Production of H{sub 2} by water radiolysis in cement paste under electron irradiation: A joint experimental and theoretical study
Long-term confinement of nuclear waste is one of the main challenges faced by the nuclear industry. Fission products such as {sup 90}Sr and {sup 137}Cs, both β{sup −} emitters known to induce serious health hazards, represent the largest fraction of nuclear waste. Cement is a good candidate to store them, provided it can resist the effects of irradiation over time. Here, we have investigated the effects of β{sup −} decay on cement by performing electron irradiation experiments on different samples. We show that H{sub 2} production in cement, the main effect of water radiolysis, depends strongly on composition and relative humidity. First-principles calculations indicate that the water-rich interlayer regions with Ca{sup 2+} ions act as electron traps that promote the formation of H{sub 2}. They also show that holes localize in water-rich regions in low Ca content samples and are then able to participate in H{sub 2} production. This work provides new understanding of radiolysis effects in cements. - Graphical abstract: H{sub 2} produced by radiolysis in cement paste is investigated by experimental and computational studies.