不同电子供体对水稻土中铁还原的影响
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摘要
氧化铁是土壤中最为丰富的金属氧化物，在土壤的氧化还原反应和土壤形成过程中起着十分重要的作用。淹水又是促进氧化铁形态转化的重要因素之一。土壤淹水后，微生物利用外界的Fe(Ⅲ)作为电子受体，氧化体内的基质（电子供体），从而使Fe(Ⅲ)还原为Fe(Ⅱ)。这种过程被称为异化铁还原作用。他能够直接影响土壤中N、P、K及Si等营养元素的有效性，并且对有机污染物的降解具有重要的意义。因此，研究异化铁还原作用的环境学意义已成为当今土壤环境化学的热点问题。
水稻土中氧化铁的还原程度受土壤中不同电子供体和受体的制约。通过添加有机物，一方面可以增加电子供体数量，同时也改变土壤中氧化铁的络合与溶解作用能力。利用这种电子竞争的特征，可以作为消除或减少土壤污染物的有效途径。
本文选用铁的氧化还原周期性发生的水稻土为材料，采用室内淹水密闭恒温培养的方法研究了不同土壤以及不同土壤的不同微团聚体中铁还原特征，通过在不同的培养时间添加醋酸盐、丙酸盐和葡萄糖3种有机物作为电子受体对原土和耗竭有机质后的土壤中铁还原的影响的研究，比较来源于不同水稻土的微生物在异化铁还原过程中对乙酸盐、丙酸盐、葡萄糖利用能力的差异，为更深入地研究该过程及其环境意义提供科学依据。五种水稻土样分别采自吉林、湖南、四川、江西和广东等省区。实验获得以下主要结果：
1. 不同水稻土中Fe(II)生成的平衡浓度是不同水稻土的重要特征，其数量与土壤中微生物的种类、易还原氧化铁的数量、其它电子受体的种类和数量、电子供体的数量有关。铁还原反应趋于稳定时所产生的Fe(II)的浓度各不相同，大小顺序是：土样1(JL)>土样3(SC)>土样5(GD)>土样4(JX)。
2. 不同土壤及不同反应阶段的铁还原速率有着明显的区别。土样1(JL)和土样3(SC)没有测出明显的启动期，这与培养温度(30℃)较高有关。江西水稻土和广东水稻土中微生物繁殖具有明显的启动时间。在铁还原反应快速增加阶段，表观平均还原速率大小为：土样3(SC)>土样4(JX)>土样1(JL)>土样5(GD)。在铁还原稳定期，除土样5(GD)以外，其它土壤的平均反应速率差别不大。土样5(GD)的反应速率较大由其土壤中富含氧化铁所致。
3. 不同土壤及不同团聚体中铁还原差异主要是由不同组分中氧化铁的化学形态及有机质含量，微生物数量及其活性决定。对不同大小的微团聚体来说，除广东的水稻土外，不同大小的微团聚体之间的铁还原程度都表现为：（<0.001mm的微团聚体）>?.001～0.05 mm的微团聚体）>?.05～0.25mm的微团聚体）；对于广东水稻土，其<0.001mm和0.05～0.25mm的微团聚体中的有机质数量可能是限制铁还原的关键因素。
4. 淹水土壤中的微生物还原铁的过程同时受到电子供体及电子受体的限制，添加不同有机酸，明显促进了铁的还原。在添加氧化铁处理中，葡萄糖对铁还原的促进作用更为明显。在有机质耗竭的水稻土中，添加乙酸盐(+Ac－)及丙酸盐(Prop)处理对土壤中氧化铁的还原在培养前期有一定的促进作用，但后期的Fe(II)量与对照(CK)比较并无明显的差异，仅在土样3(SC)中添加葡萄糖处理(+Glu)的Fe(II)量与对照(CK)比较有所增大。然而，对添加了易还原氧化铁(+Fe)处理，添加葡萄糖、乙酸盐及丙酸盐均明显增加了Fe(II)的产生量，影响程度表现为：(+Fe+Glu)处理>(+Fe+Ac－-)处理>(+Fe+Prop)处理>(CK+Fe)处理。当土壤中易还原氧化铁过量时，有机物缺乏或许成为主要限制因素，此时添加有机物可提供足够的电子供体，有效地促进了氧化铁的还原。
5. 添加外源有机物可以有效地促进氧化铁的微生物还原过程。从铁的还原量比较，土壤中易还原铁的总量大体为9.23 mg/g(JX)和12.06 mg/g(SC)。添加葡萄糖(+Fe+Glu)处理，两种土壤的铁还原量可达9.910和9.925 mg/g(JX)及12.67和14.55 mg/g(SC)，表明添加的氧化铁已被充分的还原。在不加有机物的对照(CK+Fe)处理中，Fe(II)还原量分别为4.875和5.135 mg/g(JX)及7.855和9.295 mg/g(SC)，添加的氧化铁在先添加有机物试验中的还原率为17.28%和19.23%，而在培养过程中添加有机物试验的氧化铁还原率为20.79%和47.28%；添加乙酸盐(+Fe+Ac－)处理的外源铁还原效率分别为73.05%和82.97%(JX)及94.04%和91.82%(SC)。
Ferric oxide is the most abundant metal oxide, and it is very important in oxidization- reduction of soil and in soil-shaped process. Inundation is an in important factor in accelerating the invert of ferric oxide conformation. After inundation, microbe can use outside Fe(Ⅲ) as its electron acceptor, oxygenation its matrix(electron donor), thereby Fe(Ⅲ) deoxidize to Fe(Ⅱ).This process go by the name of dissimilatory reduction. It can affect availability of nutrients such as N、P、K and Si in the soil directly, and it is important to degradation of organic pollutant, Iron reduction is likely to a new available approach of soil decontamination. Therefore, the process is turned into a hotspot issue of soil environmental chemistry that studied the significance of dissimilatory reduction.
The degree of iron reduction is restrained by the different electron acceptor and provider in the paddy slurry. Through adding organic matter, one way can increase the quantity of electron, at the same time, another way can change the ability of iron combination and dissolution. Making use of the characteristic of electron competition, as a valid way, may remove or reduce soil contamination.
In this study, the soil samples were used in which red-oxy-reaction periodically occurred. The characteristics of iron reduction in different soil samples and different sized aggregates were investigated by flooding incubation in sealed vials at fixed temperature under airtight condition. We also investigated the differences of iron reduction in intact soil and organic exhausted paddy soil sample by adding acetate, propaniate and glucoses as electron donors and the differences of acetate, propaniate and glucose utilities in the dissimilatory iron reduction by microorganism from different soil samples, providing some scientific data and suggestion in dissimilatory iron reduction and its related environmental effects. The five paddy soil samples were collected from JiLin, HuNan, SiChuan, JiangXi, GuangDong.
The main results in this study were showed as the following:
1. The equilibrium concentrations of accumulative Fe(II) were differed from these soil samples, which were correlated with microorganism groups, labile iron oxidizes, other electron acceptors and electron donor spices. The accumulative Fe(II) in stable phase were different in these soil samples and followed the order: sample 1 (JL)> sample 3 (SC)>sample 5 (GD)> sample 4 (JX).
2. Iron reducing rates were distinct in different phase of these soils. No obvious initial phase were found in sample(JL) and sample(SC), maybe for the reasons of higher incubation
temperature(30℃). Microbial activities in JX and GD paddy soil samples showed an apparent initial phase. In the rapid reducing phase, the observed mean reducing rates were in the order of sample3(SC)>sample4(JX)>sample1(JL)>sample5(GD). In the stable phase of iron reduction, the mean reducing rates were no notable differences in all samples, but sample5(GD), and the higher reducing rate in sample5(GD) maybe the result of a higher content of Fe(III) oxides in it.
3. The differences in different soil samples and different soil microaggregate were mainly determined by Fe(III) oxides forms, organic matter microbial groups and activities. The degree of iron reduction in different sized aggregates of all but GD paddy soils followed the similar order: (<0.001mm aggregates)>0.001～0.05mm aggregates)>0.05～0.25mm) aggregates. Iron reduction in the aggregates with the size of less than 0.001mm and 0.05 to 0.25mm in GD soil sample were limited by the availability of organic matter.
4. The microbial iron reduction in the flooding soil were limited by the availability of electron donor as well as the electron acceptor. Iron reduction were notable stimulated by the addition of organic acid. Glucose showed a more significant stimulation with the addition of Fe(III) oxides. In the organic exhausted paddy soils, addition of acetate and propaniate stimulate the iron reduction in the beginning period but not in the stable period compared to
水稻土中氧化铁的还原程度受土壤中不同电子供体和受体的制约。通过添加有机物，一方面可以增加电子供体数量，同时也改变土壤中氧化铁的络合与溶解作用能力。利用这种电子竞争的特征，可以作为消除或减少土壤污染物的有效途径。
本文选用铁的氧化还原周期性发生的水稻土为材料，采用室内淹水密闭恒温培养的方法研究了不同土壤以及不同土壤的不同微团聚体中铁还原特征，通过在不同的培养时间添加醋酸盐、丙酸盐和葡萄糖3种有机物作为电子受体对原土和耗竭有机质后的土壤中铁还原的影响的研究，比较来源于不同水稻土的微生物在异化铁还原过程中对乙酸盐、丙酸盐、葡萄糖利用能力的差异，为更深入地研究该过程及其环境意义提供科学依据。五种水稻土样分别采自吉林、湖南、四川、江西和广东等省区。实验获得以下主要结果：
1. 不同水稻土中Fe(II)生成的平衡浓度是不同水稻土的重要特征，其数量与土壤中微生物的种类、易还原氧化铁的数量、其它电子受体的种类和数量、电子供体的数量有关。铁还原反应趋于稳定时所产生的Fe(II)的浓度各不相同，大小顺序是：土样1(JL)>土样3(SC)>土样5(GD)>土样4(JX)。
2. 不同土壤及不同反应阶段的铁还原速率有着明显的区别。土样1(JL)和土样3(SC)没有测出明显的启动期，这与培养温度(30℃)较高有关。江西水稻土和广东水稻土中微生物繁殖具有明显的启动时间。在铁还原反应快速增加阶段，表观平均还原速率大小为：土样3(SC)>土样4(JX)>土样1(JL)>土样5(GD)。在铁还原稳定期，除土样5(GD)以外，其它土壤的平均反应速率差别不大。土样5(GD)的反应速率较大由其土壤中富含氧化铁所致。
3. 不同土壤及不同团聚体中铁还原差异主要是由不同组分中氧化铁的化学形态及有机质含量，微生物数量及其活性决定。对不同大小的微团聚体来说，除广东的水稻土外，不同大小的微团聚体之间的铁还原程度都表现为：（<0.001mm的微团聚体）>?.001～0.05 mm的微团聚体）>?.05～0.25mm的微团聚体）；对于广东水稻土，其<0.001mm和0.05～0.25mm的微团聚体中的有机质数量可能是限制铁还原的关键因素。
4. 淹水土壤中的微生物还原铁的过程同时受到电子供体及电子受体的限制，添加不同有机酸，明显促进了铁的还原。在添加氧化铁处理中，葡萄糖对铁还原的促进作用更为明显。在有机质耗竭的水稻土中，添加乙酸盐(+Ac－)及丙酸盐(Prop)处理对土壤中氧化铁的还原在培养前期有一定的促进作用，但后期的Fe(II)量与对照(CK)比较并无明显的差异，仅在土样3(SC)中添加葡萄糖处理(+Glu)的Fe(II)量与对照(CK)比较有所增大。然而，对添加了易还原氧化铁(+Fe)处理，添加葡萄糖、乙酸盐及丙酸盐均明显增加了Fe(II)的产生量，影响程度表现为：(+Fe+Glu)处理>(+Fe+Ac－-)处理>(+Fe+Prop)处理>(CK+Fe)处理。当土壤中易还原氧化铁过量时，有机物缺乏或许成为主要限制因素，此时添加有机物可提供足够的电子供体，有效地促进了氧化铁的还原。
5. 添加外源有机物可以有效地促进氧化铁的微生物还原过程。从铁的还原量比较，土壤中易还原铁的总量大体为9.23 mg/g(JX)和12.06 mg/g(SC)。添加葡萄糖(+Fe+Glu)处理，两种土壤的铁还原量可达9.910和9.925 mg/g(JX)及12.67和14.55 mg/g(SC)，表明添加的氧化铁已被充分的还原。在不加有机物的对照(CK+Fe)处理中，Fe(II)还原量分别为4.875和5.135 mg/g(JX)及7.855和9.295 mg/g(SC)，添加的氧化铁在先添加有机物试验中的还原率为17.28%和19.23%，而在培养过程中添加有机物试验的氧化铁还原率为20.79%和47.28%；添加乙酸盐(+Fe+Ac－)处理的外源铁还原效率分别为73.05%和82.97%(JX)及94.04%和91.82%(SC)。
Ferric oxide is the most abundant metal oxide, and it is very important in oxidization- reduction of soil and in soil-shaped process. Inundation is an in important factor in accelerating the invert of ferric oxide conformation. After inundation, microbe can use outside Fe(Ⅲ) as its electron acceptor, oxygenation its matrix(electron donor), thereby Fe(Ⅲ) deoxidize to Fe(Ⅱ).This process go by the name of dissimilatory reduction. It can affect availability of nutrients such as N、P、K and Si in the soil directly, and it is important to degradation of organic pollutant, Iron reduction is likely to a new available approach of soil decontamination. Therefore, the process is turned into a hotspot issue of soil environmental chemistry that studied the significance of dissimilatory reduction.
The degree of iron reduction is restrained by the different electron acceptor and provider in the paddy slurry. Through adding organic matter, one way can increase the quantity of electron, at the same time, another way can change the ability of iron combination and dissolution. Making use of the characteristic of electron competition, as a valid way, may remove or reduce soil contamination.
In this study, the soil samples were used in which red-oxy-reaction periodically occurred. The characteristics of iron reduction in different soil samples and different sized aggregates were investigated by flooding incubation in sealed vials at fixed temperature under airtight condition. We also investigated the differences of iron reduction in intact soil and organic exhausted paddy soil sample by adding acetate, propaniate and glucoses as electron donors and the differences of acetate, propaniate and glucose utilities in the dissimilatory iron reduction by microorganism from different soil samples, providing some scientific data and suggestion in dissimilatory iron reduction and its related environmental effects. The five paddy soil samples were collected from JiLin, HuNan, SiChuan, JiangXi, GuangDong.
The main results in this study were showed as the following:
1. The equilibrium concentrations of accumulative Fe(II) were differed from these soil samples, which were correlated with microorganism groups, labile iron oxidizes, other electron acceptors and electron donor spices. The accumulative Fe(II) in stable phase were different in these soil samples and followed the order: sample 1 (JL)> sample 3 (SC)>sample 5 (GD)> sample 4 (JX).
2. Iron reducing rates were distinct in different phase of these soils. No obvious initial phase were found in sample(JL) and sample(SC), maybe for the reasons of higher incubation
temperature(30℃). Microbial activities in JX and GD paddy soil samples showed an apparent initial phase. In the rapid reducing phase, the observed mean reducing rates were in the order of sample3(SC)>sample4(JX)>sample1(JL)>sample5(GD). In the stable phase of iron reduction, the mean reducing rates were no notable differences in all samples, but sample5(GD), and the higher reducing rate in sample5(GD) maybe the result of a higher content of Fe(III) oxides in it.
3. The differences in different soil samples and different soil microaggregate were mainly determined by Fe(III) oxides forms, organic matter microbial groups and activities. The degree of iron reduction in different sized aggregates of all but GD paddy soils followed the similar order: (<0.001mm aggregates)>0.001～0.05mm aggregates)>0.05～0.25mm) aggregates. Iron reduction in the aggregates with the size of less than 0.001mm and 0.05 to 0.25mm in GD soil sample were limited by the availability of organic matter.
4. The microbial iron reduction in the flooding soil were limited by the availability of electron donor as well as the electron acceptor. Iron reduction were notable stimulated by the addition of organic acid. Glucose showed a more significant stimulation with the addition of Fe(III) oxides. In the organic exhausted paddy soils, addition of acetate and propaniate stimulate the iron reduction in the beginning period but not in the stable period compared to
引文
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