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    Laser-Induced Methanol Decomposition for Ultrafast Hydrogen Production

    Weiwei CaoYinwu LiBo YanZhiping Zeng...
    131-137页
    查看更多>>摘要:Methanol(CH3OH)is a liquid hydrogen(H2)source that effectively releases H2 and is convenient for transportation.Traditional thermocatalytic CH3OH reforming reaction is used to produce H2,but this process needs to undergo high reaction temperature(e.g.,200 ℃)along with a catalyst and a large amount of carbon dioxide(C02)emission.Although photocatalysis and photothermal catalysis under mild conditions are proposed to replace the traditional thermal catalysis to produce H2 from CH3OH,they still inevitably produce CO2 emissions that are detrimental to carbon neutrality.Here,we,for the first time,report an ultrafast and highly selective production of H2 without any catalysts and no CO2 emission from CH3OH by laser bubbling in liquid(LBL)at room temperature and atmospheric pressure.We demonstrate that a super high H2 yield rate of 33.41 mmol·h-1 with 94.26%selectivity is achieved upon the laser-driven process.This yield is 3 orders of magnitude higher than the best value reported for photocatalytic and photothermal catalytic H2 production from CH3OH to date.The energy conversion efficiency of laser light to H2 and CO can be up to 8.5%.We also establish that the far from thermodynamic equilibrium state with high temperature inside the laser-induced bubble and the kinetic process of rapid quenching of bubbles play crucial roles in H2 production upon LBL.Thermodynamically,the high temperature induced using laser in bubbles ensures fast and efficient release of H2 from CH3OH decomposition.Kinetically,rapidly quenching of laser-induced bubbles can inhibit reverse reaction and can keep the products in the initial stage,which guarantees high selectivity.This study presents a laser-driven ultrafast and highly selective production of H2 from CH3OH under normal conditions beyond catalytic chemistry.

    Traditional Chinese Medicine Integrated Responsive Microneedles for Systemic Sclerosis Treatment

    Xi LuanXiaoxuan ZhangMin NieYuanjin Zhao...
    139-147页
    查看更多>>摘要:Traditional Chinese medicine,such as Tripterygium wilfordii and Paeonia lactiflora,has potential values in treating systemic sclerosis(SSc)and other autoimmune diseases,while their toxic side effect elimination and precise tropical drug delivery are still challenges.Here,we present multiple traditional Chinese medicine integrated photoresponsive black phosphorus(BP)microneedles(MNs)with the desired features for the SSc treatment.By employing a template-assisted layer-by-layer curing method,such MNs with triptolide(TP)/paeoniflorin(Pae)needle tips and BP-hydrogel needle bottoms could be well generated.The combined administration of TP and Pae can not only provide anti-inflammatory,detoxification,and immunomodulatory effects to treat skin lesions in the early stage of SSc but also remarkably reduce the toxicity of single drug delivery.Besides,the additive BPs possess good biocompatibility and near-infrared(NIR)responsiveness,imparting the MN photothermal-controlled drug release capability.Based on these features,we have demonstrated that the traditional Chinese medicine integrated responsive MNs could effectively improve skin fibrosis and telangiectasia,reduce collagen deposition,and reduce epidermal thickness in the SSc mouse models.These results indicated that the proposed Chinese medicine integrated responsive MNs had enormous potential in clinical therapy of SSc and other diseases.

    An Aerial-Wall Robotic Insect That Can Land,Climb,and Take Off from Vertical Surfaces

    Qian LiHaoze LiHuan ShenYangguang Yu...
    149-163页
    查看更多>>摘要:Insects that can perform flapping-wing flight,climb on a wall,and switch smoothly between the 2 locomotion regimes provide us with excellent biomimetic models.However,very few biomimetic robots can perform complex locomotion tasks that combine the 2 abilities of climbing and flying.Here,we describe an aerial-wall amphibious robot that is self-contained for flying and climbing,and that can seamlessly move between the air and wall.It adopts a flapping/rotor hybrid power layout,which realizes not only efficient and controllable flight in the air but also attachment to,and climbing on,the vertical wall through a synergistic combination of the aerodynamic negative pressure adsorption of the rotor power and a climbing mechanism with bionic adhesion performance.On the basis of the attachment mechanism of insect foot pads,the prepared biomimetic adhesive materials of the robot can be applied to various types of wall surfaces to achieve stable climbing.The longitudinal axis layout design of the rotor dynamics and control strategy realize a unique cross-domain movement during the flying-climbing transition,which has important implications in understanding the takeoff and landing of insects.Moreover,it enables the robot to cross the air-wall boundary in 0.4 s(landing),and cross the wall-air boundary in 0.7 s(taking off).The aerial-wall amphibious robot expands the working space of traditional flying and climbing robots,which can pave the way for future robots that can perform autonomous visual monitoring,human search and rescue,and tracking tasks in complex air-wall environments.

    Body-Shaping Membrane to Regenerate Breast Fat by Elastic Structural Holding

    Hye-Seon KimJeongeun ParkHyun-Su HaSewoom Baek...
    165-180页
    查看更多>>摘要:Tissue regeneration requires structural holding and movement support using tissue-type-specific aids such as bone casts,skin bandages,and joint protectors.Currently,an unmet need exists in aiding breast fat regeneration as the breast moves following continuous body motion by exposing the breast fat to dynamic stresses.Here,the concept of elastic structural holding is applied to develop a shape-fitting moldable membrane for breast fat regeneration("adipoconductive")after surgical defects are made.The membrane has the following key characteristics:(a)It contains a panel of honeycomb structures,thereby efficiently handling motion stress through the entire membrane;(b)a strut is added into each honeycomb in a direction perpendicular to gravity,thereby suppressing the deformation and stress concentration upon lying and standing;and(c)thermo-responsive moldable elastomers are used to support structural holding by suppressing large deviations of movement that occur sporadically.The elastomer became moldable upon a temperature shift above Tm.The structure can then be fixed as the temperature decreases.As a result,the membrane promotes adipogenesis by activating mechanotransduction in a fat miniature model with pre-adipocyte spheroids under continuous shaking in vitro and in a subcutaneous implant placed on the motion-prone back areas of rodents in vivo.

    Magnetic Fields Reduce Apoptosis by Suppressing Phase Separation of Tau-441

    Wen-Juan LinWen-Pu ShiWan-Yi GeLiang-Liang Chen...
    181-197页
    查看更多>>摘要:The biological effects of magnetic fields(MFs)have been a controversial issue.Fortunately,in recent years,there has been increasing evidence that MFs do affect biological systems.However,the physical mechanism remains unclear.Here,we show that MFs(16 T)reduce apoptosis in cell lines by inhibiting liquid-liquid phase separation(LLPS)of Tau-441,suggesting that the MF effect on LLPS may be one of the mechanisms for understanding the"mysterious"magnetobiological effects.The LLPS of Tau-441 occurred in the cytoplasm after induction with arsenite.The phase-separated droplets of Tau-441 recruited hexokinase(HK),resulting in a decrease in the amount of free HK in the cytoplasm.In cells,HK and Bax compete to bind to the voltage-dependent anion channel(VDAC I)on the mitochondrial membrane.A decrease in the number of free HK molecules increased the chance of Bax binding to VDAC I,leading to increased Bax-mediated apoptosis.In the presence of a static MF,LLPS was marked inhibited and HK recruitment was reduced,resulting in an increased probability of HK binding to VDAC I and a decreased probability of Bax binding to VDAC I,thus reducing Bax-mediated apoptosis.Our findings revealed a new physical mechanism for understanding magnetobiological effects from the perspective of LLPS.In addition,these results show the potential applications of physical environments,such as MFs in this study,in the treatment of LLPS-related diseases.

    Orthogonal Combinatorial Raman Codes Enable Rapid High-Throughput-Out Library Screening of Cell-Targeting Ligands

    Yuchen TangXingxing ZhengTingjuan Gao
    199-208页
    查看更多>>摘要:High-throughput assays play an important role in the fields of drug discovery,genetic analysis,and clinical diagnostics.Although super-capacity coding strategies may facilitate labeling and detecting large numbers of targets in a single assay,practically,the constructed large-capacity codes have to be decoded with complicated procedures or are lack of survivability under the required reaction conditions.This challenge results in either inaccurate or insufficient decoding outputs.Here,we identified chemical-resistant Raman compounds to build a combinatorial coding system for the high-throughput screening of cell-targeting ligands from a focused 8-mer cyclic peptide library.The accurate insitu decoding results proved the signal,synthetic,and functional orthogonality for this Raman coding strategy.The orthogonal Raman codes allowed for a rapid identification of 63 positive hits at one time,evidencing a high-throughput-out capability in the screening process.We anticipate this orthogonal Raman coding strategy being generalized to enable efficient high-throughput-out screening of more useful ligands for cell targeting and drug discovery.

    Recent Advances in Electrochemical-Based Silicon Production Technologies with Reduced Carbon Emission

    Feng TianZhongya PangShen HuXueqiang Zhang...
    209-236页
    查看更多>>摘要:Sustainable and low-carbon-emission silicon production is currently one of the main focuses for the metallurgical and materials science communities.Electrochemistry,considered a promising strategy,has been explored to produce silicon due to prominent advantages:(a)high electricity utilization efficiency;(b)low-cost silica as a raw material;and(c)tunable morphologies and structures,including films,nanowires,and nanotubes.This review begins with a summary of early research on the extraction of silicon by electrochemistry.Emphasis has been placed on the electro-deoxidation and dissolution-electrodeposition of silica in chloride molten salts since the 21st century,including the basic reaction mechanisms,the fabrication of photoactive Si films for solar cells,the design and production of nano-Si and various silicon components for energy conversion,as well as storage applications.Besides,the feasibility of silicon electrodeposition in room-temperature ionic liquids and its unique opportunities are evaluated.On this basis,the challenges and future research directions for silicon electrochemical production strategies are proposed and discussed,which are essential to achieve large-scale sustainable production of silicon by electrochemistry.

    Inhibition of Defect-Induced Ice Nucleation,Propagation,and Adhesion by Bioinspired Self-Healing Anti-Icing Coatings

    Shu TianRuiqi LiXinmeng LiuJiancheng Wang...
    237-246页
    查看更多>>摘要:Anti-icing coatings on outdoor infrastructures inevitably suffer from mechanical injuries in numerous icing scenarios such as hailstorms,sandstorms,impacts of foreign objects,and icing-deicing cycles.Herein,the mechanisms of surface-defect-induced icing are clarified.At the defects,water molecules exhibit stronger adsorption and the heat transfer rate increases,accelerating the condensation of water vapor as well as ice nucleation and propagation.Moreover,the ice-defect interlocking structure increases the ice adhesion strength.Thus,a self-healing(at-20 ℃)antifreeze-protein(AFP)-inspired anti-icing coating is developed.The coating is based on a design that mimics the ice-binding and non-ice-binding sites in AFPs.It enables the coating to markedly inhibit ice nucleation(nucleation temperature<-29.4 ℃),prevent ice propagation(propagation rate<0.00048 cm2/s),and reduce ice adhesion on the surface(adhesion strength<38.9 kPa).More importantly,the coating can also autonomously self-heal at-20 ℃,as a result of multiple dynamic bonds in its structure,to inhibit defect-induced icing processes.The healed coating sustains high anti-icing and deicing performance even under various extreme conditions.This work reveals the in-depth mechanism of defect-induced ice formation as well as adhesion,and proposes a self-healing anti-icing coating for outdoor infrastructures.

    Discovery of Partial Differential Equations from Highly Noisy and Sparse Data with Physics-Informed Information Criterion

    Hao XuJunsheng ZengDongxiao Zhang
    247-259页
    查看更多>>摘要:Data-driven discovery of partial differential equations(PDEs)has recently made tremendous progress,and many canonical PDEs have been discovered successfully for proof of concept.However,determining the most proper PDE without prior references remains challenging in terms of practical applications.In this work,a physics-informed information criterion(PIC)is proposed to measure the parsimony and precision of the discovered PDE synthetically.The proposed PIC achieves satisfactory robustness to highly noisy and sparse data on 7 canonical PDEs from different physical scenes,which confirms its ability to handle difficult situations.The PIC is also employed to discover unrevealed macroscale governing equations from microscopic simulation data in an actual physical scene.The results show that the discovered macroscale PDE is precise and parsimonious and satisfies underlying symmetries,which facilitates understanding and simulation of the physical process.The proposition of the PIC enables practical applications of PDE discovery in discovering unrevealed governing equations in broader physical scenes.

    Fast Blood Oxygenation through Hemocompatible Asymmetric Polymer of Intrinsic Microporosity Membranes

    Xinxi HuangJunping HuangPengcheng SuWanbin Li...
    261-270页
    查看更多>>摘要:Membrane technology has attracted considerable attention for chemical and medical applications,among others.Artificial organs play important roles in medical science.A membrane oxygenator,also known as artificial lung,can replenish 02 and remove C02 of blood to maintain the metabolism of patients with cardiopulmonary failure.However,the membrane,a key component,is subjected to inferior gas transport property,leakage propensity,and insufficient hemocompatibility.In this study,we report efficient blood oxygenation by using an asymmetric nanoporous membrane that is fabricated using the classic nonsolvent-induced phase separation method for polymer of intrinsic microporosity-1.The intrinsic superhydrophobic nanopores and asymmetric configuration endow the membrane with water impermeability and gas ultrapermeability,up to 3,500 and 1,100 gas permeation units for C02 and 02,respectively.Moreover,the rational hydrophobic-hydrophilic nature,electronegativity,and smoothness of the surface enable the substantially restricted protein adsorption,platelet adhesion and activation,hemolysis,and thrombosis for the membrane.Importantly,during blood oxygenation,the asymmetric nanoporous membrane shows no thrombus formation and plasma leakage and exhibits fast 02 and C02 transport processes with exchange rates of 20 to 60 and 100 to 350 ml m-2 min-1,respectively,which are 2 to 6 times higher than those of conventional membranes.The concepts reported here offer an alternative route to fabricate high-performance membranes and expand the possibilities of nanoporous materials for membrane-based artificial organs.