Articles | Volume 25, issue 11
https://doi.org/10.5194/acp-25-5695-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-25-5695-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
11 Jun 2025
Research article |
| 11 Jun 2025
| 11 Jun 2025
Enhancing SO3 hydrolysis and nucleation: the role of formic sulfuric anhydride
Rui Wang
Shaanxi Key Laboratory of Catalysis, School of Chemical & Environment Science, Shaanxi University of Technology, Hanzhong, Shaanxi 723001, P. R. China
Rongrong Li
Shaanxi Key Laboratory of Catalysis, School of Chemical & Environment Science, Shaanxi University of Technology, Hanzhong, Shaanxi 723001, P. R. China
Shasha Chen
Shaanxi Key Laboratory of Catalysis, School of Chemical & Environment Science, Shaanxi University of Technology, Hanzhong, Shaanxi 723001, P. R. China
Ruxue Mu
Shaanxi Key Laboratory of Catalysis, School of Chemical & Environment Science, Shaanxi University of Technology, Hanzhong, Shaanxi 723001, P. R. China
Changming Zhang
Shaanxi Key Laboratory of Catalysis, School of Mechanical Engineering, Shaanxi University of Technology, Hanzhong, Shaanxi 723001, P. R. China
Xiaohui Ma
CORRESPONDING AUTHOR
School of Environmental Engineering, Henan University of Technology, Zhengzhou, Henan 450001, P. R. China
Majid Khan
College of Chemistry, Fuzhou University, Fuzhou, Fujian 350116, P. R. China
Tianlei Zhang
CORRESPONDING AUTHOR
Shaanxi Key Laboratory of Catalysis, School of Chemical & Environment Science, Shaanxi University of Technology, Hanzhong, Shaanxi 723001, P. R. China
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In the gaseous reaction, the activation energy for the hydrolysis of HNSO2 catalyzed by MSA was only 0.8 kcal mol−1. Atmospheric Cluster Dynamic Code kinetic simulations disclosed that sulfamic acid markedly enhances the assembly of a methanesulfonic acid–methylamine-based cluster. At the air–water interface, the NH2SO3− and H3O+ ion formation mechanism and the proton exchange mechanism were observed.
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In the gaseous reaction, the activation energy for the hydrolysis of HNSO2 catalyzed by MSA was only 0.8 kcal mol−1. Atmospheric Cluster Dynamic Code kinetic simulations disclosed that sulfamic acid markedly enhances the assembly of a methanesulfonic acid–methylamine-based cluster. At the air–water interface, the NH2SO3− and H3O+ ion formation mechanism and the proton exchange mechanism were observed.
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Short summary
Gaseous results indicated that SO3 hydrolysis with formic sulfuric anhydride (FSA) has a Gibbs free energy barrier as low as 1.5 kcal mol-1 and can effectively compete with other SO3 hydrolysis. Interfacial BOMD (Born–Oppenheimer molecular dynamics) simulations illustrated that FSA-mediated SO3 hydrolysis at the gas–liquid interface occurs through a stepwise mechanism and can be completed within a few picoseconds. ACDC (Atmospheric Clusters Dynamics Code) kinetic simulations indicated that FSA significantly enhances cluster formation rates in the H2SO4–NH3 system.
Gaseous results indicated that SO3 hydrolysis with formic sulfuric anhydride (FSA) has a Gibbs...
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