Schenker Urs, Scheringer Martin, Sohn Michael D, Maddalena Randy L, McKone Thomas E, Hungerbühler Konrad
Institute for Chemical and Bioengineering, ETH Zurich, CH-8093 Zurich, Switzerland.
Environ Sci Technol. 2009 Jan 1;43(1):128-34. doi: 10.1021/es801161x.
Present and future concentrations of DDT in the environment are calculated with the global multimedia model CliMoChem. Monte Carlo simulations are used to assess the importance of uncertainties in substance property data, emission rates, and environmental parameters for model results. Uncertainties in the model results, expressed as 95% confidence intervals of DDT concentrations in various environmental media, in different geographical locations, and at different points in time are typically between 1 and 2 orders of magnitude. An analysis of rank correlations between model inputs and predicted DDT concentrations indicates that emission estimates and degradation rate constants, in particular in the atmosphere, are the most influential model inputs. For DDT levels in the Arctic, temperature dependencies of substance properties are also influential parameters. A Bayesian Monte Carlo approach is used to update uncertain model inputs based on measurements of DDT in the field. The updating procedure suggests a lower value for half-life in air and a reduced range of uncertainty for Kow of DDT. As could be expected, the Bayesian updating yields model results that are closer to observations, and model uncertainties have decreased. Sensitivity analysis and Bayesian Monte Carlo approach in combination provide new insight into important processes that govern the global fate and persistence of DDT in the environment.
利用全球多介质模型CliMoChem计算了环境中滴滴涕的当前和未来浓度。采用蒙特卡罗模拟方法评估物质属性数据、排放率和环境参数的不确定性对模型结果的重要性。模型结果的不确定性,以不同环境介质、不同地理位置和不同时间点的滴滴涕浓度的95%置信区间表示,通常在1到2个数量级之间。对模型输入与预测的滴滴涕浓度之间的秩相关分析表明,排放估计值和降解速率常数,特别是在大气中的,是最有影响的模型输入。对于北极地区的滴滴涕水平,物质属性的温度依赖性也是有影响的参数。采用贝叶斯蒙特卡罗方法,根据野外滴滴涕测量值更新不确定的模型输入。更新过程表明,空气中的半衰期值较低,滴滴涕的辛醇-水分配系数的不确定性范围减小。不出所料,贝叶斯更新得到的模型结果更接近观测值,模型不确定性也降低了。敏感性分析和贝叶斯蒙特卡罗方法相结合,为控制滴滴涕在环境中的全球归宿和持久性的重要过程提供了新的见解。