Document Type

Honors Project On-Campus Access Only

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Advisor: Keith Kuwata

Abstract

Carbonyl oxides, or Criegee intermediates, formed in ozonolysis, are very difficult to isolate and study experimentally. Computation has been used to clarify how Criegee intermediates in the troposphere contribute to hydroxyl radical levels and to acid rain. Quantum chemistry, transition state theory, and RRKM theory were used to predict rate constants and branching ratios for the unimolecular and bimolecular reaction of simple Criegee intermediates with water, sulfur dioxide, and nitrogen dioxide. Analysis finds that tunneling accelerates hydrogen shift rates into competition with water addition rates at equilibrium vapor pressure, sulfur dioxide and water both react faster with carbonyl oxides than does nitrogen dioxide, and that sulfur dioxide adducts decompose promptly while some fraction of nitrogen dioxide adducts are collisionally stabilized at atmospheric pressure.

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