TY - JOUR
T1 - Redox of Dual-Radical Intermediates in a Methylene-Linked Covalent Triazine Framework for High-Performance Lithium-Ion Batteries
AU - Wang, Zhiqiang
AU - Gu, Shuai
AU - Cao, Lujie
AU - Kong, Long
AU - Wang, Zhenyu
AU - Qin, Ning
AU - Li, Muqing
AU - Luo, Wen
AU - Chen, Jingjing
AU - Wu, Sisi
AU - Liu, Guiyu
AU - Yuan, Huimin
AU - Bai, Yunfei
AU - Zhang, Kaili
AU - Lu, Zhouguang
N1 - Publisher Copyright:
© 2020 American Chemical Society.
PY - 2021/1/13
Y1 - 2021/1/13
N2 - Covalent triazine frameworks (CTFs) are promising electrodes for rechargeable batteries due to their adjustable structures, rich redox sites, and tunable porosity. However, the CTFs usually exhibit inferior electrochemical stability because of the inactivation of the unstable radical intermediates. Here, a methylene-linked CTF has been synthesized and evaluated as a cathode for rechargeable lithium-ion batteries. Electron paramagnetic resonance (EPR) and in situ Raman characterizations demonstrated that the redox activity and reversibility of α-C and triazine radical intermediates are essentially important for the charging/discharging process, which have been efficiently stabilized by the synergetic πconjugation and hindrance effect caused by the adjacent rigid triazine rings and benzene rings in the unique CTF-p framework. Additionally, the methylene groups provided extra redox-active sites. As a result, high capacity and cycling stability were achieved. This work inspires the rational modulation of the radical intermediates to enhance the electrochemical performance of organic electrode materials for the next-generation energy storage devices.
AB - Covalent triazine frameworks (CTFs) are promising electrodes for rechargeable batteries due to their adjustable structures, rich redox sites, and tunable porosity. However, the CTFs usually exhibit inferior electrochemical stability because of the inactivation of the unstable radical intermediates. Here, a methylene-linked CTF has been synthesized and evaluated as a cathode for rechargeable lithium-ion batteries. Electron paramagnetic resonance (EPR) and in situ Raman characterizations demonstrated that the redox activity and reversibility of α-C and triazine radical intermediates are essentially important for the charging/discharging process, which have been efficiently stabilized by the synergetic πconjugation and hindrance effect caused by the adjacent rigid triazine rings and benzene rings in the unique CTF-p framework. Additionally, the methylene groups provided extra redox-active sites. As a result, high capacity and cycling stability were achieved. This work inspires the rational modulation of the radical intermediates to enhance the electrochemical performance of organic electrode materials for the next-generation energy storage devices.
KW - covalent triazine frameworks (CTFs)
KW - lithium-ion storage
KW - organic α-C radical
KW - p-xylylene dicyanide
KW - radical intermediates
UR - http://www.scopus.com/inward/record.url?scp=85098785353&partnerID=8YFLogxK
U2 - 10.1021/acsami.0c17692
DO - 10.1021/acsami.0c17692
M3 - 文章
C2 - 33326203
AN - SCOPUS:85098785353
SN - 1944-8244
VL - 13
SP - 514
EP - 521
JO - ACS Applied Materials and Interfaces
JF - ACS Applied Materials and Interfaces
IS - 1
ER -