Formation of radioactive cesium microparticles originating from the Fukushima Daiichi Nuclear Power Plant accident: characteristics and perspectives

ABSTRACT

Following identification of radioactive Cs microparticles (CsMPs) in aerosol samples from the Fukushima Daiichi Nuclear Power Plant (FDNPP), numerous reports on CsMPs have been published. This paper reviews recent progress in the measurement and characterization of CsMPs by advanced analytical techniques, including advanced transmission electron microscopy (TEM) and synchrotron X-ray analysis. These analyses revealed that the CsMPs contained Si, Fe, Zn, Cs, and minor quantities of U together with some fission products. Uranium in the CsMPs was identified as being in the form of uraninite and (U,Zr)O₂. Detailed advanced TEM analysis has clarified some of the processes resulting in the alteration of constituents of the nuclear fuels and containment vessel materials during this severe accident. In addition, a detailed report on the elemental compositions and structures of the fuel debris fragments collected inside and outside of the primary containment vessel²⁵ highlighted the fact that the fuel debris fragments contained nanoparticles with the U and Zr components having similar structures to that of the CsMPs. This similarity in structures has stimulated further research on the structure and elemental constituents, especially for U and Zr in the CsMPs, and has opened up new avenues for studying the chemical characteristics of the fuel debris.     

A new composite of crystalline silicotitanate for sequestration of 137Cs and 90Sr from low-level aqueous waste solution

ABSTRACT

A new composite of crystalline silicotitanate (CST) has been synthesized for the sequestration of Cs and Sr from low-level liquid waste generated in the nuclear industry. The product characterization using X-RAY DEFRACTION (XRD) and Fourier-transform infrared spectroscopy (FTIR) confirmed the presence of CST crystals in the composite. Sorption studies carried out under various test conditions showed that the composite has high affinity for both Cs and Sr. Results of structural characterization of Cs and Sr-loaded CST indicated that the overall structural integrity remained intact after substitution of Na⁺ by Cs⁺ or Sr²⁺. The exceedingly good Cs and Sr sorption performance displayed by the CST composite will find applications in the treatment of nuclear waste.     

Measurements of thermal-neutron capture cross-section of Cesium-135 by applying mass spectrometry

ABSTRACT

The thermal-neutron capture cross-section (σ₀) and resonance integral (I₀) were measured for the ¹³⁵Cs(n,γ)¹³⁶Cs reaction by an activation method and mass spectrometry. Because of difficulty in the preparation of pure ¹³⁵Cs samples, we used ¹³⁵Cs contained as an impurity in a normally available ¹³⁷Cs standard solution. An isotope ratio of ¹³⁵Cs and ¹³⁷Cs in a standard ¹³⁷Cs solution was measured by mass spectrometry to quantify ¹³⁵Cs. Cesium-135 impurity along with the ¹³⁷Cs standard solution was irradiated at the hydraulic conveyer of the research reactor in the Institute for Integral Radiation and Nuclear Science, Kyoto University. Wires of Co/Al and Au/Al alloys were used as neutron monitors to measure thermal-neutron fluxes and epi-thermal Westcott’s indices at an irradiation position. A gadolinium filter was used to measure the σ₀, and a value of 0.133 eV was taken as the cut-off energy. Gamma-ray spectroscopy was used to measure induced activities of ¹³⁷Cs, ¹³⁶Cs and monitor wires. On the basis of Westcott’s convention, the σ₀ and I₀ values were derived as 8.57 ± 0.25 barn, and 45.3 ± 3.2 barn, respectively. The value of σ₀ obtained in the present study agreed within the limits of uncertainties with the past-reported value of 8.3 ± 0.3 barn.     

一维普鲁士蓝/硅藻土复合材料对Cs+的吸附

含137Cs的放射性废水处理在核能及核技术应用中具有重要意义。以表面活性剂十六烷基三甲基溴化钾和十二烷基磺酸钠为模版，合成了一维结构的普鲁士蓝并将其附着在硅藻土表面，制备成一维普鲁士蓝/硅藻土复合材料；在不同的温度、吸附时间、pH值下，分别探究了一维普鲁士蓝/硅藻土复合材料对Cs⁺的吸附性能，并研究了溶液中其他阳离子对吸附的影响。结果表明：一维普鲁士蓝/硅藻土对Cs⁺的吸附能力随温度（293～318 K）的升高而增加（从42.4 mg/L到61.6 mg/L），其吸附行为符合Langmuir等温线和准二级动力学方程。     

Ion Exchange of Selected Group II Metals and Lead by Crystalline Silicotitanate and Competition for Cs Exchange Sites

ABSTRACT

A series of batch contact tests were conducted to evaluate the exchange behavior of Ba, Ca, Pb, and Sr onto crystalline silicotitanate (CST) in support of an expedited Cs removal and pretreatment system at the Hanford site. Binary Na/M²⁺ and ternary Na/Cs/M²⁺ isotherms were generated to understand selectivity, capacity, and competitive impact of each analyte on Cs uptake from a simple 1 M NaOH/4.6 M NaNO₃ simulant. Analyte loading from a 0.1 M NaOH/5.5 M NaNO₃ simulant was assessed to determine the effect of hydroxide concentration on binary Na/M²⁺ isotherms. Results from binary and ternary isotherms indicated that Group II metals Ca, Sr, and Ba (and Pb) do not impact CST performance toward Cs removal at concentrations expected in Hanford tank-waste supernate.     

Bphen掺杂Cs_2CO_3作为电子传输层对OLED器件性能的影响

为改善OLED器件的载子注入平衡,本文在其结构ITO/MoO3/NPB/Alq3/Cs2CO3/Al中,分别引入高电子迁移率材料Bphen及Bphen∶Cs2CO3作为电子传输层。通过改变Bphen的厚度以及Bphen中Cs2CO3的体积掺杂浓度,研究其对器件发光亮度、电流密度和效率等性能的影响。实验结果表明,采用Bphen或者Bphen∶Cs2CO3作为电子传输层,均能提高器件的电子注入能力,改善器件的性能。相比于未引入Bphen的器件,采用25nm的Bphen作为电子传输层,改善了器件的电子注入,使器件的最大电流效率提高112%;采用体积掺杂浓度为15%,厚度为5nm的Bphen∶Cs2CO3作为电子传输层,减小了电子注入势垒,使器件的最大电流效率提高27%,并且掺杂层厚度的改变对器件的电子注入影响很小。该方法可用于OLED器件的阴极修饰,对器件性能的提升将起到一定的促进作用。     

海水中134Cs、137Cs和60Co的联合分析

建立了小体积海水中¹³⁴Cs、¹³⁷Cs和⁶⁰Co的联合分析方法，确定了最佳实验条件。采用磷钼酸铵富集法对海水中放射性铯进行浓集后，其上清液利用氢氧化钴沉淀载带海水中的⁶⁰Co，用γ能谱仪进行测量。结果表明：该法对海水中放射性¹³⁴Cs、¹³⁷Cs和⁶⁰Co的回收率分别为87%~95%、87%~95%和89%~93%，检测限分别为0.048、0.051、0.046 Bq/L。另外，对2017年IAEA国际比对（IAEA-RML-2017-01）海水样品中的¹³⁴Cs、¹³⁷Cs和⁶⁰Co进行分析测量，核素分析结果的最终评价均为“通过”，验证了本实验室采用的¹³⁴Cs、¹³⁷Cs和⁶⁰Co联合分析方法的可行性和可靠性，为今后该方法在常规海洋环境放射性监测中的应用推广奠定了基础。     

The dispersed SiO2 microspheres supported Ru catalyst with enhanced activity for ammonia decomposition

Ru nanoparticles supported on SiO₂ microspheres (Ru/SiO₂-GUS) were prepared by the glucose-urea-metallic salt method and applied in the decomposition of ammonia. In the glucose-urea-metallic salt method, glucose as the carbon template plays a significant role in the formation of diffusion-beneficial structural properties of Ru/SiO₂-GUS, and also induceds the modification of the electronic state of Ru. Ru/SiO₂-GUS exhibited higher catalytic activity compared with the catalyst prepared with the impregnation method. The catalytic performance of Ru/SiO₂-GUS was further enhanced with the addition of either K or Cs——the addition order and amount strongly affecting the catalytic performance. When the ratio of K/Cs to Ru is 2, the alkali metal (KOH/CsOH) solution is added in the homogeneous solution of glucose, urea, RuCl₃ and the colloidal silica, the promotion effect of K/Cs is the strongest, particularly under lower reaction temperatures. However, the promotion effects of K and Cs are different as reveled by the combined results of H₂-TPR, XPS and NH₃-TPSR. More NH₃ can be absorbed on K–Ru/SiO₂-GUS and the electron density of Ru decreased. By contrast, more metallic Ru formed on Cs–Ru/SiO₂-GUS, facilitating N₂ recombination.     

利用福岛第一核电厂事故期间环境监测资料反推事故释放源项

2011年3月11日,日本福岛核事故导致放射性物质向大气环境的大规模释放。本工作利用大气数值预报模式WRFV2.2.1和大气弥散模式CALPUFF,对事故期间放射性物质的大气输运和弥散进行了模拟。应用大气释放源项的逆推算方法,结合单位释放率条件下的大气弥散模拟结果和环境监测数据,对福岛第一核电厂1到3号机组向大气环境释放的放射性核素总量进行了评估,推算的131I和137 Cs气载释放量分别为8.6×1016 Bq和8.6×1015 Bq。     

Temporal changes in vertical distribution of 137Cs in litter and soils in mixed deciduous forests in Fukushima,Japan

Downward migration of ¹³⁷Cs in soils was studied in three mixed deciduous forests c.a. 40 km northwest of the Fukushima Daiichi Nuclear power plant (FDNPP), Japan. We selected three different types of forest regarding to environmental condition such as slope inclinations and snow coverage conditions at the time of deposition. We examined temporal changes in the vertical distribution of ¹³⁷Cs from litter layers to 10 cm soil depth for two years (2.3 to 4.3 years after the FDNPP accident in 2011). At all three study sites, the ¹³⁷Cs in the litter layer had largely migrated to surface soil by 2013. After 2014, about 80% of the ¹³⁷Cs in forest soils (litter layer to 10 cm soil depth) remained within 0–5 cm soil layer. The vertical distribution had not changed substantially since 2014, suggesting that changes to the downward migration rates of ¹³⁷Cs in soils drastically decreased with time. In addition, small amounts of migrating ¹³⁷Cs could not be detected by the present method because there was a large spatial variation in the distribution of soil ¹³⁷Cs. The results showed similar patterns of soil ¹³⁷Cs distribution among the three study sites although there were differences in the environmental conditions.