Evaluation of 137Cs ageing by dynamics of 137Cs/133Cs ratio in Andosol paddy fields with/without potassium fertilizer application

The mobility of 137Cs in soil decreases with time owing to fixation by micaceous minerals. Such ageing is a critical parameter for estimating and predicting annual change in 137Cs contamination risk of agricultural products. The decrease in the exchangeable fraction of 137Cs has traditionally been used as an index of the 137Cs ageing. Under field conditions, however, exchangeable 137Cs is influenced by several environmental factors. In this study, we propose a new index to evaluate the 137Cs ageing with minimum influence of environmental factors. The ratio of the exchangeable 137Cs fraction to exchangeable fraction of 133Cs ((137Cs/133Cs)exch) eliminates the influence of environmental factors on exchangeable 137Cs. We assessed the applicability of the (137Cs/133Cs)exch index, using a four-year field study of a rice paddy in allophanic Andosol, starting 200 days after the Fukushima Dai-ichi Nuclear Power Plant accident. The influence of K fertilization was also investigated. The 137Cs and 133Cs exchangeable fractions varied together, indicating that both were similarly controlled by environmental factors. The values of (137Cs/133Cs)exch decreased with time, reflecting 137Cs fixation by the ageing. The half-time of the (137Cs/133Cs)exch decline was 6.6–17.7 years. Relative to K fertilization, the lack of K fertilization seemed to affect the 137Cs ageing in two ways: the early 137Cs fixation progressed more rapidly, probably because fewer competing K+ ions were present, and the long-term ageing process was occasionally hampered, probably by the release of reserve K from micaceous minerals. The (137Cs/133Cs)exch values were similar to the ratio of the 137Cs to 133Cs transfer factor of the rice straw. Thus, we conclude that the (137Cs/133Cs)exch index is reliable for evaluating the 137Cs ageing, decrease in 137Cs mobility caused by the diffusion into micaceous mineral interlayer, in the field. •Exchangeable 137Cs and 133Cs in Andosol of rice paddy was monitored.•Exchangeable 137Cs and 133Cs varied together under control of environmental factors.•Ratio of 137Cs/133Cs in the exchangeable fraction declined, reflecting 137Cs ageing.•The half-time of 137Cs/133Cs decline was 6.6–17.7 years.•Early 137Cs fixation was enhanced in the absence of K fertilizer application.