Vapor pressure and thermochemical properties of ZrCl4 for ZrC coating of coated fuel particles

Vapor pressure of zirconium tetrachloride(ZrCl4) under vacuum and an argon pressure of 1×105 Pa was measured. The thermochemical changes of ZrCl4 during evaporation were studied by thermogravimetry-differential thermal analysis(TG-DTA), X-ray diffractometry(XRD), scanning electron microscopy(SEM) and energy-dispersive X-ray(EDX) analysis. At the same temperature, vapor pressures of ZrCl4 under vacuum and an argon pressure of 1×105 Pa are approximately the same. The vapor pressure exceeds 1×105 Pa at 340 ℃, which is high enough for ZrC coating of coated fuel particles. ZrCl4 sample is hydrolyzed to some extent to give ZrO2 and HCl, which however, has little influence on vapor pressure of ZrCl4 at high temperature. No ZrCl3 and Cl2 are produced by decomposition of ZrCl4 during evaporation, which is confirmed by thermodynamic calculation.

A review of TRISO-coated particle nuclear fuel performance models

The success of high temperature gas cooled reactor depends upon the safety and quality of the coated particle fuel. The understanding and evaluation of this fuel requires the development of an integrated mechanistic fuel performance model that fully describes the mechanical and physicochemical behavior of the fuel particle under irradiation. In this paper, a review of the analytical capability of some of the existing computer codes for coated particle fuel was performed. These existing models and codes include FZJ model, JAERI model, Stress3 model, ATLAS model, PARFUME model and TIMCOAT model. The theoretic model, methodology, calculation parameters and benchmark of these codes were classified. Based on the failure mechanism of coated particle, the advantage and limits of the models were compared and discussed. The calculated results of the coated particles for China HTR-10 by using some existing code are shown. Finally, problems and challenges in fuel performance modeling were listed.

Research on the Silicon Carbide Layer of Coated Fuel Particles

The 10MW high temperature gas-cooled test reactor (HTR-10) under construction at INET uses whole ceramic fuel elements. The main barrier which prevents fission product release is the SiC layer of the coated fuel particles. Fabrication of high quality SiC layers is one of the key R&D tasks for the HTR-10 fuel element. The SiClayer was deposited on the fuel particles in a 50 mm conical fluidized bed using the CVD (chemical vapour deposition) technique. The density, thickness, strength and elastic modulus of the SiC layer were measured. The microstructure was observed using SEM (scanning electron microscope ). Parameters were established for manufacturing the SiC layer of the coated fuel particles to be used in the HTR-10. It was found that the traditional density measurement by the sink-float method is questionable in the low density region and that the SiC layer may be contaminated by uranium under certain conditions.

Denoising method of X-ray phase contrast DR image for TRISO-coated fuel particles

TRISO （tristructural-isotropic） fuel is a type of micro fuel particles used in high-temperature gas-cooled reactors （HTGRs）. Among the quality evaluation methods for such particles, inqine phase contrast imaging technique （PCI） is more feasible for nondestructive measurement. Due to imaging hardware limitations, high noise level is a distinct feature of PCI images, and as a result, the dimensional measurement accuracy of TRISO-coated fuel particles decreases. Therefore, we propose an improved denoising hybrid model named as NL P-M model which introduces non-local theory and retains the merits of the Perona-Malik （P-M） model. The improved model is applied to numerical simulation and practical PCI images. Quanti- tative analysis proves that this new anisotropic diffusion model can preserve edge or texture information effectively, while ruling out noise and distinctly decreasing staircasing artifacts. Especially during the process of coating layer thickness measurement, the NL P-M model makes it easy to obtain continuous contours without noisy points or fake contour segments, thus enhancing the measurement accuracy. To address calculation complexity, a graphic processing unit （GPU） is adopted to realize the acceleration of the NL P-M denoising.

A novel coated-particle design and fluidized-bed chemical vapor deposition preparation method for fuel-element identification in a nuclear reactor

Particle coating is an important method that can be used to expand particle-technology applications. Coated-particle design and preparation for nuclear fuel-element trajectory tracing were focused on in this paper. Particles that contain elemental cobalt were selected because of the characteristic gamma ray spectra of 60Co. A novel particle-structure design was proposed by coating particles that contain elemental cobalt with a high-density silicon-carbide （SiC） layer. During the coating process with the high-density SiC layer, cobalt metal was formed and diffused towards the coating, so an inner SiC–CoxSi layer was designed and obtained by fluidized-bed chemical vapor deposition coupled with in-situ chemical reaction. The coating layers were studied by X-ray diffractometry, scanning electron microscopy, and energy dispersive X-ray spectroscopy techniques. The chemical composition was also determined by inductively coupled plasma optical emission spectrometry. The novel particle design can reduce the formation of metallic cobalt and prevent cobalt diffusion in the coating process, which can maintain safety in a nuclear reactor for an extended period. The experimental results also validated that coated particles maintain their structural integrity at extremely high temperatures （～1950 °C）, which meets the requirements of next-generation nuclear reactors.

Manufacture of HTR Fuel Element

The HTR Fuel Element R & D Program,set in 1987,aims to develop the manufacturetechnology of HTR fuel element and to produce the fuel element for the first core of our 10MW experimental reactor.Now the work on laboratory scale is phased out.In this paper,the fuel element manufacture technology is described and the test results are given.

超音速火焰喷涂微纳WC-Cr_(3)C_(2)-CoNi涂层的结构与性能

为了研究双相碳化物金属陶瓷沉积行为对涂层结构性能的影响,分析了原始粉末、低碳钢基体上扁平粒子的表面形貌与截面结构,研究了超音速火焰喷涂微纳WC-Cr_(3)C_(2)-CoNi粒子的沉积涂层的组织结构、相结构和力学性能。研究结果表明:基体上沉积粒子呈现表面光滑浮凸的饼状,且粒子周边出现了径向溅射条纹,扁平粒子厚度远小于其径向尺寸。涂层截面显微组织结构呈现一定的层状特征,硬质相与粘结相、扁平粒子与扁平粒子、扁平粒子与基体及不同硬质相之间的界面结合良好。涂层相结构主要为WC、少量脱碳相、非晶相。Cr_(2)O_(5)涂层的显微硬度、弹性模量、断裂韧性、结合强度和磨损失重量分别为(13.19±0.52)GPa,(145.17±3.89)GPa,(2.59±0.64)MPa・m^(1/2),(38.41±0.51)MPa和(6.08±0.68)mg。相比WC-Co12涂层,超音速火焰喷涂WC-Cr_(3)C_(2)-CoNi涂层WC分解及其失碳相显著降低,力学性能明显提高。

放电等离子烧结包覆颗粒弥散燃料芯块的性能研究

包覆颗粒弥散燃料是耐事故燃料研究的热点。采用放电等离子烧结制备包覆颗粒弥散燃料芯块,研究了烧结工艺对芯块性能的影响,并对芯块进行了物相检测、金相检测以及微观结构表征分析。研究发现,包覆颗粒弥散燃料芯块放电等离子烧结的最佳工艺为助烧剂添加量7%,在1850℃、45 MPa下保温15 min,芯块相对密度可达98.5%;烧结后芯块为纯β相,表明SPS快速烧结能够较好地控制物相转变;在最佳工艺条件下获得的芯块中未观察到芯块中TRISO颗粒出现明显接触的现象,TRISO颗粒整体完整性较好;热冲击试验中,芯块在一次热冲击后表面未出现贯穿的微裂纹,保持较好的完整性。综上,放电等离子烧结工艺可用于快速制备致密度高、无物相转变且抗热冲击性能良好的包覆颗粒弥散燃料芯块。

气冷快堆燃料组件设计及中子学特性分析

气冷快堆兼具高温气冷堆的经济性和快堆的可持续性等优点,在四代堆型中具有独特的技术优势。为了适应气冷快堆高温、高中子通量的堆芯环境,本文基于耐事故燃料模型,提出了一种块状气冷快堆燃料组件设计方案,并对该组件中铀钚混合燃料中的钚含量、冷却孔道的直径及数量、栅距比、包壳及组件盒厚度等物理参数对中子学特性的影响规律开展了敏感性分析研究。分析结果表明:在研究的6个参数中,钚含量和栅距比对组件的中子学特性影响最大,冷却孔道数量主要影响组件内的功率分布,其余参数对组件中子学特性几乎无影响。最后针对块状燃料组件低冷却剂份额的特点,利用单通道模型进行组件内的温度分布计算,给出了热工限值对组件参数的要求。

高温气冷堆包覆燃料颗粒破损机制及失效模型

高温气冷堆的燃料元件的基本构成单元是全陶瓷型的包覆燃料颗粒,其性能决定了高温气冷堆的安全性。除了传统的辐照实验检测外,建立理论模型对其研究具有重要的意义。本文主要介绍了TRI-SO型包覆燃料颗粒的结构及破损机制,以及国外现有的几个主要模型的基本假设,计算原理和特点,通过对比几个模型的优缺点,提出今后研究的方向。

核燃料颗粒化学气相沉积包覆铌层的热力学分析

燃料颗粒表面涂覆Nb层采用的是流态化化学气相沉积(CVD)技术。采用HSC Chemistry 6.0软件,对该工艺过程进行热力学模拟计算,分析各工艺参数对反应产物的影响。结果表明:提高沉积温度,有利于金属Nb的生成,并减少副产物的含量;随着氢气与NbCl5的摩尔比的增加,反应所得产物中的Nb含量也随之增加;Ar气也可以一定程度上影响平衡反应产物的组成,一定量的Ar气有助于金属Nb的生成,减少副产物。

ZrCl_4蒸汽沉积法制备高温气冷堆包覆燃料颗粒ZrC涂层

采用ZrCl4蒸汽、H2和C3H6作为化学反应体系,以Ar为载气,在流化床沉积炉中制备高温气冷堆包覆燃料颗粒ZrC涂层。对所制备涂层进行了分析表征,结果显示:ZrC涂层剖面均匀光滑,无明显孔洞;与内致密热解炭层的界面清晰,厚度约为35μm;涂层主要成分为Zr和C,Zr/C摩尔比接近化学计量比1∶1,其主要相组成为面心立方的ZrC;晶粒生长无明显的择优取向。

球形燃料元件中包覆颗粒的分布效应研究

在球形燃料元件中,包覆颗粒的填充因子低于10%,分布具有很大的随机性。本文利用MATLAB程序实现了4种填充的建模方式,即体积等效规则填充、扰动的规则填充、随机的规则填充和完全随机填充模拟燃料球中包覆颗粒的分布。基于固态燃料钍基熔盐堆(Thorium-based Molten Salt Reactor with Solid Fuel,TMSR-SF1)设计中选用的包覆颗粒燃料参数,使用蒙特卡罗程序MCNP6 1.0和ENDF/B VII.0数据库进行了全反射边界条件下的单燃料球临界计算,精确量化了不同的建模方式引起的中子物理特性参数的差异。计算表明,这4种建模方式形成了不同的包覆颗粒聚集程度。包覆颗粒的聚集会导致丹可夫效应的增强,从而增大了中子被燃料吸收的概率,无限增殖因数随之增大,燃料温度系数随之减小。

固体颗粒表面改性及其在推进剂领域中的应用研究

对推进剂组分中的氧化剂、燃料等固体颗粒进行表面改性处理,不仅能提高单组分的使用性能,也是提高推进剂力学性能、改善燃烧性能和推进剂工艺条件的重要途径.本文综述了固体颗粒表面改性的方法及表面改性后的表征,分析了包覆颗粒性能变化及其对推进剂性能的影响.

10MW高温气冷堆包覆燃料颗粒的研制

我国10MW高温气冷堆采用全陶瓷型包覆颗粒球形燃料元件。TRISO型包覆燃料颗粒由燃料核芯、疏松热解碳层、内致密热解碳层、碳化硅层和外致密热解碳层组成。采用丙烯和乙炔混合气体制备致密热解碳层以及四层连续包覆的新工艺,开展生产工艺条件试验,系统地研究了生产工艺和性能之间的关系,摸索出最佳生产工艺条件。用化学气相沉积方法在150mm流化床沉积炉系统中批量生产出TRISO型包覆燃料颗粒。用扫描电镜观察分析了包覆燃料颗粒的微观结构,包覆燃料颗粒的制造破损率为3.4×10-6,冷态性能达到我国10MW高温气冷堆设计要求。包覆燃料颗粒辐照考验结果(放射性裂变产物释放率R/B为1×10-6左右)表明,包覆燃料颗粒的质量可以满足10MW高温气冷堆安全运行的要求。

硼颗粒的包覆机理及工艺研究进展

阐述了不同包覆材料对硼颗粒的包覆机理,从5个方面总结了硼颗粒包覆材料的选取原则,包括:去除硼颗粒表面氧化膜、提高燃烧温度、降低硼的点火温度、提高表面相容性、催化硼颗粒的氧化反应。总结了沉淀法、表面反应包覆法、高分子吸附聚合法、气相包覆法和机械球磨法等多种硼颗粒包覆工艺的研究状况,分析并比较了不同工艺的作用机理和实际应用效果。介绍了现代硼颗粒表面包覆效果测试技术的特点和应用范围。评述了目前硼颗粒包覆技术的研究现状和不足,并对未来的研究方向进行了展望。

高温气冷堆包覆燃料颗粒ZrC涂层的研究进展

高温气冷堆包覆燃料颗粒关键涂层为SiC涂层,随着高温气冷堆提升功率和向超高温气冷堆发展的趋势,SiC涂层已不能满足包覆燃料颗粒性能要求。ZrC材料具有优良的组织和性能,作为一种最具潜力的包覆颗粒涂层材料,其研究和应用逐渐得到重视和发展。本文介绍了高温气冷堆包覆燃料颗粒ZrC涂层的研究背景、晶体性质、制备方法、组织结构和性能特征。指出了ZrC涂层研究中的现存问题,并预言了进一步的发展趋势。

碳化硅基新型包覆燃料颗粒的设计及制备

TRISO型包覆燃料颗粒可将核裂变产生的气体、固体裂变产物束缚在燃料颗粒内部,是高温气冷堆安全性的重要保障。为满足未来超高温气冷堆在更高温度及更高燃耗条件下对燃料元件的要求,需对传统TRISO颗粒进行优化和改进。基于包覆颗粒的破损机制,设计了两种SiC基新型包覆颗粒,一种采用疏松SiC层替代疏松热解炭层,包覆层由内而外依次为疏松SiC层、内致密热解炭层、致密SiC层、外致密热解炭层;另一种为全SiC包覆结构,包覆层由内而外依次为内层疏松SiC层、SiC过渡层、外层致密SiC层。根据结构设计,采用流化床化学气相沉积法实验探索了疏松SiC的形成机制及包覆工艺条件,并利用SEM、XRD等进行材料分析,最终成功实现了两种新型包覆颗粒的大规模制备。更进一步,提出了全SiC基燃料元件的概念,并制备了球形和柱形全SiC基模拟燃料元件。

高温气冷堆燃料颗粒SiC包覆层性质研究

高温气冷堆(HTGR)燃料颗粒中的SiC包覆层是阻挡裂变产物释放最为关键的一层。本文采用XRD、Raman光谱以及SEM等方法对不同温度下在大内径喷射流化床内通过化学气相沉积法制备的燃料颗粒SiC包覆层进行微观结构分析,研究SiC包覆层在不同制备条件下的微观结构、成分以及密度变化的影响因素。结果发现,在实验设定的MTS(三氯硅烷)浓度范围内,在1 520～1 600℃之间均可制备出C、Si等杂质不明显的β-SiC包覆层,密度略有差异。通过微观结构分析发现,SiC包覆层密度的变小主要是由包覆层内微孔引起,且此微孔在包覆层内呈线性分布,同时基本位于某一相同的沉积表面,因此,微孔的生成与颗粒流化状态密切相关。可见,改善流化质量应是下一步工艺改进的主要方向。