Despite the promising potential of transition metal oxides(TMOs)as capacitive deionization(CDI)electrodes,the actual capacity of TMOs electrodes for sodium storage is significantly lower than the theoretical capacity,...Despite the promising potential of transition metal oxides(TMOs)as capacitive deionization(CDI)electrodes,the actual capacity of TMOs electrodes for sodium storage is significantly lower than the theoretical capacity,posing a major obstacle.Herein,we prepared the kinetically favorable Zn_(x)Ni_(1−x)O electrode in situ growth on carbon felt(Zn_(x)Ni_(1−x)O@CF)through constraining the rate of OH^(−)generation in the hydrothermal method.Zn_(x)Ni_(1−x)O@CF exhibited a high-density hierarchical nanosheet structure with three-dimensional open pores,benefitting the ion transport/electron transfer.And tuning the moderate amount of redox-inert Zn-doping can enhance surface electroactive sites,actual activity of redox-active Ni species,and lower adsorption energy,promoting the adsorption kinetic and thermodynamic of the Zn_(0.2)Ni_(0.8)O@CF.Benefitting from the kinetic-thermodynamic facilitation mechanism,Zn_(0.2)Ni_(0.8)O@CF achieved ultrahigh desalination capacity(128.9 mgNaCl g^(-1)),ultra-low energy consumption(0.164 kW h kgNaCl^(-1)),high salt removal rate(1.21 mgNaCl g^(-1) min^(-1)),and good cyclability.The thermodynamic facilitation and Na^(+)intercalation mechanism of Zn_(0.2)Ni_(0.8)O@CF are identified by the density functional theory calculations and electrochemical quartz crystal microbalance with dissipation monitoring,respectively.This research provides new insights into controlling electrochemically favorable morphology and demonstrates that Zn-doping,which is redox-inert,is essential for enhancing the electrochemical performance of CDI electrodes.展开更多
Coal catalytic hydrogasification(CCHG)is a straightforward approach for producing CH_(4),which shows advantages over the mature coal-to-CH_(4) technologies from the perspectives of CH_(4) yield,thermal efficiency,and ...Coal catalytic hydrogasification(CCHG)is a straightforward approach for producing CH_(4),which shows advantages over the mature coal-to-CH_(4) technologies from the perspectives of CH_(4) yield,thermal efficiency,and CO_(2) emission.The core of CCHG is to make carbon in coal convert into CH_(4) efficiently with a catalyst.In the past decades,intensive research has been devoted to catalytic hydrogasification of model carbon(pitch coke,activated carbon,coal char).However,the chemical process of CCHG is still not well understood because the coal structure is more complicated,and CCHG is a combination of coal catalytic hydropyrolysis and coal char catalytic hydrogasification.This review seeks to shed light on the catalytic process of raw coal during CCHG.The configuration of suitable catalysts,operating conditions,and feedstocks for tailoring CH_(4) formation were identified,and the underlying mechanisms were elucidated.Based on these results,the CCHG process was evaluated,emphasizing pollutant emissions,energy efficiency,and reactor design.Furthermore,the opportunities and strategic approaches for CCHG under the restraint of carbon neutrality were highlighted by considering the penetration of“green”H2,biomass,and CO_(2) into CCHG.Preliminary investigations from our laboratories demonstrated that the integrated CCHG and biomass/CO_(2) hydrogenation process could perform as an emerging pathway for boosting CH_(4) production by consuming fewer fossil fuels,fulfilling the context of green manufacturing.This work not only provides systematic knowledge of CCHG but also helps to guide the efficient hydrogenation of other carbonaceous resources such as biomass,CO_(2),and coal-derived wastes.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
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
Chitin is a widely used important industrial polymer mainly from shrimp shells, but its commercial preparation is under the great challenge of serious pollution due to the requirement of HCl and Na OH.Herein, we demon...Chitin is a widely used important industrial polymer mainly from shrimp shells, but its commercial preparation is under the great challenge of serious pollution due to the requirement of HCl and Na OH.Herein, we demonstrated that high purity chitin can be obtained from waste shrimp shells(WSSs) by cascade separation with transition metal salt aqueous solution and ionic liquid(IL). Firstly, calcium carbonate of WSSs was effectively removed in the metal salt aqueous solution driven by the ion exchange interaction. Subsequently, 1-butyl-3-methylimidazolium chloride([Bmim]Cl) had bifunctional abilities to remove residual protein and introduced metal salts simultaneously by hydrogen bonding and coordination interactions. The key experimental factors affecting the separation process were systematically studied, including the type of metal salts, temperature, and [Bmim]Cl loading. After sequential treatment with a 20%(mass) Ni SO4aqueous solution at 130 ℃ and [Bmim]Cl at 150 ℃, the purity of a-chitin can be up to 96.5%(mass) that meets commercial requirements. The use of metal salts with higher coordination ability makes the preparation of chitin no longer depend on the commonly acid-base reaction, which is conducive to the preservation of chitin structure.展开更多
Trifunctional Cu-mesh/Cu_(2)O@FeO nanoarrays heterostructure is designed and fabricated by integrating CuCu_(2)O@FeO nanoarrays onto Cu-mesh(CM)via an in situ growth and phase transformation process.It is successfully...Trifunctional Cu-mesh/Cu_(2)O@FeO nanoarrays heterostructure is designed and fabricated by integrating CuCu_(2)O@FeO nanoarrays onto Cu-mesh(CM)via an in situ growth and phase transformation process.It is successfully applied to efficiently mitigate the antibiotic pollution,including degradation of antibiotics,inactivation of antibiotic-resistant bacteria(ARB),and damage of antibiotics resistance genes(ARGs).Under visible-light irradiation,CM/CuCu_(2)O@FeO nanoarrays exhibit a superior degradation efficiency on antibiotics(e.g.,up to 99%in 25 min for tetracycline hydrochloride,TC),due to the generated reactive oxygen species(ROS),especially the dominant·O^(2−).It can fully inactivate E.coli(HB101)with initial number of~108 CFU mL^(−1) in 10 min,which is mainly attributed to the synergistic effects of 1D nanostructure,dissolved metal ions,and generated ROS.Meanwhile,it is able to damage ARGs after 180 min of photodegradation,including tetA(vs TC)of 3.3 log 10,aphA(vs kanamycin sulfate,KAN)of 3.4 log 10,and tnpA(vs ampicillin,AMP)of 4.4 log 10,respectively.This work explores a green way for treating antibiotic pollution under visible light.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
The massive use of antibiotics has led to the aggravation of bacterial resistance and also brought environmental pollution problems.This poses a great threat to human health.If the dosage of antibiotics is reduced by ...The massive use of antibiotics has led to the aggravation of bacterial resistance and also brought environmental pollution problems.This poses a great threat to human health.If the dosage of antibiotics is reduced by increasing its bactericidal performance,the emergence of drug resistance is certainly delayed,so that there's not enough time for developing drug resistance during treatment.Therefore,we selected typical representative materials of metal Ag and semiconductor ZnO nano-bactericides to design and synthesize Ag/ZnO hollow core-shell structures(AZ for short).Antibiotics are grafted on the surface of AZ through rational modification to form a composite sterilization system.The research results show that the antibacterial efficiency of the composite system is significantly increased,from the sum(34.7%+22.8%-57.5%)of the antibacterial efficiency of AZ and gentamicin to 80.2%,net synergizes 22.7%,which fully reflects the effect of 1+1>2.Therefore,the dosage of antibiotics can be drastically reduced in this way,which makes both the possibility of bacterial resistance and medical expenses remarkably decrease.Subsequently,residual antibiotics can be degraded under simple illumination using AZ-self as a photocatalyst,which cuts off the path of environmental pollution.In short,such an innovative route has guiding significance for drug resistance.展开更多
Resin and asphaltene were separated from Liaohe heavy oil. Catalytic aquathermolysis of asphaltene and resin was investigated by using water soluble catalysts (NiSO4 and FeSO4) and oil soluble catalysts (nickel nap...Resin and asphaltene were separated from Liaohe heavy oil. Catalytic aquathermolysis of asphaltene and resin was investigated by using water soluble catalysts (NiSO4 and FeSO4) and oil soluble catalysts (nickel naphthenate and iron naphthenate). Before and after aquathermolysis, the properties of the resin and asphaltene was compared by means of ultimate analysis, vapor pressure osmometer (VPO) average molecular weight, X-ray diffraction (XRD),^13C and ^1H nuclear magnetic resonance (NMR). The conversion sequence was as follows: No-catalyst〈NiSO4〈FeSO4〈nickel naphthenate〈iron naphthenate. In the presence of catalysts, the amount of H2 and CO increased significantly, while H2S in the gas product decreased. The molecular weight of asphaltene and resin increased after reaction without catalyst. But the catalysts restrained this trend. The H/C ratio of asphaltene and resin decreased after reaction. From the results of average structural parameters and molecular weight, it was found that asphaltene and resin were partly aggregated after aquathermolysis.展开更多
Metal-air batteries,like Zn-air batteries(ZABs)are usually suffered from low energy conversion efficiency and poor cyclability caused by the sluggish OER and ORR at the air cathode.Herein,a novel bimetallic Co/CoFe na...Metal-air batteries,like Zn-air batteries(ZABs)are usually suffered from low energy conversion efficiency and poor cyclability caused by the sluggish OER and ORR at the air cathode.Herein,a novel bimetallic Co/CoFe nanomaterial supported on nanoflower-like N-doped graphitic carbon(NC)was prepared through a strategy of coordination construction-cation exchange-pyrolysis and used as a highly efficient bifunctional oxygen electrocatalyst.Experimental characterizations and density functional theory calculations reveal the formation of Co/CoFe heterostructure and synergistic effect between metal layer and NC support,leading to improved electric conductivity,accelerated reaction kinetics,and optimized adsorption energy for intermediates of ORR and OER.The Co/CoFe@NC exhibits high bifunctional activities with a remarkably small potential gap of 0.70 V between the half-wave potential(E_(1/2))of ORR and the potential at 10 mA cm^(-2)(E_(j=10))of OER.The aqueous ZAB constructed using this air electrode exhibits a slight voltage loss of only 60 mV after 550-cycle test(360 h,15 days).A sodium polyacrylate(PANa)-based hydrogel electrolyte was synthesized with strong water-retention capability and high ionic conductivity.The quasi-solid-state ZAB by integrating the Co/CoFe@NC air electrode and PANa hydrogel electrolyte demonstrates excellent mechanical stability and cyclability under different bending states.展开更多
The effects of L-cysteine concentration on biohydrogen production by Enterobacterium Bacterium M580 were investigated in batch cultivation.The experimental results showed that L-cysteine could enhance the cell growth,...The effects of L-cysteine concentration on biohydrogen production by Enterobacterium Bacterium M580 were investigated in batch cultivation.The experimental results showed that L-cysteine could enhance the cell growth,hydrogen production rate and hydrogen yield when its concentration was less than 500 mg·L-1,while it had negative effects when its concentration was higher than 500 mg·L-1.The hydrogen production was the highest 1.29 mol·mol-1(H2/glucose) when 300 mg·L-1L-cysteine was added into the culture,and the yield was 9.4% higher than that in the control.The oxidation-reduction potential(ORP) ,which was influenced by L-cysteine,also affected hydrogen production.The ORP values were in the range-300 mV to-150 mV when the L-cysteine concentration was higher than 500 mg·L-1.Although the ORP in this range was favorable for hydrogen production,it was not suitable for the biomass growth.Hence,less hydrogen was produced.When the L-cysteine concentration was lower than 500 mg·L-1,the ORP was more suitable for both biomass growth and hydrogen production.In addition,at least 91%glucose was consumed when L-cysteine was added to the culture media,compared to the 97.37% consumption without L-cysteine added.展开更多
This paper suggests development of a flexible,lightweight,and ultra-sensitive piezoresistive flow sensor based on vertical graphene nanosheets(VGNs) with a mazelike structure.The sensor was thoroughly characterized fo...This paper suggests development of a flexible,lightweight,and ultra-sensitive piezoresistive flow sensor based on vertical graphene nanosheets(VGNs) with a mazelike structure.The sensor was thoroughly characterized for steady-state and oscillatory water flow monitoring applications.The results demonstrated a high sensitivity(103.91 mV(mm/s)-1) and a very low-velocity detection threshold(1.127 mm s-1) in steady-state flow monitoring.As one of many potential applications,we demonstrated that the proposed VGNs/PDMS flow sensor can closely mimic the vestibular hair cell sensors housed inside the semicircular canals(SCCs).As a proof of concept,magnetic resonance imaging of the human inner ear was conducted to measure the dimensions of the SCCs and to develop a 3D printed lateral semicircular canal(LSCC).The sensor was embedded into the artificial LSCC and tested for various physiological movements.The obtained results indicate that the flow sensor is able to distinguish minute changes in the rotational axis physical geometry,frequency,and amplitude.The success of this study paves the way for extending this technology not only to vestibular organ prosthesis but also to other applications such as blood/urine flow monitoring,intravenous therapy(Ⅳ),water leakage monitoring,and unmanned underwater robots through incorporation of the appropriate packaging of devices.展开更多
A ternary solid complex Yb(Et2dtc)3(phen) was obtained from the reaction of hydrous ytterbium chloride with sodium diethyldithiocarbamate (NaEt2dtc), and 1, 10-phenanthroline (o-phen·H2O) in absolute etha...A ternary solid complex Yb(Et2dtc)3(phen) was obtained from the reaction of hydrous ytterbium chloride with sodium diethyldithiocarbamate (NaEt2dtc), and 1, 10-phenanthroline (o-phen·H2O) in absolute ethanol. The bonding characteristics of the complex were characterized by IR. The result shows Yb3^+ bands with two sulfur atoms in the Na(Et2dtc)3 and two nitrogen atoms in the o-phen. The enthalpy change of liquid-phase reaction of formation of the complex △rHm^θ(Ⅰ), was determined as being (-24.838±0.114) kJ·mol^-1 at 298.15 K, by an RD-496 Ⅲ type heat conduction microcalormeter. The enthalpy change of the solid-phase reaction of formation of the complex △rHm^θ(s), was calculated as being (108.015±0.479) kJ·mol^-1 on the basis of an appropriate thermochemistry cycle. The thermodynamics of liquid-phase reaction of formation of the complex was investigated by changing the temperature during the liquid-phase reaction. Fundamental parameters, the activation enthalpy, △H≠^θ, the activation entropy, △S≠^θ, the activation free energy,△G≠^θ, the apparent reaction rate constant k, the apparent activation energy E, the pre-exponential constant A, and the reaction order n, were obtained by a combination of the reaction thermodynamic and kinetic equations with the data from the thermokinetic expenments. At the same time, the molar heat capacity of the complex cm. p, Was determined to be (86.34± 1.74) J·mol^-1·K^-1 by the same microcalormeter. The constant-volume combus- tion energy of the complex, △cU, was determined to be ( - 17954.08 ± 8.11) kJ·mol^-1 by an RBC-Ⅱ type rotating-bomb calo- rimeter at 298.15 K. Its standard enthalpy of combustion, △cHm^θ, and standard enthalpy of formation, △fHm^θ, were calculated to be (- 17973.29±8.11) kJ·mol^-1 and (-770.36±9.02) kJ·mol^-1, respectively.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
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
High quality 0.02 mol%,0.05 mol%,and 0.08 mol%Fe:β-Ga2O3 single crystals were grown by the floating zone method.The crystal structure,optical,electrical,and thermal properties were measured and discussed.Fe:β-Ga2O3 ...High quality 0.02 mol%,0.05 mol%,and 0.08 mol%Fe:β-Ga2O3 single crystals were grown by the floating zone method.The crystal structure,optical,electrical,and thermal properties were measured and discussed.Fe:β-Ga2O3 single crystals showed transmittance of higher than 80%in the near infrared region.With the increase of the Fe doping concentration,the optical bandgaps reduced and room temperature resistivity increased.The resistivity of 0.08 mol%Fe:β-Ga2O3 crystal reached to 3.63×1011Ω·cm.The high resistivity Fe:β-Ga2O3 single crystals could be applied as the substrate for the high-power field effect transistors(FETs).展开更多
Studies on the degradation process of waste polyethylene terephthalate(PET)have become increasingly mature,but there are relatively few studies on the separation of degradation products.The products contain many compo...Studies on the degradation process of waste polyethylene terephthalate(PET)have become increasingly mature,but there are relatively few studies on the separation of degradation products.The products contain many components and the separation of which is difficult.Therefore,the study on phase equilibrium thermodynamics of bis-2-hydroxyethyl terephthalate(BHET)is of great theoretical significance and practical value to provide basic data for the BHET crystallization separation.In this work,the degraded products were purified and characterized.The solubility of BHET in methanol,ethanol,ethylene glycol,water and the mixture of ethylene glycol+water were determined by static method.The experimental results were correlated with different models,such as ideal solution(IS)model,λh equation,Apelblat equation and NRTL model.Based on the van’t Hoff equation,the mixing Gibbs energy,enthalpy and entropy were calculated.From this work,the basic data which can be used to guide the crystallization process of BHET were obtained,including solubility data,correlation model and thermodynamic properties.展开更多
The development of efficient molecular catalysts for visible-light driven CO2 reduction, based on abundant materials, is necessary to meet energy demands and address environment problems. In this work,a Co(bpy)2Cl2 ...The development of efficient molecular catalysts for visible-light driven CO2 reduction, based on abundant materials, is necessary to meet energy demands and address environment problems. In this work,a Co(bpy)2Cl2 catalyst was developed and showed high efficiency and durability for the photocatalytic reduction of CO2 and protons. Yields of CO and H2 as high as 62.3 and 69.9 μmol were achieved and the turnover numbers(TONs) reached 6230 and 6990, respectively, under light irradiation(λ 〉 420 nm)for 4 h, indicating that the mixture gases could be a candidate as syngas. The apparent quantum yield was determined to be 2.1% for CO. Mechanistic studies revealed oxidative quenching of the photosensitizer Ru(bpy)3Cl2 by the catalyst. The photocatalytic performance, flexible synthesis and non-noble metal catalyst in our system show great promise for the practical application of Co(bpy)2Cl2 to photocatalytic reduction of CO2.展开更多
Among the folate compounds, 5-methyltetrahydrofolic acid (5-CH3THF) is regarded as one of the most bioactive forms of folate. It is regarded as the better source of folate to humans as compared to folic acid, a synthe...Among the folate compounds, 5-methyltetrahydrofolic acid (5-CH3THF) is regarded as one of the most bioactive forms of folate. It is regarded as the better source of folate to humans as compared to folic acid, a synthetic form of folate, which is used for fortifying foods to prevent the incidence of neural tube defects in the new born babies. The use of 5-CH3THF as an alternative fortificant, in place of folic acid, has been explored by various researchers. However, fortification of 5-CH3THF is problematic due to its lower stability. This study investigated the stability of microencapsulated 5-CH3THF in biscuits baked at various temperatures and times as well as changes in their physical properties. Microcapsule with pectin and alginate ratio of 80:20, prepared by spray drying, gave the highest retention (68.6%) of the 5-CH3THF, therefore, chosen for fortification. The encapsulated and unencapsulated 5-CH3THF were mixed separately with flour and biscuit ingredients and baked at 180℃, 200 and 220℃, each for 5, 9 and 12 min. The inclusion of encapsulated and unencapsulated 5-CH3THF in the biscuit formulation and subsequent baking at various temperatures and times resulted in retention of 5-CH3THF from 19.1% to 1.7%. Microencapsulation of 5-CH3THF slightly improved the retention of 5-CH3THF over unencapsuated biscuits at 180℃ for 5 min, but almost no such effect was achieved under baking temperatures of 200℃ and 220℃. Physical analysis showed darker colour, harder texture and lower moisture content for biscuits baked at higher test temperatures. It seems intense heating condition that caused “over baking” of the biscuit likely to be responsible for the loss of the vitamin as well as less desirable physical properties of the biscuits.展开更多
基金supported by The National Natural Science Foundation of China(22276137,52170087)the Fundamental Research Funds for the Central Universities(XJEDU2023Z009).
文摘Despite the promising potential of transition metal oxides(TMOs)as capacitive deionization(CDI)electrodes,the actual capacity of TMOs electrodes for sodium storage is significantly lower than the theoretical capacity,posing a major obstacle.Herein,we prepared the kinetically favorable Zn_(x)Ni_(1−x)O electrode in situ growth on carbon felt(Zn_(x)Ni_(1−x)O@CF)through constraining the rate of OH^(−)generation in the hydrothermal method.Zn_(x)Ni_(1−x)O@CF exhibited a high-density hierarchical nanosheet structure with three-dimensional open pores,benefitting the ion transport/electron transfer.And tuning the moderate amount of redox-inert Zn-doping can enhance surface electroactive sites,actual activity of redox-active Ni species,and lower adsorption energy,promoting the adsorption kinetic and thermodynamic of the Zn_(0.2)Ni_(0.8)O@CF.Benefitting from the kinetic-thermodynamic facilitation mechanism,Zn_(0.2)Ni_(0.8)O@CF achieved ultrahigh desalination capacity(128.9 mgNaCl g^(-1)),ultra-low energy consumption(0.164 kW h kgNaCl^(-1)),high salt removal rate(1.21 mgNaCl g^(-1) min^(-1)),and good cyclability.The thermodynamic facilitation and Na^(+)intercalation mechanism of Zn_(0.2)Ni_(0.8)O@CF are identified by the density functional theory calculations and electrochemical quartz crystal microbalance with dissipation monitoring,respectively.This research provides new insights into controlling electrochemically favorable morphology and demonstrates that Zn-doping,which is redox-inert,is essential for enhancing the electrochemical performance of CDI electrodes.
基金National Natural Science Foundation of China(22308170)A Project Supported by Scientific Research Fund of Zhejiang Provincial Education Department(Y202250270)+2 种基金Key research and development project of Shanxi Province(202102090301029)Scientific Research Incubation Program of Ningbo University of Technology(2022TS12)Scientific Research Project Funded by Ningbo University of Technology(2022KQ04).
文摘Coal catalytic hydrogasification(CCHG)is a straightforward approach for producing CH_(4),which shows advantages over the mature coal-to-CH_(4) technologies from the perspectives of CH_(4) yield,thermal efficiency,and CO_(2) emission.The core of CCHG is to make carbon in coal convert into CH_(4) efficiently with a catalyst.In the past decades,intensive research has been devoted to catalytic hydrogasification of model carbon(pitch coke,activated carbon,coal char).However,the chemical process of CCHG is still not well understood because the coal structure is more complicated,and CCHG is a combination of coal catalytic hydropyrolysis and coal char catalytic hydrogasification.This review seeks to shed light on the catalytic process of raw coal during CCHG.The configuration of suitable catalysts,operating conditions,and feedstocks for tailoring CH_(4) formation were identified,and the underlying mechanisms were elucidated.Based on these results,the CCHG process was evaluated,emphasizing pollutant emissions,energy efficiency,and reactor design.Furthermore,the opportunities and strategic approaches for CCHG under the restraint of carbon neutrality were highlighted by considering the penetration of“green”H2,biomass,and CO_(2) into CCHG.Preliminary investigations from our laboratories demonstrated that the integrated CCHG and biomass/CO_(2) hydrogenation process could perform as an emerging pathway for boosting CH_(4) production by consuming fewer fossil fuels,fulfilling the context of green manufacturing.This work not only provides systematic knowledge of CCHG but also helps to guide the efficient hydrogenation of other carbonaceous resources such as biomass,CO_(2),and coal-derived wastes.
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 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support of the Startup Foundation of China(3160011181808)the National Natural Scientific Foundation of China(21878292,81673400)K.C.Wong Education Foundation(GJTD-2018-04).
文摘Chitin is a widely used important industrial polymer mainly from shrimp shells, but its commercial preparation is under the great challenge of serious pollution due to the requirement of HCl and Na OH.Herein, we demonstrated that high purity chitin can be obtained from waste shrimp shells(WSSs) by cascade separation with transition metal salt aqueous solution and ionic liquid(IL). Firstly, calcium carbonate of WSSs was effectively removed in the metal salt aqueous solution driven by the ion exchange interaction. Subsequently, 1-butyl-3-methylimidazolium chloride([Bmim]Cl) had bifunctional abilities to remove residual protein and introduced metal salts simultaneously by hydrogen bonding and coordination interactions. The key experimental factors affecting the separation process were systematically studied, including the type of metal salts, temperature, and [Bmim]Cl loading. After sequential treatment with a 20%(mass) Ni SO4aqueous solution at 130 ℃ and [Bmim]Cl at 150 ℃, the purity of a-chitin can be up to 96.5%(mass) that meets commercial requirements. The use of metal salts with higher coordination ability makes the preparation of chitin no longer depend on the commonly acid-base reaction, which is conducive to the preservation of chitin structure.
基金This work was financially sup-ported by the National Natural Science Foundation of China(NSFC Nos:22171212,21771140,51771138,51979194)International Corporation Project of Shanghai Committee of Science and Technology by China(No.21160710300)International Exchange Grant(IEC/NSFC/201078)through Royal Society UK and NSFC.
文摘Trifunctional Cu-mesh/Cu_(2)O@FeO nanoarrays heterostructure is designed and fabricated by integrating CuCu_(2)O@FeO nanoarrays onto Cu-mesh(CM)via an in situ growth and phase transformation process.It is successfully applied to efficiently mitigate the antibiotic pollution,including degradation of antibiotics,inactivation of antibiotic-resistant bacteria(ARB),and damage of antibiotics resistance genes(ARGs).Under visible-light irradiation,CM/CuCu_(2)O@FeO nanoarrays exhibit a superior degradation efficiency on antibiotics(e.g.,up to 99%in 25 min for tetracycline hydrochloride,TC),due to the generated reactive oxygen species(ROS),especially the dominant·O^(2−).It can fully inactivate E.coli(HB101)with initial number of~108 CFU mL^(−1) in 10 min,which is mainly attributed to the synergistic effects of 1D nanostructure,dissolved metal ions,and generated ROS.Meanwhile,it is able to damage ARGs after 180 min of photodegradation,including tetA(vs TC)of 3.3 log 10,aphA(vs kanamycin sulfate,KAN)of 3.4 log 10,and tnpA(vs ampicillin,AMP)of 4.4 log 10,respectively.This work explores a green way for treating antibiotic pollution under visible light.
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supported by the National Natural Science Foundation of China(Nos.22176145,82172612)the State Key Laboratory of Fine Chemicals,Dalian University of Technology(KF 2001)the Fundamental Research Funds for the Central Universities(22120210137).
文摘The massive use of antibiotics has led to the aggravation of bacterial resistance and also brought environmental pollution problems.This poses a great threat to human health.If the dosage of antibiotics is reduced by increasing its bactericidal performance,the emergence of drug resistance is certainly delayed,so that there's not enough time for developing drug resistance during treatment.Therefore,we selected typical representative materials of metal Ag and semiconductor ZnO nano-bactericides to design and synthesize Ag/ZnO hollow core-shell structures(AZ for short).Antibiotics are grafted on the surface of AZ through rational modification to form a composite sterilization system.The research results show that the antibacterial efficiency of the composite system is significantly increased,from the sum(34.7%+22.8%-57.5%)of the antibacterial efficiency of AZ and gentamicin to 80.2%,net synergizes 22.7%,which fully reflects the effect of 1+1>2.Therefore,the dosage of antibiotics can be drastically reduced in this way,which makes both the possibility of bacterial resistance and medical expenses remarkably decrease.Subsequently,residual antibiotics can be degraded under simple illumination using AZ-self as a photocatalyst,which cuts off the path of environmental pollution.In short,such an innovative route has guiding significance for drug resistance.
基金supported by the Chinese Natural Science Foundation (No. 40472061)Funding Project for Academic Human Resources Development in Institutions of Higher Learning of Beijing Municipality (No. PXM2007-014222-044654)Funding Project of Organization Department of Beijing Municipal Party Committee (No. 20071D0500500163)
文摘Resin and asphaltene were separated from Liaohe heavy oil. Catalytic aquathermolysis of asphaltene and resin was investigated by using water soluble catalysts (NiSO4 and FeSO4) and oil soluble catalysts (nickel naphthenate and iron naphthenate). Before and after aquathermolysis, the properties of the resin and asphaltene was compared by means of ultimate analysis, vapor pressure osmometer (VPO) average molecular weight, X-ray diffraction (XRD),^13C and ^1H nuclear magnetic resonance (NMR). The conversion sequence was as follows: No-catalyst〈NiSO4〈FeSO4〈nickel naphthenate〈iron naphthenate. In the presence of catalysts, the amount of H2 and CO increased significantly, while H2S in the gas product decreased. The molecular weight of asphaltene and resin increased after reaction without catalyst. But the catalysts restrained this trend. The H/C ratio of asphaltene and resin decreased after reaction. From the results of average structural parameters and molecular weight, it was found that asphaltene and resin were partly aggregated after aquathermolysis.
基金This work was supported by the National Natural Science Foundation of China(21872105,22072107)the Science&Technology Commission of Shanghai Municipality(19DZ2271500).
文摘Metal-air batteries,like Zn-air batteries(ZABs)are usually suffered from low energy conversion efficiency and poor cyclability caused by the sluggish OER and ORR at the air cathode.Herein,a novel bimetallic Co/CoFe nanomaterial supported on nanoflower-like N-doped graphitic carbon(NC)was prepared through a strategy of coordination construction-cation exchange-pyrolysis and used as a highly efficient bifunctional oxygen electrocatalyst.Experimental characterizations and density functional theory calculations reveal the formation of Co/CoFe heterostructure and synergistic effect between metal layer and NC support,leading to improved electric conductivity,accelerated reaction kinetics,and optimized adsorption energy for intermediates of ORR and OER.The Co/CoFe@NC exhibits high bifunctional activities with a remarkably small potential gap of 0.70 V between the half-wave potential(E_(1/2))of ORR and the potential at 10 mA cm^(-2)(E_(j=10))of OER.The aqueous ZAB constructed using this air electrode exhibits a slight voltage loss of only 60 mV after 550-cycle test(360 h,15 days).A sodium polyacrylate(PANa)-based hydrogel electrolyte was synthesized with strong water-retention capability and high ionic conductivity.The quasi-solid-state ZAB by integrating the Co/CoFe@NC air electrode and PANa hydrogel electrolyte demonstrates excellent mechanical stability and cyclability under different bending states.
基金Supported by the National High Technology Research and Development Program of China(2006AA02Z246 2007AA03Z456) the National Natural Science Foundation of China(20776119)+2 种基金 the Specialized Research Fund for the Doctoral Program of Higher Education of China(20096101120023) Shaanxi Provincial Natural Science Foundation(SJ08B03) Shaanxi Key Subject Program China
文摘The effects of L-cysteine concentration on biohydrogen production by Enterobacterium Bacterium M580 were investigated in batch cultivation.The experimental results showed that L-cysteine could enhance the cell growth,hydrogen production rate and hydrogen yield when its concentration was less than 500 mg·L-1,while it had negative effects when its concentration was higher than 500 mg·L-1.The hydrogen production was the highest 1.29 mol·mol-1(H2/glucose) when 300 mg·L-1L-cysteine was added into the culture,and the yield was 9.4% higher than that in the control.The oxidation-reduction potential(ORP) ,which was influenced by L-cysteine,also affected hydrogen production.The ORP values were in the range-300 mV to-150 mV when the L-cysteine concentration was higher than 500 mg·L-1.Although the ORP in this range was favorable for hydrogen production,it was not suitable for the biomass growth.Hence,less hydrogen was produced.When the L-cysteine concentration was lower than 500 mg·L-1,the ORP was more suitable for both biomass growth and hydrogen production.In addition,at least 91%glucose was consumed when L-cysteine was added to the culture media,compared to the 97.37% consumption without L-cysteine added.
基金financial support from Australian Research Council(ARC)via Discovery Early Career Researcher Awards(DE180100688 and DE170100284).
文摘This paper suggests development of a flexible,lightweight,and ultra-sensitive piezoresistive flow sensor based on vertical graphene nanosheets(VGNs) with a mazelike structure.The sensor was thoroughly characterized for steady-state and oscillatory water flow monitoring applications.The results demonstrated a high sensitivity(103.91 mV(mm/s)-1) and a very low-velocity detection threshold(1.127 mm s-1) in steady-state flow monitoring.As one of many potential applications,we demonstrated that the proposed VGNs/PDMS flow sensor can closely mimic the vestibular hair cell sensors housed inside the semicircular canals(SCCs).As a proof of concept,magnetic resonance imaging of the human inner ear was conducted to measure the dimensions of the SCCs and to develop a 3D printed lateral semicircular canal(LSCC).The sensor was embedded into the artificial LSCC and tested for various physiological movements.The obtained results indicate that the flow sensor is able to distinguish minute changes in the rotational axis physical geometry,frequency,and amplitude.The success of this study paves the way for extending this technology not only to vestibular organ prosthesis but also to other applications such as blood/urine flow monitoring,intravenous therapy(Ⅳ),water leakage monitoring,and unmanned underwater robots through incorporation of the appropriate packaging of devices.
文摘A ternary solid complex Yb(Et2dtc)3(phen) was obtained from the reaction of hydrous ytterbium chloride with sodium diethyldithiocarbamate (NaEt2dtc), and 1, 10-phenanthroline (o-phen·H2O) in absolute ethanol. The bonding characteristics of the complex were characterized by IR. The result shows Yb3^+ bands with two sulfur atoms in the Na(Et2dtc)3 and two nitrogen atoms in the o-phen. The enthalpy change of liquid-phase reaction of formation of the complex △rHm^θ(Ⅰ), was determined as being (-24.838±0.114) kJ·mol^-1 at 298.15 K, by an RD-496 Ⅲ type heat conduction microcalormeter. The enthalpy change of the solid-phase reaction of formation of the complex △rHm^θ(s), was calculated as being (108.015±0.479) kJ·mol^-1 on the basis of an appropriate thermochemistry cycle. The thermodynamics of liquid-phase reaction of formation of the complex was investigated by changing the temperature during the liquid-phase reaction. Fundamental parameters, the activation enthalpy, △H≠^θ, the activation entropy, △S≠^θ, the activation free energy,△G≠^θ, the apparent reaction rate constant k, the apparent activation energy E, the pre-exponential constant A, and the reaction order n, were obtained by a combination of the reaction thermodynamic and kinetic equations with the data from the thermokinetic expenments. At the same time, the molar heat capacity of the complex cm. p, Was determined to be (86.34± 1.74) J·mol^-1·K^-1 by the same microcalormeter. The constant-volume combus- tion energy of the complex, △cU, was determined to be ( - 17954.08 ± 8.11) kJ·mol^-1 by an RBC-Ⅱ type rotating-bomb calo- rimeter at 298.15 K. Its standard enthalpy of combustion, △cHm^θ, and standard enthalpy of formation, △fHm^θ, were calculated to be (- 17973.29±8.11) kJ·mol^-1 and (-770.36±9.02) kJ·mol^-1, respectively.
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the Scientific and Innovative Action Plan of Shanghai,China(Grant No.18511110502)Equipment Pre-research Fund Key Project,China(Grant No.6140922010601).
文摘High quality 0.02 mol%,0.05 mol%,and 0.08 mol%Fe:β-Ga2O3 single crystals were grown by the floating zone method.The crystal structure,optical,electrical,and thermal properties were measured and discussed.Fe:β-Ga2O3 single crystals showed transmittance of higher than 80%in the near infrared region.With the increase of the Fe doping concentration,the optical bandgaps reduced and room temperature resistivity increased.The resistivity of 0.08 mol%Fe:β-Ga2O3 crystal reached to 3.63×1011Ω·cm.The high resistivity Fe:β-Ga2O3 single crystals could be applied as the substrate for the high-power field effect transistors(FETs).
基金financially supported by the National Key Research and Development Program of China(2019YFC1908204)the National Natural Scientific Fund of China(No.21878292,21776289,21908232,21978291)+1 种基金Innovation Academy forGreen Manufacture,Chinese Academy of Sciences(No.IAGM2020C12,IAGM2020C21 and IAGM-2019-A06)K.C.Wong Education Foundation(No.GJTD-2018-04)。
文摘Studies on the degradation process of waste polyethylene terephthalate(PET)have become increasingly mature,but there are relatively few studies on the separation of degradation products.The products contain many components and the separation of which is difficult.Therefore,the study on phase equilibrium thermodynamics of bis-2-hydroxyethyl terephthalate(BHET)is of great theoretical significance and practical value to provide basic data for the BHET crystallization separation.In this work,the degraded products were purified and characterized.The solubility of BHET in methanol,ethanol,ethylene glycol,water and the mixture of ethylene glycol+water were determined by static method.The experimental results were correlated with different models,such as ideal solution(IS)model,λh equation,Apelblat equation and NRTL model.Based on the van’t Hoff equation,the mixing Gibbs energy,enthalpy and entropy were calculated.From this work,the basic data which can be used to guide the crystallization process of BHET were obtained,including solubility data,correlation model and thermodynamic properties.
基金supported by the National Basic Research Program of China (973 program, 2014CB239402)the National Natural Science Foundation of China (21573033)+1 种基金the Basic Research Project of Key Laboratory of Liaoning (LZ2015015)the Swedish Energy Agency and the K & A Wallenberg Foundation
文摘The development of efficient molecular catalysts for visible-light driven CO2 reduction, based on abundant materials, is necessary to meet energy demands and address environment problems. In this work,a Co(bpy)2Cl2 catalyst was developed and showed high efficiency and durability for the photocatalytic reduction of CO2 and protons. Yields of CO and H2 as high as 62.3 and 69.9 μmol were achieved and the turnover numbers(TONs) reached 6230 and 6990, respectively, under light irradiation(λ 〉 420 nm)for 4 h, indicating that the mixture gases could be a candidate as syngas. The apparent quantum yield was determined to be 2.1% for CO. Mechanistic studies revealed oxidative quenching of the photosensitizer Ru(bpy)3Cl2 by the catalyst. The photocatalytic performance, flexible synthesis and non-noble metal catalyst in our system show great promise for the practical application of Co(bpy)2Cl2 to photocatalytic reduction of CO2.
文摘Among the folate compounds, 5-methyltetrahydrofolic acid (5-CH3THF) is regarded as one of the most bioactive forms of folate. It is regarded as the better source of folate to humans as compared to folic acid, a synthetic form of folate, which is used for fortifying foods to prevent the incidence of neural tube defects in the new born babies. The use of 5-CH3THF as an alternative fortificant, in place of folic acid, has been explored by various researchers. However, fortification of 5-CH3THF is problematic due to its lower stability. This study investigated the stability of microencapsulated 5-CH3THF in biscuits baked at various temperatures and times as well as changes in their physical properties. Microcapsule with pectin and alginate ratio of 80:20, prepared by spray drying, gave the highest retention (68.6%) of the 5-CH3THF, therefore, chosen for fortification. The encapsulated and unencapsulated 5-CH3THF were mixed separately with flour and biscuit ingredients and baked at 180℃, 200 and 220℃, each for 5, 9 and 12 min. The inclusion of encapsulated and unencapsulated 5-CH3THF in the biscuit formulation and subsequent baking at various temperatures and times resulted in retention of 5-CH3THF from 19.1% to 1.7%. Microencapsulation of 5-CH3THF slightly improved the retention of 5-CH3THF over unencapsuated biscuits at 180℃ for 5 min, but almost no such effect was achieved under baking temperatures of 200℃ and 220℃. Physical analysis showed darker colour, harder texture and lower moisture content for biscuits baked at higher test temperatures. It seems intense heating condition that caused “over baking” of the biscuit likely to be responsible for the loss of the vitamin as well as less desirable physical properties of the biscuits.