查看更多>>摘要：Herein,we present a photoinduced,CeCl3-catalyzed three-component decarboxylative reaction that couples carboxylic acids,alkenes and tert-butyl hydroperoxide for the formation of various organic peroxides.The ligand-to-metal charge transfer(LMCT)excitation mode allows the decarboxylative alkylation-peroxidation reaction to occur under mild conditions,and is well applicable to primary,secondary and tertiary carboxylic acids and styrene derivatives.
查看更多>>摘要：Female hormone detection,particularly non-invasive monitoring progesterone(P4)levels in body fluids,plays a critical role in female health management and disease diagnosis.However,the challenge still exists because of the ultralow abundance of P4(＜100 pmol/L)in sweat and saliva,necessitating highly sensitive methods for wearable detection.Herein,we present a simple sandpaper-templated stretchable immunosensing electrode designed for ultra-sensitive detection of P4 at sub-picomolar level.A molding technique is employed to replicate the sandpaper textures to provide a microstructured elastomeric substrate for electrode preparation.Such microstructured surface coated with poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonate)(PEDOT:PSS)/LiTFSI[LiTFSl=lithium bis(trifluoromethanesulfonyl)imide]provided a stretchable polymer electrode with high conductivity,and further decoration with gold nanoparticles(AuNPs)enabled the immunosensing for P4 by electrochemical impedance spectroscopy(EIS)measurements.Through adjusting the AuNPs deposition conditions,ultrasensitive detection of P4 is realized with a low limit of detection(LOD)of ca.10 fmol/L and a tunable dynamic range up to μmol/L.Notably,the stretchable electrode exhibits stable electrochemical performance,enabling the detection of P4 at sub-picomolar levels even under mechanical strain of 30％.This innovative electrochemical sensor holds significant promise for non-invasive,on-site monitoring of P4 levels in healthcare,as well as hormone detection in food safety and environment surveillance.
查看更多>>摘要：Polyferrocene macrocycles hold immense potential in the fields of molecular electronics and electrochemistry,primarily due to their multiple metal centers.However,developing highly efficient synthetic strategies for constructing these rings remains a significant challenge.In this study,we successfully synthesized tri-ferrocenyl macrocycles using Pt-mediated coupling strategy and determined their configuration using single-crystal X-ray diffraction analysis,revealing a structure reminiscent of the Penrose Stair.We comprehensively investigated the macrocycle's structure,photophysical properties,and employed density functional theory(DFT)calculations to gain further insights.Notably,this macrocycle exhibits several advantageous features,including a flexible structure,good solubility,and a highly efficient synthetic pathway.
查看更多>>摘要：Due to their precise atomic structures,photoluminescent copper nanoclusters(Cu NCs)have promising applications in basic research and technical applications,such as bioimaging,cell labeling,phototherapy,and photoactivation catalysis.In this work,we report a simple strategy for synthesizing novel CuNCs co-protected by alkynyl and phosphine ligands with the molecular formula[Cu7(PPh3)10(PE)3(CH3O)](Cu4@Cu3).Single-crystal X-ray crystallography reveals that the NC core exhibits an open square structure and an overall pyramid shape.Two Cu4@Cu3 units are connected through weak interactions to form dimers in crystals,creating a molecular cage that looks like two tightly closed bowls.Cu4@Cu3 exhibits dual emission in the visible region.It is also an aggregation-induced emission(AIE)-active luminescent substance,which exhibits strong emission in the visible light region when aggregated.Besides,it has the properties of radioluminescent(RL)and could be a potential scintillator material.This study not only enriches the types of atomically accurate AIE clusters,but also holds significant importance for the development of a new generation of high-performance and environmentally friendly X-ray scintillators.
查看更多>>摘要：Sensing materials possessing intrinsic color perception are indispensable prerequisites for the development of filterless photosensors,which could eliminate the need for complex device designs and avoid color distortion in post-processing.Traditional materials are constrained by complex processing methods and limited stability.Herein,a color-photosensitive array based on ionic liquid with selective photothermal conversion(ILSPC)has been developed for intrinsic color perception.Relying on the selective absorption,photothermal conversion,and thermosensitivity of ILSPC,a photo-thermo-electric sensing system has been constructed.Besides,the versatility of the two algorithms has been validated in color reconstruction and electrical signal prediction.As an exploration,the photosensitive array showcases promising color recognition capabilities,potentially propelling the evolution of flexible photosensors.
查看更多>>摘要：Perovskite quantum dots(PQDs)have demonstrated great promise in bioimaging applications owing to their outstanding photophysical properties.Nonetheless,their practicality is seriously limited by the instability of PQDs against moisture.Here we develop a post-synthetic ligand exchange strategy to construct silica-coated PQD(PQD@SiO2)nanocrystals,which results in the simultaneous improvement of photoluminescence efficiency and moisture stability.More importantly,compared to the classical in-situ ligand exchange method of fabricating PQD@SiO2,the issues of chemical etching and resultant photoluminescence degradation are judiciously overcome.Employing the proposed PQD@SiO2,we showcase their robust usefulness in labeling chlorella,paving the way for PQD-based in-vivo photoluminescence bioimaging methodology.
查看更多>>摘要：Dynamic photoresponsive molecular crystals are promising candidates for making intelligent devices and materials in the future.Here,we synthesized a new photoactive molecule(E)-2,2-dimethyl-5-[3-(naphthalen-1-yl)allylide]-1,3-dioxane-4,6-dione[(E)-DNADD]that undergoes an E-to-Z photoisomerization in both liquid solution and solids when exposed to visible light(405 nm).Compared to the bulk crystals,the photoresponsive behavior in microcrystals was profoundly improved.Highly crystalline(E)-DNADD microplate crystals exhibit robust motions,including bending,curling,and coiling under light irradiation.The photoproduct conversion of the photochemical reaction in the microplate is no more than 20％,while the large bending curvature of the coiled illuminated samples was estimated at approximately 150-300 mm-1,comparable to some photoactive nanowires.Our results indicate that shrinking crystal dimensions can boost the photoresponses in molecular crystals and provide a facile strategy for developing dynamic molecular crystals at the microscopic scale.
查看更多>>摘要：Although glucose electrochemical sensors based on enzymes play a dominant role in market,their stability remains a problem due to the inherent nature of enzymes.Therefore,glucose sensors that are independent on enzymes have attracted more attention for the development of stable detection devices.Here we present an enzyme-free glucose sensor based on Ni(OH)2 and reduced graphene oxide(rGO).The as-fabricated sensor still exhibits excellent electrocatalytic activity for detecting glucose under enzyme independent conditions.The enhanced catalytic performance may due to synergistic effect as follows:(ⅰ)the interaction between the Ni2+and π electron of graphene induces the formation of the β-phase Ni(OH)2 with higher catalytic activity;(ⅱ)the frozen dry process works as a secondary filtration,getting rid of poorly formed Ni(OH)2 particles with low catalytic activity;(ⅲ)the rGO network with good conductivity provides a good electronic pathway for promoting electron transfer to reduce the response time.Based on the synergistic effect,the sensor exhibits a wide linear detection range from 0.2 μmol/L to 1.0 μmol/L and a low detection limit(0.1 μmol/L,S/N=3).The excellent detection performance,as well as the easy and low-cost preparation method,suggests the promising applicability of the sensor in the glucose detection market.
查看更多>>摘要：Nb-based tungsten bronze oxides have emerged as attractive materials in various fields,owing to the structural openings and simple synthesis method.In this work,the tetragonal tungsten bronze(TTB)NaWNbO6 was prepared by solid state reaction at a relatively low temperature of 775 ℃.The local structure was systematically studied by solid state nuclear magnetic resonance(SSNMR)with the aid of transition electronic microscopy(TEM).The analysis indicates that NaWNbO6 has pentagonal,square,and triangular tunnels.Notably,square tunnels were partly occupied(50％)by Na,which creates the ability for the Li-ion storage with a volumetric capacity of 210 A·h·L-1 at 0.2 C.The 2D 23Na-23Na EXSY results further suggest the ability of ions to fast exchange between the tetragonal and pentagonal tunnels,resulting in a high-rate performance 20 C.
LI ChengqiuZHOU ChaoyongMEI ShilinYAO Changjiang...
927-934页
查看更多>>摘要：The energy density and lifespan of prototype Li-S batteries under high sulfur loading and lean electrolyte have been mainly restricted by the incomplete interconversion between insulating S8 and Li2S.The introduction of an electrocatalyst has been preserved as an effective way to breakthrough the bottleneck of the interconversion rate.Herein,we demonstrate a novel bidirectional redox mediator,insoluble dithiobisphthalimide(DTPI),as the electrocatalyst for both S8 reduction and Li2S oxidation.Due to the dual-functional role of both electron/Li+donor and acceptor,DTPI can efficiently accelerate the redox reactions during charge/discharge and significantly alleviate the incomplete conversion of sulfur species.Consequently,the Li-S batteries with DTPI deliver superior specific capacity and cycling stability in comparison with those without DTPI.Especially,the redox mediator is scalable for synthesis and the DTPI-based 5 A·h pouch cell delivers a specific discharge capacity of around 870 mA·h·g-1 at 0.1 C(1 C=1675 mA/g)without capacity fading over 80 cycles.The bidirectional catalysis mechanism has been studied through theoretical calculation and ex-situ characterization of the cathode materials.This work approves the effectiveness of bidirectional organic redox mediator in the construction of practical Li-S batteries.
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