苏打盐碱土氟分布及铝氟互作效应研究
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摘要
种稻已经成为苏打盐碱土改良利用的主要方式之一,硫酸铝作为改良剂在改良盐碱土种稻方面已取得了较好的效果,但是铝在降低土壤pH、改善土壤物理性状的同时,是否会对土壤中的氟产生影响还不清楚。为了探讨铝的添入对土壤中氟的影响,本研究以苏打盐碱土为供试土壤,在对电极法测定氟含量进行优化的基础上,重点研究了氟在苏打盐碱土中的含量、吸附和解吸、铝对苏打盐碱土中氟的形态、吸附以及水稻吸氟规律的影响。从新的角度来研究该区的氟危害,为降低氟的生物有效性、控制氟进入食物链提供理论支持。得到的主要结论如下：
1、在用电极法测定氟含量时,由Na3C6H5O7?2h2O、NaNO3、C6H8O7组成的总离子强度缓冲溶液,能够掩蔽共存铝离子的干扰、稳定氟离子的活度、缓冲待测溶液pH,测量结果的准确度和精确度均较高;已知添加法为最优的测量模式；碱熔法是测量植株中氟含量时较为理想的前处理方法。
2、吉林省西部苏打盐碱土表层土壤中的全氟含量并不高,低于对照黑土和全国土壤的氟背景值,但是其水溶态氟和交换态氟含量普遍较高,氟的生物有效性高,这也是当地地方性氟病流行的原因所在。土壤剖面中,由于采样期间土壤水分上移,带动氟向地表聚集,致使表层土壤(0-20cm)中的水溶态氟、交换态氟、全氟含量高于中间层(20-40cm),但是由于底层(40-60cm)土壤受自然和人为因素的影响较小,氟活化的程度较低,所以全氟含量较其它土层高。各形态氟的分布规律为残余态>水溶态>铁锰结合态、交换态>有机束缚态。交换态氟与其它形态氟的相关性显著,是氟相互转化的中间过渡形式。部分地表水和井水中的氟含量超过国家规定的农田灌溉水标准和饮用水标准。
3、随着初始氟浓度的增加,苏打盐碱土对氟的吸附量和解吸量都是增加到一定程度后趋于不变,而解吸率则呈先降低后升高的趋势,最小解吸率为62.79%。Langmuir方程能较好的拟合苏打盐碱土对氟的等温吸附过程。吸附平衡时间为48h,第1h内有近50%的氟完成了吸附,而这部分氟又极易被解吸下来。双常数方程能够较好的拟合苏打盐碱土对氟的吸附动态,且与初始氟浓度无关。pH越低,氟的吸附量越大、解吸率越小。铝可以缩短氟吸附的平衡时间,增加吸附量、降低解吸率,这与聚合羟基铝-蒙脱石复合体的形成有关。随着阴离子浓度的增加,氟的吸附量先降低后增加,但是解吸率却高于相应的单施氟处理。当阴离子-氟-铝共存时,与相应的阴离子-氟共存处理相比,氟的吸附量均有不同程度的增加,而解吸率却相应下降,与相应的铝-氟共存处理相比,解吸率却偏高,H2PO4-处理的氟吸附量和解吸量均高于其它的阴离子处理。
4、与不施铝处理相比,施铝处理能够降低氟在土壤中的淋失率,但是铝氟相对含量不同,降低的程度有所差别,这可能与施入硫酸铝以后苏打盐碱土中pH变化、铝氧化物／氢氧化物数量变化、土壤胶体带电性变化及土壤自身由于氟的吸附而产生的铝释放有关。因为吸附试验中的1:1铝氟摩尔比处理的吸附量最大、解吸率最低,所以在淋洗试验中,该处理表现出总淋失率最低的特点。
5、生物试验表明,低浓度氟能促进株高、茎叶和根的干重,高浓度则抑制,但对分蘖数和籽粒干重则始终表现为抑制作用。水稻体内的氟含量随着施氟量的增加而增加,成熟期各部位的氟浓度为稻壳>糙米>根>茎叶。随着硫酸铝用量的增加,水稻植株各部位的氟浓度呈先降低后升高的趋势,适量的铝氟比能够降低水稻体内的氟含量,但是不能改变其在各部位的分配规律。土壤中的各形态氟随着初始氟浓度的增加而增加,加入铝以后,自由态氟和水溶态氟含量随着铝添加量的增加而降低,均低于空白处理,残余态氟呈增加趋势,其余形态氟则呈先升高后降低的变化趋势。本研究得到的最佳施铝量为0.4%-0.6%,相当于铝氟的摩尔比为1:1.9-1:8.5左右,此时水稻植株各部位的氟浓度,相应土壤中的水溶态和可交换态氟含量均较低,而铁锰结合态和有机束缚态氟含量较高,并且与空白处理相比土壤对氟的吸附量较大、解吸率较小,所以该铝氟比能够减少氟向地下水的迁移,降低水稻体内的氟含量,进而可以降低人畜通过食物链而摄入的氟量。
Planting rice has been main method of improving soda saline-alkali soil. As amendment, Al2(SO4)3has performed better effect on amending the soil to plant rice.But it is not clear that wether Al can influence fluorine in the soil,though it can decrease pH and improve soil physical properties. In order to study the effect of Al applied on the fluorine in soil, the paper took soda saline-alkali soil as experimental soil, on the basis of optimizing fluorine measurement method by electrode, mainly studied the distribution characteristics of fluorine in soda saline-alkali soil, fluorine adsorption/desorption, the effect of Al on fluorine forms and adsorption in soil and the regularities of rice absorbing fluorine. The paper researched fluorine harm from a new angle and provided theoretical support for reducing fluoride bioavailability, controlling of fluorine into the food chain. The main conclusions are as follows:
1、When electrode method was used to measure the content fluorine in solution, TISAB consisted of Na3C6H5O7?2H2O、NaNO3、C6H8O7could shelter Al interference, stabilize ion activity of F, adjust pH to suitable range with higher accuracy. The best measure mode was the known addition method. And alkali fusion was better pretreatment method for measurement fluorine content in plant tissue.
2、The results of investigation fluorine content in soda saline-alkali soil and water of west Jilin province were that the total fluorine in topsoil was not high and was less than black soil and national fluorine background level in soil, but its content of water soluble and exchangeable fluorine was higher which had high bioavailability and was the reason of endemic fluorosis prevalent in the local. In the soil profile, the content of water soluble、exchangeable、total fluorine in topsoil(0-20cm) were higher than interlayer(20-40cm) because of fluorine aggregating to ground with soil water lifting during sampling period, but total fluorine content in bottom layer(40-60cm) was higher than other soil layers as fluorine was activated lighter by less influence of natural and artificial factors. The distribution of fluorine in soda saline-alkali soil was residual F>water soluble F>Fe/Mn binding F, exchangeable F>organic binding F. The correlation between exchangeable F and other forms F was significantly, so it took bridge function in the transfer of F forms in soil. Fluorine in several ground water and well water exceeded the national standard of drinking water or irrigation water.
3、The experiment of fluorine adsorption in soda saline-alkali soil showed that fluorine adsorption and desorption amount in the soil was increased with initial fluorine content increasing and then not change when it reached maximum, but the desorption rate was in trend of decreasing first and then increasing with minimum of62.79%. Langmuir faction fitted the process of F isothermal adsorption in the soil better. From the adsorption dynamics, adsorbed equilibrium time was48hours, and half of adsorbed fluorine was adsorbed in the first hour with95%-97%being desorbed. Dual constant equation could better fit the process of fluorine adsorbed without the influence of initial fluorine content. pH affected soda saline-alkali soil adsorbing fluorine, the lower the pH, the more the fluorine adsorption amount and the less desorption rate. Al shortened fluorine adsorbed equilibrium time, fluorine adsorption amount was increasing and desorption rate was decreasing with Al added improving. As anions content increasing, fluorine adsorption amount was first decreased and then increased, its desorption rate was higher than single fluorine added. When anions-fluorine-Al coexist in the solution, fluorine adsorption amount was more and desorption rate was less compared with anions-fluorine coexist, desorption rate was higher compared with Al-fluorine coexist. Amount of fluorine adsorption and desorption in H2PO4-treatments was higher than other anions.
4、In the leaching experiment, the treatments of Al added could decrease fluorine leaching rate in soil compared with no Al added treatments. But its depressed degree was different according to the relative content of Al and F with the results of pH change in soil after Al2(SO4)3applied, the change of Aluminum oxide/hydroxide amount, the charge of Soil colloid and Al releasing by fluorine adsorption. The total fluorine leaching rate was lowest in the1:ltreatment because its adsorption amount was highest and desorption rate was lowest.
5、Pot experiment showed that the low concentration of fluorine could promote plant height、stem and leaf、root growing, but the high fluorine concentration played inhibiting role. Fluorine inhibited tiller number and grain dry weight throughout. The order of fluorine content in each part of mature rice was husk>brown rice>root>stem and leaf. As Al2(SO4)3applied increasing, the fluorine content in rice plant decreased first and then increased. Thus, suitable ratio of Al and F might lower fluorine content in rice plant, but it did not change the distribution regulation in each part. Each form of fluorine in soil was increased with initial fluorine content increasing. When Al was added, free fluorine and water soluble fluorine was less than blank control and decreased with Al2(SO4)3applied increasing, residual fluorine increased, other forms of fluorine was in the trend of increasing first and then decreasing. The suitable Al2(SO4)3applied amount in this experiment was0.4%-0.6%which was equivalent to1:1.9-1:8.5of Al and F mole ratio. On this condition, fluorine in each rice plant part and water soluble/exchangeable fluorine in soil was relative low, Fe/Mn and organic binding fluorine was relative high. Although fluorine adsorption amount was not the highest and it desorption rate was not the least, fluorine adsorption amount was higher and desorption rate was lower than blank control. Thus, this ratio of Al to F inhibited fluorine migration to ground water and decreased fluorine in rice plant which reduced fluorine intake amount for animals and human through the food chain.
1、在用电极法测定氟含量时,由Na3C6H5O7?2h2O、NaNO3、C6H8O7组成的总离子强度缓冲溶液,能够掩蔽共存铝离子的干扰、稳定氟离子的活度、缓冲待测溶液pH,测量结果的准确度和精确度均较高;已知添加法为最优的测量模式；碱熔法是测量植株中氟含量时较为理想的前处理方法。
2、吉林省西部苏打盐碱土表层土壤中的全氟含量并不高,低于对照黑土和全国土壤的氟背景值,但是其水溶态氟和交换态氟含量普遍较高,氟的生物有效性高,这也是当地地方性氟病流行的原因所在。土壤剖面中,由于采样期间土壤水分上移,带动氟向地表聚集,致使表层土壤(0-20cm)中的水溶态氟、交换态氟、全氟含量高于中间层(20-40cm),但是由于底层(40-60cm)土壤受自然和人为因素的影响较小,氟活化的程度较低,所以全氟含量较其它土层高。各形态氟的分布规律为残余态>水溶态>铁锰结合态、交换态>有机束缚态。交换态氟与其它形态氟的相关性显著,是氟相互转化的中间过渡形式。部分地表水和井水中的氟含量超过国家规定的农田灌溉水标准和饮用水标准。
3、随着初始氟浓度的增加,苏打盐碱土对氟的吸附量和解吸量都是增加到一定程度后趋于不变,而解吸率则呈先降低后升高的趋势,最小解吸率为62.79%。Langmuir方程能较好的拟合苏打盐碱土对氟的等温吸附过程。吸附平衡时间为48h,第1h内有近50%的氟完成了吸附,而这部分氟又极易被解吸下来。双常数方程能够较好的拟合苏打盐碱土对氟的吸附动态,且与初始氟浓度无关。pH越低,氟的吸附量越大、解吸率越小。铝可以缩短氟吸附的平衡时间,增加吸附量、降低解吸率,这与聚合羟基铝-蒙脱石复合体的形成有关。随着阴离子浓度的增加,氟的吸附量先降低后增加,但是解吸率却高于相应的单施氟处理。当阴离子-氟-铝共存时,与相应的阴离子-氟共存处理相比,氟的吸附量均有不同程度的增加,而解吸率却相应下降,与相应的铝-氟共存处理相比,解吸率却偏高,H2PO4-处理的氟吸附量和解吸量均高于其它的阴离子处理。
4、与不施铝处理相比,施铝处理能够降低氟在土壤中的淋失率,但是铝氟相对含量不同,降低的程度有所差别,这可能与施入硫酸铝以后苏打盐碱土中pH变化、铝氧化物／氢氧化物数量变化、土壤胶体带电性变化及土壤自身由于氟的吸附而产生的铝释放有关。因为吸附试验中的1:1铝氟摩尔比处理的吸附量最大、解吸率最低,所以在淋洗试验中,该处理表现出总淋失率最低的特点。
5、生物试验表明,低浓度氟能促进株高、茎叶和根的干重,高浓度则抑制,但对分蘖数和籽粒干重则始终表现为抑制作用。水稻体内的氟含量随着施氟量的增加而增加,成熟期各部位的氟浓度为稻壳>糙米>根>茎叶。随着硫酸铝用量的增加,水稻植株各部位的氟浓度呈先降低后升高的趋势,适量的铝氟比能够降低水稻体内的氟含量,但是不能改变其在各部位的分配规律。土壤中的各形态氟随着初始氟浓度的增加而增加,加入铝以后,自由态氟和水溶态氟含量随着铝添加量的增加而降低,均低于空白处理,残余态氟呈增加趋势,其余形态氟则呈先升高后降低的变化趋势。本研究得到的最佳施铝量为0.4%-0.6%,相当于铝氟的摩尔比为1:1.9-1:8.5左右,此时水稻植株各部位的氟浓度,相应土壤中的水溶态和可交换态氟含量均较低,而铁锰结合态和有机束缚态氟含量较高,并且与空白处理相比土壤对氟的吸附量较大、解吸率较小,所以该铝氟比能够减少氟向地下水的迁移,降低水稻体内的氟含量,进而可以降低人畜通过食物链而摄入的氟量。
Planting rice has been main method of improving soda saline-alkali soil. As amendment, Al2(SO4)3has performed better effect on amending the soil to plant rice.But it is not clear that wether Al can influence fluorine in the soil,though it can decrease pH and improve soil physical properties. In order to study the effect of Al applied on the fluorine in soil, the paper took soda saline-alkali soil as experimental soil, on the basis of optimizing fluorine measurement method by electrode, mainly studied the distribution characteristics of fluorine in soda saline-alkali soil, fluorine adsorption/desorption, the effect of Al on fluorine forms and adsorption in soil and the regularities of rice absorbing fluorine. The paper researched fluorine harm from a new angle and provided theoretical support for reducing fluoride bioavailability, controlling of fluorine into the food chain. The main conclusions are as follows:
1、When electrode method was used to measure the content fluorine in solution, TISAB consisted of Na3C6H5O7?2H2O、NaNO3、C6H8O7could shelter Al interference, stabilize ion activity of F, adjust pH to suitable range with higher accuracy. The best measure mode was the known addition method. And alkali fusion was better pretreatment method for measurement fluorine content in plant tissue.
2、The results of investigation fluorine content in soda saline-alkali soil and water of west Jilin province were that the total fluorine in topsoil was not high and was less than black soil and national fluorine background level in soil, but its content of water soluble and exchangeable fluorine was higher which had high bioavailability and was the reason of endemic fluorosis prevalent in the local. In the soil profile, the content of water soluble、exchangeable、total fluorine in topsoil(0-20cm) were higher than interlayer(20-40cm) because of fluorine aggregating to ground with soil water lifting during sampling period, but total fluorine content in bottom layer(40-60cm) was higher than other soil layers as fluorine was activated lighter by less influence of natural and artificial factors. The distribution of fluorine in soda saline-alkali soil was residual F>water soluble F>Fe/Mn binding F, exchangeable F>organic binding F. The correlation between exchangeable F and other forms F was significantly, so it took bridge function in the transfer of F forms in soil. Fluorine in several ground water and well water exceeded the national standard of drinking water or irrigation water.
3、The experiment of fluorine adsorption in soda saline-alkali soil showed that fluorine adsorption and desorption amount in the soil was increased with initial fluorine content increasing and then not change when it reached maximum, but the desorption rate was in trend of decreasing first and then increasing with minimum of62.79%. Langmuir faction fitted the process of F isothermal adsorption in the soil better. From the adsorption dynamics, adsorbed equilibrium time was48hours, and half of adsorbed fluorine was adsorbed in the first hour with95%-97%being desorbed. Dual constant equation could better fit the process of fluorine adsorbed without the influence of initial fluorine content. pH affected soda saline-alkali soil adsorbing fluorine, the lower the pH, the more the fluorine adsorption amount and the less desorption rate. Al shortened fluorine adsorbed equilibrium time, fluorine adsorption amount was increasing and desorption rate was decreasing with Al added improving. As anions content increasing, fluorine adsorption amount was first decreased and then increased, its desorption rate was higher than single fluorine added. When anions-fluorine-Al coexist in the solution, fluorine adsorption amount was more and desorption rate was less compared with anions-fluorine coexist, desorption rate was higher compared with Al-fluorine coexist. Amount of fluorine adsorption and desorption in H2PO4-treatments was higher than other anions.
4、In the leaching experiment, the treatments of Al added could decrease fluorine leaching rate in soil compared with no Al added treatments. But its depressed degree was different according to the relative content of Al and F with the results of pH change in soil after Al2(SO4)3applied, the change of Aluminum oxide/hydroxide amount, the charge of Soil colloid and Al releasing by fluorine adsorption. The total fluorine leaching rate was lowest in the1:ltreatment because its adsorption amount was highest and desorption rate was lowest.
5、Pot experiment showed that the low concentration of fluorine could promote plant height、stem and leaf、root growing, but the high fluorine concentration played inhibiting role. Fluorine inhibited tiller number and grain dry weight throughout. The order of fluorine content in each part of mature rice was husk>brown rice>root>stem and leaf. As Al2(SO4)3applied increasing, the fluorine content in rice plant decreased first and then increased. Thus, suitable ratio of Al and F might lower fluorine content in rice plant, but it did not change the distribution regulation in each part. Each form of fluorine in soil was increased with initial fluorine content increasing. When Al was added, free fluorine and water soluble fluorine was less than blank control and decreased with Al2(SO4)3applied increasing, residual fluorine increased, other forms of fluorine was in the trend of increasing first and then decreasing. The suitable Al2(SO4)3applied amount in this experiment was0.4%-0.6%which was equivalent to1:1.9-1:8.5of Al and F mole ratio. On this condition, fluorine in each rice plant part and water soluble/exchangeable fluorine in soil was relative low, Fe/Mn and organic binding fluorine was relative high. Although fluorine adsorption amount was not the highest and it desorption rate was not the least, fluorine adsorption amount was higher and desorption rate was lower than blank control. Thus, this ratio of Al to F inhibited fluorine migration to ground water and decreased fluorine in rice plant which reduced fluorine intake amount for animals and human through the food chain.
引文
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