Zinc-iodine batteries have received significant attention due to their high theoretical capacity and environmental friendliness,but their performance is restricted by the growth of zinc dendrites,the hydrogen evolutio...Zinc-iodine batteries have received significant attention due to their high theoretical capacity and environmental friendliness,but their performance is restricted by the growth of zinc dendrites,the hydrogen evolution reaction,and the shuttling effect of polyiodide ions.In this study,an amidoximefunctionalized hydrogel electrolyte,created by amidoximated porous polymer of intrinsic microporosity(AO-PIM-1)and sodium alginate(Alg),is designed to address the aforementioned problems through synergistically optimizing the interfaces of the zinc anode and iodine cathode.The rigid microporous framework and amidoxime groups of AO-PIM-1 can repel polyiodides and inhibit their shuttle effect.Meanwhile,the polyanionic properties of Alg guide the uniform deposition of Zn^(2+)along the(002)crystal plane through the“egg-box”structure,thus suppressing the formation of dendrites.The AO-PIM-1/Alg electrolyte has a high ionic conductivity(18.6 mS cm^(-1)).The assembled symmetric battery can achieve highly reversible dendrite-free zinc plating/stripping(stably cycling for 2550 h at 1 mA cm^(-2)).The Zn-I_(2) full battery with the AO-PIM-1/Alg electrolyte has a long lifespan of 8700 cycles at 0.5 A g^(-1).The working mechanism of the electrolyte was elucidated through density functional theoretical calculations and molecular dynamics simulations.This study provides a new strategy for the hydrogel electrolyte of ZnI_(2) batteries.展开更多
Removal of uranium(VI)from nuclear wastewater is urgent due to the global nuclear energy exploitation.This study synthesized novel sponge-like 3D porous materials for enhanced uranium adsorption by combining electrosp...Removal of uranium(VI)from nuclear wastewater is urgent due to the global nuclear energy exploitation.This study synthesized novel sponge-like 3D porous materials for enhanced uranium adsorption by combining electrospinning and fibrous freeze-shaping techniques.The materials possessed an organic-inorganic hybrid architecture based on the electrospun fibers of polyacrylonitrile(PAN)and SiO_(2).As a sup-porting material,the surface of fibrous SiO_(2) could be further functionalized by cyano groups via(3-cyanopropyl)triethoxysilane.All the cyano groups were turned into amidoxime(AO)groups to obtain a amidoxime-functionalized sponge(PAO/SiO_(2)-AO)through the subsequent ami-doximation process.The proposed sponge exhibited enhanced uranium adsorption performance with a high removal capacity of 367.12 mg/g,a large adsorption coefficient of 4.0×10^(4)mL/g,and a high removal efficiency of 97.59%.The UO_(2)^(2+)adsorption kinetics perfectly conformed to the pseudo-second-order reaction.The sorbent also exhibited an excellent selectivity for UO_(2)^(2+) with other interfering metal ions.2023 Hohai University.Production and hosting by Elsevier B.V.展开更多
An amidoxime-based polymeric adsorbent was prepared by pre-irradiation grafting of acrylonitrile and acrylic acid onto high-density polyethylene fibers using electron beams,followed by amidoximation.Quantitative recov...An amidoxime-based polymeric adsorbent was prepared by pre-irradiation grafting of acrylonitrile and acrylic acid onto high-density polyethylene fibers using electron beams,followed by amidoximation.Quantitative recovery of uranium was investigated by flow-through experiment using simulated seawater and marine test in natural seawater.The maximum amount of uranium uptake was 2.51 mg/g-ads after 42 days of contact with simulated seawater and 0.13 mg/g-ads for 15 days of contact with natural seawater.A lower uranium uptake in marine test can be attributed to the short adsorption time and the contamination of marine microorganisms and iron.However,the high selectivity toward uranium against vanadium may be beneficial to harvest uranyl ion onto adsorbents and the economic feasibility for recovery of uranium from seawater.展开更多
A novel amidoxime-based fibrous adsorbent,denoted as PE/PP-g-(PAAc-co-PAO), was prepared by preirradiation grafting of acrylic acid and acrylonitrile onto polyethylene-coated polypropylene skin-core(PE/PP)fibers using...A novel amidoxime-based fibrous adsorbent,denoted as PE/PP-g-(PAAc-co-PAO), was prepared by preirradiation grafting of acrylic acid and acrylonitrile onto polyethylene-coated polypropylene skin-core(PE/PP)fibers using 60 Co γ-ray irradiation, followed by amidoximation. The original and modified PE/PP fibers were characterized by a series of characterization methods to demonstrate the attachment of amidoxime groups onto the PE/PP fibers. Breaking strength tests confirmed that the fibrous adsorbent could maintain good mechanical properties. The adsorption capacity of the PE/PP-g-(PAAc-coPAO) fibers was investigated in simulated seawater with an initial uranium concentration of 330 μg/L. The uranium adsorption capacity was 2.27 mg/g-adsorbent after 24 h in simulated seawater, and the equilibrium data were well described by the Freundlich isotherm model. The PE/PP-g-(PAAc-co-PAO) adsorbent exhibited good regeneration and recyclability during five adsorption-desorption cycles.The adsorption test was also performed in simulated radioactive effluents with uranium concentrations of 10 and100 μg/L. The effect of the pH value on the adsorption capacity was also studied. At a very low initial concentration 10 μg/L solution, the PE/PP-g-(PAAc-co-PAO)fiber could remove as much as 93.0% of the uranium, and up to 71.2% of the uranium in the simulated radioactive effluent. These results indicated that the PE/PP-g-(PAAcco-PAO) adsorbent could be used in radioactive effluents over a wide range of pH values. Therefore, the PE/PP-g-(PAAc-co-PAO) fibers, with their high uranium selectivity,good regeneration and recyclability,good mechanical properties, and low cost, are promising adsorbents for extracting uranium from aqueous solutions.展开更多
Uranyl （VI） amidoxime complexes are investigated using relativistic density functional theory. The equilibrium structures, bond orders, and Mulliken populations of the complexes have been systematically investigated...Uranyl （VI） amidoxime complexes are investigated using relativistic density functional theory. The equilibrium structures, bond orders, and Mulliken populations of the complexes have been systematically investigated under a generalized gradient approximation （GGA）. Comparison of （acet） uranyl amidoxime complexes （[UO2（AO）n]2-n, 1≤ n≤4） with available experimental data shows an excellent agreement. In addition, the U-O（1）, U-O（3）, C（1）-N（2）, and C（3） N（4） bond lengths of [UO2（CH3AO）4]2- are longer than experimental data by about 0.088, 0.05, 0.1, and 0.056 A. The angles of N（3） O（3）-U, O（2）-N（1）-C（1）, N（3）-C（3）-N（4）, N（4）-C（3） C（4）, and C（4）-C（3）-N（3） are different from each other, which is due to existing interaction between oxygen in uranyl and hydrogen in amino group. This interaction is found to be intra-molecular hydrogen bond. Studies on the bond orders, Mulliken charges, and Mulliken populations demonstrate that uranyl oxo group functions as hydrogen-bond acceptors and H atoms in ligands act as hydrogen-bond donors forming hydrogen bonds within the complex.展开更多
An affinity membrane was prepared by coaxial electrospinning and amidoxime(AONFA),and it was applied to selectively recovery Au(Ⅲ)from an aqueous solution.The static adsorption results showed that,when p H at 5,the m...An affinity membrane was prepared by coaxial electrospinning and amidoxime(AONFA),and it was applied to selectively recovery Au(Ⅲ)from an aqueous solution.The static adsorption results showed that,when p H at 5,the maximum adsorption capacity of AONFA membrane for Au(Ⅲ)was 509.3 mg·g^(-1).AONFA membrane exhibit much higher affinity and selectivity towards Au(Ⅲ)than other metal cations.The membrane could be regenerated effectively by mixture solution of thiourea and HCl,and the desorption ratio reached almost 100%after 4 hours desorption.The dead-end filtration results showed that,the membrane utilization efficiency and adsorption capacity can be improved by increasing the flow rate,while increasing the concentration shorted the breakthrough process and had little impact to adsorption capacity.We can flexibly adjust the flow rate and concentration according to the situation to obtain the maximum utilization efficiency of the membrane in filtration process.The dynamic adsorption capacity is higher than the static adsorption capacity.The adsorption mechanism for Au(Ⅲ)is electrostatic adsorption and reduction.Thus,AONFA membrane filtration was demonstrated to be a promising method for continuous recover Au(Ⅲ)from wastewater.展开更多
A well-known adsorbent, poly(amidoxime)ligand, was prepared from polyacrylonitrile(PAN) grafted kenaf cellulose, and subsequent characterization was performed by Fourier transform infrared spectroscopy(FTIR),field emi...A well-known adsorbent, poly(amidoxime)ligand, was prepared from polyacrylonitrile(PAN) grafted kenaf cellulose, and subsequent characterization was performed by Fourier transform infrared spectroscopy(FTIR),field emission scanning electron microscope(FESEM) and inductively coupled plasma mass spectrometry(ICP-MS).The adsorption capacities of the prepared ligand for rare earth metals are found to be excellent, with adsorptions of La^(3+), Ce^(3+), Pr^(3+), Gd^(3+) and Nd^(3+) experimentally determined to be 262, 255, 244, 241 and 233 mg·g^(-1), respectively, at pH 6. The experimental values of the adsorption of rare earth metals are well matched with the pseudosecond-order rate equation. The reusability of the adsorbent is examined for seven cycles of sorption/desorption,demonstrating that the proposed adsorbent could be reused for over seven cycles without any significant loss in the original removal capability of the ligand.展开更多
Direct collection of uranium from low uranium systems via adsorption remains challenging.Fibrous sorbent materials with amidoxime(AO)groups are promising adsorbents for uranium extraction from seawater.However,low AO ...Direct collection of uranium from low uranium systems via adsorption remains challenging.Fibrous sorbent materials with amidoxime(AO)groups are promising adsorbents for uranium extraction from seawater.However,low AO adsorption group utilization remains an issue.We herein fabricated a branched structure containing AO groups on polypropylene/polyethylene spun-laced nonwoven(PP/PE SNW)fibers using grafting polymerization induced by radiation(RIGP)to improve AO utilization.The chemical structures,thermal properties,and surface morphologies of the raw and treated PP/PE SNW fibers were studied.The results show that an adsorptive functional layer with a branching structure was successfully anchored to the fiber surface.The adsorption properties were investigated using batch adsorption experiments in simulated seawater with an initial uranium concentration of 500μg·L^(−1)(pH 4,25℃).The maximum adsorption capacity of the adsorbent material was 137.3 mg·g^(−1)within 24 h;moreover,the uranyl removal reached 96%within 240 min.The adsorbent had an AO utilization rate of 1/3.5 and was stable over a pH range of 4–10,with good selectivity and reusability,demonstrating its potential for seawater uranium extraction.展开更多
With the application of resins in various fields, numerous waste resins that are difficult to treat have been produced. The industrial wastewater containing Cr(Ⅵ) has severely polluted soil and groundwater environmen...With the application of resins in various fields, numerous waste resins that are difficult to treat have been produced. The industrial wastewater containing Cr(Ⅵ) has severely polluted soil and groundwater environments, thereby endangering human health. Therefore, in this paper, a novel functionalized mesoporous adsorbent PPR-Z was synthesized from waste amidoxime resin for adsorbing Cr(Ⅵ). The waste amidoxime resin was first modified with H3PO4 and ZnCl_(2), and subsequently, it was carbonized through slow thermal decomposition. The static adsorption of PPR-Z conforms to the pseudo-second-order kinetic model and Langmuir isotherm, indicating that the Cr(Ⅵ) adsorption by PPR-Z is mostly chemical adsorption and exhibits single-layer adsorption. The saturated adsorption capacity of the adsorbent for Cr(Ⅵ) could reach 255.86 mg/g. The adsorbent could effectively reduce Cr(Ⅵ) to Cr(Ⅲ) and decrease the toxicity of Cr(Ⅵ) during adsorption. PPR-Z exhibited Cr(Ⅵ) selectivity in electroplating wastewater. The main mechanisms involved in the Cr(Ⅵ) adsorption are the chemical reduction of Cr(Ⅵ) into Cr(Ⅲ) and electrostatic and coordination interactions. Preparation of PPR-Z not only solves the problem of waste resin treatment but also effectively controls Cr(Ⅵ) pollution and realizes the concept of “treating waste with waste”.展开更多
The freshly prepared water-wet amidoximated bacterial cellulose （Am-BC） serves as an effective nanoreactor to synthesis zinc oxide nanoparticles by in situ polyol method. The obtained ZnO/Am-BC nanocomposites have b...The freshly prepared water-wet amidoximated bacterial cellulose （Am-BC） serves as an effective nanoreactor to synthesis zinc oxide nanoparticles by in situ polyol method. The obtained ZnO/Am-BC nanocomposites have been characterized by field emission scanning electron microscopy （FE-SEM）, X-ray diffraction （XRD）, Fourier transformed infrared spectroscopy （FTIR） and thermogravimetric analysis （TGA）. The influence of the zinc acetate concentration on the morphologies and size ofZnO nanoparticles and the possible formation mechanism were discussed. The results indicated that uniform ZnO nanoparticles were homogeneously anchored on the Am-BC nanofibers through strong interaction between the hydroxyl and amino groups of Am-BC and ZnO nanoparticles. The loading content of ZnO nanoparticles is higher using Am-BC as a template than using the unmodified bacterial cellulose. The resultant nanocomposite synthesized at 0.05 wt% shows a high photocatalytic activity （92%） in the degradation of methyl orange.展开更多
The development of uranyl ion detection technology has exhibited its significance in public security and environmental fields for the radioactivity and chemical toxicity of uranyl ion.The WHO standard of uranyl ion ma...The development of uranyl ion detection technology has exhibited its significance in public security and environmental fields for the radioactivity and chemical toxicity of uranyl ion.The WHO standard of uranyl ion makes it necessary to develop highly sensitive uranyl rapid warning system in drinking water monitoring.Herein,a visualized rapid warning system for trace uranyl ion is carried out based on electrochemiluminescence(ECL) imaging technology to give an ultra-low limit of detection(LOD) and high selectivity.Amidoxime,a bi-functional group with both uranyl ion capturing and co-reactive functions,is modified on a conjugated polymer backbone with strong ECL signal to be prepared into three-in-one polymer nanoparticles(PNPs) with self-enhanced ECL property.The captured uranyl ion can enhance the ECL signal of PNPs via resonance energy transfer process to give the LOD as 0.5 ng/L,which is much lower than the known luminescent uranyl sensors.Furthermore,ECL imaging technology is introduced into realizing visualized uranyl rapid warning,and can be successfully applied on natural water samples.This study provides a novel strategy for uranyl rapid warning,and shows its potential meaning in public security and environmental fields.展开更多
Previous work suggested that amidoximed silica can be used as a highly efficient adsorbent for uranium removalfrom salt lake water. In this work, desorption of uranium from amidxoximed silica was investigated.Amidoxim...Previous work suggested that amidoximed silica can be used as a highly efficient adsorbent for uranium removalfrom salt lake water. In this work, desorption of uranium from amidxoximed silica was investigated.Amidoximed silica, which were loaded with uranium(VI) from salt lake water were used for desorption studies.0.1 mol / L of HNO3 Na2CO3, NaHCO3 and NaOH solution were used as desorbing solutions, respectively. The uranium desorbed into the solution was determined after shaking for certain time. Desorption efficiency wascalculated directly from the difference between the desorbed and absorbed uranium. The desorption ratio (%) wascalculated by the following equation:展开更多
Uranium concentration in salt lake brines is tens even thousands times higher than seawater, which makes salt lake brine being another ideal resource for uranium. However, the content of salt lake brine is very compli...Uranium concentration in salt lake brines is tens even thousands times higher than seawater, which makes salt lake brine being another ideal resource for uranium. However, the content of salt lake brine is very complicate, a large amount of K, Na, Ca, Mg elements coexisting with uranium. Hence, only sorbent with high uranium selectivity can be well used in uranium extraction from salt lake brine.展开更多
The aim is collecting uranium from groundwater in which uranium mainly exists in negative species,the amidoxime-functionalized hydrothermal carbon(AO-HTC)was synthesized.From the results of N2 adsorption-desorption an...The aim is collecting uranium from groundwater in which uranium mainly exists in negative species,the amidoxime-functionalized hydrothermal carbon(AO-HTC)was synthesized.From the results of N2 adsorption-desorption and SEM,AO-HTC is a small spherical surface;FT-IR and Elemental analysis showed that the amidoxime group was successfully grafted onto the surface of the material;Zeta-potential measurement showed that the amino nitrogen atom is protonated in the oxime group.The optimum pH value of AO-HTC for uranium adsorption is 6.0,and the adsorption equilibrium is reached within 80 min,which is in accordance with the pseudo-second order adsorption kinetic model.The adsorption of uranium by AO-HTC accords with the Langmuir isotherm adsorption model,and the single-layer saturated adsorption capacity is 254.13mg·g^-1.The thermodynamic parameters calculated by the adsorption isotherm indicate that AO-HTC adsorption of uranium is a spontaneous endothermic chemical process and Carbonate ion,calcium ion and humic acid concentration have great influence on uranium adsorption.The experiments results show that AO-HTC has the potential to elimination of U(Ⅳ)from groundwater.展开更多
Herein,a dendritic fibrous nanosilica(DFNS)-based adsorbent was constructed through bio-inspired bifunctional stimulation as a rapid and efficient trap for uranium(VI).Amino-amidoxime bifunctional polyacrylonitrile(AO...Herein,a dendritic fibrous nanosilica(DFNS)-based adsorbent was constructed through bio-inspired bifunctional stimulation as a rapid and efficient trap for uranium(VI).Amino-amidoxime bifunctional polyacrylonitrile(AOPNI-NH_(2))firmly adhered to the DFNS substrate through the polymerization of musselinspired dopamine(DA)with a large amount of amine and carbonyl groups.Meanwhile,the amine group of the introduced AOPNI-NH_(2)not only suppressed the ring-closing reaction of amidoxime groups to increase the active sites,but also improved their adsorption rate.The adsorption amount of U(VI)on asprepared DFNS/pDA/AOPNI-NH_(2)reached q_(m)=678 mg g^(-1),which represented a 118%increase compared with the original DFNS under the same conditions.Finally,the adsorption capacity demonstrated the potential for the application of this adsorbent in a seawater environment.展开更多
Photocatalytic uranium reduction has been proposed as an effective method for treating nuclear wastewater due to its advantages of cleanliness,energy efficiency,and convenience in application.In this study,a Z-scheme ...Photocatalytic uranium reduction has been proposed as an effective method for treating nuclear wastewater due to its advantages of cleanliness,energy efficiency,and convenience in application.In this study,a Z-scheme heterojunction,ZnCdS-P_(2)W_(12)Fe_(9)AO,was designed and synthesized for achieving efficient uranium reduction via an adsorption–photoreduction synergistic strategy.DFT calculation results demonstrated that polyoxometalates modified with amidoxime groups exhibited exceptional uranium adsorption performance.The construction of the Z-scheme heterojunction enhanced visible light absorption,facilitated electron transfer,and promoted the separation of photogenerated electrons and holes.Finally,ZnCdS-P_(2)W_(12)Fe_(9)AO achieved a uranium removal rate of 97.7%(610.6 mg g^(−1) under light irradiation)without the addition of any sacrificial agent.Meanwhile,ZnCdS-P_(2)W_(12)Fe_(9)AO maintained good stability and reusability.This study offers new insights and perspectives for advancing research on photocatalytic uranium reduction.展开更多
Amidoxime-functionalized polymeric adsorbents have attracted great interest for uranium extraction from seawater.However,the current graft polymerization method is time-consuming(2–6 h),wasteful in reagent,and hence ...Amidoxime-functionalized polymeric adsorbents have attracted great interest for uranium extraction from seawater.However,the current graft polymerization method is time-consuming(2–6 h),wasteful in reagent,and hence not economical.Here,amidoxime-functionalized adsorbents based on low-cost polypropylene melt-blown nonwoven fabric(MBF)are produced by a simple,fast and also low-cost surface photografting technology,by which more than 80%of reagents can be saved and grafting time can be reduced to 3 min.The fabricated adsorbents retain their mechanical properties and exhibit excellent uranium adsorption properties,with a maximum uranium adsorption capacity of 400 mg g-1 when the monomer ratio of AN to AA is 8:2.Moreover,we showed that the adsorbents could be either reused or simply incinerated for uranium recovery.The photografting technology has great potential for low-cost,continuous industrial production of uranium-adsorbing material.展开更多
Extraction of uranium from seawater offers a sustainable approach for nuclear fuel supply.Poly(amidoxime)(PAO)adsorbents have emerged as a highly promising extraction approach.However,there are still challenges that h...Extraction of uranium from seawater offers a sustainable approach for nuclear fuel supply.Poly(amidoxime)(PAO)adsorbents have emerged as a highly promising extraction approach.However,there are still challenges that hinder the practical application of PAO-based adsorbents in considering the extraction performance and durability.To address these challenges,we developed a mechanically robust PAO/polyvinyl alcohol(PAO/PVA)composite superspreading membrane(SSPP)via Marangoni effect-driven interfacial self-assembly.This strategy constructs hierarchically porous structures with gradient pore sizes,promoting efficient ion transport and access to functional adsorption sites.The PVA integration enhances hydrophilicity and forms a hydrogen-bonded network that prevents structural shrinkage,while boosting mechanical strength,making the adsorbent more suitable for practical use.Consequently,the optimized membrane achieves a high uranium adsorption capacity of 7.42 mg g^(-1) in natural seawater within 10 days.This work provides an interfacial self-assembly strategy for advanced extraction membranes and demonstrates significant potential for sustainable uranium extraction from seawater.展开更多
Uranium plays a pivotal role in nuclear energy production, and extracting it from seawater offers a promising solution to alleviate shortages in land-based uranium resources. However, the marine environment with ultra...Uranium plays a pivotal role in nuclear energy production, and extracting it from seawater offers a promising solution to alleviate shortages in land-based uranium resources. However, the marine environment with ultra-low uranium concentrations, high salinity, and microbial activity poses significant extraction challenges, compounded by selectivity and cost limitations in current methods. In the present investigation, an anti-biofouling amino oximefunctionalized collagen/sodium alginate aerogel(CF-AO/SA) was fabricated using leather waste-derived collagen. The dual cross-linked CF-AO/SA network, enhanced by Zn2+incorporation, showed improved structural stability and antibacterial properties, as well as high uranium adsorption capacity, selectivity, and reusability. It achieved 320.7 mg g-1in 14 ppm uranium solution and maintained 78.6% removal efficiency after five cycles. Additionally, the removal rate of uranium was 89% in simulated seawater. Field tests in Zhuhai's Jinwan District(113.35° E, 21.99° N) showed 5.16 mg g-1uranium adsorption and excellent mechanical strength after 30 days in seawater. Furthermore, the production cost of CF-AO/SA was estimated at $3.652 per kilogram, which is lower than other reported adsorbents. The newly developed bio-based aerogel beads have substantial potential for practical applications for uranium capture in seawater and provide a novel high-value utilization way for leather wastes.展开更多
Uranium extraction from seawater is of strategic significance for nuclear power generation.Amidoximebased functional adsorbents play indispensable roles in the recovery of seawater uranium with high efficiency.Neverth...Uranium extraction from seawater is of strategic significance for nuclear power generation.Amidoximebased functional adsorbents play indispensable roles in the recovery of seawater uranium with high efficiency.Nevertheless,balancing the adsorption capacity and selectivity is challenging in the presence of complicated interfering ions especially vanadium.Herein,a polyarylether-based covalent organic framework functionalized with open-chain amidoxime(COF-HHTF-AO)was synthesized with remarkable chemical stability and excellent crystallinity.Impressively,the adsorption capacity of COF-HHTF-AO towards uranium in natural seawater reached up to 5.12 mg/g,which is 1.61 times higher than that for vanadium.Detailed computational calculations revealed that the higher selectivity for uranium over vanadium originated from the specific bonding nature and coordination pattern with amidoxime.Combining enhanced adsorption capacity,excellent selectivity and ultrahigh stability,COF-HHTF-AO serves as a promising adsorbent for uranium extraction from the natural seawater.展开更多
基金partially supported by the National Natural Science Foundation of China(22475035 and 22071021)the Natural Science Foundation of Jilin Province(20240101170JC)。
文摘Zinc-iodine batteries have received significant attention due to their high theoretical capacity and environmental friendliness,but their performance is restricted by the growth of zinc dendrites,the hydrogen evolution reaction,and the shuttling effect of polyiodide ions.In this study,an amidoximefunctionalized hydrogel electrolyte,created by amidoximated porous polymer of intrinsic microporosity(AO-PIM-1)and sodium alginate(Alg),is designed to address the aforementioned problems through synergistically optimizing the interfaces of the zinc anode and iodine cathode.The rigid microporous framework and amidoxime groups of AO-PIM-1 can repel polyiodides and inhibit their shuttle effect.Meanwhile,the polyanionic properties of Alg guide the uniform deposition of Zn^(2+)along the(002)crystal plane through the“egg-box”structure,thus suppressing the formation of dendrites.The AO-PIM-1/Alg electrolyte has a high ionic conductivity(18.6 mS cm^(-1)).The assembled symmetric battery can achieve highly reversible dendrite-free zinc plating/stripping(stably cycling for 2550 h at 1 mA cm^(-2)).The Zn-I_(2) full battery with the AO-PIM-1/Alg electrolyte has a long lifespan of 8700 cycles at 0.5 A g^(-1).The working mechanism of the electrolyte was elucidated through density functional theoretical calculations and molecular dynamics simulations.This study provides a new strategy for the hydrogel electrolyte of ZnI_(2) batteries.
基金supported by the Opening Project of the Jiangsu Province Engineering Research Center of Agricultural Breeding Pollution Control and Resource(Grant No.2021ABPCR010)the Natural Science Research Project of Jiangsu Higher Education Institutions of China(Grants No.20KJB150035,21KJD610004,and 21KJA530004).
文摘Removal of uranium(VI)from nuclear wastewater is urgent due to the global nuclear energy exploitation.This study synthesized novel sponge-like 3D porous materials for enhanced uranium adsorption by combining electrospinning and fibrous freeze-shaping techniques.The materials possessed an organic-inorganic hybrid architecture based on the electrospun fibers of polyacrylonitrile(PAN)and SiO_(2).As a sup-porting material,the surface of fibrous SiO_(2) could be further functionalized by cyano groups via(3-cyanopropyl)triethoxysilane.All the cyano groups were turned into amidoxime(AO)groups to obtain a amidoxime-functionalized sponge(PAO/SiO_(2)-AO)through the subsequent ami-doximation process.The proposed sponge exhibited enhanced uranium adsorption performance with a high removal capacity of 367.12 mg/g,a large adsorption coefficient of 4.0×10^(4)mL/g,and a high removal efficiency of 97.59%.The UO_(2)^(2+)adsorption kinetics perfectly conformed to the pseudo-second-order reaction.The sorbent also exhibited an excellent selectivity for UO_(2)^(2+) with other interfering metal ions.2023 Hohai University.Production and hosting by Elsevier B.V.
基金supported by the National Natural Science Foundation of China(Nos.21676291,21306220,11275252,11305243 and11405249)in part supported by the "Knowledge Innovation Program of Chinese academy of sciences"
文摘An amidoxime-based polymeric adsorbent was prepared by pre-irradiation grafting of acrylonitrile and acrylic acid onto high-density polyethylene fibers using electron beams,followed by amidoximation.Quantitative recovery of uranium was investigated by flow-through experiment using simulated seawater and marine test in natural seawater.The maximum amount of uranium uptake was 2.51 mg/g-ads after 42 days of contact with simulated seawater and 0.13 mg/g-ads for 15 days of contact with natural seawater.A lower uranium uptake in marine test can be attributed to the short adsorption time and the contamination of marine microorganisms and iron.However,the high selectivity toward uranium against vanadium may be beneficial to harvest uranyl ion onto adsorbents and the economic feasibility for recovery of uranium from seawater.
基金supported by the National Natural Science Foundation of China(Nos.U1732151 and 21676291)Strategic Pilot and Technology Special Funds of the Chinese Academy of Science(No.XDA02030200)
文摘A novel amidoxime-based fibrous adsorbent,denoted as PE/PP-g-(PAAc-co-PAO), was prepared by preirradiation grafting of acrylic acid and acrylonitrile onto polyethylene-coated polypropylene skin-core(PE/PP)fibers using 60 Co γ-ray irradiation, followed by amidoximation. The original and modified PE/PP fibers were characterized by a series of characterization methods to demonstrate the attachment of amidoxime groups onto the PE/PP fibers. Breaking strength tests confirmed that the fibrous adsorbent could maintain good mechanical properties. The adsorption capacity of the PE/PP-g-(PAAc-coPAO) fibers was investigated in simulated seawater with an initial uranium concentration of 330 μg/L. The uranium adsorption capacity was 2.27 mg/g-adsorbent after 24 h in simulated seawater, and the equilibrium data were well described by the Freundlich isotherm model. The PE/PP-g-(PAAc-co-PAO) adsorbent exhibited good regeneration and recyclability during five adsorption-desorption cycles.The adsorption test was also performed in simulated radioactive effluents with uranium concentrations of 10 and100 μg/L. The effect of the pH value on the adsorption capacity was also studied. At a very low initial concentration 10 μg/L solution, the PE/PP-g-(PAAc-co-PAO)fiber could remove as much as 93.0% of the uranium, and up to 71.2% of the uranium in the simulated radioactive effluent. These results indicated that the PE/PP-g-(PAAcco-PAO) adsorbent could be used in radioactive effluents over a wide range of pH values. Therefore, the PE/PP-g-(PAAc-co-PAO) fibers, with their high uranium selectivity,good regeneration and recyclability,good mechanical properties, and low cost, are promising adsorbents for extracting uranium from aqueous solutions.
基金Project supported by the Science and Technology Development Foundation of China Academy of Engineering Physics （Grant No. 2011A0301003）.
文摘Uranyl （VI） amidoxime complexes are investigated using relativistic density functional theory. The equilibrium structures, bond orders, and Mulliken populations of the complexes have been systematically investigated under a generalized gradient approximation （GGA）. Comparison of （acet） uranyl amidoxime complexes （[UO2（AO）n]2-n, 1≤ n≤4） with available experimental data shows an excellent agreement. In addition, the U-O（1）, U-O（3）, C（1）-N（2）, and C（3） N（4） bond lengths of [UO2（CH3AO）4]2- are longer than experimental data by about 0.088, 0.05, 0.1, and 0.056 A. The angles of N（3） O（3）-U, O（2）-N（1）-C（1）, N（3）-C（3）-N（4）, N（4）-C（3） C（4）, and C（4）-C（3）-N（3） are different from each other, which is due to existing interaction between oxygen in uranyl and hydrogen in amino group. This interaction is found to be intra-molecular hydrogen bond. Studies on the bond orders, Mulliken charges, and Mulliken populations demonstrate that uranyl oxo group functions as hydrogen-bond acceptors and H atoms in ligands act as hydrogen-bond donors forming hydrogen bonds within the complex.
基金supported by the Fundamental Research Funds for the Central Universities of Central South University(10400506021718)Hunan Provincial Science and Technology Project(2018TP1003).
文摘An affinity membrane was prepared by coaxial electrospinning and amidoxime(AONFA),and it was applied to selectively recovery Au(Ⅲ)from an aqueous solution.The static adsorption results showed that,when p H at 5,the maximum adsorption capacity of AONFA membrane for Au(Ⅲ)was 509.3 mg·g^(-1).AONFA membrane exhibit much higher affinity and selectivity towards Au(Ⅲ)than other metal cations.The membrane could be regenerated effectively by mixture solution of thiourea and HCl,and the desorption ratio reached almost 100%after 4 hours desorption.The dead-end filtration results showed that,the membrane utilization efficiency and adsorption capacity can be improved by increasing the flow rate,while increasing the concentration shorted the breakthrough process and had little impact to adsorption capacity.We can flexibly adjust the flow rate and concentration according to the situation to obtain the maximum utilization efficiency of the membrane in filtration process.The dynamic adsorption capacity is higher than the static adsorption capacity.The adsorption mechanism for Au(Ⅲ)is electrostatic adsorption and reduction.Thus,AONFA membrane filtration was demonstrated to be a promising method for continuous recover Au(Ⅲ)from wastewater.
基金financially supported by the Universiti Malaysia Sabah (No. SBK0260-ST-2016)
文摘A well-known adsorbent, poly(amidoxime)ligand, was prepared from polyacrylonitrile(PAN) grafted kenaf cellulose, and subsequent characterization was performed by Fourier transform infrared spectroscopy(FTIR),field emission scanning electron microscope(FESEM) and inductively coupled plasma mass spectrometry(ICP-MS).The adsorption capacities of the prepared ligand for rare earth metals are found to be excellent, with adsorptions of La^(3+), Ce^(3+), Pr^(3+), Gd^(3+) and Nd^(3+) experimentally determined to be 262, 255, 244, 241 and 233 mg·g^(-1), respectively, at pH 6. The experimental values of the adsorption of rare earth metals are well matched with the pseudosecond-order rate equation. The reusability of the adsorbent is examined for seven cycles of sorption/desorption,demonstrating that the proposed adsorbent could be reused for over seven cycles without any significant loss in the original removal capability of the ligand.
基金supported by the National Natural Science Foundation of China(Nos.11675247,22176194).
文摘Direct collection of uranium from low uranium systems via adsorption remains challenging.Fibrous sorbent materials with amidoxime(AO)groups are promising adsorbents for uranium extraction from seawater.However,low AO adsorption group utilization remains an issue.We herein fabricated a branched structure containing AO groups on polypropylene/polyethylene spun-laced nonwoven(PP/PE SNW)fibers using grafting polymerization induced by radiation(RIGP)to improve AO utilization.The chemical structures,thermal properties,and surface morphologies of the raw and treated PP/PE SNW fibers were studied.The results show that an adsorptive functional layer with a branching structure was successfully anchored to the fiber surface.The adsorption properties were investigated using batch adsorption experiments in simulated seawater with an initial uranium concentration of 500μg·L^(−1)(pH 4,25℃).The maximum adsorption capacity of the adsorbent material was 137.3 mg·g^(−1)within 24 h;moreover,the uranyl removal reached 96%within 240 min.The adsorbent had an AO utilization rate of 1/3.5 and was stable over a pH range of 4–10,with good selectivity and reusability,demonstrating its potential for seawater uranium extraction.
基金supported by the National Natural Science Foundation of China (No.52364022)the Natural Science Foundation of Guangxi Province,China (Nos.2023JJA160192 and 2021GXNSFAA220096)+1 种基金the Guangxi Science and Technology Major Project,China (No.AA23073018)the Guangxi Chongzuo Science and Technology Plan,China (No.2023ZY00503).
文摘With the application of resins in various fields, numerous waste resins that are difficult to treat have been produced. The industrial wastewater containing Cr(Ⅵ) has severely polluted soil and groundwater environments, thereby endangering human health. Therefore, in this paper, a novel functionalized mesoporous adsorbent PPR-Z was synthesized from waste amidoxime resin for adsorbing Cr(Ⅵ). The waste amidoxime resin was first modified with H3PO4 and ZnCl_(2), and subsequently, it was carbonized through slow thermal decomposition. The static adsorption of PPR-Z conforms to the pseudo-second-order kinetic model and Langmuir isotherm, indicating that the Cr(Ⅵ) adsorption by PPR-Z is mostly chemical adsorption and exhibits single-layer adsorption. The saturated adsorption capacity of the adsorbent for Cr(Ⅵ) could reach 255.86 mg/g. The adsorbent could effectively reduce Cr(Ⅵ) to Cr(Ⅲ) and decrease the toxicity of Cr(Ⅵ) during adsorption. PPR-Z exhibited Cr(Ⅵ) selectivity in electroplating wastewater. The main mechanisms involved in the Cr(Ⅵ) adsorption are the chemical reduction of Cr(Ⅵ) into Cr(Ⅲ) and electrostatic and coordination interactions. Preparation of PPR-Z not only solves the problem of waste resin treatment but also effectively controls Cr(Ⅵ) pollution and realizes the concept of “treating waste with waste”.
基金financially supported by the Program of Introducing Talents of Discipline to Universities(B07024)Shanghai Leading Academic Discipline Project(B603)+1 种基金The National Natural Science Foundation of China(No.51273043)Project of the Action on Scientists and Engineers to Serve Enterprises(2009GJE20016)
文摘The freshly prepared water-wet amidoximated bacterial cellulose （Am-BC） serves as an effective nanoreactor to synthesis zinc oxide nanoparticles by in situ polyol method. The obtained ZnO/Am-BC nanocomposites have been characterized by field emission scanning electron microscopy （FE-SEM）, X-ray diffraction （XRD）, Fourier transformed infrared spectroscopy （FTIR） and thermogravimetric analysis （TGA）. The influence of the zinc acetate concentration on the morphologies and size ofZnO nanoparticles and the possible formation mechanism were discussed. The results indicated that uniform ZnO nanoparticles were homogeneously anchored on the Am-BC nanofibers through strong interaction between the hydroxyl and amino groups of Am-BC and ZnO nanoparticles. The loading content of ZnO nanoparticles is higher using Am-BC as a template than using the unmodified bacterial cellulose. The resultant nanocomposite synthesized at 0.05 wt% shows a high photocatalytic activity （92%） in the degradation of methyl orange.
基金financially supported by the National Natural Science Foundation of China (Nos. U1867206, 21906115)State Key Laboratory of Analytical Chemistry for Life Science (No. SKLACLS2014)+1 种基金the China Postdoctoral Science Foundation (No. 2020T130456)the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)。
文摘The development of uranyl ion detection technology has exhibited its significance in public security and environmental fields for the radioactivity and chemical toxicity of uranyl ion.The WHO standard of uranyl ion makes it necessary to develop highly sensitive uranyl rapid warning system in drinking water monitoring.Herein,a visualized rapid warning system for trace uranyl ion is carried out based on electrochemiluminescence(ECL) imaging technology to give an ultra-low limit of detection(LOD) and high selectivity.Amidoxime,a bi-functional group with both uranyl ion capturing and co-reactive functions,is modified on a conjugated polymer backbone with strong ECL signal to be prepared into three-in-one polymer nanoparticles(PNPs) with self-enhanced ECL property.The captured uranyl ion can enhance the ECL signal of PNPs via resonance energy transfer process to give the LOD as 0.5 ng/L,which is much lower than the known luminescent uranyl sensors.Furthermore,ECL imaging technology is introduced into realizing visualized uranyl rapid warning,and can be successfully applied on natural water samples.This study provides a novel strategy for uranyl rapid warning,and shows its potential meaning in public security and environmental fields.
文摘Previous work suggested that amidoximed silica can be used as a highly efficient adsorbent for uranium removalfrom salt lake water. In this work, desorption of uranium from amidxoximed silica was investigated.Amidoximed silica, which were loaded with uranium(VI) from salt lake water were used for desorption studies.0.1 mol / L of HNO3 Na2CO3, NaHCO3 and NaOH solution were used as desorbing solutions, respectively. The uranium desorbed into the solution was determined after shaking for certain time. Desorption efficiency wascalculated directly from the difference between the desorbed and absorbed uranium. The desorption ratio (%) wascalculated by the following equation:
文摘Uranium concentration in salt lake brines is tens even thousands times higher than seawater, which makes salt lake brine being another ideal resource for uranium. However, the content of salt lake brine is very complicate, a large amount of K, Na, Ca, Mg elements coexisting with uranium. Hence, only sorbent with high uranium selectivity can be well used in uranium extraction from salt lake brine.
基金This work was financially supported by the National Natural Science Foundation of China(21561002,21866004,21866003).
文摘The aim is collecting uranium from groundwater in which uranium mainly exists in negative species,the amidoxime-functionalized hydrothermal carbon(AO-HTC)was synthesized.From the results of N2 adsorption-desorption and SEM,AO-HTC is a small spherical surface;FT-IR and Elemental analysis showed that the amidoxime group was successfully grafted onto the surface of the material;Zeta-potential measurement showed that the amino nitrogen atom is protonated in the oxime group.The optimum pH value of AO-HTC for uranium adsorption is 6.0,and the adsorption equilibrium is reached within 80 min,which is in accordance with the pseudo-second order adsorption kinetic model.The adsorption of uranium by AO-HTC accords with the Langmuir isotherm adsorption model,and the single-layer saturated adsorption capacity is 254.13mg·g^-1.The thermodynamic parameters calculated by the adsorption isotherm indicate that AO-HTC adsorption of uranium is a spontaneous endothermic chemical process and Carbonate ion,calcium ion and humic acid concentration have great influence on uranium adsorption.The experiments results show that AO-HTC has the potential to elimination of U(Ⅳ)from groundwater.
基金National Natural Science Foundation of China[NSFC 51872057]Application Technology Research and Development Plan of Heilongjiang Province[GX16A009]+1 种基金Fundamental Research Funds of the Central University[HEUCFZ]Natural Science Foundation of Heilongjiang Province[QC2018010]。
文摘Herein,a dendritic fibrous nanosilica(DFNS)-based adsorbent was constructed through bio-inspired bifunctional stimulation as a rapid and efficient trap for uranium(VI).Amino-amidoxime bifunctional polyacrylonitrile(AOPNI-NH_(2))firmly adhered to the DFNS substrate through the polymerization of musselinspired dopamine(DA)with a large amount of amine and carbonyl groups.Meanwhile,the amine group of the introduced AOPNI-NH_(2)not only suppressed the ring-closing reaction of amidoxime groups to increase the active sites,but also improved their adsorption rate.The adsorption amount of U(VI)on asprepared DFNS/pDA/AOPNI-NH_(2)reached q_(m)=678 mg g^(-1),which represented a 118%increase compared with the original DFNS under the same conditions.Finally,the adsorption capacity demonstrated the potential for the application of this adsorbent in a seawater environment.
基金supported by the Natural Science Foundation of China(Grant No.22071018)the Natural Science Foundation of Jilin Province(No.20220101069JC).
文摘Photocatalytic uranium reduction has been proposed as an effective method for treating nuclear wastewater due to its advantages of cleanliness,energy efficiency,and convenience in application.In this study,a Z-scheme heterojunction,ZnCdS-P_(2)W_(12)Fe_(9)AO,was designed and synthesized for achieving efficient uranium reduction via an adsorption–photoreduction synergistic strategy.DFT calculation results demonstrated that polyoxometalates modified with amidoxime groups exhibited exceptional uranium adsorption performance.The construction of the Z-scheme heterojunction enhanced visible light absorption,facilitated electron transfer,and promoted the separation of photogenerated electrons and holes.Finally,ZnCdS-P_(2)W_(12)Fe_(9)AO achieved a uranium removal rate of 97.7%(610.6 mg g^(−1) under light irradiation)without the addition of any sacrificial agent.Meanwhile,ZnCdS-P_(2)W_(12)Fe_(9)AO maintained good stability and reusability.This study offers new insights and perspectives for advancing research on photocatalytic uranium reduction.
基金supported by internal funds from Tsinghua University.
文摘Amidoxime-functionalized polymeric adsorbents have attracted great interest for uranium extraction from seawater.However,the current graft polymerization method is time-consuming(2–6 h),wasteful in reagent,and hence not economical.Here,amidoxime-functionalized adsorbents based on low-cost polypropylene melt-blown nonwoven fabric(MBF)are produced by a simple,fast and also low-cost surface photografting technology,by which more than 80%of reagents can be saved and grafting time can be reduced to 3 min.The fabricated adsorbents retain their mechanical properties and exhibit excellent uranium adsorption properties,with a maximum uranium adsorption capacity of 400 mg g-1 when the monomer ratio of AN to AA is 8:2.Moreover,we showed that the adsorbents could be either reused or simply incinerated for uranium recovery.The photografting technology has great potential for low-cost,continuous industrial production of uranium-adsorbing material.
基金supported by the Nuclear Technology R&D Program,the specific research fund of the Innovation Platform for Academicians of Hainan Province(YSPTZX202316)the National Natural Science Foundation of China(U2167220,22327807,U23A20104)+1 种基金the Innovation Fund for Scientific and Technological Personnel of Hainan Province(KJRC2023B01)the Hainan Province Science and Technology Special Fund(ZDYF2024SHFZ066).
文摘Extraction of uranium from seawater offers a sustainable approach for nuclear fuel supply.Poly(amidoxime)(PAO)adsorbents have emerged as a highly promising extraction approach.However,there are still challenges that hinder the practical application of PAO-based adsorbents in considering the extraction performance and durability.To address these challenges,we developed a mechanically robust PAO/polyvinyl alcohol(PAO/PVA)composite superspreading membrane(SSPP)via Marangoni effect-driven interfacial self-assembly.This strategy constructs hierarchically porous structures with gradient pore sizes,promoting efficient ion transport and access to functional adsorption sites.The PVA integration enhances hydrophilicity and forms a hydrogen-bonded network that prevents structural shrinkage,while boosting mechanical strength,making the adsorbent more suitable for practical use.Consequently,the optimized membrane achieves a high uranium adsorption capacity of 7.42 mg g^(-1) in natural seawater within 10 days.This work provides an interfacial self-assembly strategy for advanced extraction membranes and demonstrates significant potential for sustainable uranium extraction from seawater.
基金funded by National Natural Science Foundation of China(52273268)Qin Chuangyuan Team Construction Project of Shaanxi Science and Technology Department(2022KXJ-165)+2 种基金Shaanxi Province Technology Innovation Guidance Project(2023GXLH-079)Open Foundation of Key Laboratory of Auxiliary Chemistry and Technology for Chemical Industry,Ministry of Education,Shaanxi University of Science and Technology(KFKT2022-07)Shaanxi Province Outstanding Youth Science Foundation Project(2025JC-JCQN-053).
文摘Uranium plays a pivotal role in nuclear energy production, and extracting it from seawater offers a promising solution to alleviate shortages in land-based uranium resources. However, the marine environment with ultra-low uranium concentrations, high salinity, and microbial activity poses significant extraction challenges, compounded by selectivity and cost limitations in current methods. In the present investigation, an anti-biofouling amino oximefunctionalized collagen/sodium alginate aerogel(CF-AO/SA) was fabricated using leather waste-derived collagen. The dual cross-linked CF-AO/SA network, enhanced by Zn2+incorporation, showed improved structural stability and antibacterial properties, as well as high uranium adsorption capacity, selectivity, and reusability. It achieved 320.7 mg g-1in 14 ppm uranium solution and maintained 78.6% removal efficiency after five cycles. Additionally, the removal rate of uranium was 89% in simulated seawater. Field tests in Zhuhai's Jinwan District(113.35° E, 21.99° N) showed 5.16 mg g-1uranium adsorption and excellent mechanical strength after 30 days in seawater. Furthermore, the production cost of CF-AO/SA was estimated at $3.652 per kilogram, which is lower than other reported adsorbents. The newly developed bio-based aerogel beads have substantial potential for practical applications for uranium capture in seawater and provide a novel high-value utilization way for leather wastes.
基金supported by the Science Challenge Project(TZ2016004)the National Natural Key Research and Development Program of China(2018YFC1900105 and 2017YFA0207002)Beijing Outstanding Young Scientist Program。
文摘Uranium extraction from seawater is of strategic significance for nuclear power generation.Amidoximebased functional adsorbents play indispensable roles in the recovery of seawater uranium with high efficiency.Nevertheless,balancing the adsorption capacity and selectivity is challenging in the presence of complicated interfering ions especially vanadium.Herein,a polyarylether-based covalent organic framework functionalized with open-chain amidoxime(COF-HHTF-AO)was synthesized with remarkable chemical stability and excellent crystallinity.Impressively,the adsorption capacity of COF-HHTF-AO towards uranium in natural seawater reached up to 5.12 mg/g,which is 1.61 times higher than that for vanadium.Detailed computational calculations revealed that the higher selectivity for uranium over vanadium originated from the specific bonding nature and coordination pattern with amidoxime.Combining enhanced adsorption capacity,excellent selectivity and ultrahigh stability,COF-HHTF-AO serves as a promising adsorbent for uranium extraction from the natural seawater.
