High‐Capacity Adsorption and Thermal Destruction Adaptable to PFAS Chain Length via Crystal‐to‐Crystal Transformation of Zirconium–Organic Framework

(Zr-PTA2) with abundant open metal sites (OMS) targets shorter-chain C4 PFAS (375 ± 9 mg/g for perfluorobutanoic acid and 414 ± 41 mg/g for perfluorobutanesulfonic acid), surpassing all previously reported MOFs. Flow-through column tests demonstrate rapid PFAS removal below 4 ng/L. This exceptional performance is due to distinct structural motifs-steric host-guest fit of Zr-PTA1 for long-chain PFAS versus OMS-driven chemisorption of short-chain PFAS by Zr-PTA2. Importantly, the framework facilitates subsequent thermal-catalytic PFAS destruction, achieving 97 ± 5% PFOA degradation efficiency with 79 ± 0.3% fluoride recovery.