Ultra-Low Emission Cathode Recycling Enabled by Programmed Adaptive Pulse Joule Heating

Sustainable recovery of valuable critical metals from spent lithium-ion batteries (LIBs) is increasingly recognized as a cornerstone of global electrification and supply-chain resilience. Joule-heating technologies have emerged as promising alternatives to conventional pyrometallurgical and hydrometallurgical routes; to advance this emerging electrothermal route, we integrate real-time thermal feedback with reaction-pathway regulation to reduce energy input, external reductant use, and greenhouse-gas (GHG) emissions. Here, we develop a programmed adaptive pulse Joule heating (PJH) platform that transforms thermal reduction into a digitally guided and self-regulating process. By maintaining an optimized temperature trajectory through adaptive current modulation, PJH promotes selective in situ reductive recovery via intrinsic carbon-mediated pathways, with isotope-tracing analysis supporting intrinsic carbon incorporation into carbonate products and life-cycle assessment indicating a low GHG footprint of 2.90 kg CO₂ eq. kg⁻¹ under defined system boundaries. Under optimized conditions, battery-grade lithium carbonate (> 99.5%), verified by product-quality analysis, is selectively recovered via acid-free rapid aqueous leaching (∼10 min) after seconds-level (20 s) heat treatment without pretreatment. Preliminary scale-up PJH demonstrations across diverse lithium-containing resources suggest potential for broader application. These results demonstrate how adaptive PJH integrates thermal feedback with lower-carbon process design, offering a potential route toward selective and low-emission recycling of cathode materials.