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

ABSTRACT 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 CO 2 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.