Application of quantum mechanical simulations for studying the radiolytic stability of prospective extractants in the nuclear fuel cycle
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Diglycolamides (DGA) play a crucial role in the advanced spent nuclear fuel reprocessing. This work extends the portfolio of theoretically calculated properties of such organic extractants related to the radiolytic stability in the partitioning processes. The radiolytic stability of selected DGA ligands (TMDGA, TEDGA, Me-TEDGA, and Me2-TEDGA) was studied by the theoretical simulation methods based on quantum mechanics. As the most suitable indicator, the calculated Fukui functions were in good correlation with the trend of increased stability with increasing molecular weight. The Fukui charges also brought the explanation why TMDGA most likely does not degrade in the ether group, unlike the other ligands.
KeywordsDiglycolamides Partitioning and transmutation Density functional theory Radiolytic stability Fukui function TEDGA
This work was supported by the GENIORS Project (H2020 Euratom Research and Innovation Programme, No. 755171) and by the Czech Technical University in Prague (Grant No. SGS16/245/OHK4/3T/14). The support is greatly appreciated.
- 11.Frisch MJ, Trucks GW, Schlegel HB, Scuseria GE, Robb MA, Cheeseman JR, Montgomery JA Jr, Vreven T, Kudin KN, Burant JC, Millam JM, Iyengar SS, Tomasi J, Barone V, Mennucci B, Cossi M, Scalmani G, Rega N, Petersson GA, Nakatsuji H, Hada M, Ehara M, Toyota K, Fukuda R, Hasegawa J, Ishida M, Nakajima T, Honda Y, Kitao O, Nakai H, Klene M, Li X, Knox JE, Hratchian HP, Cross JB, Bakken V, Adamo C, Jaramillo J, Gomperts R, Stratmann RE, Yazyev O, Austin AJ, Cammi R, Pomelli C, Ochterski JW, Ayala PY, Morokuma K, Voth GA, Salvador P, Dannenberg JJ, Zakrzewski VG, Dapprich S, Daniels AD, Strain MC, Farkas O, Malick DK, Rabuck AD, Raghavachari K, Foresman JB, Ortiz JV, Cui Q, Baboul AG, Clifford S, Cioslowski J, Stefanov BB, Liu G, Liashenko A, Piskorz P, Komaromi I, Martin RL, Fox DJ, Keith T, Al-Laham MA, Peng CY, Nanayakkara A, Challacombe M, Gill PMW, Johnson B, Chen W, Wong MW, Gonzalez C, Pople JA (2004) Gaussian 09, revision D.01. Gaussian, Inc., WallingfordGoogle Scholar
- 16.Glendening E, Badenhoop J, Reed A, Carpenter J, Bohmann J, Morales C, Landis C, Weinhold F (2013) Natural bond orbital analysis program: Nbo 6.0. Theoretical Chemistry Institute, University of Wisconsin, MadisonGoogle Scholar
- 23.Dean JA (1999) Lange’s handbook of chemistry, 15th edn. McGraw-Hill, New YorkGoogle Scholar