Metal–Organic Frameworks with Tunable Metal Node for Selective Capture and Separation of CO2 and CO from Ternary Blast Furnace Gas Mixtures

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Abstract
The simultaneous capture of carbon dioxide (CO2) and carbon monoxide (CO) from complex industrial gases represents a critical challenge. Designing framework sorbents that combine selective molecular recognition with stability is essential. Herein, a series of anthracene-based metal–organic frameworks (MOFs), M-ABHBs (M = Co, Mg, Mn, and Ni), were successfully synthesized. By regulating metal centers, which leads to different interactions between gases (CO2/CO/N2) and metal–ligand pairs in the framework, excellent CO adsorption selectivity has been discovered. Notably, Mg/Mn-ABHBs allow efficient binary CO2/N2 separation, and Co/Ni-ABHBs enable benchmark ternary CO2/CO/N2 separation by increasing the adsorption affinity toward CO. This unique phenomenon is rare among adsorbents. Such behaviors enable a stepwise separation strategy to selectively capture CO2 and CO from ternary mixtures. Co-ABHB exhibits high selectivity of CO/N2 (13.1), while Mg-ABHB shows high selectivity of CO2/N2 (66.6) and CO2/CO (5.8). In situ DRIFTS and theoretical calculations indicate that the former is the result of the strong interactions of Co-CO in the cavities of Co-ABHB, while Mg sites strongly capture only CO2, not CO. Breakthrough tests show that from a CO2/CO/N2 mixture, M-ABHBs demonstrated excellent separation performance. This work offers a design strategy for efficient carbon capture under complex industrial gas conditions.
Funding Information
  • Natural Science Foundation of Fujian Province (2024N0059)
  • National Natural Science Foundation of China (22494633)
  • National Natural Science Foundation of China (22571304)
  • National Natural Science Foundation of China (52522008)
  • Beijing Nova Program (2024072)
  • Beijing Nova Program (20250484956)

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