It
is imperative yet challenging to efficiently sequester the 137Cs+ ion from aqueous solutions because of its
highly environmental mobility and extremely high radiotoxicity. The
systematical clarification for underlying mechanism of Cs+ removal and elution at the molecular level is rare. Here, efficient
Cs+ capture is achieved by a thioantimonate [MeNH3]3Sb9S15 (FJSM–SbS) with
high capacity, fast kinetics, wide pH durability, excellent β
and γ radiation resistances, and facile elution. The Cs+ removal is not significantly impacted by coexisting Na+, K+, Ca2+, Mg2+, and Sr2+ ions which is beneficial to the remediation of Cs+-contaminated real waters. Importantly, the mechanism is directly
illuminated by revealing an unprecedented single-crystal to single-crystal
structural transformation upon Cs+ uptake and elution processes.
The superior Cs+ removal results from an unusual synergy
from strong affinity of soft S2– with Cs+, easily exchangeable [MeNH3]+ cations, and
the flexible and robust framework of FJSM–SbS with open windows
as trappers.