An Analytical model to decompose mass transfer and chemical process contributions to molecular iodine release from aqueous phase under severe accident conditions

Zablackaite, G.; 塩津 弘之; 城戸 健太朗; 杉山 智之

Nuclear Engineering and Technology, 56(2), p.536 - 545, 2024/02

https://doi.org/10.1016/j.net.2023.10.030

Radioactive iodine is a representative fission product to be quantified for the safety assessment of nuclear facilities. In integral severe accident analysis codes, the iodine behavior is usually described by a multi-physical model of iodine chemistry in aqueous phase under radiation field and mass transfer through gas-liquid interface. The focus of studies on iodine source term evaluations using the combination approach is usually put on the chemical aspect, but each contribution to the iodine amount released to the environment has not been decomposed so far. In this study, we attempted the decomposition by revising the two-film theory of molecular-iodine mass transfer. The model involves an effective overall mass transfer coefficient to consider the iodine chemistry. The decomposition was performed by regarding the coefficient as a product of two functions of pH and the overall mass transfer coefficient for molecular iodine. The procedure was applied to the EPICUR experiment and suppression chamber in BWR.

Estimation for mass transfer coefficient under two-phase flow conditions using two gas components

南上 光太郎; 塩津 弘之; 丸山 結; 杉山 智之; 岡本 孝司*

Journal of Nuclear Science and Technology, 60(7), p.816 - 823, 2023/07

https://doi.org/10.1080/00223131.2022.2146015

For proper source term evaluation, we constructed the theoretical model to estimate the mass transfer coefficient of gaseous iodine species under two-phase flow conditions, which complicates the direct experimental measurements. The mass transfer speed is determined by the product of the overall mass transfer coefficient and the interfacial area. By using the ratio of two gas components, the interfacial area, which is an important parameter that is difficult to measure, can be canceled out and the ratio of their overall mass transfer coefficients can be obtained. This ratio is expected to be equal to the ratio of their diffusion coefficients. Therefore, the unknown mass transfer coefficient such as iodine species can be estimated using the diffusion coefficients of two gas components and the reference mass transfer coefficient such as O. We carried out the experiments using the bubble column to confirm this relationship. From the results in this study, we confirmed that the ratio of the overall mass transfer coefficient was in good agreement with the ratio of diffusion coefficient under the bubbly flow conditions. Using this relationship confirmed in this study, we estimated the mass transfer coefficient of I, one of the iodine species.

Numerical analysis for FP speciation in VERDON-2 experiment; Chemical re-vaporization of iodine in air ingress condition

塩津 弘之; 伊藤 裕人*; 杉山 智之; 丸山 結

Annals of Nuclear Energy, 163, p.108587_1 - 108587_9, 2021/12

https://doi.org/10.1016/j.anucene.2021.108587

In the late phase of severe accident in light water reactor nuclear power station, re-mobilization of fission products (FPs) has a significant impact on the source term because most portion of FPs is retained in reactor coolant system and/or containment vessel. Recently, VERDON-2 experiment showed noticeable re-vaporization, which was one of the re-mobilization phenomena, of iodine under air ingress condition, but this mechanism has not been identified yet. The present study numerically investigated the FPs behaviors in VERDON-2 experiment with the mechanistic FPs transport analysis code incorporating thermodynamic chemical equilibrium model in order to further understand nature for FPs behavior, especially iodine re-vaporization under air ingress condition. Consequently, this analysis reproduced the deposition profile of cesium, one of important FPs in the source term, along the thermal gradient tube (TGT) in the experiment, which revealed that cesium was transported as CsOH in early phase of FP release from fuel, and then formed CsMoO and CsTe after the release of molybdenum and tellurium was activated. Regarding iodine as another important FP, formation of CsI was predicted in steam condition. The CsI was transported and partly deposited and condensed onto the TGTs and other components of the VERDON facility. Under the air ingress condition, the present analysis showed the agreement for iodine re-vaporization in the experiment and revealed its mechanism; the deposits of iodide were chemical re-vaporized as molecular iodine (I) gas by redox reaction with competitive elements such as molybdenum, chromium and tellurium.

CHEMKEq; 化学平衡論及び反応速度論の部分混合モデルに基づく化学組成評価コード(受託研究)

伊藤 裕人*; 塩津 弘之; 田中 洋一*; 西原 慧径*; 杉山 智之; 丸山 結

JAEA-Data/Code 2018-012, 42 Pages, 2018/10

JAEA-Data-Code-2018-012.pdf:4.93MB

原子力施設事故時において施設内を移行する核分裂生成物(FP)の化学組成は、比較的遅い反応の影響を受けることにより化学平衡を仮定して評価した組成とは異なる場合が想定される。そのため、反応速度を考慮した化学組成評価が求められる。一方で、原子力施設事故時の複雑な反応に関する反応速度の知見は現状では限られており、実機解析に適用できるデータベースの構築に至っていない。そこで、FP化学組成評価における反応速度による不確かさの低減のため、化学平衡論及び反応速度論の部分混合モデルに基づく化学組成評価コードCHEMKEqを開発した。このモデルは、系全体の質量保存則の下、前駆平衡と見なせる化学種を化学平衡論モデルにより評価し、その後の比較的遅い反応を反応速度論モデルにより解くものである。さらにCHEMKEqは、本混合モデルに加え一般的な化学平衡論モデル及び反応速度論モデルが使用可能であり、かつ、それらモデル計算に必要なデータベースを外部ファイル形式とすることで汎用性の高い化学組成評価コードとなっている。本報は、CHEMKEqコードの使用手引書であり、モデル, 解法, コードの構成とその計算例を記す。また付録には、CHEMKEqコードを使用する上で必要な情報をまとめる。

Influence of chemical speciation in reactor cooling system on pH of suppression pool during BWR severe accident

塩津 弘之; 石川 淳; 杉山 智之; 丸山 結

Journal of Nuclear Science and Technology, 55(4), p.363 - 373, 2018/04

https://doi.org/10.1080/00223131.2017.1403381

The influences of chemical speciation for Cs-I-Te-Mo-Sn-B-C-O-H system, simulating a state in the reactor cooling system (RCS) of BWR, on pH of the suppression chamber (S/C) water pool were analytically investigated with PHREEQC code. Major conditions were chosen on the basis of the outputs from a BWR severe accident analysis by THALES2 code and chemical thermodynamic analysis with VICTORIA2.0 code. The chemical thermodynamic analysis showed that the chemical speciation of important volatile FPs, Cs and I, was strongly influenced by Mo and BC control material. As a consequence, pH of the S/C water pool was predicted to range from approximately 6 to 10, depending on the fraction of volatile FPs transported from the RCS to the S/C water pool and the H/HO ratio associated with the oxygen potential. It was implied that the formation of volatile I species such as I in the S/C water pool was larger by 3 orders at the lowest pH than that at the highest pH.

Source term analysis considering BC/steel interaction and oxidation during severe accidents

石川 淳; 塩津 弘之; 杉山 智之; 丸山 結

Proceedings of 25th International Conference on Nuclear Engineering (ICONE-25) (CD-ROM), 7 Pages, 2017/07

The Japan Atomic Energy Agency (JAEA) is pursuing the development and application of the methodologies on fission product (FP) chemistry for source term analysis by using the integrated severe accident analysis code THALES2. In the present study, models for the eutectic interaction of boron carbide (BC) with steel and the BC oxidation were incorporated into THALES2 code and applied to the source term analyses for a boiling water reactor (BWR) with Mark-I containment vessel (CV). Two severe accident sequences with drywell (D/W) failure by overpressure initiated by loss of core coolant injection (TQUV sequence) and long-term station blackout (TB sequence) were selected as representative sequences. The analyses indicated that a much larger amount of species from the BC oxidation was produced in TB sequence than TQUV sequence. More than a half of carbon dioxide (CO) produced by the BC oxidation was predicted to dissolve into the water pool of the suppression chamber (S/C), which could largely influence pH of the water pool and consequent formation and release of volatile iodine species.

Radioactive Cs in the severely contaminated soils near the Fukushima Daiichi Nuclear Power Plant

金子 誠*; 岩田 孟; 塩津 弘之; 正木 翔太*; 川元 侑治*; 山崎 信哉*; 仲松 有紀*; 井元 純平*; 古木 元気*; 落合 朝須美*; et al.

Frontiers in Energy Research (Internet), 3, p.37_1 - 37_10, 2015/09

https://doi.org/10.3389/fenrg.2015.00037

高線量土壌中の放射性Csは雲母鉱物などの層状ケイ酸塩鉱物に取り込まれていることを現地調査及び模擬実験により明らかにした。

Parametric study for impact of in-vessel chemical forms of cesium and iodine on source term and pH of aqueous phase

塩津 弘之; 石川 淳; 丸山 結

Proceedings of 23rd International Conference on Nuclear Engineering (ICONE-23) (DVD-ROM), 6 Pages, 2015/05

In order to evaluate the effect of chemical forms of Cs and I on source terms and solution pH in a severe accident of a BWR, parametric analysis was performed with an integral severe accident code, THALES2, developed by JAEA. In the present analysis, THALES2 code was modified to take into account CsOH, CsMoO and CsBO as Cs chemical forms, and CsI and HI as I chemical forms. The severe accident sequence examined was similar to that occurred at unit 3 of the Fukushima Dai-ichi NPP. Due to the effective scrubbing, approximately 90% of the initial core inventory of Cs and I was predicted to be retained in the water pool of the suppression chamber, resulting in limited influence of Cs chemical form on Cs source term. On the other hand, the present analysis indicated that solution pH of the water pool was strongly affected by chemical forms of Cs and I. This outcome implies that chemical forms of Cs and I influence I source term since the formation of volatile I species such as I2 and organic iodine in the water pool depends strongly on solution pH.

Mechanism and crystallochemical signature of nano-particle formation by microorganisms

塩津 弘之; Giang, M.*; 仲松 有紀*; 大貫 敏彦; 宇都宮 聡*

no journal, , 

We investigated to understand the effect of pH, coexistent REEs and the functional group of cells surfaces on the crystal chemistry of biogenic nanoparticle formation. These nano-particles were characterized as phosphate containing a series of REEs. The nano-particles at pH 3 had monazite structure, while the particles forming at pH 4 and 5 were amorphous. REE phosphate inorganically synthesized at room temperature revealed crystalline structure (monazite, xenotime or habdophane) depending on the element. Additional inorganic model experiments using the CMC, Ln resin and Cellulose Phosphate, which have the functional groups similar to cell surfaces, demonstrated that the nano-particles precipitated without structure. Based on these data it is suggested that adsorption to the functional groups on the cell surfaces constrain the shape and structure of nanoparticles.

Formation of rare earth phosphate nano-particles by microorganisms

塩津 弘之; Jiang, M.*; 仲松 有紀*; 大貫 敏彦; 宇都宮 聡*

no journal, , 

We investigated to understand the effect of pH, coexistent REEs and the functional group of cells surfaces on the crystal chemistry of biogenic nanoparticle formation. These nano-particles were characterized as phosphate containing a series of REEs. The nano-particles at pH3 had monazite structure, while the particles forming at pH4 and 5 were amorphous. REE phosphate inorganically synthesized at room temperature revealed crystalline structure (monazite, xenotime or habdophane) depending on the element. Additional inorganic model experiments using the CMC, Ln resin and Cellulose Phosphate, which have the functional groups similar to cell surfaces, demonstrated that the nano-particles precipitated without structure. Based on these data it is suggested that adsorption to the functional groups on the cell surfaces constrain the shape and structure of nanoparticles.