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Unusual Uranium biomineralization induced by green algae: Behavior investigation and mechanism probe

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Journal of Environmental Sciences 2023年第2期124卷 915-922页

作者： Yanxia Cheng Ting Zhang Shunzhang Chen Feize Li Renwei Qing Tu Lan Yuanyou Yang Jiali Liao Ning Liu Key Laboratory of Radiation Physics and Technology of the Ministry of Education Institute of Nuclear Science and TechnologySichuan UniversityChengdu 610064China Key Laboratory of Bio-Resource and Eco-Environment of the Ministry of Education College of Life SciencesSichuan UniversityChengdu 610065China

As a biosorbent,algae are frequently used for the biotreatment or bioremediation of water contaminated by heavymetal or radionuclides.However,it is unclear that whether or not the biomineralization of these metal or radionuclides can be induced by algae in the process of bioremediation and what the mechanism is.In this work,Ankistrodsemus sp.has been used to treat the Uranium-contaminated water,and more than 98%of Uranium in the solution can be removed by the alga,when the initial Uranium concentration ranges from 10 to 80 mg/L.Especially,an unusual phenomenon of algae-induced Uranium biomineralization has been found in the process of Uranium bioremediation and its mineralization mechanism has been explored bymultiple approaches.It is worth noticing that the biomineralization of Uranium induced by Ankistrodsemus sp.is significantly affected by contact time and pH.Uranium is captured rapidly on the cell surface via complexation with the carboxylate radical,amino and amide groups of themicroalgae cells,which provides nucleation sites for the precipitation of insolubleminerals.Uranium stimulates Ankistrodsemus sp.to metabolize potassium ions(K+),which may endow algae with the ability to biomineralize Uranium into the rose-like compreignacite(K_(2)[(UO_(2))6O_(4)(OH)_(6)]•8H_(2)O).As the time increased,the amorphous gradually converted into compreignacite crystals and a large number of crystals would expand over both inside and outside the cells.To the best of our knowledge,this is the first investigated microalgae with a time-dependent Uranium biomineralization ability and superior tolerance to Uranium.This work validates that Ankistrodsemus sp.is a promising alga for the treatment of Uranium-contaminated wastewater.

关键词： Uranium algae Ankistrodesmus sp. Biomineralization

Non-targeted metabolomics reveals the stress response of a cellulase-containing penicillium to Uranium

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Journal of Environmental Sciences 2022年第10期34卷 9-17页

作者： Li Zhang Jie Li Jin-long Lai Xu Yang Yu Zhang Xue-gang Luo School of Life Science and Engineering Southwest University of Science and TechnologyMianyang 621010China Engineering Research Center of Biomass Materials Ministry of Education ofSWUSTMianyang 621010China

Human industrial activities have caused environmental Uranium(U) pollution, resulting in Uranium(Ⅵ) had radiotoxicity and chemical toxicity. Here, a cellulase-producing Penicillium fungus was screened and characterized by X-ray fluorescence(XRF), and Fourier transform infrared reflection(FT-IR), as well as by GC/MS metabolomics analysis, to study the response to Uranium(Ⅵ) stress. The biomass of Penicillium decreased after exposure to 100 mg/L U.Uranium combined with carboxyl groups, amino groups, and phosphate groups to form Uranium mineralized deposits on the surface of this fungal strain. The α-activity concentration of Uranium in the strain was 2.57×10^(6)Bq/kg, and the β-activity concentration was 2.27×10^(5)Bq/kg. Metabolomics analysis identified 118 different metabolites, as well as metabolic disruption of organic acids and derivatives. Further analysis showed that Uranium significantly affected the metabolism of 9 amino acids in Penicillium. These amino acids were related to the TCA cycle and ABC transporter. At the same time, Uranium exhibited nucleotide metabolism toxicity to Penicillium. This study provides an in-depth understanding of the Uranium tolerance mechanism of Penicillium and provides a theoretical basis for Penicillium to degrade hyper-enriched plants.

关键词： Penicillium Uranium Metabolomics Amino acid Nucleic acid

A Uranium(Ⅳ) Alkyl Complex: Synthesis and Catalytic Property in Carbonyl Hydroboration

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Chinese Journal of Chemistry 2022年第17期40卷 2047-2053页

作者： Xiong Sun Xingxing Gong Zhuoyi Xie Congqing Zhu State Key Laboratory of Coordination Chemistry Jiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjingJiangsu210093 China

The strong oxophilicity of actinide complexes prevents their applications in the transformation of oxygen-containing substrates.Herein,we report the use of a Uranium(Ⅳ)alkyl complex as a catalyst for the hydroboration of carbonyl compounds.This reaction has good functional group tolerance and chemo-selectivity under mild conditions.This study represents the rare example of catalytic reaction promoted by a Uranium alkyl complex and highlights the potential of Uranium complexes in synthetic chemistry.

关键词： Actinides Hydroboration Uranium Uraniumcatalyst Triamidoamines

A novel 3D sp2 carbon-linked covalent organic framework as a platform for efficient electro-extraction of Uranium

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Science China Chemistry 2023年第2期66卷 562-569页

作者： Cheng-Rong Zhang Jia-Xin Qi Wei-Rong Cui Xiao-Juan Chen Xin Liu Shun-Mo Yi Cheng-Peng Niu Ru-Ping Liang Jian-Ding Qiu State Key Laboratory of Nuclear Resources and Environment East China University of TechnologyNanchang330013China College of Chemistry Nanchang UniversityNanchang330031China

Extracting Uranium from seawater offers opportunities for sustainable nuclear fuel supply,but the task is quite challenging due to the low Uranium concentration(~3 ppb)in seawater.Here,based on the Knoevenagel condensation reaction of aldehyde and acetonitrile groups,a novel stable sp^(2)carbon-linked three-dimensional covalent organic framework(3D COF),TFPM-PDANAO was prepared as a porous platform for Uranium extraction from seawater.The TFPM-PDAN-AO designed with regular 3D pore channel of 7.12 A provides a specific channel for uranyl diffusion,which exhibits high selectivity and fast kinetics for Uranium adsorption.Meanwhile,the superior stability and optoelectronic properties enable it an excellent porous platform for Uranium electroextraction.By applying alternating voltages between-5 and 0 V,uranyl ions can rapidly migrate and enrich into the porous structure of TFPM-PDAN-AO,then inducing the electrodeposition of Uranium compounds to form the charge neutral species(Na_(2)O(UO_(3)H_(2)O)x)with an unprecedentedly high adsorption capacity of 4,685 mg g^(-1).This work not only expands the application prospects of functionalized 3D COFs,but also provides a technical support for the electrodeposition adsorption of Uranium from seawater.

关键词： three-dimension covalent organic framework Uranium adsorption electrosorption

Facile preparation of covalent organic frameworks@alginate composite beads for enhanced Uranium(Ⅵ) adsorption

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Rare Metals 2022年第4期41卷 1323-1331页

作者： Pan Duan Duo-Yu Lin Wei-Ting Yang Xiao-Jing Huang A-Hui Sun Qin-He Pan Key Laboratory of Advanced Materials of Tropical Island Resources Ministry of EducationChemical Engineering and TechnologyHainan UniversityHaikou 570228China

Covalent organic frameworks(COFs) have broad application prospects in adsorption and separation.Yet,as COFs are generally in powder form,their superior performance at the laboratory scale is difficult to transfer into pilot-or industrial-scale use.Thus,there is a strong and urgent need to structure COFs into monolithic materials.Herein,a facile strategy was developed to prepare COFs@alginate composite beads.Three composite beads comprising different COFs including TpPa-1(2,4,6-triformylphloroglucinol(Tp) and p-phenylenediamine(Pa-1)as monomers),TpDb(Tp and 2,5-diaminobenzonitrile(Db)as monomers) and TpTt(Tp and 1,3,5-triazine-2,4,6-triamine(Tt) as monomers) with controlled COF loading and product size have been facilely achieved via this strategy,validating the applicability of this method.Furthermore,the representative TpDb@alginate composite beads showed good adsorption performance of Uranium(VI) in aqueous solution with high adsorption capacity(635 mg·g^(-1)),good interference immunity and recyclability.This work offers a practical approach for incorporation of COFs into polymer matrix,which can serve as potential adsorbents for radioactive wastewater treatment.

关键词： Covalent organic frameworks Alginate Composite beads Uranium Adsorption

In-situ oxidized tungsten disulfide nanosheets achieve ultrafast photocatalytic extraction of Uranium through hydroxyl-mediated binding and reduction

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Nano Research 2022年第10期15卷 8810-8818页

作者： Huanhuan Liu Jia Lei Changyao Gong Ye Li Huimei Chen Jiali Chen Fengchun Wen Dengjiang Fu Yan Liu Wenkun Zhu Rong He State Key Laboratory of Environment-friendly Energy Materials National Co-innovation Center for Nuclear Waste Disposal and Environmental SafetySichuan Civil-military Integration InstituteSouthwest University of Science and TechnologyMianyang 621010China College of Chemistry and Materials Science Anhui Normal UniversityWuhu 241002China

Photoreduction of hexavalent Uranium(U(VI))by semiconductor provides a novel and effective avenue for Uranium extraction.Unfortunately,the traditional metal oxide and sulfide semiconductors suffer from the lack of confinement sites to U(VI),which resulted in the long period(~1 h)to achieve a high U(VI)extraction efficiency of>90%.Herein,we successfully constructed WS2 nanosheets and created in-situ oxidized domains on the surfaces(O-WS_(2))to promote the Uranium extraction and the corresponding removal kinetics.In this system,the O_(7.7-)WS_(2) nanosheets exhibited a considerable U(VI)extraction efficiency of>90%within 20 min in 8 mg·L^(–1) U(VI)-containing solution,which represented the highly efficient U(VI)removal performance.In 200 mg·L^(–1) U(VI)-containing solution,the O7.7-WS2 nanosheets exhibited an extraction capacity of 652.4 mg·g^(-1).The mechanism study revealed that the oxidized surface tended to trap hydrogen atom and in-situ form hydroxyl groups in defect sites.Evidenced by a series of experiment,such as kinetic isotope effect,1H nuclear magnetic resonance(NMR)spectra,and X-ray absorption near-edge structure(XANES)spectra,the in-situ formed hydroxyl groups participated in the Uranium reduction,which dramatically enhanced Uranium extraction kinetics and efficiency.

关键词： in-situ oxidization WS_(2)nanosheets hydroxyl groups Uranium photoreduction ABSTRACT

Application of sequential extraction for analyzing source and sink of Uranium in Huanghe River sediments,China

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Journal of Oceanology and Limnology 2023年第3期41卷 936-946页

作者： Xihuang ZHONG Xueyan JIANG Huijun HE Wenwen ZHANG Chunxia MENG Feng SUN Key Laboratory of Marine Chemistry Theory and Technology of Ministry of Education Ocean University of ChinaQingdao 266100China College of Chemistry and Chemical Engineering Ocean University of ChinaQingdao 266100China School of Materials Science and Engineering Ocean University of ChinaQingdao 266100China

Geochemical behaviors of heavy metals are closely related to their chemical state that can be divided by sequential extraction into exchangeable(F1),bound to carbonates(F2),bound to Fe-Mn oxides(F3),bound to organic matter or sulfide(F4),and residual(F5).Uranium in sediment of the Huanghe(Yellow)River,China,in different chemical states was extracted using the five-step procedure of Tessier and the source and sink were analyzed.Results show that more than 70%of the total Uranium was immobile residual F5 in abundance,followed in order of F4>F3>F2>F1,indicating that the main source of Uranium in the sediments was from weathered rock in the drainage basin.In addition,the Uranium in the sediments presents potential exogenous input in the Lanzhou,Baotou,and Tongguan reach.Fe-Mn oxides are main carriers of unstable Uranium,especially those of F1 and F3.Calcite and illite are secondary adsorption minerals of unstable Uranium in sediments under natural conditions.Human activities can also produce an obvious impact on Uranium speciation.This study provides a reference for the application of sequential extraction in analyzing the source and sink of Uranium in river sediments.

关键词： Uranium sequential extraction mineral composition sediment Huanghe(Yellow)River

Hydrogen-incorporated vanadium dioxide nanosheets enable efficient Uranium confinement and photoreduction

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Nano Research 2022年第4期15卷 2943-2951页

作者： Huanhuan Liu Jia Lei Jiali Chen Ye Li Changyao Gong Shangjie Yang Yamin Zheng Ning Lu Yan Liu Wenkun Zhu Rong He State Key Laboratory of Environment-friendly Energy Materials National Co-innovation Center for Nuclear Waste Disposal and Environmental SafetySichuan Civil-military Integration InstituteSouthwest University of Science and TechnologyMianyang 621010China College of Chemistry and Materials Science Anhui Normal UniversityWuhu 241002China

Photocatalytic reduction of U(VI)represents a novel and effective manner for the removal of U(VI)pollutant from radioactive wastewater.Herein,we successfully incorporated hydrogen into VO_(2)nanosheets,which strengthened the interaction between VO_(2)and U(VI),thereby achieving a highly active and stable photocatalyst for U(VI)reduction.With the increase of H content in hydric VO_(2)(H_(x)-VO_(2))nanosheets,the bandgap shrank from 2.29 to 1.66 eV,whereas the position of conduction bands remained more negative than the reduction potential of U(VI)/U(IV)(0.41 V vs.NHE).When irradiated by simulated sunlight,the U(VI)removal efficiency over H0.613-VO_(2)nanosheets reached up to 95.4%within 90 min,which largely outperformed 28.3%of pristine VO_(2)nanosheets.The mechanistic study demonstrated that the hydroxylated surface gave rise to the balanced O confinement sites in VO_(2)(011),leading to the stabilized adsorption configuration and increased binding strength of UO_(2)^(2+)on H_(x)-VO_(2)nanosheets.

关键词： VO_(2)nanosheets hydroxylated surface confinement photoreduction Uranium

New Identification of Quaternary Uranium Mineralization at the Mianhuakeng Granite-Related Uranium Deposit,South China

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地球科学学刊:英文版 2023年第5期34卷 1635-1640页

作者： Long Zhang Fangyue Wang Ore Deposit and Exploration Centre School of Resources and Environmental EngineeringHefei University of TechnologyHefei 230009China Anhui Province Engineering Research Center for Mineral Resources and Mine Environments Hefei 230009China

0 INTRODUCTION Granite-related Uranium deposits are one of the most important types of Uranium deposits in South China,and their genetic model generally involves Uranium leaching from the preexisting rocks(mainly granites),U transport as uranyl carbonate and fluoride complexes and probably chloride complexes in hydrothermal solutions,and U precipitation caused by physicochemical changes(Chi et al.,2020;Hu et al.,2008).Mineralization ages of granite-related Uranium deposits in South China have been a subject of significant controversy among researchers and were investigated using several methods,such as bulk uraninite U-Pb isotopic dating,in situ analytical techniques,pyrite Rb-Sr dating as well as bulk uraninite Sm-Nd dating(e.g.,Zhang et al.,2022;Zhong et al.,2019;Bonnetti et al.,2018;Luo et al.,2015;Huang et al.,2010;Ye,2005).

关键词： dating Uranium Bonnet