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Membranes 2022, 12, 343 10 of 27 may vary from ~1 nm to a few tens of nano-meters, consists of the Stern and Helmholtz layers, which correspond to either polarized or diffuse layers, respectively [72]. The electrical attraction generated by the diffuse layer is weaker than that of the polarized layer, which means that counter ions can diffuse with limited resistances. These interactions are typically measured in terms of the streaming or zeta potential, which decay exponentially concerning the inverse of the distance from the surface [72]. The ion selectivity within the pores may therefore be explained by accounting for differences between the hydration free energy of the ion and the energy of interaction between the ion and the charged site within the micropores [73,74]. The anionic field strength of the binding sites is the critical factor determining the selectivity sequence of the micropores for a series of cations. A typical selectivity sequence ranges from Li+ > Na+ > K+ > Rb+ > Cs+, while at the lowest anionic field strength, the micropores, corresponding to the free volume between the macromolecular chains of the ion exchange resins, may reverse the selectivity sequence as follows: Li+ < Na+ < K+ < Rb+ < Cs+ (Figure 3a). The size of the free volume, the charge of the surface, and the external driving forces applied across the membrane stack will influence the rate of diffusion and the perm- selectivity of Li ions diffusion compared to other cations across membranes [72]. The dimension of the micropores and the loss of the hydration shells of the ions upon entering the channels are crucial to diffusion since these critical dimensions are typically smaller than the hydrated radii of most alkali metal ions (Figure 3b). The charge distribution and densities across the micro-channels will also dictate the rate of ion transfer and negatively charged moieties, and polymer backbones should be used for cation diffusion and to repel anions. The impact of the pendant cation exchange groups across ion exchange resins was evaluated to optimize Li+ ion perm-selectivity. Sulphonate [76,77], carboxylic [78], as well as hydroxide groups were found to offer weak interactions supporting ion hopping 2+ + 10 of 2+7 + > K > Na > Li , Membranes 2022, 11, x FOR PEER REVIEW − (Figure 3c). Ion affinity to -SO3 was found to follow the trend Mg thus promoting the facile release of Li ions. Figure 3. Effect of nanochannel size of Li-ion selectivity (a). The ion mobility vs. hydration shell (b). Figure 3. Effect of nanochannel size of Li-ion selectivity (a). The ion mobility vs. hydration shell (b). The hydration ions diameter of light metal cations (c). Comparison of velocity of Li+, Na+, K+, and The hydration ions diameter of light metal cations (c). Comparison of velocity of Li+, Na+, K+, and Ca2+ in 0.4 nm vermiculite nanochannel (d) Reprinted based on the open access license from [72,75]. Ca2+ in 0.4 nm vermiculite nanochannel (d) Reprinted based on the open access license from [72,75]. The size of the free volume, the charge of the surface, and the external driving forces applied across the membrane stack will influence the rate of diffusion and the perm-se- lectivity of Li ions diffusion compared to other cations across membranes [72]. The dimen- sion of the micropores and the loss of the hydration shells of the ions upon entering the channels are crucial to diffusion since these critical dimensions are typically smaller than the hydrated radii of most alkali metal ions (Figure 3b). The charge distribution and den- sities across the micro-channels will also dictate the rate of ion transfer and negativelyPDF Image | Electro-Driven Materials and Processes for Lithium
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