Unravelling the Mechanism of Intermediate-Temperature CO2 Interaction with Molten-NaNO3-Salt-Promoted MgO

doi:10.1002/adma.202106677

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	Unravelling the Mechanism of Intermediate-Temperature CO2 Interaction with Molten-NaNO3-Salt-Promoted MgO
	Gao, Wanlin 2; Xiao, Jiewen 2; Wang, Qiang 2; Li, Shiyan 3; Vasiliades, Michalis A.4; Huang, Liang 2; Gao, Yanshan 2; Jiang, Qian 3; Niu, Yiming 1; Zhang, Bingsen 1
刊名	ADVANCED MATERIALS
	2021-12-06
页码	12
关键词	CO (2) capture energy barriers MgO-based adsorbents MgO carbonation surface defects
ISSN号	0935-9648
DOI	10.1002/adma.202106677
通讯作者	Wang, Qiang(qiangwang@bjfu.edu.cn) ; Liu, Yuefeng(yuefeng.liu@dicp.ac.cn) ; Efstathiou, Angelos M.(efstath@ucy.ac.cy)
英文摘要	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 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.
资助项目	National 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研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics
语种	英语
出版者	WILEY-V C H VERLAG GMBH
WOS记录号	WOS:000727236000001
资助机构	National Natural Science Foundation of China ; LiaoNing Revitalization Talents Program ; CAS Youth Innovation Promotion Association ; University of Cyprus
内容类型	期刊论文
源URL	[http://ir.imr.ac.cn/handle/321006/167560]
专题	金属研究所_中国科学院金属研究所
通讯作者	Wang, Qiang; Liu, Yuefeng; Efstathiou, Angelos M.
作者单位	1.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci SYNL, Shenyang 110016, Peoples R China 2.Beijing Forestry Univ, Coll Environm Sci & Engn, 35 Qinghua East Rd, Beijing 100083, Peoples R China 3.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China 4.Univ Cyprus, Heterogeneous Catalysis Lab, Chem Dept, 1 Univ Ave,Univ Campus, CY-2109 Nicosia, Cyprus 5.Chinese Acad Sci, Lab Atmospher Environm & Pollut Control, Res Ctr EcoEnvironm Scien, Beijing 100085, Peoples R China
推荐引用方式 GB/T 7714	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.