Unravelling the Mechanism of Intermediate-Temperature CO2 Interaction with Molten-NaNO3 -Salt-Promoted MgO
© 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.
Medienart: |
E-Artikel |
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Erscheinungsjahr: |
2022 |
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Erschienen: |
2022 |
Enthalten in: |
Zur Gesamtaufnahme - volume:34 |
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Enthalten in: |
Advanced materials (Deerfield Beach, Fla.) - 34(2022), 4 vom: 01. Jan., Seite e2106677 |
Sprache: |
Englisch |
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Beteiligte Personen: |
Gao, Wanlin [VerfasserIn] |
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Links: |
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Themen: |
CO2 capture |
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Anmerkungen: |
Date Revised 27.01.2022 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
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doi: |
10.1002/adma.202106677 |
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funding: |
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Förderinstitution / Projekttitel: |
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PPN (Katalog-ID): |
NLM332679896 |
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520 | |a 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 | ||
650 | 4 | |a Journal Article | |
650 | 4 | |a CO2 capture | |
650 | 4 | |a MgO carbonation | |
650 | 4 | |a MgO-based adsorbents | |
650 | 4 | |a energy barriers | |
650 | 4 | |a surface defects | |
700 | 1 | |a Xiao, Jiewen |e verfasserin |4 aut | |
700 | 1 | |a Wang, Qiang |e verfasserin |4 aut | |
700 | 1 | |a Li, Shiyan |e verfasserin |4 aut | |
700 | 1 | |a Vasiliades, Michalis A |e verfasserin |4 aut | |
700 | 1 | |a Huang, Liang |e verfasserin |4 aut | |
700 | 1 | |a Gao, Yanshan |e verfasserin |4 aut | |
700 | 1 | |a Jiang, Qian |e verfasserin |4 aut | |
700 | 1 | |a Niu, Yiming |e verfasserin |4 aut | |
700 | 1 | |a Zhang, Bingsen |e verfasserin |4 aut | |
700 | 1 | |a Liu, Yuefeng |e verfasserin |4 aut | |
700 | 1 | |a He, Hong |e verfasserin |4 aut | |
700 | 1 | |a Efstathiou, Angelos M |e verfasserin |4 aut | |
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