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Management of carbon dioxide released from spent nuclear fuel through voloxidation

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Abstract

The management of radioactive carbon (C-14) from spent nuclear fuel (SNF) in a voloxidation process is vital to prevent radioactive contamination of the environment. Thus, a double alkali method was applied to absorb the gaseous phase of C-14 (CO2) and to immobilize radioactive carbon into a stable structure. Based on the two-film theory, mass transfer and enhancement factor were evaluated for CO2 absorption in NaOH solution with regards to the effects of operating conditions such as the solution concentration, CO2 partial pressure, and gas flow rate on the absorbing performance. The absorption tests were carried out targeting the successful capture of CO2 released from SNF with a high decontamination factors (DF) more than 103. Causticization with Ca(OH)2 leads to the immobilization of absorbed carbon into a scalenohedral calcite (CaCO3) crystal, and its stable and nonporous characteristics suggested that calcite is a suitable structure for preparing waste forms stored in a geological repository.

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Abbreviations

E :

Enhancement factor

G :

Molar flow rate

\(g\) :

Gravitational acceleration

\(H\), \({H}_{w}\) :

Henry’s law constant for CO2 in NaOH solution and pure water, respectively

Ha :

Hatta number

\(I\) :

Ionic strength

\(P\) :

Operating pressure

\(Re\) :

Reynolds number

\(Sc\) :

Schmidt number

\(Sh\) :

Sherwood number

\(T\) :

Temperature

\({a}_{e}\) :

Effective interfacial area

\({c}_{i}\) :

Concentration for individual ions in the solution

\({D}_{{CO}_{2}}\), \({D}_{w}\) :

Diffusivity of CO2 in NaOH solution and pure water, respectively

\({D}_{OH}\) :

Diffusivity of OH– ion in the solution

\({d}_{0}\) :

Diameter of the orifice in the gas distributor

\({d}_{s}\) :

Sauter-mean diameter

E i :

Enhancement factor for instantaneous reaction

\({k}_{G}\) :

Mass transfer coefficient for the gas phase

\({k}_{L}\) :

Mass transfer coefficient for the liquid phase

\({K}_{G}{a}_{e}\) :

Gas-phase overall mass transfer coefficient

\({k}_{OH}\) :

Reaction rate constant

\({k}_{OH}^{\infty }\) :

Reaction rate constant at an infinitely diluted solution

\({m}_{{CO}_{2}, in}\), \({m}_{{CO}_{2}, out}\) :

CO2 mass at the inlet and outlet, respectively

\({N}_{{CO}_{2}}\) :

Overall CO2 absorption rate

\({P}_{{CO}_{2}}\) :

CO2 partial pressure in the feed gas

\({P}_{{CO}_{2}}^{*}\) :

CO2 partial pressure at equilibrium with the CO2 concentration in the liquid phase

\({U}_{G}\) :

Superficial gas velocity

\({V}_{b}\) :

Volume of the solution

\({z}_{i}\) :

Charge for individual ions in the solution

\({\epsilon }_{b}\) :

Gas hold-up

\({\mu }_{w}\), \({\mu }_{L}\) :

Viscosities of water and NaOH solution, respectively

\({\Delta }\rho\) :

Density difference between the gas and liquid

\(\sigma\) :

Surface tension

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Funding

This work was supported by the Korea Institute of Energy Technology Evaluation and Planning (KETEP) grant funded by the Korean government (MOTIE) (20201520300140, Development of Advanced Functional Material with C-14 from PHWR Waste).

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Authors and Affiliations

  1. Fuel Cycle Process Division, Korea Atomic Energy Research Institute, 111 Daedeok-daero 989 beon-gil, Yuseong-gu, 34057, Daejeon, Republic of Korea

    Seok-Min Hong, Hong Jang, Siwan Noh, Hyun Woo Kang & Yung-Zun Cho

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  1. Seok-Min Hong
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Correspondence to Seok-Min Hong.

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Hong, SM., Jang, H., Noh, S. et al. Management of carbon dioxide released from spent nuclear fuel through voloxidation. J Radioanal Nucl Chem 330, 695–705 (2021). https://doi.org/10.1007/s10967-021-07972-w

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