Abstract
One critical challenge of the development of seawater uranium extraction is to make uranium adsorbents perform well in the complex real seawater matrix, which is comprised of many competing ions and natural organic substances. Here, we conducted a systematic study using a continuous-flow seawater flume system to assess the potential impacts of dissolved organic matter (DOM) and dissolved iron on the uranium uptake performance, including adsorbent reusability, of amidoxime-based adsorbents. In the 28-day exposure, the adsorbent exposed in dissolved Fe-spiked seawater (low DOM/high Fe) and humic acid-spiked seawater (high DOM/high Fe) showed lower uranium adsorption loadings (73% and 56% of adsorption loading, respectively) than the same adsorbent exposed in seawater without spiking (low DOM/low Fe). The uranium adsorption loading of the reused adsorbent (after uranium stripping by a mild bicarbonate elution) in the dissolved Fe-spiked seawater dropped substantially to only 24% of the loading in the unspiked clean seawater counterpart, while not much change was observed in the performance of the adsorbent exposed to the humic acid-spiked seawater. Fourier transform infrared signatures of adsorbents suggest that the amidoxime ligands in the adsorbent exposed to dissolved Fe-spiked seawater had more severe degradation than the adsorbents exposed to humic acid-spiked seawater and unspiked clean seawater. Unlike the adsorbent exposed to dissolved Fe-spiked seawater, the adsorbent exposed to humic acid-spiked seawater did not adsorb an elevated level of Fe compared to the adsorbent in the unspiked clean seawater. This suggests that the species of Fe in the humic acid-spiked seawater (primarily humic acid bound Fe) did not interact with the amidoxime-based adsorbent, while the Fe species in the Fe-spiked seawater strongly interacted with the adsorbent and caused significant degradation of amidoxime ligands. On the other hand, highly variable uranium adsorption loadings were observed in the adsorbent in contact with humic acid-spiked seawater, but not in the adsorbents exposed to dissolved Fe-spiked seawater and seawater without spiking. Our observations indicate that seawater receiving high inputs of DOM and dissolved Fe, such as coastal waters, is not ideal for efficient extraction of uranium.
