Smithsonian Environmental Research Center, 647 Contees Wharf Rd, Edgewater, MD 21037, USA.
Environ Sci Process Impacts. 2019 Mar 20;21(3):485-496. doi: 10.1039/c8em00469b.
Activated carbon (AC) amendments have shown promise in reducing inorganic mercury (Hg(ii) complexes, "Hg") and methylmercury (MeHg) risk in contaminated soils. However, the effectiveness of AC in Hg and MeHg immobilization has varied among studies, suggesting that site biogeochemistry might dictate efficacy. In this study, we examined the effect of dissolved organic matter (DOM) on MeHg and Hg sorption to AC. We evaluated the impact of Suwannee River Humic Acid (SRHA) on sorption to AC directly using an isotherm approach and in a soil/AC mixture using slurry microcosms. Aqueous sorption coefficients to AC (log KAC) for Hg-SRHA and MeHg-SRHA complexes were one to two orders of magnitude lower (Hg-SRHA = 4.53, MeHgSRHA = 4.35) than those for chloride complexes (HgCl2 = 6.55, MeHgCl = 4.90) and more closely resembled the log KAC of SRHA (3.64). In anoxic, sulfidic soil slurries, the KAC for sulfide species appeared stronger than for chloride or SRHA species for both Hg and MeHg. AC significantly reduced porewater concentrations of both ambient MeHg and a fresh Me199Hg spike, and the addition of up to 60 mg L-1 SRHA did not reduce sorption to AC. The AC also reduced ambient Hg and 201Hg porewater concentrations, but as SRHA concentration increased, the magnitude of solid phase sorption decreased. Speciation modeling revealed that SRHA may have impacted Hg distribution to the solid phase by reducing HgS precipitation. This study highlights the need for site-specific evaluation of AC efficacy and the value in developing biogeochemical models of AC performance for Hg control.
活性炭(AC)改良剂已被证明可有效降低污染土壤中的无机汞(Hg(ii)复合物,“Hg”)和甲基汞(MeHg)风险。然而,AC 对 Hg 和 MeHg 固定的有效性在不同研究中存在差异,这表明场地生物地球化学可能会影响其效果。在这项研究中,我们研究了溶解有机质(DOM)对 AC 吸附 MeHg 和 Hg 的影响。我们直接通过等温线方法以及在土壤/AC 混合物中使用泥浆微宇宙评估了苏万尼河腐殖酸(SRHA)对 AC 吸附的影响。Hg-SRHA 和 MeHg-SRHA 络合物与 AC 的水相吸附系数(logKAC)比氯化物络合物(HgCl2 = 6.55,MeHgCl = 4.90)低一到两个数量级(Hg-SRHA = 4.53,MeHgSRHA = 4.35),更接近 SRHA 的 logKAC(3.64)。在缺氧、含硫的土壤泥浆中,对于 Hg 和 MeHg,硫化物的 KAC 似乎比氯化物或 SRHA 更强。AC 显著降低了环境 MeHg 和新添加的 Me199Hg 脉冲的孔隙水浓度,添加高达 60mg L-1 的 SRHA 并没有降低 AC 的吸附能力。AC 还降低了环境 Hg 和 201Hg 孔隙水浓度,但随着 SRHA 浓度的增加,固相吸附的幅度减小。形态建模表明,SRHA 可能通过减少 HgS 沉淀来影响 Hg 在固相中分布。本研究强调了需要对 AC 功效进行特定场地评估,并开发用于 Hg 控制的 AC 性能生物地球化学模型的价值。