Younghoon Ko

High-performance silicon-based multicomponent battery anodes produced via synergistic coupling of multifunctional coating layers

Nanostructured Si-based materials are key building blocks for next-generation energy storage devices. To meet the requirements of practical energy storage devices, Si-based materials should exhibit high-power, low volume change, and high tap density. So far, there have been no reliable materials reported satisfying all of these requirements. Here, we report a novel Si-based multicomponent design, in which the Si core is covered with multifunctional shell layers. The synergistic coupling of Si with the multifunctional shell provides vital clues for satisfying all Si anode requirements for practical batteries. The Si-based multicomponent anode delivers a high capacity of ∼1000 mA h g−1, a highly stable cycling retention (∼65% after 1000 cycles at 1 C), an excellent rate capability (∼800 mA h g−1 at 10 C), and a remarkably suppressed volume expansion (12% after 100 cycles). Our synthetic process is simple, low-cost, and safe, facilitating new methods for developing electrode materials for practical energy storage.

Programming galvanostatic rates for fast-charging lithium ion batteries: a graphite case

Galvanostatically induced lithiation of graphite, as a cathodic process of lithium ion batteries during charging, was investigated in situ by galvanostatic electrochemical impedance spectroscopy (GS-EIS). When lithiation is driven by charge rates slow enough for kinetics of the lithiation process to be considered relatively sluggish, charge transfer resistance (RCT) is slightly reduced as lithium ion intercalation proceeds from the dilute stage to stage 2L. Subsequently, RCT begins to increase during transformation of stage 2L to stage 2, followed by an abrupt increase in RCT observed during transition from stage 2 to stage 1, or after the inter-space of graphites is fully filled with lithium ions. As the ratio of charge rate to lithiated graphite increases, the potential responsible for the transition from stage 2L to stage 2 is shifted to more negative values due to significant polarization. Simultaneously, cells reach cut-off potentials before the transition from stage 2 to stage 1 proceeds. Based on the information regarding RCT profiles obtained by galvanostatic charging processes, a charging strategy is programmed with several different charge rates (C-rates). The capacity of lithiation is significantly enhanced by a C-rate switching (CRS) strategy. As a representative example, 75% of available capacity is charged for 50 minutes by a combination of 2 C, 1 C, and 0.5 C. However, only 12% and 51% of graphite is lithiated within the same time duration by a single charge rate of 0.1 C and 0.5 C, respectively.

Enlarging the d-spacing of graphite and polarizing its surface charge for driving lithium ions fast

Lithium ion transport was accelerated within graphite by controlling its d-spacing as well as its functional groups. By oxidizing bare graphite under a mild condition, expanded graphites (EG* where * = functional groups) were obtained with increasing d-spacing from 0.3359 nm to 0.3395 nm as well as with functional groups formed on the plane or at the edges of graphites. The subsequent thermal reduction of EG* led to an insignificant change of d-spacing (0.3390 nm), simultaneously eliminating a portion of the functional groups (EG). The enlargement of d-spacing reduced kinetic hindrance of lithium ion movement within the expanded graphites (EG* and EG) by reserving more space for the ionic transport route. In addition, the activation energy of lithium ion intercalation in EG* was reduced by surface charge polarization of graphites induced by hydrogen bonds between oxygen atoms of carbonates in electrolytes and hydrogen atoms of surface functional groups of the expanded graphites, even if the degree of graphitization decreased. Re-graphitization induced by the subsequent thermal reduction increased delithiation capacities (QdLi) of EG as an anode for lithium ion batteries especially at high currents: QdLi at 50 C = 243 mA h g−1 for EG versus 66 mA h g−1 for bare graphite.