Jeong Hoon Y, Klaue Bjorn, Blum Joel D, Hayes Kim F
Department of Civil and Environmental Engineering, University of Michigan, Ann Arbor, Michigan 48109, USA.
Environ Sci Technol. 2007 Nov 15;41(22):7699-705. doi: 10.1021/es070289l.
Iron sulfides are known to be efficient scavengers of heavy metals. In this study, Hg(II) sorption was investigated using synthetic nanocrystalline mackinawite (a disordered phase) as a function of initial Hg(II) concentration [Hg(II)]0, initial FeS concentration [FeS]0, total chloride concentration CIT, and pH. Hg(II) sorption mechanisms are dependent on relative concentrations of [Hg(II)]0 and [FeS]0 (the molar ratio of [Hg(II)0/[FeS]0). When the molar ratio of [Hg(II)]0/[FeS]o is as low as 0.05, adsorption is mainly responsible for Hg(II) removal, with its contribution to the overall sorption increasing at lower Cl(T). As the molar ratio increases, the adsorption capacity becomes saturated, resulting in precipitation of a sparingly soluble HgS(s). XRD analysis indicates formation of metacinnabar (beta-HgS). Concurrently with HgS(s) precipitation, the released Fe(II) from FeS(s) is resorbed by adsorption at acidic pH and either adsorption or precipitation as Fe (hydr)-oxides at neutral to basic pH. Subsequently, the Fe precipitate formed at neutral to basic pH serves as an adsorbent for Hg(II). Under the conditions where either adsorption or HgS(s) precipitation is dominant, more than 99% of [Hg(II)]0 is immobilized. When the molar ratio of [Hg(II)]0/[FeS]0 exceeds 1, the sulfide concentration is no longer sufficient for HgS(s) precipitation, and formation of chloride salts (Hg2Cl2 at acidic pH and HgCl2 x 3HgO at basic pH) occurs.
已知硫化铁是重金属的有效清除剂。在本研究中,以合成纳米晶马基诺矿(一种无序相)为吸附剂,研究了汞(II)的吸附情况,考察了初始汞(II)浓度[Hg(II)]₀、初始硫化铁浓度[FeS]₀、总氯浓度CIT和pH的影响。汞(II)的吸附机制取决于[Hg(II)]₀和[FeS]₀的相对浓度([Hg(II)]₀/[FeS]₀的摩尔比)。当[Hg(II)]₀/[FeS]₀的摩尔比低至0.05时,吸附是汞(II)去除的主要机制,在较低的Cl(T)条件下,其对总吸附的贡献增加。随着摩尔比的增加,吸附容量达到饱和,导致难溶性硫化汞(HgS(s))沉淀。XRD分析表明形成了黑辰砂(β-HgS)。在HgS(s)沉淀的同时,FeS(s)释放出的Fe(II)在酸性pH下通过吸附重新被吸收,在中性至碱性pH下则通过吸附或沉淀形成铁的氢氧化物。随后,在中性至碱性pH下形成的铁沉淀物作为汞(II)的吸附剂。在吸附或HgS(s)沉淀占主导的条件下,超过99%的[Hg(II)]₀被固定。当[Hg(II)]₀/[FeS]₀的摩尔比超过1时,硫化物浓度不再足以形成HgS(s)沉淀,而是会形成氯盐(酸性pH下为Hg₂Cl₂,碱性pH下为HgCl₂·3HgO)。