Title: Following heterogeneous nucleation of CO₂ on H₂O ice nanoparticles with microsecond resolution

Abstract

Heterogeneous nucleation of CO₂ onto H₂O ice particles may play an important role in proposed innovative CO₂ capture technologies, as well as in the formation of Martian clouds. In this work we follow the nucleation/condensation of CO₂/H₂O gas mixtures with microsecond resolution in supersonic Laval nozzles using pressure trace measurement (PTM) and small angle X-ray scattering (SAXS). The latent heat release detected by the PTM reveals that the first phase transition in the expanding CO₂/H₂O mixture is the formation of H₂O ice particles by the homogeneous nucleation/condensation and freezing of H₂O. This is followed by the heterogeneous nucleation and growth of CO₂ on the H₂O ice particles. The onset conditions for heterogeneous nucleation, i.e. the partial pressure of CO₂ and temperature from PTM and the radius of gyration of the H₂O ice particles from SAXS, were determined in the temperature range 124 to 146 K and for particles with radii of gyration in the range of 2.1 to 4.3 nm. The onset conditions suggest that the heterogeneous nucleation of CO₂ may start from the supercooled liquid phase under our conditions. Downstream of the onset point, the partial pressure of CO₂ and temperature rapidly approach the vapor–solid equilibrium line of CO₂,more » showing that even if CO₂ condensation is initiated by heterogeneous nucleation of the liquid phase, it proceeds via growth of the solid.« less

Authors:

Tanimura, Shinobu ^[1]; Park, Yensil ^[1]; Amaya, Andrew ^[1]; Modak, Viraj ^[1]; Wyslouzil, Barbara E. ^[1]

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+ Show Author Affiliations

1. The Ohio State Univ., Columbus, OH (United States)

Publication Date:

Tue Dec 01 00:00:00 EST 2015

Research Org.:

Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS); National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV, and Albany, OR (United States)

Sponsoring Org.:

National Science Foundation (NSF); USDOE Office of Science (SC)

OSTI Identifier:

1238294

Grant/Contract Number:  

FE0013122; CHE-1213959; AC02-06CH11357

Resource Type:

Accepted Manuscript

Journal Name:

RSC Advances

Additional Journal Information:

Journal Volume: 5; Journal Issue: 128; Journal ID: ISSN 2046-2069

Publisher:

Royal Society of Chemistry

Country of Publication:

United States

Language:

ENGLISH

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY