2026-10-12T19:00:19Z https://api.figshare.com/v2/oai

oai:figshare.com:article/33713844 2026-09-13T17:05:28Z category_4 category_146 category_7 category_272 category_873 category_734 category_931 portal_63 item_type_3 month_year_09_2026

Unveiling the Prediction of Lanthanide Binding Selectivity: Could 4f Electrons be Treated as the Core–Shell? Yangbo Yang (24374339) Yuefeng Zhou (21601243) Jian-Biao Liu (1711108) Jun-Jie Song (16642815) Jun-Bo Lu (2562907) Biochemistry Space Science Medicine Environmental Sciences not elsewhere classified Chemical Sciences not elsewhere classified Biological Sciences not elsewhere classified Information Systems not elsewhere classified throughput computation provides strongly correlated nature present results demonstrate major bottleneck due density functional theory demand careful selection lanthanide separation chemistry lanthanide binding selectivity experimental selectivity trends throughput computational screening core – shell could 4f electrons 4f electrons remains experimental screening lanthanide series computational efficiency reference methods recent resurgence powerful alternative highly localized efficient pathway dynamic correlation core pseudopotentials core pps core approach artificial intelligence active space There has been a recent resurgence of interest in the lanthanide separation chemistry. With the advent of artificial intelligence, the high-throughput computation provides a powerful alternative to experimental screening of extractants. However, the reliable treatment of 4f electrons remains a major bottleneck due to their highly localized and strongly correlated nature. In this work, we systematically benchmark two prominent computational strategies including 4f-in-valence and 4f-in-core for calculating lanthanide binding selectivity. Within the 4f-in-valence framework, density functional theory (DFT) calculations yield irregular energetic trends across the lanthanide series. Multi-configurational and multi-reference methods can replicate the experimental selectivity trends, but they demand careful selection of the active space and the treatment of dynamic correlation, posing considerable computational difficulties. In contrast, the 4f-in-core approach, which excludes the chemically inert 4f orbitals from the valence space via 4f-in-core pseudopotentials (PPs), offers substantial improvements in computational efficiency. More importantly, the present results demonstrate that this scheme reliably reproduces key energetic trends, validating its applicability in non-redox lanthanide separation scenarios. This work establishes an efficient pathway by using 4f-in-core PPs for high-throughput computational screening of selective extractants. 2026-09-13T00:00:00Z Dataset Dataset 10.1021/acs.inorgchem.6c01833.s002 https://figshare.com/articles/dataset/Unveiling_the_Prediction_of_Lanthanide_Binding_Selectivity_Could_4f_Electrons_be_Treated_as_the_Core_Shell_/33713844 CC BY-NC 4.0