Photoelectrochemical (PEC) small-molecule oxidation can selectively transform substrates into high-value-added fine chemicals and increase the rate of cathode hydrogen evolution. Nevertheless, achieving high-selectivi...Photoelectrochemical (PEC) small-molecule oxidation can selectively transform substrates into high-value-added fine chemicals and increase the rate of cathode hydrogen evolution. Nevertheless, achieving high-selectivity PEC oxidation of small molecules to produce specific products is a very challenging task. In general, selectivity can be improved by changing the surface catalyticsites of the photoanode and modulating the interfacial environments of the reactions. Herein, recent advances in approaches to improving selective PEC oxidation of small molecules are introduced. We first briefly discuss the basic concept and fundamentals of small-molecule PEC oxidation. The reported approaches to improving the performance of selective PEC oxidation of small molecules are highlighted from two aspects: (1) changing the surface properties of photoanodes by selecting suitable materials or modifying the photoanodes and (2) mediating the oxidation reactions using redox mediators. The PEC oxidation mechanism of these studies is emphasized. We also discuss the challenges in this research direction and offer a perspective on the further development of selective PEC-based small-molecule transformation.展开更多
Sensitive detection of Staphylococcus aureus enterotoxin B(SEB)is of importance for preventing food poisoning from threatening human health.In this work,an electrochemical and colorimetric dual-signal detection assay ...Sensitive detection of Staphylococcus aureus enterotoxin B(SEB)is of importance for preventing food poisoning from threatening human health.In this work,an electrochemical and colorimetric dual-signal detection assay of SEB was developed.The probe(Ab2/AuPt@Fe-N-C)was bound to SEB captured by Ab1,where the Ab2/AuPt@Fe-N-C triggered methylene blue degradation and resulted in the decrease of electrochemical signal.Furthermore,the probe catalyzed the oxidation of 3,3’,5,5’-tetramethyl biphenyl to generate a colorimetric absorbance at 652 nm.Once the target was captured and formed a sandwich-like complex,the color changed from colorless to blue.SEB detection by colorimetric and electrochemical methods showed a linear relationship in the concentration ranges of 0.0002-10.0000 and 0.0005-10.0000 ng/mL,with limits of detection of 0.0667 and 0.1670 pg/mL,respectively.The dual-signal biosensor was successfully used to detect SEB in milk and water samples,which has great potential in toxin detection in food and the environment.展开更多
Smart wearable devices are regarded to be the next prevailing technology product after smartphones and smart homes,and thus there has recently been rapid development in flexible electronic energy storage devices.Among...Smart wearable devices are regarded to be the next prevailing technology product after smartphones and smart homes,and thus there has recently been rapid development in flexible electronic energy storage devices.Among them,flexible solid-state zinc-air batteries have received widespread attention because of their high energy density,good safety,and stability.Efficient bifunctional oxygen electrocatalysts are the primary consideration in the development of flexible solid-state zinc-air batteries,and self-supported air cathodes are strong candidates because of their advantages including simplified fabrication process,reduced interfacial resistance,accelerated electron transfer,and good flexibility.This review outlines the research progress in the design and construction of nanoarray bifunctional oxygen electrocatalysts.Starting from the configuration and basic principles of zinc-air batteries and the strategies for the design of bifunctional oxygen electrocatalysts,a detailed discussion of self-supported air cathodes on carbon and metal substrates and their uses in flexible zinc-air batteries will follow.Finally,the challenges and opportunities in the development of flexible zinc-air batteries will be discussed.展开更多
Norovirus(NoV)is regarded as one of the most common causes of foodborne diarrhea in the world.It is urgent to identify the pathogenic microorganism of the diarrhea in short time.In this work,we developed an electroche...Norovirus(NoV)is regarded as one of the most common causes of foodborne diarrhea in the world.It is urgent to identify the pathogenic microorganism of the diarrhea in short time.In this work,we developed an electrochemical and colorimetric dual-mode detection for NoV based on the excellent dual catalytic properties of copper peroxide/COF-NH_(2)nanocomposite(CuO_(2)@COF-NH_(2)).For the colorimetric detection,NoV can be directly detected by the naked eye based on CuO_(2)@COF-NH_(2)as a laccase-like nonazyme using“peptide-NoV-antibody”recognition mode.The colorimetric assay displayed a wide and quality linear detection range from 1 copy/mL to 5000 copies/mL of NoV with a low limit of detection(LOD)of 0.125 copy/mL.For the electrochemical detection of NoV,CuO_(2)@COF-NH_(2)showed an oxidation peak of copper ion from Cu^(+)to Cu^(2+)using“peptide-NoV-antibody”recognition mode.The electrochemical assay showed a linear detection range was 1-5000 copies/mL with a LOD of 0.152 copy/mL.It's worthy to note that this assay does not need other electrical signal molecule,which provide the stable and sensitive electrochemial detection for NoV.The electrochemical and colorimetric dual-mode detection was used to detect NoV in foods and faceal samples,which has the potential for improving food safety and diagnosing of NoV-infected diarrhea.展开更多
Herein,a novel interference-free surface-enhanced Raman spectroscopy(SERS)strategy based on magnetic nanoparticles(MNPs)and aptamer-driven assemblies was proposed for the ultrasensitive detection of histamine.A core-s...Herein,a novel interference-free surface-enhanced Raman spectroscopy(SERS)strategy based on magnetic nanoparticles(MNPs)and aptamer-driven assemblies was proposed for the ultrasensitive detection of histamine.A core-satellite SERS aptasensor was constructed by combining aptamer-decorated Fe_(3)O_(4)@Au MNPs(as the recognize probe for histamine)and complementary DNA-modified silver nanoparticles carrying 4-mercaptobenzonitrile(4-MBN)(Ag@4-MBN@Ag-c-DNA)as the SERS signal probe for the indirect detection of histamine.Under an applied magnetic field in the absence of histamine,the assembly gave an intense Raman signal at“Raman biological-silent”region due to 4-MBN.In the presence of histamine,the Ag@4-MBN@Ag-c-DNA SERS-tag was released from the Fe_(3)O_(4)@Au MNPs,thus decreasing the SERS signal.Under optimal conditions,an ultra-low limit of detection of 0.65×10^(-3)ng/mL and a linear range 10^(-2)-10^5 ng/mL on the SERS aptasensor were obtained.The histamine content in four food samples were analyzed using the SERS aptasensor,with the results consistent with those determined by high performance liquid chromatography.The present work highlights the merits of indirect strategies for the ultrasensitive and highly selective SERS detection of small biological molecules in complex matrices.展开更多
The in vitro digestion models mimicking the gastrointestinal(GI)tract of general population and lipid indigestion patients(with lower levels of bile salts or pancreatic lipase)were selected to investigate whether diac...The in vitro digestion models mimicking the gastrointestinal(GI)tract of general population and lipid indigestion patients(with lower levels of bile salts or pancreatic lipase)were selected to investigate whether diacylglycerols(DAGs)are potential good lipid sources for these patients.Linseed oil-based DAG(LD)and linseed oil(LT)were selected.LD-based emulsion((83.74±1.23)%)had higher lipolysis degree than LT-based emulsion((74.47±1.16)%)when monitoring the GI tract of normal population as previously reported.Indigestion conditions seriously decreased the digestive degree of LT-based emulsion((40.23±2.48)%-(66.50±3.70)%)while showed less influence on LD-based emulsion((64.18±2.41)%-(81.85±3.45)%).As opposed to LT-based emulsion,LD-based emulsion exhibited preference for releasing unsaturated fatty acids(especially oleic acid andα-linolenic acid)due to their different glycerolipid compositions.LD-based emulsion showed potential for providing lipids and nutrients(including essential fatty acids)for lipid indigestion patients.展开更多
The sluggish kinetics of the electrochemical oxygen reduction reaction(ORR)in intermediatetemperature solid oxide fuel cells(IT-SOFCs)greatly limits the overall cell performance.In this study,an efficient and durable ...The sluggish kinetics of the electrochemical oxygen reduction reaction(ORR)in intermediatetemperature solid oxide fuel cells(IT-SOFCs)greatly limits the overall cell performance.In this study,an efficient and durable cathode material for IT-SOFCs is designed based on density functional theory(DFT)calculations by co-doping with Nb and Ta the B-site of the SrFeO_(3-δ)perovskite oxide.The DFT calculations suggest that Nb/Ta co-doping can regulate the energy band of the parent SrFeO_(3-δ)and help electron transfer.In symmetrical cells,such cathode with a SrFe_(0.8)Nb_(0.1)Ta_(0.1)O_(3-δ)(SFNT)detailed formula achieves a low cathode polarization resistance of 0.147Ωcm^(2) at 650℃.Electron spin resonance(ESR)and X-ray photoelectron spectroscopy(XPS)analysis confirm that the co-doping of Nb/Ta in SrFeO_(3-δ)B-site increases the balanced concentration of oxygen vacancies,enhancing the electrochemical performance when compared to 20 mol%Nb single-doped perovskite oxide.The cathode button cell with NiSDC|SDC|SFNT configuration achieves an outstanding peak power density of 1.3 W cm^(-2)at 650℃.Moreover,the button cell shows durability for 110 h under 0.65 V at 600℃ using wet H_(2) as fuel.展开更多
With high theoretical energy density and the natural abundance of S, lithium-sulfur(Li–S) batteries are considered to be the promising next generation high-energy rechargeable energy storage devices. However, issues ...With high theoretical energy density and the natural abundance of S, lithium-sulfur(Li–S) batteries are considered to be the promising next generation high-energy rechargeable energy storage devices. However, issues including electronical insulation of S, the lithium polysulfides(Li PSs) dissolution and the short cycle lifespan have prevented Li–S batteries from being practical applied. Feasible settlements of confining Li PSs to reduce the loss of active substances and improve the cycle stability include wrapping sulfur with compact layers, designing matrix with porous or hollow structures, adding adsorbents owning strong interaction with sulfur and inserting polysulfide barriers between cathodes and separators. This review categorizes them into physical and chemical confinements according to the influencing mechanism. With further discussion of their merits and flaws, synergy of the physical and chemical confinement is believed to be the feasible avenue that can guide Li–S batteries to the practical application.展开更多
Rubber leaf powder(an agricultural waste) was treated with potassium permanganate followed by sodium carbonate and its performance in the removal of Pb(Ⅱ) ions from aqueous solution was evaluated.The interactions bet...Rubber leaf powder(an agricultural waste) was treated with potassium permanganate followed by sodium carbonate and its performance in the removal of Pb(Ⅱ) ions from aqueous solution was evaluated.The interactions between Pb(Ⅱ) ions and functional groups on the adsorbent surface were confirmed by Fourier transform infrared(FT-IR) spectroscopy,scanning electron microscopy(SEM) coupled with X-ray energy dispersive spectroscopy(EDX).The effects of several important parameters which can affect adsorption capacity such as pH,adsorbent dosage,initial lead concentration and contact time were studied.The optimum pH range for lead adsorption was 4-5.Even at very low adsorbent dosage of 0.02 g,almost 100% of Pb(Ⅱ) ions(23 mg/L) could be removed.The adsorption capacity was also dependent on lead concentration and contact time,and relatively a short period of time(60-90 min) was required to reach equilibrium.The equilibrium data were analyzed with Langmuir,Freundlich and Dubinin-Radushkevich isotherms.Based on Langmuir model,the maximum adsorption capacity of lead was 95.3 mg/g.Three kinetic models including pseudo first-order,pseudo second-order and Boyd were used to analyze the lead adsorption process,and the results showed that the pseudo second-order fitted well with correlation coefficients greater than 0.99.展开更多
Zinc oxide(ZnO) nanoparticles of varying sizes(20, 44 and 73 nm) have been successfully synthesized by a hybrid electrochemical-thermal method using aqueous sodium bicarbonate electrolyte and sacrificial Zn anode and ...Zinc oxide(ZnO) nanoparticles of varying sizes(20, 44 and 73 nm) have been successfully synthesized by a hybrid electrochemical-thermal method using aqueous sodium bicarbonate electrolyte and sacrificial Zn anode and cathode in an undivided cell under galvanostatic mode at room temperature. The as-synthesized product was characterized by X-ray diffraction(XRD), X-ray photoelectron spectra(XPS), Scanning electron microscopy along with Energy dispersive analysis of X-ray(SEM/EDAX), Transmission electron microscopy(TEM), Ultra Violet- Diffuse reflectance spectroscopic methods(UV-DRS). and UV-DRS spectral methods.The as-synthesized compound were single-crystalline and Rietveld refinement of calcined samples exhibited hexagonal(Wurtzite) structure with space group of P63mc(No.186). The band gaps for synthesized ZnO nanoparticles were 3.07, 3.12 and 3.13 e V, respectively, based on the results of diffuse reflectance spectra(DRS). The electrochemically synthesized ZnO powder was used as photocatalysts for UV-induced degradation of Methylene blue(MB). Photodegradation was also found to be function of exposure time and dye solution p H. It has been found that as-synthesized powder has excellent photocatalytic activity with 92% degradation of MB, indicating ZnO nanoparticles can play an important role as a semiconductor photocatalyst.展开更多
Performance boosting of hybrid metal oxide and metal alloy catalyst is crucial to the water electrolysis for hydrogen generation. Herein, a novel concept of selective fluoridation of metal alloy/oxide hybrid is propos...Performance boosting of hybrid metal oxide and metal alloy catalyst is crucial to the water electrolysis for hydrogen generation. Herein, a novel concept of selective fluoridation of metal alloy/oxide hybrid is proposed to boost their catalytic performance for the oxygen evolution reaction(OER). A well-recognized OER catalyst system of FeNi3 alloy/oxide embedded in nitrogen-doped porous nanofibers(FeNiO/NCF) is employed as a proof of concept, and it is selectively fluoridated by transforming the metal oxide to metal fluoride(FeNiF/NCF). The crystal structure and surface chemical state transformation are well supported by the spectroscopic analysis and the improved electrochemical performance for OER can be well correlated to the phase and structure change. Specifically, FeNiF/NCF can drive the benchmark current density of 10 mA cm-2 at 260 mV with a Tafel slope of 67 mV dec-1, about 70 mV less than that of FeNiO/NCF.Increased catalytic kinetics, rapid charge transfer ability, high catalytic efficiency and stability are also probed by electrochemical analysis. The high surface area and roughness are found mainly generated via the high-temperature annealing for the metal alloy/metal oxide formation, and the low-temperature fluoridation process intrinsically contributes to the active structure formation. It is an efficient and universal approach to increase the catalytic performance of metal alloy/oxide for energy-relevant catalytic reactions.展开更多
An amperometric hydrogen peroxide biosensor using a nanobiocomposite based on neutral red modified carbon nanotubes and co-immobilized glucose oxidase and horseradish peroxidase is reported. Modification of the nanobi...An amperometric hydrogen peroxide biosensor using a nanobiocomposite based on neutral red modified carbon nanotubes and co-immobilized glucose oxidase and horseradish peroxidase is reported. Modification of the nanobiocomposite electrode with neutral red resulted in a sensitive, low-cost and reliable H_2O_2 sensor. The use of carbon nanotubes, as the conductive part of the composite, facilitated fast electron transfer rates. The biosensor was characterized for the influence of p H, potential and temperature. A remarkable feature of the biosensor is the detection of H_2O_2 at low applied potentials where the noise level and interferences are minimal. The sensor has a fast steady-state measuring time of 10 s with a quick response(2 s). The biosensor showed a linear range from 15 n M to 45 m M of H_2O_2 and a detection limit of 5 n M. Nafion, which is used as a binder, makes the determination free from other electroactive substances. The repeatability, reproducibility,stability and analytical performance of the sensor are very good.展开更多
Bimetallic transition metal phosphides(TMPs)as potential candidates for superior electrochemical performance are still facing great challenges in the controllable preparation of two-dimensional(2 D)structures with hig...Bimetallic transition metal phosphides(TMPs)as potential candidates for superior electrochemical performance are still facing great challenges in the controllable preparation of two-dimensional(2 D)structures with high aspect ratio.Herein,a novel structure of quasi-monolayered NiCo-bimetal-phosphide(NiCoP)has been designed and successfully synthesized by the newly developed process combined with ultrasonic-cavitation and phase-transition.This is the first time to break through the controllable preparation of 2 D bimetal-phosphides with a thickness of 0.98 nm in sub-nanoscale.Based on the advantages of 2 D quasi-monolayer structure with dense crystalline-amorphous interface and the reconfigured electronic structure between Ni^(δ+)/Co^(δ+)and P^(δ-),the optimized Ni_(5%)CoP exhibits an outstanding bifunctional performance for electrocatalyzing both hydrogen evolution reaction and oxygen evolution reaction in an alkaline medium.Ni_(5%)CoP presents lower overpotentials and voltage of 84 mV&259 mV and1.48 V at the current density of 10 mA cm^(-2)for HER&DER and overall water splitting,respectively,which are superior to most other reported 2 D bimetal-phosphides.This work provides a new strategy to optimize the performance of electrolytic water for bimetal-phosphates and it may be of significant value in extending the design of other ultrathin 2 D structured catalysts.展开更多
The development of a selective catalyst for the conversion of biomass and plastics into H2by steam reforming can combat the energy crisis and global warming.In this work,support Ni-Fe-Ca/H-Al bifunctional catalysts we...The development of a selective catalyst for the conversion of biomass and plastics into H2by steam reforming can combat the energy crisis and global warming.In this work,support Ni-Fe-Ca/H-Al bifunctional catalysts were prepared by loading Ni and Fe into pretreatment CaO/Al_(2)O_(3)(Ca/H-Al)carriers and showed high catalytic activity for the steam reforming of biomass and plastic.Moreover,the idea of bidirectional degradation was exploited to strengthen the pyrolysis of plastic with a high H/C and biomass with a high O/C.Interestingly,the products presented high H2selective(1302.10 m L/g)and low CO_(2)yield(120.23 m L/g)in 7Ni-5Fe-Ca/H-Al(2:4)catalyst compared with current reports.Here,the abundant oxygen vacancies(Ov)in the H-Al carrier exhibited an electron-deficient nature,providing active sites for anchoring Ni O.Meanwhile,Ni O interacted with Ca_(2)Fe_(2)O_(5)to produce more defective Ovsites,which stabilized the NiO particles in the 7Ni-5Fe-Ca/H-Al(2:4)catalyst,and the interaction between the catalyst and the carrier was enhanced,leading to the reduction of weakly basic sites,this property promoted the strong adsorption of CO_(2)and H2O by the catalyst,contributing to the enhancement of efficient steam conversion and the promotion of conversion of by-products to H2.Notably,7Ni-5Fe-Ca/H-Al(2:4)catalysts maintained structural integrity after regeneration and exhibited excellent regenerability in H2selection and CO_(2)adsorption.The work provides a new idea for the study of efficient H2production from steam reforming of biomass and plastics.展开更多
This is the first report on a polysaccharide(RCJ2-Ib)isolated from Rosa Chinensis Flos.RCJ2-Ib was obtained through the extraction with water,precipitation with ethanol,separation with DEAE-52 column and purification ...This is the first report on a polysaccharide(RCJ2-Ib)isolated from Rosa Chinensis Flos.RCJ2-Ib was obtained through the extraction with water,precipitation with ethanol,separation with DEAE-52 column and purification with DEAE-Sepharose Fast Flow column and Sephadex G100 column.GC,FT-IR and NMR analyses revealed that RCJ2-Ib(3.3 k Da)was a 1,4-linked polymannuronic acid containing substantialβ-Danomers units.The anticoagulant effect of RCJ2-Ib evaluated by using rabbit ear venous blood and an acute blood stasis rat model showed that RCJ2-Ib had obvious anticoagulant activity in regulating endogenous and exogenous coagulation pathways and reducing serum thromboxane B2 and endothelin-1.In addition,RCJ2-Ib could also increase the number of Lactobacillus and Escherichia coli.As a result,RCJ2-Ib has the potential to inhibit thrombosis and maintain the intestinal environment.展开更多
Chemical reduction method was employed to prepare nano-sized Sn2SbNi alloy composites used as anode material for rechargeable lithium ion batteries.This strategy was adopted to combine the virtues of both active/inact...Chemical reduction method was employed to prepare nano-sized Sn2SbNi alloy composites used as anode material for rechargeable lithium ion batteries.This strategy was adopted to combine the virtues of both active/inactive and active/active alloys to fabricate a Sn2SbNi alloy powder with two active components and one inactive component.The two active components can realize the high capacity feature of electrode and can make the volume change of electrode take place in a stepwise manner due to the different lithiation potentials of two active components,leading to a stable cycling performance.Sn2SbNi alloy provides a reversible specific capacity over 640 mA·h/g with an excellent cyclic ability.The Sn-Sb-Ni alloy composite material shows to be a good candidate anode material for the lithium ion batteries.展开更多
Radical scavenging activity (RSA) of chloro and methyl substituted benzylamine derivatives (BADs) has been studied using 1, 1-diphenyl-2-picrylhydrazyl free radical (DPPH?) through spectrophotometric and physico- chem...Radical scavenging activity (RSA) of chloro and methyl substituted benzylamine derivatives (BADs) has been studied using 1, 1-diphenyl-2-picrylhydrazyl free radical (DPPH?) through spectrophotometric and physico- chemical techniques at T = (298.15, 303.15 and 308.15) K. New experimental data on the density, sound velocity, isentropic and apparent molal compressibility of selected BADs + DPPH● solutions as a function of temperature and concentration are reported. The results are discussed with regards to structure-activity relationship (SAR) principles of BADs. The relative deviations in RSAs varied with structural potentials of BADs which were analyzed by making a comparative study for both the spectrophotometric and physicochemical results.展开更多
In Alzheimer’s disease,the transporter P-glycoprotein is responsible for the clearance of amyloid-βin the brain.Amyloid-βcorrelates with the sphingomyelin metabolism,and sphingomyelin participates in the regulation...In Alzheimer’s disease,the transporter P-glycoprotein is responsible for the clearance of amyloid-βin the brain.Amyloid-βcorrelates with the sphingomyelin metabolism,and sphingomyelin participates in the regulation of P-glycoprotein.The amyloid cascade hypothesis describes amyloid-βas the central cause of Alzheimer’s disease neuropathology.Better understanding of the change of P-glycoprotein and sphingomyelin along with amyloid-βand their potential association in the pathological process of Alzheimer’s disease is critical.Herein,we found that the expression of P-glycoprotein in APP/PS1 mice tended to increase with age and was significantly higher at 9 and 12 months of age than that in wild-type mice at comparable age.The functionality of P-glycoprotein of APP/PS1 mice did not change with age but was significantly lower than that of wild-type mice at 12 months of age.Decreased sphingomyelin levels,increased ceramide levels,and the increased expression and activity of neutral sphingomyelinase 1 were observed in APP/PS1 mice at 9 and 12 months of age compared with the levels in wild-type mice.Similar results were observed in the Alzheimer’s disease mouse model induced by intracerebroventricular injection of amyloid-β1-42 and human cerebral microvascular endothelial cells treated with amyloid-β1-42.In human cerebral microvascular endothelial cells,neutral sphingomyelinase 1 inhibitor interfered with the changes of sphingomyelin metabolism and P-glycoprotein expression and functionality caused by amyloid-β1-42 treatment.Neutral sphingomyelinase 1 regulated the expression and functionality of P-glycoprotein and the levels of sphingomyelin and ceramide.Together,these findings indicate that neutral sphingomyelinase 1 regulates the expression and function of P-glycoprotein via the sphingomyelin/ceramide pathway.These studies may serve as new pursuits for the development of anti-Alzheimer’s disease drugs.展开更多
The host structure of polymers significantly influences ion transport and interfacial stability of electrolytes,dictating battery cycle life and safety for solid-state lithium metal batteries.Despite promising propert...The host structure of polymers significantly influences ion transport and interfacial stability of electrolytes,dictating battery cycle life and safety for solid-state lithium metal batteries.Despite promising properties of ethylene oxide-based electrolytes,their typical clamp-like coordination geometry leads to crowd solvation sheath and overly strong interactions between Li^(+)and electrolytes,rendering difficult dissociation of Li+and unfavorable solid electrolyte interface(SEI).Herein,we explore weakly solvating characteristics of polyacetal electrolytes owing to their alternately changing intervals between–O–coordinating sites in the main chain.Such structural asymmetry leads to unique distorted helical solvation sheath,and can effectively reduce Li^(+)-electrolyte binding and tune Li^(+)desolvation kinetics in the insitu formed polymer electrolytes,yielding anion-derived SEI and dendrite-free Li electrodeposition.Combining with photoinitiated cationic ring-opening polymerization,polyacetal electrolytes can be instantly formed within 5 min at the surface of electrode,with high segmental chain motion and well adapted interfaces.Such in-situ polyacetal electrolytes enabled more than 1300-h of stable lithium electrodeposition and prolonged cyclability over 200 cycles in solid-state batteries at ambient temperatures,demonstrating the vital role of molecular structure in changing solvating behavior and Li deposition stability for high-performance electrolytes.展开更多
The base-free aerobic oxidation of 5-hydroxymethylfurfural(HMF) to 2,5-furandicarboxylic acid(FDCA)in water is recognized as an important and sustainable upgrading process for cellulosic carbohydrates.However,selectiv...The base-free aerobic oxidation of 5-hydroxymethylfurfural(HMF) to 2,5-furandicarboxylic acid(FDCA)in water is recognized as an important and sustainable upgrading process for cellulosic carbohydrates.However,selectivity control still remains a challenge.Here,we disclose that the unique synergy in magnetic Ni_(x)Co_(1)O_(y)(x=1,3 and 5) bimetallic oxides can induce reactive oxygen defects and simultaneously stabilize small-sized metallic Au nanoparticles in the Au/Ni_(x)Co_(1)O_(y)catalysts.Such catalytic features render effective adsorption and activation of O_(2),OH and C=O groups,realizing selective oxidation of HMF to FDCA.On a series of magnetic Au/Ni_(x)Co_(1)O_(y)catalysts with almost identical Au loadings(ca.0.5 wt%) and particle sizes(ca.2.7 nm),the variable Ni/Co molar ratios give rise to the tunable electron density of Au sites and synergistic effect between NiO and CoO_(y).The initial conversion rates of HMF and its derived intermediates(i.e., DFF,HMFCA and FFCA) show a volcano-like dependence on the number of oxygen defects(i.e.,O_(2)^(-)and O^(-)) and electron-rich Au0sites.The optimum Au/Ni3Co1Oycatalyst exhibits a highest productivity of FDCA(12.5 mmol_(FDCA)mol_(Au)^(-1)h^(-1)) among all the Au catalysts in the literature and achieves> 99% yield of FDCA at 120℃ and 10 bar of O_(2).In addition,this catalyst can be easily recovered by a magnet and show superior stability and reusability during six consecutive cycling tests.This work may shed a light on Au catalysis for the base-free oxidation of biomass compounds by smartly using the synergy in bimetallic oxide carriers.展开更多
基金the National Natural Science Foundation of China (No. 22136005)the Strategic Priority Research Program of the Chinese Academy of Sciences (No. XDB36000000).
文摘Photoelectrochemical (PEC) small-molecule oxidation can selectively transform substrates into high-value-added fine chemicals and increase the rate of cathode hydrogen evolution. Nevertheless, achieving high-selectivity PEC oxidation of small molecules to produce specific products is a very challenging task. In general, selectivity can be improved by changing the surface catalyticsites of the photoanode and modulating the interfacial environments of the reactions. Herein, recent advances in approaches to improving selective PEC oxidation of small molecules are introduced. We first briefly discuss the basic concept and fundamentals of small-molecule PEC oxidation. The reported approaches to improving the performance of selective PEC oxidation of small molecules are highlighted from two aspects: (1) changing the surface properties of photoanodes by selecting suitable materials or modifying the photoanodes and (2) mediating the oxidation reactions using redox mediators. The PEC oxidation mechanism of these studies is emphasized. We also discuss the challenges in this research direction and offer a perspective on the further development of selective PEC-based small-molecule transformation.
基金This work was financially supported by Major Science and Technology Project of Yunnan Province(202302AE090022)Key Research and Development Program of Yunnan(202203AC100010)+4 种基金the National Natural Science Foundation of China(32160597,32160236,32371463)National Key Research and Development Program of China(2022YFC2601604)Cardiovascular Ultrasound Innovation Team of Yunnan Province(202305AS350021)Spring City Plan:the High-level Talent Promotion and Training Project of Kunming(2022SCP001)the second phase of“Double-First Class”Program Construction of Yunnan University.
文摘Sensitive detection of Staphylococcus aureus enterotoxin B(SEB)is of importance for preventing food poisoning from threatening human health.In this work,an electrochemical and colorimetric dual-signal detection assay of SEB was developed.The probe(Ab2/AuPt@Fe-N-C)was bound to SEB captured by Ab1,where the Ab2/AuPt@Fe-N-C triggered methylene blue degradation and resulted in the decrease of electrochemical signal.Furthermore,the probe catalyzed the oxidation of 3,3’,5,5’-tetramethyl biphenyl to generate a colorimetric absorbance at 652 nm.Once the target was captured and formed a sandwich-like complex,the color changed from colorless to blue.SEB detection by colorimetric and electrochemical methods showed a linear relationship in the concentration ranges of 0.0002-10.0000 and 0.0005-10.0000 ng/mL,with limits of detection of 0.0667 and 0.1670 pg/mL,respectively.The dual-signal biosensor was successfully used to detect SEB in milk and water samples,which has great potential in toxin detection in food and the environment.
基金supported by the National Natural Science Foundation of China(22072107,21872105)the Natural Science Foundation of Shanghai(23ZR1464800)+1 种基金the Fundamental Research Funds for the Central Universitiesthe Science&Technology Commission of Shanghai Municipality(19DZ2271500)。
文摘Smart wearable devices are regarded to be the next prevailing technology product after smartphones and smart homes,and thus there has recently been rapid development in flexible electronic energy storage devices.Among them,flexible solid-state zinc-air batteries have received widespread attention because of their high energy density,good safety,and stability.Efficient bifunctional oxygen electrocatalysts are the primary consideration in the development of flexible solid-state zinc-air batteries,and self-supported air cathodes are strong candidates because of their advantages including simplified fabrication process,reduced interfacial resistance,accelerated electron transfer,and good flexibility.This review outlines the research progress in the design and construction of nanoarray bifunctional oxygen electrocatalysts.Starting from the configuration and basic principles of zinc-air batteries and the strategies for the design of bifunctional oxygen electrocatalysts,a detailed discussion of self-supported air cathodes on carbon and metal substrates and their uses in flexible zinc-air batteries will follow.Finally,the challenges and opportunities in the development of flexible zinc-air batteries will be discussed.
基金financially supported by National Key Research and Development Program of China(2022YFC2601604)Major science and technology project of Yunnan Province(202202AE090085)+9 种基金the National Natural Science Foundation of China(3216059732160236)Science and technology talent and platform plan of YunnanKey Scientific and Technology Project of Yunnan(202203AC100010)Spring City Plan:the High-level Talent Promotion and Training Project of Kunming(2022SCP001)the second phase of“Double-First Class”program construction of Yunnan Universitygrants from State Key Laboratory for Conservation and Utilization of Bio-Resources in Yunnan,Yunnan University(2021KF005)Key Scientific and Technology Project of Yunnan(202002AE320005)Program for Excellent Young Talents of Yunnan Universitythe Program for Donglu Scholars of Yunnan University。
文摘Norovirus(NoV)is regarded as one of the most common causes of foodborne diarrhea in the world.It is urgent to identify the pathogenic microorganism of the diarrhea in short time.In this work,we developed an electrochemical and colorimetric dual-mode detection for NoV based on the excellent dual catalytic properties of copper peroxide/COF-NH_(2)nanocomposite(CuO_(2)@COF-NH_(2)).For the colorimetric detection,NoV can be directly detected by the naked eye based on CuO_(2)@COF-NH_(2)as a laccase-like nonazyme using“peptide-NoV-antibody”recognition mode.The colorimetric assay displayed a wide and quality linear detection range from 1 copy/mL to 5000 copies/mL of NoV with a low limit of detection(LOD)of 0.125 copy/mL.For the electrochemical detection of NoV,CuO_(2)@COF-NH_(2)showed an oxidation peak of copper ion from Cu^(+)to Cu^(2+)using“peptide-NoV-antibody”recognition mode.The electrochemical assay showed a linear detection range was 1-5000 copies/mL with a LOD of 0.152 copy/mL.It's worthy to note that this assay does not need other electrical signal molecule,which provide the stable and sensitive electrochemial detection for NoV.The electrochemical and colorimetric dual-mode detection was used to detect NoV in foods and faceal samples,which has the potential for improving food safety and diagnosing of NoV-infected diarrhea.
基金financially supported by the National Natural Science Foundation of China(31972149)funding support from the MacDiarmid Institute for Advanced Materials and Nanotechnologythe Dodd-Walls Centre for Photonic and Quantum Technologies。
文摘Herein,a novel interference-free surface-enhanced Raman spectroscopy(SERS)strategy based on magnetic nanoparticles(MNPs)and aptamer-driven assemblies was proposed for the ultrasensitive detection of histamine.A core-satellite SERS aptasensor was constructed by combining aptamer-decorated Fe_(3)O_(4)@Au MNPs(as the recognize probe for histamine)and complementary DNA-modified silver nanoparticles carrying 4-mercaptobenzonitrile(4-MBN)(Ag@4-MBN@Ag-c-DNA)as the SERS signal probe for the indirect detection of histamine.Under an applied magnetic field in the absence of histamine,the assembly gave an intense Raman signal at“Raman biological-silent”region due to 4-MBN.In the presence of histamine,the Ag@4-MBN@Ag-c-DNA SERS-tag was released from the Fe_(3)O_(4)@Au MNPs,thus decreasing the SERS signal.Under optimal conditions,an ultra-low limit of detection of 0.65×10^(-3)ng/mL and a linear range 10^(-2)-10^5 ng/mL on the SERS aptasensor were obtained.The histamine content in four food samples were analyzed using the SERS aptasensor,with the results consistent with those determined by high performance liquid chromatography.The present work highlights the merits of indirect strategies for the ultrasensitive and highly selective SERS detection of small biological molecules in complex matrices.
基金National Key R&D Program of China(2022YFC2805100)National Science Fund for Key Program of National Natural Science Foundation of China(31930084)+3 种基金National Science Fund for Distinguished Young Scholars of China(31725022)China Agriculture Research System(CARS-18-ZJ0503)Guangdong Provincial Key R&D Programme(2022B0202010002)Science and Technology Innovation Project of Foshan City(FS0AAKJ919-4402-0013)。
文摘The in vitro digestion models mimicking the gastrointestinal(GI)tract of general population and lipid indigestion patients(with lower levels of bile salts or pancreatic lipase)were selected to investigate whether diacylglycerols(DAGs)are potential good lipid sources for these patients.Linseed oil-based DAG(LD)and linseed oil(LT)were selected.LD-based emulsion((83.74±1.23)%)had higher lipolysis degree than LT-based emulsion((74.47±1.16)%)when monitoring the GI tract of normal population as previously reported.Indigestion conditions seriously decreased the digestive degree of LT-based emulsion((40.23±2.48)%-(66.50±3.70)%)while showed less influence on LD-based emulsion((64.18±2.41)%-(81.85±3.45)%).As opposed to LT-based emulsion,LD-based emulsion exhibited preference for releasing unsaturated fatty acids(especially oleic acid andα-linolenic acid)due to their different glycerolipid compositions.LD-based emulsion showed potential for providing lipids and nutrients(including essential fatty acids)for lipid indigestion patients.
基金supported by the National Natural Science Foundation of China (51702039)。
文摘The sluggish kinetics of the electrochemical oxygen reduction reaction(ORR)in intermediatetemperature solid oxide fuel cells(IT-SOFCs)greatly limits the overall cell performance.In this study,an efficient and durable cathode material for IT-SOFCs is designed based on density functional theory(DFT)calculations by co-doping with Nb and Ta the B-site of the SrFeO_(3-δ)perovskite oxide.The DFT calculations suggest that Nb/Ta co-doping can regulate the energy band of the parent SrFeO_(3-δ)and help electron transfer.In symmetrical cells,such cathode with a SrFe_(0.8)Nb_(0.1)Ta_(0.1)O_(3-δ)(SFNT)detailed formula achieves a low cathode polarization resistance of 0.147Ωcm^(2) at 650℃.Electron spin resonance(ESR)and X-ray photoelectron spectroscopy(XPS)analysis confirm that the co-doping of Nb/Ta in SrFeO_(3-δ)B-site increases the balanced concentration of oxygen vacancies,enhancing the electrochemical performance when compared to 20 mol%Nb single-doped perovskite oxide.The cathode button cell with NiSDC|SDC|SFNT configuration achieves an outstanding peak power density of 1.3 W cm^(-2)at 650℃.Moreover,the button cell shows durability for 110 h under 0.65 V at 600℃ using wet H_(2) as fuel.
基金supported by Basic Science Center Project of National Natural Science Foundation of China under grant No.51788104the National Natural Science Foundation of China (grant nos.51772301 and 21773264)+1 种基金the National Key R&D Program of China (grant no.2016YFA0202500)the “Strategic Priority Research Program” of the Chinese Academy of Sciences (grant no.XDA09010300)
文摘With high theoretical energy density and the natural abundance of S, lithium-sulfur(Li–S) batteries are considered to be the promising next generation high-energy rechargeable energy storage devices. However, issues including electronical insulation of S, the lithium polysulfides(Li PSs) dissolution and the short cycle lifespan have prevented Li–S batteries from being practical applied. Feasible settlements of confining Li PSs to reduce the loss of active substances and improve the cycle stability include wrapping sulfur with compact layers, designing matrix with porous or hollow structures, adding adsorbents owning strong interaction with sulfur and inserting polysulfide barriers between cathodes and separators. This review categorizes them into physical and chemical confinements according to the influencing mechanism. With further discussion of their merits and flaws, synergy of the physical and chemical confinement is believed to be the feasible avenue that can guide Li–S batteries to the practical application.
基金the Malaysian Ministry of Higher Education for providing financial support(No.011000070004)
文摘Rubber leaf powder(an agricultural waste) was treated with potassium permanganate followed by sodium carbonate and its performance in the removal of Pb(Ⅱ) ions from aqueous solution was evaluated.The interactions between Pb(Ⅱ) ions and functional groups on the adsorbent surface were confirmed by Fourier transform infrared(FT-IR) spectroscopy,scanning electron microscopy(SEM) coupled with X-ray energy dispersive spectroscopy(EDX).The effects of several important parameters which can affect adsorption capacity such as pH,adsorbent dosage,initial lead concentration and contact time were studied.The optimum pH range for lead adsorption was 4-5.Even at very low adsorbent dosage of 0.02 g,almost 100% of Pb(Ⅱ) ions(23 mg/L) could be removed.The adsorption capacity was also dependent on lead concentration and contact time,and relatively a short period of time(60-90 min) was required to reach equilibrium.The equilibrium data were analyzed with Langmuir,Freundlich and Dubinin-Radushkevich isotherms.Based on Langmuir model,the maximum adsorption capacity of lead was 95.3 mg/g.Three kinetic models including pseudo first-order,pseudo second-order and Boyd were used to analyze the lead adsorption process,and the results showed that the pseudo second-order fitted well with correlation coefficients greater than 0.99.
基金CSIR, New-Delhi for SRF [Sanction No. 09/908(0002) 2K9-EMR-I]DST [No. S.R/S3/ME/014/2007]Government of India (GOI) for research grant
文摘Zinc oxide(ZnO) nanoparticles of varying sizes(20, 44 and 73 nm) have been successfully synthesized by a hybrid electrochemical-thermal method using aqueous sodium bicarbonate electrolyte and sacrificial Zn anode and cathode in an undivided cell under galvanostatic mode at room temperature. The as-synthesized product was characterized by X-ray diffraction(XRD), X-ray photoelectron spectra(XPS), Scanning electron microscopy along with Energy dispersive analysis of X-ray(SEM/EDAX), Transmission electron microscopy(TEM), Ultra Violet- Diffuse reflectance spectroscopic methods(UV-DRS). and UV-DRS spectral methods.The as-synthesized compound were single-crystalline and Rietveld refinement of calcined samples exhibited hexagonal(Wurtzite) structure with space group of P63mc(No.186). The band gaps for synthesized ZnO nanoparticles were 3.07, 3.12 and 3.13 e V, respectively, based on the results of diffuse reflectance spectra(DRS). The electrochemically synthesized ZnO powder was used as photocatalysts for UV-induced degradation of Methylene blue(MB). Photodegradation was also found to be function of exposure time and dye solution p H. It has been found that as-synthesized powder has excellent photocatalytic activity with 92% degradation of MB, indicating ZnO nanoparticles can play an important role as a semiconductor photocatalyst.
基金supported by the National Natural Science Foundation of China (21603041 and 21972124)A Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutionthe support of Six Talent Peaks Project of Jiangsu Province (XCL-070-2018)。
文摘Performance boosting of hybrid metal oxide and metal alloy catalyst is crucial to the water electrolysis for hydrogen generation. Herein, a novel concept of selective fluoridation of metal alloy/oxide hybrid is proposed to boost their catalytic performance for the oxygen evolution reaction(OER). A well-recognized OER catalyst system of FeNi3 alloy/oxide embedded in nitrogen-doped porous nanofibers(FeNiO/NCF) is employed as a proof of concept, and it is selectively fluoridated by transforming the metal oxide to metal fluoride(FeNiF/NCF). The crystal structure and surface chemical state transformation are well supported by the spectroscopic analysis and the improved electrochemical performance for OER can be well correlated to the phase and structure change. Specifically, FeNiF/NCF can drive the benchmark current density of 10 mA cm-2 at 260 mV with a Tafel slope of 67 mV dec-1, about 70 mV less than that of FeNiO/NCF.Increased catalytic kinetics, rapid charge transfer ability, high catalytic efficiency and stability are also probed by electrochemical analysis. The high surface area and roughness are found mainly generated via the high-temperature annealing for the metal alloy/metal oxide formation, and the low-temperature fluoridation process intrinsically contributes to the active structure formation. It is an efficient and universal approach to increase the catalytic performance of metal alloy/oxide for energy-relevant catalytic reactions.
基金Department of Science and Technology(DST)Government of India,for sanctioning financial assistance for executing this programme under Nanomaterials Science and Technology Initiative Programmethe Council of Scientific and Industrial Research(CSIR),Government of India,for granting her fellowship for executing this programme
文摘An amperometric hydrogen peroxide biosensor using a nanobiocomposite based on neutral red modified carbon nanotubes and co-immobilized glucose oxidase and horseradish peroxidase is reported. Modification of the nanobiocomposite electrode with neutral red resulted in a sensitive, low-cost and reliable H_2O_2 sensor. The use of carbon nanotubes, as the conductive part of the composite, facilitated fast electron transfer rates. The biosensor was characterized for the influence of p H, potential and temperature. A remarkable feature of the biosensor is the detection of H_2O_2 at low applied potentials where the noise level and interferences are minimal. The sensor has a fast steady-state measuring time of 10 s with a quick response(2 s). The biosensor showed a linear range from 15 n M to 45 m M of H_2O_2 and a detection limit of 5 n M. Nafion, which is used as a binder, makes the determination free from other electroactive substances. The repeatability, reproducibility,stability and analytical performance of the sensor are very good.
基金financially supported by the National Natural Science Foundation(22171212)the Science and Technology Committee of Shanghai Municipality(21160710300,19DZ2271500)of Chinathe International Exchange Grant(IEC/NSFC/201078)through Royal Society UK and NSFC。
文摘Bimetallic transition metal phosphides(TMPs)as potential candidates for superior electrochemical performance are still facing great challenges in the controllable preparation of two-dimensional(2 D)structures with high aspect ratio.Herein,a novel structure of quasi-monolayered NiCo-bimetal-phosphide(NiCoP)has been designed and successfully synthesized by the newly developed process combined with ultrasonic-cavitation and phase-transition.This is the first time to break through the controllable preparation of 2 D bimetal-phosphides with a thickness of 0.98 nm in sub-nanoscale.Based on the advantages of 2 D quasi-monolayer structure with dense crystalline-amorphous interface and the reconfigured electronic structure between Ni^(δ+)/Co^(δ+)and P^(δ-),the optimized Ni_(5%)CoP exhibits an outstanding bifunctional performance for electrocatalyzing both hydrogen evolution reaction and oxygen evolution reaction in an alkaline medium.Ni_(5%)CoP presents lower overpotentials and voltage of 84 mV&259 mV and1.48 V at the current density of 10 mA cm^(-2)for HER&DER and overall water splitting,respectively,which are superior to most other reported 2 D bimetal-phosphides.This work provides a new strategy to optimize the performance of electrolytic water for bimetal-phosphates and it may be of significant value in extending the design of other ultrathin 2 D structured catalysts.
基金the National Natural Science of China(21968037)the Reserve Program for Young and Middle-aged Academic and Technical Leaders in Yunnan Province(202205AC160031)+1 种基金the Research Innovation Project of Yunnan University for Graduate Students on Exemption,the Highlevel Talent Promotion and Training Project of Kunming(2022SCP003)advanced analysis and measurement center of Yunnan university for the sample testing service。
文摘The development of a selective catalyst for the conversion of biomass and plastics into H2by steam reforming can combat the energy crisis and global warming.In this work,support Ni-Fe-Ca/H-Al bifunctional catalysts were prepared by loading Ni and Fe into pretreatment CaO/Al_(2)O_(3)(Ca/H-Al)carriers and showed high catalytic activity for the steam reforming of biomass and plastic.Moreover,the idea of bidirectional degradation was exploited to strengthen the pyrolysis of plastic with a high H/C and biomass with a high O/C.Interestingly,the products presented high H2selective(1302.10 m L/g)and low CO_(2)yield(120.23 m L/g)in 7Ni-5Fe-Ca/H-Al(2:4)catalyst compared with current reports.Here,the abundant oxygen vacancies(Ov)in the H-Al carrier exhibited an electron-deficient nature,providing active sites for anchoring Ni O.Meanwhile,Ni O interacted with Ca_(2)Fe_(2)O_(5)to produce more defective Ovsites,which stabilized the NiO particles in the 7Ni-5Fe-Ca/H-Al(2:4)catalyst,and the interaction between the catalyst and the carrier was enhanced,leading to the reduction of weakly basic sites,this property promoted the strong adsorption of CO_(2)and H2O by the catalyst,contributing to the enhancement of efficient steam conversion and the promotion of conversion of by-products to H2.Notably,7Ni-5Fe-Ca/H-Al(2:4)catalysts maintained structural integrity after regeneration and exhibited excellent regenerability in H2selection and CO_(2)adsorption.The work provides a new idea for the study of efficient H2production from steam reforming of biomass and plastics.
基金supported by Research on Precision Nutrition and Health Food,Department of Science and Technology of Henan Province(CXJD2021006)Key Project in Science and Technology Agency of Henan Province(202102110283 and 202102110149)。
文摘This is the first report on a polysaccharide(RCJ2-Ib)isolated from Rosa Chinensis Flos.RCJ2-Ib was obtained through the extraction with water,precipitation with ethanol,separation with DEAE-52 column and purification with DEAE-Sepharose Fast Flow column and Sephadex G100 column.GC,FT-IR and NMR analyses revealed that RCJ2-Ib(3.3 k Da)was a 1,4-linked polymannuronic acid containing substantialβ-Danomers units.The anticoagulant effect of RCJ2-Ib evaluated by using rabbit ear venous blood and an acute blood stasis rat model showed that RCJ2-Ib had obvious anticoagulant activity in regulating endogenous and exogenous coagulation pathways and reducing serum thromboxane B2 and endothelin-1.In addition,RCJ2-Ib could also increase the number of Lactobacillus and Escherichia coli.As a result,RCJ2-Ib has the potential to inhibit thrombosis and maintain the intestinal environment.
基金Project(2008cd148)supported by the Social Development Plan of Yunnan Province,ChinaProject(2010)supported by Key Science and Technology Fund of Education Department,China
文摘Chemical reduction method was employed to prepare nano-sized Sn2SbNi alloy composites used as anode material for rechargeable lithium ion batteries.This strategy was adopted to combine the virtues of both active/inactive and active/active alloys to fabricate a Sn2SbNi alloy powder with two active components and one inactive component.The two active components can realize the high capacity feature of electrode and can make the volume change of electrode take place in a stepwise manner due to the different lithiation potentials of two active components,leading to a stable cycling performance.Sn2SbNi alloy provides a reversible specific capacity over 640 mA·h/g with an excellent cyclic ability.The Sn-Sb-Ni alloy composite material shows to be a good candidate anode material for the lithium ion batteries.
文摘Radical scavenging activity (RSA) of chloro and methyl substituted benzylamine derivatives (BADs) has been studied using 1, 1-diphenyl-2-picrylhydrazyl free radical (DPPH?) through spectrophotometric and physico- chemical techniques at T = (298.15, 303.15 and 308.15) K. New experimental data on the density, sound velocity, isentropic and apparent molal compressibility of selected BADs + DPPH● solutions as a function of temperature and concentration are reported. The results are discussed with regards to structure-activity relationship (SAR) principles of BADs. The relative deviations in RSAs varied with structural potentials of BADs which were analyzed by making a comparative study for both the spectrophotometric and physicochemical results.
基金supported by the National Key Research and Development Program of ChinaNos.2021YFC2 701800 and 2021YFC2 701805 (to QY)+2 种基金Open Research Fund of State Key Laboratory of Genetic EngineeringFudan UniversityNo.SKLGE-21 19 (to TXH and QY)
文摘In Alzheimer’s disease,the transporter P-glycoprotein is responsible for the clearance of amyloid-βin the brain.Amyloid-βcorrelates with the sphingomyelin metabolism,and sphingomyelin participates in the regulation of P-glycoprotein.The amyloid cascade hypothesis describes amyloid-βas the central cause of Alzheimer’s disease neuropathology.Better understanding of the change of P-glycoprotein and sphingomyelin along with amyloid-βand their potential association in the pathological process of Alzheimer’s disease is critical.Herein,we found that the expression of P-glycoprotein in APP/PS1 mice tended to increase with age and was significantly higher at 9 and 12 months of age than that in wild-type mice at comparable age.The functionality of P-glycoprotein of APP/PS1 mice did not change with age but was significantly lower than that of wild-type mice at 12 months of age.Decreased sphingomyelin levels,increased ceramide levels,and the increased expression and activity of neutral sphingomyelinase 1 were observed in APP/PS1 mice at 9 and 12 months of age compared with the levels in wild-type mice.Similar results were observed in the Alzheimer’s disease mouse model induced by intracerebroventricular injection of amyloid-β1-42 and human cerebral microvascular endothelial cells treated with amyloid-β1-42.In human cerebral microvascular endothelial cells,neutral sphingomyelinase 1 inhibitor interfered with the changes of sphingomyelin metabolism and P-glycoprotein expression and functionality caused by amyloid-β1-42 treatment.Neutral sphingomyelinase 1 regulated the expression and functionality of P-glycoprotein and the levels of sphingomyelin and ceramide.Together,these findings indicate that neutral sphingomyelinase 1 regulates the expression and function of P-glycoprotein via the sphingomyelin/ceramide pathway.These studies may serve as new pursuits for the development of anti-Alzheimer’s disease drugs.
基金financially supported by National Natural Science Foundation of China(52003231,22065037)Yunnan Fundamental Research Projects(202201AW070015)。
文摘The host structure of polymers significantly influences ion transport and interfacial stability of electrolytes,dictating battery cycle life and safety for solid-state lithium metal batteries.Despite promising properties of ethylene oxide-based electrolytes,their typical clamp-like coordination geometry leads to crowd solvation sheath and overly strong interactions between Li^(+)and electrolytes,rendering difficult dissociation of Li+and unfavorable solid electrolyte interface(SEI).Herein,we explore weakly solvating characteristics of polyacetal electrolytes owing to their alternately changing intervals between–O–coordinating sites in the main chain.Such structural asymmetry leads to unique distorted helical solvation sheath,and can effectively reduce Li^(+)-electrolyte binding and tune Li^(+)desolvation kinetics in the insitu formed polymer electrolytes,yielding anion-derived SEI and dendrite-free Li electrodeposition.Combining with photoinitiated cationic ring-opening polymerization,polyacetal electrolytes can be instantly formed within 5 min at the surface of electrode,with high segmental chain motion and well adapted interfaces.Such in-situ polyacetal electrolytes enabled more than 1300-h of stable lithium electrodeposition and prolonged cyclability over 200 cycles in solid-state batteries at ambient temperatures,demonstrating the vital role of molecular structure in changing solvating behavior and Li deposition stability for high-performance electrolytes.
基金supported by the National Natural Science Foundation of China(22272149,22062025,21763031)the Yunnan Fundamental Research Projects(202001AW070012,202101AT070171)+3 种基金the Yunnan University’s Research Innovation Fund for Graduate Students(KC-22221892)the Open Research Fund of School of Chemistry and Chemical Engineering of Henan Normal Universitythe Workstation of Academician Chen Jing of Yunnan Province(202105AF150012)the Free Exploration Fund for Academician(202205AA160007)。
文摘The base-free aerobic oxidation of 5-hydroxymethylfurfural(HMF) to 2,5-furandicarboxylic acid(FDCA)in water is recognized as an important and sustainable upgrading process for cellulosic carbohydrates.However,selectivity control still remains a challenge.Here,we disclose that the unique synergy in magnetic Ni_(x)Co_(1)O_(y)(x=1,3 and 5) bimetallic oxides can induce reactive oxygen defects and simultaneously stabilize small-sized metallic Au nanoparticles in the Au/Ni_(x)Co_(1)O_(y)catalysts.Such catalytic features render effective adsorption and activation of O_(2),OH and C=O groups,realizing selective oxidation of HMF to FDCA.On a series of magnetic Au/Ni_(x)Co_(1)O_(y)catalysts with almost identical Au loadings(ca.0.5 wt%) and particle sizes(ca.2.7 nm),the variable Ni/Co molar ratios give rise to the tunable electron density of Au sites and synergistic effect between NiO and CoO_(y).The initial conversion rates of HMF and its derived intermediates(i.e., DFF,HMFCA and FFCA) show a volcano-like dependence on the number of oxygen defects(i.e.,O_(2)^(-)and O^(-)) and electron-rich Au0sites.The optimum Au/Ni3Co1Oycatalyst exhibits a highest productivity of FDCA(12.5 mmol_(FDCA)mol_(Au)^(-1)h^(-1)) among all the Au catalysts in the literature and achieves> 99% yield of FDCA at 120℃ and 10 bar of O_(2).In addition,this catalyst can be easily recovered by a magnet and show superior stability and reusability during six consecutive cycling tests.This work may shed a light on Au catalysis for the base-free oxidation of biomass compounds by smartly using the synergy in bimetallic oxide carriers.