, SEM, TEM, Raman, and AFM. The possible electrochemical exfoliation mechanism has been proposed. Oxygen evolution reaction occurs at the anode due to the transition metal catalysts, and hydrogen ions (H+) are generated along with oxygen, H+ and SO42− ions will form a local strong acid. The formation of strong acidic H2SO4 in-situ around electrode will oxidize the edge of the graphite, allowing the intercalation of SO42−, H2O, SO2 and O2 into the graphite sheets, which will inflate the graphite and exfoliate of graphite into graphene. This strategy is reliable, environmentally friendly, and suitable for industrial production.

Comparative study of sodium and potassium compounds as promoters for growth of monolayer MoS2 with high crystal quality on SiO2/Si substrate

Monolayer MoS2 is promising candidate for fabrication of optoelectronic devices due to its direct bandgap nature and high carrier mobility. Alkali metal compounds have been demonstrated to be helpful promoters for the growth of large single crystal monolayer MoS2 on SiO2/Si substrate. However, the catalytic mechanism of alkali metal compounds is still under debate. Herein, we compared the surface morphology, optical properties, and electrical properties of monolayer MoS2 flakes grown on SiO2/Si substrate assisted by promoters containing potassium or sodium cations and halogen (chlorine) or non-halogen (hydroxide) anions, i.e. NaCl, NaOH, KCl and KOH. Based on the analysis of existing growth mechanism, we proposed that the alkali metal cation, plays a dominant role in promoting the lateral growth of monolayer MoS2 and obtaining high crystal quality. Furthermore, potassium has a greater promoting effect than sodium. By optimizing growth conditions, monolayer triangular MoS2 flakes with large lateral size over 160 μm were grown assisted by KCl promoter. Raman and PL spectra verified excellent crystal quality of the flakes, with typical electron mobilities of 2.98 and 20 cm2 V−1 s−1 for the back-gated filed effect transistors fabricated on as-grown and fresh SiO2/Si substrates, respectively.

Upscaling Brønsted acid intercalation and exfoliation of graphite into graphene by polyoxometalate clusters for sodium-ion battery application

Non-oxidative intercalation of graphite avoids damage to graphene lattices and is a suitable method to produce high-quality graphene. However, the yield of exfoliated graphene is low in this process due to the poor delamination efficiency of guest species. In this study, a Brønsted acid intercalation protocol is developed involving polyoxometalate (POM) clusters (H6P2W18O62) as guests and intercalation of graphite is realized at the sub-nanometer scale. Theoretical simulation based on DFT elucidates the stepwise intercalation mechanism of Brønsted acid molecules and clusters. Unlike common molecules/ionic guests, intercalation of POM clusters induces large expansion and extensive donor–acceptor interactions among graphite interlayers. This significantly weakens the van der Waals forces and promotes exfoliation efficiency of graphene layers. The exfoliated graphene possesses outstanding features of large lateral size, thin thickness, and high purity, and shows excellent performance as the anode for high power sodium-ion batteries. This work proffers a new pathway toward non-oxidative intercalation of graphite for large-scale production of graphene.

Microwave-Assisted Efficient Intercalation for Fast Fabrication of High-Quality and Large-Size Single-Layer Ti3C2Tx Nanosheets.

A novel microwave-assisted intercalation (MAI) strategy is proposed for fast and efficient intercalation of layered MXene to prepare large-size single-layer MXene. After LiF-HCl etching of Ti3AlC2, the as-prepared multi-layer Ti3C2Tx (M-T) are intercalated with Li3AlF6 as an intercalator and ethylene glycol (EG) as a solvent under microwave irradiation for 5min. Furthermore, the dispersed high-quality large-sized single-layer Ti3C2Tx (S-T) nanosheets with a thickness of 1.66nm and a large lateral size over 20µm are achieved with a yield of over 60% after a further ultrasonic delamination followed by electrostatic precipitation, acid washing, and calcination. In addition, Pd/S-T composite catalyst, which is constructed with Pd nanoparticles supported on the as-prepared S-T nanosheets, exhibits an excellent performance for rapid and efficient selective hydrogenation of nitroarenes with H2 under a mild condition. At room temperature, full conversion of nitrobenzene and 100% aniline selectivity are achieved over Pd/S-T catalyst in 20min with 0.5MPa of H2 pressure. This work provides a novel method for facile, fast, and large-scale preparation of single-layer MXene and develops a new approach for constructing efficient nanocatalytic systems.

Fiber Optic Sensor Coated with Multiple Layers of Hexagonal Boron Nitride Nanosheets (BNNS) for the Detection of Volatile Organic Compounds.

Nowadays, volatile organic compound (VOC) detection is imperative to ensure environmental safety in industry and indoor environments, as well as to monitor human health in medical diagnosis. Gas sensors with the best sensor response, selectivity, and stability are in high demand. Simultaneously, the advancement of nanotechnology facilitates novel nanomaterial-based gas sensors with superior sensor characteristics and low power consumption. Recently, boron nitride, a 2D material, has emerged as an excellent candidate for gas sensing and demonstrated exceptional sensing characteristics for new-generation gas sensing devices. Herein, ultrathin porous boron nitride nanosheets (BNNSs) with large lateral sizes were synthesized using a facile synthesis approach, and their material characteristics were investigated utilizing a variety of analytical techniques, including X-ray diffraction, Fourier transform infrared spectroscopy, ultraviolet spectroscopy, X-ray photoelectron spectroscopy, and scanning electron microscopy. A BNNS-coated cladding-modified fiber optic sensor (FOS) probe was prepared and employed for VOC (ammonia, ethanol, and acetone) sensing across concentrations varying from 0 to 300 ppm. The BNNSs-coated FOS demonstrated better selectivity toward 300 ppm ammonia, and specifically annealed BNNSs displayed a maximum sensor response of 55% along with a response/recovery times of 15 s/34 s compared to its counterparts. The superior ammonia sensing performances could be attributed to the formation of ultrathin nanosheets and a porous surface with slit-like features in hexagonal boron nitride.

Observation of Mermin-Wagner behavior in LaFeO3/SrTiO3 superlattices

Two-dimensional magnetic materials can exhibit new magnetic properties due to the enhanced spin fluctuations that arise in reduced dimension. However, the suppression of the long-range magnetic order in two dimensions due to long-wavelength spin fluctuations, as suggested by the Mermin-Wagner theorem, has been questioned for finite-size laboratory samples. Here we study the magnetic properties of a dimensional crossover in superlattices composed of the antiferromagnetic LaFeO3 and SrTiO3 that, thanks to their large lateral size, allowed examination using a sensitive magnetic probe — muon spin rotation spectroscopy. We show that the iron electronic moments in superlattices with 3 and 2 monolayers of LaFeO3 exhibit a static antiferromagnetic order. In contrast, in the superlattices with single LaFeO3 monolayer, the moments do not order and fluctuate to the lowest measured temperature as expected from the Mermin-Wagner theorem. Our work shows how dimensionality can be used to tune the magnetic properties of ultrathin films.

Additive-Free Anode with High Stability: Nb2CTx MXene Prepared by HCl-LiF Hydrothermal Etching for Lithium-Ion Batteries.

MXenes, represented by Ti3C2Tx, have been widely studied in the electrochemical energy storage fields, including lithium-ion batteries, for their unique two-dimensional structure, tunable surface chemistry, and excellent electrical conductivity. Recently, Nb2CTx, as a new type of MXene, has attracted more and more attention due to its high theoretical specific capacity of 542 mAh g-1. However, the preparation of few-layer Nb2CTx nanosheets with high-quality remains a challenge, which limits their research and application. In this work, high-quality few-layer Nb2CTx nanosheets with a large lateral size and a high conductivity of up to 500 S cm-1 were prepared by a simple HCl-LiF hydrothermal etching method, which is 2 orders of magnitude higher than that of previously reported Nb2CTx. Furthermore, from its aqueous ink, the viscosity-tunable organic few-layer Nb2CTx ink was prepared by HCl-induced flocculation and N-methyl-2-pyrrolidone treatment. When using the organic few-layer Nb2CTx ink as an additive-free anode of lithium-ion batteries, it showed excellent cycling performance with a reversible specific capacity of 524.0 mAh g-1 after 500 cycles at 0.5 A g-1 and 444.0 mAh g-1 after 5000 cycles at 1 A g-1. For rate performance, a specific capacity of 159.8 mAh g-1 was obtained at a high current density of 5 A g-1, and an excellent capacity retention rate of about 95.65% was achieved when the current density returned to 0.5 A g-1. This work presents a simple and scalable process for the preparation of high-quality Nb2CTx and its aqueous/organic ink, which demonstrates important application potential as electrodes for electrochemical energy storage devices.

On-Water Surface Synthesis of Vinylene-Linked Cationic Two-Dimensional Polymer Films as the Anion-Selective Electrode Coating.

Vinylene-linked two-dimensional polymers (V-2DPs) and their layer-stacked covalent organic frameworks (V-2D COFs) featuring high in-plane π-conjugation and robust frameworks have emerged as promising candidates for energy-related applications. However, current synthetic approaches are restricted to producing V-2D COF powders that lack processability, impeding their integration into devices, particularly within membrane technologies reliant upon thin films. Herein, we report the novel on-water surface synthesis of vinylene-linked cationic 2DPs films (V-C2DP-1 and V-C2DP-2) via Knoevenagel polycondensation, which serve as the anion-selective electrode coating for highly-reversible and durable zinc-based dual-ion batteries (ZDIBs). Model reactions and theoretical modeling revealed the enhanced reactivity and reversibility of the Knoevenagel reaction on the water surface. On this basis, we demonstrated the on-water surface 2D polycondensation towards V-C2DPs films that show large lateral size, tunable thickness, and high chemical stability. Representatively, V-C2DP-1 presents as a fully crystalline and face-on oriented film with in-plane lattice parameters of a=b≈43.3 Å. Profiting from its well-defined cationic sites, oriented 1D channels, and stable frameworks, V-C2DP-1 film possesses superior bis(trifluoromethanesulfonyl)imide anion (TFSI-)-transport selectivity (transference, t_=0.85) for graphite cathode in high-voltage ZDIBs, thus triggering additional TFSI--intercalation stage and promoting its specific capacity (from ~83 to 124 mAh g-1) and cycling life (>1000 cycles, 95 % capacity retention).

Synthese an der Wasseroberfläche von Vinylen‐Verbundenen Kationischen Zwei‐Dimensionalen Polymerfilmen als Beschichtung für Anion‐Selektive Elektroden

AbstractVinylen verbrückte zwei‐dimensionale Polymere (V‐2DPs) und deren schichtgestapelten kovalent organische Gerüstverbindungen (V‐2D COFs) zeichnen sich durch ihre hohe π‐Konjugation in der Ebene und ihre robuste Struktur als vielversprechnende Kanidaten für energiebezogene Anwendungen aus. Allerdings sind derzeitige syntheisische Ansätze auf die Herstellung von V‐2D COF Pulver beschränkt, welche schlecht prozessierbar sind, was die Integration in Geräte, insbesondere für Membranthechnologien, welche auf dünnen Filmen beruhen erschwert. Im folgenden berichten wir über die neu‐artige Synthese von kationischen 2DPs‐Filmen an der Wasseroberfläche, die über Vinyleneinheiten verbrückt sind (V‐C2DP‐1 und V‐C2DP‐2) mittels Knoevenagel‐Polykondensation, diese dienen als anionenselektive Elektrodenbeschichtung für hochreversible und langlebige Zink‐basierte Dual‐Ionen‐Batterien (ZDIBs). Modellreaktionen und theoretische Modellierung zeigen eine erhöte Reaktivität und Reversibilität der Knoevenagel‐Reaktion an der Wasseroberfläche an. Basierend darauf zeigten wir die 2D Polykondensation hin zu V‐C2DP‐Filmen an der Wasseroberfläche, welche eine weitreichen‐de laterale Größe, anpassbare Dicke und hohe chemischer Stabilität besitzen. Repräsentativ zeigt sich V‐C2DP‐1 als ein vollständig crystalliner und flächen‐orientierter Film mit den in der Ebene liegenden Gitterparametern von a=b≈43.3 Å. Dank der gut definierten katinoischen Funktionalitäten, orientierten 1D‐Kanälen und des sabilen Gerüstes besitzt der V‐C2DP‐1 Film eine herausragende Transportselektivität von Bis(trifluormethansulfon)imid‐anion (TFSI−) (Transferrate, t =0.85) für die Graphitkathode in Hochspannungs‐ZDIBs. Die hohe Selektivität führt zu zusätzlichen TFSI−‐Intercalationsstufen wodurch eine höhere spezifischen Kapazität (von ~83 bis 124 mAh g−1), sowie Zyklusdauer (>1000 Zyklen, 95 % Kapazitätserhaltung) gefördert wird.

Hummers' method-assisted liquid-phase exfoliation enables the fabrication of few-layer borophene from bulk boron.

The fabrication of few-layer borophene (BP) from bulk boron (b-B) is of great importance and still a scientific challenge due to the complex structure and crystallinity of b-B. Herein, we propose a novel technique to prepare a few-layer BP on a large scale with a large lateral size in a well-controlled manner. For this, we employed the Hummers' method-assisted liquid-phase exfoliation. In the first step, the chemical exfoliation of the b-B as a precursor was performed by the modified Hummers' method. After chemical exfoliation, mechanical delamination was employed by using an immersion sonicator. Finally, BP sheets were collected with dimensions ranging from several hundred nanometers to a few micrometers and an average thickness of 4.2 nm. We envision that the proposed low-cost, flexible, and large-scale production method will provide unique advantages for the application of few-layer BP in the realization of high-performance electronics, optoelectronics, flexible devices, sensing systems, energy conversion, and storage devices.

Solution-processed 2D van der Waals networks: Fabrication strategies, properties, and scalable device applications

Solution-based processing of two-dimensional (2D) materials has garnered significant interest as a facile and versatile route for the large-scalable production of 2D material films. Despite the benefits in process, these films were not considered suitable for device applications during the early stages of research because their electronic properties were far from those of 2D materials obtained through micromechanical exfoliation or chemical vapor deposition. Due to the small lateral dimensions and polydisperse thickness of constituent 2D nanosheets, the resulting film tends to be porous and exhibits numerous inter-sheet junctions, primarily contacting edge-to-edge. This nanosheet morphology leads to poor electrical conductivity of the network, and also hinders the film functioning as a semiconductor or an insulator. To produce ultrathin 2D nanosheets with narrow thickness distribution and large lateral sizes, various chemical exfoliation strategies have been explored, but these are limited by long process times, involvement of harsh chemicals, and/or undesired structural damage or phase changes. Recent breakthroughs in electrochemical exfoliation using tetraalkylammonium intercalants enabled the production of high-quality 2D nanosheets with structural characteristics favorable for producing ultrathin, conformal films of 2D materials, which allow for scalable production of high-performance electronic components that can readily be assembled into functional devices via solution-processing. In this review article, we aim to offer an extensive introduction solution-based processing techniques for acquiring 2D nanosheets, their subsequent assembly into thin films, and their diverse applications, primarily focusing on electronics and optoelectronics but also extending to other fields. Remaining challenges and potential avenues for advancement will also be discussed.

Smart epoxy coating: g-C3N4 nanosheets loaded MOFs for enhanced anti-corrosion and UV resistance

Large lateral size g-C3N4 nanosheets (Graphite-like carbon nitride) were successfully prepared by surface polymerization. NH2-MIL-101 (Amino-functionalized iron-based metal–organic framework) was then modified on the surface of g-C3N4 nanosheets (NH2-MIL-101@g-C3N4) by an in-situ loading method to construct a long-term smart coating with high barrier, activity inhibition, and anti-UV aging. This novel approach marks a significant advancement in the development of smart coatings for long-term corrosion protection. Evaluation of the active corrosion inhibition of NH2-MIL-101@g-C3N4 (MCN) nanoparticles showed that the corrosion inhibition efficiency of MCN nanoparticles on carbon steel reached 79.3 % after 5 h. The addition of MCN nanoparticles to the epoxy coatings (MCN/EP) endowed the coatings with the ability to actively inhibit corrosion. The release of Fe3+ cations and NH2-BDC (2-aminoterephthalic acid) organic ligands from MCN at defects formed a protective film, effectively preventing further corrosion. The MCN/EP coating maintained a high Log|Z|0.01 Hz value (Impedance modulus at a frequency of 0.01 Hz) during the immersion period with excellent barrier properties. Notably, MCN significantly improved the water resistance, water contact angle, tensile properties, and thermomechanical properties of epoxy coatings after ultraviolet (UV) radiation, highlighting a remarkable enhancement in the coating's performance. The anti-corrosion of MCN/EP coating was unaffected by UV radiation, extending service life of the smart coating, with Log|Z|0.01 Hz values two orders of magnitude higher than pure EP after 300 h of UV radiation. This work presented innovative coating design and preparation methods to improve the performance and functionality of anti-corrosion coatings, making significant attempts in the field.

In-situ exfoliation of hexagonal boron nitride during the forced flow of highly elastic polylactide to fabricate electrospun fibrous film with high thermal conductivity and low dielectric loss

Boron nitride nanosheets (BNNS) have promising applications in thermal management materials, due to their high thermal conductivity and low dielectric loss. However, it is still challenging to fabricate BNNS with large lateral size and structural integrity via solvent-free methods. Here, we report a novel processing method for in-situ exfoliation of hexagonal boron nitride (h-BN) to fabricate BNNS with an average lateral size of 1.45 μm, average thickness of 4.88 nm and few lattice defects during the forced flow of polylactide (PLA) in a highly elastic state. We further fabricate flexible and bio-degradable PLA/BNNS electrospun fibrous film for electronic devices to replace petroleum-based composites. The PLA/BNNS fibrous film exhibits an in-plane thermal conductivity of 4.9 W/(m·K) at the BNNS loading of 20 wt%. Moreover, the fibrous film also has a low dielectric loss (0.007 at 1 kHz) and good electrical insulation. The in-situ exfoliation strategy is simple, economical and environmentally friendly, providing an effective route to design thermal management materials with high thermal conductivity and low dielectric loss in the future of electronic devices.

Scalable Production of Highly Conductive 2D NbSe2 Monolayers with Superior Electromagnetic Interference Shielding Performance.

Thin, flexible, and electrically conductive films are in demand for electromagnetic interference (EMI) shielding. Two-dimensional NbSe2 monolayers have an electrical conductivity comparable to those of metals (106-107 S m-1) but are challenging for high-quality and scalable production. Here, we show that electrochemical exfoliation of flake NbSe2 powder produces monolayers on a large scale (tens of grams), at a high yield (>75%, monolayer), and with a large average lateral size (>20 μm). The as-exfoliated NbSe2 monolayer flakes are easily dispersed in diverse organic solvents and solution-processed into various macroscopic structures (e.g., free-standing films, coatings, patterns, etc.). Thermal annealing of the free-standing NbSe2 films reduces the interlayer distance of restacked NbSe2 from 1.18 to 0.65 nm and consequently enhances the electrical conductivity to 1.16 × 106 S m-1, which is superior to those of MXenes and reduced graphene oxide. The optimized NbSe2 film shows an EMI shielding effectiveness (SE) of 65 dB at a thickness of 5 μm (>110 dB for a 48-μm-thick film), among the highest in materials of similar thicknesses. Moreover, a laminate of two layers of the NbSe2 film (2 μm thick) with an insulating interlayer shows a high SE of 85 dB, surpassing that of the 20-μm-thick NbSe2 film (83 dB). A two-layer theoretical model is proposed, and it agrees with the experimental EMI SE of the laminated NbSe2 films. The ability to produce NbSe2 monolayers on a tens of grams scale will enable their diverse applications beyond EMI shielding.

Solid‐Liquid Interfacial Engineered Large‐Area Two‐Dimensional Covalent Organic Framework Films

AbstractConstructing uniform covalent organic framework (COF) film on substrates for electronic devices is highly desirable. Here, a simple and mild strategy is developed to prepare them by polymerization on a solid‐liquid interface. The universality of the method is confirmed by the successful preparation of five COF films with different microstructures. These films have large lateral size, controllable thickness, and high crystalline quality. And COF patterns can also be directly achieved on substrates via hydrophilic and hydrophobic interface engineering, which is in favor of preparing device array. For application studies, the PyTTA‐TPA (PyTTA: 4,4′,4′′,4′′′‐(1,3,6,8‐Tetrakis(4‐aminophenyl)pyrene and TPA: terephthalaldehyde) COF film has a high photoresponsivity of 59.79 μA W−1 at 420 nm for photoelectrochemical (PEC) detection. When employed as an active material for optoelectronic synaptic devices for the first attempt, it shows excellent light‐stimulated synaptic plasticity properties such as short‐term plasticity (STP), long‐term plasticity (LTP), and the conversion of STP to LTP, which can be used to simulate biological synaptic functions.

Solid-Liquid Interfacial Engineered Large-Area Two-Dimensional Covalent Organic Framework Films.

Constructing uniform covalent organic framework (COF) film on substrates for electronic devices is highly desirable. Here, a simple and mild strategy is developed to prepare them by polymerization on a solid-liquid interface. The universality of the method is confirmed by the successful preparation of five COF films with different microstructures. These films have large lateral size, controllable thickness, and high crystalline quality. And COF patterns can also be directly achieved on substrates via hydrophilic and hydrophobic interface engineering, which is in favor of preparing device array. For application studies, the PyTTA-TPA (PyTTA: 4,4',4'',4'''-(1,3,6,8-Tetrakis(4-aminophenyl)pyrene and TPA: terephthalaldehyde) COF film has a high photoresponsivity of 59.79 μA W-1 at 420 nm for photoelectrochemical (PEC) detection. When employed as an active material for optoelectronic synaptic devices for the first attempt, it shows excellent light-stimulated synaptic plasticity properties such as short-term plasticity (STP), long-term plasticity (LTP), and the conversion of STP to LTP, which can be used to simulate biological synaptic functions.