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.