首页|Strategies for improving extraction capacity through preorganization structure:A novel 5,6-bicyclicmalonamide extractant(THPPD)
Strategies for improving extraction capacity through preorganization structure:A novel 5,6-bicyclicmalonamide extractant(THPPD)
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Rational design of extractant structure to improve the extraction and separation capacity of rare earth elements(REEs)is a long-standing challenge.Herein,a new strategy was proposed to improve the stability of the chelating structure formed by malonamide and REEs.The stability of the chelating structure is greatly improved by using a double-ring framework structure which makes the two carbonyl groups of malonamide unable to rotate freely and both of them point to the metal ion position.Three benzyl groups were used to construct the hydrophobicity of the extractant and the organic shell of the extracted species.Tribenzylhexahydro-pyrrolo-pyridine-dione(THPPD)was designed and synthesized.The structure reduces the energy consumed by rotating carbonyl group in the coordination with metal ions and then improves the extraction ability of extractant.The crystal structure was preorganized as expected,with the two carbonyls pointing in a favorable coordination direction to the structural com-plement of the metal ion.The extraction behaviors of REEs with THPPD in a nitric acid medium were studied.Compared with N,N'-dibenzyl-N,N'-dimethylmalonamide(DBDM-MA)with a chain structure,the extraction capacity of THPPD is 360 times higher than that of DBDM-MA at 5.0 mol/L sodium nitrate.Furthermore,the binding energy and Gibbs free energy were investigated by density functional theory(DFT)in conjunction with the B3LYP.The theoretical results show that THPPD has more effective interaction with Pr(NO3)3 than DBDM-MA.The construction of chelating groups conformation is a worthy direction to improve the coordination ability and even selectivity of extractant.
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