腐殖酸胶体对超铀核素存在形态的影响研究

研究了在腐殖酸存在时，地下水中^237Np,^238Pu和^241Am的存在形态以及在黄土上的吸附。研究结果表明，在地下水中存在腐殖酸时，^237Np形成了假胶体，且胶体份额随腐殖酸浓度的增大而增大；^238Pu和^241Am的胶体份额也随腐殖酸浓度增大而增大。在地下水中存在腐殖酸时，这几种核素在黄土上吸附能力减弱。     

核素迁移试验现场砂源中核素的淋洗及其形态研究

用地下水淋洗了核素迁移试验现场中使用的石英砂源，用超过滤法研究了淋洗液中核素的形态，用连续浸取法研究了淋洗后石英砂上残留核素的存在形态。结果表明，当淋洗液为110倍柱体积时，地下水可将砂源上90％以上的^237Np淋洗下来，且主要以可交换的离子态存在；淋洗后残留在石英砂上的^237Np主要以碳酸盐结合态和铁锰氧化物结合态存在，其份额分别约为5．5％和1．3％；^238Pu从石英砂上的淋洗没有^237Np容易，在淋洗液中^238Pu主要以胶体存在。     

90Sr、237Np、238Pu和241Am在含水层中迁移的模拟实验

在中国辐射防护研究院野外试验场的地下研究设施内进行了^90Sr、^237Np、^238Pu和^241Am在含水层介质中迁移的模拟实验。实验用的非扰动原状土柱取自地下研究设施内的含水层，实验用水为地下水。实验结果表明，试验场含水层介质对^238Pu和^241Am具有很强的吸附能力，对^237Np的吸附能力相对次之，对^90Sr的吸附能力相对较弱。在实际水流速为6.13cm/d条件下，经过527.5天，各核素的活度浓度峰分别迁移了16cm(^90Sr)、3.9cm(^237Np)、小于0.2cm(^238Pu和^241Am)。采用核素二维迁移方程和本文提出的核素从源层释放的洗脱模型对浓度分布进行了拟合，得到了核素迁移参数，实验数据和拟合曲线符合较好。     

237Np、238Pu、241Am和90Sr在包气带黄土、含水层和工程屏障材料中迁移行为的野外试验研究

本文介绍了^237Np、^238Pu、^241Am和^90Sr在包气带黄土、含水层和工程屏障材料(膨润土、水泥、变质水泥、水泥砂浆粉)中迁移行为的野外试验的方法和结果。在包气带黄土和工程屏障材料中的迁移试验是在天然和喷淋(15mm／d)两种条件下进行的，含水层迁移试验包括核素在用未扰动含水介质填装的组件试验与核素在未扰动含水介质中的示踪试验。经过3年试验，核素在天然条件下的包气带黄土中以及无论在天然还是喷淋条件下的工程屏障材料中，示踪剂未见明显迁移(即未迁移出示踪源层外)；在喷淋条件下，在包气带黄土中通过石英砂示踪源层^90Sr(质心)向下迁移2．7cm，通过示踪源层外边缘上的黄土向下迁移13cm(峰位)；^237Np、^238Pu、^241Am未见明显迁移。发现石英砂做示踪剂载体对黄土非饱和水有屏流作用，影响核素迁移，以石英砂和黄土做载体的对比实验证实了这一点。^90Sr、^237Np、^238Pu和^241Am在未扰动含水层介质示踪试验中经1023d未见明显迁移，仍在示踪源点。含水层组件试验中^238Pu和^241Am未见明显迁移，在组件8(面源)中，^237Np向后迁移0．95cm，^90Sr(质心)迁移4．7cm。试验结果还表明，核素在变质水泥和普通水泥中迁移(3年)规律未见明显差异。     

237Np、238Pu、241Am和90Sr近地表迁移行为及含超铀核素中低放废物处置安全评价方法研究

主要介绍在包气带黄土、含水层黄土和工程屏障材料(膨润土、水泥、变质水泥、砂浆粉)中,237Np、238Pu、241Am和90Sr迁移的野外试验、实验室模拟实验及工程屏障材料性能测定、黄土对核素吸附特性、化学形态等研究结果.在天然和喷淋两种条件下,237Np、238Pu和241Am在包气带、含水层和工程屏障材料的野外试验中三年时间基本未移动.喷淋条件下,野外试验中90Sr通过石英砂示踪源层其质心位置1 079 d向下迁移2.7 cm,在示踪源层外6 cm处黄土中90Sr浓度峰在1 215 d向下迁移13 cm左右.在包气带模拟实验中,90Sr、237Np、238Pu和241Am在1号柱中经1 073 d分别向下迁移9.8 cm、3.25 cm、0.5 cm和0.25 cm.在含水层模拟实验中,经970.5 d,90Sr、237Np、238Pu和241Am分别迁移16 cm,4 cm、0.2 cm和0.2 cm.野外对比试验验证,在包气带中核素通过踪源层黄土载体向下迁移的距离是通过石英砂载体的3.6倍多.在完全相同条件下,Br迁移速度比3H略快.包气带石英砂示踪源层处,核素浓度分布出现低谷现象.CIRP试验场地下水中,237Np以离子态(V、V1价)存在为主,238Pu主要由以Ⅳ价离子态存在.237Np不易形成真胶体.工程屏障材料、HA和FA的存在对核素化学形态有影响.     

建造用于含水层中核素迁移试验的地下研究设施的地下研究设施的技术要求

在中国辐射防护研究院（CIRP）野外试验场建造了用于在浅部含水层中进行核素（^237Np、^238Pu、^241Am和^90Sr等）迁移试验的地下研究设施（URF）。该设施须满足的主要技术要求包括：保持周围试验区土体结构稳定，保持地下水化学条件和水动力条件不被改变。采用人工小进尺开挖和快速支护衬砌以及沉井法建造竖井等措施保护了周围土体结构未被破坏。衬砌前用四层聚乙烯膜铺衬洞壁，竖井体下沉前外壁涂刷氯烯烃防水胶液，基本防止了对地下水化学条件的影响。严格控制施工降水方式，由于施工中未采用抽水降低水位方式，保持了地下水动力条件没有变化。施工和运行过程中对有关指标进行了监测，结果表明采取有效措施后使URF达到了预定技术要求，满足了核素迁移试验条件。     

核素在弱含水层三维迁移的现场示踪试验

对核素在弱含水层中的三维迁移进行了现场试验。试验结果表明:经过1023d的试验,示踪核素90Sr、237Np、238Pu和241Am纵向分布的浓度峰均在最初释放的源层位置未动,迁移最快的90Sr的质心移动了0 32cm;按质心计算,90Sr、237Np、238Pu和241Am的延迟系数(Rd)分别为4 0×102、1 6×103、2 7×105和∞。这表明,黄土介质对这几种示踪核素具有强的吸附能力。     

核纱在水平组件迁移的现场示踪试验

在水平组件中的迁移试验是核素在含水层迁移试验的重要组成部分。本文主要介绍在中国辐射防护研究院野外试验场地下研究设施（URF）试验竖井中进行的水平组件试验的方法和结果。水平组件中装有示踪剂和在含水层采集的未扰动土壤，通过试验竖井壁水平插入含水层，天然地下水通过与含水层介质紧密相连的一端流地 件，在接取样管的另一端接取水样；通过测量试验期间采集的水样和试验结束后切割的土壤样品中示踪剂的浓度，得到核素的迁移数据。试验结果表明，黄土对试验所用的^90Sr、^237Np、^238Pu和^241Am以及Sr、Nd和Ce都有较强或很强的吸附能力；核素迁移具有偏心现象；腐殖酸延缓了^90Sr的迁移；^3H的迁移速度慢于Br^-。     

腐殖酸对Np胶体行为的影响

在模拟高放废物深地质处置的低氧低浓条件下,探讨用膜过滤法研究Np胶体行为的可行性。实验研究结果表明:无腐殖酸存在时,在pH=1～13条件下,无机离子对237Np的测定无明显影响,237Np的液闪探测效率可达100%;增加闪烁液用量可消除腐殖酸对237Np的淬灭效应,过滤器对237Np的吸附可忽略不计,说明将过滤法应用于Np的胶体行为研究准确、可靠,操作简便。应用该方法对Np的不同价态和腐殖酸存在下的胶体行为进行了研究。Np(Ⅴ)无明显胶体行为,Np(Ⅳ)以真胶体形态存在,其浓度显著影响胶体行为;腐殖酸与Np(Ⅳ)能形成假胶体,从而提高了Np(Ⅳ)在溶液中的含量,有利于Np的迁移。腐殖酸是核素迁移研究必须考虑的重要影响因素。     

腐殖酸存在条件下镎胶体行为研究

腐殖酸广泛存在于土壤和水体中,具有较强配合能力、还原能力,并能在一定条件下形成胶体,影响核素化学形态,进而影响核素在地下水中的化学行为及溶解、吸附、扩散等迁移行为。锕系核素。237Np属高毒α核素,在放射性废物中含量较大、半衰期（2．14×10^7a）长.     

水溶液中Np、Pu、Am和Cm同时电沉积制备α测量源

为制备高分辨率Np、Pu、Am和Cm的α混合测量源,研究了电沉积液介质浓度、pH值、电流密度、电沉积时间等条件对电沉积效率及沉积源质量的影响。结果表明,在pH为2.0~2.5的0.2mol/L硫酸铵介质中,电流密度为0.40~0.50A/cm2,室温条件下电沉积60min,~(237)Np、~(238)Pu、~(243)Am和~(244)Cm在阴极不锈钢片上的电沉积效率均大于96%,制备的α测量源能量分辨率较好。     

Enhancing BWR proliferation resistance fuel with minor actinides

To reduce spent fuel for storage and enhance the proliferation resistance for the intermediate-term, there are two major approaches (a) increase the discharged spent fuel burnup in the advanced light water reactor- LWR (Gen-III Plus), which not only can reduce the spent fuel for storage, but also increase the ²³⁸Pu isotopes ratio to enhance the proliferation resistance, and (b) use of transuranic nuclides (²³⁷Np and ²⁴¹Am) in the high burnup fuel, which can drastically increase the proliferation resistance isotope ratio of ²³⁸Pu/Pu. For future advanced nuclear systems, minor actinides (MA) are viewed more as a resource to be recycled, and transmuted to less hazardous and possibly more useful forms, rather than simply disposed of as a waste stream in an expensive repository facility. As a result, MAs play a much larger part in the design of advanced systems and fuel cycles, not only as additional sources of useful energy, but also as direct contributors to the reactivity control of the systems into which they are incorporated. In the study, a typical boiling water reactor (BWR) fuel unit lattice cell model with UO₂ fuel pins will be used to investigate the effectiveness of minor actinide reduction approach (MARA) for enhancing proliferation resistance and improving the fuel cycle performance in the intermediate-term goal for future nuclear energy systems. To account for the water coolant density variation from the bottom (0.76 g/cm³) to the top (0.35 g/cm³) of the core, the axial coolant channel and fuel pin were divided to 24 nodes. The MA transmutation characteristics at different elevations were compared and their impact on neutronics criticality discussed. The concept of MARA, which involves the use of transuranic nuclides (²³⁷Np and/or ²⁴¹Am), significantly increases the ²³⁸Pu/Pu ratio for proliferation resistance, as well as serves as a burnable absorber to hold-down the initial excess reactivity. It is believed that MARA can play an important role in atoms for peace and the intermediate-term of nuclear energy reconnaissance.     

Colloid-facilitated effects on migration of radionuclides in fractured rock with a kinetic solubility-limited dissolution model

<正>Nuclides can move with groundwater either as solutes or colloids,where the latter mechanism generally results in much shorter traveling time as the nuclides interact strongly with solid phases,such as actinides.In the performance assessment,it is therefore essential to assess the relative importance of these two transport mechanisms for different nuclides.The relative importance of colloids depends on the nature and concentration of the colloids in groundwater.Plutonium(Pu),neptunium(Np),uranium(U) and americium(Am) are four nuclides of concern for the long-term emplacement of nuclear wastes at potential repository sites.These four actinides have a high potential for migrating if attached to iron oxide,clay or silica colloids in the groundwater.Strong sorption of the actinides by colloids in the groundwater may facilitate the transport of these nuclides along potential flow paths.The solubility-limited dissolution model can be used to assess the safety of the release of nuclear waste in geological disposal sites.Usually,it has been assumed that the solubility of the waste form is constant.If a nuclide reaches its solubility limit at an inner location near the waste form,it is unlikely that the same nuclide will reach its solubility limit at an outer location unless this nuclide has a parent nuclide.It is unlikely that the daughter nuclides will exceed their solubility limit due to decay of their parent nuclide.The present study investigates the effect of colloids on the transport of solubility-limited nuclides under the kinetic solubility-limited dissolution(KSLD) boundary condition in fractured media.The release rate of the nuclides is proportional to the difference between the saturation concentration and the inlet aqueous concentration of the nuclides.The presence of colloids decreases the aqueous concentration of nuclides and,thus,increases the release flux of nuclides from the waste form.     

Aspects of 238Pu production in the experimental fast reactor JOYO

Experimental determination of ²³⁸Pu in ²³⁷Np samples irradiated in the experimental fast reactor JOYO was done as part of the demonstration of ²³⁸Pu production from ²³⁷Np in fast reactors within the framework of the protected Pu production project, which aims at reinforcement of proliferation resistance of Pu by increasing the ²³⁸Pu isotopic ratio. ²³⁸Pu production amount in the irradiated ²³⁷Np samples was determined by a radioanalytical technique. Aspects of ²³⁸Pu production were examined on the basis of the present radioanalysis. The ²³⁸Pu production amount depends on the neutron spectrum which can range from that of a typical fast reactor to a nearly epi-thermal spectrum. It is concluded that the fast reactor has not only high potential for use in protected Pu production, but also as an incinerator for excess Pu.     

我国环境土壤中的重要超铀核素分布

Pu、Am、Np是3种重要的超铀核素,环境中的这些核素主要来源于人类的核活动,包括大气层核武器试验、核设施排放和核事故释放等。这些超铀核素不仅具有放射性,还兼具化学毒性。我国地域辽阔,环境土壤类型丰富,在当前核电事业蓬勃发展的背景下,建立和扩大我国环境土壤中这些重要超铀核素的“准本底”数据库是辐射环境安全评价的重要组成部分,也是公众关心的热点问题。近30多年来,研究人员对我国不同环境土壤中这几种超铀核素从不同科学角度开展了调查测量研究。本文对此进行整理和分析,对我国环境土壤中这些重要超铀核素（主要是Pu核素,还包括241Am和237Np）的来源、浓度水平和分布特征进行讨论和综述,为辐射环境安全评价奠定基础。     

237Np在黄土和石英砂中迁移的影响因素

通过静态实验和动态实验,研究了放射性溶液活度、液-固比、pH值、碳酸盐、离子强度和黄土粒度等对超铀核素^237Np在黄土中的吸附分配系数的影响,以及有机质HA对^237Np在石英砂柱中迁移的影响。     

PhreePlot绘制某些可变价核素Eh-pH图

U、Np、Pu、~(99)Tc、~(79)Se等放射性元素或核素对氧化还原条件敏感,存在多种价态,且锕系元素(U、Np、Pu)具有丰富的配位化学,其在生物圈和地质圈中的化学行为较为复杂。电势(Eh)-pH图对解决在水溶液中发生的一系列反应及平衡问题具有广泛的应用。本工作采用PhreePlot软件绘制了这些元素或核素在人体血清、唾液、胃液、DMEM培养基和北山地下水中的Eh-pH图以研究它们的主要氧化态和赋存形态。结果表明,U在生物圈中的主要氧化态是Ⅵ,Np是Ⅳ,Pu是Ⅳ和Ⅲ,99 Tc是Ⅶ和Ⅳ,79Se是0和Ⅳ。相比其他元素或核素,pH对铀的赋存形态影响更大。在地质圈中,根据Eh-pH图来看,北山处置库有利于Np、Pu的长期储存而对于U、99 Tc、79Se的储存不利。本工作的对比研究也表明,在热力学数据库一致的情况下,采用免费软件PhreePlot绘制的元素Eh-pH图与Geochemist’s Workbench(GWB)程序绘制的Eh-pH图具有高度的一致性。     

Dependence of Fast Reactor Fuel Burnup Characteristics on Nuclear Data Libraries

In the framework of the development of burnup calculation method for commercial fast reactors, a sensitivity analysis was carried out to clarify the dependence of fuel burnup characteristics on nuclear data libraries (NDLs). The following NDLs were compared: JEF-2.2, ENDF/B-VI Release 5, JENDL-3.2 and JENDL-3.3. The NDL-dependence of material balance for main heavy metal nuclides (²³⁵U, ²³⁸U, ²³⁹Pu, ²⁴⁰Pu and ²⁴¹Pu) was small, since the number densities at the end of one-cycle burnup did not change over 1 or 2% among the above-mentioned libraries. Relatively large differences were found for minor actinide nuclides, especially for ²³⁶U, ²³⁷Np, ^242mAm, ²⁴³Am and curium isotopes. The number densities for these nuclides after burning up showed remarkable NDL-dependence over 5% through 50%. A burnup sensitivity analysis system based on the generalized perturbation theory enabled us to find out quantitatively the causative nuclides and reactions, as well as their energy regions.