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Critical Factors Affecting the Catalytic Activity of Redox Mediators on Li-O 2 Battery Discharge.

Yaying DouDongxiao KanYuwei SuYantao ZhangYingjing WeiZhang ZhangZhang Zhang
Published in: The journal of physical chemistry letters (2022)
Redox mediators (RMs) have a substantial ability to govern oxygen reduction reaction (ORR) in Li-O 2 batteries, which can realize large capacity and high-rate capability. However, studies on understanding RM-assisted ORR mechanisms are still in their infancy. Herein, a quinone-based molecule, vitamin K1 (VK1), is first used as the ORR RM for Li-O 2 batteries, together with 2,5-di- tert -butyl-1,4-benzoquinone (DBBQ), to elucidate key factors on the catalytic activity of RMs. By combining experiments and first-principle computations, we demonstrate that the reduced VK1 has strong oxygen affinity and can effectively retard the deposition of Li 2 O 2 films on the electrode surface, thereby guaranteeing enough active sites for electron transfer. Besides, the low reaction free energy of disproportionation of the Li(VK1)O 2 intermediate into Li 2 O 2 also significantly accelerates the ORR process. Consequently, the catalytic activity of VK1 is significantly boosted, and the discharge capacity of VK1-assisted batteries is 3.2-4.5 times that of DBBQ-assisted batteries. This study provides new insight for better understanding the working roles of RMs in Li-O 2 batteries.
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