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<p>Although complexes with monatomic zero-valent main group centers have been reported, diatomic zero-valent complexes are extremely rare and all previously reported examples were stabilized by either carbene or silylene ligands. Here, we present the isolation of diatomic E(0)-E(0) (E = Sn, Pb) species supported by two [N{CH₂CH₂NP<sup>i</sup>Pr₂}₃Sn] fragments. The reaction of trilithium salt N{CH<sub>2</sub>CH<sub>2</sub>NLiP<sup>i</sup>Pr<sub>2</sub>}<sub>3</sub> with SnCl<sub>2</sub> yields complex [N{CH<sub>2</sub>CH<sub>2</sub>NP<sup>i</sup>Pr<sub>2</sub>}<sub>3</sub>]<sub>2</sub>Sn<sub>3</sub> (<b>1</b>) with a Sn<sub>3</sub> chain. The reduction of the mixture of <b>1</b> and SnCl<sub>2</sub> with KC<sub>8</sub> produces the catenated Sn<sub>4</sub> chain [N{CH<sub>2</sub>CH<sub>2</sub>NP<sup>i</sup>Pr<sub>2</sub>}<sub>3</sub>Sn<sub>2</sub>]<sub>2</sub> (<b>2</b>), featuring a diatomic Sn(0)-Sn(0) unit. Further reduction of <b>2</b> with KC<sub>8</sub> yields the alkali metal ion-bridged complex [N{CH<sub>2</sub>CH<sub>2</sub>NP<sup>i</sup>Pr<sub>2</sub>}<sub>3</sub>SnK]<sub>2</sub> (<b>3</b>). Moreover, the reaction of <b>3</b> with PbI<sub>2</sub> and KC<sub>8</sub> affords [N{CH<sub>2</sub>CH<sub>2</sub>NP<sup>i</sup>Pr<sub>2</sub>}<sub>3</sub>SnPb]<sub>2</sub> (<b>4</b>), which can also be generated by the reaction of KC<sub>8</sub> with PbI<sub>2</sub> and [N{CH<sub>2</sub>CH<sub>2</sub>NP<sup>i</sup>Pr<sub>2</sub>}<sub>3</sub>SnLi]<sub>2</sub> (<b>5</b>). Complex <b>4</b> features a diatomic Pb(0)-Pb(0) unit, representing a heavy diatomic zero-valent main group complex. The presence of diatomic E(0)-E(0) (E = Sn, Pb) units in complexes <b>2</b> and <b>4</b>, respectively, is further confirmed by computational studies.</p>

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Isolable zero-valent Ditin(0) and Diplumbum(0) complexes

  • 期刊论文

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  • 发表日期：

    2025年3月16日

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  • Jinghang Shen,
  • Zhengting Zhang,
  • Xiaokang Ke,
  • Luming Peng,
  • Qianyi Zhao,
  • Congqing Zhu,
  • Qin Zhu

摘要

Although complexes with monatomic zero-valent main group centers have been reported, diatomic zero-valent complexes are extremely rare and all previously reported examples were stabilized by either carbene or silylene ligands. Here, we present the isolation of diatomic E(0)-E(0) (E = Sn, Pb) species supported by two [N{CH₂CH₂NPiPr₂}₃Sn] fragments. The reaction of trilithium salt N{CH2CH2NLiPiPr2}3 with SnCl2 yields complex [N{CH2CH2NPiPr2}3]2Sn3 (1) with a Sn3 chain. The reduction of the mixture of 1 and SnCl2 with KC8 produces the catenated Sn4 chain [N{CH2CH2NPiPr2}3Sn2]2 (2), featuring a diatomic Sn(0)-Sn(0) unit. Further reduction of 2 with KC8 yields the alkali metal ion-bridged complex [N{CH2CH2NPiPr2}3SnK]2 (3). Moreover, the reaction of 3 with PbI2 and KC8 affords [N{CH2CH2NPiPr2}3SnPb]2 (4), which can also be generated by the reaction of KC8 with PbI2 and [N{CH2CH2NPiPr2}3SnLi]2 (5). Complex 4 features a diatomic Pb(0)-Pb(0) unit, representing a heavy diatomic zero-valent main group complex. The presence of diatomic E(0)-E(0) (E = Sn, Pb) units in complexes 2 and 4, respectively, is further confirmed by computational studies.