持续淋溶条件下有机酸对土壤磷素释放的影响及机理研究
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摘要
随着根际微生态系统研究的不断开展，有机酸的生态功能逐渐被人们所关注。模拟植物根系分泌有机酸，并探讨其对植物根际土壤中磷素的活化效果和活化机制，一直是植物营养和土壤化学领域的重要研究课题。虽然国内外已相继开展了一些相关研究，并且取得了一定的进展，但大部分研究结果是在间歇浸提方式下获得的，有关持续淋溶条件下有机酸对土壤磷素的活化过程、特征以及有机酸对土壤磷素迁移转化影响方面的研究仍然极少涉及，存在进一步探讨和拓展的空间。
本文采用土柱淋洗持续淋溶的方法，研究了几种低分子量有机酸在不同条件下对供试土壤中磷素的持续释放特征、淋溶过程中有机酸自身、溶液pH值以及淋出液中Ca、Mg、Fe、Al的变化特征，分析了淋溶结束后土壤磷素的垂直分布情况及各形态磷的变化情况，并以实验室合成磷酸盐为材料，探讨了供试有机酸对五种人工合成磷酸盐的活化效应及活化途径。主要研究结论如下：
1．持续淋溶条件下，不同种类有机酸对单一阳离子饱和状态下土壤磷素的持续活化能力不同。在相同浓度条件下，柠檬酸对土壤磷素的累积活化能力最强；草酸在浓度高时对磷素的活化能力可与柠檬酸相当，而在中、低浓度时则低于柠檬酸和乙酸；乙酸对土壤磷素的活化表现出较强的持续能力。
2．持续淋溶条件下，有机酸浓度对有机酸持续活化土壤磷素的能力也不相同。不论浓度高低，柠檬酸对土壤磷素都表现出很强的的活化能力，草酸只有在高浓度条件下才表现出与柠檬酸相当的磷素活化能力，乙酸各处理则表现为相对低水平的持续活化。Elovich、权函数方程和抛物线扩散方程均可用来拟合有机酸淋溶下土壤磷素的释放过程，根据方程的相关参数a、b得出有机酸各处理中土壤磷素释放的初始瞬时速率大小顺序为：柠檬酸＞草酸＞乙酸，且有机酸对土壤磷的活化率随时间的延长而下降；三种有机酸均能增大土壤磷的相对扩散系数R，促进土壤磷素扩散行为。
3．持续淋溶过程中有机酸所提供的酸度（以氢离子衡量）、有机酸与土壤的作用时间（以淋溶速度衡量）以及微生物的活动均可以对有机酸持续活化土壤磷素能力起到一定程度的影响。较低浓度有机酸持续淋溶条件下，柠檬酸、乙酸所提供的酸度有利于促进磷的释放，酸度的促进作用主要体现在淋溶中、后期，低浓度草酸由于受钙的影响其酸度作用并不显著；高流速持续淋溶条件下，柠檬酸与乙酸对土壤磷的活化量有所增加，而草酸处理未见显著变化；微生物的存在一定程度上减缓了三种有机酸对土壤磷素的持续活化作用，其中对柠檬酸的抑制作用最为明显。
4．持续淋溶作用下，淋出液中各形态有机酸浓度均在不断变化，但最终趋于稳定。淋溶过程中淋出液中溶解态有机酸占总有机酸的比例相应增大，分解态有机酸所占比例减少，吸附态有机酸占总有机酸的比例并无规律性变化。在整个淋溶过程当中，溶解态有机酸在赋存形态中所占比例最大，但它与土壤磷素累积释放量并无显著相关关系，而吸附态和分解态有机酸可以分别与土壤累积释磷量达显著和极显著相关关系。
5．持续淋溶过程中，随着磷素的活化，土壤中的Ca、Mg、Fe、Al也在不断释放。有机酸浓度越高，淋出液中的Ca、Mg、Fe、Al数量越多。就有机酸种类而言，柠檬酸促进各离子释放的能力与柠檬酸活化土壤磷素的能力呈现很好的一致性。草酸对Fe、Al的释放能力总体上优于柠檬酸。
6．有机酸持续淋溶有助于土壤中磷素的下移，且高浓度有机酸可以加速土壤磷的迁移。在各形态磷素组分中，高浓度有机酸淋溶可以显著降低土壤NaOH-Pi和HCl-P的含量，说明高浓度有机酸有利于Fe、Al结合态磷酸盐和稳定性钙磷的释放，但即使是高浓度有机酸也很难活化Residual-P，有机酸持续淋溶对土壤有机磷的影响并无特定规律。
7．五种合成磷酸盐中较易被活化的为Ca_2-P、Ca_8-P，其次为Al-P、Fe-P，Ca_(10)-P最不易活化。低分子量有机酸对合成磷酸盐的活化作用情况受有机酸浓度的影响，高浓度处理条件下有机酸对五种合成磷酸盐的活化能力顺序为草酸≥柠檬酸＞乙酸，中浓度条件下则为柠檬酸≥草酸＞乙酸，低浓度有机酸很难活化各合成磷源。陈化作用可以在一定程度上降低合成磷酸盐的有效性，草酸对合成磷源的活化能力受陈化作用的影响程度要小于柠檬酸和乙酸。
8．柠檬酸对合成磷酸盐中Ca_2-P、Ca_8-P和Al-P的活化机理为质子和有机阴离子的共同作用，对磷酸铁中磷的释放主要源于有机酸根的活化，而对Ca_(10)-P活化则几乎完全依靠质子作用。高分子量的腐殖酸也可以促进五种人工合成磷酸盐中磷素的释放，且对三种钙磷的释放效果较好。
As the continuously development of root micro ecological system, the ecological function of organicacid has been gradually concerns. To simulate plant roots secreting organic acid, and to investigate theactivation and mechanism of organic acid on phosphorus release in plant rhizosphere is still an importantresearch subject of plant nutrition and soil chemistry field. Although some related researches have alreadycarried out both at home and abroad, and made some progress, most of the results were came from themethods of batch experiments. The effect of organic acid on the activation process of P release,characteristics and vertical migration and transformation of soil P under the continuous leaching conditionsis still limited, and so that there is more space for discussing and developing.
In this article, adopted the method of continuous leaching of soil column leaching, studied the effect ofseveral low molecular weight organic acid on constantly release characteristics of soil P in differentconditions, and the variation characteristics of organic acid, the solution pH value and Ca, Mg, Fe, Al in theleachates, analyzed the vertical distribution and the variation of different P fractions after the soft leaching,disscussed the mobilization of five different synthetic phosphate compounds by organic acids and itsactivation pathway. The main research conclusions of this article was shown as follows:
1. In the continuous leaching condition, the continuous activation ability of different kinds of organicacid on soil P in the single saturated cationic state is different. In the condition of same concentration, theaccumulated activation ability of citric acid on soil P is the most powerful; the activation ability of oxalicacid can be quite with citric acid in high concentration, while it is will below citric acid and acetic acid inthe middle and low concentration; continuous activation ability of acetic acid on soil P is stronger.
2. In the continuous leaching condition, the effect of organic acid concentration on continuousactivation ability of organic acid on soil P is not same. No matter high concentration or low concentration,citric acid always show a strong activation ability on soil P, activation ability of oxalic acid be quite withcitric acid only in high concentrations, while activation ability of acetic acid is relatively low in anyconcentration conditions. Elovich, weight function equation and parabolic diffusion equation can fittingrelease process of soil P very well. in the organic acid leaching conditions, the size order of the initialinstantaneous release rate of soil P leaching with each organic acid is: citric acid> oxalic acid> acetic acid,and the activation rate of organic acid on soil P decrease with the extension of time; all the three organicacids can increase the relative diffusion coefficient R of soil phosphorus and all of them promote thediffusion behavior of soil P.
3. In continuous leaching process, acidity provide by organic acid (measured on hydrogen ion), timeof organic acid reacted in soil (measure on leaching speed), and microbial activity can influence continuousactivation ability of organic acid on soil at some degree. In the condition of low concentration organic acidcontinued leaching, acidity a provide by citric acid and acetic acid can promote the release of P, thepromoting function of acidity mainly embodied in the leaching middle and late, role of acidity provide bylow concentration oxalic acid is not significant due to the influence of calcium oxalate; In high velocitycontinued leaching condition, activation quantity of soil P made by citric acid and acetic acid increase, while oxalic acid treatment has not significant change; microbial slow the continuous activation function ofthree organic acid on soil p at certain degree, and its inhibitory on citric acid is most obvious.
4. In continuous leaching function conditions, the concentration of organic acid forms in drench liquidare changing, but eventually be stable. In leaching process, the proportion of solution state organic acid indrench liquid account total organic acid increases accordingly, the proportion of decomposition state reduce,the proportion of sorption state organic acids change irregular. In the whole leaching process, theproportion of dissolve state organic acid is biggest, but between it with accumulation release quantity ofsoil phosphorus no significant correlation, while sorption state and decomposition state organic acid withaccumulation release quantity of soil p is significant and very significant correlation respectively.
5. In continuous leaching process, Ca, Mg, Fe, Al in soil are constantly released with the activation ofsoil P. The higher concentration of organic acid, the more of Ca, Mg, Fe, Al ion pour out. The releaseability promote by citric acid with its activation ability on soil P have very good consistency. Releaseability on Fe, Al of Oxalic acid better than citric acid in general.
6. Organic acid continued leaching can promote phosphorus to move down in soil, and highconcentration organic acid can accelerate the transfer of soil phosphorus. In the form of phosphorus, highconcentration organic acid leaching can significantly reduce the content of NaOH-Pi and HCl-P, and thisshow that high concentration organic acids is beneficial to the release of Fe, Al combination state phosphateand calcium bound phosphorus, but even if high concentration organic acid is also still hard to activate theResidual-P, influence of organic acid continued leaching on soil organic P is no specific order.
7. In Five kinds of synthetic phosphate, Ca_2-P and Ca_8-P is most easily activated, followed by Al-P,Fe-P, and Ca_(10)-P is the most difficult activated. Activation function of low molecular weight organic acidon synthesis phosphate affect by the concentration of organic acid, in high concentration processingconditions, the sequence of activation ability of the five types of synthesis phosphate is oxalic acid≥citricacid> acetic acid; under the middle concentration condition, the sequence is citric acid≥oxalate quartile>acetic acid, but low concentration organic acid is hard to activate the synthetic phosphorus source. Agingfunction can reduce the effectiveness of the synthesis phosphate to certain extent, the effect of agingfunction on activation function of oxalic acid on synthesis of phosphorus source is smaller than effect oncitric acid and acetic acid.
8. The activation mechanism of citric acid on Ca_2-P, Ca_8-P and Al-P in synthesis phosphate is thecommon function of protons and organic anion, the release of phosphorus in iron phosphate mainly comesfrom the activation organic acid radical, and the activation of Ca_(10)-P is almost entirely depends on protonrole. High molecular weight humic acid can also promote the release phosphorus in the five kind syntheticphosphates, and all the three calcium bound phosphate can be well activited by humic acid.
本文采用土柱淋洗持续淋溶的方法，研究了几种低分子量有机酸在不同条件下对供试土壤中磷素的持续释放特征、淋溶过程中有机酸自身、溶液pH值以及淋出液中Ca、Mg、Fe、Al的变化特征，分析了淋溶结束后土壤磷素的垂直分布情况及各形态磷的变化情况，并以实验室合成磷酸盐为材料，探讨了供试有机酸对五种人工合成磷酸盐的活化效应及活化途径。主要研究结论如下：
1．持续淋溶条件下，不同种类有机酸对单一阳离子饱和状态下土壤磷素的持续活化能力不同。在相同浓度条件下，柠檬酸对土壤磷素的累积活化能力最强；草酸在浓度高时对磷素的活化能力可与柠檬酸相当，而在中、低浓度时则低于柠檬酸和乙酸；乙酸对土壤磷素的活化表现出较强的持续能力。
2．持续淋溶条件下，有机酸浓度对有机酸持续活化土壤磷素的能力也不相同。不论浓度高低，柠檬酸对土壤磷素都表现出很强的的活化能力，草酸只有在高浓度条件下才表现出与柠檬酸相当的磷素活化能力，乙酸各处理则表现为相对低水平的持续活化。Elovich、权函数方程和抛物线扩散方程均可用来拟合有机酸淋溶下土壤磷素的释放过程，根据方程的相关参数a、b得出有机酸各处理中土壤磷素释放的初始瞬时速率大小顺序为：柠檬酸＞草酸＞乙酸，且有机酸对土壤磷的活化率随时间的延长而下降；三种有机酸均能增大土壤磷的相对扩散系数R，促进土壤磷素扩散行为。
3．持续淋溶过程中有机酸所提供的酸度（以氢离子衡量）、有机酸与土壤的作用时间（以淋溶速度衡量）以及微生物的活动均可以对有机酸持续活化土壤磷素能力起到一定程度的影响。较低浓度有机酸持续淋溶条件下，柠檬酸、乙酸所提供的酸度有利于促进磷的释放，酸度的促进作用主要体现在淋溶中、后期，低浓度草酸由于受钙的影响其酸度作用并不显著；高流速持续淋溶条件下，柠檬酸与乙酸对土壤磷的活化量有所增加，而草酸处理未见显著变化；微生物的存在一定程度上减缓了三种有机酸对土壤磷素的持续活化作用，其中对柠檬酸的抑制作用最为明显。
4．持续淋溶作用下，淋出液中各形态有机酸浓度均在不断变化，但最终趋于稳定。淋溶过程中淋出液中溶解态有机酸占总有机酸的比例相应增大，分解态有机酸所占比例减少，吸附态有机酸占总有机酸的比例并无规律性变化。在整个淋溶过程当中，溶解态有机酸在赋存形态中所占比例最大，但它与土壤磷素累积释放量并无显著相关关系，而吸附态和分解态有机酸可以分别与土壤累积释磷量达显著和极显著相关关系。
5．持续淋溶过程中，随着磷素的活化，土壤中的Ca、Mg、Fe、Al也在不断释放。有机酸浓度越高，淋出液中的Ca、Mg、Fe、Al数量越多。就有机酸种类而言，柠檬酸促进各离子释放的能力与柠檬酸活化土壤磷素的能力呈现很好的一致性。草酸对Fe、Al的释放能力总体上优于柠檬酸。
6．有机酸持续淋溶有助于土壤中磷素的下移，且高浓度有机酸可以加速土壤磷的迁移。在各形态磷素组分中，高浓度有机酸淋溶可以显著降低土壤NaOH-Pi和HCl-P的含量，说明高浓度有机酸有利于Fe、Al结合态磷酸盐和稳定性钙磷的释放，但即使是高浓度有机酸也很难活化Residual-P，有机酸持续淋溶对土壤有机磷的影响并无特定规律。
7．五种合成磷酸盐中较易被活化的为Ca_2-P、Ca_8-P，其次为Al-P、Fe-P，Ca_(10)-P最不易活化。低分子量有机酸对合成磷酸盐的活化作用情况受有机酸浓度的影响，高浓度处理条件下有机酸对五种合成磷酸盐的活化能力顺序为草酸≥柠檬酸＞乙酸，中浓度条件下则为柠檬酸≥草酸＞乙酸，低浓度有机酸很难活化各合成磷源。陈化作用可以在一定程度上降低合成磷酸盐的有效性，草酸对合成磷源的活化能力受陈化作用的影响程度要小于柠檬酸和乙酸。
8．柠檬酸对合成磷酸盐中Ca_2-P、Ca_8-P和Al-P的活化机理为质子和有机阴离子的共同作用，对磷酸铁中磷的释放主要源于有机酸根的活化，而对Ca_(10)-P活化则几乎完全依靠质子作用。高分子量的腐殖酸也可以促进五种人工合成磷酸盐中磷素的释放，且对三种钙磷的释放效果较好。
As the continuously development of root micro ecological system, the ecological function of organicacid has been gradually concerns. To simulate plant roots secreting organic acid, and to investigate theactivation and mechanism of organic acid on phosphorus release in plant rhizosphere is still an importantresearch subject of plant nutrition and soil chemistry field. Although some related researches have alreadycarried out both at home and abroad, and made some progress, most of the results were came from themethods of batch experiments. The effect of organic acid on the activation process of P release,characteristics and vertical migration and transformation of soil P under the continuous leaching conditionsis still limited, and so that there is more space for discussing and developing.
In this article, adopted the method of continuous leaching of soil column leaching, studied the effect ofseveral low molecular weight organic acid on constantly release characteristics of soil P in differentconditions, and the variation characteristics of organic acid, the solution pH value and Ca, Mg, Fe, Al in theleachates, analyzed the vertical distribution and the variation of different P fractions after the soft leaching,disscussed the mobilization of five different synthetic phosphate compounds by organic acids and itsactivation pathway. The main research conclusions of this article was shown as follows:
1. In the continuous leaching condition, the continuous activation ability of different kinds of organicacid on soil P in the single saturated cationic state is different. In the condition of same concentration, theaccumulated activation ability of citric acid on soil P is the most powerful; the activation ability of oxalicacid can be quite with citric acid in high concentration, while it is will below citric acid and acetic acid inthe middle and low concentration; continuous activation ability of acetic acid on soil P is stronger.
2. In the continuous leaching condition, the effect of organic acid concentration on continuousactivation ability of organic acid on soil P is not same. No matter high concentration or low concentration,citric acid always show a strong activation ability on soil P, activation ability of oxalic acid be quite withcitric acid only in high concentrations, while activation ability of acetic acid is relatively low in anyconcentration conditions. Elovich, weight function equation and parabolic diffusion equation can fittingrelease process of soil P very well. in the organic acid leaching conditions, the size order of the initialinstantaneous release rate of soil P leaching with each organic acid is: citric acid> oxalic acid> acetic acid,and the activation rate of organic acid on soil P decrease with the extension of time; all the three organicacids can increase the relative diffusion coefficient R of soil phosphorus and all of them promote thediffusion behavior of soil P.
3. In continuous leaching process, acidity provide by organic acid (measured on hydrogen ion), timeof organic acid reacted in soil (measure on leaching speed), and microbial activity can influence continuousactivation ability of organic acid on soil at some degree. In the condition of low concentration organic acidcontinued leaching, acidity a provide by citric acid and acetic acid can promote the release of P, thepromoting function of acidity mainly embodied in the leaching middle and late, role of acidity provide bylow concentration oxalic acid is not significant due to the influence of calcium oxalate; In high velocitycontinued leaching condition, activation quantity of soil P made by citric acid and acetic acid increase, while oxalic acid treatment has not significant change; microbial slow the continuous activation function ofthree organic acid on soil p at certain degree, and its inhibitory on citric acid is most obvious.
4. In continuous leaching function conditions, the concentration of organic acid forms in drench liquidare changing, but eventually be stable. In leaching process, the proportion of solution state organic acid indrench liquid account total organic acid increases accordingly, the proportion of decomposition state reduce,the proportion of sorption state organic acids change irregular. In the whole leaching process, theproportion of dissolve state organic acid is biggest, but between it with accumulation release quantity ofsoil phosphorus no significant correlation, while sorption state and decomposition state organic acid withaccumulation release quantity of soil p is significant and very significant correlation respectively.
5. In continuous leaching process, Ca, Mg, Fe, Al in soil are constantly released with the activation ofsoil P. The higher concentration of organic acid, the more of Ca, Mg, Fe, Al ion pour out. The releaseability promote by citric acid with its activation ability on soil P have very good consistency. Releaseability on Fe, Al of Oxalic acid better than citric acid in general.
6. Organic acid continued leaching can promote phosphorus to move down in soil, and highconcentration organic acid can accelerate the transfer of soil phosphorus. In the form of phosphorus, highconcentration organic acid leaching can significantly reduce the content of NaOH-Pi and HCl-P, and thisshow that high concentration organic acids is beneficial to the release of Fe, Al combination state phosphateand calcium bound phosphorus, but even if high concentration organic acid is also still hard to activate theResidual-P, influence of organic acid continued leaching on soil organic P is no specific order.
7. In Five kinds of synthetic phosphate, Ca_2-P and Ca_8-P is most easily activated, followed by Al-P,Fe-P, and Ca_(10)-P is the most difficult activated. Activation function of low molecular weight organic acidon synthesis phosphate affect by the concentration of organic acid, in high concentration processingconditions, the sequence of activation ability of the five types of synthesis phosphate is oxalic acid≥citricacid> acetic acid; under the middle concentration condition, the sequence is citric acid≥oxalate quartile>acetic acid, but low concentration organic acid is hard to activate the synthetic phosphorus source. Agingfunction can reduce the effectiveness of the synthesis phosphate to certain extent, the effect of agingfunction on activation function of oxalic acid on synthesis of phosphorus source is smaller than effect oncitric acid and acetic acid.
8. The activation mechanism of citric acid on Ca_2-P, Ca_8-P and Al-P in synthesis phosphate is thecommon function of protons and organic anion, the release of phosphorus in iron phosphate mainly comesfrom the activation organic acid radical, and the activation of Ca_(10)-P is almost entirely depends on protonrole. High molecular weight humic acid can also promote the release phosphorus in the five kind syntheticphosphates, and all the three calcium bound phosphate can be well activited by humic acid.
引文
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