莠去津和硝磺草酮在环境中的迁移行为与光催化降解研究
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摘要
有毒有机物莠去津和硝磺草酮是两种效果较好的玉米田除草剂,在我国具有很好的应用前景。为了更好的掌握这两种农药在玉米田环境中的危害并对它们进行有效的污染控制,本文研究了莠去津和硝磺草酮在玉米田环境中的迁移行为和莠去津在土壤中的光催化降解。开发出了这两种农药的分析方法并对它们在玉米田环境中的动态迁移和累积分布规律进行了系统研究。同时,以介孔分子筛为载体合成了TiO2光催化剂,并应用这种光催化剂对土壤中莠去津降解行为进行了研究。
论文通过研究,开发出了莠去津的气相色谱分析方法和硝磺草酮的液相色谱分析方法。其中,莠去津的提取剂为丙酮,回收率在83.28%～110.16%之间,变异系数在0.96%～3.24%之间;硝磺草酮的提取剂为乙腈,回收率在82.46%～97.38%之间,变异系数在0.92%～2.86%之间。
采用田间试验方法,研究了莠去津和硝磺草酮在土壤和玉米中动态迁移和累积分布规律。研究结果表明,莠去津和硝磺草酮在土壤和玉米中的降解过程均符合一级动力学数学模型,降解半衰期均小于30d,属易降解农药。玉米收获期,莠去津在玉米中的最终残留未检出,硝磺草酮在玉米中的最终残留量为0.004mg·kg-1。参照我国国家标准,在原粮中莠去津的最高残留限量(MRL)值为0.05mg·kg-1,按照推荐使用剂量2倍使用,其有效成分莠去津在玉米中的最终残留是安全的。参照美国国家标准,玉米中硝磺草酮的MRL值为0.01mg·kg-1。按照推荐使用剂量2倍使用,其有效成分硝磺草酮在玉米中的最终残留是安全的。
论文合成了一种介孔分子筛材料并考察了晶化时间和表面活性剂比率对介孔分子筛形成结构的影响。研究结果表明,当晶化时间为24 h,表面活性剂比率为0.24时可以获得最佳结晶度的六角形相介孔分子筛。将TiO2负载在介孔分子筛表面制备出新型光催化剂并将其应用到莠去津在土壤中的光催化降解中。结果表明,实验室制得的此种负载型光催化剂对土壤中莠去津具有较好的光催化降解效果。
Toxic organic pollutants atrazine and mesotrione are two kinds of effective herbicides in maize field and they possess broad application foreground in China. To master the two herbicides hazard and control their pollution, this paper has studied on the migration behavior of atrazine and mesotrione in maize field and the photodegradation of atrazine with a novel photocatalyst. The analysis methods of these two herbicides in maize and soil were developed. The dynamic migration and accumulation distribution laws were studied systematically. Besides, TiO2 photocatalysts coated mesoporous molecular sieves were prepared. The degradation behaviors of atrazine in soil were studied by using the TiO2 photocatalysts.
GC analysis method of atrazine and HPLC analysis method of mesotrione were established by study in this paper. The extractant of atrazine is acetone. The recovery rates are between 83.28% and 110.16% and the coefficients of variation are between 0.96% and 3.24%. The extractant of mesotrione is acetonitrile. The recovery rates are between 82.46% and 97.38% and the coefficients of variation are between 0.92% and 2.86%.
The dynamic migration and accumulation distribution laws of atrazine and mesotrione in maize and soil were studied by field experiment. The results show that the dynamic degradation processes of atrazine and mesotrione in maize accord with the first order kinetic model. Both of the half-lives of these two herbicides are less than 30 days. So they are easy degradation herbicides. At harvest time, the final residuals of atrazine in maize are not detected and the final residual of mesotrione in maize is 0.004 mg/kg. The maximum residue limit (MRL) of atrazine in raw grain according to the China--National Standard System (GB) is 0.05 mg/kg. With sprayed atrazine at recommended two times dosage, the residuals of atrazine in maize are safe. The MRL of mesotrione in maize according to the US--National Standard System is 0.01 mg/kg. With sprayed mesotrione at recommended two times dosage, the residuals of mesotrione in maize are safe.
In this paper, the crystallization time and the surfactant ratio have been examined for the synthesis of the mesoporous molecular sieve materials. The results show that the best crystallization time is 24 hours and the best surfactant ratio is 0.24. Under this condition, the hexagonal phase mesoporous molecular sieves with high crystallinity degree are prepared. After the preparation of the novel photocatalysts coated the mesoporous molecular sieves, the photocatalysts were used in the experiment of atrazine photodegradation in soil. The results show that the photocatalysts prepared in this paper are more effective in the degradation of atrazine.
论文通过研究,开发出了莠去津的气相色谱分析方法和硝磺草酮的液相色谱分析方法。其中,莠去津的提取剂为丙酮,回收率在83.28%～110.16%之间,变异系数在0.96%～3.24%之间;硝磺草酮的提取剂为乙腈,回收率在82.46%～97.38%之间,变异系数在0.92%～2.86%之间。
采用田间试验方法,研究了莠去津和硝磺草酮在土壤和玉米中动态迁移和累积分布规律。研究结果表明,莠去津和硝磺草酮在土壤和玉米中的降解过程均符合一级动力学数学模型,降解半衰期均小于30d,属易降解农药。玉米收获期,莠去津在玉米中的最终残留未检出,硝磺草酮在玉米中的最终残留量为0.004mg·kg-1。参照我国国家标准,在原粮中莠去津的最高残留限量(MRL)值为0.05mg·kg-1,按照推荐使用剂量2倍使用,其有效成分莠去津在玉米中的最终残留是安全的。参照美国国家标准,玉米中硝磺草酮的MRL值为0.01mg·kg-1。按照推荐使用剂量2倍使用,其有效成分硝磺草酮在玉米中的最终残留是安全的。
论文合成了一种介孔分子筛材料并考察了晶化时间和表面活性剂比率对介孔分子筛形成结构的影响。研究结果表明,当晶化时间为24 h,表面活性剂比率为0.24时可以获得最佳结晶度的六角形相介孔分子筛。将TiO2负载在介孔分子筛表面制备出新型光催化剂并将其应用到莠去津在土壤中的光催化降解中。结果表明,实验室制得的此种负载型光催化剂对土壤中莠去津具有较好的光催化降解效果。
Toxic organic pollutants atrazine and mesotrione are two kinds of effective herbicides in maize field and they possess broad application foreground in China. To master the two herbicides hazard and control their pollution, this paper has studied on the migration behavior of atrazine and mesotrione in maize field and the photodegradation of atrazine with a novel photocatalyst. The analysis methods of these two herbicides in maize and soil were developed. The dynamic migration and accumulation distribution laws were studied systematically. Besides, TiO2 photocatalysts coated mesoporous molecular sieves were prepared. The degradation behaviors of atrazine in soil were studied by using the TiO2 photocatalysts.
GC analysis method of atrazine and HPLC analysis method of mesotrione were established by study in this paper. The extractant of atrazine is acetone. The recovery rates are between 83.28% and 110.16% and the coefficients of variation are between 0.96% and 3.24%. The extractant of mesotrione is acetonitrile. The recovery rates are between 82.46% and 97.38% and the coefficients of variation are between 0.92% and 2.86%.
The dynamic migration and accumulation distribution laws of atrazine and mesotrione in maize and soil were studied by field experiment. The results show that the dynamic degradation processes of atrazine and mesotrione in maize accord with the first order kinetic model. Both of the half-lives of these two herbicides are less than 30 days. So they are easy degradation herbicides. At harvest time, the final residuals of atrazine in maize are not detected and the final residual of mesotrione in maize is 0.004 mg/kg. The maximum residue limit (MRL) of atrazine in raw grain according to the China--National Standard System (GB) is 0.05 mg/kg. With sprayed atrazine at recommended two times dosage, the residuals of atrazine in maize are safe. The MRL of mesotrione in maize according to the US--National Standard System is 0.01 mg/kg. With sprayed mesotrione at recommended two times dosage, the residuals of mesotrione in maize are safe.
In this paper, the crystallization time and the surfactant ratio have been examined for the synthesis of the mesoporous molecular sieve materials. The results show that the best crystallization time is 24 hours and the best surfactant ratio is 0.24. Under this condition, the hexagonal phase mesoporous molecular sieves with high crystallinity degree are prepared. After the preparation of the novel photocatalysts coated the mesoporous molecular sieves, the photocatalysts were used in the experiment of atrazine photodegradation in soil. The results show that the photocatalysts prepared in this paper are more effective in the degradation of atrazine.
引文
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