In situ observation of the electrochemical behavior of Li–CO2/O2 batteries in an environmental transmission electron microscope
Peng Jia,
Yunna Guo,
Dongliang Chen,
Jingming Yao,
Xuedong Zhang,
Jianguo Lu,
Yuqing Qiao,
Liqiang Zhang
Affiliations
Peng Jia
Hebei Key Laboratory of Applied Chemistry College of Environmental and Chemical Engineering Yanshan University Qinhuangdao China
Yunna Guo
State Key Laboratory of Metastable Materials Science and Technology Clean Nano Energy Center Yanshan University Qinhuangdao China
Dongliang Chen
State Key Laboratory of Silicon and Advanced Semiconductor Materials School of Materials Science and Engineering Zhejiang University Hangzhou China
Jingming Yao
State Key Laboratory of Metastable Materials Science and Technology Clean Nano Energy Center Yanshan University Qinhuangdao China
Xuedong Zhang
Key Laboratory of Low Dimensional Materials and Application Technology of Ministry of Education School of Materials Science and Engineering Xiangtan University Xiangtan China
Jianguo Lu
State Key Laboratory of Silicon and Advanced Semiconductor Materials School of Materials Science and Engineering Zhejiang University Hangzhou China
Yuqing Qiao
Hebei Key Laboratory of Applied Chemistry College of Environmental and Chemical Engineering Yanshan University Qinhuangdao China
Liqiang Zhang
State Key Laboratory of Metastable Materials Science and Technology Clean Nano Energy Center Yanshan University Qinhuangdao China
Abstract Li–CO2/O2 batteries, a promising energy storage technology, not only provide ultrahigh discharge capacity but also capture CO2 and turn it into renewable energy. Their electrochemical reaction pathways' ambiguity, however, creates a hurdle for their practical application. This study used copper selenide (CuSe) nanosheets as the air cathode medium in an environmental transmission electron microscope to in situ study Li–CO2/O2 (mix CO2 as well as O2 at a volume ratio of 1:1) and Li–O2 batteries as well as Li–CO2 batteries. Primary discharge reactions take place successively in the Li–CO2/O2–CuSe nanobattery: (I) 4Li+ + O2 + 4e− → 2Li2O; (II) Li2O + CO2 → Li2CO3. The charge reaction proceeded via (III) 2Li2CO3 → 4Li+ + 2CO2 + O2 + 4e−. However, Li–O2 and Li–CO2 nanobatteries showed poor cycling stability, suggesting the difficulty in the direct decomposition of the discharge product. The fluctuations of the Li–CO2/O2 battery's electrochemistry were also shown to depend heavily on O2. The CuSe‐based Li–CO2/O2 battery showed exceptional electrochemical performance. The Li–CO2/O2 battery offered a discharge capacity apex of 15,492 mAh g−1 and stable cycling 60 times at 100 mA g−1. Our research offers crucial insight into the electrochemical behavior of Li–CO2/O2, Li–O2, and Li–CO2 nanobatteries, which may help the creation of high‐performance Li–CO2/O2 batteries for energy storage applications.