Abstract

We developed a 3D-printing technology and printed 3D lithium-ion batteries (LIBs) based on LiFe0.79Mn0.21PO4@C nanocrystal cathodes to achieve both ultrahigh rate and high capacity. Coin cells with 3D-printedcathodes showed impressive electrochemical performance: a capacity of 108.45mAh g-1 at 100C, and reversible capacities of 150.21and 140.67 mAh g-1at 10Cand 20C after 1000cycles.APseudo Two-Dimensional Hidden Markov Model (P2D-HMM) was employed to clarify the relationship between layer number (i.e., thickness) and efficiency porosity of the electrode material and the rate performance and to better understand the mechanism behind both ultrahigh rate and high capacityperformance. The calculations indicate that factors such assolution intrinsic diffusion coefficient, efficiency porosity, and electrode thickness play a dominant role in the equivalent diffusion coefficient with the electrode beyond a certain thickness, which determines the whole kinetic process in LIBs. This fundamental studyshould provide helpful guidance forfuture design of LIBs with both high capacity and rate capability.

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