Controllably tailoring alloying anode materials to achieve fast charging and enhanced structural stability is crucial for sodium‐ion batteries with high rate and high capacity performance, yet remains a significant challenge owing to the huge volume change and sluggish sodiation kinetics. Here, a chemical tailoring tool is proposed and developed by atomically dispersing high‐capacity Ge metal into the rigid and conductive sulfide framework for controllable reconstruction of GeS bonds to synergistically realize high capacity and high rate performance for sodium storage. The integrated GeTiS3 material with stable Ti–S framework and weak GeS bonding delivers high specific capacities of 678 mA h g−1 at 0.3 C over 100 cycles and 209 mA h g−1 at 32 C over 10 000 cycles, outperforming most of the reported alloying type anode materials for sodium storage. Interestingly, in situ Raman, X‐ray diffraction (XRD), and ex situ transmission electron microscopy (TEM) characterizations reveal the formation of well‐dispersed NaxGe confined in the rigid Ti–S matrix with suppressed volume change after discharge. The synergistically coupled alloying‐conversion and surface‐dominated redox reactions with enhanced capacitive contribution and high reaction reversibility by a binding‐energy‐driven atomic scissors method would break new ground on designing a high‐rate and high‐capacity sodium‐ion batteries.
Alloying-type bismuth with high volumetric capacity has emerged as a promising anode for sodium-ion batteries but suffers from large volume expansion and continuous pulverization. Herein, a coordination constraint strategy is proposed, that is, chemically confining atomic Bi in an intercalation host framework via reconstruction-favorable linear coordination bonds, enabling a novel quasi-topological intercalation mechanism. Specifically, micron-sized Bi 0.67 NbS 2 is synthesized, in which the Bi atom is linearly coordinated with two S atoms in the interlayer of NbS 2 . The robust Nb−S host framework provides fast ion/electron diffusion channels and buffers the volume expansion of Na + insertion, endowing Bi 0.67 NbS 2 with a lower energy barrier (0.141 vs. 0.504 eV of Bi). In situ and ex situ characterizations reveal that Bi atom alloys with Na + via a solid-solution process and is constrained by the reconstructed Bi−S bonds after dealloying, realizing complete recovery of crystalline Bi 0.67 NbS 2 phase to avoid the migration and aggregation of atomic Bi. Accordingly, the Bi 0.67 NbS 2 anode delivers a reversible capacity of 325 mAh g −1 at 1 C and an extraordinary ultrahigh-rate stability of 226 mAh g −1 at 100 C over 25 000 cycles. The proposed quasi-topological intercalation mechanism induced by coordinated mode modulation is expected to be be conducive to the practical electrode design for fast-charging batteries.
Lithium-ion batteries with both low-temperature (low-T) adaptability and high energy density demand advanced cathodes. However, state-of-the-art high-voltage (high-V) cathodes still suffer insufficient performance at low T, which originates from the poor cathode–electrolyte interface compatibility. Herein, we developed a shallow surface Zr-doped and Li+ conductive Li2Zr(PO4)2 (LZPO) interspersed massage-ball-like LiCoO2 (LZPO-LCO). The surface-interspersed LZPO can induce an electrolyte superwettability of LZPO-LCO, which helps to form a high-quality cathode–electrolyte interphase with strong stability and low interface resistance. Without changing electrolyte, even at a low T of −25 °C and a high V of 4.6 V, LZPO-LCO shows an ultrahigh capacity of ∼200 mAh g–1 at 0.2C and 137 mAh g–1 at 5C, maintaining 94% capacity after 100 cycles with an average Coulombic efficiency of 99.9%. Besides, the fabricated full cells deliver a high energy density of ∼340 Wh kg–1 and maintain 92% capacity after 200 cycles at −25 °C. This work provides a significant leap forward for high-performance low-T cathodes.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.
hi@scite.ai
10624 S. Eastern Ave., Ste. A-614
Henderson, NV 89052, USA
Copyright © 2024 scite LLC. All rights reserved.
Made with 💙 for researchers
Part of the Research Solutions Family.