Abstract

EPR and ENDOR investigations have been carried out on polycrystalline samples of self( α)-irradiated PuO 2C 2O 4·3H 2O (cumulative dose = 1 MGy). The 239Pu ( I=1/2) hyperfine structure on the EPR signal of the CO 2 − radical ion has given clear evidence for participation of 5f electrons of 239Pu in chemical bonding. The ENDOR spectra were used to identify unambiguously the hyperfine interaction between the unpaired electron on the CO 2 − radical ion and the nuclear spin of 239Pu. In addition to the CO 2 − radical ion, EPR evidence was also obtained for the formation of O 2 − during the autoradiolysis of PuO 2C 2O 4·3H 2O.

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