Janus Quasi‑Solid Electrolyte Membranes with Asymmetric Porous Structure for High‑Performance Lithium‑Metal Batteries

Quasi-solid electrolytes(QSEs)based on nanoporous materials are promising candidates to construct high-performance Limetal batteries(LMBs).However,simultaneously boosting the ionic conductivity(σ)and lithium-ion transference number(t^(+)) of liquid electrolyte confined in porous matrix remains challenging.Herein,we report a novel Janus MOFLi/MSLi QSEs with asymmetric porous structure to inherit the benefits of both mesoporous and microporous hosts.This Janus QSE composed of mesoporous silica and microporous MOF exhibits a neat Li^(+) conductivity of 1.5.10^(–4)S cm^(−1) with t^(+) of 0.71.A partially de-solvated structure and preference distribution of Li^(+)near the Lewis base O atoms were depicted by MD simulations.Meanwhile,the nanoporous structure enabled efficient ion flux regulation,promoting the homogenous deposition of Li^(+).When incorporated in Li||Cu cells,the MOFLi/MSLi QSEs demonstrated a high Coulombic efficiency of 98.1%,surpassing that of liquid electrolytes(96.3%).Additionally,NCM 622||Li batteries equipped with MOFLi/MSLi QSEs exhibited promising rate performance and could operate stably for over 200 cycles at 1 C.These results highlight the potential of Janus MOFLi/MSLi QSEs as promising candidates for next-generation LMBs.

Dual-targeted nanoformulation with Janus structure for synergistic enhancement of sonodynamic therapy and chemotherapy

The accurate delivery of nanoparticles and organic small molecule drugs remains a serious challenge in nanoparticle-based tumor therapy.Dual-targeted therapy combining tumor cell targeting and organelle targeting is an effective solution.Here,an anticancer nanoformulation accurate delivery system was prepared using hyaluronic acid (HA) targeting CD44 receptors on the surface of tumor cells and IR780iodine (IR780) targeting mitochondrial for delivery.The system is based on an ultra-small Janus structured inorganic sensitizer TiO_(2-x)@NaGdF_(4) nanoparticles (TN NPs) prepared by one-step pyrolysis,further loaded with organic small molecule acoustic sensitizer IR780 and mitochondrial hexokinase Ⅱ inhibitor lonidamine (LND),followed by encapsulation of HA.Ultra-small size nanoparticles exhibit strong tissue penetration,tumor inhibition and in vivo metabolism.Under ultrasound radiation,TN NPs and IR780could produce a synergistic effect,effectively increased the efficiency of reactive oxygen species (ROS)production.Meanwhile,the released IR780 could smoothly target the mitochondria,and the ROS produced by IR780 can destroy the mitochondrial structure and disrupt the mitochondrial respiration.LND could inhibit the energy metabolism of tumor cells by reducing the activity of hexokinase Ⅱ (HK Ⅱ),which further accelerates the process of apoptosis.Furthermore,since the Janus structure allows the integration of multifunctional components into a single system,TN NPs can not only serve as an acoustic sensitizer to generate ROS,but the Gd element contained can also act as the nuclear magnetic resonance (MR)imaging contrast agent,suggesting that the nanoformulation can enable imaging-guided diagnosis and therapy.In conclusion,a new scheme to enhance sonodynamic therapy (SDT) and chemotherapy synergistically is proposed here based on ultra-small dual-targeted nanoformulation with Janus structure in the ultrasound radiation environment.

New Janus structure photocatalyst having widely tunable electronic and optical properties with strain engineering

Photoelectrochemical water splitting using solar energy,generating oxygen and hydrogen is one of the clean fuel production processes.Inspired by surface-dependent characteristics of Janus structures,a newly designed Janus monolayer Silicon Phosphorous Arsenide(SiPAs)was analyzed with Density Functional Theory(DFT)methods.Hybrid exchange-correlation functional(HSE06)combined with Wannier90-based analysis for electronic and optical properties of SiPAs reveals that it can act as a photocatalyst.SiPAs show an indirect bandgap of 1.88 eV,absorbing visible light range is 350 to 500 nm.The phonon spectrum confirms dynamic stability.The exciton binding energy is computed with GW/BSE methods.The electronic band edge positions are at-5.75 and-4.43 eV,perfectly straddling the water redox potentials.Interestingly the strain application modifies the bandgap and also non-homogenously widens the absorption band.A novel range of photocatalyst designs with Group IV-V elements with great promise for water-splitting,photovoltaic,and narrow bandgap semiconductor(optoelectronics)applications may be feasible.

Janus hydrogel/electrospun-membrane dressing enhancing wound healing in rats

Background:Excessive exudate secreted from chronic wounds often leads to overhydration and infection.Although a variety of dressings are currently available in clinical applications,they frequently fail to provide multifunction to promote chronic wound healing.The dressings with a Janus structure,featuring distinct properties on each side,are potential to improve wound healing.Methods:Composite dressings with a Janus structure were fabricated,comprising freeze-dried polycaprolactone(PCL)electrospun membrane and alginate-based hydrogel.The PCL fibrous membrane provided air permeability,while the hydrogel loaded with Deferoxamine,composed of alginate and poly(N-isopropylacrylamide)(PNIPAM),exhibited hygroscopic properties.The inclusion of PNIPAM imparted thermo-responsivity.Results:The hydrogel(thickness of 2.778±0.082 mm)exhibited a robust adhesion to the fiber membrane(thickness of 0.261±0.041 mm).For ANDC(Alginate-PNIPAM hydrogel with Deferoxamine/PCL membrane)samples,the water vapor transmission rate(WVTR)was measured to be 3364.80±23.23 g∙m−2∙day−1 and the swelling ratio at 2 h was determined to be 1179±125%.The thermo-responsivity of ANDC samples manifested in an increased swelling rate,escalating from 797±189%at 37°C to 1132±147%at 4°C.The elastic modulus was assessed for lyophilized and rehydrated ANDC sample.When theωof the rheometer rotor was decreased from 10 rad/s to 0.1 rad/s,the lyophilized dressing exhibited a decrease from 2.65±0.01 MPa to 1.80±0.90 MPa,while the rehydrated dressing demonstrated an increase from 133.65±55.68 Pa to 264.23±141.71 Pa.The pro-healing properties of the dressings were evaluated using full-thickness skin defect model on SD rats,and a circular wound of diameter 10 mm healed completely by day 12.Conclusion:The dressings not only protected the wound and absorbed excess exudate,but also demonstrated nondestructive peelability upon cooling,providing a novel approach for accelerating wound healing and management.

Multifunctional Ti_(3)C_(2)T_(x)-(Fe_(3)O_(4)/polyimide)composite films with Janus structure for outstanding electromagnetic interference shielding and superior visual thermal management

Flexible multifunctional polymer-based electromagnetic interference(EMI)shielding composite films have important application values in the fields of 5G communication technology,wearable electronic devices and artificial intelligence.In this work,Fe_(3)O_(4)/polyamic acid(PAA)nanofiber films are prepared by in-situ polymerization and electrospinning technology,and Ti_(3)C_(2)T_(x)nanosheets are deposited on the surface of the Fe_(3)O_(4)/PAA nanofiber films via vacuum-assisted filtration.Then,Janus Ti_(3)C_(2)T_(x)-(Fe_(3)O_(4)/polyimide(PI))composite films are obtained by thermal imidization.The two sides of the Janus films exhibit completely different properties.The Fe_(3)O_(4)/PI side has excellent hydrophobicity and insulation property,and the Ti_(3)C_(2)T_(x)side has hydrophilicity and terrific conductivity.When the mass fraction of Ti_(3)C_(2)T_(x)is 80 wt.%,the Janus Ti_(3)C_(2)T_(x)-(Fe_(3)O_(4)/PI)composite film has excellent EMI shielding performances and mechanical properties,with EMI shielding effectiveness,tensile strength and Young’s modulus reaching 66 dB,114.5 MPa and 5.8 GPa,respectively.At the same time,electromagnetic waves show different absorption shielding effectiveness(SEA)when incident from two sides of the Janus films.When the electromagnetic waves are incident from the Fe_(3)O_(4)/PI side,the SEA of the Janus film is 58 dB,much higher than that when the electromagnetic waves are incident from the Ti_(3)C_(2)T_(x)side(39 dB).In addition,the Ti_(3)C_(2)T_(x)side of the Janus Ti_(3)C_(2)T_(x)-(Fe_(3)O_(4)/PI)composite films also has excellent electrothermal and photothermal conversion performances.When the applied voltage is 4 V,the stable surface temperature reaches 108°C;when it is irradiated by simulated sunlight with power density of 200 mW/cm2,the stable surface temperature reaches 95℃.

Encryption/decryption and microtarget capturing by pH-driven Janus microstructures fabricated by the same femtosecond laser printing parameters

Several natural organism can change shape under external stimuli. These natural phenomena have inspired a vast amount of research on exploration and implementation of reconfigurable shape transformation. The Janus structure is a promising approach to achieve shape transformation based on its heterogeneous chemical or physical properties on opposite sides.However, the heterogeneity is generally realized by multi-step processing, different materials,and/or different processing parameters. Here, we present a simple and flexible method of producing p H-sensitive Janus microactuators from a single material, using the same laser printing parameters. These microactuators exhibit reversible structural deformations with large bending angles of ~31°and fast response(~0.2 s) by changing the p H value of the aqueous environment. Benefited from the high flexibility of the laser printing technique and the spatial arrangements, pillar heights, and bending directions of microactuators are readily controlled,enabling a variety of switchable ordered patterns and complex petal-like structures on flat surfaces and inside microchannels. Finally, we explore the potential applications of this method in information encryption/decryption and microtarget capturing.

Simultaneous Detection and Removal of Formaldehyde at Room Temperature: Janus Au@ZnO@ZIF-8 Nanoparticles

The detection and removal of volatile organic compounds(VOCs) are of great importance to reduce the risk of indoor air quality concerns. This study reports the rational synthesis of a dual-functional Janus nanostructure and its feasibility for simultaneous detection and removal of VOCs.The Janus nanostructure was synthesized via an anisotropic growth method, composed of plasmonic nanoparticles,semiconductors, and metal organic frameworks(e.g.,Au@ZnO@ZIF-8). It exhibits excellent selective detection to formaldehyde(HCHO, as a representative VOC) at room temperature over a wide range of concentrations(from 0.25 to100 ppm), even in the presence of water and toluene molecules as interferences. In addition, HCHO was also found to be partially oxidized into non-toxic formic acid simultaneously with detection. The mechanism underlying this technology was unraveled by both experimental measurements and theoretical calculations: ZnO maintains the conductivity, while ZIF-8 improves the selective gas adsorption; the plasmonic effect of Au nanorods enhances the visible-light-driven photocatalysis of ZnO at room temperature.

Highly ordered Janus CdS-Au-TiO_(2) Z-scheme structure with high efficiency in photocatalysis

Precise structural control had attracted tremendous interest in nanosynthesis due to its great importance in tailoring the physical properties of nanomaterials.Here we report the synthesis of highly ordered Cd S-Au-TiO_(2) ternary Janus structure via templateprotected sequential growth and conversion method.Arising from the integration of the rectification effect of Au-CdS and AuTiO_(2) Schottky barriers,the Janus configuration of the Cd S-TiO_(2) domains,the plasmonic effect of Au nanosphere,and the Zscheme charge transportation,the Cd S-Au-TiO_(2) Janus structure showed high efficiency in the model photocatalytic degradation of methyl orange(MO)dye.Importantly,the well-defined structural order allowed the identification of the correlation between the structure and the catalytic performance.We believe that the synthetic control and the mechanism insights would help the design and synthesis of sophisticated nanostructures,and would eventually promote their applications in photocatalysis fields.

Bioinspired design of integral molded Janus silk fibroin-MXene evaporator for efficient solar vapor generation

Solar vapor generation is a promising sustainable technology that uses solar distillation to produce fresh water from seawater and wastewater,helping relieve global water resource shortage.Here,inspired by naturally grown integrally molded mulberry leaves with a Janus hydrophilic and hydrophobic structure,a novel,simple,and efficient integrated molding method is proposed to break through the limitations of the traditional split manufacturing strategy and realizes the integrated formation of Janus evaporator.Based on the spontaneous sedimentation characteristics of MXene in silk fibroin solution and its regulation of mesoscopic structure and hydrophilicity of silk fibroin,layered structures with different compositions and hydrophilicities were obtained in one step.Meanwhile,ethanol and glutaraldehyde were added to construct a physical crystallization-chemical crosslinking dual stabilization structure in silk fibroin.Our evaporator has the evaporation rate of 3.07 kg·m^(-2)·h^(-1) and the efficiency of 86.8%under 1 sun and maintains high evaporation performance under various extreme test conditions including vigorous washing,repeated compression,and high-intensity ultraviolet(UV)irradiation.Additionally,the evaporator performs well in practical application scenarios,its evaporation rate in the simulated Dead Sea seawater exceeds 2.13 kg·m^(-2)·h^(-1),and more than 99.9%of the salt,heavy metal ions,oil pollution,and dyes are purified.

A unique Janus PdZn-Co catalyst for enhanced photocatalytic syngas production from CO_(2) and H_(2)O

The development of excellent catalyst to achieve photocatalytic syngas production from CO_(2) and H_(2)O is a prospective and sustainable strategy to alleviate environment and energy crisis. In this study, a unique Janus PdZn-Co catalyst is prepared by annealed the Pd/IRMOF-3(Co, Zn) precursor. Due to the strong interaction, the electron transfers from PdZn terminal to Co terminal in the Janus structure. The electron-received Co terminal facilitates Co sites coordinate with the electrophilic C atom of CO_(2) and the electron-donated PdZn center is easier to coordinate with nucleophilic O atoms of H_(2)O or C=O bonds.The charge redistribution enhances the absorption of CO_(2) and H2O, which promotes H_(2) evolution and CO production. In addition, the carbon shell effectively suppresses the metal core agglomeration and facilitates the electron transmission from photosensitizer to metallic active sites. Meanwhile, the ratio of CO/H_(2) can be regulated(~3:1 to 2:1) by adjusting the proportion of Co and PdZn. The Janus structure and graphite carbon synergistically play a profound impact on improving the photocatalytic performance.The optimized PdZn-Co catalyst exhibits a superior photocatalytic CO production rate(20.03 μmol/h) and the H_(2) generation rate(9.90 μmol/h) with a ratio of CO/H_(2)= 2.02.

Janus(BNNS/ANF)-(AgNWs/ANF)thermal conductivity composite films with superior electromagnetic interference shielding and Joule heating performances

Highly thermal conductivity materials with excellent electromagnetic interference shielding and Joule heating performances are ideal for thermal management in the next generation of communication industry,artificial intelligence and wearable electronics.In this work,silver nanowires(AgNWs)are prepared using silver nitrate as the silver source and ethylene glycol as the solvent and reducing agent,and boron nitride(BN)is performed to prepare BN nanosheets(BNNS)with the help of isopropyl alcohol and ultrasonication-assisted peeling method,which are compounded with aramid nanofibers(ANF)prepared by chemical dissociation,respectively,and the(BNNS/ANF)-(AgNWs/ANF)thermal conductivity and electromagnetic interference shielding composite films with Janus structures are prepared by the"vacuum-assisted filtration and hot-pressing"method.Janus(BNNS/ANF)-(AgNWs/ANF)composite films exhibit"one side insulating,one side conducting"performance,the surface resistivity of the BNNS/ANF surface is 4.7×10^(13) Ω,while the conductivity of the AgNWs/ANF surface is 5,275 S/cm.And Janus(BNNS/ANF)-(AgNWs/ANF)composite film with thickness of 95 pm has a high in-plane thermal conductivity coefficient of 8.12 W/(m·K)and superior electromagnetic interference shielding effectiveness of 70 dB.The obtained composite film also has excellent tensile strength of 122.9 MPa and tensile modulus and 2.7 GPa.It also has good temperature-voltage response characteristics(high Joule heating temperature at low supply voltage(5 V,215.0℃),fast response time(10 s)),excellent electrical stability and reliability(stable and constant real-time relative resistance under up to 300 cycles and 1,500 s of tensile-bending fatigue work tests).

一种面向高稳定锂金属负极的具有仿生离子通道的人工界面层

锂金属具有氧化还原电位低、理论比容量大等优点,是下一代高比能电池极具发展前景的负极.然而,锂枝晶生长和低可逆性严重阻碍了高比能锂金属电池的发展.受启发于生物细胞膜结构,本文采用涂布法在锂金属表面成功构筑了一种具有仿生离子通道的人工界面固体电解质层(CAL).该CAL中大量带负电荷的离子通道可以促进锂离子均匀、快速的输运,有利于稳定、均匀地进行锂沉积/剥离.此外,在循环过程中,CAL底部与锂金属发生原位转化反应,生成了一层富含亲锂性无机组分的过渡层,促进了锂离子的扩散并抑制了锂金属与电解液的连续副反应.因此,形成的具有双面神结构的人工界面固体电解质层(CAJL)使得锂金属负极可以在10 mA cm^(-2)的高电流密度和10 mAh cm^(-2)的高面积容量下长期稳定循环.更重要的是,基于CAJL功能化锂金属负极的锂硫软包电池实现了429.2 Wh kg^(-1)的高能量密度.

In Situ Transmission Electron Microscopy Observations of the Growth Process of Fe3O4–Ag Nanoparticles

The properties of nanocrystals are highly dependent on their morphology, composition and structure. To obtain full control over their properties, the behavior of nanocrystals under external stimuli, such as heat treatment, needs to be understood. Herein, to in situ observe their microstructure and morphology changes, Fe3O4–Ag heterodimers were selected as a model system. Their structural changes after heat treatment were investigated by in situ transmission electron microscopy. A combination of real-time imaging with elemental analysis enabled observation of the transformation of Fe3O4–Ag heterodimers having a loose interface configuration to those with a Janus structure at the atomic scale after heating from room temperature to 600 °C. After incubation at 600 °C for 32 min, two kinds of Janus structures could be seen, including a clear linear interface in the Fe3O4–Ag heterodimers and a semi-crescent-shaped interface between the Ag and Fe3O4 nanoparticles(NPs). These dynamic observations provide unique insights into NP growth mechanisms, which are essential for understanding and controlling the structure and morphology of nanoparticles.

Polar materials for photocatalytic applications:A critical review

The critical challenges of the energy crisis and environmental degradation promote innovative approaches for energy conversion.Semiconductor-based photocatalytic technology,which transforms solar energy into chemical energy,emerges as a promising solution.However,the practical application of this technology faces several challenges,such as the rapid recombination of photogenerated electrons and holes,significantly limiting photocatalytic efficiency.In this review,we provide a detailed discussion,an insightful perspective,and a critical evaluation of recent advances,challenges,and opportunities in the field of photocatalysis using polar materials.We present a comprehensive examination of the photocatalytic mechanisms,activity,and diverse applications of photocatalysts based on polar materials.We also briefly discuss the engineering design of polar photocatalysis in experiments and its scalability in the industry.This review outlines future trends and potential breakthroughs in the photocatalytic field using polar materials,projecting their transformative impact on environmental chemistry and energy engineering.