Journal
APPLIED SURFACE SCIENCE
Volume 598, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apsusc.2022.153852
Keywords
CO2 sorption; MgO-based sorbent; Elevated operating condition; Cyclic stability; Density functional theory
Categories
Funding
- Zhejiang Provincial Natural Science Foundation [LR20E060001]
- Innovative Research Groups of the National Natural Science Foundation of China [51621005]
- Program of Introducing Talents of Discipline to University (111 Program) [B08026]
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In this study, MgO-Na2CO3-KNO3 sorbents with fast sorption kinetics, high capture capacity, and good cyclic stability at elevated conditions were reported. The results showed that KNO3 is the nitrate species with the highest MgO conversion, and Na2CO3 plays a key role in the initial fast sorption rate. The sorbent with 60 mol% Na2CO3 doping amount achieved the highest MgO conversion.
MgO-based sorbents are promising candidates for precombustion CO2 capture performed at elevated temperature and pressure in thermodynamics, where the development of efficient sorbents is of great importance. Herein, we report MgO-Na2CO3-KNO3 sorbents with fast sorption kinetics, high capture capacity and good cyclic stability at elevated conditions. The effects of nitrate species, Na2CO3 doping amounts and sorption conditions on the MgO conversion were investigated during cyclic test. In comparison with LiNO3 and NaNO3, the sample with KNO3 possesses the highest MgO conversion, which increases from 0.78 to 0.86 after 30 cycles with sorption at 400 ?C, 2 MPa. For nitrate-promoted MgO, Na2CO3 plays an essential role in the initial fast sorption rate. The sorbent with 60 mol%Na2CO3 possesses the highest MgO conversion of 0.89 after 30 cycles. Moreover, during the operation range of 400 degrees C-480 degrees C, 2 MPa, the sorbent exhibits an excellent cyclic stability with porous structure. Density functional theory calculations are further conducted to investigate the mechanism of performance improvement brought by Na2CO(3). We find dissolved CO32- ions will provide chemisorption sites through the formation of C(CO2)-O(CO32-) bonds and can serve as the CO(2 )carrier in molten nitrate salts, thus improving both sorption and diffusion rates of CO2.
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