基于多物理场耦合的U3Si2燃料与双层SiC包壳组合的轻水堆燃料性能分析

基于COMSOL平台开发了一套基于多物理场全耦合的燃料性能分析程序,并通过径向功率分布模型对比验证了该程序的正确性与准确性;然后进一步分析了U₃Si₂燃料与双层SiC包壳组合、U₃Si₂燃料与锆合金包壳组合在反应堆正常运行工况下的性能,并与UO₂燃料与锆合金的组合进行了对比分析。计算结果发现U₃Si₂燃料与锆合金包壳组合相比UO₂燃料与锆合金的组合具有更低的燃料中心温度、裂变气体释放量及内压,但气隙闭合时间会提前;而U₃Si₂燃料与双层SiC包壳的组合相比U₃Si₂燃料与锆合金的组合具有更高的燃料中心温度、更大的裂变气体释放量及内压,且随着燃耗的增加,其燃料中心温度大幅增加,与锆合金包壳相比,双层SiC包壳能够有效延迟气隙闭合,缓解燃料与包壳的力学相互作用。      

A generalized model for radiation-induced amorphization and crystallization of U3Si and U3Si2 and recrystallization of UO2

A rate-theory model of radiation-induced amorphization and crystallization of U₃Si during ion irradiation has been generalized to include U₃Si₂ and UO₂. The generalized model has been applied to ion-irradiation and in-reactor experiments on U₃Si and U₃Si₂ and provides an interpretation for the amorphization curve (dose required to amorphize the material as a function of temperature), for the ion-radiation-induced nanoscale polycrystallization of these materials at temperatures above the critical temperature for amorphization, as well as for the role of the small crystallites in retarding amorphization. An alternative mechanism for the evolution of recrystallization nuclei is described for a model of irradiation-induced recrystallization of UO₂ wherein the stored energy in the UO₂ is concentrated in a network of sinklike nuclei that diminish with dose due to interaction with radiation-produced defects. The sinklike nuclei are identified as cellular dislocation structures that evolve relatively early in the irradiation period. The complicated kinetics involved in the formation of a cellular dislocation network are approximated by the formation and growth of subgrains due to the interaction of shock waves produced by fission-induced damage to the UO₂.     

The effect of fission products on the rate of U3O8 formation in SIMFUEL oxidized in air at 250°C

The effect of fission products on the rate of U₃O₈ formation was investigated by oxidizing UO₂-based SIMFUEL (simulated high burnup nuclear fuel) and unirradiated UO₂ fuel specimens in air at 250°C for different times (1–317 days). The progress of oxidation was monitored by X-ray diffraction, revealing that the rate of U₃O₈ formation declines with increasing burnup. An expression was derived to describe quantitatively the time for U₃O₈ powder formation as a function of simulated burnup. These findings were supported by additional isochronal oxidation experiments conducted between 200 and 300°C.     

耐事故燃料用于高性能压水堆的分析研究

为明确未来高性能压水堆(PWR)可采用的耐事故燃料(ATF)元件设计方案,本研究采用燃料性能、核设计、反应堆热工安全的适用分析方法,从安全性、经济性和燃料性能等方面对几种潜在的ATF设计方案进行综合分析。结果表明：采用SiC复合包壳+高铀密度燃料的方案较好;由于高铀密度燃料(包括UN、U₃Si₂及UN-U₃Si₂复合燃料)各自均具有鲜明的特点,其中UN-U₃Si₂复合燃料在理论上可以成为高铀密度燃料的一大特色,但从中子经济性的角度考虑需要将UN中¹⁵N进行富集,而目前的富集技术将大大提高该型燃料的制造成本。因此本研究建议高性能PWR的ATF燃料元件设计宜选择SiC复合包壳+U₃Si₂燃料的设计方案。     

U3Si2粉末氟化制备UF4工艺研究

在元件生产过程中，不合格的含铀物料种类多、存量大，为了提高铀的可利用率，满足日益增多燃料元件生产任务所需物料的稳定供给，需要进行铀回收。本实验研究了将U₃Si₂粉末先煅烧氧化制成U氧化物，再将U氧化物与固体氟化铵反应制备UF₄的干法工艺，通过研究氟化物加入量、反应温度、反应时间等因素对产品UF₄质量的影响，摸索出最佳工艺参数。实验结果表明，U₃Si₂粉末煅烧氧化后与固体氟化铵或氟化氢铵反应能制备出符合质量要求的UF₄产品，反应温度在500℃左右、保温时间4.5 h可将UF₄中的UO₂F₂含量降到较低水平。      

U3Si2燃料芯块的制备与显微组织研究

使用电弧熔炼破碎制备U₃Si₂粉末，通过粉末冶金工艺制备获得U₃Si₂燃料芯块，研究了芯块制备过程中U₃Si₂芯块成型能力以及烧结工艺对密度和显微组织的影响。结果表明，加入质量分数为0.5%的聚乙二醇（PEG）成型剂，在260~300?MPa压力下压制成型，在1550℃烧结2~4?h后，U₃Si₂芯块密度最高达到11.4?g/cm3，达到理论密度的的93%以上；芯块晶粒大小均匀，约为60 μm，局部区域存在着少量U相或UO₂相夹杂；芯块的热导率明显优于UO₂，且随温度的升高，其热导率呈线性升高趋势。      

An investigation on the green properties of U-10wt.%Mo/Al and U3Si2/Al powder compacts

The effects of fuel powder volume fraction and fuel particle shape on green properties of compacts, which were produced by processing the blended U-10wt.%Mo and U₃Si₂ with Al powders were investigated respectively, with respective to the compacting pressure range of 50–400 MPa. The relative density of the compacts increases with decreasing volume fraction of fuel powder. The compressibility of comminuted powder compacts was larger than that of the atomized powder compacts due to the fragmentation of comminuted particles, and the compressibility of the compacts of U-10wt.%Mo was larger than that of the compacts of U₃Si₂ due to the deformation of U-10wt.%Mo particles. The green strength of the comminuted powder compacts is higher than that of the atomized powder compact. This seems to have resulted from the smaller pore size and the larger contact area between the comminuted fuel powders and Al powders. It is suggested that the compacting condition adjustment be required to fabricate the atomized powder compacts having comparable green strength.     

Ternary silicides Pu2T3Si5, T = Fe, Tc, Re

The crystal structures of Pu₂T₃Si₅ with T = Fe, Tc, Re synthesized from the elements by argon arc melting have been characterized from X-ray powder diffraction data. All compounds crystallize with the Sc₂Fe₃Si₅ type. The distribution of the various structure types An(RE)₂T₃Si₅ was plotted for An = U, Np, Pu and T = Mn to Pt. The crystallographic relationships among these structure types is discussed.     

氯化锂熔盐中八氧化三铀电解还原基础研究

将氧化物乏燃料直接电解还原为粗金属的过程是目前以电解还原-电解精炼为特征的主流干法后处理流程的重要步骤。二氧化铀（UO₂）是乏燃料的最主要成分,将致密的UO₂芯块转化为八氧化三铀（U₃O₈）粉末后,再进行电化学还原能有效提高还原速率。因此,以U₃O₈为研究对象,开展其在氯化锂（LiCl）熔盐中的电解还原机理研究,对后处理干法流程的开发具有重要的现实意义。本文在650 ℃的LiCl熔盐中,采用循环伏安法和恒电位电解法,研究U₃O₈的电解还原行为;对电解后的样品,运用XRD、SEM等手段分析其组成和形貌,并推测相应的还原机理。     

含TBP-HNO3超临界CO2流体静态络合萃取U3O8

建立了一种快速降低萃取系统压力的静态络合萃取实验装置。在此装置上研究了含TBP-HNO₃超临界CO₂静态络合U₃O₈的快速气化测量方法,探索了含TBP-HNO₃超临界CO₂静态络合萃取U₃O₈的行为规律。     

Thermal stability and brazing characteristics of Zr0.7−xMxBe0.3 (M=Ti or Nb) ternary amorphous filler metals

The effects of Ti or Nb substitution on the thermal stability and brazing characteristics of Zr_0.7−xM_xBe_0.3 (M=Ti or Nb) ternary amorphous alloys were investigated in order to improve properties of Zr–Be binary amorphous alloy as a new filler metal for joining zirconium alloy. The Zr_0.7−xM_xBe_0.3 (M=Ti or Nb; 0x0.1) ternary amorphous alloys were produced by melt-spinning method. In the selected compositional range, the thermal stability of Zr_0.7−xTi_xBe_0.3 and Zr_0.7−xNb_xBe_0.3 amorphous alloys are improved by the substitution of titanium or niobium for zirconium. As the Ti and Nb content increases, the crystallization temperatures increase from 610°C to 717°C and 610°C to 678°C, respectively. These amorphous alloys were put into practical use in joining bearing pads on zircaloy cladding sheath. Using Zr–Ti–Be amorphous alloys as filler metals, smooth interface and spherical primary particles (proeutectic phase) appear in the brazed layer, which is the similar microstructure of using Zr_0.7Be_0.3 binary amorphous alloys. In the case of Zr–Nb–Be amorphous alloys, Ni-precipitated Zr phase that may cause some degradation in ductility and corrosion-resistance is formed at both sides of the brazed layer.     

CCl_(4)和HCl气体氯化铀氧化物北大核心CSCD

分别以CCl_(4)和HCl气体作为氯化试剂,进行了铀氧化物(主要为U_(3)O_(8))的氯化机理和各影响因素研究。以CCl_(4)为氯化试剂对U_(3)O_(8)粉末进行氯化,通过热重分析研究了氯化反应过程的机理及动力学行为,氯化产物主要为UCl_(4)。同时研究了CCl_(4)对不同种类和形态铀氧化物的氯化,UO_(2)芯块由于结构致密很难进行氯化,UO_(2)粉末和UO_(3)粉末很容易被CCl_(4)氯化,产物分别为UCl_(4)和UCl_(6)。以HCl气体为氯化试剂对LiCl-KCl熔盐中的U_(3)O_(8)粉末进行氯化,研究了反应温度、氯化时间、HCl气体流速、U_(3)O_(8)粉末投料量以及铀氧化物种类和形态的影响。结果表明,提高反应温度、延长反应时间、提高HCl气体流速,有利于氯化率的提高。推荐HCl气体氯化U_(3)O_(8)粉末的工艺参数为:氯化反应温度为500℃、HCl气体流速为0.6 L/min。     

UO2核芯制备工艺中U的回收再利用研究

介绍了清华大学核能与新能源技术研究院制备高温气冷堆燃料元件UO₂核芯的溶胶凝胶工艺各种废料的产生情况。针对各种废料的特性,分别进行处理,实现回收再利用。对工艺中产生的含U废液先进行沉淀处理,经1次煅烧后溶解性差,必须将沉淀进行煅烧 还原 煅烧工序后才能实现再利用。对最终烧结球中的不合格品直接进行煅烧处理,将UO₂转化为U₃O₈,即可再利用。各种废料回收后均可作为原料生产UO₂核芯,综合回收率为99.98%。     

Conversion of uranium nuclear fuel into U3O8 at the head end of HTR reprocessing

Corresponding to the reference procedure for the head-end treatment of HTR fuel elements, separation of the moderator graphite from the materials uranium and plutonium is envisaged by combustion in the fluidized bed. Due to the defective silicon carbide layers of the uranium fuel particles a chemical conversion of the UO₂ kernel into U₃O₈ takes place in the oxidizing atmosphere of the combustion process. This reaction proceeds spontaneously and quantitatively, and causes a disintegration of the heavy metal kernel. It is observed that the degree of hardness of the kernel fragments is clearly dependent on the heat-up rate. In the commercial design of the head-end process step, attention must be paid to the cross-over of fuel from the stationary fluidized bed into the dust discharge.     

Enthalpy and heat capacity of LiAlO2 between 298 and 1700 K by drop calorimetry

The enthalpy of γ-LiAlO₂ was measured between 403 and 1673 K by isothermal drop calorimetry. The smoothed enthalpy curve between 298 and 1700 K results in H⁰(T) − H⁰(298 K)=−37 396 + 93.143 · T + 0.00557 · T² + 2 725 221 · T⁻¹ J/mol. The standard deviation is 2.2%. The heat capacity was derived by differentiation of the enthalpy curve. The value extrapolated to 298 K is C_p,298=(65.8 ± 2.0) J/K mol.     

热压烧结UN陶瓷芯块的性能

UN燃料具有铀密度高、熔点高、热导率高、热膨胀系数低、辐照稳定性好等优点,是未来空间核电源、核火箭、快堆和ADS的重要候选燃料。本文采用金属铀粉与氮气在300～400℃直接发生化合反应,制得单相U₂N₃粉末。粒度为38.3 μm的U₂N₃粉末在1 600 ℃真空热压烧结,制得相对密度为93.5%、存在少量金属铀相的UN陶瓷;而18.1 μm的U₂N₃粉末在1 550 ℃真空热压烧结,制得相对密度为96.1%、不残留金属铀相的UN陶瓷,U与N的总质量分数为99.57%,每个金属杂质含量均低于50 μg/g,氧含量为1 048 μg/g,碳含量为502 μg/g。U₂N₃在1 027 ℃以上将会完全分解成UN,UN在1 627 ℃以上也会发生分解。     

CARR用U-Mo合金燃料的堆芯物理方案研究

U-Mo合金燃料具有铀密度高、辐照稳定性好和后处理简单等优点,是未来研究堆燃料的理想选择。在保持中国先进研究堆(CARR)主体结构不变的基础上,使用合适的U-Mo合金燃料替换CARR现有燃料,进行堆芯方案初步研究。通过对中子注量率、循环长度等关键参数的对比分析,给出了较优的堆芯物理设计方案。该堆芯物理方案具有更好的设计参数,并可节省大量的燃料经费支出,提高了反应堆运营的经济性。     

UO2?-Er2O3燃料芯块制备技术初步研究

对Er₂O₃质量分数为4.32%的UO₂-Er₂O₃可燃毒物燃料芯块的制备技术进行了初步研究。通过对比不同工艺条件（混料、成型、烧结）下，芯块的外观完整度、密度、晶粒度等性能，初步得到了UO₂-Er₂O₃燃料芯块的制备技术。试验表明:干法球磨混合6?h，添加5‰的聚乙烯醇（PVA），300~350?MPa压力下冷压成型，1700~1750℃、H₂气氛中烧结2~3?h，可得到外观完整、密度大于等于95%理论密度（T.D.）、晶粒尺寸大于8?μm的UO₂?-Er₂O₃燃料芯块。      

Fission product precipitates in irradiated uranium carbonitride fuel

Austenitic steel-cladded uranium carbonitride fuel pins were irradiated in the BR2 up to 6.4% burnup. A cross-section of the pin RV 24 with the fuel composition UC_0.86N_0.09O_0.05 was prepared for X-ray microanalysis of the fission product precipitates. Rare-earth oxide and U(Mo,Tc)C₂ phases were observed in the whole fuel region. Bright phases present in annular rings of the outer fuel zone were identified as U₂(Tc, Ru, Rh)C₂. Alkaline-earth oxide and U–Pd–Ni phases were shown in the fuel-cladding gap. The rare-earth and alkaline-earth fission products extracted the oxygen from the fuel matrix which became nearly oxygen free. The formation of nitrides could not be detected.     

Segregation effects on the corrosion behaviour of a phosphorus-doped AISI type 304L stainless steel

The effect of grain boundary (GB) segregation on intergranular stress corrosion cracking (IGSCC) in hot water environments at 150°C and 250°C was studied in a P-doped AISI type 304L stainless steel. The extent of segregation was measured by an exposure test in boiling 5 N HNO₃ + 8g/L K₂Cr₂O₇ solution as well as by a potentiostatic etch test at +1325 mV (SHE) in 5 N H₂SO₄ solution. Although GB segregation was detected in all the aged specimens, IGSCC was shown by only the specimens aged for 550°C/1000 h. The results suggest that it is the GB chromium depletion, rather than the segregation of phosphorus at the GBs, that controls IGSCC of stainless steels in the hot water environments studied.