文献类型：期刊文献

英文题名：N-Doped Nonalternant Molecular Bowl/Saddle Hybrids

作者：Qiu, Shuhai[1];Chen, Kai[2];Deng, Ziqi[3];Jin, Xuan[4];Li, Zuoyu[5];Liu, Guogang[4];Zhang, Li[4];Jiang, Wei[2];Chen, Teng-Teng[3];Liu, Junzhi[1,6,7,8];Wang, Zhaohui[5]

机构：[1]Univ Hong Kong, Dept Chem, Pokfulam Rd, Hong Kong, Peoples R China;[2]Univ Chinese Acad Sci, Sch Chem Sci, Beijing 100049, Peoples R China;[3]Hong Kong Univ Sci & Technol, Dept Chem, Hong Kong, Peoples R China;[4]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Frontiers Sci Ctr Materiobiol & Dynam Chem, Inst Fine Chem,Sch Chem & Mol Engn,Key Lab Adv Mat, Shanghai 200237, Peoples R China;[5]Tsinghua Univ, Dept Chem, Key Lab Organ Optoelect & Mol Engn, Beijing 100084, Peoples R China;[6]Univ Hong Kong, State Key Lab Synthet Chem, HKU CAS Joint Lab New Mat, Pokfulam Rd, Hong Kong, Peoples R China;[7]Univ Hong Kong, Shanghai Hong Kong Joint Lab Chem Synth, Pokfulam Rd, Hong Kong, Peoples R China;[8]HKU SIRI, Mat Innovat Inst Life Sci & Energy MILES, Shenzhen, Peoples R China

年份：2025

卷号：64

期号：48

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20254119306194);WOS:【SCI-EXPANDED(收录号:WOS:001583639300001)】；

基金：This work was supported by the Hong Kong Research Grants Council (27301720, 17304021, and 17309023), National Natural Science Foundation of China (No.: 22350005, 22235005, and 22122114). J.L. is grateful for the funding from The University of Hong Kong (HKU) and ITC to the SKL. The authors thank the UGC funding administered by HKU for supporting the Time-of-Flight Mass Spectrometry Facilities under the Support for Interdisciplinary Research in Chemical Science. The authors acknowledge the computer cluster (HPC2021) of HKU for generous allocations of computer resources. The work described in this paper was partially supported by a grant from the Co-funding Mechanism on Joint Laboratories with the Chinese Academy of Sciences (CAS) sponsored by the Research Grants Council of the Hong Kong Special Administrative Region, China and the CAS (Project No. JLFS/P-701/24 and Project No. JLFS/P-404/24), Guangdong-Hong Kong Joint Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province (2023B1212120011), and a grant from the NSFC/RGC Joint Research Scheme sponsored by the Research Grants Council of the Hong Kong Special Administrative Region, China and the National Natural Science Foundation of China (Project No. N_HKU753/24, NSFC 22461160284).

语种：英文

外文关键词：Bowl chirality; Molecular bowl; Molecular saddle; N-doping; Nonalternant hydrocarbons

摘要：Herein, we report the straightforward synthesis and properties of N-doped molecular bowl/saddle hybrids with nonalternant topologies via successive palladium-catalyzed annulations. Structural evolutions from twisted, bowl-shaped to bowl/saddle-hybridized structures are involved during the core-expansion process, as confirmed by X-ray crystallographic analyses. Notably, this resultant bowl/saddle-hybridized molecular carbon shows unique molecular dynamics, as revealed by 1H NMR, chiral HPLC analyses and theoretical calculations. These molecules exhibit interesting photophysical properties, including moderate fluorescence quantum yields and narrowband emissions. Steady-state and transient spectroscopy reveal the different photophysical properties in these molecular bowl and bowl/saddle hybrids. Moreover, the molecular bowl/saddle hybrid exhibits the shape-adaptive character, and allow for multiple bindings with fullerene guests in a stoichiometry ratio of 1:3, which is seldomly observed in most nonplanar molecular carbons. This study not only presents an efficient strategy to construct a new family of N-doped nonalternant molecular bowl/saddle hybrids, but also provides insights into molecular design of topological nanocarbons with potential applications of chiral materials and organic electronics.