Structure of Na Species in Promoted CaO-Based Sorbents and Their Effect on the Rate and Extent of the CO2 Uptake


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Date

2023-10-02

Publication Type

Journal Article

ETH Bibliography

yes

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Abstract

To advance CaO-based CO₂ sorbents it is crucial to understand how their structural parameters control the cyclic CO₂ uptake. Here, CaO-based sorbents with varying ratios of Na₂CO₃:CaCO₃ are synthesized via mechanochemical activation of a mixture of Na₂CO₃ and CaCO₃ to investigate the effect of sodium species on the structure, morphology, carbonation rate and cyclic CO₂ uptake of the CO₂ sorbents. The addition of Na₂CO₃ in the range of 0.1–0.2 mol% improves the CO₂ uptake by up to 80% after 10 cycles when compared to ball-milled bare CaCO₃, while for Na₂CO₃ loadings >0.3 mol% the cyclic CO₂ uptake decreases by more than 40%. Energy dispersive X-ray spectroscopy (EDX), transmission electron microscopy, X-ray absorption spectroscopy (XAS), and ²³Na MAS NMR, reveal that in sorbents with Na₂CO₃ contents <0.3 mol% Na exists in highly distributed, noncrystalline [Na₂Ca(CO₃)₂] units. These species stabilize the surface area of the sorbent in pores of diameters >100 nm, and enhance the diffusion of CO₂ through CaCO₃. For Na₂CO₃ contents >0.3 mol%, the accelerated deactivation of the sorbents via sintering is related to the formation of crystalline Na₂Ca(CO₃)₂ and the high mobility of Na.

Publication status

published

Editor

Book title

Volume

33 (40)

Pages / Article No.

2302916

Publisher

Wiley-VCH

Event

Edition / version

Methods

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Subject

CaO; Na; Na2CO3; promotion; sorbents; species; structures

Organisational unit

03865 - Müller, Christoph R. / Müller, Christoph R. check_circle
03872 - Copéret, Christophe / Copéret, Christophe check_circle

Notes

Funding

819573 - Advancing CO2 Capture Materials by Atomic Scale Design: the Quest for Understanding (EC)
180544 - NCCR Catalysis (phase I) (SNF)

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