Unravelling the Mechanism of Intermediate-Temperature CO2 Interaction with Molten-NaNO3-Salt-Promoted MgO
Gao, Wanlin1; Xiao, Jiewen1; Wang, Qiang1; Li, Shiyan2; Vasiliades, Michalis A.3; Huang, Liang1; Gao, Yanshan1; Jiang, Qian2; Niu, Yiming4; Zhang, Bingsen4; Liu, Yuefeng2; He, Hong5; Efstathiou, Angelos M.3
Corresponding AuthorWang, Qiang( ; Liu, Yuefeng( ; Efstathiou, Angelos M.(
AbstractThe 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 O-18-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 degrees 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 O-18-NaNO3 (use of O-18(2)) and (COO)-O-16-O-18 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+ horizontal ellipsis O2-] ion pairs preventing the development of an impermeable MgCO3 shell, which largely increases the rate of bulk MgO carbonation.
KeywordCO (2) capture energy barriers MgO-based adsorbents MgO carbonation surface defects
Funding OrganizationNational Natural Science Foundation of China ; LiaoNing Revitalization Talents Program ; CAS Youth Innovation Promotion Association ; University of Cyprus
Indexed BySCI
Funding ProjectNational Natural Science Foundation of China[42075169] ; National Natural Science Foundation of China[U1810209] ; National Natural Science Foundation of China[21872144] ; National Natural Science Foundation of China[21972140] ; LiaoNing Revitalization Talents Program[XLYC1907053] ; CAS Youth Innovation Promotion Association[2018220] ; University of Cyprus
WOS Research AreaChemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
WOS SubjectChemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter
WOS IDWOS:000727236000001
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Cited Times:13[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Corresponding AuthorWang, Qiang; Liu, Yuefeng; Efstathiou, Angelos M.
Affiliation1.Beijing Forestry Univ, Coll Environm Sci & Engn, 35 Qinghua East Rd, Beijing 100083, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
3.Univ Cyprus, Heterogeneous Catalysis Lab, Chem Dept, 1 Univ Ave,Univ Campus, CY-2109 Nicosia, Cyprus
4.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci SYNL, Shenyang 110016, Peoples R China
5.Chinese Acad Sci, Lab Atmospher Environm & Pollut Control, Res Ctr EcoEnvironm Scien, Beijing 100085, Peoples R China
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Gao, Wanlin,Xiao, Jiewen,Wang, Qiang,et al. Unravelling the Mechanism of Intermediate-Temperature CO2 Interaction with Molten-NaNO3-Salt-Promoted MgO[J]. ADVANCED MATERIALS,2021:12.
APA Gao, Wanlin.,Xiao, Jiewen.,Wang, Qiang.,Li, Shiyan.,Vasiliades, Michalis A..,...&Efstathiou, Angelos M..(2021).Unravelling the Mechanism of Intermediate-Temperature CO2 Interaction with Molten-NaNO3-Salt-Promoted MgO.ADVANCED MATERIALS,12.
MLA Gao, Wanlin,et al."Unravelling the Mechanism of Intermediate-Temperature CO2 Interaction with Molten-NaNO3-Salt-Promoted MgO".ADVANCED MATERIALS (2021):12.
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