Mesh-like structure integrated core-shell-shell nanocomposites for enhanced stability and performance in carbon capture.

Yang, Sizhuo; Mao, Haiyan; Dun, Chaochao; Liu, Jianfang; Hou, Kaipeng; Cai, Angela; Wang, Jing; Lee, Jane K J et al. · Nat Commun · 2025

basic_science · Level V

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Abstract

Carbon capture is essential for mitigating climate change, yet most sorbents struggle to combine high capacity with chemical stability. Here we report core-shell-shell (CSS) nanocomposites that integrate adsorption efficiency with exceptional robustness. The design couples a metal-organic framework (MOF) core, which enriches local CO<sub>2</sub> concentration, with a polyamine shell that is reorganized into a porous, ordered network through entanglement with an outer covalent organic framework (COF) shell. This hierarchical architecture enables dual amine functionalization via sequential "click" and Schiff-base reactions, achieving a CO<sub>2</sub> uptake of 3.4 mmol g<sup>-1</sup> at 1 bar. The COF outer layer also acts as a protective barrier, suppressing humidity interference and doubling cycling stability under simulated flue gas. Remarkably, the nanocomposites maintain structural integrity after one week in strongly acidic (3 M HNO<sub>3</sub>) or basic (NaOH, pH=14) environments, underscoring their chemical resilience. By uniting high capacity, cycling durability, and environmental tolerance, this CSS strategy offers a versatile platform for next-generation carbon capture materials.