The performance of aqueous zinc metal batteries is significantly
compromised by the stability of the solid electrolyte interphase (SEI),
which is intimately linked to the structure of the electrical double
layer (EDL) between the zinc anode and electrolyte. Furthermore, understanding
the mechanical behavior of SEI is crucial, as it governs its response
to stress induced by volume changes, fracture, or deformation. In
this study, we introduce l-glutamine (Gln) as an additive
to regulate the adsorbed environment of the EDL and in situ produce
a hybrid SEI consisting of ZnS and Gln-related species. The results
of the nanoindentation test indicate that the hybrid SEI exhibits
a low modulus and low hardness, alongside exceptional shape recovery
capability, which effectively limits side reactions and enables topological
adaptation to volume fluctuations in zinc anodes during zinc ion plating/stripping,
thereby enabling Zn//Zn symmetric cells to exhibit an ultralong cycle
life of 4000 h in coin cells and a high cumulative capacity of 18,000
mA h in pouch cells. More importantly, the superiority of the formulated
strategy is further demonstrated in Zn//NH4V4O10 full cells at different N/P ratios of 5.2, 4.9, 3.5,
and 2.4. This provides a promising approach for future interfacial
modulation in aqueous battery chemistry.