Building a Reactive Armor Using S-Doped Graphene for Protecting Potassium Metal Anodes from Oxygen Crossover in K–O2 Batteries
- Kailong HuKailong HuDepartment of Chemistry and Biochemistry, The Ohio State University, 100 West 18th Avenue, Columbus, Ohio 43210, United StatesInstitute of Applied Physics, Graduate School of Pure and Applied Sciences, University of Tsukuba, Tsukuba 305-8573, JapanMore by Kailong Hu,
- Lei QinLei QinDepartment of Chemistry and Biochemistry, The Ohio State University, 100 West 18th Avenue, Columbus, Ohio 43210, United StatesMore by Lei Qin,
- Songwei ZhangSongwei ZhangDepartment of Chemistry and Biochemistry, The Ohio State University, 100 West 18th Avenue, Columbus, Ohio 43210, United StatesMore by Songwei Zhang,
- Jingfeng ZhengJingfeng ZhengDepartment of Chemistry and Biochemistry, The Ohio State University, 100 West 18th Avenue, Columbus, Ohio 43210, United StatesMore by Jingfeng Zheng,
- Jiaonan SunJiaonan SunDepartment of Chemistry and Biochemistry, The Ohio State University, 100 West 18th Avenue, Columbus, Ohio 43210, United StatesMore by Jiaonan Sun,
- Yoshikazu Ito*Yoshikazu Ito*[email protected]Institute of Applied Physics, Graduate School of Pure and Applied Sciences, University of Tsukuba, Tsukuba 305-8573, JapanMore by Yoshikazu Ito, and
- Yiying Wu*Yiying Wu*[email protected]Department of Chemistry and Biochemistry, The Ohio State University, 100 West 18th Avenue, Columbus, Ohio 43210, United StatesMore by Yiying Wu
Abstract

Protecting alkali metals from oxygen crossover is a key unsolved challenge in metal–oxygen batteries. Herein, we report a new “reactive-armor strategy” by using freestanding three-dimensional sulfur (S)-doped graphene with bicontinuous pore channels for protecting potassium (K) anodes from the undesired oxygen crossover. X-ray photoelectron spectroscopy and Fourier-transform infrared results show that the S-dopants react with oxygen/superoxide species to form anionic sulfonate/sulfate that locally promotes the nucleation and growth of KO2. The resultant KO2 layer anchored on the graphene outer surface acts as a barrier layer that prevents oxygen from reaching the K metal surface. After 140 cycles (>550 h), the protected K metal anodes still maintain metallic luster with little accumulation of byproducts. We think the use of organosulfur to build a reactive armor can be applicable to other metal–oxygen batteries in suppressing the parasitic damage from oxygen crossover.
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