Institute of Resource Ecology, Helmholtz-Zentrum Dresden-Rossendorf e.V., P.O. Box 510119, D-01314, Dresden, Germany.
Dalton Trans. 2013 May 21;42(19):6979-88. doi: 10.1039/c3dt33032j.
Bacterial cell walls have a high density of ionizable functional groups available for U(VI) binding, hence have a great potential to affect the speciation of this contaminant in the environment. The studied strain of the genus Paenibacillus is a novel isolate originating from the Mont Terri Opalinus clay formations (Switzerland) which are currently investigated as a potential host rock for future nuclear waste storage. U(VI) binding to the cell surface functional groups was studied by potentiometry combined with time-resolved laser-induced fluorescence spectroscopy (TRLFS). Four bacterial U(VI) surface complexes were identified: R-COO-UO2(+), R-O-PO3-UO2, R-O-PO3H-UO2(+), and (R-O-PO3)2-UO2(2-). The corresponding complex stability constants were calculated to be 5.33 ± 0.08, 8.89 ± 0.04, 12.92 ± 0.05, and 13.62 ± 0.08, respectively. Hence UO2(2+) displays a moderate to strong interaction with the bacterial surface functional groups. In the acidic pH range (pH 3) UO2(2+) binding onto the cell envelope is governed by coordination to hydrogen phosphoryl sites. Upon increasing the pH an increasing coordination of UO2(2+) to carboxylic and deprotonated phosphoryl sites was found. At a pH greater than 7 uranyl hydroxides dominate the speciation. Additionally the bacteria-mediated release of inorganic phosphate in dependence on [U(VI)] at different pH values was studied to assess the influence of phosphate release on U(VI) mobilization.
细菌细胞壁具有丰富的可离解功能基团,可与 U(VI)结合,因此具有很大的潜力影响环境中这种污染物的形态。所研究的芽孢杆菌属菌株是一种新型分离株,源自蒙泰里奥帕利纳斯黏土地层(瑞士),目前正在作为未来核废料储存的潜在宿主岩石进行研究。通过电位法结合时间分辨激光诱导荧光光谱法(TRLFS)研究了 U(VI)与细胞表面功能基团的结合。鉴定了四种细菌 U(VI)表面配合物:R-COO-UO2(+)、R-O-PO3-UO2、R-O-PO3H-UO2(+) 和 (R-O-PO3)2-UO2(2-)。相应的配合物稳定常数分别计算为 5.33 ± 0.08、8.89 ± 0.04、12.92 ± 0.05 和 13.62 ± 0.08。因此,UO2(2+)与细菌表面功能基团显示出中等至强的相互作用。在酸性 pH 范围(pH 3),UO2(2+)与细胞包膜的结合受与氢磷酸基配位的控制。随着 pH 的增加,发现 UO2(2+)与羧酸和去质子化磷酸基的配位增加。在 pH 大于 7 时,铀酰氢氧化物主导形态。此外,还研究了不同 pH 值下细菌介导的无机磷酸盐释放与 [U(VI)]的关系,以评估磷酸盐释放对 U(VI)迁移的影响。