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1.
ACS Appl Mater Interfaces ; 16(15): 18971-18979, 2024 Apr 17.
Artículo en Inglés | MEDLINE | ID: mdl-38578663

RESUMEN

The formation of a solid electrolyte interphase on carbon anodes causes irreversible loss of Na+ ions, significantly compromising the energy density of Na-ion full cells. Sodium compensation additives can effectively address the irreversible sodium loss but suffer from high decomposition voltage induced by low electrochemical activity. Herein, we propose a universal electrocatalytic sodium compensation strategy by introducing a carbon nanotube (CNT)/MnO2 catalyst to realize full utilization of sodium compensation additives at a much-reduced decomposition voltage. The well-organized CNT/MnO2 composite with high catalytic activity, good electronic conductivity, and abundant reaction sites enables sodium compensation additives to decompose at significantly reduced voltages (from 4.40 to 3.90 V vs Na+/Na for sodium oxalate, 3.88 V for sodium carbonate, and even 3.80 V for sodium citrate). As a result, sodium oxalate as the optimal additive achieves a specific capacity of 394 mAh g-1, almost reaching its theoretical capacity in the first charge, increasing the energy density of the Na-ion full cell from 111 to 158 Wh kg-1 with improved cycle stability and rate capability. This work offers a valuable approach to enhance sodium compensation efficiency, promising high-performance energy storage devices in the future.

2.
Chem Asian J ; 17(12): e202200213, 2022 Jun 15.
Artículo en Inglés | MEDLINE | ID: mdl-35560519

RESUMEN

With the ever increasing demand for low-cost and economic sustainable energy storage, Na-ion batteries have received much attention for the application on large-scale energy storage for electric grids because of the worldwide distribution and natural abundance of sodium element, low solvation energy of Na+ ion in the electrolyte and the low cost of Al as current collectors. Starting from a brief comparison with Li-ion batteries, this review summarizes the current understanding of layered oxide cathode/electrolyte interphase in NIBs, and discusses the related degradation mechanisms, such as surface reconstruction and transition metal dissolution. Recent advances in constructing stable cathode electrolyte interface (CEI) on layered oxide cathode are systematically summarized, including surface modification of layered oxide cathode materials and formulation of electrolyte. Urgent challenges are detailed in order to provide insight into the imminent developments of NIBs.

3.
Angew Chem Int Ed Engl ; 61(21): e202116865, 2022 May 16.
Artículo en Inglés | MEDLINE | ID: mdl-35132759

RESUMEN

Chemical modification of electrode materials by heteroatom dopants is crucial for improving storage performance in rechargeable batteries. Electron configurations of different dopants significantly influence the chemical interactions inbetween and the chemical bonding with the host material, yet the underlying mechanism remains unclear. We revealed competitive doping chemistry of Group IIIA elements (boron and aluminum) taking nickel-rich cathode materials as a model. A notable difference between the atomic radii of B and Al accounts for different spatial configurations of the hybridized orbital in bonding with lattice oxygen. Density functional theory calculations reveal, Al is preferentially bonded to oxygen and vice versa, and shows a much lower diffusion barrier than BIII . In the case of Al-preoccupation, the bulk diffusion of BIII is hindered. In this way, a B-rich surface and Al-rich bulk is formed, which helps to synergistically stabilize the structural evolution and surface chemistry of the cathode.

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