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Enhanced CO2 capture and separation in two-dimensional carbonaceous materials through Li metal doping and coordination environment modification

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Abstract

As a major greenhouse gas, CO2 significantly contributes to environmental challenges, necessitating advanced capture and separation technologies to mitigate emissions. Herein, we systematically explore CO2 capture and separation using a two-dimensional C2O framework, specifically constructing C2X and Li-doped C2X (X = O, N, CH, B) through Li doping and coordination environment modifications. The study comprehensively analyzes structural stability, pore characteristics, electronic properties, CO2 adsorption capacity and separation performance, gas-structure interactions, and CO2 spatial distribution patterns within both C2X and Li-C2X systems. Results demonstrate that Li-C2X structures exhibit significantly enhanced binding energies of − 1.75 to − 7.81 eV and cohesive energies of 5.91 to 6.77 eV/atom, attributable to the optimized coordination environment promoting strong interactions. Li–C2B achieves an exceptional CO2 adsorption capacity of 12.60 mmol/g at 298 K and 1.0 bar, along with high selectivity for CO2 over N2 of ~ 593 and CH4 of ~ 2109. These results are from the modified coordination environment and Li incorporation. Analyses of CO2 spatial arrangements confirm that electropositive Li atoms, engaging in interactions with electronegative O atoms of CO2, facilitating vertical configurations and compact distributions. These results underscore the ultra-high-performance potential of Li-C2X adsorbents, where coordination environment refinement synergistically enhances CO2 capture and separation efficacy.

Graphical abstract

Strategic dual-Li doping coupled with coordination-engineered 2D carbon frameworks (C2X, X = O/N/CH/B) demonstrates breakthrough CO2 capture and separation performance, where precisely tailored Li-X coordination motifs synergistically enhance adsorbent-adsorbate interactions while achieving remarkable CO2 adsorption capacity and exceptional selectivity.

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Acknowledgments

This work was supported by the National Natural Science Foundation of China (Grant No.12404300) and the Doctoral Research Initiation Fund of Liaoning Province (2024-BS-010) and Interdisciplinary Team Projects under the University Fundamental Research Program (LJ222510140002).

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Authors and Affiliations

  1. School of Physics, Liaoning University, Shenyang, Liaoning, 110036, People’s Republic of China

    Ziyi Han, Sainan Zhou, Tiantian Qiao, Hongyu Pan, Zishuo Zhang & Yongqing Li

  2. School of Materials Science and Engineering, China University of Petroleum, Qingdao, Shandong, 266580, People’s Republic of China

    Xiaoqing Lu

Authors
  1. Ziyi Han
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  2. Sainan Zhou
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  3. Tiantian Qiao
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  4. Hongyu Pan
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  7. Yongqing Li
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Contributions

Ziyi Han: Writing-original draft; Sainan Zhou: Methodology, Writing-review and editing; Tiantian Qiao: Conceptualization; Hongyu Pan: Data curation; Zishuo Zhang: Investigation; Xiaoqing Lu: Software; Yongqing Li: Supervision, Validation, Investigation.

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Correspondence to Yongqing Li.

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Han, Z., Zhou, S., Qiao, T. et al. Enhanced CO2 capture and separation in two-dimensional carbonaceous materials through Li metal doping and coordination environment modification. J Mater Sci (2026). https://doi.org/10.1007/s10853-026-12227-8

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  • DOI: https://doi.org/10.1007/s10853-026-12227-8