Research Article

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2020, 13(12): 3224–3229

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https://doi.org/10.1007/s12274-020-2991-6

An in-situ spectroscopy investigation of alkali metal interaction mechanism with the imide functional group

Xu Lian1, 2, Zhirui Ma1, Zhonghan Zhang3, Jinlin Yang1, 4, Shuo Sun1, Chengding Gu1, Yuan Liu1, 5, Honghe Ding6, Jun Hu6, Xu Cao6, Junfa Zhu6, Shuzhou Li3 (✉), and Wei Chen1, 4, 5, 7 (✉)

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1 Department of Chemistry, National University of Singapore, Singapore 117543, Singapore
2 Centre for Advanced 2D Materials, National University of Singapore, Singapore 117546, Singapore
3 School of Materials Science and Engineering, Nanyang Technological University, Singapore 639798, Singapore
4 National University of Singapore (Suzhou) Research Institute, Suzhou 215123, China
5 Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Fuzhou 350207, China
6 National Synchrotron Radiation Laboratory, Department of Chemical Physics, University of Science and Technology of China, Hefei 230029, China
7 Department of Physics, National University of Singapore, Singapore 117542, Singapore

Keywords: perylene-3,4,9,10-tetracarboxylic diimide (PTCDI), lithium storage, organic anode, imide, electron transfer
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  • Abstract
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Organic anode materials have attracted considerable interest owing to their high tunability by adopting various active functional groups. However, the interaction mechanisms between the alkali metals and the active functional groups in host materials have been rarely studied systematically. Here, a widely used organic semiconductor of perylene-3,4,9,10-tetracarboxylic diimide (PTCDI) was selected as a model system to investigate how alkali metals interact with imide functional groups and induce changes in chemical and electronic structures of PTCDI. The interaction at the alkali/PTCDI interface was probed by in-situ X-ray photoelectron spectroscopy (XPS), ultraviolet photoelectron spectroscopy (UPS), synchrotron-based near edge X-ray absorption fine structure (NEXAFS), and corroborated by density functional theory (DFT) calculations. Our results indicate that the alkali metal replaces the hydrogen atoms in the imide group and interact with the imide nitrogen of PTCDI. Electron transfer induced gap states and downward band-bending like effects are identified on the alkali-deposited PTCDI surface. It was found that Na shows a stronger electron transfer effect than Li. Such a model study of alkali insertion/intercalation in PTCDI gives insights for the exploration of the potential host materials for alkali storage applications.
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An in-situ spectroscopy investigation of alkali metal interaction mechanism with the imide functional group. Nano Res. 2020, 13(12): 3224–3229 https://doi.org/10.1007/s12274-020-2991-6

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