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Benzene: A Secondary Pollutant Formed in the Three-Way Catalyst
Bruehlmann, S., A.M. Forss, D. Steffen and N.V. Heeb [W. Giger] Benzene
emissions from a relevant proportion of today's gasoline-driven
passenger cars and light-duty vehicles can increase by up to 2 orders
of magnitude when driving at high engine load (e.g., on highways).
Under such conditions, post-catalyst benzene levels exceeded those
found precatalyst. As a consequence, formation of benzene in the
catalyst was postulated. To further reduce ambient air concentrations
of benzene, these critical operating conditions must be carefully
avoided. Here, we report in detail to what extent and at what operating
conditions catalyst-induced benzene and toluene formation can occur.
For that purpose, a EURO-1 passenger car (1.8 L, model year 1995)
fulfilling the valid regulations, equipped with a new, two layered,
Pd-CeO2-Al2O3/Rh-ZrO2-Al2O3 three-way catalyst was operated at steady
state on a chassis dynamometer at 100, 125, and 150 km/h at variable
air to fuel ratios. Pre- and post-catalyst exhaust gas concentrations
of benzene, toluene, C-2-, and C-3-benzenes were monitored at a time
resolution of 0.5 Hz by means of chemical ionization mass spectrometry.
A net benzene formation window, ranging from pre-catalyst exhaust gas
temperatures of 600-730 °C and A-values of 0.83-0.95, with a
pronounced minimum at 0.87, was observed. Dealkylation reactions of
aromatic hydrocarbons are assumed to be the major pathway leading to
benzene. |
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