Reversible multi-electron redox chemistry of π-conjugated N-containing heteroaromatic molecule-based organic cathodes

Chengxin Peng, Guo-Hong Ning, Jie Su, Guiming Zhong, Wei Tang, Bingbing Tian, Chenliang Su, Dingyi Yu, Lianhai Zu, Jinhu Yang, Man-Fai Ng, Yong-Sheng Hu, Yong Yang (), Michel Armand and Kian Ping Loh ()
Additional contact information
Chengxin Peng: Centre for Advanced 2D Materials and Graphene Research Centre, National University of Singapore
Guo-Hong Ning: Centre for Advanced 2D Materials and Graphene Research Centre, National University of Singapore
Jie Su: Centre for Advanced 2D Materials and Graphene Research Centre, National University of Singapore
Guiming Zhong: State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Collaborative Innovation Center of Chemistry for Energy Materials(iChEM), Xiamen University
Wei Tang: Centre for Advanced 2D Materials and Graphene Research Centre, National University of Singapore
Bingbing Tian: Centre for Advanced 2D Materials and Graphene Research Centre, National University of Singapore
Chenliang Su: Centre for Advanced 2D Materials and Graphene Research Centre, National University of Singapore
Dingyi Yu: Centre for Advanced 2D Materials and Graphene Research Centre, National University of Singapore
Lianhai Zu: Tongji University
Jinhu Yang: Tongji University
Man-Fai Ng: Institute of High Performance Computing, Agency for Science, Technology and Research
Yong-Sheng Hu: Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, School of Physical Sciences, University of Chinese Academy of Sciences
Yong Yang: State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Collaborative Innovation Center of Chemistry for Energy Materials(iChEM), Xiamen University
Michel Armand: Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, School of Physical Sciences, University of Chinese Academy of Sciences
Kian Ping Loh: Centre for Advanced 2D Materials and Graphene Research Centre, National University of Singapore

Nature Energy, 2017, vol. 2, issue 7, 1-9

Abstract: Abstract Even though organic molecules with well-designed functional groups can be programmed to have high electron density per unit mass, their poor electrical conductivity and low cycle stability limit their applications in batteries. Here we report a facile synthesis of π-conjugated quinoxaline-based heteroaromatic molecules (3Q) by condensation of cyclic carbonyl molecules with o-phenylenediamine. 3Q features a number of electron-deficient pyrazine sites, where multiple redox reactions take place. When hybridized with graphene and coupled with an ether-based electrolyte, an organic cathode based on 3Q molecules displays a discharge capacity of 395 mAh g−1 at 400 mA g−1 (1C) in the voltage range of 1.2–3.9 V and a nearly 70% capacity retention after 10,000 cycles at 8 A g−1. It also exhibits a capacity of 222 mAh g−1 at 20C, which corresponds to 60% of the initial specific capacity. Our results offer evidence that heteroaromatic molecules with multiple redox sites are promising in developing high-energy-density, long-cycle-life organic rechargeable batteries.

Date: 2017
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DOI: 10.1038/nenergy.2017.74

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