Boukhalfa Hakim, Icopini Gary A, Reilly Sean D, Neu Mary P
Chemistry Division, Los Alamos National Laboratory, Los Alamos, NM 87545, USA.
Appl Environ Microbiol. 2007 Sep;73(18):5897-903. doi: 10.1128/AEM.00747-07. Epub 2007 Jul 20.
The bacterial reduction of actinides has been suggested as a possible remedial strategy for actinide-contaminated environments, and the bacterial reduction of Pu(VI/V) has the potential to produce highly insoluble Pu(IV) solid phases. However, the behavior of plutonium with regard to bacterial reduction is more complex than for other actinides because it is possible for Pu(IV) to be further reduced to Pu(III), which is relatively more soluble than Pu(IV). This work investigates the ability of the metal-reducing bacteria Geobacter metallireducens GS15 and Shewanella oneidensis MR1 to enzymatically reduce freshly precipitated amorphous Pu(IV) (OH)(4) [Pu(IV)(OH)(4(am))] and soluble Pu(IV)(EDTA). In cell suspensions without added complexing ligands, minor Pu(III) production was observed in cultures containing S. oneidensis, but little or no Pu(III) production was observed in cultures containing G. metallireducens. In the presence of EDTA, most of the Pu(IV)(OH)(4(am)) present was reduced to Pu(III) and remained soluble in cell suspensions of both S. oneidensis and G. metallireducens. When soluble Pu(IV)(EDTA) was provided as the terminal electron acceptor, cell suspensions of both S. oneidensis and G. metallireducens rapidly reduced Pu(IV)(EDTA) to Pu(III)(EDTA) with nearly complete reduction within 20 to 40 min, depending on the initial concentration. Neither bacterium was able to use Pu(IV) (in any of the forms used) as a terminal electron acceptor to support growth. These results have significant implications for the potential remediation of plutonium and suggest that strongly reducing environments where complexing ligands are present may produce soluble forms of reduced Pu species.
细菌对锕系元素的还原作用被认为是一种治理受锕系元素污染环境的可能策略,而细菌对 Pu(VI/V) 的还原作用有可能产生极难溶的 Pu(IV) 固相。然而,钚在细菌还原方面的行为比其他锕系元素更为复杂,因为 Pu(IV) 有可能进一步被还原为 Pu(III),而 Pu(III) 的溶解度相对高于 Pu(IV)。本研究考察了金属还原菌嗜金属地杆菌 GS15 和奥奈达希瓦氏菌 MR1 对新沉淀的无定形 Pu(IV)(OH)(4) [Pu(IV)(OH)(4(am))] 和可溶性 Pu(IV)(EDTA) 进行酶促还原的能力。在未添加络合配体的细胞悬液中,在含有奥奈达希瓦氏菌的培养物中观察到少量 Pu(III) 的生成,但在含有嗜金属地杆菌的培养物中几乎未观察到 Pu(III) 的生成。在 EDTA 存在的情况下,存在的大部分 Pu(IV)(OH)(4(am)) 被还原为 Pu(III),并在奥奈达希瓦氏菌和嗜金属地杆菌的细胞悬液中保持可溶状态。当提供可溶性 Pu(IV)(EDTA) 作为末端电子受体时,奥奈达希瓦氏菌和嗜金属地杆菌的细胞悬液都能迅速将 Pu(IV)(EDTA) 还原为 Pu(III)(EDTA),根据初始浓度,在 20 至 40 分钟内几乎完全还原。两种细菌都不能利用 Pu(IV)(以任何所用形式)作为末端电子受体来支持生长。这些结果对钚的潜在治理具有重要意义,并表明存在络合配体的强还原环境可能会产生还原态钚的可溶形式。