【摘 要】
：
theoretically.The structures of the reactant clusters with and without ammonia and subsequent hydrolysis pathways were determined at the CCSD(T)/aug-cc-pVDZ//MP2/aug-cc-PVDZ level of theory.Our result
【机 构】
：
Institute of Theoretical Chemistry,State Key Laboratory of Theoretical and Computational Chemistry,J
论文部分内容阅读
theoretically.The structures of the reactant clusters with and without ammonia and subsequent hydrolysis pathways were determined at the CCSD(T)/aug-cc-pVDZ//MP2/aug-cc-PVDZ level of theory.Our results show that for the water-catalyzed hydrolysis of SO2(SO2 + n H2O → H2SO3…(H2O)n-1,n=1-5),the decrease trend in energy barrier becomes little as the number of water molecules is increased,still with an energy barrier of 9.5 kcal/mol for the reaction containing five water molecules.However,ammonia is found to have an enhancing catalytic effect for SO2 hydrolysis in small water clusters(SO2 + nH2O + NH3,n=1-3),substantially lowering the energy barrier from n = 1 to 3,and the ammonia-assisted hydrolysis of SO2 involving three water molecules to form hydrated ammonium bisulfate is a barrierless process.The rate constants analysis of NH3-catalyzed hydrolysis of SO2 combined with the concentration of NH3 in the atmosphere condition demonstrate that the NH3-catalyzed gas-phase SO2 hydrolysis is feasible and could be of great importance for the sink of SO2.Given the importance of SO2 and NH3 in atmospheric aerosols,our results may also give a new insight in understanding the atmospheric nucleation and sulfur-containing aerosol formation.
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