Highlights
The chemical process of local oxidation–partial reduction–deep coupling for
stibnite reduction of carbon dots (CDs) is revealed by in-situ high-temperature X-ray
diffraction.
Sb2S3@xCDs anode delivers high initial coulombic efficiency in lithium ion
batteries (85.2%) and sodium ion batteries (82.9%), respectively.
C–S bond influenced by oxygen-rich carbon matrix can restrain the conversion of
sulfur to sulfite, well confirmed by X-ray photoelectron spectroscopy
characterization of solid electrolyte interphase layers helped with density
functional theory calculations.
CDs-induced Sb–O–C bond is proved to effectively regulate the interfacial
electronic structure.
Abstract
The application of Sb2S3 with marvelous theoretical capacity for alkali metal-ion batteries is seriously limited by its poor electrical conductivity and low initial coulombic efficiency (ICE). In this work, natural stibnite modified by carbon dots (Sb2S3@xCDs) is elaborately designed with high ICE. Greatly, chemical processes of local oxidation–partial reduction–deep coupling for stibnite reduction of CDs are clearly demonstrated, confirmed with in situ high-temperature X-ray diffraction. More impressively, the ICE for lithium-ion batteries (LIBs) is enhanced to 85%, through the effect of oxygen-rich carbon matrix on C–S bonds which inhibit the conversion of sulfur to sulfite, well supported by X-ray photoelectron spectroscopy characterization of solid electrolyte interphase layers helped with density functional theory calculations. Not than less, it is found that Sb–O–C bonds existed in the interface effectively promote the electronic conductivity and expedite ion transmission by reducing the bandgap and restraining the slip of the dislocation. As a result, the optimal sample delivers a tremendous reversible capacity of 660 mAh g−1 in LIBs at a high current rate of 5 A g−1. This work provides a new methodology for enhancing the electrochemical energy storage performance of metal sulfides, especially for improving the ICE.
The aqueous zinc-ion battery is considered as one of the best alternatives to lithium-ion batteries due to its low cost and high safety. However, the inevitable dendrite growth, byproduct formation, and the side reactions have inhibited the application of aqueous zinc-ion batteries. In this work, the electronegative nitrogen and sulfur-codoped carbon dots (NSCDs) are proposed as an electrolyte additive to regulate the uniform distribution of zinc ions and inhibit the growth of dendrites. It was found that only a small amount of NSCD additive (0.2 mg mL −1 ) exerted a significant influence in electrochemical performance; the symmetrical cell can operate stably for 2000 h with a low voltage hysteresis of 33 mV at the current density of 1 mA cm −2 , and a high Coulombic efficiency (CE) of 99.5% can be obtained after 250 cycles.
Comprehensive Summary
The severe dendrite growth on zinc anode in alkaline electrolyte brings great challenge to the development of zinc‐based batteries. It is a simple and effective strategy to inhibit zinc dendrite formation by introducing additives into the electrolyte. In this study, N, S‐doped carbon dots (TU‐CQDs) were synthesized and used as additives to regulate zinc deposition in a typical KOH electrolyte. The experimental and three‐dimensional transient nucleation model disclosed that the special functional groups of carbon dots can change the electrode surface state and the coordination behaviors of zinc species in the electrolyte. Therefore, TU‐CQDs can not only inhibit the hydrogen evolution reaction, but also achieve uniform zinc deposition. The in‐situ synchrotron radiation X‐ray imaging elucidated that TU‐CQDs can effectively inhibit the dendrite growth and improve the reversibility of zinc plating/stripping process. This work provides a feasible route for regulating the reversibility of zinc metal anode in alkaline electrolyte.
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