Kamolpornwijit W, Liang L
Environmental Sciences Division, Oak Ridge National Laboratory, P.O. Box 2008, Oak Ridge, TN 37830-6036, USA.
J Contam Hydrol. 2006 Jan 10;82(3-4):338-56. doi: 10.1016/j.jconhyd.2005.10.009. Epub 2005 Dec 5.
A method for measuring gas entrapment in granular iron (Fe0) was developed and used to estimate the impact of gas production on porosity loss during the treatment of a high NO3- groundwater (up to approximately 10 mM). Over the 400-d study period the trapped gas in laboratory columns was small, with a maximum measured at 1.3% pore volume. Low levels of dissolved H2(g) were measured (up to 0.07+/-0.02 M). Free moving gas bubbles were not observed. Thus, porosity loss, which was determined by tracer tests to be 25-30%, is not accounted for by residual gas trapped in the iron. The removal of aqueous species (i.e., NO3-, Ca, and carbonate alkalinity) indicates that mineral precipitation contributed more significantly to porosity loss than did the trapped gases. Using the stoichiometric reactions between Fe0 and NO3-, an average corrosion rate of 1.7 mmol kg-1 d-1 was derived for the test granular iron. This rate is 10 times greater than Fe0 oxidation by H2O alone, based on H2 gas production. NO3- ion rather than H2O was the major oxidant in the groundwater in the absence of molecular O2. The N-mass balance [e.g., N2g and NH4+ and NO3-] suggests that abiotic reduction of NO3- dominated at the start of Fe0 treatment, whereas N2 production became more important once the microbial activity began. These laboratory results closely predict N2 gas production in a separated large column experiment that was operated for approximately 2 yr in the field, where a maximum of approximately 600 ml d-1 gas volumes was detected, of which 99.5% (v/v) was N2. We conclude that NO3- suppressed the production of H2(g) by competing with water for Fe0 oxidation, especially at the beginning of water treatment when Fe0 is highly reactive. Depends on the groundwater composition, gas venting may be necessary in maintaining PRB performance in the field.
开发了一种测量颗粒铁(Fe0)中气体截留的方法,并用于估计高硝酸盐地下水(高达约10 mM)处理过程中气体产生对孔隙率损失的影响。在400天的研究期内,实验室柱中截留的气体量很少,最大测量值为孔隙体积的1.3%。测量到的溶解H2(g)水平较低(高达0.07±0.02 M)。未观察到自由移动的气泡。因此,通过示踪剂测试确定为25%-30%的孔隙率损失,并非由截留于铁中的残留气体所致。水中物质(即NO3-、Ca和碳酸盐碱度)的去除表明,矿物沉淀对孔隙率损失的贡献比截留气体更为显著。利用Fe0与NO3-之间的化学计量反应,得出测试颗粒铁的平均腐蚀速率为1.7 mmol kg-1 d-1。基于H2气体产生,该速率比仅由H2O引起的Fe0氧化速率高10倍。在没有分子O2的情况下,NO3-离子而非H2O是地下水中的主要氧化剂。N质量平衡[例如,N2g、NH4+和NO3-]表明,在Fe0处理开始时,NO3-的非生物还原占主导,而一旦微生物活动开始,N2的产生变得更为重要。这些实验室结果与在野外运行约2年的单独大柱实验中的N2气体产生情况密切预测,在该实验中,检测到的最大气体体积约为600 ml d-1,其中99.5%(v/v)为N2。我们得出结论,NO3-通过与水竞争Fe0氧化而抑制了H2(g)的产生,尤其是在水处理开始时Fe0具有高反应性的时候。根据地下水成分,在野外维持PRB性能可能需要排气。