A universal interfacial strategy for suppressing aluminum corrosion by confining H+/OH− dynamics in aqueous energy storage systems

Abstract

Aqueous electrochemical energy storage (EES) systems offer promise for large-scale applications, yet their practical deployment is fundamentally constrained by the persistent corrosion of an aluminum current collector (AlCC) in aqueous environments. Existing strategies primarily suppressing water–electrode interactions still encounter serious Al corrosion issues and elevated interfacial resistance. Guided by insights into the two-step corrosion mechanisms, we propose a new mechanistic anti-corrosion paradigm that suppresses H⁺/OH⁻–AlCC interactions for suppressing corrosion of the AlCC. As a proof of concept, representative nanomaterials with stronger H⁺/OH⁻ adsorption capability (e.g., aluminum phosphate, AlPO₄) are electrochemically deposited onto a commercial AlCC to form an AlPO₄-modified current collector (APCC). The dual-functional APCC effectively blocks the corrosive attack of highly reactive H⁺/OH⁻ ions on the AlCC and reduces interfacial resistance, thereby overcoming the long-standing limitations of conventional strategies. The universality and robustness of the APCC are demonstrated across both energy-type (lithium-ion batteries) and power-type (supercapacitors) systems. Notably, APCC-based pouch-cell supercapacitors exhibit an impressive capacity retention of ∼86.4% after 15 000 cycles, significantly outperforming the commercial AlCC (∼32.0% after 5000 cycles). In aqueous lithium-ion batteries, the APCC enables an ∼2.4-fold improvement in capacity retention compared to commercial AlCC counterparts. This work highlights interfacial H⁺/OH⁻ dynamic regulation as a generalizable and scalable strategy for achieving stable, high-performance aqueous EES systems.