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FeS 的 pH 敏感氧化:Cr(VI)的矿物转化和固定。

The pH-sensitve oxygenation of FeS: Mineral transformation and immobilization of Cr(VI).

机构信息

State Key Laboratory of Coal Mine Disaster Dynamics and Control, Chongqing University, Chongqing 400044, China; Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment of Ministry of Education, Chongqing University, Chongqing 400044, China.

State Key Laboratory of Coal Mine Disaster Dynamics and Control, Chongqing University, Chongqing 400044, China; Key Laboratory of the Three Gorges Reservoir Region's Eco-Environment of Ministry of Education, Chongqing University, Chongqing 400044, China.

出版信息

Water Res. 2023 Apr 15;233:119722. doi: 10.1016/j.watres.2023.119722. Epub 2023 Feb 8.

Abstract

Iron sulfide (FeS) has been widely used to reduce toxic Cr(VI) into Cr(III) in anoxic aquatic environments, where pH could strongly influence Cr(VI) removal. However, it remains unclear how pH regulates the fate and transformation of FeS under oxic conditions and the immobilization of Cr(VI). The results of this study showed that typical pH conditions of natural aquatic environment significantly affected the mineral transformation of FeS. Under acidic conditions, FeS was principally transformed to goethite, amarantite, and elemental sulfur with minor lepidocrocite through proton-promoted dissolution and oxidation. Instead, under basic conditions, the main products were lepidocrocite and elemental sulfur via surface-mediated oxidation. In typical acidic or basic aquatic environment, the pronounced pathway for the oxygenation of FeS solids may alter their ability to remove Cr(VI). Longer oxygenation impeded Cr(VI) removal at acidic pH, and a decreasing ability to reduce Cr(VI) caused a drop in Cr(VI) removal performance. Cr(VI) removal decreased from 733.16 to 36.82 mg g with the duration of FeS oxygenation increasing to 5760 min at pH 5.0. In contrast, newly generated pyrite from brief oxygenation of FeS improved Cr(VI) reduction at basic pH, followed by a drop in Cr(VI) removal performance due to the impaired reduction capacity with increasing to the complete oxygenation. Cr(VI) removal increased from 669.58 to 804.83 mg g with increasing oxygenation time to 5 min and then decreased to 26.27 mg g after the full oxygenation for 5760 min at pH 9.0. These findings provide insight into the dynamic transformation of FeS in oxic aquatic environments with various pHs and the impact on Cr(VI) immobilization.

摘要

硫化亚铁 (FeS) 已广泛用于在缺氧水生环境中将有毒的六价铬 (Cr(VI)) 还原为三价铬 (Cr(III)),其中 pH 值会强烈影响 Cr(VI) 的去除。然而,在有氧条件下,pH 值如何调节 FeS 的命运和转化以及 Cr(VI) 的固定仍不清楚。本研究结果表明,天然水生环境的典型 pH 值条件显著影响 FeS 的矿物转化。在酸性条件下,FeS 主要通过质子促进的溶解和氧化转化为针铁矿、水铁矾和少量纤铁矿。相比之下,在碱性条件下,主要产物是通过表面介导氧化生成的纤铁矿和元素硫。在典型的酸性或碱性水生环境中,FeS 固体的氧化明显改变了它们去除 Cr(VI) 的能力。较长时间的氧化会阻碍酸性 pH 值下 Cr(VI)的去除,降低还原 Cr(VI)的能力会导致 Cr(VI)去除性能下降。在 pH 5.0 时,随着 FeS 氧化时间延长至 5760 min,Cr(VI)的去除率从 733.16 降至 36.82 mg g。相比之下,在碱性 pH 值下,FeS 短暂氧化生成的新黄铁矿提高了 Cr(VI)的还原,随后由于还原能力随着完全氧化的增加而下降,Cr(VI)的去除性能下降。在 pH 9.0 时,随着氧化时间从 5 分钟增加到 5760 分钟,Cr(VI)的去除率从 669.58 增加到 804.83 mg g,然后在完全氧化 5760 分钟后降至 26.27 mg g。这些发现为不同 pH 值下有氧水生环境中 FeS 的动态转化及其对 Cr(VI)固定的影响提供了深入了解。

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