An interactive design for sustainable oxygen capacity in alkali-ion batteries

Abstract

Nonhysteretic and reversible (nHR) oxygen redox is desirable for high-energy-density cathodes in lithium-ion batteries (LIBs); however, serious challenges remain. An interactive design concept that mimics the nHR anionic activity of...

Inconsistency between superstructure stability and long-term cyclability of oxygen redox in Na layered oxides

“…Toward this goal, oxygen anionic redox (OAR) in Li-and Na-ion oxide cathodes has been the topic of sustained interest owing to its ability to furnish extra high-voltage capacity beyond that of the orthodox transition metal (TM) redox. [1][2][3][4] Unfortunately, such extra capacity comes with a price since the OAR-active cathodes typically suffer from sluggish kinetics, huge voltage hysteresis, and persistent voltage fading over cycling. 5,6 In addition, the OAR has been revealed to implicate a series of oxygen-centred structural rearrangements that are thermodynamically favorable, during which its reversibility or cyclability is progressively compromised with prolonged cycling.…”

Unified Interplay of Chemical Bond and Solid‐State Kinetics in Lithium–Sulfur Batteries

“…Phase transition occurs in conjunction with the dynamic variation of the Li concentration throughout the charging and discharging operations. [44][45][46] The three model systems were prepared by chemical alloying, fabrication of a composite, and subsequent in-cell electrochemical reactions. A brief illustration of the chemical reaction is shown in Figure S1 (Supporting Information).…”

Data‐Driven Decoupling Structural Feature Correlation for Harnessing Anionic Capacity in Na Layered Oxide

“…[1][2][3][4][5][6][7][8] The motivation in utilizing the OR for Nabased layered oxides was systematically derived from a well-known Li-excess Mn oxide (Li 2 MnO 3 ) that exhibits the anionic oxidation upon charging for lithium-ion batteries (LIBs), leading to the design of O3-type Na[Li 1/3 Mn 2/3 ]O 2 , operated by the pure oxygen oxidation above ≈4.0 V versus Na + /Na, delivering a high theoretical capacity of 285 mAh g −1 (if all Na ions are used) during desodiation. [9][10][11][12][13][14] This mechanism-driven computational design resulted in the successful synthesis of a Na intercalation cathode, and advanced experimental analyses clearly confirmed that the anionic reaction compensated for the charge imbalance induced by Na extraction from the host material. [15][16][17] Unfortunately, this promising cathode produces undesired electrochemical features, such as a large irreversible capacity and severe voltage drop in the subsequent discharge process after the first activation.…”