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<p>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.</p>

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

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年11月26日

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  • Sizhuo Yang,
  • Haiyan Mao,
  • Chaochao Dun,
  • Jianfang Liu,
  • Kaipeng Hou,
  • Angela Cai,
  • Jing Wang,
  • Jane K. J. Lee,
  • Donglin Li,
  • Hao Lyu,
  • Zhouyi Chen,
  • Xudong Lv,
  • Hao Zhuang,
  • Xueer Xu,
  • Xueli Zheng,
  • Gang Ren,
  • Jeffrey A. Reimer,
  • Yi Cui,
  • Jeffrey J. Urban

摘要

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 CO2 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 CO2 uptake of 3.4 mmol g−1 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 HNO3) 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.