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<p>The homocatenation of electron-deficient Group 13 metals to form metal-metal multiple bonds through covalent self-assembly remains extremely challenging. Herein we demonstrate the synthesis and characterizations of N-heterocyclic carbene (NHC)-stabilized digallyl digallenes (<b>1a</b> and <b>1b</b>), which exhibit unsaturated Ga-Ga=Ga-Ga chains with <i>trans</i>-bent geometries. These compounds were synthesized through salt-metathesis reactions using Cp*Ga, (L<sup>1</sup>)K<sub>2</sub>/(L<sup>2</sup>)Li<sub>2</sub>, and 1,3-diisopropyl-4,5-dimethylimidazol-2-ylidene (I<i>i</i>Pr). Employing both experimental and computational techniques, our investigation reveals that the chain elongation of <b>1a</b> was initiated by the in-situ generation of a gallium(I) carbene analog [(L<sup>1</sup>)GaK]. Additionally, the reactivity of compound <b>1a</b> with I<sub>2</sub>, PhS-SPh, Ph<sub>3</sub>P = S, and Ph<sub>2</sub>C = O was explored, leading to the formation of tetra-gallium subhalides (<b>4</b>), disulfide addition product (<b>5</b>), a gallium thiirane analog (<b>6</b>), and a [2 + 2] cycloaddition product (<b>7</b>), respectively.</p>

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Synthesis, structural characterization, and reactivity of homocatenated Ga₄ complexes with unsaturated Ga–Ga=Ga–Ga chains

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月22日

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  • Ning Zhang,
  • Bing Wang,
  • Yanliang Wu,
  • Wenhao Chen,
  • Shuxia Zhu,
  • Linfang Lu,
  • Zhigang Ni,
  • Di Wu

摘要

The homocatenation of electron-deficient Group 13 metals to form metal-metal multiple bonds through covalent self-assembly remains extremely challenging. Herein we demonstrate the synthesis and characterizations of N-heterocyclic carbene (NHC)-stabilized digallyl digallenes (1a and 1b), which exhibit unsaturated Ga-Ga=Ga-Ga chains with trans-bent geometries. These compounds were synthesized through salt-metathesis reactions using Cp*Ga, (L1)K2/(L2)Li2, and 1,3-diisopropyl-4,5-dimethylimidazol-2-ylidene (IiPr). Employing both experimental and computational techniques, our investigation reveals that the chain elongation of 1a was initiated by the in-situ generation of a gallium(I) carbene analog [(L1)GaK]. Additionally, the reactivity of compound 1a with I2, PhS-SPh, Ph3P = S, and Ph2C = O was explored, leading to the formation of tetra-gallium subhalides (4), disulfide addition product (5), a gallium thiirane analog (6), and a [2 + 2] cycloaddition product (7), respectively.