Carbonic anhydrase (CA)-mediated carbon conversion and utilization (CCU) technology is recognized as an eco-friendly and cost-effective strategy for carbon reduction. However, the broader application of this technology is significantly constrained by the operational instability and challenging recyclability of free CA. Fortunately, nano-integrated biocatalysis has emerged as an effective solution to these challenges. In this study, we immobilized CA for the first time as a CA-embedded ferriferous oxide-zeolite imidazolium framework-8 (Fe3O4@ZIF-8@CA) nanocomposite enzyme through a one-pot co-precipitation strategy, integrating both the in-situ growth of ZIF-8 around the Fe3O4 core and the immobilization of CA within a single step. Subsequently, this nanocomposite was employed as a nano-integrated biocatalyst to facilitate an innovative CCU pathway. This pathway leverages bicarbonate, produced from the enzymatic hydration of carbon dioxide (CO2), as a substantive uranyl complexing agent to facilitate the neutral leaching of sandstone uranium ore. Systematic characterization techniques, including SEM, TEM, XRD, FTIR, TGA, CLSM, and MPMS, confirmed that Fe3O4@ZIF-8@CA, which possesses a core–shell structure and excellent magnetic responsiveness, has been successfully synthesized. Enzymatic assays revealed that Fe3O4@ZIF-8@CA retains approximately 79% of the activity compared to its free counterparts while demonstrating significantly enhanced thermal and storage stability. The outcome of CO2 hydration conversion for facilitating uranium extraction indicated that, compared with the non-enzymatic reaction group, the bicarbonate yield increased up to 1.5 times, and the uranium extraction efficiency was nearly 10% higher in the Fe3O4@ZIF-8@CA-mediated reaction group. These findings suggest that Fe3O4@ZIF-8@CA possesses excellent catalytic properties for CO2 hydration and can achieve multiplied decarbonization by mediating this innovative CCU pathway. Furthermore, Fe3O4@ZIF-8@CA demonstrated superb reusability and durability, experiencing no significant degradation in its catalytic performance after eight consecutive hydration regeneration cycles. Our research is anticipated to be a viable option for advancing the goals of carbon neutrality and sustainable development.
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