气相色谱氩、氪、氙、氡分离度初步研究

核爆炸产生多种稀有气体核素,这些核素可作为核泄露监测对象。气相色谱是组分分离的重要手段,在核爆炸监测取样中有重要应用。本文以5分子筛作为固定相,高纯氮作为流动相,测量了氩、氪、氙、氡在气相色谱中的分离效果。结果表明,在相同色谱条件下,氩、氪分离度小于氪、氙分离度;在柱流量35.6 mL/min、柱温353 K条件下,气相色谱氩、氪,氪、氙,氙、氡分离度均大于2.25。     

一个放射性氪、氙净化装置简介

本文介绍了放射性氪、氙净化装置的功用、特性和概况。实验数据表明,活性炭吸附氪的透过时间计算方法是正确的。     

低温精馏分离氪

【西德《科学概况》1982年第4期第116页报道】在西德,人们认为在从核燃料后处理的排气中分离氪-85的许多方法中,低温精馏是最好的方法。这主要是由于西德在空分方面已有几十年的经验。不过,裂变产生的氪与氙的比例和空气中的正好相反,所以这里要防止氙冻结,因此,精馏必须在5巴压力下进行。     

CO_2对活性炭捕集氙工程的影响

很多核设施会产生放射性水平较高的氙等稀有气体同位素,须经过特殊处理后才能向环境排放,研究以空气或其它气体为介质的氙的吸附净化方法具有较强的实用价值。研究了常温下多组分气体在活性炭上直接吸附时,杂质组分CO2对捕集氙效果的影响,比较了多级柱和单级柱两种方案的效果和活性炭用量,以及条件参数的影响。结果表明:相比较多级柱除杂质吸附氙的方法,单级柱直接吸附氙更易于实现工程应用;在流速约0.33cm/s下,活性炭单级柱常温常压吸附对氙捕集效率达到90%;在一定流速(0.02~1.2cm/s)范围内,可以忽略炭床阻力的影响。     

核电站滞留床用活性炭的性能研究和选择

建立可模拟核电站不同气流参数条件下的活性炭吸附剂性能评价系统,对不同活性炭样品分别进行了物理性能表征测试和放射性氪与氙滞留性能实验。同时针对不同影响因素条件下活性炭滞留惰性气体性能的影响进行了研究,包括系统气流压力、温度、气流比速及辐照强度。试验结果显示系统气流压力越高、温度越低,氪动态吸附系数越大;一定范围的气流比速、辐照强度对活性炭动态吸附系数的影响可以忽略。得到的活性炭吸附剂样品具有良好的物理性能与惰性气体滞留性能,可应用于核电站废气处理系统活性炭滞留单元。     

放射性氙分离纯化技术

采用制备色谱技术并结合吸附材料性能的差异的方法,对不同温度下4A MS柱、5A MS柱、碳黑小球(601)柱、活性碳柱的性能进行了测定,根据测定结果确定了氙分离纯化流程的设计参数及实验参数.在设计的氙分离纯化流程的基础上,通过模拟实验测得该流程获得氙样品的产额好于90％,获得氙样品的纯度好于98％,样品能满足放射性测量...     

~(133)Xe示踪剂法研究活性碳纤维对大气本底水平氙的吸附性能

用133Xe作示踪剂研究了市售活性碳纤维对大气本底水平氙的吸附性能 ,并与粒状活性炭的吸附性能作了比较 ;测定了市售活性碳纤维的吸附效率。结果表明 ,市售的几种活性碳纤维在低温下对大气中氙的吸附性能均优于粒状椰壳活性炭     

氦气氛中氙在石墨球中扩散系数的测定

在核反应堆设计中,氙在石墨中的扩散是计算氙毒的一个重要因素。Salzano等曾在石英玻璃装置中利用不同扩散时间氙气向石墨球内的扩散量来测量高温负压下氙在石墨球中的扩散系数。Decken等简单地介绍了由石墨球中的氪向球外的不稳定扩散过程,测量氪在石墨球中的扩散系数。他把与一定氪分压(含有~(85)Kr)相平衡的石墨球从平衡容器中     

利用活性炭从氙气中分离碘的技术研究

利用吸附在活性炭上氙和碘解吸附温度的不同,建立了从氙气中分离碘的方法。以CF-1450椰壳活性炭为吸附材料,利用纯氙作载气,在200℃的温度下从氙气中提取碘,对氙的去污系数达到105,对碘的回收率接近100%。     

^133Xe示踪剂法研究活性碳纤维对大气本底水平氙的吸附性能

用^133Xc作示踪剂研究了市售活性碳纤维对大气本底水平氙的吸附性能,并与粒状活性炭的吸附性能作了比较;测定了市售活性碳纤维的吸附效率。结果表明,市售的几种活性碳纤维在低温下对大气中氙的吸附性能均优于粒状椰壳活性炭。     

低温下活性炭吸附分离Kr和Xe

研究了低温下活性炭吸附分离Kr和Xe的方法。Kr和Xe混合气在-78 ℃活性炭吸附柱上进行富集,根据Kr、Xe在活性炭柱上脱附条件的差异实现了Kr和Xe的分离。结果表明,Kr和Xe的回收率均大于90%,Kr样品中Xe的去污系数达10⁴以上,Xe样品中Kr的去污系数达10³以上。     

后处理厂释放气体中稳定惰性气体同位素在核保障监督中的应用研究

用Origen2．1计算模式对压水堆元件中Kr,Xe相关同位素与燃耗的关系进行了计算,并估算了后处理厂烟囱释放气体中Kr,Xe各稳定同位素的来源,丰度和原子浓度.^82Kr,^129Xe可用作环境样品中惰性气体同位素的天然本底;裂片^83Kr／^86Kr．^84Kr／^86Kr、^131Xe／^134Xe和^132Xe／^134Xe的丰度比值,可用于指示乏燃料燃耗,进而估算正在被分离的钚同位素组成,并有可能对后处理厂实行保障监督。     

Performance evaluation of a resonance ionization mass spectrometer developed for the FFDL system of fast reactors

To prevent a fuel failure event from becoming a serious radiation accident, sodium-cooled fast reactors are equipped with a system for failed fuel detection and location (FFDL). The FFDL instrument employed in the prototype fast breeder reactor Monju is based on the gas tagging method, in which precise and accurate measurements of krypton and xenon isotope ratios (⁷⁸Kr/⁸⁰Kr, ⁸²Kr/⁸⁰Kr and ¹²⁶Xe/¹²⁹Xe) must be performed in a short time. Burnup measurements also contribute to accurate determination of ⁸²Kr/⁸⁰Kr. We have developed a highly sensitive resonance ionization mass spectrometer for the isotopic analyses, which uses resonance ionization of Kr and Xe atoms by a pulsed laser at wavelengths of 216.7 and 249.6 nm, respectively. In evaluating the performance of our spectrometer, we find that systematic errors caused by isotope shifts can be reduced to negligible levels, and that statistical errors of 3% at a nuclide concentration of 7 ppt can be achieved with a single measurement time of about 40 minutes for each Kr and Xe isotope ratio. This means that, within one hour, about 200 fuel assemblies can be individually identified with a probability of 99%, verifying the applicability of our spectrometer to the FFDL system of fast reactors.     

Production of Multiply-Charged Ions of Ne, Ar, Kr and Xe by the Electron-Bonbarded Hot Cathode IoN Source of IPCR

Production of multiply-charged ions of Ne, Ar, Kr and Xe has been studied by use of an electron-bombarded hot cathode type ion source of the IPCR 160cm cyclotron, which is similar to Morozov's source. These multiply-charged ions were accelerated by a 3rd harmonics acceleration mode in the cyclotron and detected with a beam probe fixed at the radius of 55cm. Observed multiply-charged ions are Ne2+, Ne3+, Ne4+, Ne5+, Ar3+, Ar4+ Ar5+, Ar6+, Ar7+, Ar8+, Kr6+, Kr7+, Kr8+, Kr9+, Xe9+, Xe10+ and Xe11+. Relative abundance of each charge state of four elements were measured. In case of Kr and Xe , the intensity of observed multiply-charged ions decreased to 1/3 or 1/4 when the charge number is increased by one. Intensities of Ar4+, Ar6+, Ar8+, Kr6+ and Kr8+ were measured as a function of the operation conditions of the ion source, such as arc voltage, arc power and gas flow rate. It was found that a smaller gas flow and a higher arc power brought about a higher yield in all the measured ions. Obtained current intensities of ion source output are 40?A Ar8+, 600?A Kr6+, 40?A Kr9+, 150?A Xe9+ and 10?A Xe11+ respectively.     

复杂混合气体组分在低温活性炭表面的吸附特性

为实现大体积气体中微量放射性气体Kr、Xe同位素的测量,须将混合气体进行浓集并将目标气体吸附于10 mL左右的活性炭源盒中。本实验对混合气体中各组分在活性炭分离柱上的吸附性能进行研究,建立了通过去除其他杂质气体、浓集大体积气体制备放射性Kr和Xe活度源的方法。根据反应堆流出气体和核爆可能生成的气体组分,配制了模拟气体,使用活化的4A分子筛对其中的水和CO₂进行模拟去除,获得了流程中去除水和CO₂的实验条件;选择5个低温点(273、264、255、246、238 K),在低温活性炭柱上对H₂、CO、CH₄、Kr和Xe的吸附特性进行研究,测定了各气体在不同温度下的吸附穿透曲线。结果表明,室温下4A分子筛对水和CO₂有较好的吸附效果。低温下,H₂、CO不易在活性炭表面吸附;CH₄、Kr吸附性质相似;Xe吸附能力较强。低温下难以去除的CH₄可在高温下氧化去除。因此,可根据混合气体中各组分性质的不同实现杂质气体的去除和目标气体Kr、Xe的回收测量。     

碳分子筛上氪、氙的动态吸附及脱附性能

为筛选快速分离Kr/Xe的材料,研究了不同碳分子筛(CMS)对氙(Xe)和氪(Kr)的动态吸附性能与脱附性能,探讨了压力、气体流量、温度等因素对Kr、Xe的动态吸附系数与脱附率的影响。结果表明,碳分子筛Aladdin TDX-01对Xe的吸附容量最大,其次为光复TDX-01,低温时,Aladdin TDX-01对Kr的动态吸附系数大于光复TDX-01。Aladdin TDX-01碳分子筛对Kr和Xe的吸附能力均随压力升高而增强,随着原料气流量增加而减少,动态吸附系数随着温度升高而降低;采用N₂吹扫对Kr、Xe进行脱附,随着N₂流量增大、温度升高,Kr、Xe的脱附时间缩短。Aladdin TDX-01碳分子筛在25℃、100 kPa条件下对Xe的动态穿透吸附系数为1 283 mL/g,在-50℃、100 kPa条件下对Kr的动态穿透吸附系数为474 mL/g。     

Indirect assessment of 135Cs activity in the ventilation system of the Ignalina NPP RBMK-1500 reactor

The accumulation of long-lived ¹³⁵Cs isotope in the ventilation system components of the Ignalina NPP Unit 2 was investigated by spectrometric measurements and mathematical modeling. Volumetric activities of fission noble gas and other short-lived isotopes (⁴¹Ar, ^85mKr, ⁸⁷Kr, ⁸⁸Kr, ⁸⁸Rb, ¹³³Xe, ^133mXe, ¹³⁵Xe, ¹³⁸Xe, ¹³⁸Cs) have been measured by gamma spectrometric technique. Modeling of radionuclide transport in the ventilation system provides possibility of determining essential transport parameters: effective gas flow, mean gas retention time, deposition rate of aerosols. Estimated parameters were used for indirect evaluation of difficult to measure ¹³⁵Cs isotope activity in the ventilation system components: a delay chamber and aerosol filters. The results show that the major part of ¹³⁵Cs activity is accumulated in aerosol filters, whereas the total surface activity of the delay chamber is considerably lower. Specific activities of the ventilation system components of the Ignalina NPP Unit 2 are below the clearance levels for ¹³⁵Cs.     

AFM and STM investigation of carbon nanotubes produced by high energy ion irradiation of graphite

Carbon nanotubes (CNT) were produced by high energy, heavy ion irradiation (215 MeV Ne, 246 MeV Kr, 156 MeV Xe) of graphite. On samples irradiated with Kr and Xe ions large craters were found by atomic force microscopy, these are attributed to sputtering. Frequently one or several CNTs emerge from the craters. Some of the observed CNTs showed a regular vibration pattern. No other carbon based materials, like amorphous carbon or fullerenes were evidenced. Focused ion beam cuts were used to compare CNTs with surface folds on graphite.     

Studies of Ceramic Fuels with the Use of Fission Gas Release Loop, (II)

The γ-ray spectra of fission gases released from UO₂-graphite pellets under neutron irradiation were measured. With and without separating fission gases into xenon and krypton, 25 kinds of γ-ray were observed and assigned to nine nuclides, ^85mKr, ⁸⁷Kr, ⁸⁸Kr(⁸⁸Rb), ¹³³Xe, ¹³⁵Xe, ^135mXe and ¹³⁸Xe (¹³⁸Cs). A value of 15 min is proposed for the half-life of ¹³⁸Xe, based on analysis of the decay curves. Discussion is given on problems related to determination of the release rate of each fission product through measurement of the height of each peak in the γ-ray spectrum.     

Adsorption Equilibria of Krypton,Xenon, Nitrogen and Their Mixtures on Molecular Sieve 5A and Activated Charcoal

The adsorption equilibria of Kr, Xe and N₂, which are constituents of the off-gas from nuclear reprocessing processes, on representative adsorbents (Molecular Sieve 5A (MS5A) and activated charcoal) were studied. Adsorption experiments were conducted in the temperature range of 77 to 323 K using a packed bed column. The adsorption isotherms for the activated charcoal adsorbent were successfully correlated by the vacancy-solution model. The adsorption isotherms for the MS5A adsorbent were properly correlated by the Langmuir model and the vacancy solution model. The adsorption experiments for the binary component systems (Kr—Xe, Kr—N₂ systems) were also performed, and the results suggest that the coexistence of Xe greatly inhibits the adsorption of Kr. The coexistence of large amounts of N₂ was also found to inhibit the adsorption of Kr. The experimental results for the adsorption equilibrium of binary component systems on the activated charcoal adsorbent were well reproduced by the vacancy solution model without parameter fitting. The binary adsorption equilibrium on the MS5A adsorbent is rather well predicted by the ideal adsorbed solution model without parameter fitting. The use of the vacancy solution model for this adsorption system requires the optimization of parameters, but the binary adsorption equilibrium is well reproduced with the optimized parameters.