| Algae reduce and methylate arsenate, producing arsenite (As(III)) when the growth rates are high and dimethylarsinic acid (DMA) when the growth rates are low. In lakes, this leads to high As(III) concentrations in the early stages of spring and fall blooms and high DMA concentrations in the summer. I hypothesize that under phosphorus (P)-limited conditions, which usually exist in the summer, algae take up phosphate (PO4) and, because of similar chemical characteristics, As(V) as well. Inside the cell, As(V) is reduced to As(III), methylated to monomethylarsonic acid (MMA) and DMA, and then excreted. However, under non-P-limited conditions, which exist in the early stages of blooms, algae up-regulate their PO4 transport system to take up excess P, a phenomenon known as luxury uptake. Since As(V) is taken up by the PO4 transport system, As(V) uptake also increases at this time. Within the cell, the reduction of As(V) to As(III) is fast, but methylation is slower, causing As(III) to build up in the cell and be excreted, which, in turn, causes an increase in extracellular As(III). This mechanism permits the synergistic (luxury uptake) and antagonistic (competition) effects of PO4 on As(V) uptake and can therefore explain the seemingly contradictory results found in the literature. A mathematical model is constructed on the basis of existing established algal-nutrient interaction models and is used to simulate as transformation in two laboratory batch experiments. In addition to algal and P responses, the model can reasonably well reproduce the observed As(III) peak during the log growth phase and the more gradual appearance of DMA during the stationary phase. To further test the proposed mechanism, the process model is integrated into a full ecological model and applied to Lake Biwa, Japan. The model application allows for a quantitative analysis of the field data, consistent with the ecological dynamics of the lake. The newly developed ecological model includes a variable phytoplankton composition, which is needed to simulate luxury uptake. This is in contrast to most existing ecological models, which typically assume a fixed “Redfield” composition. The model adequately reproduces the observed ecology in Lake Biwa including the rapid uptake of phosphate by phytoplankton without immediate growth (luxury uptake) following lake overturn. The model also reproduces the observed arsenic speciation, including the gradual appearance of DMA during the summer and peaks in As(III) concentration at the onset of spring and fall algal blooms. |
