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北美对流层中氟调醇和全氟羧酸的高分辨率大气模拟。

High-resolution atmospheric modeling of fluorotelomer alcohols and perfluorocarboxylic acids in the North American troposphere.

作者信息

Yarwood Greg, Kemball-Cook Susan, Keinath Michael, Waterland Robert L, Korzeniowski Stephen H, Buck Robert C, Russell Mark H, Washburn Stephen T

机构信息

ENVIRON International Corporation, Golden Gate Plaza, 101 Rowland Way, Novato, California 94945, USA.

出版信息

Environ Sci Technol. 2007 Aug 15;41(16):5756-62. doi: 10.1021/es0708971.

DOI:10.1021/es0708971
PMID:17874783
Abstract

A high spatial and temporal resolution atmospheric model is used to evaluate the potential contribution of fluorotelomer alcohol (FTOH) and perfluorocarboxylate (PFCA) emissions associated with the manufacture, use, and disposal of DuPont fluorotelomer-based products in North America to air concentrations of FTOH, perfluorooctanoic acid (PFOA), and perfluorononanoic acid (PFNA) in North America and the Canadian Arctic. A bottom-up emission inventory for PFCAs and FTOHs was developed from sales and product composition data. A detailed FTOH atmospheric degradation mechanism was developed to simulate FTOH degradation to PFCAs and model atmospheric transport of PFCAs and FTOHs. Modeled PFCA yields from FTOH degradation agree with experimental smog-chamber results supporting the degradation mechanism used. Estimated PFCA and FTOH air concentrations and PFCA deposition fluxes are compared to monitoring data and previous global modeling. Predicted FTOH air concentrations are generally in agreement with available monitoring data. Overall emissions from the global fluorotelomer industry are estimated to contribute approximately 1-2% of the PFCAs in North American rainfall, consistent with previous global emissions estimates. Emission calculations and modeling results indicate that atmospheric inputs of PFCAs in North America from fluorotelomer-based products will decline by an order of magnitude in the near future as a result of current industry commitments to reduce manufacturing emissions and lower the residual fluorotelomer alcohol raw material and trace PFCA product content.

摘要

利用高时空分辨率大气模型,评估与北美杜邦含氟调聚物产品的制造、使用和处置相关的氟调聚物醇(FTOH)和全氟羧酸盐(PFCA)排放对北美和加拿大北极地区空气中FTOH、全氟辛酸(PFOA)和全氟壬酸(PFNA)浓度的潜在贡献。基于销售和产品成分数据,编制了PFCA和FTOH的自下而上排放清单。开发了详细的FTOH大气降解机制,以模拟FTOH降解为PFCA,并对PFCA和FTOH的大气传输进行建模。FTOH降解产生的PFCA模拟产量与支持所使用降解机制的实验烟雾箱结果一致。将估计的PFCA和FTOH空气浓度以及PFCA沉积通量与监测数据和先前的全球模型进行比较。预测的FTOH空气浓度通常与现有监测数据一致。全球含氟调聚物行业的总体排放估计占北美降雨中PFCA的约1-2%,与先前的全球排放估计一致。排放计算和建模结果表明,由于目前行业承诺减少制造排放并降低残留氟调聚物醇原料和痕量PFCA产品含量,北美基于含氟调聚物产品的PFCA大气输入在不久的将来将下降一个数量级。

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