Prussian blue analogues(PBAs) with inherent ordered structures and abundant metal ion sites are widely explored as precursors for various electrochemical applications,including oxygen evolution reaction(OER).Using a r...Prussian blue analogues(PBAs) with inherent ordered structures and abundant metal ion sites are widely explored as precursors for various electrochemical applications,including oxygen evolution reaction(OER).Using a range of characterization techniques including Fourier-transform infrared spectroscopy(FT-IR),X-ray photoelectron spectroscopy(XPS),X-ray diffraction(XRD) and energy dispersive spectroscopy(EDS),this work discloses the process of replacement of K^(+)by NH4^(+)in the interstitial spaces of the CoFe PBA by a hot aqueous urea solution,which influences the transformation of PBAs under further heat treatment and the OER performance of the deriva tives.After heat treatment at 400℃ under Ar flow,high-resolution transmission electron microscopy(HRTEM) images reveal that CoFe alloy nanoparticles grew on the crystalline cubes of CoFe PBA with K^(+),while CoFe PBA cubes with NH4^(+)become amorphous.Besides,the derivative of CoFe PBA with NH4^(+)(Ar-U-CoFe PBA) performs better than the derivative of CoFe PBA with K^(+)(Ar-CoFe PBA) in OER,registering a lower overpotential of 305 mV at 10 mA cm^(-2),a smaller Tafel slope of 36.1 mV dec^(-1),and better stability over a testing course of 20 h in 1.0 M KOH.A single-cell alkaline electrolyzer,using Ar-U-CoFe PBA and Pt/C for the anodic and cathodic catalyst,respectively,requires an initial cell voltage of 1.66 V to achieve 100 mA cm^(-2)at 80℃,with negligible degradation after100 h.展开更多
This work examines the origin of the abnormal magnetism exhibited by Cu Mn Fe-PBAs modified with multi-walled carbon nanotubes(MWCNTs).The system of Cu Mn Fe-PBAs@MWCNTs coexists with both large and small clusters.Cu ...This work examines the origin of the abnormal magnetism exhibited by Cu Mn Fe-PBAs modified with multi-walled carbon nanotubes(MWCNTs).The system of Cu Mn Fe-PBAs@MWCNTs coexists with both large and small clusters.Cu Mn Fe-PBAs clusters have an average particle size of 28 nm,and some of the smaller particles are adsorbed on the surface of MWCNTs.Surprisingly,the magnitude of magnetization increases linearly with decreasing temperature.When above the Curie temperature,the magnitude of magnetization is significantly greater than that of PBAs without being modified.This phenomenon can be attributed to magnetostatic interactions between ultra-fine magnetic nanoparticles adsorbed on the surface of MWCNTs.Using the Monte Carlo method,we simulated the magnetostatic interaction of cylindrical adsorbed particles,and the simulation results are almost identical to those observed experimentally.The results indicate that 0.089Cu Mn Fe-PBAs clusters per 1 nm^(2)can be adsorbed onto the surface area of MWCNTs.We demonstrate that MWCNTs adsorbing magnetic particles exhibit magnetic behavior,and suggest a method for producing ultrafine materials.It also introduces a new method of calculating the adsorption efficiency of carbon nanotubes,offering theoretical guidance for future research on nanomaterials with enhanced adsorption efficiency.展开更多
The high-rate cyclability of Li-rich Mn-based oxide(LMO)is highly limited by the electrochemical polarization resulting from the slow kinetic of the Li2MnO3 phase.Herein,the Prussian blue(PB)coating layer with specifi...The high-rate cyclability of Li-rich Mn-based oxide(LMO)is highly limited by the electrochemical polarization resulting from the slow kinetic of the Li2MnO3 phase.Herein,the Prussian blue(PB)coating layer with specific redox potential is introduced as a functionalized interface to overcome the side effect and the escaping of O on the surface of LMO,especially its poor rate capability.In detail,the PB layer can restrict the large polarization of LMO by sharing overloaded current at a high rate due to the synchronous redox of PB and LMO.Consequently,an enhanced high rate performance with capacity retention of 87.8%over 300 cycles is obtained,which is superior to 50.5%of the pristine electrode.Such strategies on the high-rate cyclability of Li-rich Mn-based oxide compatible with good low-rate performances may attract great attention for pursuing durable performances.展开更多
In the applications of large-scale energy storage,aqueous batteries are considered as rivals for organic batteries due to their environmentally friendly and low-cost nature.However,carrier ions always exhibit huge hyd...In the applications of large-scale energy storage,aqueous batteries are considered as rivals for organic batteries due to their environmentally friendly and low-cost nature.However,carrier ions always exhibit huge hydrated radius in aqueous electrolyte,which brings difficulty to find suitable host materials that can achieve highly reversible insertion and extraction of cations.Owing to open threedimensional rigid framework and facile synthesis,Prussian blue analogues(PBAs)receive the most extensive attention among various host candidates in aqueous system.Herein,a comprehensive review on recent progresses of PBAs in aqueous batteries is presented.Based on the application in different aqueous systems,the relationship between electrochemical behaviors(redox potential,capacity,cycling stability and rate performance)and structural characteristics(preparation method,structure type,particle size,morphology,crystallinity,defect,metal atom in highspin state and chemical composition)is analyzed and summarized thoroughly.It can be concluded that the required type of PBAs is different for various carrier ions.In particular,the desalination batteries worked with the same mechanism as aqueous batteries are also discussed in detail to introduce the application of PBAs in aqueous systems comprehensively.This report can help the readers to understand the relationship between physical/chemical characteristics and electrochemical properties for PBAs and find a way to fabricate high-performance PBAs in aqueous batteries and desalination batteries.展开更多
Indocyanine green(ICG) is capable of inducing a photothermal effect and the production of cytotoxic reactive oxygen species for cancer therapy. However, the major challenge in applying ICG molecules for antitumor ther...Indocyanine green(ICG) is capable of inducing a photothermal effect and the production of cytotoxic reactive oxygen species for cancer therapy. However, the major challenge in applying ICG molecules for antitumor therapy is associated with their instability in aqueous conditions and rapid clearance from blood circulation,which causes insufficient bioavailability at the tumor site.Herein, we conjugated ICG molecules with Prussian blue nanoparticles enclosing a Fe_3O_4 nanocore, which was facilitated by cationic polyethyleneimine via electrostatic adsorption. The nanocarrier-loaded ICG formed stable aggregates that enhanced cellular uptake and prevented fluorescence quenching. Moreover, the strong superparamagnetism of the Fe_3O_4 core in the obtained nanocomposites further improved cellular internalization of the drugs guided by a localized magnetic field. The therapeutic efficacy of this nanoplatform was evaluated using tumor models established in nude mice, which demonstrated remarkable tumor ablation in vivo due to strong photothermal/photodynamic effects. This study provides promising evidence that this multifunctional nanoagent might function as an efficient mediator for combining photothermal and photodynamic cancer therapy.展开更多
Prussian blue analogue(PBA)material is a promising cathode for applications in Na-ion and K-ion batteries which can support high c-rates for charge and discharge.In this study,the material of composition[K2 CuIIFeII(C...Prussian blue analogue(PBA)material is a promising cathode for applications in Na-ion and K-ion batteries which can support high c-rates for charge and discharge.In this study,the material of composition[K2 CuIIFeII(CN)6]was synthesized and its structural and electrochemical redox behavior was investigated with 5 different alkali insertion cations(Li^+,Na^+,K^+,Rb^+,Cs^+).Galvanostatic measurements indicate that the redox potential strongly depends on the ionic radius of the inserted cation.The redox potential varies by 400 m V between using Li^+(0.79A)or Cs^+(1.73A)in the electrolyte.The underlying modification of the Fe2^+/Fe3^+redox potential in PBA is proposed to be due to the weakening of the Fe–C bond in the material.This hypothesis is supported by XRD measurements which reveal that the lattice parameter of the de-intercalated host structure follows the same trend of monotonic increase with the cation size.The relatively minor volume changes accompanying the redox(1.2%–2.4%)allow the PBA to accommodate differently sized cations,although the structural hindrances are quite pronounced at high c-rates for the larger ones(Rb^+and Cs^+).Cycle aging studies indicate that the minimum capacity fade rate is observed in case of K^+ and Rb^+ containing electrolyte.The peak intensity corresponding to the[220]crystallographic plane varies depending on the state of charge of PBA,since this plane contains the insertion cations.Owing to the sensitivity of the redox potential to the insertion cation coupled with the observed fast ion-exchange ability,the PBA material may find additional analytical applications such as ion sensing or filtration devices.展开更多
Prussian blue analogue Na2Ni[Fe(CN)6](Ni-PB)has been widely studied as a cathode material for sodium-ion battery due to its excellent cycling performance.However,Ni-PB has a low theoretical capacity of 85 mAh g^(−1) b...Prussian blue analogue Na2Ni[Fe(CN)6](Ni-PB)has been widely studied as a cathode material for sodium-ion battery due to its excellent cycling performance.However,Ni-PB has a low theoretical capacity of 85 mAh g^(−1) because of the electrochemical inertness of Ni.Herein,ternary Ni-PB is successfully synthesized by double doping with Co and Fe at Ni-site,and the effect of doping with Co and Fe on the electrochemical performance of Ni-PB is systematically investigated through theoretical calculations and electrochemical tests.The first principles calculations confirm that double doping with Co and Fe can significantly reduce the energy barrier and bandgap of Ni-PB.X-ray diffraction and composition analysis results indicate that ternary NiCoFe-PB composite not only has good crystallinity and high Na content but also has low defects and crystal water.Electrochemical tests reveal that,besides the capacity contribution of high-spin Co/Fe and low-spin Fe,Co-doping enhances the electrochemical activity of low-spin Fe and Fe-doping improves the activity of high-spin Co;moreover,double doping can decrease the diffusion resistance of Na+ions through solid electrolyte interface film,accelerate the kinetics for both ion diffusion process and Faradic reaction,and increase active sites.Under the synergistic effect of Co and Fe,this ternary NiCoFe-PB exhibits outstanding electrochemical performance with a high initial discharge capacity of 120.4 mAh g^(−1) at 20mA g^(−1) and an extremely low capacity fading rate of 0.0044%per cycle at a high current density of 2 A g^(−1) even after 10,000 cycles,showing great application potential of ternary NiCoFe-PB in the field of large-scale energy storage.展开更多
Exploring highly efficient bifunctional photocatalysts for simultaneous H2 evolution and organic chemical production in pure water represents a green route for sustainable solar energy storage and conversion.Herein,a ...Exploring highly efficient bifunctional photocatalysts for simultaneous H2 evolution and organic chemical production in pure water represents a green route for sustainable solar energy storage and conversion.Herein,a facile strategy was explored for preparing a hierarchical porous heterostructure of Fe_(4)Ni_(5)S_(8)@ZnIn_(2)S_(4)(FNS@ZIS)by the in situ growth of ZIS nanosheets on Prussian blue analogue(PBA)-derived bimetallic FNS sulfides.A series of FNS@ZIS hierarchical structures were facilely prepared by adjusting the loading amount(n%)of FNS(n=19,26,and 32 for FNS@ZIS-1-3).These structures can efficiently drive the solar co-production of H_(2) and organic chemicals.The optimal co-production was achieved with FNS@ZIS-2,affording a H_(2) evolution rate of 10465μmol·g^(-1)·h^(-1),along with high selectivity for the oxidation of benzyl alcohol to benzaldehyde(>99.9%).The performance was 22 and 31 times higher than that of FNS and ZIS,respectively,and even superior to the state-of-the-art results achieved using various sacrificial agents.Further mechanistic study indicated that the unique hierarchical core/shell architecture can facilitate interfacial charge separation,afford bimetallic synergy,abundant active sites and excellent photostability.This work highlights a simple and efficient method for preparing porous multimetallic hierarchical structures for the solar co-production of organic chemicals and H_(2) fuel.展开更多
The reversible storage of Zn^(2+)ions in Prussian blue analogues with typical aqueous solution was challenged by fast degradation and poor coulombic efficiency,while the mechanism is yet to be uncovered.This study cor...The reversible storage of Zn^(2+)ions in Prussian blue analogues with typical aqueous solution was challenged by fast degradation and poor coulombic efficiency,while the mechanism is yet to be uncovered.This study correlates the performance of the nickel hexacyanoferrate to the dynamics of H_(2)O in the electrolyte and the associated phase stability of the electrode.It demonstrates severe Ni dissolution in conventional diluted aqueous electrolyte(1 M ZnSO^(4)or 1 M Zn(TFSI)^(2)),leading to structure collapse with the formation of an electrochemical inert phase.This is regarded as the descriptor for the fast decay of nickel hexacyanoferrate in diluted aqueous electrolyte.However,a well-preserved open framework for zinc storage was obtained in concentrated aqueous electrolyte(1 M Zn(TFSI)_(2)+21 M LiTFSI)—the H_(2)O activity is highly suppressed by extensive coordination—thus,reversible capacity of 60.2 m Ah g^(-1)over 1600 cycles could be delivered.展开更多
Nowadays,water pollution has become more serious,greatly affecting human life and healthy.Electrochemical biosensor,a novel and rapid detection technique,plays an important role in the realtime and trace detection of ...Nowadays,water pollution has become more serious,greatly affecting human life and healthy.Electrochemical biosensor,a novel and rapid detection technique,plays an important role in the realtime and trace detection of water pollutants.However,the stability and sensitivity of electrochemical biosensors remain a great challenge for practical detections in real samples to the strong interferences derived from complex components and coagulation effects.In this work,we reported a novel threedimensional architecture of Prussian blue nanoparticles(PBNPs)/Pt nanoparticles(PtNPs)composite film,using 3 D interweaved carbon nanofibers as a supporting matrix,for the construction of screenprinted microchips-based biosensor.PtNPs with diameters of-2.5 nm was highly dispersed on the carbon nanofibers(CNFs)to build a 3 D skeleton nanostructure through a solvothermal reduction.Subsequently,uniform PBNPs were in-situ self-assembled on this skeleton to construct a 3 D architecture of PB/Pt-CNF composite film.Due to the synergistic effects derived from this special feature,the as-prepared hydroquinone(HQ)biosensor chips can synchronously promote both surface area and conductivity to greatly enhance the electrocatalysis from enzymatic reaction.This biosensor has exhibited a high sensitivity of 220.28μA·L·mmol^(-1)·cm^(-2) with an ultrawide linear range from 2.5μmol·L^(-1) to 1.45 mmol·L^(-1) at a low potential of 0.15 V,as well as the satisfactory reproducibility and usage stability.Besides,its accuracy was also verified in the assays of real water samples.It is highly expected that the 3 D PB/Pt-CNF based screen-printed microchips will have wide applications in dynamic monitoring and early warning of analytes in the various practical fields.展开更多
Transition-metal(TM)-based Prussian blue and its analogues(TM-PBAs) have attracted considerable attention as cathode materials owing to their versatile ion storage capability with tunable working voltages. TM-PBAs wit...Transition-metal(TM)-based Prussian blue and its analogues(TM-PBAs) have attracted considerable attention as cathode materials owing to their versatile ion storage capability with tunable working voltages. TM-PBAs with different crystal structures, morphologies, and TM combinations can exhibit excellent electrochemical properties because of their unique and robust host frameworks with well-defined<100> ionic diffusion channels. Nonetheless, there is still a lack of understanding regarding the performance dependence of TM-PBAs on structural changes during charging/discharging processes. In this study, in situ X-ray diffraction and X-ray absorption fine structure analyses elucidate the TMdependent structural changes in a series of TM-PBAs during the charging and discharging processes.During the discharging process, the lattice volume of Fe-PBA increased while those of Ni-and Cu-PBAs decreased. This discrepancy is attributed to the extent of size reduction of the cyanometallate complex([Fe(CN)_(6)]) via pi-backbonding from Fe to C due to redox flips of the low-spin Fe^(3+/2+) ion. This study presents a comprehensive understanding of how TM selection affects capacity acquisition and phase transition in TM-PBAs, a promising class of cathode materials.展开更多
Quite a great proportion of known tumor cells carry mutation in TP53 gene,expressing mutant p53 proteins(mutp53)missing not only original genome protective activities but also acquiring gain-of-functions that favor tu...Quite a great proportion of known tumor cells carry mutation in TP53 gene,expressing mutant p53 proteins(mutp53)missing not only original genome protective activities but also acquiring gain-of-functions that favor tumor progression and impede treatment of cancers.Zinc ions were reported as agents cytocidal to mutp53-carrying cells by recovering p53 normal functions and abrogating mutp53.Meanwhile in a hyperthermia scenario,the function of wild type p53 is required to ablate tumors upon heat treatment hence the effects might be hindered in a mutp53 background.We herein synthesized zinc-doped Prussian blue(ZP)nanoparticles(NPs)to combine Zn 2+based and photothermal therapeutic effects.An efficient release of Zn 2+in a glutathione-enriched tumor intracellular microenvironment and a prominent photothermal conversion manifested ZP NPs as zinc ion carriers and photothermal agents.Apoptotic death and autophagic mutp53 elimination were found to be induced by ZP NPs in R280K mutp53-containing MDA-MB-231 cells and hyperthermia was rendered to ameliorate the treatment in vitro through further mutp53 elimination and increased cell death.The combinatorial therapeutic effect was also confirmed in vivo in a mouse model.This study might expand zinc delivery carriers and shed a light on potential interplay of hyperthermia and mutp53 degradation in cancer treatment.展开更多
Supercapacitors(SCs)with high power output have attracted increasing attention as efficient and environmentally friendly energy storage devices.Prussian blue and its analogues(PB/PBAs)are simple coordination polymers ...Supercapacitors(SCs)with high power output have attracted increasing attention as efficient and environmentally friendly energy storage devices.Prussian blue and its analogues(PB/PBAs)are simple coordination polymers with tunable chemical compositions and open framework.Prussian blue can act as electrode materials in its pristine form and has also been utilized to derive various metallic nanostructures for electrochemical applications due to their simple fabrication process,non-toxic characteristics,and low price.Here,we firstly describe the charge storage mechanisms of SCs briefly followed by an introduction of the fabrication methods of PB/PBAs and their derivatives.Then,a comprehensive review on recent studies of the use of PB/PBAs and their derivatives as the electrode materials for SCs are given with a focus on strategies to improve their electrochemical performances.Finally,we discuss critical challenges in this research area and propose some general ideas for future research.展开更多
A simple and sensitive flow injection(FI) spectrophotometric method was reported for the determination of uric acid based on the reduction of Fe(III)/ferricyanide in the presence of uric acid. The in situ reduced ions...A simple and sensitive flow injection(FI) spectrophotometric method was reported for the determination of uric acid based on the reduction of Fe(III)/ferricyanide in the presence of uric acid. The in situ reduced ions reacted with unreduced portion of ferricyanide/Fe(III) to form soluble Prussian blue, which was monitored at an absorption wavelength of 735 nm. The optimized conditions allow a linear calibration graph in a concentration range of 1―100 μmol/L. The relative standard deviation was in a range of 0.5%―2.5%, with a detection limit(3σ blank) of 0.3 μmol/L and a sampling frequency of 60 injection/h was obtained. The effect of common substances present in human physiological fluids on the determination of uric acid was examined. The method was applied to determining uric acid in human urine samples with the recoveries in a range of 96%―105%. The results agree well with those by spectrophotometric reference method at a confidence level of 95%. Spectrophotometric procedures for uric acid determination in clinical samples were reviewed briefly.展开更多
AIM:To explore the value of Prussian blue staining in the diagnosis of ocular siderosis.METHODS:Between January 2012 and January 2013,the Prussian blue stain used in anterior lens capsule and vitreous liquid after cen...AIM:To explore the value of Prussian blue staining in the diagnosis of ocular siderosis.METHODS:Between January 2012 and January 2013,the Prussian blue stain used in anterior lens capsule and vitreous liquid after centrifugation from patients with definitive diagnosis and suspicious diagnosed of ocular siderosis. At the same time, give a negative control.RESULTS:Anterior lens capsule membrane and liquid of vitreous cavity from patients with definitive diagnosis and suspicious diagnosed of ocular siderosis revealed ferric ions that stained positively with Prussian blue. In the control group, there is no positive reaction.CONCLUSION:Prussian blue staining in the diagnosis of ocular siderosis has a very significant worth,suspected cases can be definitive diagnosed.展开更多
The magnetization of ternary metal Prussian blue analogues A1xA21-x B,formed by three different sublattices A1,A2 and B,is studied by using the effective-field theory with self-spin correlations.Effects of the mole fr...The magnetization of ternary metal Prussian blue analogues A1xA21-x B,formed by three different sublattices A1,A2 and B,is studied by using the effective-field theory with self-spin correlations.Effects of the mole fraction x,the anisotropy and the transverse magnetic field on the magnetization are discussed.展开更多
Prussian blue(PB) was used as catalyst to improve the extent of graphitization of polyacrylonitrile(PAN)-based carbon fibers.PB was deposited on carbon fibers by anodic electrodeposition and the thickness of PB coatin...Prussian blue(PB) was used as catalyst to improve the extent of graphitization of polyacrylonitrile(PAN)-based carbon fibers.PB was deposited on carbon fibers by anodic electrodeposition and the thickness of PB coating(PB content) was controlled by adjusting the electrodeposition time.PAN-based carbon fibers with PB coating were heat-treated and the extent of graphitization was measured by X-ray diffractometry and Raman spectroscopy.The results indicate that the extent of graphitization of PAN-based carbon fibers is enhanced in the presence of the coating.When the PB-coated carbon fibers were heat-treated at 1 900 ℃,interlayer spacing(d002) and crystallite size(Lc) reach 0.336 8 and 21.2 nm respectively.Contrarily,the values of d002 and Lc are 0.341 4 and 7.4 nm respectively when the bare carbon fibers were heat-treated at 2 800 ℃.Compared with the bare carbon fibers,PB can make the heat treatment temperature(HTT) drop more than 500 ℃ in order to reach the same extent of graphitization.Furthermore,the research results show that PB content also has a certain influence on the extent of graphitization at the same HTT.展开更多
Prussian blue (PB) modified carbon felt electrodes were prepared. The electrochemical behavior was investigated by cyclic voltammetry, electrochemical impedance spectroscopy and charge-discharge experiments. In order ...Prussian blue (PB) modified carbon felt electrodes were prepared. The electrochemical behavior was investigated by cyclic voltammetry, electrochemical impedance spectroscopy and charge-discharge experiments. In order to distinguish the mechanism of the PB modified carbon felt electrode, the electrochemical quartz crystal microbalance (EQCM) was employed. The results of cyclic voltammetry show that the modification can improve the reversibility and the suitable PB deposition is the amount of 10 circles deposition. PB modified carbon felt electrode can effectively decrease the charge transfer resistance. The voltage efficiency of VRB employing PB modified carbon felt electrode can be increased by 12%. The mass change of the PB modified Pt crystal electrode in the process of the potential scan is obvious. The reaction of substitution of VO2+ for high-spin Fe ion in PB is probable to happen and the possible reaction equation is given. The preliminary exploration shows that PB modified carbon felt is electrochemically promising for redox flow battery.展开更多
Thallium is a highly toxic metal,and trace amount of thallium(I)(Tl+)in potable water could cause a severe water crisis,which arouses the exploitation of highly-effective technology for purification of Tl+contaminated...Thallium is a highly toxic metal,and trace amount of thallium(I)(Tl+)in potable water could cause a severe water crisis,which arouses the exploitation of highly-effective technology for purification of Tl+contaminated water.This report proposes the multi-layered Prussian blue(PB)-decorated composite membranes(PBx@PDA/PEI-FP)based on the aminated filter papers for Tl+uptake.Extensively characterization by Fourier transform infrared spectrometer-attenuated total reflectance,scanning electron microscope,thermogravimetric analysis,X-ray photoelectron spectroscopy and X-ray diffraction were performed to confirm the in situ growth of cubic PB crystals on filter paper membrane surfaces via the aminated layers,and the successful fabrication of multi-layered PB overcoats via the increasing of aminated layers.The effect of PB layers on Tl+removal by PBx@PDA/PEI-FP from simulated drinking water was evaluated as well as the influence of different experimental conditions.A trade-off between PB decoration layer number and PB distribution sizes is existed in Tl+uptake by PBx@PDA/PEI-FP.The double-layered PB2@PDA/PEI-FP membrane showed the maximum sorption capacity,but its Tl+uptake performance was weakened by the acid,coexisting ions(K+and Na+)and powerful operation pressure,during filtrating a large volume of low-concentrated Tl+-containing water.However,the negative effect of coexisting ions on the Tl+uptake could be effectively eliminated in weak alkaline water,and the Tl+removal was increased up to 100%without any pressure driving for PB2@PDA/PEI-FP membrane.Most importantly,PB2@PDA/PEI-FP displayed the high-efficiency and high-selectivity in purifying the Tl+-spiked Pearl River water,in which the residual Tl+in filtrate was less than 2μg·L^(–1) to meet the drinking water standard of United States Environmental Protection Agency.This work provides a feasible avenue to safeguard the drinking water in remote and underdeveloped area via the energy-free operation.展开更多
基金Financial support from the China Scholarship Council(201806220068,201806650009) to F.Dthe Villum Experiment(grant No.35844) to X.X.
文摘Prussian blue analogues(PBAs) with inherent ordered structures and abundant metal ion sites are widely explored as precursors for various electrochemical applications,including oxygen evolution reaction(OER).Using a range of characterization techniques including Fourier-transform infrared spectroscopy(FT-IR),X-ray photoelectron spectroscopy(XPS),X-ray diffraction(XRD) and energy dispersive spectroscopy(EDS),this work discloses the process of replacement of K^(+)by NH4^(+)in the interstitial spaces of the CoFe PBA by a hot aqueous urea solution,which influences the transformation of PBAs under further heat treatment and the OER performance of the deriva tives.After heat treatment at 400℃ under Ar flow,high-resolution transmission electron microscopy(HRTEM) images reveal that CoFe alloy nanoparticles grew on the crystalline cubes of CoFe PBA with K^(+),while CoFe PBA cubes with NH4^(+)become amorphous.Besides,the derivative of CoFe PBA with NH4^(+)(Ar-U-CoFe PBA) performs better than the derivative of CoFe PBA with K^(+)(Ar-CoFe PBA) in OER,registering a lower overpotential of 305 mV at 10 mA cm^(-2),a smaller Tafel slope of 36.1 mV dec^(-1),and better stability over a testing course of 20 h in 1.0 M KOH.A single-cell alkaline electrolyzer,using Ar-U-CoFe PBA and Pt/C for the anodic and cathodic catalyst,respectively,requires an initial cell voltage of 1.66 V to achieve 100 mA cm^(-2)at 80℃,with negligible degradation after100 h.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11447231 and 12105137)the National Undergraduate Innovation and Entrepreneurship Training Program Support Projects of China+3 种基金the Natural Science Foundation of Hunan Province,China(Grant No.2020JJ4517)the Research Foundation of Education Bureau of Hunan Province,China(Grant Nos.19A434,19A43319C1621)the Opening Project of Cooperative Innovation Center for Nuclear Fuel Cycle Technology and Equipment,University of South China(Grant Nos.2019KFY10 and2019KFY09)。
文摘This work examines the origin of the abnormal magnetism exhibited by Cu Mn Fe-PBAs modified with multi-walled carbon nanotubes(MWCNTs).The system of Cu Mn Fe-PBAs@MWCNTs coexists with both large and small clusters.Cu Mn Fe-PBAs clusters have an average particle size of 28 nm,and some of the smaller particles are adsorbed on the surface of MWCNTs.Surprisingly,the magnitude of magnetization increases linearly with decreasing temperature.When above the Curie temperature,the magnitude of magnetization is significantly greater than that of PBAs without being modified.This phenomenon can be attributed to magnetostatic interactions between ultra-fine magnetic nanoparticles adsorbed on the surface of MWCNTs.Using the Monte Carlo method,we simulated the magnetostatic interaction of cylindrical adsorbed particles,and the simulation results are almost identical to those observed experimentally.The results indicate that 0.089Cu Mn Fe-PBAs clusters per 1 nm^(2)can be adsorbed onto the surface area of MWCNTs.We demonstrate that MWCNTs adsorbing magnetic particles exhibit magnetic behavior,and suggest a method for producing ultrafine materials.It also introduces a new method of calculating the adsorption efficiency of carbon nanotubes,offering theoretical guidance for future research on nanomaterials with enhanced adsorption efficiency.
基金supported by the National Natural Science Foundation of China (51802261,52072298,and 52172228)the Natural Science Foundation of Shaanxi (2019GHJD-13 and 2020JC-41)+2 种基金the Natural Science Basic Research Plan in Shaanxi province of China (2019JLP-04)Xi'an Science and Technology Project of China (2019219714SYS012CG034)the foundation of National Key Laboratory (6142808200202),PR China.
文摘The high-rate cyclability of Li-rich Mn-based oxide(LMO)is highly limited by the electrochemical polarization resulting from the slow kinetic of the Li2MnO3 phase.Herein,the Prussian blue(PB)coating layer with specific redox potential is introduced as a functionalized interface to overcome the side effect and the escaping of O on the surface of LMO,especially its poor rate capability.In detail,the PB layer can restrict the large polarization of LMO by sharing overloaded current at a high rate due to the synchronous redox of PB and LMO.Consequently,an enhanced high rate performance with capacity retention of 87.8%over 300 cycles is obtained,which is superior to 50.5%of the pristine electrode.Such strategies on the high-rate cyclability of Li-rich Mn-based oxide compatible with good low-rate performances may attract great attention for pursuing durable performances.
基金This work was sponsored by NSAF Joint Fund(U1830106)Science and Technology Innovation 2025 Major Program of Ningbo(2018B10061)K.C.Wong Magna Fund in Ningbo University.
文摘In the applications of large-scale energy storage,aqueous batteries are considered as rivals for organic batteries due to their environmentally friendly and low-cost nature.However,carrier ions always exhibit huge hydrated radius in aqueous electrolyte,which brings difficulty to find suitable host materials that can achieve highly reversible insertion and extraction of cations.Owing to open threedimensional rigid framework and facile synthesis,Prussian blue analogues(PBAs)receive the most extensive attention among various host candidates in aqueous system.Herein,a comprehensive review on recent progresses of PBAs in aqueous batteries is presented.Based on the application in different aqueous systems,the relationship between electrochemical behaviors(redox potential,capacity,cycling stability and rate performance)and structural characteristics(preparation method,structure type,particle size,morphology,crystallinity,defect,metal atom in highspin state and chemical composition)is analyzed and summarized thoroughly.It can be concluded that the required type of PBAs is different for various carrier ions.In particular,the desalination batteries worked with the same mechanism as aqueous batteries are also discussed in detail to introduce the application of PBAs in aqueous systems comprehensively.This report can help the readers to understand the relationship between physical/chemical characteristics and electrochemical properties for PBAs and find a way to fabricate high-performance PBAs in aqueous batteries and desalination batteries.
基金financial support from Fundamental Research Funds for Central Universities (XDJK2016A010 and XDJK2017C001)National Natural Science Foundation of China (51703186 and 31671037)Southwest University (SWU116032 and SWU115059)
文摘Indocyanine green(ICG) is capable of inducing a photothermal effect and the production of cytotoxic reactive oxygen species for cancer therapy. However, the major challenge in applying ICG molecules for antitumor therapy is associated with their instability in aqueous conditions and rapid clearance from blood circulation,which causes insufficient bioavailability at the tumor site.Herein, we conjugated ICG molecules with Prussian blue nanoparticles enclosing a Fe_3O_4 nanocore, which was facilitated by cationic polyethyleneimine via electrostatic adsorption. The nanocarrier-loaded ICG formed stable aggregates that enhanced cellular uptake and prevented fluorescence quenching. Moreover, the strong superparamagnetism of the Fe_3O_4 core in the obtained nanocomposites further improved cellular internalization of the drugs guided by a localized magnetic field. The therapeutic efficacy of this nanoplatform was evaluated using tumor models established in nude mice, which demonstrated remarkable tumor ablation in vivo due to strong photothermal/photodynamic effects. This study provides promising evidence that this multifunctional nanoagent might function as an efficient mediator for combining photothermal and photodynamic cancer therapy.
基金“Le Studium Loire Valley Institute for Advanced Studies” for financial and logistical support to the researchers involved in this study“Region Centre” for financial support under the “Lavoisier” program
文摘Prussian blue analogue(PBA)material is a promising cathode for applications in Na-ion and K-ion batteries which can support high c-rates for charge and discharge.In this study,the material of composition[K2 CuIIFeII(CN)6]was synthesized and its structural and electrochemical redox behavior was investigated with 5 different alkali insertion cations(Li^+,Na^+,K^+,Rb^+,Cs^+).Galvanostatic measurements indicate that the redox potential strongly depends on the ionic radius of the inserted cation.The redox potential varies by 400 m V between using Li^+(0.79A)or Cs^+(1.73A)in the electrolyte.The underlying modification of the Fe2^+/Fe3^+redox potential in PBA is proposed to be due to the weakening of the Fe–C bond in the material.This hypothesis is supported by XRD measurements which reveal that the lattice parameter of the de-intercalated host structure follows the same trend of monotonic increase with the cation size.The relatively minor volume changes accompanying the redox(1.2%–2.4%)allow the PBA to accommodate differently sized cations,although the structural hindrances are quite pronounced at high c-rates for the larger ones(Rb^+and Cs^+).Cycle aging studies indicate that the minimum capacity fade rate is observed in case of K^+ and Rb^+ containing electrolyte.The peak intensity corresponding to the[220]crystallographic plane varies depending on the state of charge of PBA,since this plane contains the insertion cations.Owing to the sensitivity of the redox potential to the insertion cation coupled with the observed fast ion-exchange ability,the PBA material may find additional analytical applications such as ion sensing or filtration devices.
基金National Natural Science Foundation of China,Grant/Award Number:52072217,51802261,51772169National Key R&D Program of China,Grant/Award Number:2018YFB0905400Major Technological Innovation Project of Hubei Science and Technology Department,Grant/Award Number:2019AAA164。
文摘Prussian blue analogue Na2Ni[Fe(CN)6](Ni-PB)has been widely studied as a cathode material for sodium-ion battery due to its excellent cycling performance.However,Ni-PB has a low theoretical capacity of 85 mAh g^(−1) because of the electrochemical inertness of Ni.Herein,ternary Ni-PB is successfully synthesized by double doping with Co and Fe at Ni-site,and the effect of doping with Co and Fe on the electrochemical performance of Ni-PB is systematically investigated through theoretical calculations and electrochemical tests.The first principles calculations confirm that double doping with Co and Fe can significantly reduce the energy barrier and bandgap of Ni-PB.X-ray diffraction and composition analysis results indicate that ternary NiCoFe-PB composite not only has good crystallinity and high Na content but also has low defects and crystal water.Electrochemical tests reveal that,besides the capacity contribution of high-spin Co/Fe and low-spin Fe,Co-doping enhances the electrochemical activity of low-spin Fe and Fe-doping improves the activity of high-spin Co;moreover,double doping can decrease the diffusion resistance of Na+ions through solid electrolyte interface film,accelerate the kinetics for both ion diffusion process and Faradic reaction,and increase active sites.Under the synergistic effect of Co and Fe,this ternary NiCoFe-PB exhibits outstanding electrochemical performance with a high initial discharge capacity of 120.4 mAh g^(−1) at 20mA g^(−1) and an extremely low capacity fading rate of 0.0044%per cycle at a high current density of 2 A g^(−1) even after 10,000 cycles,showing great application potential of ternary NiCoFe-PB in the field of large-scale energy storage.
基金financial support from the National Natural Science Foundation of China(21722104,21671032 and 21501072)the Natural Science Foundation of Tianjin City of China(18JCJQJC47700 and 17JCQNJC05100)。
文摘Exploring highly efficient bifunctional photocatalysts for simultaneous H2 evolution and organic chemical production in pure water represents a green route for sustainable solar energy storage and conversion.Herein,a facile strategy was explored for preparing a hierarchical porous heterostructure of Fe_(4)Ni_(5)S_(8)@ZnIn_(2)S_(4)(FNS@ZIS)by the in situ growth of ZIS nanosheets on Prussian blue analogue(PBA)-derived bimetallic FNS sulfides.A series of FNS@ZIS hierarchical structures were facilely prepared by adjusting the loading amount(n%)of FNS(n=19,26,and 32 for FNS@ZIS-1-3).These structures can efficiently drive the solar co-production of H_(2) and organic chemicals.The optimal co-production was achieved with FNS@ZIS-2,affording a H_(2) evolution rate of 10465μmol·g^(-1)·h^(-1),along with high selectivity for the oxidation of benzyl alcohol to benzaldehyde(>99.9%).The performance was 22 and 31 times higher than that of FNS and ZIS,respectively,and even superior to the state-of-the-art results achieved using various sacrificial agents.Further mechanistic study indicated that the unique hierarchical core/shell architecture can facilitate interfacial charge separation,afford bimetallic synergy,abundant active sites and excellent photostability.This work highlights a simple and efficient method for preparing porous multimetallic hierarchical structures for the solar co-production of organic chemicals and H_(2) fuel.
基金financial support provided by National Key Research and Development Program(No.2019YFA0210600)the National Natural Science Foundation of China(No.21905085+2 种基金No.51972107)the State Grid Shanghai Municipal Electric Power Company(No.B30970190001)the Innovative Research Groups of Hunan Province(No.2019JJ10001)
文摘The reversible storage of Zn^(2+)ions in Prussian blue analogues with typical aqueous solution was challenged by fast degradation and poor coulombic efficiency,while the mechanism is yet to be uncovered.This study correlates the performance of the nickel hexacyanoferrate to the dynamics of H_(2)O in the electrolyte and the associated phase stability of the electrode.It demonstrates severe Ni dissolution in conventional diluted aqueous electrolyte(1 M ZnSO^(4)or 1 M Zn(TFSI)^(2)),leading to structure collapse with the formation of an electrochemical inert phase.This is regarded as the descriptor for the fast decay of nickel hexacyanoferrate in diluted aqueous electrolyte.However,a well-preserved open framework for zinc storage was obtained in concentrated aqueous electrolyte(1 M Zn(TFSI)_(2)+21 M LiTFSI)—the H_(2)O activity is highly suppressed by extensive coordination—thus,reversible capacity of 60.2 m Ah g^(-1)over 1600 cycles could be delivered.
基金financially supported by the National Natural Science Foundation of China(22078148 and 21727818)the Innovative Research Team Program by the Ministry of Education of China(IRT_17R54)+3 种基金the Top-notch Academic Programs Project of Jiangsu Higher Education Institutions(TAPP)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)the Key Project by Medical Science and Technology Development Foundation of Nanjing Department of Health(ZKX17014)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX20_1021)。
文摘Nowadays,water pollution has become more serious,greatly affecting human life and healthy.Electrochemical biosensor,a novel and rapid detection technique,plays an important role in the realtime and trace detection of water pollutants.However,the stability and sensitivity of electrochemical biosensors remain a great challenge for practical detections in real samples to the strong interferences derived from complex components and coagulation effects.In this work,we reported a novel threedimensional architecture of Prussian blue nanoparticles(PBNPs)/Pt nanoparticles(PtNPs)composite film,using 3 D interweaved carbon nanofibers as a supporting matrix,for the construction of screenprinted microchips-based biosensor.PtNPs with diameters of-2.5 nm was highly dispersed on the carbon nanofibers(CNFs)to build a 3 D skeleton nanostructure through a solvothermal reduction.Subsequently,uniform PBNPs were in-situ self-assembled on this skeleton to construct a 3 D architecture of PB/Pt-CNF composite film.Due to the synergistic effects derived from this special feature,the as-prepared hydroquinone(HQ)biosensor chips can synchronously promote both surface area and conductivity to greatly enhance the electrocatalysis from enzymatic reaction.This biosensor has exhibited a high sensitivity of 220.28μA·L·mmol^(-1)·cm^(-2) with an ultrawide linear range from 2.5μmol·L^(-1) to 1.45 mmol·L^(-1) at a low potential of 0.15 V,as well as the satisfactory reproducibility and usage stability.Besides,its accuracy was also verified in the assays of real water samples.It is highly expected that the 3 D PB/Pt-CNF based screen-printed microchips will have wide applications in dynamic monitoring and early warning of analytes in the various practical fields.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(Ministry of Science and ICT)(NRF-2021R1G1A1092280 and NRF2019R1A6A3A03031343)the Dongil Culture and Scholarship Foundationthe technical support provided at 1-D(KIST-PAL XRD and XAFS)and 7-D beamlines(XAFS)of the Pohang Light Source-II at the Pohang Accelerating Laboratory。
文摘Transition-metal(TM)-based Prussian blue and its analogues(TM-PBAs) have attracted considerable attention as cathode materials owing to their versatile ion storage capability with tunable working voltages. TM-PBAs with different crystal structures, morphologies, and TM combinations can exhibit excellent electrochemical properties because of their unique and robust host frameworks with well-defined<100> ionic diffusion channels. Nonetheless, there is still a lack of understanding regarding the performance dependence of TM-PBAs on structural changes during charging/discharging processes. In this study, in situ X-ray diffraction and X-ray absorption fine structure analyses elucidate the TMdependent structural changes in a series of TM-PBAs during the charging and discharging processes.During the discharging process, the lattice volume of Fe-PBA increased while those of Ni-and Cu-PBAs decreased. This discrepancy is attributed to the extent of size reduction of the cyanometallate complex([Fe(CN)_(6)]) via pi-backbonding from Fe to C due to redox flips of the low-spin Fe^(3+/2+) ion. This study presents a comprehensive understanding of how TM selection affects capacity acquisition and phase transition in TM-PBAs, a promising class of cathode materials.
基金by the National Natural Science Foundation of China(No.81772278).
文摘Quite a great proportion of known tumor cells carry mutation in TP53 gene,expressing mutant p53 proteins(mutp53)missing not only original genome protective activities but also acquiring gain-of-functions that favor tumor progression and impede treatment of cancers.Zinc ions were reported as agents cytocidal to mutp53-carrying cells by recovering p53 normal functions and abrogating mutp53.Meanwhile in a hyperthermia scenario,the function of wild type p53 is required to ablate tumors upon heat treatment hence the effects might be hindered in a mutp53 background.We herein synthesized zinc-doped Prussian blue(ZP)nanoparticles(NPs)to combine Zn 2+based and photothermal therapeutic effects.An efficient release of Zn 2+in a glutathione-enriched tumor intracellular microenvironment and a prominent photothermal conversion manifested ZP NPs as zinc ion carriers and photothermal agents.Apoptotic death and autophagic mutp53 elimination were found to be induced by ZP NPs in R280K mutp53-containing MDA-MB-231 cells and hyperthermia was rendered to ameliorate the treatment in vitro through further mutp53 elimination and increased cell death.The combinatorial therapeutic effect was also confirmed in vivo in a mouse model.This study might expand zinc delivery carriers and shed a light on potential interplay of hyperthermia and mutp53 degradation in cancer treatment.
基金supported by the National Natural Science Foundation of China(Nos.51672055,51972342,51872656,and 51702275)Taishan Scholar Project of Shandong Province(ts20190922)Key Basic Research Project of Natural Science Foundation of Shandong Province(ZR2019ZD51)
文摘Supercapacitors(SCs)with high power output have attracted increasing attention as efficient and environmentally friendly energy storage devices.Prussian blue and its analogues(PB/PBAs)are simple coordination polymers with tunable chemical compositions and open framework.Prussian blue can act as electrode materials in its pristine form and has also been utilized to derive various metallic nanostructures for electrochemical applications due to their simple fabrication process,non-toxic characteristics,and low price.Here,we firstly describe the charge storage mechanisms of SCs briefly followed by an introduction of the fabrication methods of PB/PBAs and their derivatives.Then,a comprehensive review on recent studies of the use of PB/PBAs and their derivatives as the electrode materials for SCs are given with a focus on strategies to improve their electrochemical performances.Finally,we discuss critical challenges in this research area and propose some general ideas for future research.
基金Supported by the CIIT-Project Funded by COMSATS Institute of Information Technology,Pakistan
文摘A simple and sensitive flow injection(FI) spectrophotometric method was reported for the determination of uric acid based on the reduction of Fe(III)/ferricyanide in the presence of uric acid. The in situ reduced ions reacted with unreduced portion of ferricyanide/Fe(III) to form soluble Prussian blue, which was monitored at an absorption wavelength of 735 nm. The optimized conditions allow a linear calibration graph in a concentration range of 1―100 μmol/L. The relative standard deviation was in a range of 0.5%―2.5%, with a detection limit(3σ blank) of 0.3 μmol/L and a sampling frequency of 60 injection/h was obtained. The effect of common substances present in human physiological fluids on the determination of uric acid was examined. The method was applied to determining uric acid in human urine samples with the recoveries in a range of 96%―105%. The results agree well with those by spectrophotometric reference method at a confidence level of 95%. Spectrophotometric procedures for uric acid determination in clinical samples were reviewed briefly.
基金Supported by Education Department Funding of Sichuan Province,China(No.2005B020)
文摘AIM:To explore the value of Prussian blue staining in the diagnosis of ocular siderosis.METHODS:Between January 2012 and January 2013,the Prussian blue stain used in anterior lens capsule and vitreous liquid after centrifugation from patients with definitive diagnosis and suspicious diagnosed of ocular siderosis. At the same time, give a negative control.RESULTS:Anterior lens capsule membrane and liquid of vitreous cavity from patients with definitive diagnosis and suspicious diagnosed of ocular siderosis revealed ferric ions that stained positively with Prussian blue. In the control group, there is no positive reaction.CONCLUSION:Prussian blue staining in the diagnosis of ocular siderosis has a very significant worth,suspected cases can be definitive diagnosed.
基金Project supported by the Open Project of Key Laboratory for Magnetism and Magnetic Materials of the Ministry of Education, Lanzhou University,China(Grant No.LZUMMM2010010)the Scientific Foundation of the Educational Department of Liaoning Province,China(Grant No.L2010390)+3 种基金the Natural Science Foundation of Liaoning Province,China(Grant No.20102171)the Scientific Technology Plan of Shenyang,China(Grant No.F10-205-1-33)the Excellent Talents Program of the University of Liaoning Province,China(Grant No.LR201031)the Hong Kong Polytechnic University through the University Research Grant,China(Grant No.A-PA8W)
文摘The magnetization of ternary metal Prussian blue analogues A1xA21-x B,formed by three different sublattices A1,A2 and B,is studied by using the effective-field theory with self-spin correlations.Effects of the mole fraction x,the anisotropy and the transverse magnetic field on the magnetization are discussed.
基金Project(2006CB600903) supported by the National Basic Research Program of China
文摘Prussian blue(PB) was used as catalyst to improve the extent of graphitization of polyacrylonitrile(PAN)-based carbon fibers.PB was deposited on carbon fibers by anodic electrodeposition and the thickness of PB coating(PB content) was controlled by adjusting the electrodeposition time.PAN-based carbon fibers with PB coating were heat-treated and the extent of graphitization was measured by X-ray diffractometry and Raman spectroscopy.The results indicate that the extent of graphitization of PAN-based carbon fibers is enhanced in the presence of the coating.When the PB-coated carbon fibers were heat-treated at 1 900 ℃,interlayer spacing(d002) and crystallite size(Lc) reach 0.336 8 and 21.2 nm respectively.Contrarily,the values of d002 and Lc are 0.341 4 and 7.4 nm respectively when the bare carbon fibers were heat-treated at 2 800 ℃.Compared with the bare carbon fibers,PB can make the heat treatment temperature(HTT) drop more than 500 ℃ in order to reach the same extent of graphitization.Furthermore,the research results show that PB content also has a certain influence on the extent of graphitization at the same HTT.
基金Project (2008ZX07313-005) supported by the National Water Pollution Control and Management of Major Special Science and Technology Foundation
文摘Prussian blue (PB) modified carbon felt electrodes were prepared. The electrochemical behavior was investigated by cyclic voltammetry, electrochemical impedance spectroscopy and charge-discharge experiments. In order to distinguish the mechanism of the PB modified carbon felt electrode, the electrochemical quartz crystal microbalance (EQCM) was employed. The results of cyclic voltammetry show that the modification can improve the reversibility and the suitable PB deposition is the amount of 10 circles deposition. PB modified carbon felt electrode can effectively decrease the charge transfer resistance. The voltage efficiency of VRB employing PB modified carbon felt electrode can be increased by 12%. The mass change of the PB modified Pt crystal electrode in the process of the potential scan is obvious. The reaction of substitution of VO2+ for high-spin Fe ion in PB is probable to happen and the possible reaction equation is given. The preliminary exploration shows that PB modified carbon felt is electrochemically promising for redox flow battery.
基金supported by the National Natural Science Foundation of China(Grant Nos.22006026,52270001)Guangdong Basic and Applied Basic Research Foundation(Grant Nos.2023A1515012506,2019A1515110546)+4 种基金Science and Technology Program of Guangzhou(Grant No.202102080160)Project of Young Innovative Talents in Colleges and Universities of Guangdong Province(Grant No.2019KQNCX111)Outstanding Youth Project of Guangdong Natural Science Foundation(Grant No.2022B1515020030)Guangzhou Science and Technology Project(Grant Nos.202201020530,202201020200)Research Project of Guangzhou University(Grant No.YJ2023026).
文摘Thallium is a highly toxic metal,and trace amount of thallium(I)(Tl+)in potable water could cause a severe water crisis,which arouses the exploitation of highly-effective technology for purification of Tl+contaminated water.This report proposes the multi-layered Prussian blue(PB)-decorated composite membranes(PBx@PDA/PEI-FP)based on the aminated filter papers for Tl+uptake.Extensively characterization by Fourier transform infrared spectrometer-attenuated total reflectance,scanning electron microscope,thermogravimetric analysis,X-ray photoelectron spectroscopy and X-ray diffraction were performed to confirm the in situ growth of cubic PB crystals on filter paper membrane surfaces via the aminated layers,and the successful fabrication of multi-layered PB overcoats via the increasing of aminated layers.The effect of PB layers on Tl+removal by PBx@PDA/PEI-FP from simulated drinking water was evaluated as well as the influence of different experimental conditions.A trade-off between PB decoration layer number and PB distribution sizes is existed in Tl+uptake by PBx@PDA/PEI-FP.The double-layered PB2@PDA/PEI-FP membrane showed the maximum sorption capacity,but its Tl+uptake performance was weakened by the acid,coexisting ions(K+and Na+)and powerful operation pressure,during filtrating a large volume of low-concentrated Tl+-containing water.However,the negative effect of coexisting ions on the Tl+uptake could be effectively eliminated in weak alkaline water,and the Tl+removal was increased up to 100%without any pressure driving for PB2@PDA/PEI-FP membrane.Most importantly,PB2@PDA/PEI-FP displayed the high-efficiency and high-selectivity in purifying the Tl+-spiked Pearl River water,in which the residual Tl+in filtrate was less than 2μg·L^(–1) to meet the drinking water standard of United States Environmental Protection Agency.This work provides a feasible avenue to safeguard the drinking water in remote and underdeveloped area via the energy-free operation.
