Probing Mechanistic Insights into Highly Efficient Lithium Storage of C-60 Fullerene Enabled via Three-Electron-Redox Chemistry

Qiu, Haifa1,2; Wan, Jing3; Zhang, Junxian2; Wang, Xin4; Zhang, Nianji2; Chen, Rouxi2; Xia, Yu2; Huang, Li3; Wang, Hsing-Lin1,2,5

2021-07-01

10.1002/advs.202101759

ADVANCED SCIENCE   影响因子和分区

2198-3844

Renewable organic cathodes with abundant elements show promise for sustainable rechargeable batteries. Herein, for the first time, utilizing C-60 fullerene as organic cathode for room-temperature lithium-ion battery is reported. The C-60 cathode shows robust electrochemical performance preferably in ether-based electrolyte. It delivers discharge capacity up to 120 mAh g(-1) and specific energy exceeding 200 Wh kg(-1) with high initial Coulombic efficiency of 91%. The as-fabricated battery holds a capacity of 90 mAh g(-1) after 50 cycles and showcases remarkable rate performance with 77 mAh g(-1) retained at 500 mA g(-1). Noteworthily, three couples of unusual flat voltage plateaus recur at approximate to 2.4, 1.7, and 1.5 V, respectively. Diffusion-dominated three-electron-redox reactions are revealed by cyclic voltammogram and plateau capacities. Intriguingly, it is for the first time unveiled by in situ X-ray diffraction (XRD) that the C-60 cathode underwent three reversible phase transitions during lithiation/delithiation process, except for the initial discharge when irreversible polymerization in between C-60 nanoclusters existed as suggested by the characteristic irreversible peak shifts in both in situ XRD pattern and in situ Raman spectra. Cs-corrected transmission electron microscope corroborated these phase evolutions. Importantly, delithiation potentials derived from density-functional-theory simulation based on proposed phase structures qualitatively consists with experimental ones.

C-60 fullerene lithium storage organic cathode phase transition three-electron-redox

SCI ; EI

英语

第一 ; 通讯

National Key Research and Development Program of China[2018YFB0704100] ; Leading Talents Program of Guangdong Province program[2016LJ06N507] ; Research and Development Program of Guangdong province for Key Areas[2019B010941001] ; Shenzhen Basic Research Fund[CYJ20170817110652558] ; Shenzhen Key Laboratory of Solid State Batteries[ZDSYS20180208184346531] ; Guangdong Provincial Key Laboratory of Energy Materials for Electric Power[2018B030322001]

Chemistry ; Science & Technology - Other Topics ; Materials Science

Chemistry, Multidisciplinary ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary

WOS:000671747400001

WILEY

20212810623407

Cathodes ; Density functional theory ; Electrolytes ; Fullerenes ; Phase structure ; Redox reactions ; Transmission electron microscopy ; X ray diffraction

Electric Batteries and Fuel Cells:702 ; Nanotechnology:761 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Probability Theory:922.1 ; Solid State Physics:933

Web of Science

1.Southern Univ Sci & Technol, Shenzhen Key Lab Solid State Batteries, Shenzhen 518055, Peoples R China
2.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China
3.Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Peoples R China
4.Southern Univ Sci & Technol, Acad Adv Interdisciplinary Studies, Shenzhen 518055, Peoples R China
5.Southern Univ Sci & Technol, Guangdong Prov Key Lab Energy Mat Elect Power, Shenzhen 518055, Peoples R China

Qiu, Haifa,Wan, Jing,Zhang, Junxian,et al. Probing Mechanistic Insights into Highly Efficient Lithium Storage of C-60 Fullerene Enabled via Three-Electron-Redox Chemistry[J]. ADVANCED SCIENCE,2021,8.

Qiu, Haifa.,Wan, Jing.,Zhang, Junxian.,Wang, Xin.,Zhang, Nianji.,...&Wang, Hsing-Lin.(2021).Probing Mechanistic Insights into Highly Efficient Lithium Storage of C-60 Fullerene Enabled via Three-Electron-Redox Chemistry.ADVANCED SCIENCE,8.

Qiu, Haifa,et al."Probing Mechanistic Insights into Highly Efficient Lithium Storage of C-60 Fullerene Enabled via Three-Electron-Redox Chemistry".ADVANCED SCIENCE 8(2021).