Direct air capture of CO2 by metal cation‐exchanged LTA zeolites: Effect of the charge‐to‐size ratio of cations

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Authors

Zeyu Tao, Yuanmeng Tian, Sze Yiu Ou, Qinfen Gu, Jin Shang

First published: 17 May 2023

https://doi.org/10.1002/aic.18139

Abstract

Direct air capture of CO2 (DAC) has been increasingly recognized as a promising carbon‐negative technology. The challenge in deploying energy‐efficient DAC lies in effective sorbent materials. In this research, we comprehensively investigated the DAC behavior of LTA zeolites exchanged with different metal cations (Na+, K+, Mg2+, Ca2+, Mn2+, Co2+, Ni2+, Cu2+, Zn2+, Y3+, La3+, Ce3+, Eu3+, Tb3+, and Yb3+) by both static single‐component gas adsorption and dynamic mixture gas adsorptive separation tests. We found that a large charge‐to‐size ratio of cations is critical to imparting a high DAC capacity of LTA zeolites, which is ascribed to the enhanced electrostatic interaction and/or π‐back bonding toward CO2. Meanwhile, a detrimental effect is associated with an excessively large charge‐to‐size ratio, that is, a significant "shielding effect" of (pre‐) adsorbed contaminants (e.g., H2O and CO2) on cations (e.g., Mn2+ and Mg2+) reduce the accessible CO2 capacity. Ca‐LTA featuring Ca2+ with an appropriate charge‐to‐size ratio exhibits the highest DAC capacity (350 ppm CO2 in the air, 1.20 mmol/g) with fast kinetics and good reusability. These results provide valuable insights for the design of zeolites‐based physisorbents for DAC.

Source: ScienceDirect