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

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This study characterized surface functional groups on diesel and hydrotreated vegetable oil (HVO) soot using heterogeneous chemistry. HVO and diesel soot exhibit more acidic, carbonyl, and reducing groups than amorphous carbon, impacting their reactivity.

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Area of Science:

  • Environmental Chemistry
  • Materials Science
  • Surface Chemistry

Background:

  • Combustion aerosols, including diesel and hydrotreated vegetable oil (HVO) soot, possess surface functional groups that influence their environmental behavior and reactivity.
  • Understanding these surface properties is crucial for predicting aerosol interactions and atmospheric fate.

Purpose of the Study:

  • To investigate and compare the surface functional groups of conventional diesel soot, HVO soot, and amorphous carbon using heterogeneous chemistry.
  • To quantify the acidic, basic, carbonyl, and reducing sites on these aerosol types.

Main Methods:

  • Utilized a Knudsen flow reactor under molecular flow conditions for gas-particle surface reactions.
  • Employed gas titration experiments with trimethylamine (N(CH3)3), hydroxylamine (NH2OH), trifluoroacetic acid (CF3COOH), hydrochloric acid (HCl), ozone (O3), and nitrogen dioxide (NO2).
  • Analyzed a commercial amorphous carbon (Printex XE2-B) as a reference substrate.

Main Results:

  • Diesel and HVO soot showed higher densities of acidic and carbonyl functionalities compared to amorphous carbon.
  • HVO soot exhibited the largest abundance of carbonyl groups.
  • Weak basic oxides were present, interacting preferentially with strong acids.
  • Diesel and HVO soot possessed significantly more reducing sites (10x and 30x, respectively) than amorphous carbon, indicating higher reactivity with oxidizers.

Conclusions:

  • Combustion aerosols from diesel and HVO have distinct surface chemistries with higher concentrations of reactive functional groups compared to amorphous carbon.
  • The increased abundance of acidic, carbonyl, and reducing sites on HVO and diesel soot suggests greater potential for heterogeneous reactions in the atmosphere.
  • These findings are vital for understanding aerosol-driven atmospheric processes and developing emission control strategies.