State Key Lab of Biogeology and Environmental Geology, China University of Geosciences, 388 Lumo Road, Wuhan, Hubei 430074, PR China.
Water Res. 2014 Jan 1;48:326-34. doi: 10.1016/j.watres.2013.09.043. Epub 2013 Oct 6.
Pd-catalytic process is effective for reducing a wide range of contaminants in groundwater. However, limited attention is paid to Cr(VI) reduction presumably due to the weakly oxidizing potential of Cr(VI) under circumneutral conditions. In this study, a new concept of in situ reducing Cr(VI) in groundwater by a hybrid electro-Pd process with automatic pH adjustments is proposed and justified. In an undivided electrolytic cell, Cr(VI) at 5 mg/L is reduced by 95% within 30 min under conditions of pH 3, 1 g/L Pd/Al2O3 and 20 mA current. Reduction of Cr(VI) increases with decreasing pH and increasing current and Pd/Al2O3 dosage. Inhibition of anodic O2 is significant but decreases with drop of pH. Atomic H is assigned as the predominant reactive species contributing to Cr(VI) reduction. Although H2O2 is effective for reducing Cr(VI), its production on Pd surface is completed inhibited by the presence of Cr(VI). The concept is ultimately justified using a specially configured three-electrode column. Cr(VI) is effectively reduced to Cr(3+) in the locally acidic Pd zone, and Cr(3+) is then precipitated in the downstream neutral zone. This hybrid electro-Pd process could be potentially applied in the in situ remediation of Cr(VI)-contaminated groundwater.
钯催化工艺可有效去除地下水中的多种污染物。然而,由于中性条件下六价铬(Cr(VI))的氧化还原电位较弱,Cr(VI)的还原问题并未得到太多关注。本研究提出并论证了一种新型原位还原地下水中 Cr(VI)的电-Pd 混合工艺,该工艺具有自动 pH 调节功能。在非分隔电解槽中,在 pH 值为 3、1 g/L Pd/Al2O3 和 20 mA 电流的条件下,Cr(VI)(浓度为 5 mg/L)可在 30 min 内被还原 95%。还原反应随 pH 值降低、电流和 Pd/Al2O3 用量增加而增强。阳极 O2 的抑制作用显著,但随 pH 值降低而减弱。原子 H 被认为是主要的活性物质,有助于 Cr(VI)的还原。尽管 H2O2 可有效还原 Cr(VI),但 Cr(VI)的存在完全抑制了其在 Pd 表面的生成。通过专门设计的三电极柱验证了该概念。Cr(VI)可在局部酸性的 Pd 区被有效还原为 Cr(3+),随后在下游中性区沉淀。该电-Pd 混合工艺有望应用于原位修复 Cr(VI)污染地下水。