Two-dimensional polymer nanosheets for efficient energy storage and conversion

As a promising graphene analogue, two-dimensional (2D) polymer nanosheets with unique 2D features, diversified topological structures and as well as tunable electronic properties, have received extensive attention in recent years. Here in this review, we summarized the recent research progress in the preparation methods of 2D polymer nanosheets, mainly including interfacial polymerization and solution polymerization. We also discussed the recent research advancements of 2D polymer nanosheets in the fields of energy storage and conversion applications, such as batteries, supercapacitors, electrocatalysis and photocatalysis. Finally, on the basis of their current development, we put forward the existing challenges and some personal perspectives.

     

Coarse and fine-tuning of lasing transverse electromagnetic modes in coupled all-inorganic perovskite quantum dots

Inorganic perovskite lasers are of particular interest,with much recent work focusing on Fabry-P6rot cavity-forming nanowires.We demonstrate the direct observation of lasing from transverse electromagnetic(TEM)modes with a long coherence time-9.5ps in coupled CsPbBr₃ quantum dots,which dispense with an external cavity resonator and show how the wavelength of the modes can be controlled via two independent tuning-mechanisms.Controlling the pump power allowed us tofine-tune the TEM mode structure to the emission wavelength,thus providing a degree of control over the properties of the lasing signal.The temperature-tuning provided an additional degree of control over the wavelength of the lasing peak,importantly,maintained a constant full width at half maximum(FWHM)over the entire tuning range without mode-hopping.     

Rapid room-temperature synthesis of a porphyrinic MOF for encapsulating metal nanoparticles

While metal nanoparticles(NPs)have shown great promising applications as heterogeneous catalysts,their agglomeration caused by thermodynamic instability is detrimental to the catalytic performance.To tackle this hurdle,we successfully prepared a functional and stable porphyrinic metal-organic framework(MOF),PCN-224-RT,as a host for encapsulating metal nanoparticles by direct stirring at room temperature.As a result,Pt@PCN-224-RT composites with well-dispersed Pt NPs can be constructed by introducing pre-synthesized Pt NPs into the precursor solution of PCN-224-RT.Of note,the rapid and simple stirring method in this work is more in line with the requirements of environmental friendly and industrialization compared with traditional solvothermal methods.     

Scalable salt-templated directed synthesis of high-quality MoS2 nanosheets powders towards energetic and environmental applications

Two-dimensional (2D) transition metal dichalcogenides (TMDCs) have emerged as perfect platforms for developing applications in nano-electronics, catalysis, energy storage and environmental-related fields due to their superior properties. However, the low-cost, batch production of high-quality 2D TMDCs remains a huge challenge with the existing synthetic strategies. Herein, we present a scalable chemical vapor deposition (CVD) approach for the batch production of high-quality MoS₂ nanosheet powders, by using naturally abundant, water-soluble and recyclable NaCl crystal powders as templates. The high-quality MoS₂ nanosheets powders are achieved by a facile water dissolution-filtration process, by virtue of the excellent dispersibility of the as-grown products in water. The internal mechanism for the scalable synthesis strategy is explored. The applications of the MoS₂ nanosheets powders are also demonstrated as catalysts or adsorbents in hydrogen evolution reaction (HER) and organic dyes adsorption, respectively. This work should hereby pave ways for the mass production and application of powdery TMDCs in energetic and environmental related fields.

     

Recent progress about 2D metal dichalcogenides: Synthesis and application in photodetectors

In recent years, two-dimensional (2D) layered metal dichalcogenides (MDCs) have received enormous attention on account of their excellent optoelectronic properties. Especially, various MDCs can be constructed into vertical/lateral heterostructures with many novel optical and electrical properties, exhibiting great potential for the application in photodetectors. Therefore, the batch production of 2D MDCs and their heterostructures is crucial for the practical application. Recently, the vapour phase methods have been proved to be dependable for growing large-scale MDCs and related heterostructures with high quality. In this paper, we summarize the latest progress about the synthesis of 2D MDCs and their heterostructures by vapour phase methods. Particular focus is paid to the control of influence factors during the vapour phase growth process. Furthermore, the application of MDCs and their heterostructures in photodetectors with outstanding performance is also outlined. Finally, the challenges and prospects for the future application are presented.

     

Superbroad-band actively tunable acoustic metamaterials driven from poly(ethylene terephthalate)/carbon nanotube nanocomposite membranes

Actively tunable acoustic metamaterials have attracted ever increasing attention.However,their tunable frequency range is quite narrow(tens of Hz)even under ultrahigh applied voltage(about 1,000 V).Here,we report a superbroad-band actively tunable acoustic metamaterials with the bandwidth over 400 Hz under a low voltage.In the actively tunable acoustic metamaterials,the acoustic membrane is a laminated nanocomposite consisting of a poly(ethylene terephthalate)(PET)and super-aligned carbon nanotube(CNT)drawn from CN T forest array.The laminated nanocomposite membrane exhibits adjustable acoustic properties,whose modulus can be adjusted by applying external electric field.The maximum frequency bandwidth of PET/CN T nanocomposite membrane reaches 419 Hz when applying an external DC voltage of 60 V.Our actively tunable acoustic metamaterials with superbroad-band and lightweight show very promising foreground in noise reduction applications.     

Bioengineering of nano metal-organic frameworks for cancer immunotherapy

Immunotherapy techniques,such as immune checkpoint inhibitors,chimeric antigen receptor(CAR)T cell therapies and cancer vaccines,have been burgeoning with great success,particularly for specific cancer types.However,side effects with fatal risks,dysfunction in tumor microenvironment and low immune response rates remain the bottlenecks in immunotherapy.Nano metal-organic frameworks(nMOFs),with an accurate structure and a narrow size distribution,are emerging as a solution to these problems.In addition to their function of temporospatial delivery,a large library of their compositions,together with flexibility in chemical interaction and inherent immune efficacy,offers opportunities for various designs of nMOFs for immunotherapy.In this review,we overview state-of-the-art research on nMOFs-based immunotherapies as well as their combination with other therapies.We demonstrate that nMOFs are predominantly customized for vaccine delivery or tumor-microenvironment modulation.Finally,a prospect of nMOFs in cancer immunotherapy will be discussed.     

Regulating surface state of WO3 nanosheets by gamma irradiation for suppressing hydrogen evolution reaction in electrochemical N2 fixation

Realizing the reduction of N₂ to NH₃ at low temperature and pressure is always the unremitting pursuit of scientists and then electrochemical nitrogen reduction reaction offers an intriguing alternative. Here, we develop a feasible way, gamma irradiation, for constructing defective structure on the surface of WO₃ nanosheets, which is clearly observed at the atomic scale by high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM). The abundant oxygen vacancies ensure WO₃ nanosheets with a Faradaic efficiency of 23% at −0.3 V vs. RHE. Moreover, we start from the regulation of the surface state to suppress proton availability towards hydrogen evolution reaction (HER) on the active site and thus boost the selectivity of nitrogen reduction.

     

Ambipolar two-dimensional bismuth nanostructures in junction with bismuth oxychloride

Despite the unique properties of bismuth(Bi),there is a lack of two-dimensional(2D)heterostructures between Bi and other functional 2D materials.Here,a coherent strategy is reported to simultaneously synthesize rhombohedral phase Bi nanoflakes and bismuth oxychloride(BiOCI)nanosheets.The delicate balance between several reactions is mediated mainly for the reduction and chlorination in the chemical vapor transport(CVT)process.The Bi-BiOCI lateral heterostructures have been constructed via the coalescence of the two different 2D nanostructures.The characteristics of ambipolar conducting Bi and insulator-like BiOCI are elaborated by scanning microwave impedance microscopy(sMIM).This work demonstrates a way to construct a 2D Bi nanostructure in junction with its oxyhalide.     

Direct aerobic oxidation of monoalcohol and diols to acetals using tandem Ru@MOF catalysts

The aerobic oxidation of monoalcohols and diols to acetals is an important academic and industrial challenge for the production of fine chemicals and intermediates.The existing methods usually rely on a two-step process in which alcohols are first oxidized to aldehydes over metal catalysts(Ru,Pt,Pd)and then acetalized using acids.Due to the instability of aldehydes,how to avoid over-oxidation to their respective carboxylic acids and esters is a long-standing challenge.For this reason,certain non-conjugated dialdehydes have never been successfully produced from diol oxidation.Hereby we report a Ru@metal-organic framework(MOF)tandem catalyst containing ultra-fine Ru nanoparticles(<2 nm)for direct alcohol to acetal conversion of monoalcohol and diols with noformation of carboxylic acids.Mechanistic study reveals that the presence of Lewis acid sites in the MOF work in concert with Ru active sites to promptly convert aldehydes to acetals thereby effectively suppressing the formation of over-oxidation byproducts.     

Synthesis of magnetic two-dimensional materials by chemical vapor deposition

The development of magnetic two-dimensional (2D) materials in its infancy has generated an enormous amount of attention as it offers an ideal platform for the exploration of magnetic properties down to the 2D limit, paving the way for spintronic devices. Due to the nonnegligible advantages including time efficiency and simplified process, the facile bottom-up chemical vapor deposition (CVD) is regarded as a robust method to fabricate ultrathin magnetic nanosheets. Recently, some ultrathin magnets possessing fascinating properties have been successfully synthesized via CVD. Here, the recent researches toward magnetic 2D materials grown by CVD are systematically summarized with special emphasis on the fabrication methods. Then, heteroatoms doping and phase transition induced in CVD growth to bring or tune the magnetic properties in 2D materials are discussed. Characterizations and applications of these magnetic materials are also discussed and reviewed. Finally, some perspectives in need of urgent attention regarding the development of CVD-grown magnetic 2D materials are proposed.

     

Two-dimensional oxide derived from high-temperature liquid metals via bubble templating

Two-dimensional (2D) oxide can be continuously produced by bubbling oxygen into liquid metals and the harvesting of these oxide relies on the proper choice of dispersion solvents. The mass-production of ligand-free 2D materials from high melting-point metals will not be possible if the limited stability of the traditional dispersion solvents is not circumvented. Herein, liquid tin was used for the first time in the bubbling protocol and 2D tin oxide was obtained in molten salts. The nanosheets were studied with combined microscopic and spectroscopic techniques, and high-density grain boundaries was identified between the sub-5-nm nano-crystallites in the nanosheets. It gives rise to the high performance in electrocatalytic CO₂ reduction reaction. Density-functional-theory based calculation was applied to achieve a deeper understanding of the relationship between the activity, selectivity, and the grain-boundary features. The molten-salt based protocol could be explored for the synthesis of a library of functional 2D oxides.

     

Superhydrophobic,photo-sterilize,and reusable mask based on graphene nanosheet-embedded carbon(GNEC)film

The 2019 coronavirus disease(COVID-19)has affected more than 200 countries.Wearing masks can effectively cut off the virus spreading route since the coronavirus is mainly spreading by respiratory droplets.However,the common surgical masks cannot be reused,resulting in the increasing economic and resource consumption around the world.Herein,we report a superhydrophobic,photo-sterilize,and reusable mask based on graphene nanosheet-embedded carbon(GNEC)film,with high-density edges of standing structured graphene nanosheets.The GNEC mask exhibits an excellent hydrophobic ability(water contact angle:157.9°)and an outstanding filtration efficiency with 100%bacterial filtration efficiency(BFE).In addition,the GNEC mask shows the prominent photo-sterilize performance,heating up to 110℃quickly under the solar illumination.These high performances may facilitate the combat against the COVID-19 outbreaks,while the reusable masks help reducing the economic and resource consumption.     

Control of vertical phase separation in high performance non-fullerene organic solar cell by introducing oscillating stratification preprocessing

Non-fullerene organic solar cell(NFOSC)has attracted tremendous attention due to their great potential for commercial applications.To improve its power conversion efficiency(PCE),generally,sequential solution deposition(SSD)methods have been employed to construct the graded vertical phase separation(VPS)of the bulk-heterojunction(BHJ)active layer for efficient exciton separation and charge transition.However,a variety of orthogonal solvents used in the SSD may lead to the unpredicted change in the BHJ morphology and introduce additional defects inside the BHJ bulk thus complicate the fabrication process.Here,a simple oscillating stratification preprocessing(OSP)is developed to facilitate the formation of graded VPS among the BHJ layer.As a result,a significant improvement is obtained in PCE from 10.96%to 12.03%,which is the highest value reported among PBDB-T:ITIC based NFOSC.     

Reticular exploration of uranium-based metal-organic frameworks with hexacarboxylate building units

The rational reticular design of metal-organic frameworks(MOFs)from building units of known geometries is essential for enriching the diversity of MOF structures.Unexpected and intriguing structures,however,can also arise from subtle changes in the rigidity/length of organic linkers and/or synthetic conditions.Herein,we report three uranium-based MOF structures—i.e.,NU-135X(X=0,1,2)—synthesized from trigonal planar uranyl nodes and triptycene-based hexacarboxylate ligands with variable arm lengths.A new chiral 3,6-connected nuc net was observed in NU-1350,while the extended versions of the ligand led to 3-fold catenated MOFs(NU-1351 and NU-1352)with rare 3,6-connected cml-c3 nets.The differences in the topology of NU-1350 and NU-1351/NU-1352 could be attributed to the slight distortions of the shorter linker in the former from the ideal trigonal prism geometry to an octahedral geometry when coordinated to the trigonal planar uranyl nodes.     

Recent advances in engineered nanomaterials for acute kidney injury theranostics

Acute kidney injury(AKI),has become the focus of increasing attention due to its high risk of death.The early diagnosis and treatment of AKI significantly reduce the risk of renal tissue damage and kidney dysfunction.However,the efficient early diagnosis and treatment approach for AKI remains a challenge.AKI screening via precise nanomaterial theranostics is a new alternative approach.This study summarizes the recent advances in functional nanomaterials in the early detection and treatment of AKI.The challenges and problems in the use of nanomaterials for AKI in clinical applications are also discussed.It is anticipated that highlighting these new advances will lay the foundation for further translational research on the promising application of nanomaterials for AKI.     

All-inorganic dual-phase halide perovskite nanorings

In the present work, we report the growth of all-inorganic perovskite nanorings with dual compositional phases of CsPbBr₃ and CsPb₂Br₅ via a facile hot injection process. The self-coiling of CsPbBr₃-CsPb₂Br₅ nanorings is driven by the axial stress generated on the outside surface of the as-synthesized nanobelts, which results from the lattice mismatch during the transformation of CsPbBr₃ to CsPb₂Br₅. The tailored growth of nanorings could be achieved by adjusting the key experimental parameters such as reaction temperature, reaction time and stirring speed during the cooling process. The photoluminescence intensity and quantum yield of nanorings are higher than those of CsPbBr₃ nanobelts, accompanied by a narrower full width at half maximum (FWHM), suggesting their high potential for constructing self-assembled optoelectronic nanodevices.

     

Advances of biological-camouflaged nanoparticles delivery system

Nanoparticles (NPs) which are innovation and research focus in drug delivery systems, still have some disadvantages limiting its application in clinical use, such as short circulation time, recognition and clearance by reticuloendothelial system (RES) and passive targeting in certain organs. However, the recent combination of natural components and nanotechnology has offered new solutions to address these problems. A novel biomimetic platform consisting of nanoparticle core and membrane shell, such as cell membrane, exosome or vesicle vastly improves properties of nanoparticles. These coated nanoparticles can replicate the unique functions of the membrane, such as prolonged blood circulation, active targeting capability and enhanced internalization. In this review, we focus on the newest development of biological-camouflaged nanoparticles and mainly introduce its application related to cancer therapy and toll-like receptor.

     

Corrosion formation and phase transformation of nickel-iron hydroxide nanosheets array for efficient water oxidation

Designing earth-abundant electrocatalysts with high performance towards water oxidation is highly decisive for the sustainable energy technologies. This study develops a facile natural corrosion approach to fabricate nickel-iron hydroxides for water oxidation. The resulted electrode demonstrates an outstanding activity and stability with an overpotential of 275 mV to deliver 10 mA·cm⁻². Experimental and theoretical results suggest the corrosion-induced formation of hydroxides and their transformation to oxyhydroxides would account for this excellent performance. This work not only provides an interesting corrosion approach for the fabrication of excellent water oxidation electrode, but also bridges traditional corrosion engineering and novel materials fabrication, which would offer some insights in the innovative principles for nanomaterials and energy technologies.

     

Discovery of Zr-based metal-organic polygon:Unveiling new design opportunities in reticular chemistry

Metal-based secondary building unit and the shape of organic ligands are the two crucial factors for determining the final topology of metal-organic materials.A careful choice of organic and inorganic structural building units occasionally produces unexpected structures,facilitating deeper fundamental understanding of coordination-driven self-assembly behind metal-organic materials.Here,we have synthesized a triangular metal-organic polygon(MOT-1),assembled from bulky tetramethyl terephthalate and Zr-based secondary building unit.Surprisingly,the Zr-based secondary building unit serves as an unusual ditopic Zr-connector,toform metal-organic polygon MOT-1,proven to be a good candidate for water adsorption with recyclability.This study highlights the interplay of the geometrically frustrated ligand and secondary building unit in controlling the connectivity of metal-organic polygon.Such a strategy can be further used to unveil a new class of metal-organic materials.