Scalable Carbon Dioxide Capture Using Clay-Derived Zeolites via Atomic Rearrangement.

Effective carbon capture materials are crucial for mitigating climate change and supporting sustainable industrial processes. However, developing scalable, cost-effective adsorbents with high carbon dioxide capacity, superior selectivity, and long-term stability remains a major challenge. Here, we report the scalable synthesis of Linde Type A zeolite via atomic reassembly of halloysite clay using mature industrial processes, achieving a high carbon dioxide adsorption capacity of 5.0 mmol g-1 with good cyclic stability. The transformation from a layered to a cubic framework with enlarged vacant spaces significantly enhances carbon dioxide accommodation. Additionally, the as-prepared zeolite demonstrates outstanding carbon dioxide/nitrogen selectivity (178 for 5% carbon dioxide) and robust thermal stability over multiple adsorption-desorption cycles. In situ tests reveal that adsorption is primarily governed by weakly bound interactions, allowing for the easy regeneration. This study presents a promising and scalable strategy for developing high-performance adsorbents toward gigaton-scale carbon dioxide capture applications.