Heterogeneous Interface Design for Enhanced Sodium Storage: Sb Quantum Dots Confined by Functional Carbon

Qiu, Tianyun; Yang, Li; Xiang, Yinger; Yu, Ye; Zou, Guoqiang; Hou, Hongshuai; Ji, Xiaobo

doi:10.1002/smtd.202100188

Cited by 20 publications

(14 citation statements)

References 56 publications

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“…Besides, as in Fig. 4 d, the peaks located at 528.7 and 538.1 eV are attributed to the Sb 0 [ 36 ], which reveals the existence of metallic Sb. Additionally, the peaks of C 1 s (Fig.…”

Section: Resultsmentioning

confidence: 99%

Natural Stibnite for Lithium-/Sodium-Ion Batteries: Carbon Dots Evoked High Initial Coulombic Efficiency

Xiang

et al. 2022

Nano-Micro Lett.

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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.

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“…Besides, as in Fig. 4 d, the peaks located at 528.7 and 538.1 eV are attributed to the Sb 0 [ 36 ], which reveals the existence of metallic Sb. Additionally, the peaks of C 1 s (Fig.…”

Section: Resultsmentioning

confidence: 99%

Natural Stibnite for Lithium-/Sodium-Ion Batteries: Carbon Dots Evoked High Initial Coulombic Efficiency

Xiang

et al. 2022

Nano-Micro Lett.

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“…The cause of declined work functions is largely ascribed to the existence of the BiOC bond inducing the interface dipoles and changing the phase interfacial electron clouds arrangement. [25] The distinct difference in work functions between Bulk Bi and 2D Bi@ NOC was consistent with their sharp contrast of rate performance and K + diffusion coefficient.…”

Section: Resultsmentioning

confidence: 56%

2D Bismuth@N‐Doped Carbon Sheets for Ultrahigh Rate and Stable Potassium Storage

Zhu

et al. 2022

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Metallic Bi, as an alloying‐type anode material, has demonstrated tremendous potential for practical application of potassium‐ion batteries. However, the giant volume expansion, severe structure pulverization, and sluggish dynamics of Bi‐based materials result in unsatisfied rate performance and unstable cycling stability. Here, 2D bismuth@N‐doped carbon sheets with BiOC bond and internal void space (2D Bi@NOC) are successfully fabricated via a self‐template strategy to address these issues, which own ultrafast electrochemical kinetics and impressive long‐term cycling stability for delivering an admirable capacity of 341.7 mAh g−1 after 1000 cycles at 10 A g−1 and impressive rate capability of 220.6 mAh g−1 at 50 A g−1. Particularly, the in situ transmission electron microscopy observations visualize the real‐time alloying/dealloying process and reveal that plastic carbon shell and void space can availably relieve dramatic volume stress and powerfully maintain structural integrity. Density functional theory calculation and ultraviolet photoelectron spectroscopy test certify that the robust BiOC bond is thermodynamically and kinetically beneficial for adsorption/diffusion of K+. This work will light on designing advanced high‐performance energy materials and provide important evidence for understanding the energy storage mechanism of alloy‐based materials.

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“…In the first cyclic voltammetry (CV) cycle at a scan rate of 0.2 mV s −1 ( Figure A), two cathodic peaks located at 0.45 and 0.1 V versus Na/Na + might be attributed to the step‐wise alloying of Na with Sb(Sn)@C and the formation of solid‐electrolyte interphase, respectively. [ 24 ] In the subsequent scans, two cathodic peaks (0.4 and 0.16 V) and one anodic peak (0.85 V) were observed, [ 25 ] reflecting the dealloying process. [ 26 ] The CV profiles for the Sb and Sb(Sn) electrodes was also tested as shown in Figure S8 (Supporting Information), and the shift of the peak position of Sb was more significant than that of Sb(Sn) and Sb(Sn)@C, suggesting more polarization in the former than the latter.…”

Section: Resultsmentioning

confidence: 99%

Strain Retarding in Multilayered Hierarchical Sn‐Doped Sb Nanoarray for Durable Sodium Storage

Zhang

Niu

et al. 2023

Adv Funct Materials

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Antimony (Sb) is a potential electrode material for sodium (Na) storage due to its high theoretical capacity of 660 mAh g−1. Yet, the alloy/dealloy reaction between Na and Sb induces detrimental structural strain that inevitably leads to electrode failure, further resulting in deteriorated rate performance and cycle life. Herein, inspired by the multilayered structure of the pine trees, 3D hierarchical multilayered tin (Sn)‐doped Sb nanoarray coated with a thin carbon (C) layer (Sb(Sn)@C) is developed. Density functional theory calculation results suggest that Sb(Sn)@C offers better kinetic properties for Na diffusion, and lower volume expansion upon sodium intercalation as compared to the counterparts without Sn dopant or carbon coating. Moreover, the simulation results based on finite element analysis suggest that the unique hierarchical multilayered construction not only provides highly efficient Na+ utilization, but also builds a uniform von Mises stress distribution that effectively confines structural strain induced during Na+ insertion. This is also verified by nanoindentation measurement that Sb(Sn)@C shows higher elastic modulus and hardness than Sb(Sn) and pure Sb, indicating best mechanical stability. As expected, Sb(Sn)@C achieves excellent electrochemical capability for sodium storage with high reversible capacity, enhanced cyclability, and remarkable rate performance.

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Heterogeneous Interface Design for Enhanced Sodium Storage: Sb Quantum Dots Confined by Functional Carbon

Abstract: Figure 8. a) Band structure of a) SbQD@C and c) Sb (R-3m); the total density of states and partial density of states for b) SbQD@C and d) Sb (R-3m).

Cited by 20 publications

References 56 publications

Natural Stibnite for Lithium-/Sodium-Ion Batteries: Carbon Dots Evoked High Initial Coulombic Efficiency

Natural Stibnite for Lithium-/Sodium-Ion Batteries: Carbon Dots Evoked High Initial Coulombic Efficiency

2D Bismuth@N‐Doped Carbon Sheets for Ultrahigh Rate and Stable Potassium Storage

Strain Retarding in Multilayered Hierarchical Sn‐Doped Sb Nanoarray for Durable Sodium Storage

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