Citation: Chunhui Wang, Zhe Han, Yuan Gao, Chaoyue Fan, Puyong He, Bojun Li, Dong Ma, Yang Zhang, Lei Zhang, Jie Qiu. Aluminate-mediated assembly of Keggin-type thorium-oxo clusters with a substitutable central octahedron and tunable shell ligands[J]. Chinese Chemical Letters, ;2026, 37(10): 111563. doi: 10.1016/j.cclet.2025.111563 shu

Aluminate-mediated assembly of Keggin-type thorium-oxo clusters with a substitutable central octahedron and tunable shell ligands

Chunhui Wang ^a ,
Zhe Han ^a ,
Yuan Gao ^a ,
Chaoyue Fan ^a ,
Puyong He ^a ,
Bojun Li ^a ,
Dong Ma ^a ,
Yang Zhang ^a ,
Lei Zhang ^b ,
Jie Qiu ^{a, *,}

a.
School of Energy and Power Engineering, Xi'an Jiaotong University, Xi'an 710049, China
b.
Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo 315201, China

qiujie1228@xjtu.edu.cn

Received Date: 26 May 2025
Revised Date: 2 July 2025
Accepted Date: 8 July 2025
Available Online: 8 July 2025

Figures(7)

Metal-oxo clusters (MOCs), particularly those with renowned Keggin-type architecture, have been extensively studied for their facile synthesis, robust stability, and diverse applications. However, the isolation of thorium-oxo clusters with novel structural motifs remains elusive due to the distinctive hydrolytic behaviour of Th⁴⁺ ions. Herein, we report nine electropositive α-Keggin-type thorium-oxo clusters, M@Th₁₂@L₈ (where M is fully or co-occupied by Al³⁺, W⁶⁺, Mo⁶⁺, V⁵⁺, Cr³⁺, or Mn⁴⁺; L = Al or Ga), synthesized via aluminate-regulated Th⁴⁺ hydrolysis. Unlike Th₆(O/OH)₈-based structures for most reported thorium-oxo clusters, M@Th₁₂@L₈ features an unprecedented triple-layered Platonic architecture: a central MO₆ octahedron, a Th₁₂ icosahedron, and an outer cube of eight LO₅ ligands. Structural rigidity maintains invariant M–O bond lengths despite variable MO₆ and LO₅ units, while the central M ion dictates solution pH during cluster formation, crystallization kinetics, crystal yield, and tunable optical properties. Time-resolved small-angle X-ray scattering (SAXS) and ²⁷Al magic-angle spinning (MAS) nuclear magnetic resonance (NMR) unveil the partial decomposition of aluminate precursors and the synchronized self-assembly of M@Th₁₂@L₈. This work advances our understanding of thorium hydrolysis in heterometallic systems and establishes a modular strategy to prepare MOCs with tailored architectures and functionalities.
- Metal-oxo cluster,
- Keggin-type architecture,
- Thorium-oxo cluster,
- Self-assembly,
- Hydrolysis,
- Heterometallic ions
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