Solution and Microbial Controls on the Formation of Reduced U(IV) Species

被引:112
作者
Boyanov, Maxim I. [1 ]
Fletcher, Kelly E. [2 ]
Kwon, Man Jae [1 ]
Rui, Xue [3 ]
O'Loughlin, Edward J. [1 ]
Loeffler, Frank E. [4 ,5 ,6 ]
Kemner, Kenneth M. [1 ]
机构
[1] Argonne Natl Lab, Biosci Div, Argonne, IL 60439 USA
[2] Georgia Inst Technol, Sch Civil & Environm Engn, Atlanta, GA 30332 USA
[3] Univ Notre Dame, Dept Phys, Notre Dame, IN 46545 USA
[4] Univ Tennessee, Dept Microbiol, Knoxville, TN 37996 USA
[5] Univ Tennessee, Dept Civil & Environm Engn, Knoxville, TN 37996 USA
[6] Oak Ridge Natl Lab, Biosci Div, Oak Ridge, TN 37831 USA
关键词
U(VI) REDUCTION; URANINITE NANOPARTICLES; CONTAMINATED SUBSURFACE; URANIUM(VI) PHOSPHATE; ELECTRON-TRANSFER; BIOREDUCTION; ADSORPTION; SEDIMENTS; UO2; BIOMINERALIZATION;
D O I
10.1021/es2014049
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Reduction of U(VI) to U(IV) as the result of direct or indirect microbial activity is currently being explored for in situ remediation of subsurface U plumes, under the assumption that U(IV) solubility is controlled by the low-solubility mineral uraninite (U(IV)-dioxide). However, recent characterizations of U in sediments from biostimulated field sites, as well as laboratory U(VI) bioreduction studies, report on the formation of U(IV) species that lack the U=O(2)=U coordination of uraninite, suggesting that phases other than uraninite may be controlling U(IV) solubility in environments with complexing surfaces and ligands. To determine the controls on the formation of such nonuraninite U(IV) species, the current work studied the reduction of carbonate-complexed U(VI) by (1) five Gram-positive Desulfitobacterium strains, (2) the Gram-negative bacteria Anaeromyxobacter dehalogenans 2CP-C and Shewanella putrefaciens CN32, and (3) chemically reduced 9,10-anthrahydroquinone-2,6-disulfonate (AH(2)QDS, a soluble reductant). Further, the effects of 0.3 mM dissolved phosphate on U(IV) species formation were explored. Extended X-ray absorption fine structure (EXAFS) spectroscopy analysis demonstrated that the addition of phosphate causes the formation of a nonuraninite, phosphate-complexed U(IV) species, independent of the biological or abiotic mode of U(VI) reduction. In phosphate-free medium, U(VI) reduction by Desulfitobacterium spp. and by AH(2)QDS resulted in nonuraninite, carbonate-complexed U(IV) species, whereas reduction by Anaeromyxobacter or Shewanella yielded nanoparticulate uraninite. These findings suggest that the Gram-positive Desulfitobacterium strains and the Gram-negative Anaeromyxobacter and Shewanella species use distinct mechanisms to reduce U(VI).
引用
收藏
页码:8336 / 8344
页数:9
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