Operando modeling and measurements: Powerful tools for revealing the mechanism of alkali carbonate-based sorbents for CO₂ capture in real conditions

Abstract

Alkali carbonate-based sorbents (ACSs), including Na₂CO₃- and K₂CO₃-based sorbents, are promising for CO₂ capture. However, the complex sorbent components and operation conditions lead to the versatile kinetics of CO₂ sorption on these sorbents. This paper proposed that operando modeling and measurements are powerful tools to understand the mechanism of sorbents in real operating conditions, facilitating the sorbent development, reactor design, and operation parameter optimization. It reviewed the theoretical simulation achievements during the development of ACSs. It elucidated the findings obtained by utilizing density functional theory (DFT) calculations, ab initio molecular dynamics (AIMD) simulations, and classical molecular dynamics (CMD) simulations as well. The hygroscopicity of sorbent and the humidity of gas flow are crucial to shifting the carbonation reaction from the gas−solid mode to the gas−liquid mode, boosting the kinetics. Moreover, it briefly introduced a machine learning (ML) approach as a promising method to aid sorbent design. Furthermore, it demonstrated a conceptual compact operando measurement system in order to understand the behavior of ACSs in the real operation process. The proposed measurement system includes a micro fluidized-bed (MFB) reactor for kinetic analysis, a multi-camera sub-system for 3D particle movement tracking, and a combined Raman and IR sub-system for solid/gas components and temperature monitoring. It is believed that this system is useful to evaluate the real-time sorbent performance, validating the theoretical prediction and promoting the industrial scale-up of ACSs for CO₂ capture.

Key words： CO₂ capture; carbonation; theoretical modeling; operando techniques; reaction visualization

Acknowledgements

This work was supported by the Shanghai Sailing Program (Grant No. 22YF1429600), and the Scientific and Technological Innovation Project of Carbon Emission Peak and Carbon Neutrality of Jiangsu Province (Grant No. BK20220001).

Competing interests

The authors declare that they have no competing interests.

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