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

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 () and Jeffrey J. Urban ()
Additional contact information
Sizhuo Yang: Lawrence Berkeley National Laboratory, The Molecular Foundry
Haiyan Mao: Stanford University, Department of Materials Science and Engineering
Chaochao Dun: Lawrence Berkeley National Laboratory, The Molecular Foundry
Jianfang Liu: Lawrence Berkeley National Laboratory, The Molecular Foundry
Kaipeng Hou: Berkeley, Department of Chemistry, University of California
Angela Cai: Stanford University, Department of Materials Science and Engineering
Jing Wang: Stanford University, Department of Materials Science and Engineering
Jane K. J. Lee: Stanford University, Department of Structural Biology
Donglin Li: Stanford University, Department of Materials Science and Engineering
Hao Lyu: Stanford University, Department of Chemical Engineering
Zhouyi Chen: Stanford University, Department of Materials Science and Engineering
Xudong Lv: University of California, Department of Chemical and Biomolecular Engineering
Hao Zhuang: University of California, Department of Chemical and Biomolecular Engineering
Xueer Xu: Stanford University, Department of Materials Science and Engineering
Xueli Zheng: Stanford University, Department of Materials Science and Engineering
Gang Ren: Lawrence Berkeley National Laboratory, The Molecular Foundry
Jeffrey A. Reimer: University of California, Department of Chemical and Biomolecular Engineering
Yi Cui: Stanford University, Department of Materials Science and Engineering
Jeffrey J. Urban: Lawrence Berkeley National Laboratory, The Molecular Foundry

Nature Communications, 2025, vol. 16, issue 1, 1-11

Abstract: 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 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.

Date: 2025
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DOI: 10.1038/s41467-025-65531-3

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