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Peer-reviewedCC BYACS central science

Outer-Sphere Hydrogen Bonds Amplify Mutual Actinide Separation

  • Bin Li1
  • Zhiyuan Zeng1
  • Ziyi Zhang2,3
  • Yu Kang1
  • Zehui Xu2
  • Xiaoyan Tang3
  • Li Wang2
  • Chao Xu1
  1. 1Institute of Nuclear and New Energy Technology, Tsinghua University, Haidian District, Beijing 100084, China
  2. 2Department of Chemistry, Capital Normal University, Haidian District, Beijing 100048 China
  3. 3Beijing National Laboratory for Molecular Sciences, Key Laboratory of Polymer Chemistry and Physics of Ministry of Education, Center for Soft Matter Science and Engineering, College of Chemistry and Molecular Engineering, Peking University, Haidian District, Beijing 100871, China
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Abstract

Mutual actinide separation is critical for nuclear waste remediation, superheavy-element production, and f-block-element-based radiopharmaceuticals, yet it remains a formidable challenge owing to the high chemical similarity of these elements and the harsh conditions typically encountered, such as high acidity and intense radioactivity. Here, we show that combining lipophilic TODGA with the histidine-decorated hydrophilic ligand Phen-2DIHis enables the efficient separation of Am­(III), Cm­(III), and Cf­(III) under highly acidic conditions. This system provides substantially enhanced separation factors for both Am­(III)/Cf­(III) (383) and Cm­(III)/Cf­(III) (36.9) compared to benchmark methods while maintaining practical metal distributions by directing the targeted actinide ions into opposite phases. Spectroscopic titrations and slope analyses support predominant 1:1 metal–ligand complexation. Theoretical calculations further suggest that nitrate-involved outer-sphere hydrogen bonding from the histidine termini may contribute unexpectedly to the thermodynamic bias for separation processes. These results highlight weak interactions beyond the inner coordination sphere as a critical design handle for mutual actinide separation under strongly acidic conditions.

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Cite

BibTeXRIS
BibTeX
@article{li2026outersphere,
  title = {{Outer-Sphere Hydrogen Bonds Amplify Mutual Actinide Separation}},
  author = {Bin Li and Zhiyuan Zeng and Ziyi Zhang and Yu Kang and Zehui Xu and Xiaoyan Tang and Li Wang and Chao Xu},
  journal = {ACS central science},
  year = {2026},
  month = sep,
  doi = {10.1021/acscentsci.6c01133},
  url = {https://europepmc.org/article/PMC/PMC13720919},
  note = {CC BY},
}
RIS
TY  - JOUR
TI  - Outer-Sphere Hydrogen Bonds Amplify Mutual Actinide Separation
AU  - Bin Li
AU  - Zhiyuan Zeng
AU  - Ziyi Zhang
AU  - Yu Kang
AU  - Zehui Xu
AU  - Xiaoyan Tang
AU  - Li Wang
AU  - Chao Xu
PY  - 2026
DA  - 2026/09/01
JO  - ACS central science
DO  - 10.1021/acscentsci.6c01133
UR  - https://europepmc.org/article/PMC/PMC13720919
AB  - Mutual actinide separation is critical for nuclear waste remediation, superheavy-element production, and f-block-element-based radiopharmaceuticals, yet it remains a formidable challenge owing to the high chemical similarity of these elements and the harsh conditions typically encountered, such as high acidity and intense radioactivity. Here, we show that combining lipophilic TODGA with the histidine-decorated hydrophilic ligand Phen-2DIHis enables the efficient separation of Am­(III), Cm­(III), and Cf­(III) under highly acidic conditions. This system provides substantially enhanced separation factors for both Am­(III)/Cf­(III) (383) and Cm­(III)/Cf­(III) (36.9) compared to benchmark methods while maintaining practical metal distributions by directing the targeted actinide ions into opposite phases. Spectroscopic titrations and slope analyses support predominant 1:1 metal–ligand complexation. Theoretical calculations further suggest that nitrate-involved outer-sphere hydrogen bonding from the histidine termini may contribute unexpectedly to the thermodynamic bias for separation processes. These results highlight weak interactions beyond the inner coordination sphere as a critical design handle for mutual actinide separation under strongly acidic conditions.
SN  - 2374-7943
SN  - 2374-7951
ER  -