Piperazine enhancing sulfuric acid-based new particle formation: implications for the atmospheric fate of piperazine

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DOI

  • Fangfang Ma, Dalian Univ Technol, Dalian University of Technology, Sch Environm Sci & Technol, Key Lab Ind Ecol & Environm Engn, Minist Educ
  • ,
  • Hong-Bin Xie, Dalian Univ Technol, Dalian University of Technology, Sch Environm Sci & Technol, Key Lab Ind Ecol & Environm Engn, Minist Educ
  • ,
  • Jonas Elm
  • Jiewen Shen, Dalian Univ Technol, Dalian University of Technology, Sch Environm Sci & Technol, Key Lab Ind Ecol & Environm Engn, Minist Educ
  • ,
  • Jingwen Chen, Dalian Univ Technol, Dalian University of Technology, Sch Environm Sci & Technol, Key Lab Ind Ecol & Environm Engn, Minist Educ
  • ,
  • Hanna Vehkamaki, Univ Helsinki, University of Helsinki, Inst Atmospher & Earth Syst Res Phys

Piperazine (PZ), a cyclic diamine, is one of 160 detected atmospheric amines and an alternative solvent to the widely used monoethanolamine in post-combustion CO2 capture. Participating in H2SO4 (sulfuric acid, SA)-based new particle formation (NPF) could be an important removal pathway for PZ. Here, we employed quantum chemical calculations and kinetics modeling to evaluate the enhancing potential of PZ on SA-based NPF by examining the formation of PZ-SA clusters. The results indicate that PZ behaves more like a monoamine in stabilizing SA and can enhance SA-based NPF at the parts per trillion (ppt) level. The enhancing potential of PZ is less than that of the chainlike diamine putrescine and greater than that of dimethylamine, which is one of the strongest enhancing agents confirmed by ambient observations and experiments. After the initial formation of the (PZ)(1)(SA)(1) cluster, the cluster mainly grows by gradual addition of SA or PZ monomer, followed by addition of (PZ)(1)(SA)(1) cluster. We find that the ratio of PZ removal by NPF to that by the combination of NPF and oxidations is 0.5-0.97 at 278.15 K. As a result, we conclude that participation in the NPF pathway could significantly alter the environmental impact of PZ compared to only considering oxidation pathways.

Original languageEnglish
JournalEnvironmental Science & Technology
Volume53
Issue15
Pages (from-to)8785-8795
ISSN0013-936X
DOIs
Publication statusPublished - Aug 2019

    Research areas

  • GAS-PHASE OXIDATION, IONIZATION MASS-SPECTROMETER, DENSITY-FUNCTIONAL THEORY, OH RADICALS KINETICS, METHANESULFONIC-ACID, OXALIC-ACID, NITRIC-ACID, MOLECULAR-INTERACTIONS, GASEOUS METHYLAMINES, INITIATED OXIDATION

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