ICE optimization strategies of hard carbon anode for sodium-ion batteries: from the perspective of material synthesis

doi: 10.1088/2752-5724/ad5d7f

School of Materials Science and Engineering, Guangdong Provincial Key Laboratory of Advanced Energy Storage Materials, South China University of Technology, Guangzhou 510641, People’s Republic of China

摘要

Abstract: AbstractWith the continuous exploration of researchers in the field of sodium-ion batteries, the performance of these batteries has been greatly improved, and they have a wide range of application prospects in large-scale energy storage, traffic power and other fields. Hard carbon is the most important anode material for sodium-ion batteries. Although it has the advantages of low cost, stable structure and performance, it still has the problems of low initial Coulombic efficiency (ICE) and poor rate performance in application. In order to solve the problem of low ICE of hard carbon anode in sodium-ion batteries, in recent years the literature about hard carbon anode in sodium-ion batteries has been comprehensively reviewed. Based on the microstructure of hard carbon material, the causes of low ICE of hard carbon are analyzed. At the same time, from the point of view of material structure design and regulation, the current optimization strategies of hard carbon anode ICE are summarized, including the following aspects: optimization and improvement of the carbonization process, precursor screening and design, surface coating strategy, micro-pore structure control, catalytic carbonization strategy. We hope that this review will provide reference for further optimization of hard carbon properties and its large-scale application in sodium-ion batteries.
- sodium-ion batteries /
- anode materials /
- hard carbon /
- initial Coulombic efficiency
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Figure 1. Schematic diagram: the relationship between the microstructure of hard carbon, the causes of low ICE and optimization strategies.

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Figure 2. (a) ‘House of cards’ model and ‘insertion-adsorption’ mechanism. Reproduced from [21]. © 2000 ECS-The Electrochemical Society. All rights reserved. (b) ‘Adsorption-intercalation-filling’ mechanism. Reprinted with permission from [49]. Copyright (2015) American Chemical Society. (c) ‘Adsorption-filling’ mechanism. [46] John Wiley & Sons.© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (d) ‘Adsorption-intercalation’ mechanism. [47] John Wiley & Sons.© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (e) Extended ‘adsorption-intercalation’ mechanism’. [51] John Wiley & Sons. © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (f) ‘Adsorption-intercalation-pore filling-sodium cluster formation’ mechanism. [52] John Wiley & Sons.© 2023 WileyVCH GmbH.

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Figure 3. (a) Steady-state Na⁺ distribution and sodium-ion storage between graphite layers at constant potential for the vacancy defect free electrode and non-vacancy defect free electrode; (b) first charge-discharge curve of hard carbon prepared at different heating rates at 20 mA g^-1. [65] John Wiley & Sons.© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (c) Diagram of the spark plasma sintering (SPS) system diagram and annealing mechanism; the structural models obtained by molecular dynamics simulation under different conditions, respectively: initial structure (d), no external field (e), only external pressure (f) and simultaneous application of bias and external pressure (g). Reproduced with permission from [77]. © 2021. Published under the PNAS license. (h) Life cycle diagram of hard carbon prepared by two different pathways, and carbon production by different routes at various stages. Reproduced from [75]. CC BY 4.0.

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Figure 4. (a) Schematic diagram of the synthesis of epoxy phenol aldehyde resin and schematic diagram of the structure of hard carbon; (b) FTIR spectra of maleic anhydride (MA), epoxy phenolic novolac resin (EPN) and cured epoxy phenol novolac resin (cured EPN). Reprinted from [79], © 2023 Elsevier Ltd. All rights reserved. (c) Charge and discharge curves of untreated samples (CPP-1400 °C) and pre-treated samples (CPOP-1400 °C) at 0.1C in the first cycle; (d) (e) HRTEM and SAED images of the two samples; (f) (g) Raman spectra of two samples. [81] John Wiley & Sons.© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (h) XRD pattern of hard carbon prepared under different conditions; (i) Raman spectrum of hard carbon prepared under different conditions. (j) (k) Physical parameters and electrochemical properties of hard carbon under different preparation conditions. Reprinted from [85], Copyright © 2015 Elsevier B.V. All rights reserved.

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Figure 5. (a) Diagram of preparation of hard carbon by gaseous treatment of cyclohexane; (b) (c) XPS spectra and FTIR spectra of C-HC and P-HC samples; (d) First charge and discharge curves of different samples at 20 mA g^-1. Reprinted from [59], © 2019 Published by Elsevier Ltd. (e) TEM-EDX map of HC-Al₂O₃-5% for elemental mapping of C, Al and O; (f) diagram of SEI layer on hard carbon surface improved by Al₂O₃; (g) EIS results of HC and HC-Al₂O₃-5% after the first cycle. Reproduced from [108]. CC BY 4.0.

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Figure 6. Curves of different samples based on BET nitrogen adsorption and desorption measurements: (a) CMS; (b) AC; (c) graphite. First three cycles of different samples: (d) CMS; (e) AC; (f) graphite. Reprinted from [112], Copyright © 2016 Elsevier B.V. All rights reserved. (g) Diagram of controlled port diameter and interface charge distribution; (h) (i) charge and discharge curves in the first cycle of the materials before and after gas-phase adjustment; (j) (k) ²³Na MAS ssNMR spectra of the material before and after gas-phase regulation at low voltage; (l) reversible capacity of materials with different specific surface areas obtained by gas-phase regulation. Reproduced from [54]. CC BY 4.0.

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Figure 7. (a) Diagram of material synthesis route; (b) cycling performance of hard carbon (HCM-1300-ZBE) prepared by assisting with ZnO. [118] John Wiley & Sons.© 2022 WileyVCH GmbH. (c) Diagram of hard carbon microspheres etched with carbon dioxide; (d) (e) charge and discharge curves and ICE of the first three cycles of the unetched and etched material; (f) slope capacity and platform capacity of unetched and etched materials in the second cycle. [120] John Wiley & Sons. © 2023 WileyVCH GmbH.

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Figure 8. (a) Diagram of the effect of ion concentration on the microstructure of hard carbon; (b) charge and discharge curve of hard carbon prepared at different concentrations in the first cycle; (c) cycle performance of hard carbon prepared at different concentrations. [52] John Wiley & Sons.© 2023 WileyVCH GmbH. (d) Diagram of two routes for synthesizing hard carbon using graphite plate sandwich. Reprinted with permission from [132]. Copyright (2021) American Chemical Society. (e) Diagram of hexagonal cell structure of graphite-like crystal (a = b = 3.528 Å, c = 9.6 Å, α = β = 90°, γ = 120°), the picture on the right shows the graphite phase; (f) (g) HRTEM image of hard carbon and SAED map of typical graphite-like crystals. [133] John Wiley & Sons.© 2021 Wiley-VCH GmbH.

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Figure 9. (a) Schematic illustration of the IBL-regulated presodiation process. [135]. John Wiley & Sons.© 2023 WileyVCH GmbH. (b) Schematic of sodium powder application procedure onto hard carbon anode. Reprinted from [136], Published by Elsevier B.V. (c) ⁷Li and (d) ²³Na NMR of the lithium-pretreated HC rested in carbonate and TEGDME. (e) C 1s XPS of the lithium-pretreated HC cycled in carbonate ten times. [138] John Wiley & Sons.© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (f) Charge/discharge curves of pHC and HC at 50 mA g^-1 in the first cycle. (g) Normalized charge/discharge profiles of half cells of pHC and NVP and their full cell. (h) Cycle performance of full cells at 500 mA g^-1. [141] John Wiley & Sons.© 2022 WileyVCH GmbH. (i) Cycling performance of NVP||HC full cell with (6%) and without Na₃P coated on the separator within the potential range of 2.0-4.0 V at 0.5 C for the following cycles. [144] John Wiley & Sons.© 2023 WileyVCH GmbH.

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Figure 10. CVs obtained in three-electrode Swagelok cells with (a) 1 M NaClO₄ dissolved in single solvents, (b) low-current zoom plots of (a), (c) 1 M NaClO₄ dissolved in solvent mixtures, (d) low-current zoom plots of (c), (e). Electrochemical potential window stability (black bars) and thermal range (green bars) values of electrolytes based on 1 M NaClO₄ dissolved in various solvents and solvent mixtures. Reproduced from [149] with permission from the Royal Society of Chemistry. Comparison of LUMO and HOMO levels of (f) EC, DEC, PC, DME and DEGDME solvents and (g) their corresponding solvent-ion complexes. [152] John Wiley & Sons.© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (h), (i),(j), (k) The performance of the first three cycles of hard carbon anodes in different electrolytes (DME, DEGDME, EC/DMC and PC). Reprinted from [153], © 2020 Elsevier Ltd All rights reserved. HRTEM images of HCNS electrode after being cycled in DEGDME-based electrolyte (l) and EC/DEC-based electrolyte (m); the insets show the corresponding SAED images. Depth-profiling XPS spectra of O 1s and F 1s of the formed SEI films in DEGDME-based electrolyte (n) and EC/DEC-based electrolyte (o); the insets show the corresponding percentage of inorganic and organic species in the formed SEI films. [154] John Wiley & Sons.© 2021 Wiley-VCH GmbH.

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Figure 11. Ashby plot: comparison of the performance of hard carbon prepared by different methods. Naming of sample nomenclature: references, current density and year of publication.

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Table 1. Performance of half cell of hard carbon prepared from different biomass.

Precursor	Electrolyte	Voltage range (V)	ICE (%)	Reversible capacity/current density (mAh g^-1/mA^-1 g^-1)	References
Macadamia nut shell	1 M NaPF6 in EC:DMC(1:1 Vol%) with 2% FEC	0-2.0	91.4	300.9/30	[93]
Waste wine corks	1 M NaPF6 in EC:DMC(1:1 Vol%)	0-2.0	81	358/30	[94]
Natural cork	1 M NaPF₆ in EC:DEC(1:1 Vol%)	0-2.5	88.0	276/20	[95]
Cotton	0.8 m NaPF6 in ethylene and DMC(1:1 Vol%)	0-2.0	83	315/30	[46]
Banana peel	1 M NaClO₄ in EC:DEC(1:1 Vol%)	0.001-2.8	85.5	376/50	[96]
Camphor residue	1 M NaClO₄ in EC:DMC(1:1 Vol%)	0-2.0	82.8	324.6/20	[66]
Hazelnut shell	1 M NaPF₆ in EC:DMC(1:1 Vol%)	0-2.5	91.0	342/20	[97]
Bamboo	1 M NaPF₆ in DEG:DME(1:1 Vol%)	0-2.5	84.1	348.5/30	[98]
Corncob	1 M NaPF₆ in EC:DMC(1:1 Vol%)	-0.008-2.5	85.0	299/20	[99]
Tea stalk	1 M NaCF₃SO₃ in Diglyme	0.01-3.0	90.8	308/28	[100]
Reed straw	1 M NaClO₄ in EC:DEC(1:1 Vol%)	0.01-3.0	77.0	370/25	[101]
Starch	1 M NaPF₆ in DEGDME	0.01-2.0	87.2	335/30	[102]
Gelatin	1 M NaPF₆ in Diglyme	0.01-2.0	74.4	400/100	[103]
Sycamore fruit seed	1 M NaClO₄ in EC:DMC(1:1 Vol%)	0-2.8	73.8	296/25	[104]

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Table 2. Properties of hard carbon materials prepared by different methods in the full battery.

Full battery	Voltage range (V)	Specific capacity/current density (mAh g^-1 mA^-1 g^-1)	Energy density/current density (Wh kg^-1 mA^-1 g^-1)	Cyclic stability (capacity retention/cycle number/rate)	References
SHCs-1500\|\|Na_0.9(Cu_0.22Fe_0.30Mn_0.48)O₂	1.5-4.0	260/30	189/30	93.8%/300/1 C	[76]
MHC-1400\|\|Na(Cu_1/9Ni_2/9Fe_1/3Mn_1/3)O₂	1.5-4.0	297/0.1 C	215/0.1 C	70%/1300/1 C	[93]
CC-1600\|\|O3-Na[Cu_1/9Ni_2/9Fe_1/3Mn_1/3]O₂	1.0-4.0	362/0.1 C	230/2 C	71%/2000/2 C	[94]
HCT1300\|\|Na_0.9[Cu_0.22Fe_0.30Mn_0.48]O₂	1.0-4.05	290/0.2 C	207/0.2 C	92%/100/1 C	[46]
PPAC111400\|\|Na_0.9[Cu_0.22Fe_0.30Mn_0.48]O₂	1.0-4.0	240/0.2 C	195/1 C	91%/100/0.2 C	[85]
C-HC\|\|Na₃V₂(PO₄)₂F₃	2.0-4.3	98/20 (base on cathode)	239/20	80%/50/20 mA g^-1	[59]
Zn-HC\|\|NVP	1.5-3.9	524/50	323/50	86%/650/2 A g^-1	[118]
HC-21-1400\|\|O3-NaNi_1/3Fe_1/3Mn_1/3O₂	0.1-4.0	413/0.1 C	300/0.1 C	87%/50/0.2 C	[119]
CAC1300\|\|NVP	1.5-3.7	251.3/0.1 C	231.2/0.2 C	84%/200/0.2 C	[125]
GHC-80\|\|O3-Na_0.9[Cu_0.22Fe_0.30Mn_0.48]O₂	1.0-4.0	Unreported	210/0.1 C	91%/100/2 C	[131]
HC-0.2P-1000\|\|NVP	1.5-3.7	343.3/50	251.1/50	73.3%/450/1 A g^-1	[162]
RG-1300\|\|NaNi_1/3Fe_1/3Mn_1/3O₂	0.5-4.0	283/20	239/20	Unreported	[163]
CM180\|\|O3-NaNi_1/3Fe_1/3Mn_1/3O₂	0.5-4.0	291.6/0.1 C	238.7/2 C	75%/200/2 C	[164]
CHC1300\|\|Na_0.83Mg_0.11Ni_0.22Mn_0.63O₂	1.5-4.3	331.1/30	265.4/30	75.6%/400/1 C	[165]
GCHC-1400\|\|NVP	2.2-3.6	321/1 C	270/1 C	99%/200/1 C	[166]
HCM\|\|NVP	1.0-3.4	307/0.1 C	190/1 C	90.2%/200/1 C	[167]
HCM55-1400\|\|Na_0.9[Cu_0.22Fe_0.30Mn_0.48]O₂	1.0-4.05	291/0.1 C	247/0.1 C	Unreported	[168]

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