Atmospheric Corrosion-Driven Redox Coordination Enables Spontaneous Carbonate Conversion of Lithium-Ion Battery Cathodes

The growing demand for lithium-ion batteries (LIBs) has intensified the need for sustainable methods to recover critical metals. Current recycling strategies, including pyrometallurgy and hydrometallurgy, often involve high energy consumption, harsh reagents, and poor selectivity, limiting their environmental and economic viability. Here, we report a chemically autonomous and energy-neutral cathode recycling process driven by atmospheric corrosion. Under humid air and dissolved CO₂, aluminum current collectors undergo sustained oxidative dissolution, releasing electrons that selectively reduce transition metals (TM) in the layered oxide to TM(II). This redox reaction triggers H⁺ insertion, Li⁺/H⁺ exchange, and lattice destabilization, forming Li_<i>x</i>H_<i>y</i>TMO₂ intermediates that spontaneously coordinate with CO₃^2- to yield TMCO₃ or Ni₂(OH)₂CO₃, while Li⁺ precipitates as Li₂CO₃. CO₂ acts both as a proton carrier and as a coordinating ligand, sustaining the redox-coordination loop. This chemistry-driven approach redefines corrosion as a tool for selective redox transformations and offers a reagent-free, scalable pathway for LIB recycling under ambient conditions.