Technetium-99 (99Tc) is one of the most-problematic
radioisotopes in used nuclear fuel owing to its intrinsic features
of a high fission yield, long half-life, high environmental mobility,
volatile nature during waste vitrification, and its redox interface
capability with actinides during used fuel repossessing. The selective
separation of pertechnetate (TcO4
–) from
legacy nuclear waste and contaminated natural water is therefore highly
desirable but still a significant challenge, because the conditions
of a strong radiation field, high ionic strength, high acidity/alkalinity,
and large amounts of competing anions are often involved in these
systems. Until now, there are a handful of functional materials that
can efficiently remove TcO4
– from nuclear
waste solutions with high uptake capacities, fast kinetics, and good
selectivity, but room still remains to further improve our capabilities
for controlling the contamination/separation of TcO4
–. In this Perspective, we discuss the current state
of the art TcO4
– separation materials
including precipitation agents, reducing materials, ion-exchange resins,
inorganic cationic frameworks, cationic metal–organic frameworks
(MOFs), and cationic polymeric networks (CPNs) materials. The intriguing
separation mechanisms of these materials for TcO4
– are also disclosed, which may hopefully shed light on further development
in this field.