不同钝化剂对土壤中Cu的钝化能力及其对土壤速效养分影响的研究
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摘要
随着土壤重金属污染日益加剧,土壤重金属污染的治理已成为当前研究的热点。原位固定技术是修复重金属污染土壤治理过程中一种非常有效的方法,该技术的关键在于钝化剂的选择。纳米黑碳的比表面积大,吸附能力强,是一种很有应用前景的土壤改良剂。猪粪降解液改性钠基膨润土由天然材料制备而成,对环境影响较小,同样是一种很有应用前景的土壤改良剂。
本文在已有研究的基础上,以山东三种典型土壤(褐土、潮土、酸性棕壤)为供试土壤,以硝酸改性纳米黑碳、酸性高锰酸钾改性纳米黑碳、硫酸改性纳米黑碳、HDTMA(十六烷基三甲基溴化铵)改性钠基膨润土及猪粪降解液改性钠基膨润土为钝化剂,通过吸附动力学实验、吸附等温线实验研究钝化剂对Cu~(2+)的吸附动力学及吸附热力学特征;通过水培养实验研究营养盐浓度对钝化剂吸附Cu~(2+)能力的影响;通过土壤培养试验,研究施肥对硝酸改性纳米黑碳、猪粪降解液改性钠基膨润土固定土壤中重金属Cu能力的影响以及硝酸改性纳米黑碳、猪粪降解液改性膨润土在修复重金属Cu污染土壤过程中对土壤养分有效性的影响。本文获得主要研究结果如下:
1、Cu~(2+)在五种不同钝化剂上的吸附等温线都能用Freundlich和Langmuir方程很好的拟合;硝酸改性纳米黑碳、硫酸改性纳米黑碳、猪粪降解液改性钠基膨润土、HDTMA改性钠基膨润土用Langmuir方程拟合的相关系数大于用Freundlich拟合的相关系数,酸性高锰酸钾改性纳米黑碳用Freundlich拟合的相关系数要大于用Langmuir方程拟合的相关系数,这与用酸性高锰酸钾改性纳米黑碳时引入的K~+影响有关;
2、NO_3~-对两种有机改性膨润土吸附能力的影响与对改性纳米黑碳吸附能力的影响不同。随着NO_3~-浓度的增加,两种改性膨润土对Cu~(2+)的吸附量呈现先增加后减少的趋势;改性纳米黑碳对Cu~(2+)的吸附量呈现先减小后增大的趋势;HPO_4~(2-)对两种有机改性膨润土吸附能力的影响与对改性纳米黑碳吸附能力的影响相同。随着HPO_4~(2-)浓度的增加,五种钝化剂对Cu~(2+)的吸附量均呈现增加趋势,这与HPO_4~(2-)能与Cu~(2+)发生沉淀有关。K~+对两种有机改性膨润土吸附能力的影响与对改性纳米黑碳吸附能力的影响相同。随着K~+浓度的增加,五种钝化剂对Cu~(2+)的吸附量均逐渐减小,K~+与Cu~(2+)存在明显的竞争吸附现象。
3、施肥可使褐土、潮土、酸性棕壤中DTPA-Cu含量升高;随着时间的增加,各施肥处理重金属有效态含量降低,对照随时间没有表现出明显的规律;只施钝化剂处理铜有效态含量低于同时施加钝化剂和肥处理,说明同时施加钝化剂和肥会降低钝化剂的有效性;
4、在三种土壤中同时施加肥和硝酸改性纳米黑碳处理及同时施加肥和猪粪降解液改性钠基膨润土处理比只施肥的处理速效磷的含量低,钝化剂对磷有固定作用;在三种土壤中施加硝酸改性纳米黑碳都可以使土壤中碱解氮的含量增加,以酸性棕壤增加最多,这主要是由于在利用硝酸对纳米黑碳进行改性的过程中引入了硝酸根,施入土壤后使土壤中碱解氮的含量增加,增加的量大于由于纳米黑碳的钝化作用减少的量;在三种土壤中施加硝酸改性纳米黑碳都可以使土壤中速效钾的含量增加,以褐土增加最多,这主要是由于土壤中的Cu~(2+)和K~+存在竞争吸附,将硝酸改性纳米黑碳施入土壤中,吸附了土壤中的Cu~(2+),土壤溶液中正电荷减少,从而使土壤胶体中的钾离子从土壤胶粒上解吸下来,使土壤中速效钾的含量增加。
5、先施加钝化剂一段时间后施肥,能够有效提高土壤中速效磷,碱解氮,速效钾的含量,建议在施加钝化剂20天后施肥。
With the increasing of heavy metal contamination of soil, the pollution of heavy metal in the soil has become a hot spot in current research. The immobilization is an effective remediation technique of contaminated soils by heavy metals and the choice of passivant is the key of the technology. Nano- black carbon has large surface area, adsorption capacity, is a promising soil conditioner. Na-bentonite modified by pig manure degradation liquid made by natural materials is friendly to the environment and it is also a promising soil conditioner.
Based on existing research, three soils Cinnamon soil, Aquic soil, and Acid brown soil were researched. Nano- black carbon oxidized by nitric acid, nano- black carbon oxidized by sulfuric acid, nano-black carbon oxidized by acidic potassium permanganate, Na-bentonite modified by pig manure degradation liquid and Na-bentonite modified by hexadecyl trimethyl ammonium bromide were used as passivators. The adsorption kinetcis and adsorption thermodynamics and effects of nutrients to the adsorption capacity for Cu~(2+) of the passivators were studied. Effects of nutrients to the adsorption ability for Cu~(2+) of nano- black carbon oxidized by nitric acid and Na-bentonite modified by pig manure degradation liquid are studied in the soils, at the same time, effects of the passivators to nutrients were studied.
The main results of this paper are as follows:
1. The adsorption kinetcis of Cu~(2+) on the five different passivators fit the Langmuir model very well.To nano-black carbon oxidized by nitric acid, nano- black carbon oxidized by sulfuric acid, Na-bentonite modified by hexadecyl trimethyl ammonium bromide and Na-bentonite modified by pig manure degradation liquid, Langmuir model is better than Freundlich model, but as to nano-black carbon oxidized by acidic potassium permanganate, Freundlich model is better than Langmuir model.
2. As the concentration of NO_3~- increased, the adsorption ability for Cu~(2+) of Na-bentonite modified by hexadecyl trimethyl ammonium bromide and Na-bentonite modified by pig manure degradation liquid increased at first and then decreased. As to nano- black carbon, it deseased first and then increased; As the concentration of HPO_4~(2-) increased, the adsorption ability for Cu~(2+) of the five kind of passivators increased; As the concentration of K~+increased, the adsorption ability for Cu~(2+) of the five kind of passivators increased.Between K~+and Cu~(2+) there is a clear competitive adsorption.
3. Fertilization can make the content of DTPA-Cu increase in the three soils; The available Cu in fertilizer treatments decreased as time went on, controls showed no obvious rule; Treatments applied with passivators available Cu was lower than treatments applied with passivators and fertilizer, indicating that fertilizer applied at the same time with passivators will reduce the effectiveness of passivation;
4. In the three soils, the available phosphorus in treatments applied with fertilizer and nano-black carbon oxidized by nitric acid and treatments applied with fertilizer and na-bentonite modified by pig manure degradation liquid is lower than treatments applied with fertilizer, indicating passivators fixed phosphorus in the soils. The available nitrogen in treatments applied with fertilizer and nano-black carbon oxidized by nitric acid is higher than treatments applied with fertilizer because nano-black carbon oxidized by nitric acid take in some NO_3~-. The available potassium in treatments applied with fertilizer and nano-black carbon oxidized by nitric acid is higher than treatments applied with fertilizer because of the desorption of K~+ from soil colloid.
5. The content of available phosphorus, available nitrogen and available potassium will increase if passivators were applied some days after fertilization and 20 days was suggested.
本文在已有研究的基础上,以山东三种典型土壤(褐土、潮土、酸性棕壤)为供试土壤,以硝酸改性纳米黑碳、酸性高锰酸钾改性纳米黑碳、硫酸改性纳米黑碳、HDTMA(十六烷基三甲基溴化铵)改性钠基膨润土及猪粪降解液改性钠基膨润土为钝化剂,通过吸附动力学实验、吸附等温线实验研究钝化剂对Cu~(2+)的吸附动力学及吸附热力学特征;通过水培养实验研究营养盐浓度对钝化剂吸附Cu~(2+)能力的影响;通过土壤培养试验,研究施肥对硝酸改性纳米黑碳、猪粪降解液改性钠基膨润土固定土壤中重金属Cu能力的影响以及硝酸改性纳米黑碳、猪粪降解液改性膨润土在修复重金属Cu污染土壤过程中对土壤养分有效性的影响。本文获得主要研究结果如下:
1、Cu~(2+)在五种不同钝化剂上的吸附等温线都能用Freundlich和Langmuir方程很好的拟合;硝酸改性纳米黑碳、硫酸改性纳米黑碳、猪粪降解液改性钠基膨润土、HDTMA改性钠基膨润土用Langmuir方程拟合的相关系数大于用Freundlich拟合的相关系数,酸性高锰酸钾改性纳米黑碳用Freundlich拟合的相关系数要大于用Langmuir方程拟合的相关系数,这与用酸性高锰酸钾改性纳米黑碳时引入的K~+影响有关;
2、NO_3~-对两种有机改性膨润土吸附能力的影响与对改性纳米黑碳吸附能力的影响不同。随着NO_3~-浓度的增加,两种改性膨润土对Cu~(2+)的吸附量呈现先增加后减少的趋势;改性纳米黑碳对Cu~(2+)的吸附量呈现先减小后增大的趋势;HPO_4~(2-)对两种有机改性膨润土吸附能力的影响与对改性纳米黑碳吸附能力的影响相同。随着HPO_4~(2-)浓度的增加,五种钝化剂对Cu~(2+)的吸附量均呈现增加趋势,这与HPO_4~(2-)能与Cu~(2+)发生沉淀有关。K~+对两种有机改性膨润土吸附能力的影响与对改性纳米黑碳吸附能力的影响相同。随着K~+浓度的增加,五种钝化剂对Cu~(2+)的吸附量均逐渐减小,K~+与Cu~(2+)存在明显的竞争吸附现象。
3、施肥可使褐土、潮土、酸性棕壤中DTPA-Cu含量升高;随着时间的增加,各施肥处理重金属有效态含量降低,对照随时间没有表现出明显的规律;只施钝化剂处理铜有效态含量低于同时施加钝化剂和肥处理,说明同时施加钝化剂和肥会降低钝化剂的有效性;
4、在三种土壤中同时施加肥和硝酸改性纳米黑碳处理及同时施加肥和猪粪降解液改性钠基膨润土处理比只施肥的处理速效磷的含量低,钝化剂对磷有固定作用;在三种土壤中施加硝酸改性纳米黑碳都可以使土壤中碱解氮的含量增加,以酸性棕壤增加最多,这主要是由于在利用硝酸对纳米黑碳进行改性的过程中引入了硝酸根,施入土壤后使土壤中碱解氮的含量增加,增加的量大于由于纳米黑碳的钝化作用减少的量;在三种土壤中施加硝酸改性纳米黑碳都可以使土壤中速效钾的含量增加,以褐土增加最多,这主要是由于土壤中的Cu~(2+)和K~+存在竞争吸附,将硝酸改性纳米黑碳施入土壤中,吸附了土壤中的Cu~(2+),土壤溶液中正电荷减少,从而使土壤胶体中的钾离子从土壤胶粒上解吸下来,使土壤中速效钾的含量增加。
5、先施加钝化剂一段时间后施肥,能够有效提高土壤中速效磷,碱解氮,速效钾的含量,建议在施加钝化剂20天后施肥。
With the increasing of heavy metal contamination of soil, the pollution of heavy metal in the soil has become a hot spot in current research. The immobilization is an effective remediation technique of contaminated soils by heavy metals and the choice of passivant is the key of the technology. Nano- black carbon has large surface area, adsorption capacity, is a promising soil conditioner. Na-bentonite modified by pig manure degradation liquid made by natural materials is friendly to the environment and it is also a promising soil conditioner.
Based on existing research, three soils Cinnamon soil, Aquic soil, and Acid brown soil were researched. Nano- black carbon oxidized by nitric acid, nano- black carbon oxidized by sulfuric acid, nano-black carbon oxidized by acidic potassium permanganate, Na-bentonite modified by pig manure degradation liquid and Na-bentonite modified by hexadecyl trimethyl ammonium bromide were used as passivators. The adsorption kinetcis and adsorption thermodynamics and effects of nutrients to the adsorption capacity for Cu~(2+) of the passivators were studied. Effects of nutrients to the adsorption ability for Cu~(2+) of nano- black carbon oxidized by nitric acid and Na-bentonite modified by pig manure degradation liquid are studied in the soils, at the same time, effects of the passivators to nutrients were studied.
The main results of this paper are as follows:
1. The adsorption kinetcis of Cu~(2+) on the five different passivators fit the Langmuir model very well.To nano-black carbon oxidized by nitric acid, nano- black carbon oxidized by sulfuric acid, Na-bentonite modified by hexadecyl trimethyl ammonium bromide and Na-bentonite modified by pig manure degradation liquid, Langmuir model is better than Freundlich model, but as to nano-black carbon oxidized by acidic potassium permanganate, Freundlich model is better than Langmuir model.
2. As the concentration of NO_3~- increased, the adsorption ability for Cu~(2+) of Na-bentonite modified by hexadecyl trimethyl ammonium bromide and Na-bentonite modified by pig manure degradation liquid increased at first and then decreased. As to nano- black carbon, it deseased first and then increased; As the concentration of HPO_4~(2-) increased, the adsorption ability for Cu~(2+) of the five kind of passivators increased; As the concentration of K~+increased, the adsorption ability for Cu~(2+) of the five kind of passivators increased.Between K~+and Cu~(2+) there is a clear competitive adsorption.
3. Fertilization can make the content of DTPA-Cu increase in the three soils; The available Cu in fertilizer treatments decreased as time went on, controls showed no obvious rule; Treatments applied with passivators available Cu was lower than treatments applied with passivators and fertilizer, indicating that fertilizer applied at the same time with passivators will reduce the effectiveness of passivation;
4. In the three soils, the available phosphorus in treatments applied with fertilizer and nano-black carbon oxidized by nitric acid and treatments applied with fertilizer and na-bentonite modified by pig manure degradation liquid is lower than treatments applied with fertilizer, indicating passivators fixed phosphorus in the soils. The available nitrogen in treatments applied with fertilizer and nano-black carbon oxidized by nitric acid is higher than treatments applied with fertilizer because nano-black carbon oxidized by nitric acid take in some NO_3~-. The available potassium in treatments applied with fertilizer and nano-black carbon oxidized by nitric acid is higher than treatments applied with fertilizer because of the desorption of K~+ from soil colloid.
5. The content of available phosphorus, available nitrogen and available potassium will increase if passivators were applied some days after fertilization and 20 days was suggested.
引文
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