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nuclear Science and Techniques 2023年第4期34卷 1-13页

作者： Hang Zhang Yin-Yong Ao Yue Wang Shang-Jie Zhao Jia-Yang Sun Mao-Lin Zhai Jiu-Qiang Li Jing Peng Hui-Bo Li Department of radiochemistry China Institute of Atomic EnergyBeijing 102413China Beijing National Laboratory for Molecular Sciences Radiochemistry and Radiation Chemistry Key Laboratory for Fundamental ScienceCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Institute of nuclear Physics and Chemistry China Academy of Engineering PhysicsMianyang 621900China

N,N,N′,N′-Tetraoctyl diglycolamide(TODGA)is one of the most promising extractants tailored for high-level liquid radioactive waste treatment during nuclear fuel ***γ-radiolysis of TODGA(0.2 mol/L)in n-dodecane(n DD)solution with and without pre-equilibrated 3.0 mol/L HNO_(3)was investigated using HPLC and UPLC-QTOF-MS and compared with theγ-radiolysis of neat TODGA in this *** increased absorbed doses,the concentration of TODGA decreased exponentially for the studied ***,pre-equilibration with HNO_(3)(3.0 mol/L)slightly influenced theγ-radiolysis of TODGA in n *** radiolytic products generated from the rupture of the C–C,C–O,and C–N bonds in TODGA were identified in the studied extraction *** influence ofγ-radiation on TODGA/n DD for the extraction of Eu(Ⅲ)was evaluated using the first combination of extraction experiments and density functional theory(DFT)calculations,in which the complexations of Eu(Ⅲ)with TODGA and its radiolytic products were systematically *** on the radiolysis kinetic model of TODGA,the slope curve of the distribution ratio of Eu(Ⅲ)(D_(Eu))and the absorbed dose,and fluorescence titration analysis,the empirical equation of the absorbed dose and D_(Eu)was obtained *** 300 kGy,the experimental D_(Eu)agreed well with the obtained empirical equation for TODGA/n ***,at a high absorbed dose,the experimental D_(Eu)was higher than the theoretical D_(Eu)based on the empirical equation because the radiolytic products of TODGA with similar coordination structures still possessed partial complexation toward Eu(Ⅲ),which was confirmed by DFT *** work provides a method to predict the extraction distribution ratio of an irradiated extractant system and to understand the complex extraction process.

关键词： TODGA Radiolytic products Extraction Density functional theory Complexation

Synthetic Control of Thorium Metal-Organic Frameworks for Sequencing and Sensing of Radioiodine Species

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Chinese Journal of Chemistry 2024年第1期42卷 20-28,I0004页

作者： Yu Ju Zi-Jian Li xue Wang Jie Qiu Yiuhon Chan Zhi-Hui Zhang Mingyang He Jian Lin Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology Changzhou UniversityNo.21Gehu Middle RoadChangzhouJiangsu 213164China Schoolof nuclear Science and Technology Xi'an Jiaotong UniversityNo.28West Xianning RoadXianShaanxi 710049China Key Laboratoryof Interfacial Physics and Technology Shanghai Institute of Applied PhysicsChinese Academy of Sciences2019JiaLuoRoadShanghai 201800China

Exploring the physiochemical properties and expanding the applications of actinide-containing materials is paramount to address the escalating challenge of radioactive waste ***,unlocking the full potential of these materials is largely crippled by the radiotoxicity of the *** report here two porous and luminescent thorium-based metal-organic frameworks(Th-BITD-1 and Th-BITD-2)that serve as a bifunctional platform for sequencing and sensing of radioiodine,a much more radioactive fission product discharged during the nuclear fuel *** particular,Th-BITD-1 displays better iodine uptake performance than Th-BITD-2 via the solution-based process and vapor diffusion with the maximum adsorption capacities of 831 and 1099 mg/g,*** thermore,Th-BITD-1 can function as a highly sensitive luminescence sensor for iodate with a quenching constant(Ksv)of 6.6(5)×10^(3) M^(-1)and a detection limit of 2.02μM,respectively,outperforming 2.96(6)×10^(3)M^(-1)and 10.5μM of ***,a positive correlation between the sensing efficacy and the iodate adsorption capacity has been *** work highlights the opportunity in designing novel actinide-based MOFs for their potential applications in radiological fields,e.g.,radionuclide separation and detection.

关键词： Thorium Metal-organic frameworks Adsorption Detection lodine Actinides radiochemistry Luminescence

Effect of pH,fulvic acid and temperature on the sorption of uranyl on ZrP_2O_7

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Science China Chemistry 2010年第6期53卷 1429-1437页

作者： QIAN LiJuan,HU PeiZhuo,JIANG ZhenJiang,GENG YanXia & WU WangSuo radiochemistry Laboratory,School of nuclear Science and Technology,Lanzhou University,Lanzhou 73000,China radiochemistry Laboratory School of Nuclear Science and Technology Lanzhou University Lanzhou China

The sorption of UO22+ onto ZrP2O7 was studied using the batch technique and the point of zero charge of ZrP2O7 was obtained through mass *** results indicated that sorption of UO22+ onto ZrP2O7 was strongly affected by pH,solid-to-liquid ratio (m/V),the species of electrolyte in solution and fulvic acid (FA),but was insensitive to ionic *** sorption of UO22+ increased with increasing pH and m/*** presence of FA enhanced UO22+ sorption onto ZrP2O7 at low *** presence of phosphate or sulfate caused opposite effects on the sorption of UO22+ onto *** of citrate also significantly affected UO22+ *** sorption of UO22+ increased as the temperature of the system *** Langmuir and Freundlich models were used to simulate the sorption isotherms of UO22+ onto ZrP2O7 at different *** results indicated that the Freundlich model described UO22+ sorption better than the Langmuir *** parameters for the sorption process were calculated from the temperature dependent sorption *** results suggested that the sorption process of UO22+ onto ZrP2O7 is spontaneous and *** desorption process of UO22+ from ZrP2O7 was also investigated and it was found that sorption onto ZrP2O7 was irreversible.

关键词： ZrP2O7 uranyl sorption desorption thermodynamic data

The sorption mechanisms of Th(Ⅳ) on attapulgite

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Science China Chemistry 2011年第7期54卷 1138-1147页

作者： PAN DuoQiang FAN QiaoHui DING KeFei LI Ping LU Yan YU Tao XU Jiang WU WangSuo radiochemistry Laboratory School of Nuclear Science and Technology Lanzhou University Lanzhou 730000 China

The surface properties of intrinsic and activated attapulgite were studied using potentiometric *** sorption mechanisms of Th(IV) on intrinsic and activated attapulgite were investigated by employing surface complexation model and FITEQL 3.2 *** results indicated that the sorption sites of intrinsic attapulgite involved in the sorption process were main ion exchange site(≡ XNa/K),strong site(≡ SsOH) and weak site(≡ SwOH),while only strong site(≡ SsOH) and weak site(≡ SwOH) were predominant for activated *** pH < 2.5,the species of Th(IV) was main Th4+ in aqueous solution;then the hydrolysis species of Th(IV)(i.e.,Th(OH)22+,Th(OH)+3 and Th(OH)04) gradually formed as pH *** the sorption of Th(IV) on intrinsic attapulgite,both ion exchange species(≡ X2Th) and inner-sphere surface complexes(≡ SsOTh) were dominant,while only inner-sphere surface complexes(i.e.,≡ SsOThOH and ≡ SwOTh) were observed for Th(IV) sorption to activated *** the presence of humic acid(HA),the sorption of Th(IV) on activated attapulgite was obviously enhanced;and both ≡ SsOH-HA-Th and ≡ SsOTh were the predominant *** was also interesting to find that the addition of HA obviously provoked the desorption behavior of Th(IV).

关键词：凹凸棒石粘土吸附机制表面复合物钍表面络合模型离子交换电位滴定法表面性能

Eu(III) adsorption on rutile:Batch experiments and modeling

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Science China Chemistry 2010年第12期53卷 2628-2636页

作者： WANG XueFeng,SHI KeLiang,GUO ZhiJun & WU WangSuo radiochemistry Lab,School of nuclear Science and Technology,Lanzhou University,Lanzhou 730000,China radiochemistry Lab School of Nuclear Science and Technology Lanzhou University Lanzhou China

Eu(III) adsorption on rutile was investigated as a function of contact time,pH,ionic strength and Eu(III) concentration by using a batch experimental *** effects of carbonate,sulfate,and phosphate were also *** was found that the kinetics of Eu(III) adsorption on rutile could be described by a pseudo-second-order *** adsorption of Eu(III) on rutile is strongly pH-dependent,but relatively insensitive to ionic strength.A double layer model (DLM) with two inner-sphere Eu(III) surface complexes was applied to quantitatively interpret the adsorption of Eu(III) on *** were no apparent effects of carbonate and sulfate on Eu(III) adsorption,whereas the presence of phosphate promoted Eu(III) adsorption on *** surface complexes of Eu(III) on rutile were evidenced by X-ray photoelectron spectroscopy (XPS).

关键词： Eu(III) adsorption rutile kinetics surface complexation modeling XPS

China's progress in radionuclide migration study over the past decade(2010–2021):Sorption,transport and radioactive colloid

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Chinese Chemical Letters 2022年第7期33卷 3405-3412页

作者： Zongyuan Chen Siyuan Wang Huijuan Hou Kang Chen Pengyuan Gao Zhen Zhang Qiang Jin Duoqiang Pan Zhijun Guo Wangsuo Wu Frontiers Science Center for Rare Isotopes Lanzhou UniversityLanzhou 730000China The Key Laboratory of Special Function Materials and Structure Design Ministry of EducationLanzhou UniversityLanzhou 730000China radiochemistry Laboratory School of Nuclear Science and TechnologyLanzhou UniversityLanzhou 730000China

The radionuclide(RN)migration study is not only helpful to understand environmental behavior of RNs,but also can establish the basis for the safety assessment of geological disposal of high-level radioactive waste(HLW).In the context of China’s HLW disposal,this review briefly summaries the progress of China’s RN migration studies over the past decade regarding three aspects,RN sorption,RN transport and radioactive *** studies from other disciplines(such as geology and environmental science)are also included in this review because they can provide references for the RN migration ***,China has achieved clear progress in RN migration study over the past decade,although large-scaled field experiments are lacked and a gap still exists comparing with the international advanced ***,several suggestions are proposed for future RN migration research in China.

关键词： High-level radioactive waste Sorption Transport Colloid Spectroscopic analysis Theoretical calculation

Dication-accelerated anion transport inside micropores for the rapid decontamination of pertechnetate

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nuclear Science and Techniques 2022年第4期33卷 19-32页

作者： Peng Zhang Yi-Zhi Chen Han-Qin Weng Zi-Fang Guo Jia-Liang Chen Xing Zhao Guo-An Ye Ming-Zhang Lin School of nuclear Science and Technology University of Science and Technology of ChinaHefei 230026China Department of Beam Material Science SANKENThe Institute of Scientific and Industrial ResearchOsaka University8-1 MihogaokaIbarakiOsaka 567-0047Japan radiochemistry Department of China Institute of Atomic Energy China Institute of Atomic EnergyBeijing 102413China

Over 70%of the treated contaminated water at the Fukushima Daiichi nuclear Power Station contains radionuclides beyond the regulatory standard for discharge that need to be ***-99(^(99)Tc),mainly in the form of pertechnetate Tc(VII)O_(4)^(-),is one of the main sources of long-term radiotoxicity that jeopardizes the environment and human ***,we used a series of dicationic pyridinium(DCP)derivative groups(–Py^(+)C_(n)H_(2n)N^(+)Me_(3),n=2,3,and 5)to modify commercial Reillex 425 resins containing tertiary pyridyl groups to improve the adsorption performance of rhenium(Re,an analog of radioactive Tc)and *** the quaternary pyridinium and ammonium sites in one DCP group can adsorb ReO_(4)^(-) simultaneously,DCP-modified Reillex 425(Reillex-Cn)exhibited high maximum adsorption capacities for Re under neutral *** capacities reached 344.8,416.7,and 588.2 mg g^(-)1 for Reillex 425-C2,Reillex 425-C3,and Reillex 425-C5,*** diffusion of ReO_(4)^(-)/TcO_(4)^(-) in Reillex 425-Cn was verified to be the rate-limiting step of ***,adsorption can be adjusted by the length of the alkyl spacers between the two positively charged N sites in DCP.–Py^(+)C_(2)H_(4)N^(+)Me_(3) significantly enhanced intraparticle diffusion compared to–Py^(+)C_(5)H_(10)N^(+)Me_(3).The two positive sites in–Py^(+)C_(2)H_(4)N^(+)Me_(3) would be laterally distributed,leading to a smaller steric hindrance for ReO_(4)–/TcO_(4)^(-) transport inside the microporous ***,the longer alkyl spacers in–Py^(+)C_(5)H_(10)N^(+)Me_(3) formed hydrophobic microphases,repulsing the hydrated ReO_(4)–/TcO_(4)^(-) ***,the adsorptions of both ReO_(4)^(-) and TcO_(4)^(-) on Reillex 425-C2 were faster than those on Reillex ***,Reillex 425-Cn exhibited an exothermic nature,good selectivity,excellent reusability,and strong salinity *** study provides a simple strategy to enhance the Tc removal performance

关键词： Quaternary pyridinium Dicationic pyridyl derivatives Pertechnetate Intraparticle diffusion

Gamma and alpha radiolysis of TBP solvent

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nuclear Science and Techniques 2015年第1期26卷 72-77页

作者：高杨郑卫芳曹晓明陈少雷 Fundamental Science on nuclear Safety and Simulation Technology Lab Harbin Engineering University Department of radiochemistry China Institute of Atomic Energy

In light of the problem of radiolysis of the solvent system in PUREX(plutonium uranium recovery by extraction) process, γ and α irradiation stabilities of tributylphosphate(TBP)/n-dodecane/nitric acid system were studied using60 Co γ-rays and α particles from238 Pu. The main degradation products, dibutyl phosphate(HDBP)and monobutyl phosphate(H2MBP) were detected by the gas chromatography-mass spectrometry(GC-MS),and the degradation products that could not be easily removed by the washing procedure were measured by the Pu retention. Effects of the absorbed dose, the HNO3 concentration, and the cumulative dose on the irradiation stability of the systems were investigated. The yields of HDBP, H2 MBP and the Pu retention increased with the absorbed dose. The HNO3 concentration affected significantly on the yield of HDBP, but had little impact on the output of H2 MBP and Pu retention. For a similar absorbed dose, the Pu retention of the solvent by alpha irradiation is larger than that by gamma irradiation.

关键词：溶剂体系 TBP 磷酸三丁酯 HDBP 吸收剂量钚238 降解产物磷酸二丁酯

Altitude-dependent distribution of 137Cs in the environment:a case study of Aragats massif, Armenia

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Acta Geochimica 2020年第1期39卷 127-138页

作者： Konstantin Pyuskyulyan Stephen P.LaMont Vovik Atoyan Olga Belyaeva Nona Movsisyan Armen Saghatelyan Armenian nuclear Power Plant MetsamorArmenia nuclear and radiochemistry Los Alamos National LaboratoryLos AlamosUSA Radioecology Department Center for Ecological-Noosphere StudiesNAS RA.YerevanArmenia

This paper considers the distribution of technogenic 137Cs and naturally occurring radionuclides:238 U,232 Th and40 R concentrations in soils and 137Cs in atmospheric dry depositions by altitudinal belts of the Aragats mountain massif,Republic of *** soil samples were collected at altitudes from 1000 to 3200 *** the determination of geochemical variability,two soil sampling campaigns were *** dry depositions were sampled from five stations at1100-3200 m collected onto organic fiber filters between June and December 2016.137Cs activity was measured using a high-purity Germanium detector coupled to a multichannel analyzer(Canberra).Results indicated that specific activity of 137Cs in soils at 1000 m is495-528 Bq m^-2,andat3200 mis10,500-11,470 Bq m^-*** correlation observed for 137Cs versus naturally occurring radionuclides,which varies in distribution by *** activities of 137Cs in dry atmospheric depositions varies from 1.06 at 846 m to2.37 Bq m^-2 per quarter at 3200 m and increases as the altitude *** of 137Cs in soil and dry atmospheric deposition correlated significantly,and 137Cs activity in soils and atmospheric dry depositions decrease as the absolute altitude *** 50-year effective dose from exposure to 137Cs fallout varies with altitude from 0.007 to 1.42 m Sv.

关键词： 137Cs Distribution by altitude Naturally occurring radionuclides Topsoil Dry atmospheric depositions Gamma radiation Mountain regions