Unravelling the Mechanism of Intermediate-Temperature CO2 Interaction with Molten-NaNO3 -Salt-Promoted MgO
© 2021 Wiley-VCH GmbH.
Veröffentlicht in: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 34(2022), 4 vom: 01. Jan., Seite e2106677 |
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1. Verfasser: | |
Weitere Verfasser: | , , , , , , , , , , , |
Format: | Online-Aufsatz |
Sprache: | English |
Veröffentlicht: |
2022
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Zugriff auf das übergeordnete Werk: | Advanced materials (Deerfield Beach, Fla.) |
Schlagworte: | Journal Article CO2 capture MgO carbonation MgO-based adsorbents energy barriers surface defects |
Zusammenfassung: | © 2021 Wiley-VCH GmbH. The optimization of MgO-based adsorbents as advanced CO2 -capture materials is predominantly focused on their molten-salt modification, for which theoretical and experimental contributions provide great insights for their high CO2 -capture performance. The underlying mechanism of the promotion effect of the molten salt on CO2 capture, however, is a topic of controversy. Herein, advanced experimental characterization techniques, including in situ environmental transmission electron microscopy (eTEM) and CO2 chemisorption by diffuse-reflectance infrared Fourier transform spectroscopy (DRIFTS), transient 18 O-isotopic exchange, and density functional theory (DFT), are employed to elucidate the mechanism of the CO2 interaction with molten-salt-modified MgO in the 250-400 °C range. Herein, eTEM studies using low (2-3 mbar) and high (700 mbar) CO2 pressures illustrate the dynamic evolution of the molten NaNO3 salt promoted and unpromoted MgO carbonation with high magnification (<50 nm). The formation of 18 O-NaNO3 (use of 18 O2 ) and C16 O18 O following CO2 interaction, verifies the proposed reaction path: conversion of NO3 - (NO3 - → NO2 + + O2- ), adsorption of NO2 + on MgO with significant weakening of CO2 adsorption strength, and formation of [Mg2+ … O2- ] ion pairs preventing the development of an impermeable MgCO3 shell, which largely increases the rate of bulk MgO carbonation |
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Beschreibung: | Date Revised 27.01.2022 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
ISSN: | 1521-4095 |
DOI: | 10.1002/adma.202106677 |