期刊
ADVANCED SCIENCE
卷 6, 期 24, 页码 -出版社
WILEY
DOI: 10.1002/advs.201902129
关键词
Ca-ion batteries; calcium intercalation; cointercalation; graphite anodes; organic cathodes
资金
- National Research Foundation of Korea (NRF) - Ministry of Science, ICT and Future [2015M3D1A1069710]
- National Research Foundation of Korea (NRF) - Ministry of Education [NRF-2014R1A6A1030419]
- National Research Foundation of Korea [PAL-2019, 2015M3D1A1069710] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
Herein, graphite is proposed as a reliable Ca2+-intercalation anode in tetraglyme (G(4)). When charged (reduced), graphite accommodates solvated Ca2+-ions (Ca-G(4)) and delivers a reversible capacity of 62 mAh g(-1) that signifies the formation of a ternary intercalation compound, Ca-G(4)center dot C-72. Mass/volume changes during Ca-G(4) intercalation and the evolution of in operando X-ray diffraction studies both suggest that Ca-G(4) intercalation results in the formation of an intermediate phase between stage-III and stage-II with a gallery height of 11.41 angstrom. Density functional theory calculations also reveal that the most stable conformation of Ca-G(4) has a planar structure with Ca2+ surrounded by G(4), which eventually forms a double stack that aligns with graphene layers after intercalation. Despite large dimensional changes during charge/discharge (C/D), both rate performance and cyclic stability are excellent. Graphite retains a substantial capacity at high C/D rates (e.g., 47 mAh g(-1) at 1.0 A g(-1) s vs 62 mAh g(-1) at 0.05 A g(-1)) and shows no capacity decay during as many as 2000 C/D cycles. As the first Ca2+-shuttling calcium-ion batteries with a graphite anode, a full-cell is constructed by coupling with an organic cathode and its electrochemical performance is presented.
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