Soot Nanoparticles Could Partake in Nucleation of Biogenic Particles in the Atmosphere: Using Fullerene as a Model Compound

Abstract

The detection of existence of fullerenes (C60 and C70) makes it necessary to explore whether soot nanoparticles can participate in new nanometer-sized particle formation and growth in the atmosphere. This study describes a theoretical investigation at multiple levels on the role of the fullerenes (as model compounds to represent nanoparticles of soot) in the formation of complexes with a common atmospheric nucleating precursor (sulfuric acid, SA) and a biogenic organic acid (cis-pinonic acid, CPA), as well as initial growth of nano-sized biogenic aerosols. Quantum chemical density-functional theory calculations identify the formation of stable fullerene-[CPA-SA] ternary complexes, which likely leads to an enhanced nucleation of SA with CPA. Relevant thermochemical parameters including the changes of Gibbs free energy, enthalpy, and entropy for the complex formation also support that fullerene-[CPA-SA] is most likely to be a newly formed nuclei. The sizes of the critical nucleus of the fullerene-[CPA-SA-H2O] systems were found to be approximately 1.3 nm by large-scale molecular dynamics simulations. This study may provide a new insight into the mechanisms underlying the formation of new particle in the atmospheric environment.

Keywords

• fullerenes
• biogenic particles
• nucleation
• growth
• molecular simulation