Carbonaceous debris(CD) is widely disseminated within sandstones in the Shuanglong uranium deposit,southern Ordos Basin,and is the dominant enrichment agent for uranium precipitation.The occurrence and chemical compos...Carbonaceous debris(CD) is widely disseminated within sandstones in the Shuanglong uranium deposit,southern Ordos Basin,and is the dominant enrichment agent for uranium precipitation.The occurrence and chemical composition of uranium minerals within CD were investigated by using scanning electron microscope and electron microprobe analyses.The results show that uranium minerals mostly occur in cell pores in the forms of fructus aurantia and concentric band structure.Pitchblende and coffinite are the main uranium minerals,and the former is dominant.According to the crystal morphology and composition of trace elements of uranium minerals,uranium precipitation on the pores is grouped into two periods,orderly Ⅰ,Ⅱ.Moreover,the Ⅰ period is further divided into two sub-period,orderly Ⅰ1,Ⅰ2.Moreover,askew sphere uranium minerals could indicate fluid migration.Under certain geological environment condition,uranium is unevenly adsorbed on the surface of the pore by the Van der Waals(i.e.,Ⅰ1 period),and then is precipitated towards to the center of the pore until the whole pore is filled up with uranium minerals by complicated process such as microorganism activities(i.e.,Ⅰ2,Ⅱ period).It will provide some guidance for studying the metallogenic environment and genesis of sandstone-type uranium deposit.展开更多
The article is devoted to the problems of the influence of global processes of Great Oxygenation Event of the Earth’s atmosphere on the genesis of Proterozoic unconformity-type uranium deposits in the Canadian sedime...The article is devoted to the problems of the influence of global processes of Great Oxygenation Event of the Earth’s atmosphere on the genesis of Proterozoic unconformity-type uranium deposits in the Canadian sedimentary Athabasca basin,which are the most prominent representatives of large-scale uranium deposits with uniquely rich ores with uranium content up to a few tens of percentages in the world.The influence of the formation of an oxygen atmosphere on the process of ore formation is considered with a comparative analysis of single-stage and multi-stage models of the formation of unconformity uranium deposits.The appearance of free oxygen in the Earth’s atmosphere,necessary for the formation of the unconformity deposits,occurred approximately 2.5-2.0 billion years ago during the Great Oxygenation Event(GOE).The Great Oxidation Event caused the atmosphere to form high levels of oxygen,leading to the production of more primary biological matter on the early Earth,thereby forming more organic-rich sediments,which played an important role in U-mineralization of Proterozoic unconformity-related uranium deposits.The formation of the Athabasca basin began approximately 1740 Ma ago.Uranium mineralization in the deposits occurred 1590 Ma ago.This was followed by a series of putative post-ore events with rejuvenated ages from 1525 to 1000-950 Ma,which in the single-stage deposit formation model were interpreted as re precipitation of primary ore mineralization with the formation of the deposits’ore resource from both of its main sources:the mobilization of uranium from uranium-bearing minerals of the Athabasca Group sandstones and from the basement rocks of the basin.We adopted an alternative genetic model the way from their source to the basin reservoirs,which formed the resource of primary uranium of the initial stage,and 2)initially barren(after the depletion of the ore reserve of the Athabasca sandstones on basin fluids that leached uranium from uranium-bearing especially organic of multi-stage deposit formation with two spatially and temporally separated uranium sources:1)ore-forming basin brines of the Athabasca sandstones with an initially elevated uranium content during its mobilization from uranium-bearing rocks along the brine migration route on rocks of the basin basement with the formation of an‘additional’uranium resource at subsequent stages with a rejuvenated ages.The deposition of primary uranium of the initial stage and‘additional’uranium occurred in structural traps localizing the initial stage uranium,with a concomitant increase in the total reserves and ore grades of the deposits.After the depletion of the‘additional’uranium in the basement available for mobilization,the formation of the ore resource of the deposits was completed.We adopted this conclusion as a hypothesis for a possible interpretation of the mechanism for the final completion of the geological history of the Athabasca basin deposits in the Mesoproterozoic Era,1600-1000 Ma ago.展开更多
The Mianhuakeng uranium deposit,characterized by uranium-rich granite,serves as a key site for research into crustal radioactive heating.Based on 45 rock samples,this study reviews that the host granite in the Mianhua...The Mianhuakeng uranium deposit,characterized by uranium-rich granite,serves as a key site for research into crustal radioactive heating.Based on 45 rock samples,this study reviews that the host granite in the Mianhuakeng uranium deposit has a high radioactive heat production rate(avg.5.50μW/m³)and a low Th/U ratio(avg.2.62).Uranium-rich granite and its alteration zone within the upper crust(0-5 km depth)contribute about 45%of the total radioactive heat production,wich is crucial for controlling geothermal resource distribution.For uranium-thermal at tectonic plate margins,a symbiotic geological model was proposed:Firstly,subduction of the Pacific Plate caused upwelling of the asthenosphere,generating a high heat-flow background.Secondly,heat transfer is enhanced by major faults such as the Youdong and Mianhuakeng faults.Subsequently,uranium was mobilized,transported,and enriched within the granite through deep siliceous hydrothermal activity and associated alteration.Ultimately,the uranium enrichment in granite leads to increased radioactive heat production,resulting in local thermal anomalies.This model provides a theoretical support for exploring and developing uranium-thermal symbiotic resources in South China.展开更多
Studies on the phytotoxicity of cadmium(Cd)and uranium(U)in rice mainly focus on single exposure.However,water,soil,and other environmental media are always co-contaminated by Cd and U.The effects of Cd(5 mg/L)and U(1...Studies on the phytotoxicity of cadmium(Cd)and uranium(U)in rice mainly focus on single exposure.However,water,soil,and other environmental media are always co-contaminated by Cd and U.The effects of Cd(5 mg/L)and U(10 mg/L)single and combined exposure for 7 days on rice seedlings were explored by hydroponic experiment.The synergism of U and Cd intensified the inhibitory effect of combined exposure on the rice seedling’s growth,accompanied by a remarkable reduction in chlorophyll content,alterations in antioxidant capacity,imbalances in mineral element metabolism,lipid peroxidation-induced destruction observed in rice seedlings,and significantly regulated expression of OsNramp5,OsHMA3,and OsHMA2,the adverse effects on the roots were more severe compared to those on the shoots.Combined exposure of U and Cd altered the distribution of U and Cd in the rice plant and subcellular.The accumulation of U and Cd in the rice seedlings’roots observably exceeded the shoot.Cd is mainly isolated in the vacuole and cell wall;U is primarily trapped in the cell wall.Cd promoted U accumulation in rice seedlings,while U inhibited Cd accumulation in rice seedlings.These findings can not only expand the understanding of the phytotoxicity of heavy metal combined exposure but also have important theoretical and practical significance for evaluating and remedying heavy metals contaminated-paddy soil and ensure for safe production of rice.展开更多
Composite systems of soil organic matter and iron hydroxides hold significant potential for the remediation of heavy metal pollution.However,the synergistic immobilization mechanisms of U(Ⅵ)by humin(HM)—iron hydroxi...Composite systems of soil organic matter and iron hydroxides hold significant potential for the remediation of heavy metal pollution.However,the synergistic immobilization mechanisms of U(Ⅵ)by humin(HM)—iron hydroxide composites remain insufficiently understood.In this study,goethite(Ge)—HM and magnetite(Mag)—HM composites with varying C-to-Fe molar ratios were synthesized via co-precipitation,and their adsorption behavior and underlying mechanisms towards U(Ⅵ)in aqueous solutions were systematically investigated.The results showed that under conditions of a pH value of 5.0 and temperature of 298 K,the maximum U(Ⅵ)adsorption capacities of Ge—HM and Mag—HM reached 60.56 mg/g and 64.12 mg/g,respectively,significantly surpassing those of pure Ge(39.6 mg/g),Mag(22.5 mg/g),and HM(20.2 mg/g).Kinetic studies revealed that the adsorption processes for both Ge—HM and Mag—HM conformed to the pseudo-second-order kinetic model,indicating chemical reaction control.Isothermal adsorption results were well described by the Langmuir model,suggesting monolayer adsorption on the composite surfaces.Crucially,characterization results elucidated distinct reaction mechanisms.Fourier transform infrared spectroscopy(FTIR)and X-ray photoelectron spectroscopy(XPS)analyses revealed that U(Ⅵ)primarily complexed with oxygencontaining functional groups,such as carboxyl and hydroxyl groups,on both composite surfaces,leading to stable immobilization.For Mag—HM,a notable reduction of U(Ⅵ)to U(Ⅳ)was observed,with XPS U 4f spectra showing characteristic U(Ⅳ)peaks,indicating a significant reductive immobilization pathway facilitated by the presence of both Mag and HM.In contrast,for the Ge—HM composite with a Cto-Fe ratio of 0.5,the complete consumption of Fe(Ⅱ)after U(Ⅵ)adsorption,with its proportion in total Fe decreasing from 53.7%to zero,strongly suggested that Fe(Ⅱ)played a key role in electron transfer during the immobilization process.This study elucidates the synergistic enhancement mechanisms of HM—iron hydroxide composites in U(Ⅵ)removal,providing new insights for developing green and efficient materials for the remediation of heavy metal pollution.展开更多
Uranium extraction from seawater is a promising strategy to alleviate global uranium scarcity,yet its implementation is hindered by extremely low concentrations and complex ionic environments.Concentrated seawater bri...Uranium extraction from seawater is a promising strategy to alleviate global uranium scarcity,yet its implementation is hindered by extremely low concentrations and complex ionic environments.Concentrated seawater brine,a byproduct of salt production and desalination,contains 2-10 times more uranium than natural seawater,yet its high salinity presents additional challenges for extraction.Conventional polyamidoxime(PAO)hydrogels exhibit salt-induced shrinkage,compromising functional group accessibility and adsorption efficiency.Herein,we develop an anti-polyelectrolyte effect hydrogel by composing polyvinylphosphonic acid(PVPA)and the PAO.Under high-salinity conditions,cations and anions accumulate via diffusion around the positively charged amidoxime and negatively charged phosphonic acid groups,weakening interchain electrostatic attractions.This anti-polyelectrolyte effect promotes hydrogel swelling,significantly improving the exposure of binding sites and uranyl ion uptake.The PVPA-PAO hydrogel achieves a uranium adsorption capacity of 43.89 mg·g-1 after 24 days in concentrated natural seawater derived from solar saltworks,significantly surpassing that of previously reported PAO hydrogels(~10 mg·g-1).In addition,it exhibits excellent antibacterial performance,mechanical robustness,and ion selectivity.This work presents an effective strategy for improving uranium recovery from marine resources and advances the comprehensive development and utilization of seawater resources.展开更多
Several sandstone-type uranium deposits were identified within the Upper Cretaceous red-variegated strata in the Qianjiadian area of the Songliao Basin,NE China.However,a consensus regarding the genesis of multilayer ...Several sandstone-type uranium deposits were identified within the Upper Cretaceous red-variegated strata in the Qianjiadian area of the Songliao Basin,NE China.However,a consensus regarding the genesis of multilayer tabular ore bodies within a sandstone reservoir remains elusive.This paper investigates the provenance,palaeoenvironment,and unique mineralisation characteristics of the Qingshankou Formation within the newly discovered Dalin deposit on the basis of lithofacies,element-environmentorganic geochemistry and stable isotopes.The results indicate that the fragment provenance of the ore-bearing strata is primarily composed of intermediate-felsic rocks,and the source areas are characterised by a complex tectonic background that encompasses both passive and active continental margins,as well as continental arcs.Its sedimentary environment shows a general(semi-) arid and hot palaeoclimate,with ancient lacustrine water exhibiting both fresh and brackish properties.Pure grey mudstone(PGM)features low Fe2O3T but exhibits elevated levels of ferrous iron,uranium,molybdenum,Fe2+/Fe3+ratio and reduction capacity;pure red mudstone(PRM) displays contrasting characteristics;and certain geochemical indicators of mottled mudstone(MD) are intermediate between those of the above-mentioned mudstones.Green alteration within the MD is identified as having a synsedimentary origin,as opposed to the previously assumed secondary reduction of foreign hydrocarbons.The associated organic matter is classified as Type-Ⅲ kerogen,initially derived from aquatic plankton and herbaceous plants.Finally,a sedimentary model is proposed for the red-variegated Qingshankou Formation in the study area,where the original interbedded architecture with varying geochemical properties is influenced by alternations in palaeoclimate and associated redox stratification of ancient lacustrine water.Some lenticular native grey beds,which were deposited in local low-lying lands during semi-arid and pluvial interphases,exhibit pronounced uranium pre-concentration due to phreatic oxidation during the sedimentary stage.Subsequently,differential redox activities in the Cenozoic era led to the development of multilayer geochemical zoning and tabular ore bodies in a reservoir.This research offers valuable insights into the uranium mineralisation of oxidative red-variegated strata within global basins and contributes to the development of uranium exploration strategies.展开更多
The Guidong complex in northern Guangdong constitutes a key segment of the Nanling Metallogenic Belt and hosts significant granite-related uranium deposits.However,the petrogenesis of the Yanshanian intrusions in its ...The Guidong complex in northern Guangdong constitutes a key segment of the Nanling Metallogenic Belt and hosts significant granite-related uranium deposits.However,the petrogenesis of the Yanshanian intrusions in its western part remains poorly constrained because of insufficient high-precision geochronological and mineralogical data.This limitation hinders a comprehensive understanding of regional metallogenesis.To address this,we conducted an integrated study of the Siqian two-mica granite and the Changping biotite granite,incorporating zircon U-Pb geochronology,whole-rock geochemistry,Hf-Nd isotope analysis,and mineral chemistry.Our objectives were to determine their emplacement ages and to investigate their petrogenesis and relationship with uranium mineralization.Zircon U-Pb dating indicates that the Siqian and Changping granites formed at 160±1 Ma and 156±1 Ma,respectively,suggesting both were emplaced during the Early Yanshanian magmatic event.These high-K calc-alkaline rocks are peraluminous(A/CNK=1.04-1.44),enriched in large-ion lithophile elements(LILEs;e.g.,Rb,Th,U),and depleted in high-field-strength elements(HFSEs;e.g.,Ba,Nb,Ta).They exhibit negative zircon εHf(t)values ranging from-15.4 to-8.4,with corresponding crustal model ages of 1668-2142 Ma.Whole-rock samples show εNd(t)values from-11.2 to-9.1 and Nd model ages of 1693-1860 Ma.These isotopic features indicate that both plutons represent moderately differentiated S-type granites derived from partial melting of Paleo-to Mesoproterozoic metasedimentary sources(e.g.,pelitic and psammitic rocks),accompanied by fractional crystallization of minerals such as ilmenite and apatite.Integrated geochemical and mineralogical data reveal that the Siqian and Changping granites are characterized by low Th/U ratios,high F contents,and low magmatic oxygen fugacity—signatures typical of U-rich granites.These attributes provided a favorable lithogeochemical environment for uranium enrichment and acted as primary sources for uranium-bearing,high-temperature hydrothermal fluids,thereby playing a critical role in regional uranium mineralization.展开更多
Many adsorbents have been developed for uranium recovery to ensure global energy and environmental security.However,most reported adsorbents involve complex preparation process and rely heavily on petrochemical feedst...Many adsorbents have been developed for uranium recovery to ensure global energy and environmental security.However,most reported adsorbents involve complex preparation process and rely heavily on petrochemical feedstocks,which undoubtedly increases carbon emissions from production in the nuclear industry.Here,a biomass aerogel(CS-BT)is prepared by the facile cross-linking of chitosan and bayberry tannins with glutaraldehyde.U(Ⅵ)can be adsorbed by hydroxyl groups on CS-BT aerogel via chelation,and the maximum adsorption capacity of the obtained aerogel to U(Ⅵ)is 140 mg·g-1and the removal rate reaches up to 99%(at 298.15 K,pH=5.0).The pseudo-second-order kinetics model and Freundlich model can better match the adsorption process of CS-BT aerogel,implying that its adsorption is a chemical adsorption process dominated by multilayer adsorption.The thermodynamic results show that the adsorption process of U(Ⅵ)by CS-BT aerogel is spontaneous and exothermic.Hence,our biomass aerogel can effectively extract uranium from water,contributing to the sustainable development of the nuclear industry.展开更多
Knowing the precise relationship between fuel loading and reactivity is essential for guiding reactor criticality extrapolation and online refueling in molten salt reactors(MSRs).This study aims to explore and explain...Knowing the precise relationship between fuel loading and reactivity is essential for guiding reactor criticality extrapolation and online refueling in molten salt reactors(MSRs).This study aims to explore and explain the linear relationship between reactivity and the reciprocal of uranium concentration in thermal-spectrum MSRs.By applying neutron balance theory,we analyzed the neutron absorption cross sections of various nuclides in single-lattice models with varying fuel concentrations.Our findings reveal a simple linear correlation between reactivity and the reciprocal of uranium concentration,which can be explained from the perspective of nuclear reaction cross sections that adhere to the 1/v law in the thermal neutron spectrum.Furthermore,we identified that the neutron absorption single-group cross sections of structural materials and carrier salts exhibit an approximately linear relationship with the fission single-group cross section of 235 U;similarly,the reciprocal of 235U’s fission cross section exhibits an approximately linear relationship with uranium concentration.This linear relationship deviates as the volume fraction of molten salt increases,due to a greater proportion of neutrons being captured in the resonance energy spectrum.However,it remains valid for molten salt volume fractions up to 25%and demonstrates broad applicability in the physical design and operation of thermal molten salt reactors.展开更多
As a key low-carbon energy source,nuclear power plays a vital role in the global transition toward sustainable energy.Photocatalytic uranium extraction from seawater(UES)offers a promising solution to ensure long-term...As a key low-carbon energy source,nuclear power plays a vital role in the global transition toward sustainable energy.Photocatalytic uranium extraction from seawater(UES)offers a promising solution to ensure long-term uranium supply but is challenged by ultra-low uranium concentrations and ion interference.To overcome these issues,we design three diketopyrrolopyrrole-based covalent organic frameworks(COFs)via a synergisticπ-extended lock and carboxyl-functionalized anchor molecular engineering strategy.Among them,TPy-DPP-COF features a covalently lockedπ-conjugated structure that enhances planarity,optimizes energy alignment,and minimizes exciton binding energy,thereby promoting charge transfer and suppressing recombination.Concurrently,carboxyl groups enable uranyl-specific coordination and create local electric fields to facilitate charge separation.These features contribute to the outstanding performance of TPy-DPP-COF,which achieves a high uranium adsorption capacity of 16.33 mg g−1 in natural seawater under irradiation,with only 29.3%capacity loss after 10 cycles,surpassing industrial benchmarks.Density functional theory(DFT)calculations and experimental studies reveal a synergistic photocatalysis-adsorption pathway,with DPP units acting as active sites for uranium reduction.This work highlights a molecular design strategy for developing efficient COF-based photocatalysts for practical marine uranium recovery.展开更多
The domestically developed prompt fission neutron uranium logging(PFNUL)instrument for uranium exploration represents a significant advancement in China’s deep uranium mining efforts,although it has considerable chal...The domestically developed prompt fission neutron uranium logging(PFNUL)instrument for uranium exploration represents a significant advancement in China’s deep uranium mining efforts,although it has considerable challenges and complexity.This paper presents the development of a new prompt fission neutron uranium logging instrument(named UNL4)that integrates a domestic D-T neutron generator,two 3He proportional detectors,a lanthanum bromide(LaBr3)gamma-ray detector,and a digital multi-channel pulse amplitude analyzer.The near 3He detector is shielded with 1 mm of cadmium(Cd)and 5 mm of high-density polyethylene(HDPE),enabling efficient epithermal neutron detection,whereas the far 3He detector measures thermal neutrons.A LaBr3 detector is employed for gamma-ray detection,primarily originating from uranium decay.Highspeed analog-to-digital converter(ADC)and field-programmable gate array(FPGA)technologies are used to achieve rapid acquisition and transmission of both dual-energy neutron time spectra and gamma spectra.Moreover,this paper proposes a fast signal-shaping method,which reduces the dead time effect in 3He detectors on neutron time spectra.Experiments conducted in standard model boreholes with varying uranium contents demonstrated a strong linear relationship between the epithermal-to-thermal neutron ratio(E/T)and uranium content,with a fitting coefficient of R2>0.999,confirming the accuracy of the instrument.The E/T value repeatability,in both short-term(3.16%RSD)and long-term(1.2%RSD)measurements,showed excellent stability.In addition,the instrument demonstrated good performance at neutron-logging speeds of 0.3∼3 m∕min(E/T values)and gamma logging speeds of 1∼10 m∕min.Through measurements in two ore sections of the PU model with uranium contents of 87.1 ppm and 45.6 ppm showed that RD remained below approximately 10%at logging speeds of 0–2 m/s in both cases,satisfying the requirements for engineering applications.This marks the first successful development of a neutron-logging instrument for uranium exploration based on a domestic neutron generator and signifies an important contribution to uranium resource exploration.展开更多
The lack of macro-continuity and mechanical strength of covalent organic frameworks(COFs)has significantly limited their practical applications.Here,we propose an“alcohol-triggered defect cleavage”strategy to precis...The lack of macro-continuity and mechanical strength of covalent organic frameworks(COFs)has significantly limited their practical applications.Here,we propose an“alcohol-triggered defect cleavage”strategy to precisely regulate the growth and stacking of COF grains through a moderate reversed Schiff base reaction,realizing the direct synthesis of COF nanofibers(CNFs)with high aspect ratio(L/D=103.05)and long length(>20μm).An individual CNF exhibits a biomimetic scale-like architecture,achieving superior flexibility and fatigue resistance under dynamic bending via a multiscale stress dissipation mechanism.Taking advantages of these structural features,we engineer CNF aerogels(CNF-As)with programmable porous structures(e.g.,honeycomb,lamellar,isotropic)via directional ice-template methodology.CNF-As demonstrate 100%COF content,high specific surface area(396.15 m2g-1)and superelasticity(~0%elastic deformation after 500 compression cycles at 50%strain),outperforming most COF-based counterparts.Compared with the conventional COF aerogels,the unique structural features of CNF-A enable it to perform outstandingly in uranium extraction,with an 11.72-fold increment in adsorption capacity(920.12 mg g-1)and adsorption rate(89.9%),and a 2.48-fold improvement in selectivity(U/V=2.31).This study provides a direct strategy for the development of next-generation COF materials with outstanding functionality and structural robustness.展开更多
The extraction of uranium from seawater via membrane adsorption is a promising strategy for ensuring a long-term supply of uranium and the sustainability of nuclear energy.However,this approach has been hindered by th...The extraction of uranium from seawater via membrane adsorption is a promising strategy for ensuring a long-term supply of uranium and the sustainability of nuclear energy.However,this approach has been hindered by the longstanding challenge of identifying sustainable membrane materials.In response,we propose a prototypal hybridization strategy to design a novel series of aminated conjugated microporous polymer(CMPN)@collagen fiber membrane(COLM).These sustainable and low-cost membrane materials allow a rapid and high-affinity kinetic to capture 90%of the uranium in just 30 min from 50 ppm with a high selectivity of Kd>105 mL·g−1.They also afford a robustly reusable adsorption capacity as high as 345 mg·g−1that could harvest 1.61 mg·g−1of uranium in a short 7-day real marine engineering in Fujian Province,even though suffered from very low uranium concentration of 3.29μg·L−1and tough influence of salts such as 10.77 g·L−1of Na+,1.75μg·L−1of VO3−etc.in the rough seas.The structural evidence from both experimental and theoretical studies confirmed the formation of favorable chelating motifs from the amino group on CMPN-COLM,and the intensification by the synergistic effect from the size-sieving action of CMPN and the capillary inflow effect of COLM.展开更多
Uranium,the heaviest natural element,exhibits rich and complex physical behavior,including three types of charge density wave transitions and superconductivity at low temperatures.It is widely believed that these phen...Uranium,the heaviest natural element,exhibits rich and complex physical behavior,including three types of charge density wave transitions and superconductivity at low temperatures.It is widely believed that these phenomena are closely linked to the properties of 5f electrons,which are highly susceptible to external perturbations.To elucidate the detailed electronic structure,particularly the 5f electron signatures,we fabricated high-quality single-crystal uranium films on W(110)substrates using molecular beam epitaxy and investigated their fine electronic properties and temperature-dependent evolution by angle-resolved photoemission spectroscopy(ARPES).Our experiments reveal three electron pockets around the Γ point and direct hybridization between 5f electrons and conduction electrons at regions distant from Γ.The Kondo temperature extracted from ARPES and electrical resistance measurements is approximately 131 K,indicating that the 5f electrons transition from a high-temperature localized state to a low-temperature itinerant state in the thin film system.Additionally,we observe another flat band with an energy scale of 148 meV.The detailed electronic structure and direct evidence of the localized-to-itinerant transition of 5f electrons provided in this study advance the understanding of strong electronic correlations in uranium-based materials.展开更多
Simultaneous uranium recovery,organic pollutant degradation,and electricity generation were achieved by employing a self-driven photoelectrochemical(PEC)system equipped with a modified carbon felt(MCF)cathode for the ...Simultaneous uranium recovery,organic pollutant degradation,and electricity generation were achieved by employing a self-driven photoelectrochemical(PEC)system equipped with a modified carbon felt(MCF)cathode for the treatment of complex radioactive wastewater.The MCF cathode was synthesized via a facile hydrothermal method,which modified the surface functional groups on carbon felt(CF)with enhanced active site availability and facilitated interfacial charge transfer,thus improving its UO22+adsorption and reduction capacities.The self-driven PEC system with the MCF cathode demonstrated remarkable removal efficiencies and rate constants(k)for UO22+(98.8%and 0.111 min−1)and chlortetracycline hydrochloride(CTC)(92.9%and 0.028 min−1)within 40 min and 90 min,respectively,coupled with an excellent power output of 1.41 mW/cm2.Additionally,the system with the MCF cathode exhibited superior removal performance for UO22+and CTC in treating model complex wastewater under wide conditions.Even under natural sunlight,the system achieved over 80%removal efficiency for both UO22+and CTC.Moreover,the uranium immobilized on the MCF cathode was mainly reduced to U(Ⅳ)species(90.51%),and performance remained robust over ten operational cycles.The cathode surface modification strategy and its application in the system provide a cost-effective,multi-functional and high-efficiency approach to controlling nuclides and organic pollutants in complex radioactive wastewater.展开更多
The intrinsic scintillation property of uranium has recently endowed this heaviest naturally occurring element with new opportunities for X-ray radiation detection and visualization.However,the low radiation stability...The intrinsic scintillation property of uranium has recently endowed this heaviest naturally occurring element with new opportunities for X-ray radiation detection and visualization.However,the low radiation stability of most uranium compounds hinders their practical application,particularly in X-ray imaging.Here,we presented a flexible two-dimensional uranium-organic framework(UOF,SCU-334)as an air-stable scintillating material for X-ray detection and,for the first time,a systematic investigation of X-ray imaging in UOFs.Following continuous high dose rate X-ray irradiation exceeding 50 Gy,which equals thousands of chest X-ray diagnoses,SCU-334 retains over 90%of its initial performance,representing a significant improvement over previously reported scintillating UOFs.The upgraded radiation resistance of SCU-334 is attributed to its flexible structure that dissipates energy more efficiently under high-energy particle bombardment through conformation fluctuation and relaxation.This work offers a promising approach to improve the radiation resistance of uranium-based scintillators.展开更多
This study proposes a method for99Mo production via electron accelerator irradiation of a natural-uranium-bearing liquid molten salt target,with advantages including low nuclear proliferation risk,online extraction...This study proposes a method for99Mo production via electron accelerator irradiation of a natural-uranium-bearing liquid molten salt target,with advantages including low nuclear proliferation risk,online extraction capability,and low construction costs.The approach primarily produces99Mo through photofission of uranium(~95%),specifically238U(γ,f).Secondary neutrons,originating from photonuclear interactions or fission processes,contribute minimally(~5%)to99Mo production owing to their high energies and low fission cross sections.Key parameter analyses revealed that fluoride salt systems exhibit higher99Mo yield.Their performance stems from high bremsstrahlung energy loss rate and superior photon yield,making them optimal molten salt target materials.To maximize photofission and photoneutron cross sections while minimizing highenergy gamma ray shielding requirements,an electron beam energy range of 40-80 MeV is recommended.To suppress local hot spots and prevent molten salt boiling,flow conditions were introduced to enhance convective heat transfer,effectively reducing the peak temperature.At a flow velocity of 0.5 m/s and under 80 MeV energy conditions,the maximum system temperature is only 808.9 K,which is significantly lower than the boiling point of 1773 K.Under optimized parameters,the maximum annual production capacity of~(99)Mo reaches 4486.49 Ci,sufficient for millions of diagnostic procedures and equivalent to 16.37% of China's projected demand for 2030.This method provides a viable pathway for stable,large-scale99Mo production.展开更多
The extraction of uranium from seawater is essential for the sustainable development of the nuclear industry.Covalent organic frameworks(COFs)exhibit significant potential in uranium extraction from seawater due to th...The extraction of uranium from seawater is essential for the sustainable development of the nuclear industry.Covalent organic frameworks(COFs)exhibit significant potential in uranium extraction from seawater due to their high stability,designability,and large specific surface area.Herein,a vinyl-decorated covalent organic framework,designated as COF-IHEP5,was synthesized through acid-catalyzed solvothermal method.COF-IHEP5-COOH was constructed by post-modification strategy through the“thiol-ene”click reaction,where COF-IHEP5-COOH contains hydrazone-carbonyl and flexible carboxylic acid chelating sites on pore wall.This modification facilitates synergistic adsorption of uranium by utilizing a“nano trap”that is embedded within the COF framework.The maximum adsorption capacity of the postmodified COF-IHEP5-COOH for UO22+has reached 543.8 mg/g,representing a 1.5-fold increase compared to the unmodified COF-IHEP5.Additionally,COF-IHEP5-COOH demonstrates an extraction efficiency of approximately 80%for uranium from spiked natural seawater,featuring 4.5 times higher selectivity than vanadium.The DFT calculation results show that the adsorption of uranium orginated from the synergistic coordination of the skeleton in COF-IHEP5-COOH and carboxyl group on the side arm.This research highlights the remarkable potential of pore surface engineering in customizing active adsorption sites and offers new insights for the design of functionalized uranium adsorbents with superior binding affinity and adsorption capacities.展开更多
One of the main issues in designing optimum tapered cascades for uranium enrichment for annual fuel production in a power reactor is whether to employ large(fat)or small(thin)cascades.What will be the permissible and ...One of the main issues in designing optimum tapered cascades for uranium enrichment for annual fuel production in a power reactor is whether to employ large(fat)or small(thin)cascades.What will be the permissible and optimal ranges of the number of machines that can be used in a cascade?For the first time,the permissible and optimal ranges of the number of gas centrifuges that can be utilized in a cascade were investigated using two types of centrifuges,and the performance of small and large tapered cascades was discussed.The particle swarm optimization algorithm(PSO)has been used to optimize tapered cascades.The results show:(1)For the first centrifuge,41 cascades(91≤n≤4897)and for the second centrifuge,49 cascades(18≤n≤3839)with small and large sizes can be used in enrichment facilities,and the best cascade for them has 530(with 23 stages)and 39(with 7 stages)centrifuges,respectively.(2)For both centrifuges,when 600≤n(number of centrifuges=n),the large cascade performance changes are relatively insignificant.(3)For both types of gas centrifuges,the annual los s of separation power in enrichment facilities is approximately 1.25%-4.82%of the total separation work required.展开更多
基金supported by the China Postdoctoral Science Foundation (No.2021M703001)Fundamental Research Funds for the Central Universities,China University of Geosciences (Wuhan) (No.G1323521101)+3 种基金open fund of State Key Laboratory of Nuclear Resources and Environment (East China University of Technology) (No.2022NRE02)open fund of Key Laboratory of Tectonics and Petroleum Resources (China University of Geosciences (Wuhan)),Ministry of Education (No.TPR2019-08)Fund of Outstanding Talents in Discipline of China University of Geosciences (Wuhan) (No.102162301192664)support from SINO Shaanxi Industry Group in this study。
摘要Carbonaceous debris(CD) is widely disseminated within sandstones in the Shuanglong uranium deposit,southern Ordos Basin,and is the dominant enrichment agent for uranium precipitation.The occurrence and chemical composition of uranium minerals within CD were investigated by using scanning electron microscope and electron microprobe analyses.The results show that uranium minerals mostly occur in cell pores in the forms of fructus aurantia and concentric band structure.Pitchblende and coffinite are the main uranium minerals,and the former is dominant.According to the crystal morphology and composition of trace elements of uranium minerals,uranium precipitation on the pores is grouped into two periods,orderly Ⅰ,Ⅱ.Moreover,the Ⅰ period is further divided into two sub-period,orderly Ⅰ1,Ⅰ2.Moreover,askew sphere uranium minerals could indicate fluid migration.Under certain geological environment condition,uranium is unevenly adsorbed on the surface of the pore by the Van der Waals(i.e.,Ⅰ1 period),and then is precipitated towards to the center of the pore until the whole pore is filled up with uranium minerals by complicated process such as microorganism activities(i.e.,Ⅰ2,Ⅱ period).It will provide some guidance for studying the metallogenic environment and genesis of sandstone-type uranium deposit.
基金Suppored by the National Natural Science Foundation of China(No.U2341292)the framework of a state assignment for the Institute of Geology of Ore Deposits,Petrography,Mineralogy and Geochemistry of the Russian Academy of Sciences(IGEM RAS)and framework agreement for cooperation between IGEM RAS and Beijing Research Institute of Uranium Geology(BRIUG),China National Nuclear Corporation。
摘要The article is devoted to the problems of the influence of global processes of Great Oxygenation Event of the Earth’s atmosphere on the genesis of Proterozoic unconformity-type uranium deposits in the Canadian sedimentary Athabasca basin,which are the most prominent representatives of large-scale uranium deposits with uniquely rich ores with uranium content up to a few tens of percentages in the world.The influence of the formation of an oxygen atmosphere on the process of ore formation is considered with a comparative analysis of single-stage and multi-stage models of the formation of unconformity uranium deposits.The appearance of free oxygen in the Earth’s atmosphere,necessary for the formation of the unconformity deposits,occurred approximately 2.5-2.0 billion years ago during the Great Oxygenation Event(GOE).The Great Oxidation Event caused the atmosphere to form high levels of oxygen,leading to the production of more primary biological matter on the early Earth,thereby forming more organic-rich sediments,which played an important role in U-mineralization of Proterozoic unconformity-related uranium deposits.The formation of the Athabasca basin began approximately 1740 Ma ago.Uranium mineralization in the deposits occurred 1590 Ma ago.This was followed by a series of putative post-ore events with rejuvenated ages from 1525 to 1000-950 Ma,which in the single-stage deposit formation model were interpreted as re precipitation of primary ore mineralization with the formation of the deposits’ore resource from both of its main sources:the mobilization of uranium from uranium-bearing minerals of the Athabasca Group sandstones and from the basement rocks of the basin.We adopted an alternative genetic model the way from their source to the basin reservoirs,which formed the resource of primary uranium of the initial stage,and 2)initially barren(after the depletion of the ore reserve of the Athabasca sandstones on basin fluids that leached uranium from uranium-bearing especially organic of multi-stage deposit formation with two spatially and temporally separated uranium sources:1)ore-forming basin brines of the Athabasca sandstones with an initially elevated uranium content during its mobilization from uranium-bearing rocks along the brine migration route on rocks of the basin basement with the formation of an‘additional’uranium resource at subsequent stages with a rejuvenated ages.The deposition of primary uranium of the initial stage and‘additional’uranium occurred in structural traps localizing the initial stage uranium,with a concomitant increase in the total reserves and ore grades of the deposits.After the depletion of the‘additional’uranium in the basement available for mobilization,the formation of the ore resource of the deposits was completed.We adopted this conclusion as a hypothesis for a possible interpretation of the mechanism for the final completion of the geological history of the Athabasca basin deposits in the Mesoproterozoic Era,1600-1000 Ma ago.
基金supported by the National Natural Science Foundation of China(41902310,42372348,42372286)Deep Earth Probe and Mineral Resources Exploration-National Science and Technology Major Project(2024ZD1003607)+2 种基金China Geological Survey Projects(DD20230700802,DD20221819)the Basic Research Fund of the Chinese Academy of Geological Sciences(JKYQN202306)Key Research and Development Program of Shanxi Province,China(202102090301009).
摘要The Mianhuakeng uranium deposit,characterized by uranium-rich granite,serves as a key site for research into crustal radioactive heating.Based on 45 rock samples,this study reviews that the host granite in the Mianhuakeng uranium deposit has a high radioactive heat production rate(avg.5.50μW/m³)and a low Th/U ratio(avg.2.62).Uranium-rich granite and its alteration zone within the upper crust(0-5 km depth)contribute about 45%of the total radioactive heat production,wich is crucial for controlling geothermal resource distribution.For uranium-thermal at tectonic plate margins,a symbiotic geological model was proposed:Firstly,subduction of the Pacific Plate caused upwelling of the asthenosphere,generating a high heat-flow background.Secondly,heat transfer is enhanced by major faults such as the Youdong and Mianhuakeng faults.Subsequently,uranium was mobilized,transported,and enriched within the granite through deep siliceous hydrothermal activity and associated alteration.Ultimately,the uranium enrichment in granite leads to increased radioactive heat production,resulting in local thermal anomalies.This model provides a theoretical support for exploring and developing uranium-thermal symbiotic resources in South China.
基金supported by Hunan Provincial Natural Science Foundation of China(No.2025JJ50152)the Project of Hunan Province Postgraduate Research and Innovation(No.CX20251481)+2 种基金the Open Funding of the Key Laboratory of Monitoring for Heavy Metal Pollutants,Ministry of Ecology and Environment(No.KLMHM202433)the Project of College Students’Innovative Entrepreneurial Training of Hunan Province(Nos.S202510555304,S202410555048 and S202410555224)the College Students’Research Learning and Innovative Experimental Project of University of South China(No.DC20250155).
摘要Studies on the phytotoxicity of cadmium(Cd)and uranium(U)in rice mainly focus on single exposure.However,water,soil,and other environmental media are always co-contaminated by Cd and U.The effects of Cd(5 mg/L)and U(10 mg/L)single and combined exposure for 7 days on rice seedlings were explored by hydroponic experiment.The synergism of U and Cd intensified the inhibitory effect of combined exposure on the rice seedling’s growth,accompanied by a remarkable reduction in chlorophyll content,alterations in antioxidant capacity,imbalances in mineral element metabolism,lipid peroxidation-induced destruction observed in rice seedlings,and significantly regulated expression of OsNramp5,OsHMA3,and OsHMA2,the adverse effects on the roots were more severe compared to those on the shoots.Combined exposure of U and Cd altered the distribution of U and Cd in the rice plant and subcellular.The accumulation of U and Cd in the rice seedlings’roots observably exceeded the shoot.Cd is mainly isolated in the vacuole and cell wall;U is primarily trapped in the cell wall.Cd promoted U accumulation in rice seedlings,while U inhibited Cd accumulation in rice seedlings.These findings can not only expand the understanding of the phytotoxicity of heavy metal combined exposure but also have important theoretical and practical significance for evaluating and remedying heavy metals contaminated-paddy soil and ensure for safe production of rice.
基金supported by the National Natural Science Foundation of China(Grant No.42207306)the Natural Science Foundation of Chongqing,China(Grant No.cstc2021jcyj-bshX0231).
摘要Composite systems of soil organic matter and iron hydroxides hold significant potential for the remediation of heavy metal pollution.However,the synergistic immobilization mechanisms of U(Ⅵ)by humin(HM)—iron hydroxide composites remain insufficiently understood.In this study,goethite(Ge)—HM and magnetite(Mag)—HM composites with varying C-to-Fe molar ratios were synthesized via co-precipitation,and their adsorption behavior and underlying mechanisms towards U(Ⅵ)in aqueous solutions were systematically investigated.The results showed that under conditions of a pH value of 5.0 and temperature of 298 K,the maximum U(Ⅵ)adsorption capacities of Ge—HM and Mag—HM reached 60.56 mg/g and 64.12 mg/g,respectively,significantly surpassing those of pure Ge(39.6 mg/g),Mag(22.5 mg/g),and HM(20.2 mg/g).Kinetic studies revealed that the adsorption processes for both Ge—HM and Mag—HM conformed to the pseudo-second-order kinetic model,indicating chemical reaction control.Isothermal adsorption results were well described by the Langmuir model,suggesting monolayer adsorption on the composite surfaces.Crucially,characterization results elucidated distinct reaction mechanisms.Fourier transform infrared spectroscopy(FTIR)and X-ray photoelectron spectroscopy(XPS)analyses revealed that U(Ⅵ)primarily complexed with oxygencontaining functional groups,such as carboxyl and hydroxyl groups,on both composite surfaces,leading to stable immobilization.For Mag—HM,a notable reduction of U(Ⅵ)to U(Ⅳ)was observed,with XPS U 4f spectra showing characteristic U(Ⅳ)peaks,indicating a significant reductive immobilization pathway facilitated by the presence of both Mag and HM.In contrast,for the Ge—HM composite with a Cto-Fe ratio of 0.5,the complete consumption of Fe(Ⅱ)after U(Ⅵ)adsorption,with its proportion in total Fe decreasing from 53.7%to zero,strongly suggested that Fe(Ⅱ)played a key role in electron transfer during the immobilization process.This study elucidates the synergistic enhancement mechanisms of HM—iron hydroxide composites in U(Ⅵ)removal,providing new insights for developing green and efficient materials for the remediation of heavy metal pollution.
基金supported by the National Key Research and Development Program of China(2023YFC2809000)the National Natural Science Foundation of China(22422603,52201315,22266015,22327807,U23A20104,and U2167220)+3 种基金the Natural Science Foundation of Hainan Province(225YXQN585)the Hainan Province Science and Technology Special Fund(ZDYF2024SHFZ066)the Young Elite Scientists Sponsorship Program by Chinese Association for Science and Technology(CAST2023QNRC001)。
摘要Uranium extraction from seawater is a promising strategy to alleviate global uranium scarcity,yet its implementation is hindered by extremely low concentrations and complex ionic environments.Concentrated seawater brine,a byproduct of salt production and desalination,contains 2-10 times more uranium than natural seawater,yet its high salinity presents additional challenges for extraction.Conventional polyamidoxime(PAO)hydrogels exhibit salt-induced shrinkage,compromising functional group accessibility and adsorption efficiency.Herein,we develop an anti-polyelectrolyte effect hydrogel by composing polyvinylphosphonic acid(PVPA)and the PAO.Under high-salinity conditions,cations and anions accumulate via diffusion around the positively charged amidoxime and negatively charged phosphonic acid groups,weakening interchain electrostatic attractions.This anti-polyelectrolyte effect promotes hydrogel swelling,significantly improving the exposure of binding sites and uranyl ion uptake.The PVPA-PAO hydrogel achieves a uranium adsorption capacity of 43.89 mg·g-1 after 24 days in concentrated natural seawater derived from solar saltworks,significantly surpassing that of previously reported PAO hydrogels(~10 mg·g-1).In addition,it exhibits excellent antibacterial performance,mechanical robustness,and ion selectivity.This work presents an effective strategy for improving uranium recovery from marine resources and advances the comprehensive development and utilization of seawater resources.
基金supported by the Fund Project from the National Key Laboratory of Uranium Resource Exploration-Mining and Nuclear Remote Sensing (NKLUR-2024-ZD-003)the National Natural Science Foundation of China (U2441201)the Fourth of Talent Projects of China National Nuclear Corporation (QNYC 2102)。
摘要Several sandstone-type uranium deposits were identified within the Upper Cretaceous red-variegated strata in the Qianjiadian area of the Songliao Basin,NE China.However,a consensus regarding the genesis of multilayer tabular ore bodies within a sandstone reservoir remains elusive.This paper investigates the provenance,palaeoenvironment,and unique mineralisation characteristics of the Qingshankou Formation within the newly discovered Dalin deposit on the basis of lithofacies,element-environmentorganic geochemistry and stable isotopes.The results indicate that the fragment provenance of the ore-bearing strata is primarily composed of intermediate-felsic rocks,and the source areas are characterised by a complex tectonic background that encompasses both passive and active continental margins,as well as continental arcs.Its sedimentary environment shows a general(semi-) arid and hot palaeoclimate,with ancient lacustrine water exhibiting both fresh and brackish properties.Pure grey mudstone(PGM)features low Fe2O3T but exhibits elevated levels of ferrous iron,uranium,molybdenum,Fe2+/Fe3+ratio and reduction capacity;pure red mudstone(PRM) displays contrasting characteristics;and certain geochemical indicators of mottled mudstone(MD) are intermediate between those of the above-mentioned mudstones.Green alteration within the MD is identified as having a synsedimentary origin,as opposed to the previously assumed secondary reduction of foreign hydrocarbons.The associated organic matter is classified as Type-Ⅲ kerogen,initially derived from aquatic plankton and herbaceous plants.Finally,a sedimentary model is proposed for the red-variegated Qingshankou Formation in the study area,where the original interbedded architecture with varying geochemical properties is influenced by alternations in palaeoclimate and associated redox stratification of ancient lacustrine water.Some lenticular native grey beds,which were deposited in local low-lying lands during semi-arid and pluvial interphases,exhibit pronounced uranium pre-concentration due to phreatic oxidation during the sedimentary stage.Subsequently,differential redox activities in the Cenozoic era led to the development of multilayer geochemical zoning and tabular ore bodies in a reservoir.This research offers valuable insights into the uranium mineralisation of oxidative red-variegated strata within global basins and contributes to the development of uranium exploration strategies.
基金supported by the National Natural Science Foundation of China(grants 42362011 and 42272090)。
摘要The Guidong complex in northern Guangdong constitutes a key segment of the Nanling Metallogenic Belt and hosts significant granite-related uranium deposits.However,the petrogenesis of the Yanshanian intrusions in its western part remains poorly constrained because of insufficient high-precision geochronological and mineralogical data.This limitation hinders a comprehensive understanding of regional metallogenesis.To address this,we conducted an integrated study of the Siqian two-mica granite and the Changping biotite granite,incorporating zircon U-Pb geochronology,whole-rock geochemistry,Hf-Nd isotope analysis,and mineral chemistry.Our objectives were to determine their emplacement ages and to investigate their petrogenesis and relationship with uranium mineralization.Zircon U-Pb dating indicates that the Siqian and Changping granites formed at 160±1 Ma and 156±1 Ma,respectively,suggesting both were emplaced during the Early Yanshanian magmatic event.These high-K calc-alkaline rocks are peraluminous(A/CNK=1.04-1.44),enriched in large-ion lithophile elements(LILEs;e.g.,Rb,Th,U),and depleted in high-field-strength elements(HFSEs;e.g.,Ba,Nb,Ta).They exhibit negative zircon εHf(t)values ranging from-15.4 to-8.4,with corresponding crustal model ages of 1668-2142 Ma.Whole-rock samples show εNd(t)values from-11.2 to-9.1 and Nd model ages of 1693-1860 Ma.These isotopic features indicate that both plutons represent moderately differentiated S-type granites derived from partial melting of Paleo-to Mesoproterozoic metasedimentary sources(e.g.,pelitic and psammitic rocks),accompanied by fractional crystallization of minerals such as ilmenite and apatite.Integrated geochemical and mineralogical data reveal that the Siqian and Changping granites are characterized by low Th/U ratios,high F contents,and low magmatic oxygen fugacity—signatures typical of U-rich granites.These attributes provided a favorable lithogeochemical environment for uranium enrichment and acted as primary sources for uranium-bearing,high-temperature hydrothermal fluids,thereby playing a critical role in regional uranium mineralization.
基金supported by Doctoral Scientific Fund Project of Southwest University of Science and Technology(20zx7130)Seawater Uranium Extraction Innovation and Development Fund Project(China National Nuclear Corporation)(CNNCCXLM-202215)。
摘要Many adsorbents have been developed for uranium recovery to ensure global energy and environmental security.However,most reported adsorbents involve complex preparation process and rely heavily on petrochemical feedstocks,which undoubtedly increases carbon emissions from production in the nuclear industry.Here,a biomass aerogel(CS-BT)is prepared by the facile cross-linking of chitosan and bayberry tannins with glutaraldehyde.U(Ⅵ)can be adsorbed by hydroxyl groups on CS-BT aerogel via chelation,and the maximum adsorption capacity of the obtained aerogel to U(Ⅵ)is 140 mg·g-1and the removal rate reaches up to 99%(at 298.15 K,pH=5.0).The pseudo-second-order kinetics model and Freundlich model can better match the adsorption process of CS-BT aerogel,implying that its adsorption is a chemical adsorption process dominated by multilayer adsorption.The thermodynamic results show that the adsorption process of U(Ⅵ)by CS-BT aerogel is spontaneous and exothermic.Hence,our biomass aerogel can effectively extract uranium from water,contributing to the sustainable development of the nuclear industry.
基金supported by the Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.2020261)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA02010000)the Young Potential Program of the Shanghai Institute of Applied Physics,Chinese Academy of Sciences(No.SINAP-YXJH-202412)。
摘要Knowing the precise relationship between fuel loading and reactivity is essential for guiding reactor criticality extrapolation and online refueling in molten salt reactors(MSRs).This study aims to explore and explain the linear relationship between reactivity and the reciprocal of uranium concentration in thermal-spectrum MSRs.By applying neutron balance theory,we analyzed the neutron absorption cross sections of various nuclides in single-lattice models with varying fuel concentrations.Our findings reveal a simple linear correlation between reactivity and the reciprocal of uranium concentration,which can be explained from the perspective of nuclear reaction cross sections that adhere to the 1/v law in the thermal neutron spectrum.Furthermore,we identified that the neutron absorption single-group cross sections of structural materials and carrier salts exhibit an approximately linear relationship with the fission single-group cross section of 235 U;similarly,the reciprocal of 235U’s fission cross section exhibits an approximately linear relationship with uranium concentration.This linear relationship deviates as the volume fraction of molten salt increases,due to a greater proportion of neutrons being captured in the resonance energy spectrum.However,it remains valid for molten salt volume fractions up to 25%and demonstrates broad applicability in the physical design and operation of thermal molten salt reactors.
基金the Young Elite Scientists Sponsorship Program by JXAST(2024QT11)the National Natural Science Foundation of China(22465001,22309003)the Jiangxi Provincial Natural Science Foundation(20232BAB203042,20242BAB22002).
摘要As a key low-carbon energy source,nuclear power plays a vital role in the global transition toward sustainable energy.Photocatalytic uranium extraction from seawater(UES)offers a promising solution to ensure long-term uranium supply but is challenged by ultra-low uranium concentrations and ion interference.To overcome these issues,we design three diketopyrrolopyrrole-based covalent organic frameworks(COFs)via a synergisticπ-extended lock and carboxyl-functionalized anchor molecular engineering strategy.Among them,TPy-DPP-COF features a covalently lockedπ-conjugated structure that enhances planarity,optimizes energy alignment,and minimizes exciton binding energy,thereby promoting charge transfer and suppressing recombination.Concurrently,carboxyl groups enable uranyl-specific coordination and create local electric fields to facilitate charge separation.These features contribute to the outstanding performance of TPy-DPP-COF,which achieves a high uranium adsorption capacity of 16.33 mg g−1 in natural seawater under irradiation,with only 29.3%capacity loss after 10 cycles,surpassing industrial benchmarks.Density functional theory(DFT)calculations and experimental studies reveal a synergistic photocatalysis-adsorption pathway,with DPP units acting as active sites for uranium reduction.This work highlights a molecular design strategy for developing efficient COF-based photocatalysts for practical marine uranium recovery.
基金supported by the National Natural Science Foundation of China(No.42374226)Jiangxi Provincial Natural Science Foundation(Nos.20232BCJ23006,gpyc20240073,20252BAC240173 and 20243BCE51132)National Key Laboratory of Uranium Resource Exploration-Mining and Nuclear Remote Sensing(2024QZ-TD-09,2024HDX10,2025QZ018).
摘要The domestically developed prompt fission neutron uranium logging(PFNUL)instrument for uranium exploration represents a significant advancement in China’s deep uranium mining efforts,although it has considerable challenges and complexity.This paper presents the development of a new prompt fission neutron uranium logging instrument(named UNL4)that integrates a domestic D-T neutron generator,two 3He proportional detectors,a lanthanum bromide(LaBr3)gamma-ray detector,and a digital multi-channel pulse amplitude analyzer.The near 3He detector is shielded with 1 mm of cadmium(Cd)and 5 mm of high-density polyethylene(HDPE),enabling efficient epithermal neutron detection,whereas the far 3He detector measures thermal neutrons.A LaBr3 detector is employed for gamma-ray detection,primarily originating from uranium decay.Highspeed analog-to-digital converter(ADC)and field-programmable gate array(FPGA)technologies are used to achieve rapid acquisition and transmission of both dual-energy neutron time spectra and gamma spectra.Moreover,this paper proposes a fast signal-shaping method,which reduces the dead time effect in 3He detectors on neutron time spectra.Experiments conducted in standard model boreholes with varying uranium contents demonstrated a strong linear relationship between the epithermal-to-thermal neutron ratio(E/T)and uranium content,with a fitting coefficient of R2>0.999,confirming the accuracy of the instrument.The E/T value repeatability,in both short-term(3.16%RSD)and long-term(1.2%RSD)measurements,showed excellent stability.In addition,the instrument demonstrated good performance at neutron-logging speeds of 0.3∼3 m∕min(E/T values)and gamma logging speeds of 1∼10 m∕min.Through measurements in two ore sections of the PU model with uranium contents of 87.1 ppm and 45.6 ppm showed that RD remained below approximately 10%at logging speeds of 0–2 m/s in both cases,satisfying the requirements for engineering applications.This marks the first successful development of a neutron-logging instrument for uranium exploration based on a domestic neutron generator and signifies an important contribution to uranium resource exploration.
基金supported by the National Natural Science Foundation of China(No.52403035)the Shanghai Sailing Program(23YF1400300)+1 种基金the Fundamental Research Funds for the Central Universities(2232023D-05)the Weiqiao Teaching and Research Innovation Program.
摘要The lack of macro-continuity and mechanical strength of covalent organic frameworks(COFs)has significantly limited their practical applications.Here,we propose an“alcohol-triggered defect cleavage”strategy to precisely regulate the growth and stacking of COF grains through a moderate reversed Schiff base reaction,realizing the direct synthesis of COF nanofibers(CNFs)with high aspect ratio(L/D=103.05)and long length(>20μm).An individual CNF exhibits a biomimetic scale-like architecture,achieving superior flexibility and fatigue resistance under dynamic bending via a multiscale stress dissipation mechanism.Taking advantages of these structural features,we engineer CNF aerogels(CNF-As)with programmable porous structures(e.g.,honeycomb,lamellar,isotropic)via directional ice-template methodology.CNF-As demonstrate 100%COF content,high specific surface area(396.15 m2g-1)and superelasticity(~0%elastic deformation after 500 compression cycles at 50%strain),outperforming most COF-based counterparts.Compared with the conventional COF aerogels,the unique structural features of CNF-A enable it to perform outstandingly in uranium extraction,with an 11.72-fold increment in adsorption capacity(920.12 mg g-1)and adsorption rate(89.9%),and a 2.48-fold improvement in selectivity(U/V=2.31).This study provides a direct strategy for the development of next-generation COF materials with outstanding functionality and structural robustness.
基金supported by National Natural Science Foundation of China(Grant No.22378066,22108040)Collaboration&Innovation Platform Project of National Independent Innovation Demonstration Zone(Fuzhou,Xiamen&Quanzhou)(Project No:3502ZCQXT2023004).
摘要The extraction of uranium from seawater via membrane adsorption is a promising strategy for ensuring a long-term supply of uranium and the sustainability of nuclear energy.However,this approach has been hindered by the longstanding challenge of identifying sustainable membrane materials.In response,we propose a prototypal hybridization strategy to design a novel series of aminated conjugated microporous polymer(CMPN)@collagen fiber membrane(COLM).These sustainable and low-cost membrane materials allow a rapid and high-affinity kinetic to capture 90%of the uranium in just 30 min from 50 ppm with a high selectivity of Kd>105 mL·g−1.They also afford a robustly reusable adsorption capacity as high as 345 mg·g−1that could harvest 1.61 mg·g−1of uranium in a short 7-day real marine engineering in Fujian Province,even though suffered from very low uranium concentration of 3.29μg·L−1and tough influence of salts such as 10.77 g·L−1of Na+,1.75μg·L−1of VO3−etc.in the rough seas.The structural evidence from both experimental and theoretical studies confirmed the formation of favorable chelating motifs from the amino group on CMPN-COLM,and the intensification by the synergistic effect from the size-sieving action of CMPN and the capillary inflow effect of COLM.
基金Project supported by the National Key Research and Development Program of China(Grant Nos.2021YFA1601101and 2022YFA1402201)the National Natural Science Foundation of China(Grant Nos.52394161 and U2430209)+1 种基金Sichuan Science&Technology Program(Grant No.2025ZNSFSC0869)the Institute of Materials(Grant No.TP02202408)。
摘要Uranium,the heaviest natural element,exhibits rich and complex physical behavior,including three types of charge density wave transitions and superconductivity at low temperatures.It is widely believed that these phenomena are closely linked to the properties of 5f electrons,which are highly susceptible to external perturbations.To elucidate the detailed electronic structure,particularly the 5f electron signatures,we fabricated high-quality single-crystal uranium films on W(110)substrates using molecular beam epitaxy and investigated their fine electronic properties and temperature-dependent evolution by angle-resolved photoemission spectroscopy(ARPES).Our experiments reveal three electron pockets around the Γ point and direct hybridization between 5f electrons and conduction electrons at regions distant from Γ.The Kondo temperature extracted from ARPES and electrical resistance measurements is approximately 131 K,indicating that the 5f electrons transition from a high-temperature localized state to a low-temperature itinerant state in the thin film system.Additionally,we observe another flat band with an energy scale of 148 meV.The detailed electronic structure and direct evidence of the localized-to-itinerant transition of 5f electrons provided in this study advance the understanding of strong electronic correlations in uranium-based materials.
基金supported by the National Natural Science Foundation of China(Nos.52170083 and 12305352)the Science and Technology Innovation Program of Hunan Province(No.2022RC1125).
摘要Simultaneous uranium recovery,organic pollutant degradation,and electricity generation were achieved by employing a self-driven photoelectrochemical(PEC)system equipped with a modified carbon felt(MCF)cathode for the treatment of complex radioactive wastewater.The MCF cathode was synthesized via a facile hydrothermal method,which modified the surface functional groups on carbon felt(CF)with enhanced active site availability and facilitated interfacial charge transfer,thus improving its UO22+adsorption and reduction capacities.The self-driven PEC system with the MCF cathode demonstrated remarkable removal efficiencies and rate constants(k)for UO22+(98.8%and 0.111 min−1)and chlortetracycline hydrochloride(CTC)(92.9%and 0.028 min−1)within 40 min and 90 min,respectively,coupled with an excellent power output of 1.41 mW/cm2.Additionally,the system with the MCF cathode exhibited superior removal performance for UO22+and CTC in treating model complex wastewater under wide conditions.Even under natural sunlight,the system achieved over 80%removal efficiency for both UO22+and CTC.Moreover,the uranium immobilized on the MCF cathode was mainly reduced to U(Ⅳ)species(90.51%),and performance remained robust over ten operational cycles.The cathode surface modification strategy and its application in the system provide a cost-effective,multi-functional and high-efficiency approach to controlling nuclides and organic pollutants in complex radioactive wastewater.
基金financial support from the National Natural Science Foundation of China(Nos.22376153,U23A20104,22206144,22276132,22306139,22076131)Science Foundation of the Higher Education Institutions of Jiangsu Province(No.22KJA150006)+2 种基金Gusu Innovation and Entrepreneurship Leading Talent Program Project(No.ZXL2024406)Suzhou Fundamental Research Project(No.SJC2023001)a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)。
摘要The intrinsic scintillation property of uranium has recently endowed this heaviest naturally occurring element with new opportunities for X-ray radiation detection and visualization.However,the low radiation stability of most uranium compounds hinders their practical application,particularly in X-ray imaging.Here,we presented a flexible two-dimensional uranium-organic framework(UOF,SCU-334)as an air-stable scintillating material for X-ray detection and,for the first time,a systematic investigation of X-ray imaging in UOFs.Following continuous high dose rate X-ray irradiation exceeding 50 Gy,which equals thousands of chest X-ray diagnoses,SCU-334 retains over 90%of its initial performance,representing a significant improvement over previously reported scintillating UOFs.The upgraded radiation resistance of SCU-334 is attributed to its flexible structure that dissipates energy more efficiently under high-energy particle bombardment through conformation fluctuation and relaxation.This work offers a promising approach to improve the radiation resistance of uranium-based scintillators.
基金supported by the National Natural Science Foundation of China(Nos.12435012,12175300,and 12475185)Shanghai Natural Science Foundation(No.24ZR1478500)Nuclear energy development project(HNKF202210(24))。
摘要This study proposes a method for99Mo production via electron accelerator irradiation of a natural-uranium-bearing liquid molten salt target,with advantages including low nuclear proliferation risk,online extraction capability,and low construction costs.The approach primarily produces99Mo through photofission of uranium(~95%),specifically238U(γ,f).Secondary neutrons,originating from photonuclear interactions or fission processes,contribute minimally(~5%)to99Mo production owing to their high energies and low fission cross sections.Key parameter analyses revealed that fluoride salt systems exhibit higher99Mo yield.Their performance stems from high bremsstrahlung energy loss rate and superior photon yield,making them optimal molten salt target materials.To maximize photofission and photoneutron cross sections while minimizing highenergy gamma ray shielding requirements,an electron beam energy range of 40-80 MeV is recommended.To suppress local hot spots and prevent molten salt boiling,flow conditions were introduced to enhance convective heat transfer,effectively reducing the peak temperature.At a flow velocity of 0.5 m/s and under 80 MeV energy conditions,the maximum system temperature is only 808.9 K,which is significantly lower than the boiling point of 1773 K.Under optimized parameters,the maximum annual production capacity of~(99)Mo reaches 4486.49 Ci,sufficient for millions of diagnostic procedures and equivalent to 16.37% of China's projected demand for 2030.This method provides a viable pathway for stable,large-scale99Mo production.
基金supported by the Project of Uranium Extraction from Seawater(No.HNKF202216(36))。
摘要The extraction of uranium from seawater is essential for the sustainable development of the nuclear industry.Covalent organic frameworks(COFs)exhibit significant potential in uranium extraction from seawater due to their high stability,designability,and large specific surface area.Herein,a vinyl-decorated covalent organic framework,designated as COF-IHEP5,was synthesized through acid-catalyzed solvothermal method.COF-IHEP5-COOH was constructed by post-modification strategy through the“thiol-ene”click reaction,where COF-IHEP5-COOH contains hydrazone-carbonyl and flexible carboxylic acid chelating sites on pore wall.This modification facilitates synergistic adsorption of uranium by utilizing a“nano trap”that is embedded within the COF framework.The maximum adsorption capacity of the postmodified COF-IHEP5-COOH for UO22+has reached 543.8 mg/g,representing a 1.5-fold increase compared to the unmodified COF-IHEP5.Additionally,COF-IHEP5-COOH demonstrates an extraction efficiency of approximately 80%for uranium from spiked natural seawater,featuring 4.5 times higher selectivity than vanadium.The DFT calculation results show that the adsorption of uranium orginated from the synergistic coordination of the skeleton in COF-IHEP5-COOH and carboxyl group on the side arm.This research highlights the remarkable potential of pore surface engineering in customizing active adsorption sites and offers new insights for the design of functionalized uranium adsorbents with superior binding affinity and adsorption capacities.
摘要One of the main issues in designing optimum tapered cascades for uranium enrichment for annual fuel production in a power reactor is whether to employ large(fat)or small(thin)cascades.What will be the permissible and optimal ranges of the number of machines that can be used in a cascade?For the first time,the permissible and optimal ranges of the number of gas centrifuges that can be utilized in a cascade were investigated using two types of centrifuges,and the performance of small and large tapered cascades was discussed.The particle swarm optimization algorithm(PSO)has been used to optimize tapered cascades.The results show:(1)For the first centrifuge,41 cascades(91≤n≤4897)and for the second centrifuge,49 cascades(18≤n≤3839)with small and large sizes can be used in enrichment facilities,and the best cascade for them has 530(with 23 stages)and 39(with 7 stages)centrifuges,respectively.(2)For both centrifuges,when 600≤n(number of centrifuges=n),the large cascade performance changes are relatively insignificant.(3)For both types of gas centrifuges,the annual los s of separation power in enrichment facilities is approximately 1.25%-4.82%of the total separation work required.