Dependence of the extraction capacity of neutral bidentate organophosphorus compounds on their structure: a quantum chemical study

Correlations between the extraction capacities and molecular structures of organophos� phorus compounds (reagents for extraction of transplutonium elements from spent nuclear fuel) were studied using a quantum chemical approach. The results of calculations are in qualitative agreement with experimental data. The approach proposed can be used for analysis of the extraction properties of all classes of organophosphorus compounds and also for predic� tion of the most efficient organophosphorus extragents with preset properties. Processing of spent nuclear fuel (SNF) in order to extract uranium and plutonium followed by recovery into fresh nuclear fuel is an important step in a closed fuel cycle. At present, the SNF processing technology used in the Russian Federation is based on the PUREX process, 1 which was initially elaborated to provide plutonium ex� traction for military purposes from irradiated uranium lumps. Largescale PUREX processing of SNF for nuclear power engineering, especially at high nuclear fuel burnup, leads to accumulation of large amounts of liquid high� level waste (HLW). 2 Therefore, in connection with an increase in the amount of processed SNF and taking into account toughening of requirements for handling of HLW, in the Russian Federation it is planned to fractionate liquid HLW and extract the Cs, Sr, and longlived ac� tinide fractions in order to provide separate solidification and subsequent longterm storage of the corresponding products. Among methods for HLW fractionation, the leading position is occupied by the extraction techniques involving organophosphorus compounds (OPCs) as the most promising extragents. 3—6 The search for highly efficient OPCs is an urgent sci� entific and practical problem. In particular, it includes establishment of the dependence of the extraction capac�