Geometrical quasi-ballistic effects on thermal transport in nanostructured devices

We employ thermoreflectance thermal imaging to directly measure the steady-state two-dimensional(2D)temperature field generated by nanostructured heat sources deposited on silicon substrate with different geometrical configurations and characteristic sizes down to 400nm.The analysis of the results using Fourier's law not only breaks down as size scales down,but it alsofails to capture the impact of the geometry of the heat source.The substrate effective Fourier thermal conductivities fitted to wire-shaped and circular-shaped structures with identical characteristic lengths are found to display up to 40%mismatch.Remarkably,a hydrcxjynamic heat transport model reproduces the observed temperature fields for all device sizes and shapes using just intrinsic Si parameters,i.e.,a geometry and size-independent thermal conductivity and nonlocal length scale.The hydrodynamic model provides insight into the observed thermal response and of the contradictory Fourier predictions.We discuss the substantial Silicon hydrodynamic behavior at room temperature and contrast it to InGaAs,which shows less hydrodynamic effects due to dominant phonon-impurity scattering.     

Atomistic modeling and rational design of optothermal tweezers for targeted applications

Optical manipulation of micro/nanoscale objects is of importance in life sciences,colloidal science,and nanotechnology.Optothermal tweezers exhibit superior manipulation capability at low optical intensity.However,our implicit understanding of the working mechanism has limited the further applications and innovations of optothermal tweezers.Herein,we present an atomistic view of opto-thermo-electro-mechanic coupling in optothermal tweezers,which enables us to rationally design the tweezers for optimum performance in targeted applications.Specifically,we have revealed that the non-uniform temperature distribution induces water polarization and charge separation,which creates the thermoelectric field dominating the optothermal trapping.We further design experiments to systematically verify our atomistic simulations.Guided by our new model,we develop new types of optothermal tweezers of high performance using low-concentrated electrolytes.Moreover,we demonstrate the use of new tweezers in opto-thermophoretic separation of colloidal particles of the same size based on the difference in their surface charge,which has been challenging for conventional optical tweezers.With the atomistic understanding that enables the performance optimization and function expansion,optothermal tweezers will further their impacts.     

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.

     

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.     

Colloidal lead-free Cs2AgBiBr6 double perovskite nanocrystals: Synthesis,uniform thin-film fabrication,and application in solution-processed solar cells

Recently developed lead-free double perovskite nanocrystals(NCs)have been proposed for the possible application in solutionprocessed optoelectronic devices.However,the optoelectronic applications of double perovskite NCs have been hampered due to the structural and chemical instability in the presence of polar molecules.Here,we report a facile strategy for the synthesis and purification of Cs₂AgBiBr₆double perovskite NCs that remained stable even after washing with polar solvent.This is realized with our efficient colloidal route to synthesize Cs₂AgBiBr₆NCs that involve stable and strongly coordinated precursor such as silvertrioctyl phosphine complex together with bismuth neodecanoate,which leads to a significantly improved chemical and colloidal stability.Using layer-by-layer solid-state ligand exchange technique,a compact and crack-free thin film of Cs₂AgBiBr₆NCs were fabricated.Finally,perovskite solar cells consisting of Cs₂AgBiBr₆as an absorber layer were fabricated and tested.     

Layer-by-layer assembled dual-ligand conductive MOF nano-films with modulated chemiresistive sensitivity and selectivity

In this paper,a dual-ligand design strategy is demonstrated to modulate the performance of the electronically conductive metalorganic frameworks(EC-MOFs)thin film with a spray layer-by-layer assembly method.The thin film not only can be precisely prepared in nanometer scale(20-70 nm),but also shows the pin-hole-free smooth surface.The high quality nano-film of 2,3,6,7,10,11-hexaiminotriphenylene(HITP)doped Cu-HHTP enables the precise modulation of the chemiresistive sensitivity and selectivity.Selectivity improvement over 220%were realized for benzene vs.NH3>as well as enhanced response and recovery properties.In addition,the selectivity of the EC-MOF thin film sensors toward other gases(e.g.triethylamine,methane,ethylbenzene,hydrogen,butanone,and acetone)vs.NH3 at room temperature is also discussed.     

How defects influence the photoluminescence of TMDCs

Two-dimensional(2D)transition metal dichalcogenide(TMDC)monolayers,a class of ultrathin materials with a direct bandgap and high exciton binding energies,provide an ideal platform to study the photoluminescence(PL)of light-emitting devices.Atomically thin TMDCs usually contain various defects,which enrich the lattice structure and give rise to many intriguing properties.As the influences of defects can be either detrimental or beneficial,a comprehensive understanding of the internal mechanisms underlying defect behaviour is required for PL tailoring.Herein,recent advances in the defect influences on PL emission are summarized and discussed.Fundamental mechanisms are the focus of this review,such as radiative/nonradiative recombination kinetics and band structure modification.Both challenges and opportunities are present in the field of defect manipulation,and the exploration of mechanisms is expected tofacilitate the applications of 2D TMDCs in the future.     

Nanovilli electrode boosts hydrogen evolution: A surface with superaerophobicity and superhydrophilicity

Although tremendous efforts have been paid on electrocatalysts toward efficient electrochemical hydrogen generation,breakthrough is still highly needed in the design and synthesis of wonderful non-precious-metal electrocatalyst.Herein,a nanovilli Ni2P electrode,which with superaerophobic and superhydropholic can significantly facilitate the mass and electron transfer was constructed via a facial morphology control strategy.Meanwhile,the substitution of sluggish oxygen evolution with urea oxidation,lowering the two-electrode cell voltage to only 1.48 volts to achieve a current density of 10 mA·cm^-2.Thus,the as-constructed electrode achieves the operation of hydrogen generation by an AA battery.This work sheds new light on the exploration of other high-efficient electrocatalysts for hydrogen generation by using intermittent clean energy.     

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.     

Magnetic-programmable organohydrogels with reconfigurable network for mechanical homeostasis

Synthetic materials with tunable mechanical properties have great potential in soft robotics and biomedical engineering.However,current materials are limited to the mechanical duality altering their mechanical properties only between soft and hard states and lack of consecutively programmable mechanics.Herein,the magnetic-programmable organohydrogels with heterogeneous dynamic architecture are designed by encasing oleophilic ferrofluid droplets into hydrogel matrix.As magnetic field increases,the mechanical properties of organohydrogels can be consecutively modulated owing to the gradual formation of chain-like assembly structures of nanoparticles.The storage modulus G'increases by 2.5 times when magnetic field goes up to 0.35 T.Small-Angle X-ray Scattering(SAXS)confirms the reconfigurable orientation of nanoparticles and the organohydrogels show reversible modulus switching.Besides,the materials also exhibit high stretchability,magnetic actuation behavior and effective self-healing capability.Furthermore,the organohydrogels are applied into the design of effectors with mechanical adaptivity.When subjected to serious external perturbations,the effector can maintain mechanical homeostasis by regulating modulus of organohydrogel under applied magnetic field.Such materials are applicable to homeostatic systems with mechanically adaptive behaviors and programmed responses to external force stimuli.     

Recent advances in anode materials for potassium-ion batteries: A review

Potassium-ion batteries (PIBs) are appealing alternatives to conventional lithium-ion batteries (LIBs) because of their wide potential window, fast ionic conductivity in the electrolyte, and reduced cost. However, PIBs suffer from sluggish K⁺ reaction kinetics in electrode materials, large volume expansion of electroactive materials, and the unstable solid electrolyte interphase. Various strategies, especially in terms of electrode design, have been proposed to address these issues. In this review, the recent progress on advanced anode materials of PIBs is systematically discussed, ranging from the design principles, and nanoscale fabrication and engineering to the structure-performance relationship. Finally, the remaining limitations, potential solutions, and possible research directions for the development of PIBs towards practical applications are presented. This review will provide new insights into the lab development and real-world applications of PIBs.

     

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.

     

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.

     

Hierarchical structures hydrogel evaporator and superhydrophilic water collect device for efficient solar steam evaporation

Efficient light absorption and trapping are of vital importance for the solar water evaporation by hydrogel-based photothermal conversion materials.Conventional strategies are focused on the development of the composition and structure of the hydrogers internal network.In our point of view,the importance of the surface structure of hydrogel has usually been underestimated or ignored.Here inspired by the excellent absorbance and water transportation ability of biological surface structure,the hierarchical structured hydrogel evaporators(HSEs)increased the light absorption,trapping,water transportation and water-air interface,which is the beneficial photothermal conversion and water evaporation.The HSEs showed a rapid evaporation rate of 1.77 kg·m^-2·h^-1at about 92%energy efficiency under one sun(1 kW·m^-2).Furthermore,the superhydrophilic window device was used in this work to collect the condensed water,which avoids the light-blocking caused by the water mist formed by the small droplets and the problem of the droplets stick on the device dropping back to the bulk water.Integrated with the excellent photothermal conversion hydrogel and superhydrophilic window equipment,this work provides efficient evaporation and desalination of hydrogel-based solar evaporators in practical large-scale applications.     

Integrated hetero-nanoelectrodes for plasmon-enhanced electrocatalysis of hydrogen evolution

Hetero-nanostructures of plasmonic metals and semiconductors have attracted increasing attention in the field of photocatalysis.However,most of the hetero-nanostructured catalysts are randomly arranged and therefore require comprehensive structural design for optimizing their properties.Herein,we report the robust construction of hierarchical hetero-nanostructures where gold(Au)nanorods and molybdenum disulfide(Mo S₂)quantum sheets(QSs)are integrated in highly ordered arrays.Such construction is achieved through porous anodic alumina(PAA)template-assisted electrodeposition.The as-fabricated hetero-nanostructures demonstrate exciting electrocatalysis towards hydrogen evolution reaction(HER).Both plasmon-induced hot-electron injection and plasmonic scattering/reabsorption mechanisms are determinative to the enhanced electrocatalytic performances.Notably,broadband photoresponses of HER activity in the visible range are observed,indicating their superiority compared with random systems.Such integrated hetero-nanoelectrodes could provide a powerful platform for conversion and utilization of solar energy,meanwhile would greatly prompt the production and exploration of ordered nanoelectrodes.     

Unprecedently low thermal conductivity of unique tellurium nanoribbons

Tellurene, probably one of the most promising two-dimensional (2D) system in the thermoelectric materials, displays ultra-low thermal conductivity. However, a linear thickness-dependent thermal conductivity of unique tellurium nanoribbons in this study reveals that unprecedently low thermal conductivity can be achieved via well-defined nanostructures of low-dimensional tellurium instead of pursuing dimension-reduced 2D tellurene. For thinnest tellurium nanoribbon with thickness of 144 nm, the thermal conductivity is only ∼1.88 ± 0.22 W·m⁻¹·K⁻¹ at room temperature. It’s a dramatic decrease (45%), compared with the well-annealed high-purity bulk tellurium. To be more specific, an expected thermal conductivity of tellurium nanoribbons is even lower than that of 2D tellurene, as a result of strong phonon-surface scattering. We have faith in low-dimensional tellurium in which the thermoelectric performance could realize further breakthrough.

     

Spontaneous migration induced Co nanokarstcave encapsulated in N-doped carbon hybrids for efficient oxygen electrocatalyst

Despite the extensive application of porous nanostructures as oxygen electrocatalysts, it is challenging to synthesize single-metal state materials with porous structures, especially the ultrasmall ones due to the uniform diffusion of the same metal. Herein, we pioneer demonstrate a new size effect-based controllable synthesis strategy for the homogeneous Co nanokarstcaves assisted by Co-CN hybrids (CCHs). The preferential migration of cobalt atoms on the surface of small size zeolitic imidazolate framework (ZIF) with high surface energy during pyrolysis is the key factor for the formation of nanokarstcave structure. Furthermore, graphene can act as a diffusion barrier to prevent the agglomeration of nanoparticles in the synthesis process, which also plays an important role in the formation of porous nanostructures. In alkali media, CCHs achieve overpotential of 287 mV (@10 mA·cm⁻²) for oxygen evolution reaction (OER) and a half wave potential of 0.86 V (vs. RHE) for oxygen reduction reaction (ORR).

     

Graphene: A promising candidate for charge regulation in high-performance lithium-ion batteries

The development of rechargeable lithium-ion batteries (LIBs) is being driven by the ever-increasing demand for high energy density and excellent rate performance. Charge transfer kinetics and polarization theory, considered as basic principles for charge regulation in the LIBs, indicate that the rapid transfer of both electrons and ions is vital to the electrochemical reaction process. Graphene, a promising candidate for charge regulation in high-performance LIBs, has received extensive investigations due to its excellent carrier mobility, large specific surface area and structure tunability, etc. Recent progresses on the structural design and interfacial modification of graphene to regulate the charge transport in LIBs have been summarized. Besides, the structure-performance relationships between the structure of the graphene and its dedicated applications for LIBs have also been clarified in detail. Taking graphene as a typical example to explore the mechanism of charge regulation will outline ways to further understand and improve carbon-based nanomaterials towards the next generation of electrochemical energy storage devices.

     

Observing antimicrobial process with traceable gold nanoclusters

Understanding the interaction of nanomaterials with biological systems has always been of high concern and interest. An emerging type of nanomaterials, ultrasmall metal nanoclusters (NCs, < 2 nm in size), are promising in this aspect due to their well-defined molecular formulae and structures, as well as unique physical and chemical properties that are distinctly different from their larger counterparts (metal nanoparticles). For example, metal NCs possess intrinsic strong luminescence, which can be used for real-time tracking of their interactions with biological systems. Herein, luminescent gold (Au) NCs were used as traceable antimicrobial agents to study their interactions with the bacteria and to further understand their underlining antimicrobial mechanism. It is shown for the first time that the Au NCs would first attach on the bacterial membrane, penetrate, and subsequently accumulate inside the bacteria. Thereafter, the internalized Au NCs would induce reactive oxygen species (ROS) generation and damage the bacterial membrane, resulting in the leakage of bacterial contents, which can finally kill the bacteria. Traceable Au NCs (or other metal NCs) provide a promising platform to study the antimicrobial mechanisms as well as other fundamentals on the interfacing of functional nanomaterials with the biological systems, further increasing their acceptance in various biomedical applications.

     

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.