Diatom-inspired hierarchical carbon catalysts advance sustainable water decontamination via electron transfer-driven peroxide activation.

Catalysts for heterogeneous advanced oxidation processes (AOPs) in water remediation face environmental sustainability challenges, due to the intensive production of catalysts and limited stability of catalysts while maintaining high efficiency. Herein, we design a biomimetic carbon catalyst (BCC) inspired by the diatom frustule valve structure, achieving high environmental sustainability while maintaining superior water decontamination performance by a non-radical direct electron transfer (DET) pathway through activating peracetic acid (PAA). Utilizing a hydrogen-bonding strategy, BCC features pillared layered hierarchical pores with an ultrahigh specific surface area of 2710.35 m g. The nitrogen-doped carbon network combined with the unique diatom-like structure facilitates key DET steps by enhancing PAA adsorption and increasing the oxidation potential of the subsequent surface complex, thereby lowering the DET energy barrier. Additionally, this structure allows target pollutants to deeply penetrate into the hierarchical pores, facilitating enhanced mass transfer and thus reducing catalyst deactivation. Consequently, the BCC/PAA filtration system achieves complete bisphenol A removal with over 50 h of continuous operation under a high membrane permeance (1572 L m h bar). Further, BCC demonstrates a notably reduced global warming potential than state-of-the-art carbon catalysts from a "cradle-to-grave" life cycle assessment, with reductions of 74.9 % in catalyst production and 85.9 % in phenol removal. Our findings offer a facile strategy for designing hierarchical bio-inspired catalysts to boost the environmental sustainability of heterogeneous AOPs.