Computational fluid dynamics of a cylindrical nucleation flow reactor with detailed cluster thermodynamics.

Particle formation and growth with H(2)SO(4) molecules in an axially symmetric flow reactor was simulated with computational fluid dynamics. A warm (~310 K) gas containing H(2)SO(4) flows into a cooled section (296 K) that induces particle formation. The fluid dynamics gives flow fields, temperatures, and reactant and cluster distributions. Particle formation and growth are simulated with detailed H(2)SO(4) cluster kinetics with chemistry based on measured small cluster thermodynamics and on bulk thermodynamics for large clusters. Results show that particle number densities have power law dependencies on sulfuric acid of ~7, in accord with the thermodynamics of the cluster chemistry. The region where particle formation rates are largest has a temperature that is within 3 K of the wall. Additional simulations show that the H(2)SO(4) concentration in this region is 5 to 10 times greater than the measured H(2)SO(4): this information allows for direct comparisons of experiment and theory. Experiments where ammonia was added as a third nucleating species were simulated with a three-dimensional model. Ammonia was dispersed quickly and particle formation during this mixing was seen to be low. Downstream of the initial mixing region, however, ammonia greatly affected particle formation.