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<p>Conventional electrolytic methods for separating chemically similar lanthanides (Ln) and actinides (An) are limited by thermodynamics and slow reaction kinetics, restricting their efficiency in rare-earth refining and nuclear fuel recycling. Herein, we report an electroextraction and oxidative back-extraction (EOB) strategy utilizing a LiCl-KCl-KAlCl<sub>4</sub> molten salt that overcomes these limitations by leveraging divergent interfacial reactivity. The EOB process achieves an exceptional separation factor for Ln/An (&gt; 1000), while simultaneously increasing the separation rate by at least one order of magnitude. Through <i>in-situ</i> synchrotron radiation X-ray micro-computed tomography (SR-μCT) and X-ray diffraction (SR-XRD), we capture selective oxidation-induced destabilization of Ln-Al alloys while actinides retain phase stability-directly visualizing the electrochemical alloy transition mechanism. This research redefines the separation of <i>f</i>-block elements in molten salt systems and introduces a multimodal approach to investigating transient interfacial phenomena that are usually inaccessible to conventional metallurgical diagnostics under extreme conditions.</p>

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Direct visualization of f-block elements separation through electrically driven alloy phase transitions

  • 期刊论文

  • 发表日期：

    2025年10月30日

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  • Yuke Zhong,
  • Tan Tan,
  • Kui Liu,
  • Mincheng Yang,
  • Jianrong Zeng,
  • Lin Wang,
  • Shanfeng Wang,
  • Wanxia Huang,
  • Yalan Liu,
  • Dongdong Wang,
  • Weiqun Shi

摘要

Conventional electrolytic methods for separating chemically similar lanthanides (Ln) and actinides (An) are limited by thermodynamics and slow reaction kinetics, restricting their efficiency in rare-earth refining and nuclear fuel recycling. Herein, we report an electroextraction and oxidative back-extraction (EOB) strategy utilizing a LiCl-KCl-KAlCl4 molten salt that overcomes these limitations by leveraging divergent interfacial reactivity. The EOB process achieves an exceptional separation factor for Ln/An (> 1000), while simultaneously increasing the separation rate by at least one order of magnitude. Through in-situ synchrotron radiation X-ray micro-computed tomography (SR-μCT) and X-ray diffraction (SR-XRD), we capture selective oxidation-induced destabilization of Ln-Al alloys while actinides retain phase stability-directly visualizing the electrochemical alloy transition mechanism. This research redefines the separation of f-block elements in molten salt systems and introduces a multimodal approach to investigating transient interfacial phenomena that are usually inaccessible to conventional metallurgical diagnostics under extreme conditions.