两种亚稳态内嵌金属富勒烯 Sc2C2@C1(39656)-C82 和 Sc2C2@C1(51383)-C84：来自其最稳定前体的直接 C2 插入产物,Journal of the American Chemical Society

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两种亚稳态内嵌金属富勒烯 Sc2C2@C1(39656)-C82 和 Sc2C2@C1(51383)-C84：来自其最稳定前体的直接 C2 插入产物
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-07-05 , DOI: 10.1021/jacs.3c04840
Yang-Rong Yao _{1,

2} , Zuo-Chang Chen ₁ , Lingfang Chen ₁ , Shan-Yu Zheng ₁ , Shangfeng Yang ₂ , Shun-Liu Deng ₁ , Luis Echegoyen ₃ , Yuan-Zhi Tan ₁ , Su-Yuan Xie ₁ , Lan-Sun Zheng ₁

Affiliation

内嵌金属富勒烯（EMF）是具有多种应用的亚纳米碳材料，但其形成机制，特别是亚稳态异构体的形成机制仍然不明确。目前的理论方法主要关注最稳定的异构体，由于其稳定性和产率较低，导致亚稳态异构体的可预测性有限。在此，我们报告了两种亚稳态电磁场 Sc ₂ C ₂ @ C ₁ (39656)-C ₈₂和 Sc ₂ C ₂ @ C ₁ (51383)-C ₈₄的成功分离和表征，这违反了孤立五边形规则（IPR））。这两个非 IPR EMF 表现出罕见的平面和三角旗状 Sc ₂ C ₂团簇，可以将其视为常见蝴蝶形和线性构型的混合体。更重要的是，理论结果表明，尽管处于亚稳态，但这两种非 IPR EMF 作为其最稳定前体 Sc ₂ C ₂ @ C _{2 v} (5)-C ₈₀和 Sc ₂ C ₂ @ C _s的产物而得以幸存。 (6)-C ₈₂ ，通过形成后退火阶段期间的C _2插入。我们提出了一种系统的理论方法来预测形成后阶段的亚稳态电动势。明确的分子水平结构证据与理论计算结果相结合，为电磁场的形成机制提供了有价值的见解，揭示了形成后机制作为一种有前景的电磁场合成方法的潜力。

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Two Metastable Endohedral Metallofullerenes Sc2C2@C1(39656)-C82 and Sc2C2@C1(51383)-C84: Direct-C2-Insertion Products from Their Most Stable Precursors

Endohedral metallofullerenes (EMFs) are sub-nano carbon materials with diverse applications, yet their formation mechanism, particularly for metastable isomers, remains ambiguous. The current theoretical methods focus mainly on the most stable isomers, leading to limited predictability of metastable ones due to their low stabilities and yields. Herein, we report the successful isolation and characterization of two metastable EMFs, Sc₂C₂@C₁(39656)-C₈₂ and Sc₂C₂@C₁(51383)-C₈₄, which violate the isolated pentagon rule (IPR). These two non-IPR EMFs exhibit a rare case of planar and pennant-like Sc₂C₂ clusters, which can be considered hybrids of the common butterfly-shaped and linear configurations. More importantly, the theoretical results reveal that despite being metastable, these two non-IPR EMFs survived as the products from their most stable precursors, Sc₂C₂@C_2v(5)-C₈₀ and Sc₂C₂@C_s(6)-C₈₂, via a C₂ insertion during the post-formation annealing stages. We propose a systematic theoretical method for predicting metastable EMFs during the post-formation stages. The unambiguous molecular-level structural evidence, combined with the theoretical calculation results, provides valuable insights into the formation mechanisms of EMFs, shedding light on the potential of post-formation mechanisms as a promising approach for EMF synthesis.

更新日期：2023-07-05

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