Droplet evaporation characteristics on high-temperature porous surfaces for cooling fuel debris

Yuki, Kohei*; Horiguchi, Naoki; Yoshida, Hiroyuki; Yuki, Kazuhisa*

Proceedings of 31st International Conference on Nuclear Engineering (ICONE31) (Internet), 4 Pages, 2024/11

https://doi.org/10.1115/ICONE31-135281

Fuel debris in the Fukushima Nuclear Power Station is cooled under immersion condition. However, in the event of an unexpected decrease in water level, coolant contacts high-temperature fuel debris having porous structure. In this event, although fuel debris needs to be cooled rapidly, thermal behavior at liquid-solid contact, such as capillary phenomenon, remains unclear. In this paper, as basic research, we evaluate droplet evaporation characteristics after contact with metal porous media with small pores less than 1 mm. In experiment, to obtain life time curve of a droplet, bronze or stainless steel porous media having 1, 40, or 100 m pore diameter are utilized. Experimental results show that Leidenfrost phenomenon is suppressed on the porous surfaces because generated vapor can be discharged from the pores. Further, for bronze porous media, capillary phenomenon is observed as the temperature of the porous media increase because of generation of oxide film having fine structure. On the other hand, due to low wettability of stainless steel porous media, capillary phenomenon does not occur, and the droplet was not sucked and spread into pore. This indicates that rapid cooling by the capillary phenomenon can not be expected if fuel debris has the same characteristics as the stainless steel porous media.

Criticality safety evaluation of high active liquid waste during the evaporation to dryness process at Tokai Reprocessing Plant

Miura, Takatomo; Kudo, Atsunari; Koyama, Daisuke; Obu, Tomoyuki; Samoto, Hirotaka

Proceedings of 12th International Conference on Nuclear Criticality Safety (ICNC2023) (Internet), 10 Pages, 2023/10

Tokai Reprocessing Plant (TRP) had reprocessed 1,140 tons of spent fuel discharged from commercial reactors (BWR, PWR) and Advanced Thermal Reactor "Fugen" from 1977 to 2007. TRP had entered decommissioning stage in 2018. In order to reduce the risk of High Active Liquid Waste (HALW) held at the facility, the vitrification of HALW is given top priority. HALW generated from reprocessing of spent fuel contains not only fission products (FPs) but also trace amounts of uranium (U) and plutonium (Pu) within the liquid and insoluble residues (sludge). Under normal conditions, concentrations of U and Pu in HALW are very low so that it can not reach criticality. Since FPs with high neutron absorption effect coexists in HALW, even if the cooling function is lost due to serious accident and HALW evaporates to dryness, it is considered that criticality would not been reached. In order to confirm this estimation quantitatively, criticality safety evaluations were carried out for the increase of U and Pu concentrations by evaporation of HALW to the point of dryness. In this evaluation, infinite multiplication factors were calculated for each of solution system and sludge system of HALW with respect to the concentration change through evaporation to dryness. It is confirmed it could not reach criticality. The abundance ratios of U, Pu and FPs were set conservatively based on analytical data and ORIGEN calculation results. Multiplation factors for two-layer infinite slab model of solution and sludge systems of HALW were also calculated, and it was confirmed it could not reached criticality. In conclusion, the result was gaind that there could be no criticality even in the process through evaporation to dryness of HALW in TRP.

Development of simulation program; SHAWED for analysis of accident of evaporation to dryness by boiling of reprocessed high level liquid waste in tank

Yoshida, Kazuo; Tamaki, Hitoshi; Hiyama, Mina*

JAEA-Research 2022-011, 37 Pages, 2022/12

JAEA-Research-2022-011.pdf:2.88MB

An accident of evaporation to dryness by boiling of high level liquid waste (HLLW) is postulated as one of the severe accidents at a fuel reprocessing plant. Two major mechanisms are expected for fission products (FPs) transfer from liquid to vapor phase. One is non-volatiles FPs transfer in the form of mists to the vapor phase in the tank, the other is volatilization of such as Ruthenium. These FPs transferred to the vapor phase in the tank could be released with water and nitric-acid mixed steam and NO gas flow to the environment. NO is generated from denitration of nitrate fission products during dry out phase. These phenomena occurred in this accident originate from the liquid waste boiling in the tank. It is essential for the risk assessment of this accident to simulate thermo-hydraulic and chemical behaviors in the waste tank quantitatively with a versatile computer program. The SHAWED (imulation of igh-level radioctive aste vaporation and ryness) has been developed to realize these requirements. In this report, detailed description of major analytical models is explained based on the features of this accident, and some simulation examples are also described for the use in an actual risk assessment.

Analysis of risk reduction effect of supposed steam condenser implementation as accident measure for accident of evaporation to dryness by boiling of reprocessed high level liquid waste

Yoshida, Kazuo; Tamaki, Hitoshi; Hiyama, Mina*

JAEA-Research 2021-013, 20 Pages, 2022/01

JAEA-Research-2021-013.pdf:2.35MB

An accident of evaporation to dryness by boiling of high level liquid waste (HLLW) is postulated as one of the severe accidents caused by the loss of cooling function at a fuel reprocessing plant. In this case, volatile radioactive materials, such as ruthenium (Ru) are released from the tanks with water and nitric-acid mixed vapor into atmosphere. An idea has been proposed to implement a steam condenser as an accident countermeasure. This measure is expected to prevent nitric acid steam diffusing in facility building and to increase gaseous Ru trapping ratio into condensed water. A simulation study has been carried out with a hypothetical typical facility building to analyze the efficiency of steam condenser. In this study, SCHERN computer code simulates chemical behaviors of Ru in nitrogen oxide, nitric acid and water mixed vapor based on the conditions obtained from simulation with thermal-hydraulic computer code MELCOR. The effectiveness of steam condenser has been analyzed quantitively in preventing mixed vapor diffusion and gaseous Ru trapping effect. Some issues to be solved in analytical model has been also clarified in this study.

SCHERN-V2: Technical guide of computer program for chemical behavior in accident of evaporation to dryness by boiling of reprocessed high level liquid waste in Fuel Reprocessing Facilities

Yoshida, Kazuo; Tamaki, Hitoshi; Hiyama, Mina*

JAEA-Data/Code 2021-008, 35 Pages, 2021/08

JAEA-Data-Code-2021-008.pdf:3.68MB

An accident of evaporation to dryness by boiling of high level liquid waste (HLLW) is postulated as one of the severe accidents caused by the loss of cooling function at a fuel reprocessing plant. In this case, volatile radioactive materials, such as ruthenium (Ru) are released from the tanks with water and nitric-acid mixed vapor into atmosphere. In addition to this, nitrogen oxides (NO) are also released formed by the thermal decomposition of metal nitrates of fission products (FP) in HLLW. It has been observed experimentally that NOx affects to the migration behavior of Ru at the anticipated atmosphere condition in cells and/or compartments of the facility building. Chemical reactions of NO with water and nitric acid are also recognized as the complex phenomena to undergo simultaneously in the vapor and liquid phases. The analysis program, SCHERN has been under developed to simulate chemical behavior including Ru coupled with the thermo-hydraulic condition in the flow paths in the facility building. This technical guide for SCHERN-V2 presents the overview of covered accident, analytical models including newly developed models, differential equations for numerical solution, and user instructions.

Restraint effect of coexisting nitrite ion in simulated high level liquid waste on releasing volatile ruthenium under boiling condition

Yoshida, Ryoichiro; Amano, Yuki; Yoshida, Naoki; Abe, Hitoshi

Journal of Nuclear Science and Technology, 58(2), p.145 - 150, 2021/02

https://doi.org/10.1080/00223131.2020.1825235

In the "evaporation and dryness due to the loss of cooling functions" which is one of the severe accidents at reprocessing plants in Japan, ruthenium (Ru) is possible to be released much more than other elements to the environment. This cause is considered that the volatile Ru compound can be released from high level liquid waste (HLLW) as gaseous compound in adding to the release by entrainment. It was expected that the release of the volatile Ru compound from the HLLW may be able to be restrained by coexisting nitrite ion because of its reduction power. To confirm the effect of nitrite ion on the release behavior of the volatile Ru compound, four experiments of heating the simulated HLLW (SHLLW) with setting the concentration of nitrite ion in the SHLLW as a parameter ware carried out. As a result, the release of the volatile Ru compound was seemed to be restrained by adding nitrite sodium as a source of nitrite ion under certain boiling condition. This result may contribute to improve source term analysis in the evaporation and dryness due to the loss of cooling functions.

SCHERN: Analysis program for chemical behavior of nitrogen oxide in accident of evaporation to dryness by boiling of reprocessed high level liquid waste in Fuel Reprocessing Facilities

Hiyama, Mina*; Tamaki, Hitoshi; Yoshida, Kazuo

JAEA-Data/Code 2019-006, 17 Pages, 2019/07

JAEA-Data-Code-2019-006.pdf:1.84MB

An accident of evaporation to dryness by boiling of high level liquid waste (HLLW) is postulated as one of the severe accidents caused by the loss of cooling function at a fuel reprocessing plant. In this case, volatile radioactive materials, such as ruthenium (Ru) are released from the tanks with water and nitric-acid mixed vapor into atmosphere. In addition to this, nitrogen oxides (NOx) are also released formed by the thermal decomposition of metal nitrates of fission products (FP) in HLLW. It has been observed experimentally that NOx affects strongly to the transport behavior of Ru at the anticipated atmosphere condition in cells and/or compartments of the facility building. Chemical reactions of NOx with water and nitric acid are also recognized as the complex phenomena to undergo simultaneously in the vapor and liquid phases. An analysis program has been developed to simulate chemical reaction coupled with the thermo-hydraulic condition in the flow paths in the facility building.

Behavior of cesium molybdate, CsMoO, in severe accident conditions, 1; Partitioning of Cs and Mo among gaseous species

Do, Thi Mai Dung*; Sujatanond, S.*; Ogawa, Toru

Journal of Nuclear Science and Technology, 55(3), p.348 - 355, 2018/03

https://doi.org/10.1080/00223131.2017.1397560

In order to better understand the behavior of cesium in the severe accident of the LWR, the high-temperature chemistry of CsMoO in HO+H gas was studied. The pseudo-binary system, CsMoO-MoO, was thermochemically modeled with Redlich-Kister formulation to form a basis to analyze the high-temperature behavior of CsMoO. The model prediction was compared with the thermogravimetric measurements of CsMoO in dry and humid argon, which revealed that the mass-loss rate was enhanced in the humid atmosphere. Thermochemical model was further applied to predict the partitioning of cesium and molybdenum among gaseous species in the BWR core degradation condition typical of Short-Term Station Blackout.

Hydrogen production tests by hydrogen iodide decomposition membrane reactor equipped with silica-based ceramics membrane

Myagmarjav, O.; Tanaka, Nobuyuki; Nomura, Mikihiro*; Kubo, Shinji

International Journal of Hydrogen Energy, 42(49), p.29091 - 29100, 2017/12

https://doi.org/10.1016/j.ijhydene.2017.10.043

The catalytic decomposition of hydrogen iodide in a membrane reactor using silica membranes derived from hexyltrimethoxysilane (HTMOS) was investigated for the production of hydrogen in the thermochemical water splitting iodine-sulfur process. The silica membranes were prepared by counter-diffusion chemical vapor deposition using porous alumina support tubes in both the absence and presence of a -alumina layer. The silica membranes formed on -alumina-coated -alumina tubes displayed a higher H permeance than that formed directly on an -alumina tube. A silica membrane based on a 1.5 m-thick -alumina layer fabricated under deposition conditions of 450C, 1200 s, and a N carrier gas velocity of 0.044 m s exhibited a high H permeance of 9.4 10 mol Pa m s while maintaining an H/N selectivity of over 80.0. The performance of a membrane reactor based on an HTMOS-derived silica membrane was evaluated at 400C by measuring the HI conversion and H flow rates. The conversion was approximately 0.48 when the HI flow rate was 9.7 mL min.

Determination of optimal vapor pressure data by the second and third law methods

Nakajima, Kunihisa

Mass Spectrometry (Internet), 5(2), p.S0055_1 - S0055_6, 2016/12

https://doi.org/10.5702/massspectrometry.S0055

Though equilibrium vapor pressures are utilized to determine thermodynamic properties of not only gaseous species but also condensed phases, the obtained data often disagree by a factor of 100 and more. A new data analysis method is proposed using the so-called second and third law procedures to improve accuracy of vapor pressure measurements. It was found from examination of vapor pressures of cesium metaborate and silver that the analysis of the difference between the second and third law values can result in determination of an optimal data set. Since the new thermodynamic method does not require special techniques and or experiences in dealing with measured data, it is reliable and versatile to improve the accuracy of vapor pressure evaluation.