Architecturally enhanced pillared porous organic polymers for the removal of organic micropollutants with exceptional Efficiency, rapid Kinetics, and superior adsorption capacity

[Display omitted] •Constructing pillared POPs from acyl-hydrazone-linked COFs using an architecturally enhanced pillar-supported strategy.•Achieved 6.5-fold surface area and 4.5-fold pore volume over parent COFs, with 3D ordered pores and fully exposed adsorption sites.•Exceptional ~100% removal efficiency for 11 OMPs, rapid kinetics (99.9% RhB in 2 min), and high adsorption (1092.9 mg·g−1 MB)•A strategy for novel adsorbents with high crystallinity, customizable functional groups, and advanced application potential. Organic micropollutants (OMPs) pose a significant threat to water quality, endangering human health and ecosystems. The advancement of high-performance adsorbents for the effective removal of organic micropollutants (OMPs) has long been pivotal and widely studied. Despite advances, many porous organic polymers (POPs) face significant challenges in attaining three-dimensional ordered pore structures, enhanced pore properties, and maximally exposed adsorption sites. This study proposes an architecturally enhanced pillar-supported strategy to construct pillared porous organic polymers (PPOPs) from acyl-hydrazone-linked COFs, featuring high crystallinity and customizable functional groups. The pore structure and size distribution of PPOPs are precisely controlled, and the best performing PPOPs achieved a surface area of 1685 m2·g−1 and a pore volume of 1.45 cm3·g−1, 6.5 and 4.5 times higher than parent COFs, which enable them with exceptional removal efficiency, rapid kinetics, and superior adsorption capacity for OMPs.