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Molecules 2022, 27, x FOR PEER REVIEW 14 of 34 Molecules 2022, 27, 6516 pore adsorption and filling, as well as the deposition on the surfaces depends signifi- cantly on the complex HC microstructure. It requires more precise characterization a1n3dof 32 more specific structural regulation methods to reveal whether these behaviors occur simultaneously or independently. From the other aspect, the current mechanism of so- dium storage in high-potential slope curves is the same, namely adsorption on material high-potential slope curves is the same, namely adsorption on material surfaces, edges, surfaces, edges, and defect sites. It is of great significance to explore the mechanism of and defect sites. It is of great significance to explore the mechanism of sodium storage for sodium storage for directional synthesis of high-performance HC materials. As the work directional synthesis of high-performance HC materials. As the work of Liu [63] showed, of Liu [63] showed, the adsorption-embedment theory was confirmed by adjusting the the adsorption-embedment theory was confirmed by adjusting the internal size of the internal size of the material; increasing the capacity of the slope area requires maintain- material; increasing the capacity of the slope area requires maintaining a large defect ing a large defect density, but it will increase the irreversible influences of solid electro- density, but it will increase the irreversible influences of solid electrolyte interphase (SEI) lyte interphase (SEI) film on ICE. Therefore, Sodium-ion intercalation with a stable volt- film on ICE. Therefore, Sodium-ion intercalation with a stable voltage platform should be age platform should be strengthened. Under the guidance of this understanding, a strengthened. Under the guidance of this understanding, a highly ordered layered structure highly ordered layered structure with an appropriate layer spacing (0.37~0.38 nm) was with an appropriate layer spacing (0.37~0.38 nm) was designed in order to improve the designed in order to improve the storage capacity of sodium in the low potential plat- stoforramgerceagpiaocni,tywohfiscohdibuemneifnitsthtehleowcopuolotemnbtiaelfpfilcaietfnocrymtroegaiolna,rgwehiecxhtebnetn.eEfivtsenthtueaclolyulaomb efnfiocnie-npcoyrotuosaHlaCrgmeaetxetreianlt.wEitvhenatuhaigllhyraevneornsi-bploercoaupsacHitCy manadtecroiaullowmitbheaffhiciigehncryevwerasible cadpeavceitloypaenddacnodurleoamlizbeedffiincipernacyticwalaaspdpelvicealtoiopne.d and realized in practical application. InInadadidtiotino,nw, whihleilexepxlpolroirnigngthtehemmecehcahnainsimsmofosfosdoiduimumstsotroargaeg,em, metehtohdodssfofrorergeuglua-ting thleatHinCgstthreucHtuCres,trauncdtumree,tahnodsmfeotrhcohdasrafocrtecrhizairnagctethriezimngattehreiamlpartoerpiaelrtpiersopweertriesgrwaderueally gradually completed. Xu’s group [74] established an extended “adsorp- completed. Xu’s group [74] established an extended “adsorption-intercalation” model, as tion-intercalation” model, as shown in Figure 10, dividing the evolution of the structure shown in Figure 10, dividing the evolution of the structure and the storage of sodium into and the storage of sodium into five stages and three behaviors. Disordered carbons at five stages and three behaviors. Disordered carbons at low pyrolysis temperatures (with low pyrolysis temperatures (with a layer spacing larger than 0.4 nm) tend to exhibit a layer spacing larger than 0.4 nm) tend to exhibit “pseudo-adsorption” behavior on the “pseudo-adsorption” behavior on the material surface (such as adsorption at defects, material surface (such as adsorption at defects, edges, heteroatomic centre, etc.). Along edges, heteroatomic centre, etc.). Along with the temperature increasing, the disorder with the temperature increasing, the disorder degree decreases, and the interval between degree decreases, and the interval between layers is about 0.36~0.4 nm, which is enough layers is about 0.36~0.4 nm, which is enough for the Sodium-ions to achieve a reversible for the Sodium-ions to achieve a reversible interlayer intercalation. At this time, the interlayer intercalation. At this time, the pseudo-adsorption behavior is still continuing, pseudo-adsorption behavior is still continuing, which is very similar to the traditional which is very similar to the traditional adsorption-intercalation theory. The enhanced adsorption-intercalation theory. The enhanced rearrangement at high temperature leads rearrangement at high temperature leads to the deepening of the HC graphitization, and to the deepening of the HC graphitization, and the layer spacing is below 0.36 nm, the layer spacing is below 0.36 nm, which makes it difficult to complete the insertion. The which makes it difficult to complete the insertion. The residual defects and pores on the residual defects and pores on the surface attribute to the last slope capacity. surface attribute to the last slope capacity. Figure 10. Schematic illustration of the extended “adsorption-intercalation” model [74]. Figure 10. Schematic illustration of the extended “adsorption-intercalation” model [74]. It should be noted that the process of storing and releasing Sodium-ions is dynamic, It should be noted that the process of storing and releasing Sodium-ions is dynamic, and it may be defective to judge the sodium storage behavior of electrodes based on the and it may be defective to judge the sodium storage behavior of electrodes based on the experience of electrochemical kinetics alone. More accurate and visible measurement experience of electrochemical kinetics alone. More accurate and visible measurement methods are needed to prove the sodium storage mechanism of HC. In summary, it is necessary to have a more comprehensive and deeper understanding of the structure of HC to reveal the sodium storage mechanism of HC materials in SIBs, to guide the controllable synthesis of anode materials, and to approach the industrialization of high-efficiency battery materials.PDF Image | Hard Carbons as Anodes in Sodium-Ion Batteries
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