Cr(Ⅲ)-有机酸配合物的氧化及其在土壤中的吸附迁移性研究
摘要
铬是一种过渡金属元素,特殊的理化性质使其成为工业生产和人民生活的重要原料。但含铬三废(废气、废水、废渣)的不合理排放,使环境铬污染问题日益突出。铬在环境中主要以Cr(Ⅵ)和Cr(Ⅲ)两种形态存在,Cr(Ⅲ)还原性弱,毒性小,易被土壤吸附；而Cr(Ⅵ)溶解性强,毒性大,迁移性大,对环境有严重的危害。目前对铬的污染治理主要集中在对Cr(Ⅵ)的还原方面。小分子有机酸是C(Ⅵ)还原的一类常用还原剂,并且在土壤中广泛存在,但在还原过程中,小分子有机酸易和还原产物Cr(Ⅲ)形成配合物,使得Cr(Ⅲ)在土壤中的吸附性大大降低。然而,土壤中Cr(Ⅲ)有可能再被氧化为Cr(Ⅵ)重新进入土壤,应该引起更多的关注。氧化锰矿物是目前唯一可知的能氧化Cr(Ⅲ)的天然氧化剂,也是Cr(Ⅲ)氧化为Cr(Ⅵ)的重要途径。另一个Cr(Ⅲ)转变为Cr(Ⅵ)的可能途径是光化学氧化。由于Cr(Ⅲ)-有机酸配合物的形成使得Cr(Ⅲ)在土壤中的吸附性大大降低,提高了Cr(Ⅲ)被氧化为Cr(Ⅵ)的危害,所以研究Cr(Ⅲ)-有机配合物的氧化及其在土壤中的吸附和迁移性很重要。为此,本文选择了三种常用的有机酸：柠檬酸、酒石酸和苹果酸,以实验室合成的Cr(Ⅲ)-有机酸配合物为模型,系统地研究了Cr(Ⅲ)-有机酸在环境中的氧化及吸附和迁移行为。本论文共分三部分：
第一部分：实验室制备出水钠锰矿(8-MnO2),同时也制备和纯化了Cr(Ⅲ)-柠檬酸(Cr(Ⅲ)-cit)和Cr(Ⅲ)-酒石酸(Cr(Ⅲ)-tar)配合物,通过批次实验研究了不同条件下δ-MnO2对Cr(Ⅲ)-柠檬酸和Cr(Ⅲ)-酒石酸配合物的氧化。结果表明,较低pH和较高浓度的δ-MnO2能促进Cr(Ⅵ)的产生。pH主要通过影响Cr(Ⅲ)-柠檬酸和Cr(Ⅲ)-酒石酸配合物的存在形态来影响反应。NO3-、Cl-和SO42-三种离子对氧化有轻微的促进作用。P043-因和Cr(Ⅲ)形成更稳定的CrP04抑制了氧化,NH4+可能因电离产生的NH3和Cr(Ⅲ)形成[Cr(NH3)6]3+配离子促进了氧化。氧化过程中Cr(Ⅲ)-柠檬酸/酒石酸的氧化量随着反应温度的升高而增加。两种体系的氧化过程均可以分为两段,开始阶段反应迅速,符合一级动力学方程；第二阶段反应平缓,符合零级动力学规律。在所有反应情况中,Cr(Ⅲ)-柠檬酸/酒石酸的氧化量均低于自由态Cr(Ⅲ),但随着反应的继续,氧化量持续增加；Cr(Ⅲ)-酒石酸的氧化量高于Cr(Ⅲ)-柠檬酸,预示着后者的稳定性大于前者。
第二部分：本部分以苹果酸和Cr(Ⅲ)为原料,实验室合成并纯化了Cr(Ⅲ)-苹果酸配合物(Cr(Ⅲ)-mal),并对其在不同pH条件下的存在形态进行了高效液相色谱(HPLC)检测和分析。通过批次实验研究了在光照条件下Cr(Ⅲ)-苹果酸配合物氧化释放Cr(Ⅵ)的行为机理。结果表明Cr(Ⅲ)和苹果酸以2：3的配比形成配合物,配合物在pH6.0-12.0范围内主要是以[Cr2(Ⅲ)-mal3]和[Cr2(Ⅲ)-mal3-OH]两种形态存在,在pH8.0和pH12.0时,[Cr2(Ⅲ)-mal3-OH2]2和[Cr2(Ⅲ)-mal3-OH3]3分别开始出现并共存于溶液中。它们的光氧化活性顺序依次推理为：[Cr2(Ⅲ)-mal3-OH3]3->[Cr2(Ⅲ)-mal3-OH2]2->[Cr2(Ⅲ)-mal3-OH]->[Cr2(III)-mal3]。增加光照强度以及温度、pH的升高都可以促进配合物光氧化释放Cr(Ⅵ);Cr(Ⅲ)-苹果酸配合物通过金属-配体电子转移(LMCT)方式产生的Cr(Ⅱ)和·OH是Cr(Ⅵ)生成的先决条件,H202的添加增加了·OH的数量,有效促进了Cr(Ⅵ)的产生；但由光照作用释放的苹果酸会对Cr(Ⅵ)进行还原,只有在pH>7.0时,Cr(Ⅲ)-苹果酸才表现为氧化,整个氧化过程遵循初始阶段为一级动力学反应和后半段为零级动力学反应。
第三部分：实验室合成了Cr(Ⅲ)-酒石酸/苹果酸配合物,通过批次实验研究了它们在红壤、黄棕壤和黑土中的吸附和迁移性。研究表明：在pH4.0、25℃时,Cr(Ⅲ)-酒石酸/苹果酸在三种土壤中的吸附均随土液比的增加而增加,但远小于土壤对自由Cr(Ⅲ)的吸附。在pH为4.0、6.5和9.0时,pH对Cr(Ⅲ)-酒石酸在三种土壤中的吸附几乎没有影响,而对Cr(Ⅲ)-苹果酸影响较小,两者在三种土壤中的吸附均遵循红壤>黄棕壤>黑土的规律,且Cr(Ⅲ)-苹果酸大于Cr(Ⅲ)-酒石酸。去除有机质后,三种土壤对Cr(Ⅲ)-酒石酸/苹果酸的吸附均增加,但对Cr(Ⅲ)-苹果酸的吸附仍大于Cr(Ⅲ)-酒石酸。在淋溶液初始pH为4.0、6.5和9.0时,Cr(Ⅲ)-酒石酸在土壤中的迁移受pH影响较小,而Cr(Ⅲ)-苹果酸在pH9.0时产生沉淀,受pH影响较大。Cr(Ⅲ)-苹果酸在三种土壤中的迁移性均小于Cr(Ⅲ)-酒石酸,而两者在黄棕壤和黑土中的迁移性均大于红壤。
Chromium(Cr), a transition metal element, is an important material in industrial production and people's lives because of its special physical and chemical properties. However, chromium pollution has become increasingly serious due to the unreasonable emissions of chromium-containing wastes (waste gas, waste water, waste residue). Cr(Ⅲ) and Cr(Ⅵ) are the two mainly forms that exist in environment. Cr(Ⅲ) has low reductivity, weak toxicity and is easily adsorbed by soil, while Cr(Ⅵ) is highly soluble, toxic and mobile, posing serious environmental hazards. As a result, reduction of Cr(Ⅵ) has become the focus on the management of Cr pollution. Small molecular organic acids, which are ubiquitous in soil, are common reductants for Cr(Ⅵ), but the formation of complex betweenCr(Ⅲ), a reduction product, and small molecular organic acid reduces the adsorption of Cr(Ⅲ) by soils. However, more attention should be paid on the reoxidation of reduced Cr(Ⅲ) to Cr(Ⅵ) which will re-enter into the soil. Manganese oxides are known to be the only one type of nature oxidants resulting in transformation of Cr(Ⅲ) to Cr(Ⅵ) in soils, and it is an important pathway for Cr(Ⅲ) oxidation to Cr(Ⅵ). Another important pathway for Cr(Ⅲ) transformation to Cr(Ⅵ) is photo-oxidation. As the formation of Cr(Ⅲ)-organic acids greatly reduces the adsorption of Cr(Ⅲ) by soils, which virtually enhanced the hazards of Cr(Ⅲ) oxidation to Cr(Ⅵ). Therefore, it is important to study the oxidation of Cr(Ⅲ)-organic acid and its adsorption and mobility in soils. In this study, three common small molecular organic acids were selected to synthesize the Cr(Ⅲ)-organic complexes as models in order to systematically investigate the oxidation, adsorption and mobility of Cr(Ⅲ)-organic complexes in soils. The dissertation includes three parts.
In part Ⅰ:Cr(Ⅲ)-citrate (Cr(Ⅲ)-cit) and Cr(Ⅲ)-tartrate (Cr(Ⅲ)-tar) complexes were synthesized and purified, and then their stability in the presence of δ-MnO2were further investigated in batch experiments under different conditions to predict the potential oxidation behaviors of Cr(Ⅲ)-organic acid complexes in environments. Lower pH and higher concentration of δ-MnO2markedly enhanced the production of Cr(Ⅵ).The reaction was primarily affected by pH in a way of the forms of Cr(Ⅲ)-cit and Cr(Ⅲ)-tar affected by pH. Three anions, NO3-、Cl-and SO42-had a little positive promotion role in the oxidation of Cr(Ⅲ)-cit and Cr(Ⅲ)-tar in comparison with control. Ammonium ion significantly improved the oxidation of Cr(Ⅲ)-cit and Cr(Ⅲ)-tar by the formation of [Cr(NH3)6]3+, but phosphate ion demonstrated an opposite effect due to form more stable CrPO4. The oxidation amounts of Cr(Ⅲ)-cit and Cr(Ⅲ)-tar increased with the temperature increasing during the process. The oxidation process of Cr(Ⅲ)-cit and Cr(Ⅲ)-tar over δ-MnO2could be divided into two phases. At the initial phase, a relatively rapid reaction obeyed to first-order model, and then was followed by a very slow one with a characteristic of zero-order. The results indicated that although the rates and extents of Cr(Ⅲ)-cit and Cr(Ⅲ)-tar oxidation by δ-MnO2were much lower than those of aqueous Cr(Ⅲ),Cr(Ⅵ) could be gradually released through the whole reaction. It is observed that in the all cases the extent of Cr(Ⅲ)-cit oxidation was lower than Cr(Ⅲ)-tar. Thus, it is concluded that the stability of Cr(Ⅲ)-cit was higher than Cr(Ⅲ)-tar.
In part Ⅱ:Cr(Ⅲ)-malate complex(Cr(Ⅲ)-mal) was synthesized and purified and its species in different pHs were analyzed by High Performance Liquid Chromatography (HPLC). Batch photo-oxidation experiments were conducted to reveal the potential pathway of Cr(Ⅲ) to Cr(VI). The results indicated that in Cr(Ⅲ)-malate complex the chelating molar ratio of Cr(Ⅲ) and malic acid was2:3.[Cr2(Ⅲ)-mal3] and [Cr2(Ⅲ)-mal3-OH]-are the two main species of complex at pH6.0-12.0,[Cr2(Ⅲ)-mal3-OH2]2-and [Cr2(Ⅲ)-mal3-OH3]3-appeared and then coexisted in solution at pH8.0and pH12.0, respectively. The photo-oxidation activity was speculated in this order:[Cr2(Ⅲ)-mal3-OH3]3->[Cr2(Ⅲ)-mal3-OH2]2->[Cr2(Ⅲ)-mal3-OH]->[Cr2(Ⅲ)-mal3]. Higher pH, temperature and stronger light intensity promoted the conversion process. Cr(Ⅱ) and·OH, two intermediates, produced through a ligand-metal charge-transfer(LMCT) path of Cr(Ⅲ)-malate complex were the two pre-condition for Cr(Ⅵ) production. The introduction of H2O2, considered as a direct source of hydroxyl radicals (·OH) with irradiation, markedly enhanced the yield of Cr(Ⅵ). But the malic acid released from the photoexcitation could reduce Cr(Ⅵ), and the oxidation of Cr(Ⅲ)-malate complex took place only at pH>7.0. The photo-oxidation of Cr(Ⅲ)-malate complex obeyed to first-order kinetics at the initial stage of the reaction and then a zero-order one was followed.
In part Ⅲ:Cr(Ⅲ)-tar and Cr(Ⅲ)-mal complex were synthesized and purified and batch experiments were conducted to investigate their adsorption and mobility in red soil, yellow-brown soil and chernozem. The results indicated that the adsorption of Cr(Ⅲ)-tar and Cr(Ⅲ)-mal by the three soils increased with the soil concentration(ratio of soil to solution by weight) increasing at pH4.0and25℃, but far less than that of free Cr(Ⅲ)-under the same condition. Almost no effect of pH in a range of4.0to9.0on the adsorption of Cr(Ⅲ)-tar by the three soils was found, but a weak role of pH in adsorption of Cr(Ⅲ)-mal occurred. The adsorption of both Cr(Ⅲ)-tar and Cr(Ⅲ)-mal by the three soils was in the order:red soil>yellow-brown soil>chernozem, and the adsorption amount of Cr(Ⅲ)-mal was larger than that of Cr(Ⅲ)-tar. The adsorption of both Cr(Ⅲ)-tar and Cr(Ⅲ)-mal by the three soils increased when the organic matter was removed from the soils. The adsorption amount of Cr(Ⅲ)-mal, however, was still higher than that of Cr(Ⅲ)-tar. The mobility of Cr(Ⅲ)-tar in the three soils was slightly affected by pH when the initial pHs of leaching solution were4.0,6.5and9.0. In contrast, Cr(Ⅲ)-mal was greatly affected by pH and precipitation occurred in Cr(Ⅲ)-malate solution at pH9.0. The mobility of Cr(Ⅲ)-mal in the three soils is weaker than that of Cr(Ⅲ)-tar. The mobility of Cr(Ⅲ)-tar/mal in yellow-brown soil and chernozem is stronger than that in red soil.
第一部分：实验室制备出水钠锰矿(8-MnO2),同时也制备和纯化了Cr(Ⅲ)-柠檬酸(Cr(Ⅲ)-cit)和Cr(Ⅲ)-酒石酸(Cr(Ⅲ)-tar)配合物,通过批次实验研究了不同条件下δ-MnO2对Cr(Ⅲ)-柠檬酸和Cr(Ⅲ)-酒石酸配合物的氧化。结果表明,较低pH和较高浓度的δ-MnO2能促进Cr(Ⅵ)的产生。pH主要通过影响Cr(Ⅲ)-柠檬酸和Cr(Ⅲ)-酒石酸配合物的存在形态来影响反应。NO3-、Cl-和SO42-三种离子对氧化有轻微的促进作用。P043-因和Cr(Ⅲ)形成更稳定的CrP04抑制了氧化,NH4+可能因电离产生的NH3和Cr(Ⅲ)形成[Cr(NH3)6]3+配离子促进了氧化。氧化过程中Cr(Ⅲ)-柠檬酸/酒石酸的氧化量随着反应温度的升高而增加。两种体系的氧化过程均可以分为两段,开始阶段反应迅速,符合一级动力学方程；第二阶段反应平缓,符合零级动力学规律。在所有反应情况中,Cr(Ⅲ)-柠檬酸/酒石酸的氧化量均低于自由态Cr(Ⅲ),但随着反应的继续,氧化量持续增加；Cr(Ⅲ)-酒石酸的氧化量高于Cr(Ⅲ)-柠檬酸,预示着后者的稳定性大于前者。
第二部分：本部分以苹果酸和Cr(Ⅲ)为原料,实验室合成并纯化了Cr(Ⅲ)-苹果酸配合物(Cr(Ⅲ)-mal),并对其在不同pH条件下的存在形态进行了高效液相色谱(HPLC)检测和分析。通过批次实验研究了在光照条件下Cr(Ⅲ)-苹果酸配合物氧化释放Cr(Ⅵ)的行为机理。结果表明Cr(Ⅲ)和苹果酸以2：3的配比形成配合物,配合物在pH6.0-12.0范围内主要是以[Cr2(Ⅲ)-mal3]和[Cr2(Ⅲ)-mal3-OH]两种形态存在,在pH8.0和pH12.0时,[Cr2(Ⅲ)-mal3-OH2]2和[Cr2(Ⅲ)-mal3-OH3]3分别开始出现并共存于溶液中。它们的光氧化活性顺序依次推理为：[Cr2(Ⅲ)-mal3-OH3]3->[Cr2(Ⅲ)-mal3-OH2]2->[Cr2(Ⅲ)-mal3-OH]->[Cr2(III)-mal3]。增加光照强度以及温度、pH的升高都可以促进配合物光氧化释放Cr(Ⅵ);Cr(Ⅲ)-苹果酸配合物通过金属-配体电子转移(LMCT)方式产生的Cr(Ⅱ)和·OH是Cr(Ⅵ)生成的先决条件,H202的添加增加了·OH的数量,有效促进了Cr(Ⅵ)的产生；但由光照作用释放的苹果酸会对Cr(Ⅵ)进行还原,只有在pH>7.0时,Cr(Ⅲ)-苹果酸才表现为氧化,整个氧化过程遵循初始阶段为一级动力学反应和后半段为零级动力学反应。
第三部分：实验室合成了Cr(Ⅲ)-酒石酸/苹果酸配合物,通过批次实验研究了它们在红壤、黄棕壤和黑土中的吸附和迁移性。研究表明：在pH4.0、25℃时,Cr(Ⅲ)-酒石酸/苹果酸在三种土壤中的吸附均随土液比的增加而增加,但远小于土壤对自由Cr(Ⅲ)的吸附。在pH为4.0、6.5和9.0时,pH对Cr(Ⅲ)-酒石酸在三种土壤中的吸附几乎没有影响,而对Cr(Ⅲ)-苹果酸影响较小,两者在三种土壤中的吸附均遵循红壤>黄棕壤>黑土的规律,且Cr(Ⅲ)-苹果酸大于Cr(Ⅲ)-酒石酸。去除有机质后,三种土壤对Cr(Ⅲ)-酒石酸/苹果酸的吸附均增加,但对Cr(Ⅲ)-苹果酸的吸附仍大于Cr(Ⅲ)-酒石酸。在淋溶液初始pH为4.0、6.5和9.0时,Cr(Ⅲ)-酒石酸在土壤中的迁移受pH影响较小,而Cr(Ⅲ)-苹果酸在pH9.0时产生沉淀,受pH影响较大。Cr(Ⅲ)-苹果酸在三种土壤中的迁移性均小于Cr(Ⅲ)-酒石酸,而两者在黄棕壤和黑土中的迁移性均大于红壤。
Chromium(Cr), a transition metal element, is an important material in industrial production and people's lives because of its special physical and chemical properties. However, chromium pollution has become increasingly serious due to the unreasonable emissions of chromium-containing wastes (waste gas, waste water, waste residue). Cr(Ⅲ) and Cr(Ⅵ) are the two mainly forms that exist in environment. Cr(Ⅲ) has low reductivity, weak toxicity and is easily adsorbed by soil, while Cr(Ⅵ) is highly soluble, toxic and mobile, posing serious environmental hazards. As a result, reduction of Cr(Ⅵ) has become the focus on the management of Cr pollution. Small molecular organic acids, which are ubiquitous in soil, are common reductants for Cr(Ⅵ), but the formation of complex betweenCr(Ⅲ), a reduction product, and small molecular organic acid reduces the adsorption of Cr(Ⅲ) by soils. However, more attention should be paid on the reoxidation of reduced Cr(Ⅲ) to Cr(Ⅵ) which will re-enter into the soil. Manganese oxides are known to be the only one type of nature oxidants resulting in transformation of Cr(Ⅲ) to Cr(Ⅵ) in soils, and it is an important pathway for Cr(Ⅲ) oxidation to Cr(Ⅵ). Another important pathway for Cr(Ⅲ) transformation to Cr(Ⅵ) is photo-oxidation. As the formation of Cr(Ⅲ)-organic acids greatly reduces the adsorption of Cr(Ⅲ) by soils, which virtually enhanced the hazards of Cr(Ⅲ) oxidation to Cr(Ⅵ). Therefore, it is important to study the oxidation of Cr(Ⅲ)-organic acid and its adsorption and mobility in soils. In this study, three common small molecular organic acids were selected to synthesize the Cr(Ⅲ)-organic complexes as models in order to systematically investigate the oxidation, adsorption and mobility of Cr(Ⅲ)-organic complexes in soils. The dissertation includes three parts.
In part Ⅰ:Cr(Ⅲ)-citrate (Cr(Ⅲ)-cit) and Cr(Ⅲ)-tartrate (Cr(Ⅲ)-tar) complexes were synthesized and purified, and then their stability in the presence of δ-MnO2were further investigated in batch experiments under different conditions to predict the potential oxidation behaviors of Cr(Ⅲ)-organic acid complexes in environments. Lower pH and higher concentration of δ-MnO2markedly enhanced the production of Cr(Ⅵ).The reaction was primarily affected by pH in a way of the forms of Cr(Ⅲ)-cit and Cr(Ⅲ)-tar affected by pH. Three anions, NO3-、Cl-and SO42-had a little positive promotion role in the oxidation of Cr(Ⅲ)-cit and Cr(Ⅲ)-tar in comparison with control. Ammonium ion significantly improved the oxidation of Cr(Ⅲ)-cit and Cr(Ⅲ)-tar by the formation of [Cr(NH3)6]3+, but phosphate ion demonstrated an opposite effect due to form more stable CrPO4. The oxidation amounts of Cr(Ⅲ)-cit and Cr(Ⅲ)-tar increased with the temperature increasing during the process. The oxidation process of Cr(Ⅲ)-cit and Cr(Ⅲ)-tar over δ-MnO2could be divided into two phases. At the initial phase, a relatively rapid reaction obeyed to first-order model, and then was followed by a very slow one with a characteristic of zero-order. The results indicated that although the rates and extents of Cr(Ⅲ)-cit and Cr(Ⅲ)-tar oxidation by δ-MnO2were much lower than those of aqueous Cr(Ⅲ),Cr(Ⅵ) could be gradually released through the whole reaction. It is observed that in the all cases the extent of Cr(Ⅲ)-cit oxidation was lower than Cr(Ⅲ)-tar. Thus, it is concluded that the stability of Cr(Ⅲ)-cit was higher than Cr(Ⅲ)-tar.
In part Ⅱ:Cr(Ⅲ)-malate complex(Cr(Ⅲ)-mal) was synthesized and purified and its species in different pHs were analyzed by High Performance Liquid Chromatography (HPLC). Batch photo-oxidation experiments were conducted to reveal the potential pathway of Cr(Ⅲ) to Cr(VI). The results indicated that in Cr(Ⅲ)-malate complex the chelating molar ratio of Cr(Ⅲ) and malic acid was2:3.[Cr2(Ⅲ)-mal3] and [Cr2(Ⅲ)-mal3-OH]-are the two main species of complex at pH6.0-12.0,[Cr2(Ⅲ)-mal3-OH2]2-and [Cr2(Ⅲ)-mal3-OH3]3-appeared and then coexisted in solution at pH8.0and pH12.0, respectively. The photo-oxidation activity was speculated in this order:[Cr2(Ⅲ)-mal3-OH3]3->[Cr2(Ⅲ)-mal3-OH2]2->[Cr2(Ⅲ)-mal3-OH]->[Cr2(Ⅲ)-mal3]. Higher pH, temperature and stronger light intensity promoted the conversion process. Cr(Ⅱ) and·OH, two intermediates, produced through a ligand-metal charge-transfer(LMCT) path of Cr(Ⅲ)-malate complex were the two pre-condition for Cr(Ⅵ) production. The introduction of H2O2, considered as a direct source of hydroxyl radicals (·OH) with irradiation, markedly enhanced the yield of Cr(Ⅵ). But the malic acid released from the photoexcitation could reduce Cr(Ⅵ), and the oxidation of Cr(Ⅲ)-malate complex took place only at pH>7.0. The photo-oxidation of Cr(Ⅲ)-malate complex obeyed to first-order kinetics at the initial stage of the reaction and then a zero-order one was followed.
In part Ⅲ:Cr(Ⅲ)-tar and Cr(Ⅲ)-mal complex were synthesized and purified and batch experiments were conducted to investigate their adsorption and mobility in red soil, yellow-brown soil and chernozem. The results indicated that the adsorption of Cr(Ⅲ)-tar and Cr(Ⅲ)-mal by the three soils increased with the soil concentration(ratio of soil to solution by weight) increasing at pH4.0and25℃, but far less than that of free Cr(Ⅲ)-under the same condition. Almost no effect of pH in a range of4.0to9.0on the adsorption of Cr(Ⅲ)-tar by the three soils was found, but a weak role of pH in adsorption of Cr(Ⅲ)-mal occurred. The adsorption of both Cr(Ⅲ)-tar and Cr(Ⅲ)-mal by the three soils was in the order:red soil>yellow-brown soil>chernozem, and the adsorption amount of Cr(Ⅲ)-mal was larger than that of Cr(Ⅲ)-tar. The adsorption of both Cr(Ⅲ)-tar and Cr(Ⅲ)-mal by the three soils increased when the organic matter was removed from the soils. The adsorption amount of Cr(Ⅲ)-mal, however, was still higher than that of Cr(Ⅲ)-tar. The mobility of Cr(Ⅲ)-tar in the three soils was slightly affected by pH when the initial pHs of leaching solution were4.0,6.5and9.0. In contrast, Cr(Ⅲ)-mal was greatly affected by pH and precipitation occurred in Cr(Ⅲ)-malate solution at pH9.0. The mobility of Cr(Ⅲ)-mal in the three soils is weaker than that of Cr(Ⅲ)-tar. The mobility of Cr(Ⅲ)-tar/mal in yellow-brown soil and chernozem is stronger than that in red soil.
引文
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