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J. Phys. Energy 3 (2021) 031503 N Tapia-Ruiz et al Figure 9. (a) Franklin’s representations of non-graphitising and graphitising carbons [67]. Reproduced with permission from [69]. (b) A typical discharge curve for hard carbons shows two distinct regions: the sloping region and the plateau region. Figure 10. Schematic illustration of the proposed sodium storage mechanisms; stack thicknesses and plane sizes are not to scale, and defects and curvatures are not shown [70]. Reproduced from [70] with permission of The Royal Society of Chemistry. models for further optimisation based on DFT [91, 92], molecular dynamics (MD) [93], and machine learning [94] to predict the optimal structural and morphological parameters. Advances in science and technology to meet challenges Several research groups have made great advances in developing hard carbon anodes with outstanding performance from low-cost precursors, based on a careful synthetic design combined with advanced ex-situ and in situ characterisation [95]. Most debates to date have arisen from contradictory Na storage mechanisms in such carbons. Currently, there are several published theories: (a) the ‘intercalation-filling’ model: Na+ ions intercalate into graphitic layers in the sloping region, and insert themselves into nanopores in the plateau region [96]; (b) the adsorption-intercalation model: Na+ ions adsorb at the surface or defect sites of the carbon electrodes within the sloping region and intercalate into the graphitic layers within the plateau region [97]; (c) the adsorption-filling model: in the sloping region, Na+ ions adsorb at the defect sites while filling the nanopores in the plateau region [72], and (d) the ‘three-stage’ model: defect adsorption of Na+ ions takes place in the sloping region, but in the plateau region, the Na+ ions first intercalate into the graphitic layers and fill the nanopores at the end [98]. More recent investigations by my research team as well as other authors have gathered stronger evidence to propose an alternative model, with adsorption and intercalation occurring simultaneously during the sloping region, and pore filling during the plateau region, all the while keeping in mind the dependence on the structure and pore system of the respective carbons (figure 10). Great progress has been achieved in using operando characterisation techniques to probe the mechanisms of different carbon materials; in particular, operando NMR has been used to probe the metallic nature of Na in the pores [79, 80], SAXS/WAXS [100, 101] has been used to probe the Na interaction with 23PDF Image | roadmap for sodium-ion batteries
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