Constructing a homogenous and inorganic‐rich solid electrolyte interface (SEI) can efficiently improve the overall sodium‐storage performance of hard carbon (HC) anodes. However, the thick and heterogenous SEI derived from conventional ester electrolytes fails to meet the above requirements. Herein, an innovative interfacial catalysis mechanism is proposed to design a favorable SEI in ester electrolytes by reconstructing the surface functionality of HC, of which abundant CO (carbonyl) bonds are accurately and homogenously implanted. The CO (carbonyl) bonds act as active centers that controllably catalyze the preferential reduction of salts and directionally guide SEI growth to form a homogenous, layered, and inorganic‐rich SEI. Therefore, excessive solvent decomposition is suppressed, and the interfacial Na+ transfer and structural stability of SEI on HC anodes are greatly promoted, contributing to a comprehensive enhancement in sodium‐storage performance. The optimal anodes exhibit an outstanding reversible capacity (379.6 mAh g−1), an ultrahigh initial Coulombic efficiency (93.2%), a largely improved rate capability, and an extremely stable cycling performance with a capacity decay rate of 0.0018% for 10 000 cycles at 5 A g−1. This work provides novel insights into smart regulation of interface chemistry to realize high‐performance HC anodes for sodium storage.
Reducing charge−discharge overpotential of transition metal oxide catalysts can eventually enhance the cell efficiency and cycle life of Li−O 2 batteries. Here, we propose that crystal phase engineering of transition metal oxides could be an effective way to achieve the above purpose. We establish controllable crystal phase modulation of the binary Mn x Co 1−x O by adopting a cation regulation strategy. Systematic studies reveal an unprecedented relevancy between charge overpotential and crystal phase of Mn x Co 1−x O catalysts, whereas a dramatically reduced charge overpotential (0.48 V) via a rational optimization of Mn/Co molar ratio = 8/2 is achieved. Further computational studies indicate that the different morphologies of Li 2 O 2 should be related to different electronic conductivity and binding of Li 2 O 2 on crystal facets of Mn x Co 1−x O catalysts, finally leading to different charge overpotential. We anticipate that this specific crystal phase engineering would offer good technical support for developing highperformance transition metal oxide catalysts for advanced Li−O 2 batteries.
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