Open AccessOpportunities and challenges of applying advanced X‐ray spectroscopy to actinide and lanthanide N‐donor ligand systems
Author(s) -
Pruessmann Tim,
Nagel Peter,
Simonelli Laura,
Batchelor David,
Gordon Robert,
Schimmelpfennig Bernd,
Trumm Michael,
Vitova Tonya
Publication year - 2022
Publication title -
journal of synchrotron radiation
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.172
H-Index - 99
ISSN - 1600-5775
DOI - 10.1107/s1600577521012091
Subject(s) - xanes , lanthanide , x ray absorption spectroscopy , actinide , spectroscopy , absorption spectroscopy , chemistry , x ray spectroscopy , ligand (biochemistry) , raman spectroscopy , k edge , pyridine , crystallography , absorption (acoustics) , resolution (logic) , analytical chemistry (journal) , materials science , inorganic chemistry , physics , organic chemistry , ion , optics , biochemistry , receptor , quantum mechanics , composite material , artificial intelligence , computer science
N‐donor ligands such as n ‐Pr‐BTP [2,6‐bis(5,6‐dipropyl‐1,2,4‐triazin‐3‐yl)pyridine] preferentially bind trivalent actinides (An 3+ ) over trivalent lanthanides (Ln 3+ ) in liquid–liquid separation. However, the chemical and physical processes responsible for this selectivity are not yet well understood. Here, an explorative comparative X‐ray spectroscopy and computational ( L 3 ‐edge) study for the An/Ln L 3 ‐edge and the N K ‐edge of [An/Ln( n ‐Pr‐BTP) 3 ](NO 3 ) 3 , [Ln( n ‐Pr‐BTP) 3 ](CF 3 SO 3 ) 3 and [Ln( n ‐Pr‐BTP) 3 ](ClO 4 ) 3 complexes is presented. High‐resolution X‐ray absorption near‐edge structure (HR‐XANES) L 3 ‐edge data reveal additional features in the pre‐ and post‐edge range of the spectra that are investigated using the quantum chemical codes FEFF and FDMNES . X‐ray Raman spectroscopy studies demonstrate the applicability of this novel technique for investigations of liquid samples of partitioning systems at the N K ‐edge.