DescriptionRemoving a large abundant of radioactive 99TcO4- anion from nuclear waste water in Hanford Site is still a very difficult problem remaining to be solved. Functional materials with high stability, anion-exchange capacity, selectivity, and recyclability are eagerly awaited to solve this difficulty. Herein, we report two stable cationic metal-organic frameworks — Zr-tcbp-Me and Zr-tcpp-Me which were synthesized through the tetracarboxylic linkers bonding with zirconium cluster and post-synthetic modification (N-methylation). Both MOFs can retain their crystallinities under harsh condition and have high removability and selectivity towards ReO4- anion, a non-radioactive surrogate of 99TcO4- to be studied. This work represents the highest stability towards the acidic condition that cationic MOFs are used to remove perrhenate from waste water.