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Environ Sci Technol. 2016 Mar 15;50(6):2946-55. doi: 10.1021/acs.est.5b05531. Epub 2016 Feb 26.

Molecular Characterization of the Gas-Particle Interface of Soot Sampled from a Diesel Engine Using a Titration Method.

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Departamento de Química Física, Facultad de Ciencias y Tecnologías Químicas, Universidad de Castilla La Mancha , Avda. Camilo José Cela s/n, 13071 Ciudad Real, Spain.
Grupo de Combustibles y Motores, Escuela Técnica Superior de Ingenieros Industriales, Universidad de Castilla la Mancha , Avda. Camilo José Cela 10, 13071 Ciudad Real, Spain.
Labor für Atmosphärenchemie (LAC), Paul Scherrer Institute (PSI) , OBBA006, CH-5232 Villigen PSI, Switzerland.


Surface functional groups of two different types of combustion aerosols, a conventional diesel (EN 590) and a hydrotreated vegetable oil (HVO) soot, have been investigated using heterogeneous chemistry (i.e., gas-particle surface reactions). A commercial sample of amorphous carbon (Printex XE2-B) was analyzed as a reference substrate. A Knudsen flow reactor was used to carry out the experiments under molecular flow conditions. The selected gases for the titration experiments were: N(CH3)3 for the identification of acidic sites, NH2OH for the presence of carbonyl groups, CF3COOH and HCl for basic sites of different strength, and O3 and NO2 for reducing groups. Reactivity with N(CH3)3 indicates a lower density of acidic functionalities for Printex XE2-B in relation to diesel and HVO soot. Results for NH2OH experiments indicates that commercial amorphous carbon exhibits a lower abundance of available carbonyl groups at the interface compared to the results from diesel and HVO soot, the latter being the one with the largest abundance of carbonyl functions. Reactions with acids indicate the presence of weak basic oxides on the particle surface that preferentially interact with the strong acid CF3COOH. Finally, reactions with O3 and NO2 reveal that diesel and especially HVO have a significantly higher reactivity with both oxidizers compared to that of Printex XE2-B because they have more reducing sites by roughly a factor of 10 and 30, respectively. The kinetics of titration reactions have also been investigated.

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