期刊
ADVANCED MATERIALS
卷 33, 期 44, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202104039
关键词
hybrid Li; (+) storage mechanism; intercalation pseudocapacitance; organic electrode materials; secondary bonding channels; ultrahigh-capacity electrodes
类别
资金
- National Natural Science Foundation of China [21875155, 21973107, 51675275, 21473119]
- Science & Technology Commission of Shanghai Municipality [18511109400, 18511109402]
- Suzhou Key Laboratory for Advanced Carbon Materials and Wearable Energy Technologies, Suzhou, China
This study demonstrates high-rate Li+ intercalation pseudocapacitance in organic molecular crystals through weak secondary bonding channels, with the heterocyclic organic molecule BPDCA showing exceptional electrochemical performance. This opens a new avenue for developing organic intercalation pseudocapacitive materials via secondary bonding structure design.
Organic electrode materials have shown extraordinary promise for green and sustainable electrochemical energy storage devices, but usually suffer from low specific capacity and poor rate capability, which is largely caused by inactive components and diffusion-controlled Li+ intercalation. Herein, high-rate Li+ intercalation pseudocapacitance in organic molecular crystals is achieved through introducing weak secondary bonding channels, far exceeding their theoretical capacity based on redox chemistry at functional groups. The authors' combined experimentally electrochemical characterization with first-principles calculations show that the heterocyclic organic molecule 2,2 '-bipyridine-4,4 '-dicarboxylic acid (BPDCA) crystal permits a four-electron redox reaction at conventional -C(sic)O and -C(sic)N groups and a six-electron intercalation pseudocapacitance along conjugated alkene hydrogen bonding channels (-H2NC5-HMIDLINE HORIZONTAL ELLIPSISO(sic)C(OH)-) and heterocyclic aromatic stacking channels (-C5H3NMIDLINE HORIZONTAL ELLIPSISNH3C5-). The BPDCA electrode delivers an ultrahigh reversible capacity of 1206 mAh g(-1) at 0.5 A g(-1) and an exceptional rate capability. A 4.8 V high-energy/power-density BPDCA anode-based hybrid Li-ion capacitor is thus realized. This work opens a new avenue for developing organic intercalation pseudocapacitive materials via secondary bonding structure design.
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