The aim of this research is to determine structural systematics of a series of materials with compositions and structures related to the mineral umbite (K2ZrSi3O9·H2O) and some of their products after ion exchange with Sr2+ or Cs+. This work is part of an EPSRC funded proposal to produce and test new materials for removing radioactive Sr and Cs from effluent during future decommissioning and decontamination activities of the UKs legacy nuclear waste. The information on the parent umbite materials and those showing high levels of ion exchange will be correlated to the ion exchange efficacy and with complementary atomistic modelling studies be used to understand how structural changes are linked to ion exchange.