模拟ThO2辐照靶件中微量233U提取工艺研究

为了从模拟ThO2辐照靶件中分离提取微量铀,系统考察了基于TBP萃取剂的溶剂萃取法和基于Dowex 1×8阴离子交换树脂的离子交换法的工艺参数。在最优工艺条件下,通过比较铀回收率、铀中钍及裂变产物的去污因子、分离流程耗时及废物产生量等关键工艺参数,系统评估了这两种方法从钍中分离提取微量铀的优缺点。结果表明,在小批量样品分离中(5~10 g ThO2),阴离子交换法优于溶剂萃取法,该工艺得到的铀产品中裂变产物的含量均小于0.01%,钍的含量小于0.02%,铀的回收率为98.3%。一次流程耗时约5 h,产生废物量约500 mL。本文研究结果可为下一步辐照ThO2制备233U的台架实验及分离装置的设计与加工提供关键技术参数。

热堆制备低放射性233U的钍铀转换方法

233 U比235 U具有更好的燃料特性,是具有潜在重要应用价值的核燃料,但直接使用钍铀或钍钚混合燃料在堆中辐照得到的233 U,含有大量的232 U及234 U,放射性较强,难以像235 U一样作为常规核燃料使用。基于低放射性233 U的制备需求,本文分析了232 Th-233 U转化中U同位素杂质232 U及234 U的产生途径,采用可有效减少232 U生成的热堆辐照思路,研究了热堆制备低放射性233 U的辐照工艺。利用MCNP程序对232 Th样品在西安脉冲堆堆内辐照过程进行建模,分析了辐照时间、冷却时间、多个“辐照-冷却”周期法辐照及中间产物230 Th对辐照产物的影响,给出了西安脉冲堆制备低放射性233 U辐照工艺。研究结果表明,本文制备的低放射性233 U产品中233 U的质量分数为10^-5量级,232 U、234 U与233 U的质量比分别小于10^-6和10^-3,符合低放射性233 U指标要求。

GEF模型对n+233U反应裂变碎片质量分布的研究

General Fission(GEF)模型是描述裂变过程的一种半经验模型,它运用了量子力学和统计力学中的物理概念,并结合经验信息调整出了一组适用于不同裂变系统的参数,可以对大量原子核的裂变可观测量给出可靠的预测.本工作使用GEF模型计算了233U中子诱发裂变产额的质量分布.结果表明,随着入射中子能量增加,对称裂变贡献逐渐增大,非对称裂变贡献逐渐减小;考虑了多次机会裂变,(n,f)裂变道相对贡献随着入射中子能量增加逐渐降低,而其他裂变道贡献增加;裂变产物的产额能量变化趋势与其在质量分布上的不同位置有关.

Plutonium utilization in a small modular molten-salt reactor based on a batch fuel reprocessing scheme

A molten salt reactor(MSR)has outstanding features considering the application of thorium fuel,inherent safety,sustainability,and resistance to proliferation.However,fissile material^(233)U is significantly rare at the current stage,thus it is difficult for MSR to achieve a pure thorium-uranium fuel cycle.Therefore,using plutonium or enriched uranium as the initial fuel for MSR is more practical.In this study,we aim to verify the feasibility of a small modular MSR that utilizes plutonium as the starting fuel(SM-MSR-Pu),and highlight its advantages and disadvantages.First,the structural design and fuel management scheme of the SM-MSR-Pu were presented.Second,the neutronic characteristics,such as the graphite-irradiation lifetime,burn-up performance,and coefficient of temperature reactivity were calculated to analyze the physical characteristics of the SM-MSR-Pu.The results indicate that plutonium is a feasible and advantageous starting fuel for a SM-MSR;however,there are certain shortcomings that need to be solved.In a 250 MWth SM-MSR-Pu,approximately 288.64 kg^(233)U of plutonium with a purity of greater than 90% is produced while 978.00 kg is burned every ten years.The temperature reactivity coefficient decreases from -4.0 to -6.5 pcm K^(-1) over the 50-year operating time,which ensures a long-term safe operation.However,the amount of plutonium and accumulation of minor actinides(MAs)would increase as the burn-up time increases,and the annual production and purity of^(233)U will decrease.To achieve an optimal burn-up performance,setting the entire operation time to 30 years is advisable.Regardless,more than 3600 kg of plutonium eventually accumulate in the core.Further research is required to effectively utilize this accumulated plutonium.

Analysis of burnup performance and temperature coefficient for a small modular molten‑salt reactor started with plutonium

In a thorium-based molten salt reactor(TMSR),it is difficult to achieve the pure 232Th–^(233)U fuel cycle without sufficient^(233)U fuel supply.Therefore,the original molten salt reactor was designed to use enriched uranium or plutonium as the starting fuel.By exploiting plutonium as the starting fuel and thorium as the fertile fuel,the high-purity^(233)U produced can be separated from the spent fuel by fluorination volatilization.Therefore,the molten salt reactor started with plutonium can be designed as a^(233)U breeder with the burning plutonium extracted from a pressurized water reactor(PWR).Combining these advantages,the study of the physical properties of plutonium-activated salt reactors is attractive.This study mainly focused on the burnup performance and temperature reactivity coefficient of a small modular molten-salt reactor started with plutonium(SM-MSR-Pu).The neutron spectra,^(233)U production,plutonium incineration,minor actinide(MA)residues,and temperature reactivity coefficients for different fuel salt volume fractions(VF)and hexagon pitch(P)sizes were calculated to analyze the burnup behavior in the SM-SMR-Pu.Based on the comparative analysis results of the burn-up calculation,a lower VF and larger P size are more beneficial for improving the burnup performance.However,from a passive safety perspective,a higher fuel volume fraction and smaller hexagon pitch size are necessary to achieve a deep negative feedback coefficient.Therefore,an excellent burnup performance and a deep negative temperature feedback coefficient are incompatible,and the optimal design range is relatively narrow in the optimized design of an SM-MSR-Pu.In a comprehensive consideration,P=20 cm and VF=20%are considered to be relatively balanced design parameters.Based on the fuel off-line batching scheme,a 250 MWth SM-MSR-Pu can produce approximately 29.83 kg of ^(233)U,incinerate 98.29 kg of plutonium,and accumulate 14.70 kg of MAs per year,and the temperature reactivity coefficient can always be lower than−4.0pcm/K.

^(233)U评价数据的临界基准检验

为检验和改进233 U核反应全套中子评价数据的质量,从国际核临界安全手册ICSBEP中选取快谱、超热谱和热谱临界基准实验装置,对中国评价核数据库CENDL-3.1、美国评价核数据库ENDF/B-Ⅶ.0、日本评价核数据JENDL-3.3和JENDL-4.0中的233 U评价数据进行了基准检验。采用蒙特卡罗程序MCNP5计算了所选基准装置的有效增殖因数keff,并与基准值进行比较。运用基于能谱指标的趋势分析、灵敏度分析等方法进行了分析。在基准检验中,现有的233 U评价数据的主要问题是从热临界基准中能谱较硬的装置到超热谱基准装置再到部分快谱临界基准装置,较为普遍地存在keff的严重低估。从热堆设计角度考虑,ENDF/B-Ⅶ.0库233 U评价数据表现较好,但仍高估了共振俘获的贡献。

ThO2反应堆辐照后的核素分离与分析

在高通量堆(High Flux Engineering Test Reactor,HFETR)内辐照了 ThO2 样品,利用三氟甲烷磺酸(Trifluoromethanesulfonic Acid,TFMS)将辐照后的ThO2样品溶解,对辐照产生的233Pa和95Zr、103Ru、137Cs等裂片核素进行了分析,获得各核素相对于Th的产额;利用磷酸三丁酯(Tributyl Phosphate,TBP)萃淋树脂对铀/钍进行了分离,并用电感耦合等离子体质谱(Inductively Coupled Plasma Mass Spectrometry,ICP-MS)γ谱仪对辐照生成的U含量进行了测算。在热中子注量1.32×10^20 n·cm^-2(快/热中子比约2.8∶1)条件下,7.1 mg辐照后的二氧化钍中233U含量为8.01 μg(产额为0.128%,U/Th),232U含量为1.21×10^-4 μg,^232U/^233U为1.51×10^-5。

氢化锆慢化熔盐堆钍铀转换性能初步分析

中子能谱对钍基燃料在熔盐堆中的利用效率及温度反馈系数等安全问题有较大影响,所以对熔盐堆新型慢化剂的研究具有重要意义。本工作基于SCALE6计算程序,对不同几何栅元结构的氢化锆栅元组件在熔盐堆的物理性能进行了研究,分别计算了中子能谱、钍铀转换比、^(233)U浓度、总温度反馈系数以及燃耗等中子物理参量。结果表明,减小六边形栅元对边距或者增加熔盐占栅元体积比可以增加钍铀转换比和改善温度反应性系数;当加入的氢化锆慢化剂体积份额为0.1时就可以将熔盐堆^(233)U初始浓度降低到2.5×10^(-2)以内;氢化锆慢化熔盐堆在超热谱条件下,其^(233)U初装载量和超铀核素产量较小,同时堆芯较为紧凑。

^(233)U内标α谱法测定石墨中痕量^(239)Pu

在石墨粉末试样中加入2 33U作内标 ,用硝酸浸取样品中的Pu ,移取上层清液制成α源。用α谱仪测定2 33U和2 39Pu的α计数比 ,通过加入内标2 33U的已知量和2 33U、2 39Pu的相关参数 ,可求得2 39Pu的绝对量。该分析方法可测2 39Pu的含量为 0 1～ 10 μg/ g ,测量精密度 (n =6)优于 2 %。

热堆中钍铀转化规律

钍铀燃料循环以其优异的物理和化学特性,受到核能界的广泛关注。本文利用单群的点燃耗计算程序ORIGEN,分别研究了钍燃料在沸水堆(Boiling Water Reactor,BWR)、压水堆(Pressurized Water Reactor,PWR)和加拿大重水铀反应堆(Canada Deuterium Oxide Uranium,CANDU,又称坎杜堆)能谱中辐照时,232Th、233Th、233Pa、233U等核素生成量随中子注量率和中子能谱的变化规律,并探索了多次"辐照-冷却"循环对钍铀转化率的影响。计算结果表明,能谱相同时,233Th和233Pa存量的最大值与注量率有关;233U存量的最大值与注量率无关,大概在注量(注量率×时间)为4×1016 n·cm-2左右;注量率相同时,能谱越硬,233U存量的最大值越大。采取循环"辐照-冷却"可以提高233Th-233U的转化率,对于相同的总辐照时间,每次循环周期内的辐照时间越短,相对于总辐照时间相同的单次辐照,转化率增量提高越明显;当总辐照时间超过两个月时,循环辐照对转化率增量的作用较小,与单次辐照不冷却相比,转化率相对增量不超过1倍。

Th-^(233)U热中子增殖堆某些物理特性的探讨

Th-^(233)U热中子增殖堆是一种尚末问世的第二代原子核反应堆。本文用热中子的物理参数并以钍在堆中衍生的^(233)U达到饱和值时作为堆燃料的更换周期,探讨了此类堆所具有的物理特性。初步结果表明:此类堆具有:1)钍的高耗损率;2)高的中子通量运行较为有利;3)进堆的^(233)U含量应尽可能低些;4)有着较深的燃耗等物理特性。

星座型裂变燃料核反应堆的物理构想

从分析钍在持续中子辐照过程中各代子体含量的演变出发,着重研究有多代子体均达到各自的饱和值时的情况和所具有的特性,提出星座型裂变物质核反应堆的物理构想,并就此堆的特性和应用前景作了简单阐述和讨论。

Calculation of Prompt Fission Neutron from ^(233)U(n, f) Reaction byMulti-Modal Los Alamos Model

An attempt is made to improve the evaluation of the prompt fission neutron emis- sion from 233U（n, f） reaction for incident neutron energies below 6 MeV. The multi-modal fission approach is applied to the improved version of Los Alamos model and the point by point model. The prompt fission neutron spectra and the prompt fission neutron as a function of fragment mass （usually named ＂sawtooth＂ data） v（A） are calculated independently for the three most dominant fission modes （standard I, standard II and superlong）, and the total spectra and v（A） are syn- thesized. The multi-modal parameters are determined on the basis of experimental data of fission fragment mass distributions. The present calculation results can describe the experimental data very well, and the proposed treatment is thus a useful tool for prompt fission neutron emission prediction.

Experimental Studies on the Self-Shielding Effect in Fissile Fuel Breeding Measurement in Thorium Oxide Pellets Irradiated with 14 MeV Neutrons

The 14 MeV neutrons produced in the D-T fusion reactions have the potential of breeding Uranium-233 fissile fuel from fertile material Thorium-232. In order to estimate the amount of U-233 produced, experiments are carried out by irradiating thorium dioxide pellets with neutrons produced from a 14 MeV neutron generator. The objective of the present work is to measure the reaction rates of 232Th ＋ in --＊ 233Th --＊ 2a^Pa --＊ 2a3U in different pellet thicknesses to study the self-shielding effects and adopt a procedure for correction. An appropriate assembly consisting of high-density polyethylene is designed and fabricated to slow down the high-energy neutrons, in which Thorium pellets are irradiated. The amount of fissile fuel （~3~U） produced is estimated by measuring the 312 keV gammas emitted by Protactinium-233 （half-life of 27 days）. A calibrated High Purity Germanium （HPGe） detector is used to measure the gamma ray spectrum. The amount of 233U produced by Th232 （n, ~） is calculated using MCNP code. The self-shielding effect is evaluated by calculating the reaction rates for different foil thickness. MCNP calculation results are compared with the experimental values and appropriate correction factors are estimated for self-shielding of neutrons and absorption of gamma rays.

高放废物中^(238)Pu、^(240)Pu、^(242)Pu在聚变-裂变混合堆内的嬗变研究

从中子学角度研究了高放废物中２３８Ｐｕ、２４０Ｐｕ、２４２Ｐｕ在聚变一裂变混合堆内擅变的可行性。选取２３３Ｕ做中子增殖剂，对四个不同燃料组分的快谱包层进行了设计，利用输运一燃耗程序ＢＩＤＥＡＹ对所选方案进行了计算分析，结果表明：用２３３Ｕ做中子增殖剂，在聚变一裂变混合堆快谱包层内擅变２３８Ｐｕ、２４０Ｐｕ、２４２Ｐｕ是安全可行的。

Analysis of Th-U breeding capability for an accelerator-driven subcritical molten salt reactor

Accelerator-driven systems based on molten salt fuel have several unique advantages and features for advanced nuclear fuel utilization.The aim of this work was to study the Th-U breeding capability in such systems,known as‘‘accelerator-driven subcritical molten salt reactors’’(ADS–MSRs).Breeding capacities including conversion ratio and net^(233)U production for various subcriticalities and different minor actinides(MA)loadings were analyzed for an ADS–MSR.The results show that the subcriticality of the core has a considerable effect on the Th-U breeding.A high subcriticality is favorable to improving the conversion ratio,increasing the net^(233)U production,and reducing the doubling time.Specifically,the doubling time for k_(eff)of 0.99 is larger than 80 years,while the counterpart for k_(eff)of 0.93 is only approximately22 years.Nevertheless,in an ADS–MSR with a high initial MA loading,MA results in a non-negligible^(233)U depletion in the first two decades,while increasing the net^(233)U production compared to reactors without MA loading.During the 50 years of operation,for the subcritical reactor(k_(eff)0:97)with MA fraction increasing from 1 to 14%,the net^(233)U production increases from 3.94 to 8.24 t.

Computational analysis of neutronic effects of ThO_2 rods loaded in CANDU 6 fuel assemblies

Thorium as a suitable fertile with higher natural resources in comparison with uranium resources has been remarkably considered by different nuclear energy user countries in the last decades. Its prominent features such as suitable possibility for power flattening of a nuclear reactor, applicable breeder blanket to produce^(233)U fissile as well as neutron leakage prevention from a nuclear core has caused its application as power flatter, breeder material or other aimed utilizations be evaluated by the researches. In the present study, neutronics of a modeled CANDU 6loaded with Th O_2 and UO_2fuel rods have been computationally studied. The study aimed at reprocessing of burned Th O_2 seeds at CANDU 6 reactor to recover the total produced uranium, which is to be going under another compound fuel cycle. The obtained results showed all the core reactivity coefficients are sufficiently negative. The modeled core 949 GWd burn-up concluding in 99.99 %depletion of^(235)U initial loads. 18.38 kg of^(233) U was produced in the burnt Th O_2 fuel after 1-year burn-up time. In addition, 31.84 kg of^(239) Pu was produced in the UO_2 spent fuel rods after the burn-up time. After a proposed cooling time, about 50.01 kg of^(233)U will be available in the spent Th O_2 fuel.

n+^(233)U裂变碎片质量分布的唯象模型研究

本模型基于裂变多通道无规颈断裂模型,考虑宏观液滴能、壳效应能以及壳效应与温度的关系,得到参数化的势能表示形式。通过拟合不同测量方法得到的实验数据(经过评价)获得3组模型参数。3组参数计算的碎片质量分布均很好地再现了不同能点的实验数据,除了基于动能法实验数据得到的参数外,其14 MeV的计算结果与实验数据符合较差。研究发现,不同入射中子能量的裂变碎片质量分布有4个主要交叉点,在交叉点之上的产额随入射中子能量增加减少,之下的产额则随入射中子能量上升;内侧(或外侧)的两个交叉点质量数之和近似等于裂变复合核的质量数;不同裂变系统的重峰左侧的交叉点都保持在132附近。

加速器驱动的次临界系统生产^(233)U的可行性研究

加速器驱动的次临界系统(Accelerator Driven Sub-critical System,ADS)是加速器技术和核反应堆技术的结合,其主要目的是应对当今快速增长的放射性核废料处理需求.本文初步探讨了在ADS系统中利用232Th生产可裂变核233U的可能性,估计了所需加速器的性能及其生产233U的产率和效率.我们建议用Be做中子慢化剂和增殖剂,将反应堆的中子能量大部分控制在1keV–1MeV,从而最大限度地降低232U的含量.也可进一步利用重水做慢化剂高233U的纯度.所生产的233U既可经分离取后在热堆中燃烧,也可直接用于钍基熔盐堆的初始装料,发挥233U优异的热中子性能.我们的结果表明,在技术上和经济上利用ADS生产233U很可能是可行的.我们的结果还表明,如果这一ADS系统主要目的是生产233U,所选择的次临界堆的最佳是快中子堆,而不是慢中子堆或快慢结合堆.最后我们建议对钍基核反应堆、233U的取分离工和辐射防护等方面的课开展进一步深入研究.

Updated and revised neutron reaction data for ^(233)U

A complete set of n＋233U neutron reaction data from 10-6 eV-20 MeV is updated and revised based on the evaluated experimental data and the feedback information of various benchmark tests, The main revised quantities are nubars, cross sections as well as angular distributions, etc. The benchmark tests indicate that the present evaluated data achieve very promising results.