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Operando modeling and measurements: Powerful tools for revealing the mechanism of alkali carbonate-based

《能源前沿（英文）》 2023年第17卷第3期页码 380-389 doi: 10.1007/s11708-023-0872-x

摘要： 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.

关键词： CO₂ capture carbonation theoretical modeling operando techniques reaction visualization

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Engineering

Raquel Portela, Susana Perez-Ferreras, Ana Serrano-Lotina, Miguel A. Bañares

《化学科学与工程前沿（英文）》 2018年第12卷第3期页码 509-536 doi: 10.1007/s11705-018-1740-9

摘要：

The term operando was coined at the beginning of this century to gather the growing efforts devoted to establish structure-activity relationships by simultaneously characterizing a catalyst performance and the relevant surface chemistry during genuine catalytic operation. This approach is now widespread and consolidated; it has become an increasingly complex but efficient junction where spectroscopy, materials science, catalysis and engineering meet. While for some characterization techniques kinetically relevant reactor cells with good resolution are recently developing, the knowledge gained with magnetic resonance and X-ray and vibrational spectroscopy studies is already huge and the scope of operando methodology with these techniques is recently expanding from studies with small amounts of powdered solids to more industrially relevant catalytic systems. Engineering catalysis implies larger physical domains, and thus all sort of gradients. Space- and time- resolved multi-technique characterization of both the solid and fluid phases involved in heterogeneous catalytic reactions (including temperature data) is key to map processes from different perspectives, which allows taking into account existing heterogeneities at different scales and facing up- and down-scaling for applications ranging from microstructured reactors to industrial-like macroreactors (operating with shaped catalytic bodies and/or in integral regime). This work reviews how operando methodology is evolving toward engineered reaction systems.

关键词： operando structured catalysts space-resolved time-resolved spectroscopy