Heterogeneous Oxidation of SO2 by Ozone on the Surface of Black Carbon Particles

doi:10.7503/cjcu20120024

Abstract

Abstract:

Black carbon (BC) produced by incomplete combustion processes is an important aerosol species. The heterogeneous reactions of gaseous pollutants (such as SO₂, O₃ and NO_x) on the surface of BC particles are of significance because these reactions can change the particles' morphology, chemical composition, hygroscopicity and optical properties, and thus alter their climate or health effect, as well as these reactions can influence environmental chemical cycling. In this study, the heterogeneous oxidation of SO₂ by O₃ on the surface of black carbon(using Printex U as the model particles, denoted as UBC) was investigated by the method of Diffuse Reflectance Infrared Fourier Transform Spectroscopy(DRIFTS). The surface product was monitored, and confirmed by Ion Chromatographic (IC) and X-ray photoelectron spectroscopy (XPS) techniques. It was found that the main product of SO₂ heterogeneous reaction on the surface of UBC or diluted UBC [with one part of UBC diluted in 399 parts of infrared transparent NaCl powder, denoted as UBC(1:400)] was sulfate and the oxidation reaction rate could be greatly enhanced by O₃. The simultaneous presence of ozone and water vapor are necessary for the sulfate formation and the reaction rate can sustain for 3 h. UBC particles supply reactive surface sites(SS) which react with O₃ to produce oxygen atom(SSO), promoting the heterogeneous oxidation of SO₂ to SO₄^2-. O₃ is the dominating oxidant, and water vapor makes for SS regeneration. In the condition of 10¹⁴-10¹⁵ molecule/cm³ SO₂+10¹⁴-10¹⁵ molecule/cm³ O₃+40%RH, the steady state uptake coefficient of SO₂ on UBC(1:400) was (1-6)×10^-6 using BET surface area as the effective reaction area. The reaction order of O₃ was found to be 0.5. The sulfate formation rate on the surface of UBC(1:400) particles was calculated up to 10¹⁴-10¹⁵ ion·s^-1·g^-1, indicating that this kind of heterogeneous reaction may play an important role in altering the physicochemical properties of BC particles in the highly air-polluted weather conditions.

Key words: Black carbon, Sulfate, Ozone, Heterogeneous reaction, Steady state uptake coefficient

CLC Number:

O643.1

TrendMD:

SONG Han, SHANG Jing, ZHU Tong, ZHAO Li, YE Jun-Hui. Heterogeneous Oxidation of SO₂ by Ozone on the Surface of Black Carbon Particles[J]. Chem. J. Chinese Universities, 2012, 33(10): 2295.

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Heterogeneous Oxidation of SO₂ by Ozone on the Surface of Black Carbon Particles

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