压水堆中嬗变99Tc和129I的计算研究

选取大亚湾压水堆作为嬗变参考堆,研究在压水堆中嬗变长寿命裂变产物⁹⁹Tc和¹²⁹I的可行性。计算结果表明：在1个换料周期（18个月）内,⁹⁹Tc的最大嬗变率为15.69%,¹²⁹I的最大嬗变率为9.18%。通过对不同堆芯方案进行安全性分析发现：添加⁹⁹Tc和¹²⁹I后,堆芯有效增殖因数k_eff降低且随燃耗变化的幅度变小;堆芯径向中子通量密度分布无明显变化但径向功率峰因子降低;考虑燃料温度系数、慢化剂温度系数、硼微分价值以及控制棒价值等,得出在反应性温度系数及反应性控制方面不会导致安全问题,相反有优化作用。因此,从安全角度分析,在压水堆中嬗变⁹⁹Tc和¹²⁹I是可行的。     

低浓缩铀靶辐照后裂变核素产量的理论研究

用低浓缩铀靶代替高浓缩铀靶辐照进行⁹⁹Mo、¹³¹I等医用放射性核素生产是一个必然的趋势。本文利用输运计算程序DRAGON研究了靶件²³⁵U富集度、中子注量率、辐照时间对⁹⁹Mo、¹³¹I、⁹⁰Sr、⁹⁵Zr、²³⁹Pu等核素比活度变化的影响,以及不同²³⁵U富集度下裂变体系组成和总比活度的变化规律。计算结果表明,本文考察的10余种核素比活度的变化随辐照时间的不同而有所不同,其中⁹⁹Mo、¹³¹I、¹⁴⁷Nd和¹³³Xe等核素的比活度可快速达到饱和,⁸⁹Sr、¹⁰³Ru、⁹⁵Zr和¹⁴¹Ce等缓慢达到饱和,而⁹⁹Tc、⁸⁵Kr和⁹⁰Sr、²³⁹Pu在计算时间内达不到饱和,但所有核素的比活度随时间的变化趋势与靶件²³⁵U富集度无关;⁹⁹Mo、¹³¹I、⁹⁰Sr、⁹⁵Zr等核素的比活度均随靶件²³⁵U富集度提高而增加,而²³⁹Pu比活度则随着靶件富集度的减少而显著增加,提示改用低浓缩铀靶进行⁹⁹Mo、¹³¹I等医用放射性核素生产时应特别关注²³⁹Pu带来的影响;核素比活度随中子注量率的增加而线性增加,且斜率基本相同;靶件辐照时间的改变不会明显影响裂变体系的组成,在低浓缩铀（²³⁵U含量≤20%）区域,靶件²³⁵U富集度对裂变体系的组成影响很小。     

长寿命裂变产物在聚变驱动次临界堆包层中嬗变的中子学优化分析

商用裂变堆乏燃料中高放长寿命裂变产物(LLFP)由于其具有很强的放射毒性,所以对于它们的嬗变处理非常重要。在对世界上关于LLFP嬗变处理的广泛调研的基础上,考虑到LLFP的同位素分离技术的发展水平,选择了LLFP中99Tc、129I和135Cs的嬗变处理(?)料的化学形式,分析了不同慢化剂材料对嬗变能力的影响,同时针对聚变驱动次临界堆的多功能双冷核废料嬗变包层(DWTB)进行了LLFP嬗变的中子学设计和优化分析。     

SLEGS嬗变长寿命裂变产物135Cs的模拟

结合激光康普顿散射模拟程序4D-MCLCSS和Geant4软件包,模拟基于上海激光电子γ源（SLEGS）的γ光产生及其对长寿命裂变产物¹³⁵Cs的光核嬗变过程,研究嬗变率随嬗变靶几何参数的依赖关系,并初步诊断基于SLEGS的光核嬗变产物分布,获得¹³⁵Cs嬗变靶的最佳靶厚和半径分别为55 cm和0.6 cm,对应的嬗变率为1.62×10⁶ s^-1。研究结果表明,基于SLEGS的光核嬗变率较强激光驱动的轫致辐射的高1个量级,SLEGS非常适用于开展¹³⁵Cs等长寿命裂变产物的光核嬗变研究。     

西安脉冲堆~(99)Tc、~(129)I热中子嬗变计算方法与实验验证

为了研究利用西安脉冲堆(XAPR)热中子开展99Tc、129I嬗变的可行性,对乏燃料中长寿命裂变产物(LLFP)99Tc和129I核素的热中子嬗变计算方法进行理论与实验研究。利用NJOY程序,以ENDF/B VII.0库为基础,制作99Tc和129I在XAPR堆芯辐照温度下的蒙特卡罗程序(MCNP)截面库,并分析不同参数对截面数据的影响。采用ACE(A Compact ENDF)格式截面库和燃耗程序CINDER’90自带的63群活化截面,利用MCNP程序对ORIGEN2数据库中99Tc和129I的辐射俘获截面进行修正,用ORIGEN2程序分析一定规格的99Tc和129I靶件在XAPR内辐照后的嬗变情况。与实验结果值进行比较,截面数据的差异主要来自中子注量率测量值与实际值的误差,结果证明利用XAPR开展99Tc和129I嬗变是可行的。     

“华龙一号”反应堆乏燃料组件辐射源项计算

随着裂变材料的消耗,锕系核素(AC)和裂变产物(FP)随之产生。AC和FP是核电厂放射性源项的主要来源。准确地计算压水堆燃料组件中AC和FP的核素积存量可为后续燃料循环过程和乏燃料管理提供可靠的数据基础。本文中介绍了乏燃料组件源项的计算方法,并结合"华龙一号"反应堆的功率运行方案,给出了利用CASMO-SNF和SCIENCE-SMART程序计算得出的乏燃料组件放射性活度、衰变热、中子/γ能谱等结果。     

钍基ADS快热耦合次临界核系统燃耗特性分析

在钍基ADS快热耦合次临界反应堆设计的基础上,应用研制的蒙特卡罗燃耗程序MCNTRANS对次临界堆芯在恒定功率下整个寿期内的燃耗特性进行了计算,研究分析了堆芯嬗变能力、钚焚烧性能、堆芯寿期内k_eff变化及加速器束流的协调匹配。分析结果表明：所设计堆芯的次锕系核素（MA）嬗变支持比可达15个百万kW级的PWR,长寿命裂变产物（LLFP）嬗变支持比为2.2个百万kW级的PWR;热区内²³³U的裂变贡献为25％,堆芯嬗变、增殖能力强。整个堆芯寿期内k_eff变化在1%左右,降低了ADS对加速器束流强度的要求。     

干馏法从铀的裂变产物中分离131I

¹³¹I是一种重要的医用放射性同位素,但因湿法分离技术上的缺陷,使得从铀裂变产物中获取¹³¹I的工艺具有环境污染严重、提取效率低的缺点。因铀裂变产物中¹³¹I的产额较高,为拓展¹³¹I的获取途径,提高铀裂变产物的利用效率,开展铀裂变产物中¹³¹I分离的新工艺研究十分必要。与传统湿法分离工艺不同,本工作采用了干馏法进行铀裂变产物中¹³¹I的分离。为了得到高的¹³¹I分离效率,将分离过程分为低温粉化、高温干馏和中低温保温三个阶段,并研究高温干馏阶段温度对131I分离效率的影响。实验发现：当干馏温度高于950 ℃时,¹³¹I的分离效率≥98%。此外,研究结果还表明,在该干馏温度下,碘和¹⁰³Ru 均可挥发出铀靶片,但产物收集液中却仅含有碘。为了解释这一现象,对碘的分离过程进行分析,结合实验结果和理论计算,推测挥发物中碘和¹⁰³Ru分离的原因为：¹⁰³Ru与氧反应生成挥发性RuO₄,从铀的裂变产物挥发出;因加热管内温度较高,RuO₄在迁移过程中发生了分解,生成RuO₂沉积在加热管内部。因此,利用干馏法从铀的裂变产物中分离¹³¹I时,为了得到放化纯度高的碘产品,不仅要合理规划分离过程,还需科学设计加热管的长度。     

基于启明星1#的ADS嬗变研究

以ADS次临界试验平台启明星1#为研究对象,计算分析了MA和LLFP共9种核素的嬗变反应率。通过实验测量了LLFP中¹³⁷Cs的实际嬗变反应率,发现该装置对¹³⁷Cs嬗变速度是其本身自然衰变的10倍。实验结果表明启明星1#具有一定的嬗变能力,经分析确认实验测量结果和理论计算结果吻合。     

钍基熔盐堆燃料循环与启动策略研究

研究了熔盐燃料在堆内外循环以及考虑特殊核素的添加、提取等在线处理过程的熔盐堆燃耗计算模型,在多功能组件计算程序SONG的基础上开发了相应的燃料循环计算功能并进行了初步验证。在此基础上,分别针对氧化铍慢化的热谱熔盐堆和无慢化的快谱熔盐堆进行计算,并根据堆芯反应性长期稳定的基本要求,分析了利用²³³U和工业Pu启动熔盐堆时配套的在线处理方案以及相应的易裂变核添加要求。通过对核素添加、提取以及燃料内核密度的平衡计算,分析了不同的在线处理方案与启动策略对钍-铀燃料循环效率的影响,并据此提出了初步的熔盐堆燃料循环技术路线。结果表明：压水堆乏燃料提取的工业Pu较²³³U更适宜用于钍铀燃料循环启动,因工业Pu启动的快谱熔盐堆的²³³U产率明显高于²³³U启动熔盐堆,而当有了足够的²³³U积累后,²³³U启动的热谱熔盐堆是更好的选择,因其燃料倍增时间更短且燃料初装量也小得多。     

Neutron economy and nuclear data for transmutation of long-lived fission products

In the study of Self-Consistent Nuclear Energy System, the following 29 long-lived fission products (LLFPs) have been selected to be transmuted into stable or short-lived nuclides: ¹⁰⁶Ru, ¹⁰²Rh, ¹⁰⁹Cd, ¹²⁵Sb, ¹³⁴Cs, ^146,147Pm, ^154,155Eu, ¹⁷¹Tm, ⁸⁵Kr, ⁹⁰Sr, ^93mNb, ^113mCd, ^121mSn, ¹³⁷Cs, ¹⁵¹Sm, ¹⁵²Eu, ^108mAg, ¹⁵⁸Tb, ^166mHo, ⁷⁹Se, ⁹³Zr, ⁹⁴Nb, ⁹⁹Tc, ¹⁰⁷Pd, ¹²⁶Sn, ¹²⁹I, ¹³⁵Cs. In the present study, the number of neutrons necessary for the transmutation of the 29 LLFPs with an FBR was evaluated, and the present status of the (n, γ) and (n,2n) cross section data of the 29 LLFPs in JENDL-3.2 and ENDF/B-VI was investigated. The main results of the present study are as follows: (1)only 0.25 neutron per fission is necessary for the transmutation of the 29 LLFPs with isotopic separation, whereas 6.8 neutrons are necessary with chemical separation, (2)the accuracy of the cross sections is 30 to 100% except for the (n, γ) cross sections of limited nuclides in limited incident neutron energy regions.     

A consideration to reduce the potential hazard of I-129 in radioactive wastes

Transmutation of ¹²⁹I to ¹³⁰I by (n, γ) reaction and isotope dilution with stable iodine were discussed. The transmutation in LWR is calculated by supposing that targets irradiated for 25 years are substituted with new targets. The result showed that initial amount of ¹²⁹I will be reduced to 11.5%. In order to lower dose equivalent of general public than 0.1mSv/y, 400 times isotope dilution of ¹²⁹I is required. The feasibility of the isotope dilution was discussed at dissolution process of spent fuel, conditioning process of the waste and disposal conditions.     

Modeling the activity and scaling factor of I in the primary coolant and CVCS resin of operating PWR

To estimate the activity of ¹²⁹I at the primary coolant and chemical and volume control system (CVCS) resin in Korean pressurized water reactor (PWR) plants, a theoretical methodology was developed on the basis of an existing model of primary coolant activity and new model of CVCS resin activity. In order to reflect the difference between ¹²⁹I and ¹³⁷Cs, the different power-related diffusivities in the defective fuel were derived, and the variable removal efficiency of the CVCS resin for ¹³⁷Cs was applied as a function of the coolant activity ratio of ¹³¹I/¹³⁷Cs. The current computational method was validated by using the measured coolant activities of ¹³⁷Cs, and the results show better agreement than a previously suggested parameter correlation method between ¹²⁹I and ¹³⁷Cs. There was also reasonable agreement in a comparison of the results of the test resin columns of the coolant from the PWR plants of other countries. It was shown that the ratio of the effective removal efficiency of ¹²⁹I and ¹³⁷Cs in the CVCS resin linearly influences the activity ratio of ¹²⁹I/¹³⁷Cs in the coolant, but on the other hand, its influence on the activity ratio in the CVCS resin is relatively less sensitive compared with that in the coolant.     

A new back-end cycle strategy for enhancing separation, transmutation and utilization of materials (Adv.-ORIENT cycle)

To minimize the ecological burden originating in nuclear fuel recycling, a new R&D strategy, the Adv.-ORIENT (Advanced Optimization by Recycling Instructive Elements) cycle was set forth. In this context, mutual separation of f-elements, such as minor actinide (MA)/lanthanide (Ln) and Am/Cm, are essential to enhance the MA (particularly ²⁴¹Am) burning. Isotope separation before transmutation is also inevitably required in the case of some long-lived fission products (LLFPs) like ¹²⁶Sn, ¹³⁵Cs, etc. The separation and utilization of rare metal fission products (RMFPs: Ru, Rh, Pd, Tc, Se, Te, etc.) are offering a new direction in the partitioning and transmutation (P&T) field. ⁹⁹Tc and ¹⁰⁶Ru, well-known interfering nuclides in reprocessing, should be removed prior to the actinide stream. Separation of exothermic nuclides ⁹⁰Sr, ¹³⁷Cs as well as MA will significantly help to mitigate the repository tasks.

A key separation tool is ion exchange chromatography (IXC) by a tertiary pyridine resin having soft donor nitrogen atoms. This method has provided individual recovery of pure Am and Cm products with a Pu/U/Np fraction from irradiated fuel in just a 3-step separation. A catalytic electrolytic extraction (CEE) method by Pd_adatom has been employed to separate, purify and fabricate RMFP catalysts. Differently functioned ion exchangers, e.g., ammonium molybdophosphate (AMP), have been investigated for the separation of Cs⁺. Theoretical and laboratory studies on the isotope separation of LLFPs were begun for ⁷⁹Se, ¹²⁶Sn and ¹³⁵Cs.     

Recycle transmutation of MA and LLFP using BWR for sustaining geologic disposal

The actinides and fission products produced in nuclear fuels constitute an important part of the HLW. Therefore, methods for reducing the radiotoxicity of the MA and LLFP in HLW are presently under investigation. The purposes of this study are to evaluate the effectiveness of MA transmutation by taking advantage of neutron spectrum hardening due to void fraction along BWR axial direction; to understand the effectiveness of LLFP transmutation in BWR considering the large capture cross section of FP in thermal region; and to evaluate the macroscopic characteristics of longer residential period of LLFP target in the high burnup BWR core. Conceptual B/T BWR supposed in this study was reactor which the performance comparable to the current BWR. In MA transmutation case, the calculation was focused on varying the void fraction of 0 to 40% along the axial direction, which were directly associated to the lower and upper region of the BWR core. The performance of B/T BWR was evaluated in which four components of MA (²³⁷Np, ²⁴¹Am, ²⁴³Am, and ²⁴⁴Cm) with fixed fraction were blended with UO₂ in B/T fuel. While, for LLFP transmutation, the B/T BWR was assumed to have two homogeneous regions: {1} the region for UO₂ driver fuel (99% of fuel weight), and {2} the region for LLFP (⁹⁹Tc and ¹²⁹I) target capsules (1% of fuel weight), in which metallic Tc rods and iodine in the form of CeI₃ was contained in cylindrical target capsules. The evaluation functions are {1} fission-to-transmutation ratio, [F/T ratio]_MA, and {2} transmutation fraction, Tf_LLFP. Results show that the hardening neutron spectrum due to increase of void fraction in B/T BWR would result a higher [F/T ratio] of MA transmutation performance. Np and Am would be effectively loaded in the upper region of the core, while Cm could be loaded in any region of the core. At the EOC of equal or more than 50 GWd/Mg(HM), technetium has a higher transmutation fraction compared to iodine. To obtain higher LLFP transmutation fraction, the residential time in the LLFP targets in the core, should be kept for long time, for instance about 10 to 30 years. For that purpose, it was proposed that the number of B/T BWR system for LLFP treatment corresponds to the residential time of the LLFP target, i.e. 10 to 30 units.     

Transmutation of long-lived fission products with use of available excess neutrons in BWR core

Feasibility of transmutation of long-lived Fps in BWR is studied from the view point of neuron balance. Pointing out the equilibrium mass amount of LLFP such as ¹²⁹I, ⁹⁹Tc, and ¹²⁶Sn in BWR core, the neutron balance analysis shows that the available neutrons produced by the current BWR core modification is satisfactory to the required amount of neutrons for LLFP transmutation. Core performance of the LLFP-recycled BWR is then analyzed and the result shows satisfactory results for the present core design criteria.

The results confirm the potential of the transmutation of LLFP in BWR and that the eventual radioactive hazard of the radwaste coming form the LLFP recycled BWR can be reduced well below the hazard level of the burned uranium.     

A concept of nitride fuel actinide recycle system based on pyrochemical reprocessing

A fuel cycle system coupled with nitride fuel fast reactors and a pyrochemical reprocessing has been investigated in order to establish an actinide transmutation recycle system with long-lived radioactive nuclides. Core performance of the nitride fuel fast reactor can provide design flexibility of excellent safety characteristics and a new concept of core composed with Na- and He- bonded fuel assemblies is proposed. The effect of ¹⁵N enrichment on nuclear characteristics and the evaluation of toxicity of ¹⁴C generated from ¹⁴N are appeared, and futhermore, excellent performance for the minor actinide (MA) transmutation is shown.

The study of the pyrochemical process shows that the actinides are reasonably separated from fission products in the nitride spent fuels, and that the high level wastes are of nearly actinide-free form.     

Investigation on spent fuel characteristics of reduced-moderation water reactor (RMWR)

The spent fuel characteristics of the reduced-moderation water reactor (RMWR) have been investigated using the SWAT and ORIGEN codes. RMWR is an advanced LWR concept for plutonium recycling by using the MOX fuel. In the code calculation, the ORIGEN libraries such as one-group cross-section data prepared for RMWR were necessary. Since there were no open libraries for RMWR, they were produced in this study by using the SWAT code. New libraries based on the heterogeneous core modeling in the axial direction and with the variable actinide cross-section (VXSEC) option were produced and selected as the representative ORIGEN libraries for RMWR. In order to investigate the characteristics of the RMWR spent fuel, the decay heat, the radioactivity and the content of each nuclide were evaluated with ORIGEN using these libraries. In this study, the spent fuel characteristics of other types of reactors, such as PWR, BWR, high burn-up PWR, full-MOX-PWR, full-MOX-BWR and FBR, were also evaluated with ORIGEN.

It has been found that about a half of the decay heat of the RMWR spent fuel comes from the actinides nuclides. It is the same with the radioactivity. The decay heat and the radioactivity of the RMWR spent fuel are lower than those of full-MOX-LWRs and FBR, and are the same level as those of the high burn-up PWR. The decay heat and the radioactivity from the fission products (FPs) in the spent fuel mainly depend on the burn-up and the burn-up time rather than the reactor type. Therefore, the decay heat and the radioactivity from FPs in the RMWR spent fuel are smaller, reflecting its relatively long burn-up time resulted from its core characteristics with the high conversion ratio. The radioactivity from the actinides in the spent fuel mainly depends on the ²⁴¹Pu content in the initial fuel, and the decay heat mainly depends on ²³⁸Pu and ²⁴⁴Cm. The contribution of ²⁴⁴Cm is much smaller in RMWR than in MOX-LWRs because of the difference in the spectrum. In addition, from the waste disposal point of view, the characteristics of the heat generation FP elements, the platinum group metals, Mo and the long-lived FPs (LLFPs) were also investigated.     

Time-dependent Neutronic Analysis for High Level Waste Transmutation in a Fusion-driven Transmuter

This study presents time-dependent transmutations of high-level waste (HLW) including minor actinides (MAs) and long-lived fission products (LLFPs) in the fusion-driven transmuter (FDT) that is optimized in terms of the neutronic performance per fusion neutron in our previous study. Its blanket has two different transmutation zones (MA transmutation zone, TZ_MA, and LLFP transmutation zone, TZ_FP), located separately from each other. High burn-up pressured water reactor (PWR)-mixed oxide (MOX) spent fuel is used as HLW. The time-dependent transmutation analyses have been performed for an operation period (OP) of up to 10 years by 75% plant factor (η) under a first-wall neutron load (P) of 5 MW/m². The effective half-lives of the MA and LLFP nuclides can be shortened significantly in the considered FDT while substantial electricity is produced in situ along the OP.