Li3N is an excellent zero-residue positive electrode pre-lithiation additive to offset the initial lithium loss in lithium-ion capacitors. However, Li3N has an intrinsic problem of poor compatibility with commonly use...Li3N is an excellent zero-residue positive electrode pre-lithiation additive to offset the initial lithium loss in lithium-ion capacitors. However, Li3N has an intrinsic problem of poor compatibility with commonly used aprotic polar solvents in electrode manufacture procedure due to its high reactivity with commonly used solvents like N-methy-2-pyrrolidone(NMP) and etc. It is the Valley of Death between research and large-scale commercialization of Li-ion capacitors using Li3N as prelithiation agent. In this work, Li3N containing electrode is prepared by a commercially adoptable route for the first time, using N,Ndimethylformamide(DMF) to homogenate the electrode slurry. The DMF molecular stabilizing mechanism is confirmed via experiment analysis and DFT simulation, indicating that the dehydrogenation energy for DMF is obviously larger than other commonly used solvents such as NMP and etc. The soft package lithium-ion capacitors(LIC250) with only 12 wt% Li3N addition in AC positive electrode exhibits excellent rate capability, cyclic stability and ultrahigh specific energy. Its specific energy is 2.3 times higher than the Li3N-free devices, with energy retention as high as 90% after 10,000 cycles.展开更多
基金the National Natural Science Foundation of China(51673199 and 51677176)Youth Inn ovation Promotion Association of Chinese Academy of Sciences(2015148)+4 种基金Dalian National Laboratory for Clean Energy(DNL180307)Innovation Foundation of Dalian Institute of Chemical PhysicsChinese Academy of Sciences(ZZBS201615 and ZZBS201708)Dalian Science and Technology Star Program(2016RQ026)The authors also thank Lei Shi for the helpful discussion on Li3N related reaction.
文摘Li3N is an excellent zero-residue positive electrode pre-lithiation additive to offset the initial lithium loss in lithium-ion capacitors. However, Li3N has an intrinsic problem of poor compatibility with commonly used aprotic polar solvents in electrode manufacture procedure due to its high reactivity with commonly used solvents like N-methy-2-pyrrolidone(NMP) and etc. It is the Valley of Death between research and large-scale commercialization of Li-ion capacitors using Li3N as prelithiation agent. In this work, Li3N containing electrode is prepared by a commercially adoptable route for the first time, using N,Ndimethylformamide(DMF) to homogenate the electrode slurry. The DMF molecular stabilizing mechanism is confirmed via experiment analysis and DFT simulation, indicating that the dehydrogenation energy for DMF is obviously larger than other commonly used solvents such as NMP and etc. The soft package lithium-ion capacitors(LIC250) with only 12 wt% Li3N addition in AC positive electrode exhibits excellent rate capability, cyclic stability and ultrahigh specific energy. Its specific energy is 2.3 times higher than the Li3N-free devices, with energy retention as high as 90% after 10,000 cycles.
