Tailoring Local Electrolyte Solvation Structure via a Mesoporous Molecular Sieve for Dendrite‐Free Zinc Batteries

Abstract

Aqueous zinc-ion batteries (ZIBs) are low cost with a promising theoretical capacity and inherent safety, and thus have drawn increasing attention as prospective energy storage devices in large-scale energy storage systems. However, severe dendrite growth and side reaction problems hinder the practical application of ZIBs. Here, molecular sieves with ordered mesoporous channels are constructed to tailor the local electrolyte solvation structure on the zinc surface. Different high-concentration solvation structures can be realized by adjusting the pore diameter of the molecular sieve, and the optimal pore geometry is a mesoporous channel with a diameter of 2.5 nm that induces the formation of a locally concentrated electrolyte and affords a lower Zn 2+ de-solvation energy in Mobil composition of matter number 41 (MCM41). The resulting MCM41-Zn anode exhibits high cycling stability for Zn stripping/plating under different current densities (over 1800 h at 1 mA cm -2 , 1 mAh cm -2 , and 2200 h at 5 mA cm -2 , 1 mAh cm -2 ). Moreover, the CaV 8 O 20 •nH 2 O//MCM41-Zn full cell shows a high capacity of 274.2 mAh g −1 and a long lifespan (no capacity decay after 1000 cycles at 4 A g -1 ).

Oxygen vacancies and N‐doping in organic–inorganic pre‐intercalated vanadium oxide for high‐performance aqueous zinc‐ion batteries

“…To quantify the electrode reactivity, the activation energy ( E a ) of Zn 2+ diffusion was measured according to R ct in the temperature range of 25–85°C (Figure S11). E a was calculated by the Arrhenius Equation (3): 40 where A is the frequency factor, R is the gas constant and T is the temperature. Figure S11 shows a higher E a for (Zn,en)VO (15.13 kJ mol −1 ) than for N‐(Zn,en)VO (8.73 kJ·mol −1 ), revealing that the nitridation treatment effectively improved the electrochemical activity of the cathodic material.…”

Solvation Structures in Aqueous Metal‐Ion Batteries

“…For example, molecular sieves of Mobil composition of matter number 41 (MCM41) with ordered mesoporous channels are constructed to tailor the local electrolyte solvation structure on the zinc surface. [48] In this work, MCM41 is physically coupled with a Zn anode, which provides Reproduced with permission. [45] Copyright 2020, Wiley-VCH.…”

Regulating Solvation Structures Enabled by the Mesoporous Material MCM-41 for Rechargeable Lithium Metal Batteries

“…Numerous attempts at regulating the Li + solvation structure in electrolytes have been explored, such as solvents with low dipole moments, , electrolyte additives, − and high concentration or local high concentration electrolytes (HCEs or LHCEs). − However, compared with the exploration of electrolytes, the firsthand and significant impacts of separators serving as reservoirs for electrolytes on the Li + solvation structure have been severely neglected. − In addition to homogenizing the Li + flux − and improving the transference number of Li + ( t Li + ), ,, the Li + solvation sheath can also be altered by chemical bonds or nanochannels introduced by the special separator modification. , Actually, in addition to the nanochannels produced by the special treatment, the solvation structure in the electrolyte confined in nanochannels of porous inorganic particles is also disparate from the normal state. − Hence, introducing porous inorganic particles into the separator coating to regulate the solvation structure is a topic worth discussing.…”