铁矿石催化过氧化氢—过硫酸钠去除地下水中三氯乙烯的研究
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摘要
三氯乙烯(TCE)在衣物干洗,电子元件和金属部件的去油污,制药提纯的溶剂萃取等领域有着大量的应用。TCE有潜在的致癌、致畸、致突变毒性。它从地表迁移到含水层,通常以粘稠非水溶液相(DNAPL)存在,缓慢持续地溶解于地下水中,威胁着地下水的饮水安全。
原位化学氧化(In situ chemical oxidation, ISCO)是一项通过向被污染的土壤和地下水注入氧化剂去除污染物的技术。过氧化氢与二价铁离子组成的芬顿试剂生成羟基自由基(HO·),其有着非常强的氧化能力,是常用于ISCO的试剂。但芬顿反应迅速,过氧化氢分解过快,放出巨大的热量和气体,对地下水土层结构的稳定和土著生物的安全有威胁。过硫酸钠是另一种常用于ISCO的氧化剂。它在环境中比较稳定,需要热量、过渡金属、UV等活化才能生成强氧化性的硫酸根自由基(S042-·),方可去除难降解的污染物。如果把这两种氧化剂组合使用,可能取得更好的效果。本文用3种天然铁矿石：菱铁矿、磁铁矿、赤铁矿与过氧化氢、过硫酸钠分别组合成3个铁矿石单氧化体系和3个铁矿石双氧化体系,以TCE作为目标污染物,研究TCE在这些单氧化体系和双氧化体系的去除效率及机理,氧化剂的分解动力学。取得的主要成果,如下：
这些氧化体系对TCE的去除效率排序是：菱铁矿双氧化体系(9.65mmol/L/87%)>磁铁矿双氧化体系(6.66 mmol/L或60%)>菱铁矿单氧化体系(4.2mmol/L/38%)>赤铁矿单氧化体系(4.10 mmol/L/37%)>磁铁矿单氧化体系(3.85 mmol/L/34%)>赤铁矿单氧化体系(3.19mmol/L/29%)。菱铁矿、磁铁矿、赤铁矿单氧化体系中TCE释放氯离子的量分别是7.65、6.33、3.98 mmol/L,菱铁矿、磁铁矿、赤铁矿双氧化体系释放的氯离子的量分别是20.35、11.45、8.75mmol/L。
3种铁矿石对过氧化氢分解催化作用最强的是菱铁矿,然后是磁铁矿,最弱的是赤铁矿。这与铁矿石中二价铁含量、比表面积有一定关系,但更重要的是,与铁矿石在溶液中的二价铁溶出的量有关。二价铁溶出的量越高,催化过氧化氢分解的能力越强。
这些氧化体系对TCE去除的机理可概括为：过氧化氢在二价铁的催化下产生羟基自由基,在三价铁的催化下产生过氧化氢自由基(H02·)、超氧自由基阴离子(02·)和单氧自由基阴离子(O·-)。强氧化性的羟基自由基对TCE双键进行加成反应,还原性的超氧自由基和单氧自由基对TCE分子的氯进行亲核取代反应,使TCE最终转化成二氧化碳和水,并释放出氯离子。
应用过氧化氢、过硫酸钠对含有微量铁的天然含水介质中的TCE去除,发现介质中的微量铁催化过氧化氢或过硫酸钠或它们的混合物降解TCE的量有限。当外加菱铁矿后,显著提高了双氧化剂降解TCE的能力。在这个体系中,提高过硫酸钠的浓度,对提高TCE的去除没有作用,但提高过氧化氢的浓度,可以显著提高TCE的去除量。当过氧化氢的浓度由1%提高到10%,体系的TCE下降到0.62 mmol/L(初始浓度是11.15 mmol/L),去除率达到94%。在此,虽然过氧化氢的浓度提高了一个数量级,但是体系中温度增加不超过2度,pH值的变化较小,表明了该体系的温度、pH变化对地下水中生物的影响比较温和。因此,菱铁矿双氧化体系对于原位修复被TCE污染的土壤或地下水表现出了很大的潜力。
Trichloroethylene (TCE) has a large number of applications in the dry cleaning of clothing, off oil for electronic components and metal parts, solvent extraction for purifing pharmaceutical and other fields. TCE has the potential carcinogenic, teratogenic, mutagenic toxicity. It migrated to the aquifer from the surface, usually exists as dense non-aqueous phase liquid (DNAPL), slow continuously dissolves in the groundwater, threatening the safety of drinking water of groundwater.
In situ chemical oxidation (In situ chemical oxidation, ISCO) is a technology that removing pollutants by pouring oxidants into the contaminated soil and groundwater. Hydrogen peroxide mixed with ferrous ion constructing of Fenton's reagent generates hydroxyl radicals (HO) with very strong oxidation, is one oxidantion reagent commonly used in ISCO remediation. But the Fenton reaction proceeds rapidly, of which hydrogen peroxide decompose fastly, releasing a lot of heat and gas, threatening the stability of soil structure and the safety of indigenous biology in groundwater. Sodium persulfate is another commonly used oxidant in ISCO remediation. It is relatively stable in the environment, but need heat, transition metals, UV and etc to activate and produce sulfate radicals (SO42-) with strong oxidation, and then can remove the refractory pollutants. If combine these two oxidants, they are expected to possiblely have better oxidation effects. In this paper, three kinds of naturally occurring iron minerals:siderite, magnetite, hematite were used to catalyze hydrogen peroxide, sodium persulfate, forming single- and double-oxidation systems to removing the TCE target pollutants. Research the removal efficiency and mechanism of degradation for TCE in the single-oxidant systems and the double-oxidant systems and decomposition kinetics of the oxidants in these systems. Main achievements were obtained as follows:
The removal efficiency of TCE in these oxidation system were in the order: siderite-double-oxidant system (9.65 mmol/L/87%)> magnetite-double-oxidant system (6.66 mmol/L or 60%)> siderite-single-oxidant system (4.2 mmol/L/38%)> hematite-single-oxidant system (4.10 mmol/L/37%)> magnetite-single-oxidant system (3.85 mmol/L/34%)> hematite-single-oxidant system (3.19 mmol/L/29%). The amount of chloride ions released from TCE in the three siderite-, magnetite-, hematite-single-oxidant systems were 7.65,6.33,3.98 mmol/L, respectively; the amount of chloride ions released in the siderite-, magnetite-, hematite-double oxidation system were 20.35,11.45,8.75 mmol/L.
The strongest catalytic role on the decomposition of hydrogen peroxide in the three kinds of iron mineral was paid by using siderite, and then the magnetite, hematite the weakest. This is result of bivalent iron content in the iron minerals and the specific surface area, but more important, is the amount of dissolved ferrous irons in solution. The higher amount of divalent iron ions of iron minerals dissove, the stronger catalytic abilities pay on the decompositon of hydrogen peroxide.
The mechanism of degradating TCE in these systems can be summarized as follows: hydrogen peroxide catalyzed by ferrous iron. When hydrogen peroxide catalyzed by trivalent iron produces hydroxyl radicals (HO2·), perhydroxyl radicals, superoxide radical anion (O2·) and single oxygen radicals anion (O·). The Hydroxyl radicals having strong oxidation addition reacted with the double bond of TCE. Superoxide radicals and single oxygen free radicals with reduction replaced chlorine of TCE molecule nucleophilic by substitution reaction. Finally, TCE changed into carbon dioxide and water, and releasing chloride ions.
Applications of hydrogen peroxide, sodium persulfate to remove TCE in natural aqueous medium contained trace iron. It was found that the trace iron in the medium catalyzed hydrogen peroxide or sodium persulfate or mixture of them degradated limited TCE. When extra siderite added, degradation of TCE was significantly improved by using the siderite-double-oxidant system. In this system, increased the concentration of sodium persulfate, had no effect on increasing removal TCE, but increased the concentration of hydrogen peroxide, could significantly increase the amount of removal TCE. When the concentration of hydrogen peroxide increased from 1%to 10%, TCE in the system decreased to 0.62 mmol/L (initiate concentration 11.15 mmol/L), obtained the removal rate of 94%for TCE. Here, although the concentration of hydrogen peroxide was enhanced by an order of magnitude, the temperature of the system did not exceed 2 degrees higher than the compared sample, pH values changed little, indicating that change of temperature and pH value in the system has relatively mild impact on biotechnology in groundwater. Therefore, siderite-double-oxidation system has shown a great potential for in-situ remediation of TCE contamination in groundwater.
原位化学氧化(In situ chemical oxidation, ISCO)是一项通过向被污染的土壤和地下水注入氧化剂去除污染物的技术。过氧化氢与二价铁离子组成的芬顿试剂生成羟基自由基(HO·),其有着非常强的氧化能力,是常用于ISCO的试剂。但芬顿反应迅速,过氧化氢分解过快,放出巨大的热量和气体,对地下水土层结构的稳定和土著生物的安全有威胁。过硫酸钠是另一种常用于ISCO的氧化剂。它在环境中比较稳定,需要热量、过渡金属、UV等活化才能生成强氧化性的硫酸根自由基(S042-·),方可去除难降解的污染物。如果把这两种氧化剂组合使用,可能取得更好的效果。本文用3种天然铁矿石：菱铁矿、磁铁矿、赤铁矿与过氧化氢、过硫酸钠分别组合成3个铁矿石单氧化体系和3个铁矿石双氧化体系,以TCE作为目标污染物,研究TCE在这些单氧化体系和双氧化体系的去除效率及机理,氧化剂的分解动力学。取得的主要成果,如下：
这些氧化体系对TCE的去除效率排序是：菱铁矿双氧化体系(9.65mmol/L/87%)>磁铁矿双氧化体系(6.66 mmol/L或60%)>菱铁矿单氧化体系(4.2mmol/L/38%)>赤铁矿单氧化体系(4.10 mmol/L/37%)>磁铁矿单氧化体系(3.85 mmol/L/34%)>赤铁矿单氧化体系(3.19mmol/L/29%)。菱铁矿、磁铁矿、赤铁矿单氧化体系中TCE释放氯离子的量分别是7.65、6.33、3.98 mmol/L,菱铁矿、磁铁矿、赤铁矿双氧化体系释放的氯离子的量分别是20.35、11.45、8.75mmol/L。
3种铁矿石对过氧化氢分解催化作用最强的是菱铁矿,然后是磁铁矿,最弱的是赤铁矿。这与铁矿石中二价铁含量、比表面积有一定关系,但更重要的是,与铁矿石在溶液中的二价铁溶出的量有关。二价铁溶出的量越高,催化过氧化氢分解的能力越强。
这些氧化体系对TCE去除的机理可概括为：过氧化氢在二价铁的催化下产生羟基自由基,在三价铁的催化下产生过氧化氢自由基(H02·)、超氧自由基阴离子(02·)和单氧自由基阴离子(O·-)。强氧化性的羟基自由基对TCE双键进行加成反应,还原性的超氧自由基和单氧自由基对TCE分子的氯进行亲核取代反应,使TCE最终转化成二氧化碳和水,并释放出氯离子。
应用过氧化氢、过硫酸钠对含有微量铁的天然含水介质中的TCE去除,发现介质中的微量铁催化过氧化氢或过硫酸钠或它们的混合物降解TCE的量有限。当外加菱铁矿后,显著提高了双氧化剂降解TCE的能力。在这个体系中,提高过硫酸钠的浓度,对提高TCE的去除没有作用,但提高过氧化氢的浓度,可以显著提高TCE的去除量。当过氧化氢的浓度由1%提高到10%,体系的TCE下降到0.62 mmol/L(初始浓度是11.15 mmol/L),去除率达到94%。在此,虽然过氧化氢的浓度提高了一个数量级,但是体系中温度增加不超过2度,pH值的变化较小,表明了该体系的温度、pH变化对地下水中生物的影响比较温和。因此,菱铁矿双氧化体系对于原位修复被TCE污染的土壤或地下水表现出了很大的潜力。
Trichloroethylene (TCE) has a large number of applications in the dry cleaning of clothing, off oil for electronic components and metal parts, solvent extraction for purifing pharmaceutical and other fields. TCE has the potential carcinogenic, teratogenic, mutagenic toxicity. It migrated to the aquifer from the surface, usually exists as dense non-aqueous phase liquid (DNAPL), slow continuously dissolves in the groundwater, threatening the safety of drinking water of groundwater.
In situ chemical oxidation (In situ chemical oxidation, ISCO) is a technology that removing pollutants by pouring oxidants into the contaminated soil and groundwater. Hydrogen peroxide mixed with ferrous ion constructing of Fenton's reagent generates hydroxyl radicals (HO) with very strong oxidation, is one oxidantion reagent commonly used in ISCO remediation. But the Fenton reaction proceeds rapidly, of which hydrogen peroxide decompose fastly, releasing a lot of heat and gas, threatening the stability of soil structure and the safety of indigenous biology in groundwater. Sodium persulfate is another commonly used oxidant in ISCO remediation. It is relatively stable in the environment, but need heat, transition metals, UV and etc to activate and produce sulfate radicals (SO42-) with strong oxidation, and then can remove the refractory pollutants. If combine these two oxidants, they are expected to possiblely have better oxidation effects. In this paper, three kinds of naturally occurring iron minerals:siderite, magnetite, hematite were used to catalyze hydrogen peroxide, sodium persulfate, forming single- and double-oxidation systems to removing the TCE target pollutants. Research the removal efficiency and mechanism of degradation for TCE in the single-oxidant systems and the double-oxidant systems and decomposition kinetics of the oxidants in these systems. Main achievements were obtained as follows:
The removal efficiency of TCE in these oxidation system were in the order: siderite-double-oxidant system (9.65 mmol/L/87%)> magnetite-double-oxidant system (6.66 mmol/L or 60%)> siderite-single-oxidant system (4.2 mmol/L/38%)> hematite-single-oxidant system (4.10 mmol/L/37%)> magnetite-single-oxidant system (3.85 mmol/L/34%)> hematite-single-oxidant system (3.19 mmol/L/29%). The amount of chloride ions released from TCE in the three siderite-, magnetite-, hematite-single-oxidant systems were 7.65,6.33,3.98 mmol/L, respectively; the amount of chloride ions released in the siderite-, magnetite-, hematite-double oxidation system were 20.35,11.45,8.75 mmol/L.
The strongest catalytic role on the decomposition of hydrogen peroxide in the three kinds of iron mineral was paid by using siderite, and then the magnetite, hematite the weakest. This is result of bivalent iron content in the iron minerals and the specific surface area, but more important, is the amount of dissolved ferrous irons in solution. The higher amount of divalent iron ions of iron minerals dissove, the stronger catalytic abilities pay on the decompositon of hydrogen peroxide.
The mechanism of degradating TCE in these systems can be summarized as follows: hydrogen peroxide catalyzed by ferrous iron. When hydrogen peroxide catalyzed by trivalent iron produces hydroxyl radicals (HO2·), perhydroxyl radicals, superoxide radical anion (O2·) and single oxygen radicals anion (O·). The Hydroxyl radicals having strong oxidation addition reacted with the double bond of TCE. Superoxide radicals and single oxygen free radicals with reduction replaced chlorine of TCE molecule nucleophilic by substitution reaction. Finally, TCE changed into carbon dioxide and water, and releasing chloride ions.
Applications of hydrogen peroxide, sodium persulfate to remove TCE in natural aqueous medium contained trace iron. It was found that the trace iron in the medium catalyzed hydrogen peroxide or sodium persulfate or mixture of them degradated limited TCE. When extra siderite added, degradation of TCE was significantly improved by using the siderite-double-oxidant system. In this system, increased the concentration of sodium persulfate, had no effect on increasing removal TCE, but increased the concentration of hydrogen peroxide, could significantly increase the amount of removal TCE. When the concentration of hydrogen peroxide increased from 1%to 10%, TCE in the system decreased to 0.62 mmol/L (initiate concentration 11.15 mmol/L), obtained the removal rate of 94%for TCE. Here, although the concentration of hydrogen peroxide was enhanced by an order of magnitude, the temperature of the system did not exceed 2 degrees higher than the compared sample, pH values changed little, indicating that change of temperature and pH value in the system has relatively mild impact on biotechnology in groundwater. Therefore, siderite-double-oxidation system has shown a great potential for in-situ remediation of TCE contamination in groundwater.
引文
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