Iron corrosion in the “inert” supercritical CO2, ab initio dynamics insights: How impurities matter
Abstract
Metal corrosion from exposure to supercritical fluids is a long-standing challenge lacking atomistic understanding for effective corrosion prevention in diverse important applications. Here, in this work, reactions relevant to corrosion in supercritical CO2 (sCO2), with H2O and NO2 as impurities, are revealed using ab initio molecular dynamics and enhanced sampling methods. While little reactivity is observed in bulk sCO2, the iron surface is found to play a crucial almost-catalytic role in its own corrosion, activating the inert CO2 and hence facilitating $$\ast$$HCO3– and $$\ast$$CO32– formation at the interface. Moreover, the hydrogen bond network of $$\ast$$H2O assists the H shuttling to the activated CO2 and impurities, forming reactive species observed in experiments. Such atomistic insight elucidates the reaction mechanisms of metal corrosion in aqueous and supercritical fluids and can point to possible remedies.
- Authors:
-
- Rice Univ., Houston, TX (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
- Sponsoring Org.:
- USDOE Office of Fossil Energy (FE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
- OSTI Identifier:
- 1981703
- Grant/Contract Number:
- AC02-05CH11231; AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Matter (Online)
- Additional Journal Information:
- Journal Name: Matter (Online); Journal Volume: 5; Journal Issue: 2; Journal ID: ISSN 2590-2385
- Publisher:
- Cell Press/Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; ab initio molecular dynamics; corrosion mechanisms; enhanced sampling methods; supercritical fluids; surface reactivity; iron-supercritical carbon dioxide interface; iron surfaces; adsorption; impurities in supercritical carbon dioxide
Citation Formats
Li, Qin-Kun, Kutana, Alex, Penev, Evgeni S., and Yakobson, Boris I. Iron corrosion in the “inert” supercritical CO2, ab initio dynamics insights: How impurities matter. United States: N. p., 2022.
Web. doi:10.1016/j.matt.2021.12.019.
Li, Qin-Kun, Kutana, Alex, Penev, Evgeni S., & Yakobson, Boris I. Iron corrosion in the “inert” supercritical CO2, ab initio dynamics insights: How impurities matter. United States. https://doi.org/10.1016/j.matt.2021.12.019
Li, Qin-Kun, Kutana, Alex, Penev, Evgeni S., and Yakobson, Boris I. Thu .
"Iron corrosion in the “inert” supercritical CO2, ab initio dynamics insights: How impurities matter". United States. https://doi.org/10.1016/j.matt.2021.12.019. https://www.osti.gov/servlets/purl/1981703.
@article{osti_1981703,
title = {Iron corrosion in the “inert” supercritical CO2, ab initio dynamics insights: How impurities matter},
author = {Li, Qin-Kun and Kutana, Alex and Penev, Evgeni S. and Yakobson, Boris I.},
abstractNote = {Metal corrosion from exposure to supercritical fluids is a long-standing challenge lacking atomistic understanding for effective corrosion prevention in diverse important applications. Here, in this work, reactions relevant to corrosion in supercritical CO2 (sCO2), with H2O and NO2 as impurities, are revealed using ab initio molecular dynamics and enhanced sampling methods. While little reactivity is observed in bulk sCO2, the iron surface is found to play a crucial almost-catalytic role in its own corrosion, activating the inert CO2 and hence facilitating $\ast$HCO3– and $\ast$CO32– formation at the interface. Moreover, the hydrogen bond network of $\ast$H2O assists the H shuttling to the activated CO2 and impurities, forming reactive species observed in experiments. Such atomistic insight elucidates the reaction mechanisms of metal corrosion in aqueous and supercritical fluids and can point to possible remedies.},
doi = {10.1016/j.matt.2021.12.019},
journal = {Matter (Online)},
number = 2,
volume = 5,
place = {United States},
year = {Thu Jan 20 00:00:00 EST 2022},
month = {Thu Jan 20 00:00:00 EST 2022}
}
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