Harnessing renewable low-cost, bulk wood-structured materials with highly porous, anisotropic and compressible properties that fulfills sustainable water purification is imperative yet still challenging to push forward a circular bioeconomy. In this work, a bimetallic Fe-Co implanted, N-doped wood carbon aerogel (Fe-Co/NWCA) is constructed to guarantee the facile regeneration in high-performance catalytic antibiotic decomposition via activating peroxymonosulfate (PMS). A rapid, reversible and excellent tetracycline (TC) elimination performance (∼90% in 12 min) within a wide pH range of 3–11 is achieved by Fe-Co/NWCA-mediated system. Importantly, the as-prepared hydrophilic Fe-Co/NWCA not only delivers a favorable robustness to interfering anions (e.g., Cl−, H2PO4− and HCO3−), but also presents a superior recyclability with over 90% retention after the fourth cycling operation via a convenient squeezing behavior. Integration of radical quenching experiments and electron paramagnetic resonance demonstrates the participation of reactive oxygen species (ROS) into catalytic TC oxidation, wherein the dominant contributor is 1O2 followed by O2•‾, SO4•‾ and •OH. As an important non-radical route, the directly interfacial electron transfer is confirmed by electrochemical measurements and density-functional-theory computations. In the context of activating PMS, the multi-valent Fe, Co-coordinated species function as the redox reactive site to trigger diversiform ROS with accelerated kinetics, while N, O-associated surface defects and unsaturated functional groups (e.g., −COOH and ketonic C=O) contribute to the 1O2 formation and electron shuttling. This universal approach paves a critical avenue to manufacture the reactive wood-based aerogels with hierarchical microchannels in the practical pollutant remediation, shedding the valuable insights on multifunctional biomass-water nexus.
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