Stability-first design of carbon-encapsulated Fe3O4 for cyclic regeneration of acidic coordination desulfurization liquors
摘要
Using a non-aqueous desulfurization solution based on coordination interactions to capture hydrogen sulfide is a promising method, and it does not lead to the precipitation of sulfur. However, due to the low efficiency of oxidation regeneration under strong acidic conditions, its practical application has been hindered. To address this bottleneck, we developed a carbon-encapsulated iron catalyst designed to facilitate heterogeneous O2-driven regeneration while maintaining exceptional acid resistance. This catalyst was synthesized via a conformal resorcinol–formaldehyde coating on hydrothermally prepared Fe2O3 nanoparticles, followed by a controlled carbonization process. This approach yields a robust core–shell architecture, where a mixed-valence Fe3O4 core is shielded by a continuous carbon sheath. Systematic phase analysis reveals that a calcination temperature of 550 °C is critical for stabilizing the Fe3O4 phase, whereas excessive temperatures trigger over-reduction to metallic iron. In subsequent regeneration trials, the carbon-coated Fe3O4 significantly accelerated the recovery of the oxidation–reduction potential (ORP) during O2 aeration, effectively restoring the H2S absorption capacity of the liquor. Crucially, the post-reaction characteristic analysis has highlighted the durability of this design: the morphology and surface integrity of the catalyst remained intact after five cycles, and the loss of iron elements was only 0.71%. These findings highlight carbon encapsulation as a useful strategy for integrating efficient interfacial redox catalysis with long-term structural stability in corrosive acidic environments.