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<p>Thorium (Th), as the most abundant natural actinide, exhibits typical Lewis hard acid character in coordination chemistry. Constructing extended open frameworks relying, at least partially, on the weak interaction between Th and Lewis soft base (<i>e.g.</i>, N) is rare and challenging. Here, we report a novel topology extension strategy to prepare Th–N bonds supported metal-organic frameworks (MOFs). A predesigned tripodal Y-type linker with two carboxyl ends and one triazole end was selected to match the coordination requirement of the Th<sub>6</sub>O<sub>8</sub> cluster, yielding a rare N-coordinated <b>SCU-323</b>, [Th<sub>6</sub>O<sub>4</sub>(OH)<sub>4</sub>(HCOO)<sub>4</sub>L<sub>4</sub>-(H<sub>2</sub>O)<sub>2</sub>]·4DMF·14H<sub>2</sub>O. The formation of Th–N bonding as an extension of coordination dimensionality is mandatory for connecting a three-dimensional framework, and the asymmetry of the linker endows <b>SCU-323</b> with richer pore properties. Combining both Lewis acid and base sites within pores, the <b>SCU-323</b> showcases not only decent CO<sub>2</sub> adsorption but also efficient catalytic performance for the CO<sub>2</sub> cycloaddition reaction. This work expands the toolkit for designing unconventionally coordinated actinide functional materials.</p>

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Rational design of a rare N-coordinated thorium organic framework for efficient CO2 capture and catalytic conversion

  • 期刊论文

  • 发表日期：

    2025年9月19日

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  • Yingtong Fan,
  • Zhiyong Peng,
  • Zhiwei Li,
  • Sen Mei,
  • Yuhuan Jia,
  • Yang Yang,
  • Liwei Cheng,
  • Jueqiong Wang,
  • Lixi Chen,
  • Yanlong Wang,
  • Shuao Wang

摘要

Thorium (Th), as the most abundant natural actinide, exhibits typical Lewis hard acid character in coordination chemistry. Constructing extended open frameworks relying, at least partially, on the weak interaction between Th and Lewis soft base (e.g., N) is rare and challenging. Here, we report a novel topology extension strategy to prepare Th–N bonds supported metal-organic frameworks (MOFs). A predesigned tripodal Y-type linker with two carboxyl ends and one triazole end was selected to match the coordination requirement of the Th6O8 cluster, yielding a rare N-coordinated SCU-323, [Th6O4(OH)4(HCOO)4L4-(H2O)2]·4DMF·14H2O. The formation of Th–N bonding as an extension of coordination dimensionality is mandatory for connecting a three-dimensional framework, and the asymmetry of the linker endows SCU-323 with richer pore properties. Combining both Lewis acid and base sites within pores, the SCU-323 showcases not only decent CO2 adsorption but also efficient catalytic performance for the CO2 cycloaddition reaction. This work expands the toolkit for designing unconventionally coordinated actinide functional materials.