Radiation Effects on Zeolite Nanomaterials - Some Potential Implications for Cleaning Liquid Nuclear Waste and for Enhanced Radioactive Decontamination

Abstract

A series of group 1 and group 2 element cation-exchanged samples of zeolite X were prepared and exposed to a beam of spin-polarised, positive muons (of energy 28MeV/c) from a particle accelerator. Longitudinal field repolarisation measurements were made which identified, in each case, both diamagnetic and paramagnetic muon fractions. One of the paramagnetic components revealed a hyperfine field compatible with values reported previously for free muonium atoms (1585 G), while a secondary component was detected showing roughly half the hyperfine coupling measured for atomic muonium, leading to the conclusion that the muonium had become chemically-bound within the zeolite structure, probably via a single-electron bond to a coordinatively unsaturated aluminium atom. A significant “lost fraction” was also indicated along with superhyperfine and anisotropic components that repolarised in weaker magnetic fields (0-100G). As a general trend, the muonium atom yield was found to increase in order of the increasing radius/charge (riz) ratio, though it is constant within the experimental errors, while the chemically bound muonium was formed in similar proportion in all samples (14.1 + 1.9% of the total muonium polarisation), with the exception of HX and the parent NaX (from which the other zeolite samples were prepared by cation-exchange), in which it was absent. Along with data from zero-field experiments which were also undertaken, this is interpreted in terms of an entrapment or effective “scavenging” of radiolytic electrons by the cations (in the order Na+>K+; Mg2+>Ca2+>Sr2+>Ba2+) whose combination with positive muons is therefore impeded, thus reducing the yield of muonium atoms. Results for LiX are anomalous since the muonium yield is greater than expected, possibly due to a greater degree of covalency in the Li-0 bonding than pertains for the other cations. These results may have some implications for zeolites that suffer longterm radiation exposure/damage when they are used to clean radioactive cations (e.g. Cs +, Sr2+) from the waters of nuclear power stations and as materials whose cation-exchange capacity has been deliberately enhanced by prior exposure to ionising radiation.