农田土壤水分散性胶体磷的赋存形态、活化机制及阻控技术研究
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摘要
土壤胶体以巨大的比表面积,强大的吸附性能及多样的表面官能团,在污染物赋存形态、迁移转化等生物地球化学循环过程中起到重要作用。胶体易化磷素运移已成为农业面源磷污染的重要发生形式,土壤胶体磷在土-水界面的活化是胶体易化磷素运移的前提。本研究以土壤胶体磷为核心,以东苕溪流域为例调查了典型河段水体磷素粒径分布特征及东苕溪代表性流域(漕桥溪小流域)不同土地利用类型农田土壤胶体磷的流失潜能及其与土体土壤不同活性磷组分的关系；在此基础上筛选当地典型的菜地和稻田土壤深入表征土壤胶体磷及土体土壤磷分子形态,阐明了土壤胶体磷及土体土壤磷分子形态的差异；同时结合浙江省农田土壤酸化的实际环境问题,进一步探究pH变化对土壤胶体磷流失潜能的影响机制；最后还探讨了聚丙烯酰胺(PAM)对土壤胶体磷流失潜能的阻控效果。本研究可丰富当前在农田土壤磷赋存形态、流失机制及阻控技术方面的研究成果,具体结果如下：
1)东苕溪典型河段水体磷素粒径组成以颗粒态磷为主(0.020-0.492mg L-),真溶解态磷次之(0.034-0.109mg L-1),胶体磷含量最少(0-0.025mg L-I),颗粒态磷是东苕溪向太湖输送的主要磷形态；从东苕溪上游到下游,颗粒态总磷和颗粒态钼蓝反应磷(MRP)含量激增,真溶解态总磷及真溶解态MRP下降,而胶体磷及胶体MRP含量在全流域保持相对稳定；MRP在胶体上的分配系数随胶体浓度升高而降低,表现出胶体的颗粒浓度效应；以上大流域尺度的研究结果符合“胶体泵”理论,推测在磷素从真溶解态向大颗粒态运移的动态过程中,胶体作为中间介质可能起到维稳缓冲作用,其在水体磷素粒径分布中的作用不容忽视。
2)在漕桥溪小流域不同土地利用类型农田(稻田、茶园、菜地、苗木和竹林)中,胶体磷的流失潜能以菜地和竹林土壤最大,稻田和苗木次之,茶园最小；除茶园土壤外,胶体磷均是总磷(<1μm)流失的主要形态(55.1-80.9%),流失风险不容忽视。供试不同利用类型农田中土壤胶体磷均以MRP为主(59.6-96.8%)；供试土壤磷库中不同活性磷组分的分布特征各异,所有供试土壤中均以中等活性的氢氧化钠提取态磷为主(41-53%),稻田、菜地、竹林土壤中第二大磷组分为活性的水提取态磷及碳酸氢钠提取态磷,而茶园及苗木土壤中第二大磷组分为非活性的盐酸提取态磷和残留磷；土壤胶体MRP的流失潜能分别与土壤水提取态磷、碳酸氢钠提取态无机磷、氢氧化钠提取态总磷三种组分含量极显著正相关,与氢氧化钠提取态无机磷和盐酸提取态磷组分的含量显著正相关,而胶体钼蓝非反应磷(MUP)的流失潜能与土壤不同磷组分含量之间无显著相关性。
3)选择漕桥溪小流域典型的稻田和菜地土壤,以X射线吸收近边结构(XANES)及磷-31核磁共振(P-NMR)光谱技术深入表征土壤胶体磷及土体土壤磷的分子形态,结果表明铁氧化物结合态磷是两种供试土壤胶体磷(61.1-70.4%)和土体土壤磷(64.6-65.3%)的主要形态,揭示了土壤胶体MRP的流失潜能与土壤氢氧化钠提取态无机磷组分含量显著正相关的内在原因；与土体土壤相比,羟基磷灰石在两种供试土壤胶体中的比例显著升高,活性钙磷比例下降,并且稻田土壤胶体中铝氧化物结合态磷较土体土壤中升高,而正磷酸二酯与正磷酸单酯比值降低,表明土壤胶体较土体土壤更易富集稳定性高的磷形态。
4)供试菜地和稻田土壤在pH～3.0时胶体磷释放量均最低,而高pH(～7.0)可显著促发土壤胶体及胶体磷流失,同时伴随胶体zeta电位的逐渐降低,说明静电斥力增加促进了土壤胶体及胶体磷的活化；菜地和稻田土壤中胶体MRP流失潜能98.8%和99.3%的变异性均可由胶体总有机碳的流失潜能加以预测,表明胶体MRP很可能以有机质-金属-磷酸盐(OM-M-MRP)的三元复合物存在；进一步结合磷的K边XANES结果,推测供试土壤胶体MRP在pH～5.0时很可能通过外配层络合作用形成有机质-钙-磷酸盐(OM-Ca-MRP);并在pH调控下发生形态转化,在pH～7.0时主要以铁氧化物结合态磷和羟基磷灰石赋存。
5)PAM可显著抑制供试菜地和稻田土壤胶体及胶体磷的流失潜能,0.1%的PAM为阻控菜地土壤胶体及胶体总磷流失的最佳剂量；而PAM对稻田土壤胶体及胶体总磷流失潜能的抑制效果随PAM施用量增大而增强,0.2%的PAM可分别抑制75.0%和88.1%的土壤胶体和胶体总磷流失。PAM对土壤胶体MRP流失的阻控效果与其对胶体总磷的阻控效果呈相似规律。而PAM施用对真溶解态磷无明显抑制效果,还可能促进真溶解态磷的流失潜能,其影响与供试土壤土地利用类型和PAM的施用量有关。
Soil colloids, with their large specific surface area, high absorption capacity, and abundant surface functional groups, play a vital role in biogeochemical cycles (eg. speciation, transport and transformation) of contaminants. Colloid-facilitated phosphorus (P) transport has been a key mechanism of agricultural non-point source pollution of P, with the premise of colloidal P (Pcoll) mobilization at soil-water interfaces. This study targeting soil Pcoll, investigated size distribution of aquatic P in typical sections of East Tiao River, and Pcoll release potential in soils cultivated with rice (RS), tea (TS), vegetables (VS), nursery stock (NSS), and bamboo (BS) located in representative basin (Caoqiaoxi Basin) of East Tiao River, along with the relationship between Pcoll release potential and P fractions in studied soils. Then locally typical VS and RS samples were selected to further characterize P speciation in soil colloids and bulk soils at the molecular level, and differences of P species in soil colloids and bulk soils were discussed. Considering the studied area is significantly impacted by soil acidification, the release potential of soil Pcoll under different pH conditions and involved mechanism were explored. Finally, efficiency of polyacrylamide (PAM) in controlling release potential of Pcoll was researched. This work should enrich current development on speciation, release mechanism and control of soil P. Detailed results are shown below.
In typical sections of the East Tiao River, results indicated particulate P (0.020-0.492mg L-1) was dominant followed by the truly dissolved P (0.034-0.109mg L-1), while Pcoii (0-0.025mg L-1) was quantitatively the lowest in the whole river. From upstream to downstream, particulate total P (TP) and molybdate reactive P (MRP) increased sharply, along with the decrease of truly dissolved TP and MRP. However, colloidal TP (TPcoll) and colloidal MRP (MRPcoll) remained at a relatively stable level in the whole river. The partition coefficient of MRP in colloidal phase declined as colloidal particles increased, which indicated the particle concentration effect. These observations, in this large-scale field investigation, fitted the "colloidal pumping" hypothesis. It may be concluded that colloids act as the intermediate and buffer in the dynamically balanced transfer of P from truly dissolved phase to large particulate phase, having a significant role in size distribution of aquatic P.
Release potential of Pcoll was highest in VS and BS, followed by RS and NSS, and was lowest in TS. Colloidal P was the major species of the released P (<1μm), ranging from55.1%to80.9%, for all soil samples under various land use except for TS. Colloidal P mainly consisted of MRP (59.6-96.8%) in all studied soils. P fractions with various labilities in soil samples distributed differently. For all samples, the majority of P was found in the moderately labile fraction (NaOH-P,41-53%). The second largest pool for RS, VS and BS was the labile P fraction (NaHCO3-P and H2O-P), but for TS and NSS it was the nonlabile fraction (HC1-P and residual P). Release potential of MRPcoll presented a highly significant correlation with concentration of H2O-P, NaHCO3-P;, and NaOH-Pt, and a significant correlation with NaOH-Pj and HCl-P, while colloidal MUP did not show correlation with any soil P fractions.
Taken RS and VS as examples, molecular speciation of P in soil colloids and bulk soils were further identified by synchrotron-based P K-edge X-ray near edge structure (XANES) and solution P-31nuclear magnetic resonance (P-NMR) spectroscopy. Results showed that P was mainly presented as iron-associated P (Fe-P) in both studied soil colloids (61.1-70.4%) and bulk soils (64.6-65.3%), which explained the significant correlation between release potential of MRPcoll with concentration of soil NaOH-Pj. Increased proportion of hydroxyapatite (HAP) and decreased percentage of soluble calcium-associated P occured in soil colloids as compared to bulk soils. The RS colloids have higher percentage of aluminum-associated P as well as lower ratio of orthophosphate diesters to orthophosphate monoesters than the bulk soil. This indicated stable P species accumulate in soil colloids as compared to bulk soils.
The release potential of Pcoll was rather low at pH～3.0for both VS and RS, while high pH (-7.0) significantly enhanced the release of soil colloids and Pcoll, accompanied with the gradual decrease of zeta potential of colloids, which implied the increased interparticle electrostatic repulsion contributed to the release of soil colloids and Pcoll. Colloidal TOC accounted for98.8%and99.3%of the variation of MRPcoll in VS and RS respectively, which allowed for the hypothesis that MRPcoll was probably presented as organic matter (OM)-metal (M)-phosphate complex. The XANES results strongly suggested that MRPcoll occurred as OM-calcium-MRP at pH-5.0, and transformed to Fe-P and HAP at pH～7.0.
Application of PAM significantly reduced the release potential of colloids and Pcoll in studied VS and RS.0.1%PAM treatment was recommoned to reduce release of colloids and Pcoll in VS. Contrastly, the controlling effect of PAM on the release potential of colloids and Pcoll in RS increased with higher PAM application rate, and0.2%PAM treatment reduced75.0%of colloid release and88.1%of Pcoll release respectively. The controlling effect of PAM on MRPcon showed similar characteristics with that on Pcoll. No significant inhibition but a possible facilitation effect of PAM on truly dissolved P were shown, which related to land use of studied soils and application rate of PAM.
1)东苕溪典型河段水体磷素粒径组成以颗粒态磷为主(0.020-0.492mg L-),真溶解态磷次之(0.034-0.109mg L-1),胶体磷含量最少(0-0.025mg L-I),颗粒态磷是东苕溪向太湖输送的主要磷形态；从东苕溪上游到下游,颗粒态总磷和颗粒态钼蓝反应磷(MRP)含量激增,真溶解态总磷及真溶解态MRP下降,而胶体磷及胶体MRP含量在全流域保持相对稳定；MRP在胶体上的分配系数随胶体浓度升高而降低,表现出胶体的颗粒浓度效应；以上大流域尺度的研究结果符合“胶体泵”理论,推测在磷素从真溶解态向大颗粒态运移的动态过程中,胶体作为中间介质可能起到维稳缓冲作用,其在水体磷素粒径分布中的作用不容忽视。
2)在漕桥溪小流域不同土地利用类型农田(稻田、茶园、菜地、苗木和竹林)中,胶体磷的流失潜能以菜地和竹林土壤最大,稻田和苗木次之,茶园最小；除茶园土壤外,胶体磷均是总磷(<1μm)流失的主要形态(55.1-80.9%),流失风险不容忽视。供试不同利用类型农田中土壤胶体磷均以MRP为主(59.6-96.8%)；供试土壤磷库中不同活性磷组分的分布特征各异,所有供试土壤中均以中等活性的氢氧化钠提取态磷为主(41-53%),稻田、菜地、竹林土壤中第二大磷组分为活性的水提取态磷及碳酸氢钠提取态磷,而茶园及苗木土壤中第二大磷组分为非活性的盐酸提取态磷和残留磷；土壤胶体MRP的流失潜能分别与土壤水提取态磷、碳酸氢钠提取态无机磷、氢氧化钠提取态总磷三种组分含量极显著正相关,与氢氧化钠提取态无机磷和盐酸提取态磷组分的含量显著正相关,而胶体钼蓝非反应磷(MUP)的流失潜能与土壤不同磷组分含量之间无显著相关性。
3)选择漕桥溪小流域典型的稻田和菜地土壤,以X射线吸收近边结构(XANES)及磷-31核磁共振(P-NMR)光谱技术深入表征土壤胶体磷及土体土壤磷的分子形态,结果表明铁氧化物结合态磷是两种供试土壤胶体磷(61.1-70.4%)和土体土壤磷(64.6-65.3%)的主要形态,揭示了土壤胶体MRP的流失潜能与土壤氢氧化钠提取态无机磷组分含量显著正相关的内在原因；与土体土壤相比,羟基磷灰石在两种供试土壤胶体中的比例显著升高,活性钙磷比例下降,并且稻田土壤胶体中铝氧化物结合态磷较土体土壤中升高,而正磷酸二酯与正磷酸单酯比值降低,表明土壤胶体较土体土壤更易富集稳定性高的磷形态。
4)供试菜地和稻田土壤在pH～3.0时胶体磷释放量均最低,而高pH(～7.0)可显著促发土壤胶体及胶体磷流失,同时伴随胶体zeta电位的逐渐降低,说明静电斥力增加促进了土壤胶体及胶体磷的活化；菜地和稻田土壤中胶体MRP流失潜能98.8%和99.3%的变异性均可由胶体总有机碳的流失潜能加以预测,表明胶体MRP很可能以有机质-金属-磷酸盐(OM-M-MRP)的三元复合物存在；进一步结合磷的K边XANES结果,推测供试土壤胶体MRP在pH～5.0时很可能通过外配层络合作用形成有机质-钙-磷酸盐(OM-Ca-MRP);并在pH调控下发生形态转化,在pH～7.0时主要以铁氧化物结合态磷和羟基磷灰石赋存。
5)PAM可显著抑制供试菜地和稻田土壤胶体及胶体磷的流失潜能,0.1%的PAM为阻控菜地土壤胶体及胶体总磷流失的最佳剂量；而PAM对稻田土壤胶体及胶体总磷流失潜能的抑制效果随PAM施用量增大而增强,0.2%的PAM可分别抑制75.0%和88.1%的土壤胶体和胶体总磷流失。PAM对土壤胶体MRP流失的阻控效果与其对胶体总磷的阻控效果呈相似规律。而PAM施用对真溶解态磷无明显抑制效果,还可能促进真溶解态磷的流失潜能,其影响与供试土壤土地利用类型和PAM的施用量有关。
Soil colloids, with their large specific surface area, high absorption capacity, and abundant surface functional groups, play a vital role in biogeochemical cycles (eg. speciation, transport and transformation) of contaminants. Colloid-facilitated phosphorus (P) transport has been a key mechanism of agricultural non-point source pollution of P, with the premise of colloidal P (Pcoll) mobilization at soil-water interfaces. This study targeting soil Pcoll, investigated size distribution of aquatic P in typical sections of East Tiao River, and Pcoll release potential in soils cultivated with rice (RS), tea (TS), vegetables (VS), nursery stock (NSS), and bamboo (BS) located in representative basin (Caoqiaoxi Basin) of East Tiao River, along with the relationship between Pcoll release potential and P fractions in studied soils. Then locally typical VS and RS samples were selected to further characterize P speciation in soil colloids and bulk soils at the molecular level, and differences of P species in soil colloids and bulk soils were discussed. Considering the studied area is significantly impacted by soil acidification, the release potential of soil Pcoll under different pH conditions and involved mechanism were explored. Finally, efficiency of polyacrylamide (PAM) in controlling release potential of Pcoll was researched. This work should enrich current development on speciation, release mechanism and control of soil P. Detailed results are shown below.
In typical sections of the East Tiao River, results indicated particulate P (0.020-0.492mg L-1) was dominant followed by the truly dissolved P (0.034-0.109mg L-1), while Pcoii (0-0.025mg L-1) was quantitatively the lowest in the whole river. From upstream to downstream, particulate total P (TP) and molybdate reactive P (MRP) increased sharply, along with the decrease of truly dissolved TP and MRP. However, colloidal TP (TPcoll) and colloidal MRP (MRPcoll) remained at a relatively stable level in the whole river. The partition coefficient of MRP in colloidal phase declined as colloidal particles increased, which indicated the particle concentration effect. These observations, in this large-scale field investigation, fitted the "colloidal pumping" hypothesis. It may be concluded that colloids act as the intermediate and buffer in the dynamically balanced transfer of P from truly dissolved phase to large particulate phase, having a significant role in size distribution of aquatic P.
Release potential of Pcoll was highest in VS and BS, followed by RS and NSS, and was lowest in TS. Colloidal P was the major species of the released P (<1μm), ranging from55.1%to80.9%, for all soil samples under various land use except for TS. Colloidal P mainly consisted of MRP (59.6-96.8%) in all studied soils. P fractions with various labilities in soil samples distributed differently. For all samples, the majority of P was found in the moderately labile fraction (NaOH-P,41-53%). The second largest pool for RS, VS and BS was the labile P fraction (NaHCO3-P and H2O-P), but for TS and NSS it was the nonlabile fraction (HC1-P and residual P). Release potential of MRPcoll presented a highly significant correlation with concentration of H2O-P, NaHCO3-P;, and NaOH-Pt, and a significant correlation with NaOH-Pj and HCl-P, while colloidal MUP did not show correlation with any soil P fractions.
Taken RS and VS as examples, molecular speciation of P in soil colloids and bulk soils were further identified by synchrotron-based P K-edge X-ray near edge structure (XANES) and solution P-31nuclear magnetic resonance (P-NMR) spectroscopy. Results showed that P was mainly presented as iron-associated P (Fe-P) in both studied soil colloids (61.1-70.4%) and bulk soils (64.6-65.3%), which explained the significant correlation between release potential of MRPcoll with concentration of soil NaOH-Pj. Increased proportion of hydroxyapatite (HAP) and decreased percentage of soluble calcium-associated P occured in soil colloids as compared to bulk soils. The RS colloids have higher percentage of aluminum-associated P as well as lower ratio of orthophosphate diesters to orthophosphate monoesters than the bulk soil. This indicated stable P species accumulate in soil colloids as compared to bulk soils.
The release potential of Pcoll was rather low at pH～3.0for both VS and RS, while high pH (-7.0) significantly enhanced the release of soil colloids and Pcoll, accompanied with the gradual decrease of zeta potential of colloids, which implied the increased interparticle electrostatic repulsion contributed to the release of soil colloids and Pcoll. Colloidal TOC accounted for98.8%and99.3%of the variation of MRPcoll in VS and RS respectively, which allowed for the hypothesis that MRPcoll was probably presented as organic matter (OM)-metal (M)-phosphate complex. The XANES results strongly suggested that MRPcoll occurred as OM-calcium-MRP at pH-5.0, and transformed to Fe-P and HAP at pH～7.0.
Application of PAM significantly reduced the release potential of colloids and Pcoll in studied VS and RS.0.1%PAM treatment was recommoned to reduce release of colloids and Pcoll in VS. Contrastly, the controlling effect of PAM on the release potential of colloids and Pcoll in RS increased with higher PAM application rate, and0.2%PAM treatment reduced75.0%of colloid release and88.1%of Pcoll release respectively. The controlling effect of PAM on MRPcon showed similar characteristics with that on Pcoll. No significant inhibition but a possible facilitation effect of PAM on truly dissolved P were shown, which related to land use of studied soils and application rate of PAM.
引文
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