Insight on the Ultrafast Water Treatment over NiFe-Layered Double Hydroxides via Electroactivation of Ferrate(VI): The Role of Spin State Regulation

Ferrate (Fe(VI)), an emerging green oxidant and disinfectant in water treatment, faces challenges due to its limited reaction efficiency stemming from a highly electron-deficient state. To address this, we designed NiFe-Layered Double Hydroxides (NiFe-LDHs) with different spin states to enhance electron transfer efficiency in Fe(VI)-mediated advanced oxidation processes (AOPs). We hypothesized that fine-tuning the spin state of NiFe-LDHs could optimize the balance between adsorption capabilities and electronic structure regulation. Our experiments revealed that intermediate-spin NiFeLDH-1, with a magnetic moment of 0.67 μB, exhibited the best catalytic performance, achieving 100% phenol removal. The NiFeLDH-x/Fe(VI) system demonstrated a significant synergistic enhancement in degradation efficiency. In addition, NiFeLDH-1 showed excellent performance in stability and continuous flow experiments. This study unveils a novel correlation between spin polarization and catalytic efficiency, offering insights into the optimization of electrocatalysts for Fe(VI)-mediated AOPs. The findings suggest that spin state modulation is a promising strategy to enhance the electrocatalytic activity and stability of non-noble metal catalysts.