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Year-round variations in the fluvial transport load of particulate 137Cs in a forested catchment affected by the Fukushima Daiichi Nuclear Power Plant accident

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Abstract

Particulate 137Cs was collected from stream water for 2 years to assess the long-term trend of 137Cs discharge from a forest after the Fukushima Nuclear Power Plant accident. A seasonal increase in the fluvial transport load of particulate 137Cs in suspended solids (SS) was observed in July–October when rainfall was abundant. The 137Cs load was controlled by the SS load. This control was attributed to cesium affinity for phyllosilicate clay minerals as verified by the low extractability of particulate 137Cs. These findings indicate the fluvial particulate 137Cs load is significantly related to the climate and geomorphological features of Japan.

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Acknowledgments

The authors express their sincere thanks to Masahiro Hirasawa, Makiko Ishihara, and Kazumi Matsumura for their assistance with extensive laboratory work. The permission to use the preserved forest from the forestry management authorities in Ibaraki Prefecture and the Forestry Agency of Japan is gratefully acknowledged. The use of the weir was kindly permitted by the Forestry and Forest Products Research Institute. We are also grateful to a landowner for their permission to use an open plot for a precipitation gauge. Aya Sakaguchi inspired T.M. to interpret regional features of the Japanese environmental conditions.

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Appendices

Appendix 1: Equations for the mass transport load of suspended solids

In the reality in the field condition, a continuous monitoring of SS concentration is not possible. In this study, the correction factor (see the section of Correction for SS transport load in Discussion) was estimated using a value for turbidity as, a surrogate for the SS concentration with an assumption of a linear relation between the turbidity and SS concentration.

The SS load was evaluated in the following manner for each sampling period. In the following, the notation i (1, 2, 3, or 4) denotes the size fraction of F1, F2, F3 or F4. First, a nominal SS load from a time-integral collection was evaluated (Step 1). Next, a correction factor for the underestimation associated with the time-integrated method was elucidated using the turbidity record (Step 2). Finally, the probable load expected from flow-weighted collection was evaluated (Step 3). Values of the correction factor are listed in Table 2.

Table 2 Correction factors for the estimated SS load by a time-integral SS collection

Irregular turbidity records such as very high values under normal flow conditions were replaced with calculated values by a relationship between the flow rate and the turbidity (Fig. 8, Table 3): T = 1941 Q − 25, where T is the turbidity, Q is the flow rate (m3 s−1), and r = 0.60. For instances of extremely low flow rates, this calculation yields negative values because the regression line has a negative y-intercept. Because a negative turbidity value is not logical, these negative values were artificially converted to 1 (turbidity) as the minimum probable value. The influence of this adjustment is limited because this occurred only at a low flow rate. When the calculation produced a T value larger than 990, which is the upper limit of the used turbidity sensor, T was artificially converted to 990 because the regression line is valid within the dynamic range of the sensor.

Fig. 8
figure 8

Regression of turbidity for the stream water flow rate during selected rainfall events. The selected rainfall events are listed in Table 3

  1. (1)

    Step 1

    $$ W = w_{ 1} + w_{ 2} + w_{ 3} + w_{ 4} $$
    (1)
    $$ f_{\text{i}} = \, \left( {w_{\text{i}} /W} \right) \, \times { 1}00 $$
    (2)
    $$ ml_{\text{SS}} ,_{i} = W \times \, 0.00 1 { } \times (Q/q) \, \times f_{i} \times \, 0.0 1/D $$
    (3)
    $$ {\text{NML}}_{\text{SS}} = {\text{ ml}}_{\text{SS}} ,_{ 1} + {\text{ ml}}_{\text{SS}} ,_{ 2} + {\text{ ml}}_{\text{SS}} ,_{ 3} + {\text{ ml}}_{\text{SS}} ,_{ 4} $$
    (4)

    where W is the total weight of collected SS in the period (g), w i is the weight of collected SS of size fraction i in the period (g), f i is the fractional percent of w i by size fraction (%), ml SS, i is the mass transport load of SS for size i (kg days−1), q is the cumulative volume of water passing through the filtration system in the period (m3), Q is the cumulative river water discharge over the period (m3), D is the duration of the period (days) and NMLSS is the nominal total mass transport load of SS (kg days−1).

  2. (2)

    Step 2

    $$ {\text{CF}} = \mathop \sum \limits_{1}^{N} Q_{i} T_{i} /\mathop \sum \limits_{1}^{N} Q_{i} \mathop \sum \limits_{1}^{N} T_{i} $$
    (5)

    where CF is the correction factor (–), Q i is the stream water flow rate at time i (m3 s−1), T i is the turbidity at time i (NTU), i is the recording time of water flow and turbidity at every 15 min, i = 1, N and N is the the end point of the recording of the run.

  3. (3)

    Step 3

    $$ {\text{ML}}_{\text{SS}} = {\text{NML}}_{\text{SS}} /{\text{CF}} $$
    (6)

    where ML SS is the total mass transport load of SS expected in flow-weighted collection (kg days−1).

Appendix 2: Equations for radioactivity transport load of 137Cs

Similarly, the radioactivity transport load was evaluated based on the following calculation. In the present context, the radioactivity refers to that of 137Cs (Table 3).

$$ a_{i} = c_{i} w_{i} $$
(7)
$$ A = a_{ 1} + a_{ 2} + a_{ 3} + a_{ 4} $$
(8)
$$ af_{\text{i}} = \, \left( {a_{\text{i}} /A} \right)\; \times \; 100 $$
(9)
$$ al_{\text{SS}} ,_{\text{i}} = A \times (Q/q) \, \times af_{\text{i}} \times \, 0.0 1/D $$
(10)
$$ {\text{AL}}_{\text{SS}} = al_{\text{SS}} ,_{ 1} + al_{\text{SS}} ,_{ 2} + al_{\text{SS}} ,_{ 3} + al_{\text{SS}} ,_{ 4} $$
(11)

where a i is the amount of radioactivity in SS of size fraction i (Bq), c i is the radioactivity concentration in SS of size fraction i (Bq g−1), A is the total amount of radioactivity in SS (Bq), af i is the fractional percent of a i by size fraction (%), al SS, i is the radioactivity transport load with SS for size i (Bq days−1) and AL SS is the total radioactivity transport load with SS (Bq dats−1).

Table 3 Selected rainfall events for elucidation of a turbidity-flow rate relationship

Appendix 3: Comparison of radioactivity concentrations of 137Cs and 134Cs

When the two radiocesium concentrations isotopes were decay corrected to the date of the Great East Japan Earthquake (March 11, 2011, a day close to the nuclear accident) (see Table S3 of Supplementary information for used decay correction factors), the 134Cs to 137Cs ratios were all approximately 1.0 (Supplementary Information, Fig. S1). This value matches the reported value of 0.91 as of June 11, 2011, found in a large-scale soil sampling study [7]. Thus, the isotopic composition confirmed that the 137Cs measured in this study originated from the Fukushima Daiichi NPP accident.

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Matsunaga, T., Nakanishi, T., Atarashi-Andoh, M. et al. Year-round variations in the fluvial transport load of particulate 137Cs in a forested catchment affected by the Fukushima Daiichi Nuclear Power Plant accident. J Radioanal Nucl Chem 310, 679–693 (2016). https://doi.org/10.1007/s10967-016-4840-3

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