Zhang Yiqun, Zhu Yikun, Lan Danni, Pun Sai Ho, Zhou Zheng, Wei Zheng, Wang Ying, Lee Hung Kay, Lin Chao, Wang Jiangpeng, Petrukhina Marina A, Li Quan, Miao Qian
Department of Chemistry, The Chinese University of Hong Kong, Shatin, New Territories, Hong Kong, China.
Department of Chemistry, University at Albany, State University of New York, 1400 Washington Avenue, Albany, New York 12222, United States of America.
J Am Chem Soc. 2021 Apr 7;143(13):5231-5238. doi: 10.1021/jacs.1c01642. Epub 2021 Mar 25.
This study explores a bottom-up approach toward negatively curved carbon allotropes from octabenzo[8]circulene, a negatively curved nanographene. Stepwise chemical reduction reactions of octabenzo[8]circulene with alkali metals lead to a unique highly reduced hydrocarbon pentaanion, which is revealed by X-ray crystallography suggesting a local view for the reduction and alkali metal intercalation processes of negatively curved carbon allotropes. Polymerization of the tetrabromo derivative of octabenzo[8]circulene by the nickel-mediated Yamamoto coupling reaction results in a new type of porous carbon-rich material, which consists of a covalent network of negatively curved nanographenes. It has a specific surface area of 732 m g and functions as anode material for lithium ion batteries exhibiting a maximum capacity of 830 mAh·g at a current density of 100 mA·g. These results indicate that this covalent network presents the key structural and functional features of negatively curved carbon allotropes.
本研究探索了一种从八苯并[8]环轮烯（一种负曲率纳米石墨烯）出发制备负曲率碳同素异形体的自下而上的方法。八苯并[8]环轮烯与碱金属的逐步化学还原反应产生了一种独特的高度还原的烃五价阴离子，X射线晶体学揭示了这一点，这为负曲率碳同素异形体的还原和碱金属嵌入过程提供了局部视角。通过镍介导的山本偶联反应使八苯并[8]环轮烯的四溴衍生物聚合，得到了一种新型的富含碳的多孔材料，它由负曲率纳米石墨烯的共价网络组成。其比表面积为732 m²/g，用作锂离子电池的负极材料，在电流密度为100 mA/g时表现出最大容量830 mAh/g。这些结果表明，这种共价网络呈现了负曲率碳同素异形体的关键结构和功能特征。
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