冻融对土壤镉吸附解吸特性影响机理的研究
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摘要
土壤对重金属镉的吸附与解吸特征,影响着镉在土壤中的行为、在一定程度上决定着它的污染危害大小。土壤对重金属的吸附解吸特征受多种因素影响；前人已经开展了不少这方面的研究。由于冻融能直接影响到土壤中矿物、电荷种类与数量等性质,也能影响到有机物质的数量与形态,故冻融在北方寒冷地区可能是影响土壤镉吸附解吸行为的重要因素。然而,到目前为止关于冻融的影响研究尚少,而冻融影响土壤镉吸附与解吸机理的研究就更少。本文以分布于沈阳地区的棕壤作为供试土壤,采用人工控温的方法对不同水分含量条件下的供试土样做交替冻融处理,测定处理后土样对镉的静态等温吸附-解吸、动态等温吸附-解吸曲线和吸附反应后土壤中镉的赋存形态,再将镉吸附-解吸特征与土壤物理化学性质联系起来做统计分析,探讨了冻融影响土壤镉吸附解吸的机理。冻融温度为-30℃-20℃,冻融分0、1、3、6、9次不等,每次冻和融时间相同、均为24h,供试土壤水分含量分别控制在田间持水量的10%、40%、70%、100%、120%。得到的主要结果如下。
1.冻融次数和含水量使土壤pH、游离氧化铁、无定形氧化铁、氧化铁活化度、比表面积发生明显改变,冻融次数还对土壤CEC、CECP、DOC和颗粒分形维数D产生明显影响；这些土壤理化性质大部分随冻融次数增加呈周期性增减变化,这一现象得到了土壤微结构电镜扫描观察结果和红外光谱图的证实。与含水量及其与冻融次数的交互作用相比,冻融次数对土壤理化性质的影响更为明显。
2.冻融次数和含水量对土壤镉的吸附-解吸特点产生影响。土壤镉的吸附量随着冻融次数的增加先增加后降低,在冻融3次时有最大值,且在本试验范围内冻融后土壤镉的吸附量均较未冻融土壤增加；而含水量为田建持水量70-100%时土壤镉的吸附量较其他含水量处理时要小。冻融次数和冻融次数与土壤含水量的交互作用对土壤镉的吸附量影响极显著,而土壤含水量的影响未达显著水平。本试验中的土壤镉吸附能力较强,平均吸附率达到90.15%,且随着冻融次数的增加先增加后减小。反应过程中的吸附自由能变ΔG<0,且在-30～0kJ·mol-1范围内,故该吸附过程为可自发进行的物理化学吸附。土壤镉的初始吸附速率和平均吸附速率均随着冻融次数的增加先增加后降低,随着土壤含水量的增加先降低后增加。
不同冻融处理土壤镉的解吸存在滞后性,滞后程度随着冻融次数的增加呈先增强后减弱的趋势。冻融影响土壤镉的解吸过程,土壤镉的解吸率随冻融次数呈先减小后增加的变化趋势。初始解吸速率和平均解吸速率均随着冻融次数和土壤含水量的增加先降低后升高。镉解吸反应过程可分为快速、慢速解吸两个阶段,两阶段的解吸速率因土壤冻融次数而异；与两个反应阶段对应的解吸速率、由快速到慢速解吸阶段的转折时间均随着冻融次数的增加呈先降低后升高的趋势。
3.不同冻融处理土壤吸附重金属镉后,土壤中存赋的镉以交换态为主,残渣态次之,碳酸盐结合态和铁锰氧化物结合态含量较少,有机结合态更少。
冻融次数和含水量对交换态镉、碳酸盐结合态镉、铁锰氧化物结合态镉含量的影响均达到显著或极显著水平,冻融次数还与残渣态镉含量关系密切。
供试土壤吸附镉的生物可利用系数和迁移系数均随冻融次数增加呈先增加后降低的趋势变化,这两个系数的平均值分别达到66%和63%。
4.冻融土壤镉的吸附-解吸过程中的吸附容量、滞后系数、快速解吸速率、慢速解吸速率和不同赋存形态镉含量与土壤pH、CE、CECp、DOC、无定形氧化铁、比表面积和分形维数D呈显著或极显著相关关系,而交换态镉则与土壤CECp的大小呈极显著正相关关系。因此,可以认为冻融是通过改变土壤理化性质来实现对土壤镉吸附解吸特性的影响的。统计分析结果表明,pH和CECp主要通过直接作用、CEC通过间接作用增加土壤镉吸附容量,DOC主要是通过直接作用降低土壤镉吸附容量的。
综上所述,冻融处理使土壤经历冻胀-消融过程,导致土壤结构和黏土矿物的破坏、有机物质组分和土壤溶液中物质组成改变,致使土壤pH、CEC、CECp、DOC、无定形氧化铁、比表面积和土壤微团聚体的稳定性发生变化,是造成土壤对镉吸附容量大小、吸附-解吸速率快慢及土壤中镉赋存形态不同的主要原因。不同冻融处理土壤镉吸附解吸特性的变化是多个理化性质综合作用的结果。
The adsorption-desorption characteristics in soil after Cd inputed into the soils influenced the Cd behavior, and detemined the extent of Cd pollution in a way. The adsorption-desorption was affected by many factores, on which many studies have been done.Freeze/thawing may be the important factor influenced the Cd adsorption-desorption in soil in north clod area because that freeze/thawing could affected the mineral,charge type and quantity in the soil directly and also affected the organics quantity and form.However, so far the studied on effect of freeze/thawing were less,and the studied on the mechamism of effect of freeze/thawing on Cd adorption-desorption in soil were more less.In this paper,the brown soils distributing in Shenyang area were collected for tested soils, the soil samples of various water content were treated with various freeze/thawing time by artificial temperature control method. The cadmium static isothermal adsorption-desorption isotherms and kinetics isothermal adsorption-desorption isotherm, the adsorbed Cd fractionation in the soil were assayed, then contected the Cd adsorption-desorption characteristics with the soil physical and chemical properties by statistical analysis, and discussed the the mechamism of effect of freeze/thawing on Cd adorption-desorption in soil.The soil samples were incubated at-30℃and-20℃for24h, respectively. Soil samples of different water content (such as10%,40%,70%,100%and120%of the field capacity) were subsequently refrozen and thawed for0,1,3,6,9cycles. The results were as below:
1. Freeze/thawing time (FTT) and soil water content affected the soil pH, free iron oxide, amorphous iron oxide, iron oxide activation degree, the specific surface significantly, and the FTT also affected CEC, CECp, DOC and the fractal dimension(D)significantly. Most of the soil physical and chemical characteristics were fluctuant change with the FTT, and these phenomena were demonstrated by the SEM pictures of the soil particles and the FTIR spectra when the soil water content equaled to the field capacity. Compared with soil water content and its interaction with FTT, FTT had more obvious effects on soil physical and chemical characteristics.
2. FTT affected the Cd adsorption-desorption in the soil. The Cd adsorption quantity increased firstly and then decreased with the increase of the FTT, the max was at3FTT, and the freeze/thawing improved the Cd adsorption in the soils in the extent of this experiment. The Cd adsorption amount was less when the soil water content was70-100%of the field capacity. The effect of the interaction of the FTT and water content on Cd adsorption quantity in soil was significant, while that of the water content was not. The Cd adsorption ability of tested soils was higher, the mean Cd adsorption ratio reached90.15%increasing firstly and then decreasing with the increase of the FTT. The change in free energy ΔG<0, and ΔG value ranged from-30～0kJ·mol-1,so the adsorption progress belonged to spontaneous physical-chemical adsorption. Initial and average adsorption speed firstly increased and then decreased with the FTT increasing, and appeared adverse change with the water content.
The Cd desorption in soils treated with the different freeze/thawing presented hysteresis quality, and the extent of which firstly enhanced and then receded with the FTT increasing. The Cd desorption rate decreased firstly and then increased with the increase of FTT. Initial and average desorption speed firstly decreased and then increased with the FTT and soil water content increasing.The Cd desorption process in soil can be divided into two sections:fast reaction and slow reaction stage, while the desorption rate of the two reaction stage was different depending on the FTT. The desorption speed of the two reaction stage and the turn time of fast reaction to slow reaction decreased firstly and then increased with the the FTT increasing.
3. The fractionation of the absorbed Cd ordered in:exchangeable from>residual form> bound to carbonates form>bound to Fe-Mn oxides form>bound to organic matter form after adsorbing Cd of soils under various freeze/thawing treatments.
The FTT and the soil water content affected the exchangeable from Cd, Carbonates form Cd, Fe-Mn oxides form Cd significantly, and the FTT also affected the residual Cd significantly.
The availability index (K) and mobility index (M) of the adsorbed Cd in soils increased firstly then decreased with the freezing and thawing frequency increase,and the mean of them were66%and63%respectively.
4.The adsorption capacity, hysteresis coefficient,fast desorption speed, slow desorption speed and the various fractionation of the Cd in soils were connected with the pH, CEC, CECp, DOC, amorphous iron oxide, the specific surface and the fractal dimension significantly at0.05or0.01level during the progress of the Cd adsorption-desorption in freeze/thawed soils, while the exchangeable Cd and CECp were significant positive correlation at0.01level. And the statistical analysis results showed that the facilitation of pH and CECp on kF was produced through the direct action, that of CEC on kF was produced through the indirect action; the inhibition of DOC on kF was produced through direct action.
To sum up, freeze/thawing treatments made soil experience frost heave-ablation process, which lead to soil structure and mainly pure montmorillanite destruct, organic matter component and soil solution components change, caused the soil pH, CEC, CECP, DOC, amorphous iron oxide, specific surface area and D changed, so that caused the change of the soil Cd adsorption quantity,adsorption-desorption speed and the fractionation of the adsorbed Cd in the soil under different freeze/thawing treatments. The change of the Cd adsorption-desorption characteristics of soil under different freeze/thawing treatments was resulted by integrated effects of physical and chemical properties.
1.冻融次数和含水量使土壤pH、游离氧化铁、无定形氧化铁、氧化铁活化度、比表面积发生明显改变,冻融次数还对土壤CEC、CECP、DOC和颗粒分形维数D产生明显影响；这些土壤理化性质大部分随冻融次数增加呈周期性增减变化,这一现象得到了土壤微结构电镜扫描观察结果和红外光谱图的证实。与含水量及其与冻融次数的交互作用相比,冻融次数对土壤理化性质的影响更为明显。
2.冻融次数和含水量对土壤镉的吸附-解吸特点产生影响。土壤镉的吸附量随着冻融次数的增加先增加后降低,在冻融3次时有最大值,且在本试验范围内冻融后土壤镉的吸附量均较未冻融土壤增加；而含水量为田建持水量70-100%时土壤镉的吸附量较其他含水量处理时要小。冻融次数和冻融次数与土壤含水量的交互作用对土壤镉的吸附量影响极显著,而土壤含水量的影响未达显著水平。本试验中的土壤镉吸附能力较强,平均吸附率达到90.15%,且随着冻融次数的增加先增加后减小。反应过程中的吸附自由能变ΔG<0,且在-30～0kJ·mol-1范围内,故该吸附过程为可自发进行的物理化学吸附。土壤镉的初始吸附速率和平均吸附速率均随着冻融次数的增加先增加后降低,随着土壤含水量的增加先降低后增加。
不同冻融处理土壤镉的解吸存在滞后性,滞后程度随着冻融次数的增加呈先增强后减弱的趋势。冻融影响土壤镉的解吸过程,土壤镉的解吸率随冻融次数呈先减小后增加的变化趋势。初始解吸速率和平均解吸速率均随着冻融次数和土壤含水量的增加先降低后升高。镉解吸反应过程可分为快速、慢速解吸两个阶段,两阶段的解吸速率因土壤冻融次数而异；与两个反应阶段对应的解吸速率、由快速到慢速解吸阶段的转折时间均随着冻融次数的增加呈先降低后升高的趋势。
3.不同冻融处理土壤吸附重金属镉后,土壤中存赋的镉以交换态为主,残渣态次之,碳酸盐结合态和铁锰氧化物结合态含量较少,有机结合态更少。
冻融次数和含水量对交换态镉、碳酸盐结合态镉、铁锰氧化物结合态镉含量的影响均达到显著或极显著水平,冻融次数还与残渣态镉含量关系密切。
供试土壤吸附镉的生物可利用系数和迁移系数均随冻融次数增加呈先增加后降低的趋势变化,这两个系数的平均值分别达到66%和63%。
4.冻融土壤镉的吸附-解吸过程中的吸附容量、滞后系数、快速解吸速率、慢速解吸速率和不同赋存形态镉含量与土壤pH、CE、CECp、DOC、无定形氧化铁、比表面积和分形维数D呈显著或极显著相关关系,而交换态镉则与土壤CECp的大小呈极显著正相关关系。因此,可以认为冻融是通过改变土壤理化性质来实现对土壤镉吸附解吸特性的影响的。统计分析结果表明,pH和CECp主要通过直接作用、CEC通过间接作用增加土壤镉吸附容量,DOC主要是通过直接作用降低土壤镉吸附容量的。
综上所述,冻融处理使土壤经历冻胀-消融过程,导致土壤结构和黏土矿物的破坏、有机物质组分和土壤溶液中物质组成改变,致使土壤pH、CEC、CECp、DOC、无定形氧化铁、比表面积和土壤微团聚体的稳定性发生变化,是造成土壤对镉吸附容量大小、吸附-解吸速率快慢及土壤中镉赋存形态不同的主要原因。不同冻融处理土壤镉吸附解吸特性的变化是多个理化性质综合作用的结果。
The adsorption-desorption characteristics in soil after Cd inputed into the soils influenced the Cd behavior, and detemined the extent of Cd pollution in a way. The adsorption-desorption was affected by many factores, on which many studies have been done.Freeze/thawing may be the important factor influenced the Cd adsorption-desorption in soil in north clod area because that freeze/thawing could affected the mineral,charge type and quantity in the soil directly and also affected the organics quantity and form.However, so far the studied on effect of freeze/thawing were less,and the studied on the mechamism of effect of freeze/thawing on Cd adorption-desorption in soil were more less.In this paper,the brown soils distributing in Shenyang area were collected for tested soils, the soil samples of various water content were treated with various freeze/thawing time by artificial temperature control method. The cadmium static isothermal adsorption-desorption isotherms and kinetics isothermal adsorption-desorption isotherm, the adsorbed Cd fractionation in the soil were assayed, then contected the Cd adsorption-desorption characteristics with the soil physical and chemical properties by statistical analysis, and discussed the the mechamism of effect of freeze/thawing on Cd adorption-desorption in soil.The soil samples were incubated at-30℃and-20℃for24h, respectively. Soil samples of different water content (such as10%,40%,70%,100%and120%of the field capacity) were subsequently refrozen and thawed for0,1,3,6,9cycles. The results were as below:
1. Freeze/thawing time (FTT) and soil water content affected the soil pH, free iron oxide, amorphous iron oxide, iron oxide activation degree, the specific surface significantly, and the FTT also affected CEC, CECp, DOC and the fractal dimension(D)significantly. Most of the soil physical and chemical characteristics were fluctuant change with the FTT, and these phenomena were demonstrated by the SEM pictures of the soil particles and the FTIR spectra when the soil water content equaled to the field capacity. Compared with soil water content and its interaction with FTT, FTT had more obvious effects on soil physical and chemical characteristics.
2. FTT affected the Cd adsorption-desorption in the soil. The Cd adsorption quantity increased firstly and then decreased with the increase of the FTT, the max was at3FTT, and the freeze/thawing improved the Cd adsorption in the soils in the extent of this experiment. The Cd adsorption amount was less when the soil water content was70-100%of the field capacity. The effect of the interaction of the FTT and water content on Cd adsorption quantity in soil was significant, while that of the water content was not. The Cd adsorption ability of tested soils was higher, the mean Cd adsorption ratio reached90.15%increasing firstly and then decreasing with the increase of the FTT. The change in free energy ΔG<0, and ΔG value ranged from-30～0kJ·mol-1,so the adsorption progress belonged to spontaneous physical-chemical adsorption. Initial and average adsorption speed firstly increased and then decreased with the FTT increasing, and appeared adverse change with the water content.
The Cd desorption in soils treated with the different freeze/thawing presented hysteresis quality, and the extent of which firstly enhanced and then receded with the FTT increasing. The Cd desorption rate decreased firstly and then increased with the increase of FTT. Initial and average desorption speed firstly decreased and then increased with the FTT and soil water content increasing.The Cd desorption process in soil can be divided into two sections:fast reaction and slow reaction stage, while the desorption rate of the two reaction stage was different depending on the FTT. The desorption speed of the two reaction stage and the turn time of fast reaction to slow reaction decreased firstly and then increased with the the FTT increasing.
3. The fractionation of the absorbed Cd ordered in:exchangeable from>residual form> bound to carbonates form>bound to Fe-Mn oxides form>bound to organic matter form after adsorbing Cd of soils under various freeze/thawing treatments.
The FTT and the soil water content affected the exchangeable from Cd, Carbonates form Cd, Fe-Mn oxides form Cd significantly, and the FTT also affected the residual Cd significantly.
The availability index (K) and mobility index (M) of the adsorbed Cd in soils increased firstly then decreased with the freezing and thawing frequency increase,and the mean of them were66%and63%respectively.
4.The adsorption capacity, hysteresis coefficient,fast desorption speed, slow desorption speed and the various fractionation of the Cd in soils were connected with the pH, CEC, CECp, DOC, amorphous iron oxide, the specific surface and the fractal dimension significantly at0.05or0.01level during the progress of the Cd adsorption-desorption in freeze/thawed soils, while the exchangeable Cd and CECp were significant positive correlation at0.01level. And the statistical analysis results showed that the facilitation of pH and CECp on kF was produced through the direct action, that of CEC on kF was produced through the indirect action; the inhibition of DOC on kF was produced through direct action.
To sum up, freeze/thawing treatments made soil experience frost heave-ablation process, which lead to soil structure and mainly pure montmorillanite destruct, organic matter component and soil solution components change, caused the soil pH, CEC, CECP, DOC, amorphous iron oxide, specific surface area and D changed, so that caused the change of the soil Cd adsorption quantity,adsorption-desorption speed and the fractionation of the adsorbed Cd in the soil under different freeze/thawing treatments. The change of the Cd adsorption-desorption characteristics of soil under different freeze/thawing treatments was resulted by integrated effects of physical and chemical properties.
引文
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