All‑Covalent Organic Framework Nanofilms Assembled Lithium‑Ion Capacitor to Solve the Imbalanced Charge Storage Kinetics

Free-standing covalent organic framework(COFs)nanofilms exhibit a remarkable ability to rapidly intercalate/de-intercalate Li^(+) in lithium-ion batteries,while simultaneously exposing affluent active sites in supercapacitors.The development of these nanofilms offers a promising solution to address the persistent challenge of imbalanced charge storage kinetics between battery-type anode and capacitor-type cathode in lithium-ion capacitors(LICs).Herein,for the first time,custom-made COFBTMB-TP and COFTAPB-BPY nanofilms are synthesized as the anode and cathode,respectively,for an all-COF nanofilm-structured LIC.The COFBTMB-TP nanofilm with strong electronegative–CF3 groups enables tuning the partial electron cloud density for Li^(+) migration to ensure the rapid anode kinetic process.The thickness-regulated cathodic COFTAPB-BPY nanofilm can fit the anodic COF nanofilm in the capacity.Due to the aligned 1D channel,2D aromatic skeleton and accessible active sites of COF nanofilms,the whole COFTAPB-BPY//COFBTMB-TP LIC demonstrates a high energy density of 318 mWh cm^(−3) at a high-power density of 6 W cm^(−3),excellent rate capability,good cycle stability with the capacity retention rate of 77%after 5000-cycle.The COFTAPB-BPY//COFBTMB-TP LIC represents a new benchmark for currently reported film-type LICs and even film-type supercapacitors.After being comprehensively explored via ex situ XPS,7Li solid-state NMR analyses,and DFT calculation,it is found that the COFBTMB-TP nanofilm facilitates the reversible conversion of semi-ionic to ionic C–F bonds during lithium storage.COFBTMB-TP exhibits a strong interaction with Li^(+) due to the C–F,C=O,and C–N bonds,facilitating Li^(+) desolation and absorption from the electrolyte.This work addresses the challenge of imbalanced charge storage kinetics and capacity between the anode and cathode and also pave the way for future miniaturized and wearable LIC devices.

Bending Resistance Covalent Organic Framework Superlattice:“Nano‑Hourglass”‑Induced Charge Accumulation for Flexible In‑Plane Micro‑Supercapacitors

Covalent organic framework(COF)film with highly exposed active sites is considered as the promising flexible selfsupported electrode for in-plane microsupercapacitor(MSC).Superlattice configuration assembled alternately by different nanofilms based on van der Waals force can integrate the advantages of each isolated layer to exhibit unexpected performances as MSC film electrodes,which may be a novel option to ensure energy output.Herein,a mesoporous free-standing A-COF nanofilm(pore size is 3.9 nm,averaged thickness is 4.1 nm)with imine bond linkage and a microporous B-COF nanofilm(pore size is 1.5 nm,averaged thickness is 9.3 nm)withβ-keto-enamine-linkages are prepared,and for the first time,we assembly the two lattice matching films into sandwich-type superlattices via layer-by-layer transfer,in which ABA–COF superlattice stacking into a“nano-hourglass”steric configuration that can accelerate the dynamic charge transportation/accumulation and promote the sufficient redox reactions to energy storage.The fabricated flexible MSC–ABA–COF exhibits the highest intrinsic CV of 927.9 F cm^(−3) at 10 mV s^(−1) than reported two-dimensional alloy,graphite-like carbon and undoped COF-based MSC devices so far,and shows a bending-resistant energy density of 63.2 mWh cm^(−3) even after high-angle and repeat arbitrary bending from 0 to 180°.This work provides a feasible way to meet the demand for future miniaturization and wearable electronics.

Epitaxial growth of large-area and highly crystalline anisotropic ReSe2 atomic layer

The anisotropic two-dimensional （2D） layered material rhenium disulfide （ReSe2） has attracted considerable attention because of its unusual properties and promising applications in electronic and optoelectronic devices. However, because of its low lattice symmetry and interlayer decoupling, anisotropic growth and out-of-plane growth occur easily, yielding thick flakes, dendritic structure, or flower-like structure. In this stud34 we demonstrated a bottom-up method for the controlled and scalable synthesis of ReSe2 by van der Waals epitaxy. To achieve controllable growth, a micro-reactor with a confined reaction space was constructed by stacking two mica substrates in the chemical vapor deposition system. Within the confined reaction space, the nucleation density and growth rate of ReSe2 were significantly reduced, favoring the large-area synthesis of ReSe2 with a uniform monolayer thickness. The morphological evolution of ReSe2 with growth temperature indicated that the anisotropic growth was suppressed at a low growth temperature （〈600 ℃）. Field-effect transistors employing the grown ReSe2 exhibited p-type conduction with a current ON/OFF ratio up to 10s and a hole carrier mobility of 0.98 cm^2/（V·s）. Furthermore, the ReSe2 device exhibited an outstanding photoresponse to near-infrared light, with responsivity up to 8.4 and 5.1 A/W for 850- and 940-nm light, respectively. This work not only promotes the large-scale application of ReSe2 in high-performance electronic devices but also clarifies the growth mechanism of low-lattice symmetry 2D materials.

A universal etching-free transfer of MoS2 films for applications in photodetectors

Transferring MoS2 films from growth substrates onto target substrates is a critical issue for their practical applications. Moreover, it remains a great challenge to avoid sample degradation and substrate destruction, because the current transfer method inevitably employs a wet chemical etching process. We developed an etching-free transfer method for transferring MoS2 films onto arbitrary substrates by using ultrasonication. Briefly, the collapse of ultrasonication-generated microbubbles at the interface between polymer-coated MoS2 film and substrates induce sufficient force to delaminate the MoS2 films. Using this method, the MoS2 films can be transferred from all substrates （silica, mica, strontium titanate, and sapphire） and retains the original sample morphology and quality. This method guarantees a simple transfer process and allows the reuse of growth substrates, without involving any hazardous etchants. The etching-free transfer method is likely to promote broad applications of MoS2 in photodetectors.

Passively Q-switched cylindrical vector laser based on a black phosphorus saturable absorber

We demonstrate an all-fiber Q-switched cylindrical vector laser based on a black phosphorus saturable absorber and a transverse mode converter. The saturable absorber is prepared by incorporating the polyvinyl alcohol with anti-oxidized black phosphorus nanosheets exfoliated in aqueous poly(dimethyldiallyl ammonium chloride)solution. The mode converter is composed of a tapered two-mode fiber and a single-mode fiber, and it can excite switchable azimuthally and radially polarized beams by modulating the input polarization. By enhancing the pump power from 64.68 to 174.82 mW, the repetition rate of the Q-switched azimuthally/radially polarized laser enlarges from 16.72/19.25 to 30.71/37.82 kHz.