[논문]Redox-Active Phenanthrenequinone Triangles in Aqueous Rechargeable Zinc Batteries

Nam, Kwan Woo; Kim, Heejin; Beldjoudi, Yassine; Kwon, Tae-woo; Kim, Dong Jun; Stoddart, J. Fraser

doi:10.1021/jacs.9b12436

[해외논문] Redox-Active Phenanthrenequinone Triangles in Aqueous Rechargeable Zinc Batteries

Journal of the American Chemical Society, v.142 no.5, 2020년, pp.2541 - 2548

Nam, Kwan Woo (Department of Chemistry , Northwestern University , Evanston , Illinois 60208 , United States) , Kim, Heejin (Division of Analytical Science , Korea Basic Science Institute , 169-148 Gwahak-ro , Yuseong-gu, Daejeon 34133 , Republic of Korea) , Beldjoudi, Yassine (Department of Chemistry , Northwestern University , Evanston , Illinois 60208 , United States) , Kwon, Tae-woo (Department of Chemistry , Northwestern University , Evanston , Illinois 60208 , United States) , Kim, Dong Jun , Stoddart, J. Fraser

Abstract ▼ AI-Helper

Aqueous rechargeable zinc batteries (ZBs) have received considerable attention recently for large-scale energy storage systems in terms of rate performance, cost, and safety. Nevertheless, these ZBs still remain a subject for investigation, as researchers search for cathode materials enabling high performance. Among the various candidate cathode materials for ZBs, quinone compounds stand out as candidates because of their high specific capacity, sustainability, and low cost. Quinone-based cathodes, however, suffer from the critical limitation of undergoing dissolution during battery cycling, leading to a deterioration in battery life. To address this problem, we have introduced a redox-active triangular phenanthrenequinone-based macrocycle (PQ-Δ) with a rigid geometry and layered superstructure. Notably, we have confirmed that Zn2+ ions, together with H2O molecules, can be inserted into the PQ-Δ organic cathode, and, as a consequence, the interfacial resistance between the cathode and electrolytes is decreased effectively. Density functional theory calculations have revealed that the low interfacial resistance can be attributed mainly to decreasing the desolvation energy penalty as a result of the insertion of hydrated Zn2+ ions in the PQ-Δ cathode. The combined effects of the insertion of hydrated Zn2+ ions and the robust triangular structure of PQ-Δ serve to achieve a large reversible capacity of 210 mAh g-1 at a high current density of 150 mA g-1, along with an excellent cycle-life, that is, 99.9% retention after 500 cycles. These findings suggest that the utilization of electron-active organic macrocycles, combined with the low interfacial resistance associated with the solvation of divalent carrier ions, is essential for the overall performance of divalent battery systems.[FIG OMISSION]

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