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Formic acid (FA) is a prominent candidate for organic enhanced nucleation due to its high abundance and stabilizing effect on smaller clusters. Its role in new particle formation is studied through the use of state-of-the-art quantum chemical methods on the cluster systems (acid)1-2(FA)1(base)1-2 with the acids being sulfuric acid (SA)/methanesulfonic acid (MSA) and the bases consisting of ammonia (A), methylamine (MA), dimethylamine (DMA), trimethylamine (TMA), and ethylenediamine (EDA). A funneling approach is used to determine the cluster structures with initial configurations generated through the ABCluster program, followed by semiempirical PM7 and ωB97X-D/6-31++G(d,p) calculations. The final binding free energy is calculated at the DLPNO-CCSD(T0)/aug-cc-pVTZ//ωB97X-D/6-31++G(d,p) level of theory using the quasi-harmonic approximation. Cluster dynamics simulations show that FA has a minuscule or negligible effect on the MSA-FA-base systems as well as most of the SA-FA-base systems. The SA-FA-DMA cluster system shows the highest influence from FA with an enhancement of 21%, compared to its non-FA counterpart.
Original language | English |
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Journal | ACS Omega |
Volume | 8 |
Issue | 10 |
Pages (from-to) | 9621-9629 |
Number of pages | 9 |
ISSN | 2470-1343 |
DOIs | |
Publication status | Published - Mar 2023 |
Publisher Copyright:
© 2023 The Authors. Published by American Chemical Society.
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