Catalytic microdomain engineering enables low-temperature fabrication of high-rate carbon anodes

Abstract

The low-temperature fabrication of hard carbon is of significant importance for the development of lithium-ion batteries towards grid-scale energy storage. Despite their high capacity and coulombic efficiency, conventional methods suffer from high pyrolysis temperatures and/or complex procedures, resulting in high costs. Herein, we innovatively proposed a catalytic microdomain engineering strategy, where 3-aminophenol was initially coordinated with Fe³⁺ ions and then polymerized to formaldehyde, forming a catalytic microdomain composed of [Fe(3-AP)_x]³⁺ units within the resin precursor. Material characterization suggests the uniform chemical composition of the resin precursor, and in situ DRIFT spectra revealed that the resin precursor features a low N–C–O rearrangement temperature, enabling low-temperature fabrication of high-performance hard carbon. Experimentally, FeOC-400 delivered a high reversible capacity of 566 mAh g⁻¹ after 250 cycles at 0.1 A g⁻¹ and a capacity retention of 95.6% after 5000 cycles at 10.0 A g⁻¹, endowing the FeOC-400||LFP full cell with a high energy density of over 175.7 Wh kg⁻¹ (based on the total mass of FeOC-400 and LFP). The findings of this study can provide new insight into the design of high-capacity and fast-charging hard carbon, and the catalytic microdomain engineering strategy is applicable to the low-cost fabrication of hard carbon towards grid-scale energy devices.