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<p>Two-dimensional high-entropy materials offer vast opportunities, yet their low-temperature synthesis with compositional homogeneity and anisotropic morphology remains challenging, due to thermodynamic competition between entropy-driven mixing and strain-induced phase segregation. Here we report a topological anionic confinement strategy that uses MoO<sub>4</sub><sup>2−</sup> tetrahedra as spatially defined scaffolds to suppress cation segregation. This strategy enables the single-step, template-free synthesis of a series of two-dimensional high-entropy molybdate assemblies (M<sub>3</sub>(MoO<sub>4</sub>)<sub>4</sub>·4H<sub>2</sub>O, M = Mn, Fe, Co, Ni, Cu or Zn) at 120 °C. In situ liquid-phase transmission electron microscopy unveils a non-classical crystallization pathway, where metastable clusters undergo a dissolution–regrowth process for compositional homogenization before coalescing via oriented attachment into well-defined nanoplates, a process critically modulated by interfacial energy. This work not only provides a solution to a long-standing synthetic bottleneck but also establishes topological anionic confinement as a versatile method for entropy-stabilized anisotropic nanomaterial design under mild conditions, opening new avenues for diverse functional applications.</p><p></p>

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Topological anionic confinement enables synthesis of 2D high-entropy molybdates under mild conditions

  • 期刊论文

  • 发表日期：

    2026年5月22日

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  • Bin Chen,
  • Qicheng Zhang,
  • Honglin Du,
  • Pengwei Zhao,
  • Weipeng Zhao,
  • Mingjun Cen,
  • Zhuo Chen,
  • Shuya Zhang,
  • Linjie Guan,
  • Yizhe Hu,
  • Tianhao Niu,
  • Lin Gu,
  • Danyun Xu,
  • Wenchao Peng,
  • Yang Li,
  • Junliang Sun,
  • Xiaobin Fan

摘要

Two-dimensional high-entropy materials offer vast opportunities, yet their low-temperature synthesis with compositional homogeneity and anisotropic morphology remains challenging, due to thermodynamic competition between entropy-driven mixing and strain-induced phase segregation. Here we report a topological anionic confinement strategy that uses MoO42− tetrahedra as spatially defined scaffolds to suppress cation segregation. This strategy enables the single-step, template-free synthesis of a series of two-dimensional high-entropy molybdate assemblies (M3(MoO4)4·4H2O, M = Mn, Fe, Co, Ni, Cu or Zn) at 120 °C. In situ liquid-phase transmission electron microscopy unveils a non-classical crystallization pathway, where metastable clusters undergo a dissolution–regrowth process for compositional homogenization before coalescing via oriented attachment into well-defined nanoplates, a process critically modulated by interfacial energy. This work not only provides a solution to a long-standing synthetic bottleneck but also establishes topological anionic confinement as a versatile method for entropy-stabilized anisotropic nanomaterial design under mild conditions, opening new avenues for diverse functional applications.