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DOE OSTI · 3013337

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

Yang, Sizhuo [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry]·Mao, Haiyan [Stanford University, CA (United States)]·Dun, Chaochao [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000232156478)·Liu, Jianfang [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000167868873)·Hou, Kaipeng [University of California, Berkeley, CA (United States)]·Cai, Angela [Stanford University, CA (United States)]·Wang, Jing [Stanford University, CA (United States)]·Lee, Jane K. J. [Stanford University, CA (United States)]·Li, Donglin [Stanford University, CA (United States)]·Lyu, Hao [Stanford University, CA (United States)] (ORCID:0000000173932456)·Chen, Zhouyi [Stanford University, CA (United States)]·Lv, Xudong [University of California, Berkeley, CA (United States)]·Zhuang, Hao [University of California, Berkeley, CA (United States)]·Xu, Xueer [Stanford University, CA (United States)]·Zheng, Xueli [Stanford University, CA (United States)] (ORCID:0000000268002649)·Ren, Gang [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000280362321)·Reimer, Jeffrey A. [University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000241913725)·Cui, Yi [Stanford University, CA (United States)] (ORCID:0000000261036352)·Urban, Jeffrey J. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000349092869)

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 2 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 2 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 HNO 3 ) 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.

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Yang, Sizhuo [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry], Mao, Haiyan [Stanford University, CA (United States)], Dun, Chaochao [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000232156478), Liu, Jianfang [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000167868873), Hou, Kaipeng [University of California, Berkeley, CA (United States)], Cai, Angela [Stanford University, CA (United States)], Wang, Jing [Stanford University, CA (United States)], Lee, Jane K. J. [Stanford University, CA (United States)], Li, Donglin [Stanford University, CA (United States)], Lyu, Hao [Stanford University, CA (United States)] (ORCID:0000000173932456), Chen, Zhouyi [Stanford University, CA (United States)], Lv, Xudong [University of California, Berkeley, CA (United States)], Zhuang, Hao [University of California, Berkeley, CA (United States)], Xu, Xueer [Stanford University, CA (United States)], Zheng, Xueli [Stanford University, CA (United States)] (ORCID:0000000268002649), Ren, Gang [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000280362321), Reimer, Jeffrey A. [University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)] (ORCID:0000000241913725), Cui, Yi [Stanford University, CA (United States)] (ORCID:0000000261036352), Urban, Jeffrey J. [Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry] (ORCID:0000000349092869). 2025-11-26. Mesh-like structure integrated core-shell-shell nanocomposites for enhanced stability and performance in carbon capture. https://doi.org/10.1038/s41467-025-65531-3

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