Faculty of Natural Sciences

TY - JOUR

T1 - Amine-Enhanced Methanesulfonic Acid-Driven Nucleation

T2 - Predictive Model and Cluster Formation Mechanism

AU - Liu, Yu

AU - Xie, Hong-Bin

AU - Ma, Fangfang

AU - Chen, Jingwen

AU - Elm, Jonas

PY - 2022/5

Y1 - 2022/5

N2 - Atmospheric amines are considered to be an effective enhancer for methanesulfonic acid (MSA)-driven nucleation. However, out of the 195 detected atmospheric amines, the enhancing potential (EP) has so far only been studied for five amines. This severely hinders the understanding of the contribution of amines to MSA-driven nucleation. Herein, a two-step procedure was employed to probe the EP of various amines on MSA-driven nucleation. Initially, the formation free energies (Delta G) of 50 MSA-amine dimer clusters were calculated. Based on the calculated Delta G values, a robust quantitative structure-activity relationship (QSAR) model was built and utilized to predict the Delta G values of the remaining 145 amines. The QSAR model identified two guanidino-containing compounds as the potentially strongest enhancer for MSA-driven nucleation. Second, the EP of guanidino-containing compounds was studied by employing larger clusters and selecting guanidine (Gud) as a representative. The results indicate that Gud indeed has the strongest EP. The Gud- MSA system presents a unique clustering mechanism, proceeding via the initial formation of the (Gud)(1)(MSA)(1) cluster, and subsequently by cluster collisions with either a (Gud)(1)(MSA)(1) or (Gud)(2 )(MSA)(2) cluster. The developed QSAR model and the identification of amines with the strongest EP provide a foundation for comprehensively evaluating the contribution of atmospheric amines to MSA-driven nucleation.

AB - Atmospheric amines are considered to be an effective enhancer for methanesulfonic acid (MSA)-driven nucleation. However, out of the 195 detected atmospheric amines, the enhancing potential (EP) has so far only been studied for five amines. This severely hinders the understanding of the contribution of amines to MSA-driven nucleation. Herein, a two-step procedure was employed to probe the EP of various amines on MSA-driven nucleation. Initially, the formation free energies (Delta G) of 50 MSA-amine dimer clusters were calculated. Based on the calculated Delta G values, a robust quantitative structure-activity relationship (QSAR) model was built and utilized to predict the Delta G values of the remaining 145 amines. The QSAR model identified two guanidino-containing compounds as the potentially strongest enhancer for MSA-driven nucleation. Second, the EP of guanidino-containing compounds was studied by employing larger clusters and selecting guanidine (Gud) as a representative. The results indicate that Gud indeed has the strongest EP. The Gud- MSA system presents a unique clustering mechanism, proceeding via the initial formation of the (Gud)(1)(MSA)(1) cluster, and subsequently by cluster collisions with either a (Gud)(1)(MSA)(1) or (Gud)(2 )(MSA)(2) cluster. The developed QSAR model and the identification of amines with the strongest EP provide a foundation for comprehensively evaluating the contribution of atmospheric amines to MSA-driven nucleation.

KW - atmospheric cluster dynamics simulation

KW - quantum chemical calculation

KW - atmospheric particles

KW - QSAR

KW - guanidine

KW - REACTION-RATE CONSTANTS

KW - PARTICLE FORMATION

KW - SULFURIC-ACID

KW - ORGANIC-CHEMICALS

KW - OXALIC-ACID

KW - PROTON-TRANSFER

KW - GAS-PHASE

KW - AEROSOL

KW - GROWTH

KW - NANOPARTICLES

U2 - 10.1021/acs.est.2c01639

DO - 10.1021/acs.est.2c01639

M3 - Journal article

C2 - 35593326

VL - 56

SP - 7751

EP - 7760

JO - Environmental Science & Technology (Washington)

JF - Environmental Science & Technology (Washington)

SN - 0013-936X

IS - 12

ER -