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Report No.
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Heat treatment of phosphate-modified cementitious matrices for safe storage of secondary radioactive aqueous wastes in Fukushima Daiichi Nuclear Power Plant

Irisawa, Keita; Taniguchi, Takumi; Namiki, Masahiro; Garc$'i$a-Lodeiro, I.*; Osugi, Takeshi; Sakakibara, Tetsuro; Nakazawa, Osamu; Meguro, Yoshihiro; Kinoshita, Hajime*

A solidification technique with minimized water content is being developed using phosphate cements for the safe storage of secondary radioactive wastes in the Fukushima Daiichi Nuclear Power Plant. Conventional cement systems become solidified via hydration reactions, and need a certain water content. Phosphate cement systems, however, become solidified via an acid-base reaction, and so they only require water mainly for reasons of workability. A reduced water content of phosphate cement systems is beneficial for the immobilization of the radioactive wastes from mitigating the potential to generate hydrogen gas by the radiolysis of water by radioactive wastes. The current study investigated the water content and mineralogy of calcium aluminate cement (CAC) and phosphate-modified CAC (CAP) cured in open systems at 60, 90 and 120 $$^{circ}$$C and in a closed system at 20 $$^{circ}$$C as a reference case. Water contents in both the CAC and the CAP were seen to decrease as curing progressed. For $$geq$$ 90 $$^{circ}$$C, the CAP contained less water than CAC. Free water in CAC converted to structural water by heat treatment, but this was not the case for CAP. An orthophosphate hydrate salt, a precursor phase of hydroxyapatite, was found in CAP when cured at 20 and 60 $$^{circ}$$C, and a mixture of the orthophosphate hydrate salt and hydroxyapatite, Ca$$_{10}$$(PO$$_{4}$$)$$_{6}$$(OH)$$_{2}$$, were formed in the CAP when cured at 90 $$^{circ}$$C. Phosphate products in CAP cured at 120 $$^{circ}$$C appears to consist of a different phosphate phase compared with the CAP cured at 20, 60 and 90 $$^{circ}$$C.

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