Hashikawa Yoshifumi, Fujikawa Nana, Murata Yasujiro
Institute for Chemical Research, Kyoto University, Uji, Kyoto 611-0011, Japan.
J Am Chem Soc. 2022 Dec 28;144(51):23292-23296. doi: 10.1021/jacs.2c12259. Epub 2022 Dec 19.
Fullerene-graphene hybrids potentially exhibit unprecedented properties owing to interactive communication between the two units through a linkage. However, most of their discrete molecular structures have been still undisclosed thus far. With the recent rise in the awareness of facile access to molecular nanocarbon hybrids, we showcase novel π-extended fullerenes with a fused pyrazine or imidazole. Owing to the effective planar-curved π-conjugation, their absorption coefficients significantly increased in the visible region. Curiously enough, during the formation of π-extended fullerenes, an in situ generated NH molecule was spontaneously encapsulated inside the fullerene cavity. The NH molecule then underwent a timed orifice-expansion triggered by its sustained release. This is the first demonstration that fullerene captures a reactant inside, suggesting their potential usage for a sustained dosing and/or material delivery toward postfunctionalization of fullerene-graphene hybrids.
富勒烯 - 石墨烯杂化物由于两个单元之间通过连接进行相互作用，可能展现出前所未有的性质。然而，到目前为止，它们的大多数离散分子结构仍未被揭示。随着最近对易于获得分子纳米碳杂化物的认识的提高，我们展示了具有稠合吡嗪或咪唑的新型π - 扩展富勒烯。由于有效的平面 - 弯曲π共轭，它们在可见光区域的吸收系数显著增加。奇怪的是，在π - 扩展富勒烯的形成过程中，一个原位生成的NH分子自发地封装在富勒烯腔内。然后，NH分子通过其持续释放引发定时孔口扩张。这是首次证明富勒烯在内部捕获反应物，表明它们在富勒烯 - 石墨烯杂化物后功能化的持续给药和/或材料递送方面的潜在用途。
