Isotopic signature and nano-texture of cesium-rich micro-particles: Release of uranium and fission products from the Fukushima Daiichi Nuclear Power Plant.

Isotopic signature and nano-texture of cesium-rich micro-particles: Release of uranium and fission products from the Fukushima Daiichi Nuclear Power Plant.
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DOI:
10.1038/s41598-017-05910-z
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发表时间:
2017-07-14
期刊:
影响因子:
4.6
通讯作者:
Utsunomiya S
Utsunomiya S
中科院分区:
综合性期刊3区
文献类型:
--
作者:
Imoto J;Ochiai A;Furuki G;Suetake M;Ikehara R;Horie K;Takehara M;Yamasaki S;Nanba K;Ohnuki T;Law GTW;Grambow B;Ewing RC;Utsunomiya S

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从福岛第一核电站(FDNPP)释放的高放射性富铯微粒(Csmp)提供了2011年悲剧的纳米级化学指纹。在距FDNPP约10 km范围内采集了3个CsMP(3.79-780 Bq),测定了其U、Cs、Ba、Rb、K和Ca同位素比值,以确定CsMP的来源和形成机制。除了结晶铁铯榴石CsFeSi 2 O 6·nH 2 O外,CsMP主要由SiO2玻璃基质中的Zn-Fe-氧化物纳米颗粒组成(高达约30wt%的Cs和约1wt%的U主要与Zn-Fe-氧化物相关)。两种CsMP的235 U/238 U值分别为0.030(±0.005)和0.029(±0.003),与浓缩核燃料的235 U/238 U值一致。这些值高于ORIGEN代码估计的平均燃耗,低于非辐照燃料,表明U从具有不同燃耗水平的熔融燃料中的不均匀挥发,然后吸附到锌铁氧化物上。纳米尺度的结构和同位素分析提供了熔毁期间燃料中发生的化学反应的部分记录。此外,CsMP是可吸入形式释放的放射性核素的重要运输介质。
Highly radioactive cesium-rich microparticles (CsMPs) released from the Fukushima Daiichi Nuclear Power Plant (FDNPP) provide nano-scale chemical fingerprints of the 2011 tragedy. U, Cs, Ba, Rb, K, and Ca isotopic ratios were determined on three CsMPs (3.79–780 Bq) collected within ~10 km from the FDNPP to determine the CsMPs’ origin and mechanism of formation. Apart from crystalline Fe-pollucite, CsFeSi2O6 · nH2O, CsMPs are comprised mainly of Zn–Fe-oxide nanoparticles in a SiO2 glass matrix (up to ~30 wt% of Cs and ~1 wt% of U mainly associated with Zn–Fe-oxide). The 235U/238U values in two CsMPs: 0.030 (±0.005) and 0.029 (±0.003), are consistent with that of enriched nuclear fuel. The values are higher than the average burnup estimated by the ORIGEN code and lower than non-irradiated fuel, suggesting non-uniform volatilization of U from melted fuels with different levels of burnup, followed by sorption onto Zn–Fe-oxides. The nano-scale texture and isotopic analyses provide a partial record of the chemical reactions that occurred in the fuel during meltdown. Also, the CsMPs were an important medium of transport for the released radionuclides in a respirable form.
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