用于产氚率测量的碳酸锂探测片液闪样品制备方法研究

氚增殖包层中产氚率测量是聚变核能系统中需要研究的重要问题之一。本文开展了用于产氚率测量的碳酸锂探测片液闪样品制备方法的研究。结果表明:采用盐酸溶解碳酸锂探测片的方式,能制备成无色、透明度高且无分层的液闪样品,相比其他混酸处理,这种方法减少了寻找混酸间最佳体积比的步骤,简化了碳酸锂探测片液闪样品制备流程。对完善制备方法的研究表明:在20 m L的液闪测量瓶中,闪烁液的体积至少为10 m L以上;碳酸锂探测片刚好溶解后,盐酸用量不能超过0.2 m L(部分不超过0.4 m L)。该方法制备的液闪样品的兼容性在较长时间是稳定存在的,但淬灭程度会有较大变化,需考虑淬灭程度的变化对氚测量的影响。     

环境和生物样品中3H和14C的测量

研究了环境和生物样品中^3H和^14C的测量方法。^3H测量步骤包括：样品氧化燃烧,使有机结合氚(OBT)转化为氚化水,用液闪法测量^3H活度。该方法的探测下限为1．2Bq／L。^14C测量步骤包括：将8g左右的样品经过燃烧爆炸后转变为CO2,并最终合成苯,用液闪法测量^14C的活度。该方法的探测下限(以C质量计)为1．0Bq／kg。文章同时给出了树叶、牛奶、动物、土壤等多种生物样品中^3H和^14C的测量结果。     

用液闪直接测量核设施周围环境中的氚

某些核设施运行时会释放氚,从而引起周围环境中氚活度浓度水平的变化。对核设施周边区域空气、地下水、雨水和海水样品中的氚分别用内标准法(简称“内标法”)和外标准淬灭指示参数法(简称“外标法”)进行了液闪测量。两种标准方法测量数据的相对偏差在-4.0%～4.0%。根据内标法的探测效率与仪器给出的淬灭指示参数制作了4种环境水样的淬灭校正曲线。在环境样品测量中,内标法和外标法的探测效率最大差值约为1.6%,痕量¹⁴C和其它β放射性核素对³H的计数率影响可忽略。对探测效率为21.5%～24.5%无严重淬灭的样品,用液闪直接测量并根据外标法的淬灭校正曲线计算氚活度浓度,相对偏差在-6.35%～4.41%,基本可满足核设施氚常规监测的要求。     

Hidex 300SL液闪装置测量低水平氚水活度的参数优化

Hidex 300SL是基于三管符合计数/两管符合计数(TDCR)方法绝对测量低水平氚水活度的液闪装置。本工作基于该装置对标准非淬灭氚水样品进行测量研究,明确了系统的探测效率与TDCR的关系;讨论了该装置的测量模式、符合时间等参数对计数率、衰变率和TDCR的影响;并对仪器的运行参数进行选择优化,在"H-3"测量模式及35ns的符合时间窗下,系统对3 H的探测效率达73.2%,衰变率稳定性好于0.47%;最后对空气本底样品进行测量,评估了该装置对氚水样品的探测下限,为后续环境低水平样品的精确测量提供有益参考。     

水中氚的电解浓集装置设计北大核心CSCD

建立了一套水中氚的电解浓集装置,一次可以电解12个样品。水样初始体积为250 m L,电解后的体积是8 m L。每个电解槽的电压3.0±0.2 V,电流12±1 A,电解后样品中氚的浓缩倍数为20±0.5倍,完成电解总共需要72 h。用Quantulus 1220液体闪烁谱仪测量,仪器本底1.0 cpm,测量时间600 min时,最低探测限可达0.12 Bq/L。     

液闪法测环境低水平氚的探测限影响因子研究

本文对液闪法测氚探测限的影响因子进行了识别、筛选和定量分析,结合电解浓缩方法,提出了降低分析方法探测限的优化方案,并通过实验设计,对上述影响因子逐一进行了验证。实验结果表明,通过恰当选择测量道宽、本底水、闪烁瓶材质、闪烁液及其与样品配比可以在不增加工作量的前提下将探测限降低至0.87 Bq/L;增加电解浓缩的预处理步骤能够大幅降低分析方法的探测限,进一步将其优化至38.5 mBq/L。     

水中氚的电解浓集装置设计

建立了一套水中氚的电解浓集装置,一次可以电解12个样品。水样初始体积为250 m L,电解后的体积是8 m L。每个电解槽的电压3.0±0.2 V,电流12±1 A,电解后样品中氚的浓缩倍数为20±0.5倍,完成电解总共需要72 h。用Quantulus 1220液体闪烁谱仪测量,仪器本底1.0 cpm,测量时间600 min时,最低探测限可达0.12 Bq/L。     

低温解析-液闪法检测植物中氚含量

为评价涉氚活动中氚对环境的影响,建立了低温解析—液闪法检测核设施周围植物样品中氚含量的分析方法。该方法将核设施周围植物样品中组织自由水氚(TFWT)在110~120℃解析出来,用液闪计数仪测量其氚含量。该分析方法比传统分析方法缩短约120 min,对植物样中TFWT的平均回收率优于76%,能够满足涉氚场所植物中TFWT的快速分析。     

Pt-SDB疏水催化剂中残氚的测量

研究了Pt-SDB疏水催化剂中残氚测量方法。待测样品经5A分子筛三级干燥和真空热处理排除催化剂表面吸附氚、微波消解制样后,液闪测得残氚量为1.69×104Bq/g,测量不确定度为10%(K=2)。     

含氚泵油表面活性剂复配法的测氚技术

为测量含氚废旧泵油的氚浓度,研究了表面活性剂十二烷基甜菜碱(BS-12)和脂肪醇聚氧乙烯醚(FEO)复配的表面化学性质和热力学性质,通过复配体系乳化泵油,并与液闪液形成分散体系达到测氚目的。结果表明,复配胶束浓度小于10-4 mol/L、BS-12与FEO复配体积比为6∶4、泵油测量体积小于0.012mL、NaCl浓度为0.1mol/L时具有稳定的测量结果。     

Pulsed Cold Neutron Source of Solid Methylbenzene

Lithium carbonate pellets are frequently used for estimation of tritium production rate in irradiated samples in fusion blanket neutronics experiment and the activity is measured by liquid scintillation counting technique. In this measurement, it is essential to solve the lithium carbonate pellet as much as possible and to mix the pellet solution into scintillation cocktail homogeneously at stable condition. For this purpose, a novel binary-acid method has been developed to solve lithium carbonate and to mix the pellet solution into scintillation cocktail. High solubility is attained by adopting two acids, HNO₃ and CH₃COOH, and a good compatibility of the pellet solution with scintillator is obtained by emulsion cocktail resulting in high counting efficiency. Defining a product of dissolved mass and counting efficiency as a Figure of Merit (FOM), the present method has higher FOM value than the conventional method and is extremely simple in a sample preparation procedure. In the present work, solubility, compatibility and counting efficiency were systematically examined for different mixing ratios of two acids, and the condition for a maximum FOM was determined. The FOM value of a factor of two higher than the conventional method was finally attained.     

Direct tritium measurement in lithium titanate for breeding blanket mock-up experiments with D-T neutrons

At Fusion Neutronics Source (FNS) of JAERI, tritium breeding experiments with blanket mock-ups consisting of advanced fusion reactor materials are in progress. The breeding zones are thin layers of lithium titanate which is one of the candidate tritium breeder materials for the DEMO fusion power reactor. It is anticipated that the application of small pellet-shaped lithium titanate detectors manufactured from the same material as the breeding layer will reduce experimental uncertainties arising from necessary corrections due to different isotopic lithium volume concentrations in breeding material and detector. Therefore, a method was developed to measure the local tritium production by means of lithium titanate pellet detectors and a liquid scintillation counting technique. The lithium titanate pellets were dissolved in concentrated hydrochloric acid solution and the resulting acidic solution was neutralized. Two ways of further processing were followed: direct incorporation into a liquid scintillation cocktail and distillation of the solution followed by mixing with liquid scintillator. Two types of lithium titanate pellets were investigated with different ⁶Li enrichment and manufacturing procedure. It was found that lithium titanate is suitable for tritium production measurements. However some discrepancies in the measurement accuracy remained with one of the investigated pellet detectors when compared with a well-established lithium carbonate measurement technique and this issue needs further investigation.     

加速器质谱测氚及其应用

氚是环境中的主要放射性核素之一,对氚进行准确高效的监测是十分有必要的。目前常用的液体闪烁计数法所需的样品量较大,测量时间较长,不能对微量样品进行高精度测量。加速器质谱具有测量样品小、测量精度高和测量时间短的特点,能够更好地满足环境氚监测的需求,可以广泛应用于地球与环境科学、生物医学和辐射监测等方面。文中介绍了加速器质谱测氚的基本原理和发展历史、制样方法,对加速器质谱测氚的已有研究成果和主要应用进行了总结和展望。     

土壤样品中氚水的测定

本文介绍了土壤中氚水的测定方法，主要包括真空解析与冷凝、制样和液闪测量等步骤。当分析１２０ｇ湿度为２０％的土壤时，方法回收率为９６．７％，探测下限为０．７０Ｂｑ／ｋｇ。     

HTR-10一回路冷却剂中氚活度的测量

详细介绍了测量10 MW高温气冷试验堆一回路冷却剂中氚活度的方法。设计适用于HTR-10特点的氚收集装置,先后两次收集冷却剂中的氚,制成液样进而用液闪法进行测量,并根据试验结果推算HTR-10一回路冷却剂中氚的总活度。针对两次试验结果进行分析并与理论计算值相比较,验证了理论计算的正确性并由此进一步证明高温气冷堆的燃料包覆颗粒对放射性产物的阻挡作用完好,反应堆对环境的氚释放完全在设计要求范围内,符合相应的国家标准。     

~(85)Kr气体液闪测量方法研究

采用反康普顿γ谱仪对~(85)Kr样品进行活度标定作为工作参考,通过自行设计的Kr气体收集装置和液闪制样装置,建立了一种~(85)Kr气体样品的液闪测量方法。结果表明:以甲苯为溶剂、1,4-双-2-(4-甲基-5-苯基噁唑基)(POPOP)和2,5-2苯基噁唑(PPO)为溶质的闪烁液,当体积为20mL,硅胶加入质量为1.0g时,能够完全溶解0.5m~3空气中的Kr气,且样品液闪测量无需进行淬灭校正;对于~(85)Kr活度小于1Bq的样品,液闪测量相对偏差绝对值小于7%;制备的样品放置20h以内计数率稳定。该方法适用于环境大气中~(85)Kr放射性水平的测量。     

On monitoring the tritium breeder in a lead–lithium cooled ceramic breeder (LLCB) module of the ITER

The operation of a tritium breeder is a most process among engineering problems of DEMO. In this study, a design for monitoring tritium-breeding in the reactor is discussed. Additionally, a system for the experimental estimation of the tritium-breeding ratio (TBR) and the tritium-breeding dynamics in a lead–lithium cooled ceramic breeder (LLCB) test module used in the ITER is proposed. The systems are based on tritium and neutron-flux measurements under the ITER plasma D–T experiments and the use of lithium ortho-silicate and lithium carbonate samples and neutron detectors. Different lithum-6 and lithium-7 isotope contents in the samples are used to measure neutron spectrum. The samples and detectors are delivered in containers to the test breeder module (TBM) on a monitor channel connecting the TBM to an operating zone of the ITER. The tritium content in the samples is measured in a laboratory by the liquid scintillation method.Pneumatic control is used to deliver the samples to the TBM and to extract the samples using the channel during plasma-operational pauses. Neutron calculation is performed to estimate the tritium content in the samples and the heat distribution in the materials of the channel under reactor irradiation. A measurement accuracy of the tritium content in the carbonate and orthosilicate samples can attain a level of 7% and 10%, respectively. The results of the channel-cooling calculation performed under the nominal operating conditions of the TBM (a plasma pulse) are presented in the paper.