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多环芳烃从烟尘表面解吸:五环和六环(C22、C24)多环芳烃。

Desorption of polycyclic aromatic hydrocarbons from soot surface: five- and six-ring (C22, C24) PAHs.

机构信息

Institut de Combustion, Aérothermique, Réactivité et Environnement (ICARE), CNRS, 45071 Orléans Cedex 2, France.

出版信息

J Phys Chem A. 2010 Mar 18;114(10):3533-9. doi: 10.1021/jp912110b.

DOI:10.1021/jp912110b
PMID:20170139
Abstract

The kinetics of thermal desorption of five soot-bound nonvolatile (C(22), C(24)) polycyclic aromatic hydrocarbons (benzo(ghi)perylene (BghiP), indeno(1,2,3-cd)pyrene (IdP), anthanthrene (Antha), dibenz(ah)anthracene (DBahA), dibenzo(ae)pyrene (DBaeP)) identified in laboratory-generated kerosene soot were studied over the temperature range 335-370 K in a low pressure flow reactor. The PAH desorption rate constants were measured using off-line HPLC monitoring of their concentrations in soot samples as a function of desorption time. The following Arrhenius expressions were determined for the desorption rate constants of the soot-bound PAHs studied: k(des) = 8.4 x 10(15) exp[-(129.7 +/- 4.4)/RT], 1.0 x 10(16) exp[-(130.6 +/- 6.1)/RT], 1.1 x 10(16) exp[-(131.6 +/- 3.2)/RT], 1.0 x 10(16) exp[-(128.0 +/- 3.9)/RT], and 1.4 x 10(16) exp[-(134.2 +/- 10.7)/RT] (k(des) are in s(-1) and activation energies in kJ mol(-1)) for BghiP, IdP, Antha, DBahA, and DBaeP, respectively. Analysis of the present and previous experimental data showed that PAH-soot binding energies linearly correlate with the number of PAH carbon atoms. The present data and those from previous studies are discussed in the frame of the existing theoretical gas-to-particle partitioning model.

摘要

在低压流动反应器中,研究了在 335-370 K 的温度范围内,实验室生成的煤油烟尘中五种不挥发的(C(22),C(24))多环芳烃(苯并(ghi)苝(BghiP)、茚并(1,2,3-cd)芘(IdP)、蒽(Atha)、二苯并(ah)蒽(DBahA)、二苯并(ae)芘(DBaeP))的热解吸动力学。通过离线 HPLC 监测烟尘样品中 PAH 浓度随解吸时间的变化,测量了 PAH 的解吸速率常数。确定了所研究的烟尘结合 PAH 的解吸速率常数的以下 Arrhenius 表达式:k(des) = 8.4 x 10(15) exp[-(129.7 +/- 4.4)/RT],1.0 x 10(16) exp[-(130.6 +/- 6.1)/RT],1.1 x 10(16) exp[-(131.6 +/- 3.2)/RT],1.0 x 10(16) exp[-(128.0 +/- 3.9)/RT],和 1.4 x 10(16) exp[-(134.2 +/- 10.7)/RT](k(des) 以 s(-1)表示,活化能以 kJ mol(-1)表示),分别为 BghiP、IdP、Atha、DBahA 和 DBaeP。对本研究和以前的实验数据的分析表明,PAH-烟尘结合能与 PAH 碳原子数呈线性相关。本研究的数据以及以前的研究数据,都在现有的气体到颗粒分配理论模型框架内进行了讨论。

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