Unraveling the Role of Aromatic Ring Size in Tuning the Electrochemical Performance of Small-Molecule Imide Cathodes for Lithium-Ion Batteries

Chen, Jingjing1; Gu, Shuai1,2; Hao, Rui1; Liu, Kun1; Wang, Zhiqiang1; Li, Zhiqiang1; Yuan, Huimin1; Guo, Hao1; Zhang, Kaili2; Lu, Zhouguang1

2022-09-01

10.1021/acsami.2c11138

ACS Applied Materials & Interfaces   Impact Factor & Quartile

1944-8244

1944-8252

Organic electrode materials have the typical advantages of flexibility, low cost, abundant resources, and recyclability. However, it is challenging to simultaneously optimize the specific capacity, rate capability, and cycling stability. Radicals are inevitable intermediates that critically determine the redox activity and stability during the electrochemical reaction of organic electrodes. Herein, we select a series of aromatic imides, including pyromellitic diimide (PMDI), 1,4,5,8-naphthalenediimide (NDI), and 3,4,9,10-perylenetetracarboxylicdiimide (PTCDI), which contain different extending pi-conjugated aromatic rings, to study the relationship between their electrochemical performance and the size of the aromatic ring. The results show that regulating the aromatic ring size of imide molecules could finely tune the energies of the lowest unoccupied molecular orbital (LUMO), thus optimizing the redox potential. The rate performance of PMDI, NDI, and PTCDI increases with the aromatic ring size, which is consistent with the decrease in the LUMO-HOMO gap of these imide molecules. DFT calculations and experiments reveal that the redox of imide radicals dominates the charge/discharge processes. Also, extending the aromatic rings could more effectively disperse the spin electron density and improve the stability of imide radicals, contributing to the enhanced cycling stability of these imide electrodes. Hence, aromatic ring size regulation is a simple and novel approach to simultaneously enhance the capacity, rate capability, and cycling stability of organic electrodes for high-performance lithium-ion batteries.

organic electrodes aromatic imides molecular size regulation radical intermediates Li-ion battery

SCI

English

First ; Corresponding

Guangdong-Hong Kong-Macao Joint Laboratory[2019B121205001] ; National Natural Science Foundation of China[21875097] ; Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials[ZDSYS20200421111401738] ; Basic Research Project of the Science and Technology Innovation Commission of Shenzhen[JCYJ20200109141640095] ; Hong Kong Research Grants Council[CityU 11218420] ; Jiangsu Key Laboratory of Electrochemical Energy Storage Technologies[EEST2021-1] ; Stable Support Plan Program of Shenzhen Natural Science Fund[20200925154236004]

Science & Technology - Other Topics ; Materials Science

Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary

WOS:000861860900001

AMER CHEMICAL SOC

Web of Science

1.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen Key Lab Interfacial Sci & Engn Mat, Guangdong Hong Kong Macao Joint Lab Photon Thermal, Hong Kong 518055, Guangdong, Peoples R China
2.City Univ Hong Kong, Dept Mech Engn, Hong Kong 999077, Peoples R China

Chen, Jingjing,Gu, Shuai,Hao, Rui,et al. Unraveling the Role of Aromatic Ring Size in Tuning the Electrochemical Performance of Small-Molecule Imide Cathodes for Lithium-Ion Batteries[J]. ACS Applied Materials & Interfaces,2022.

Chen, Jingjing.,Gu, Shuai.,Hao, Rui.,Liu, Kun.,Wang, Zhiqiang.,...&Lu, Zhouguang.(2022).Unraveling the Role of Aromatic Ring Size in Tuning the Electrochemical Performance of Small-Molecule Imide Cathodes for Lithium-Ion Batteries.ACS Applied Materials & Interfaces.

Chen, Jingjing,et al."Unraveling the Role of Aromatic Ring Size in Tuning the Electrochemical Performance of Small-Molecule Imide Cathodes for Lithium-Ion Batteries".ACS Applied Materials & Interfaces (2022).