博士生苗书凯论文"Unraveling the synergistic mechanism of H2SO4/H2O2 system enabled by a dynamic dosing strategy for sustainable recycling of spent Li-ion batteries"被Hydrometallurgy接收发表
发布时间：2026-08-17
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The rapid decomposition of hydrogen peroxide (H2O2) in bulk acidic solution remains a major obstacle impeding the economic and environmental sustainability of recycling spent lithium-ion batteries. Herein, a “static-acid & dynamic-reductant” (SL_H2SO4 & DL_H2O2) leaching strategy is proposed to reduce this conventional limitation by engineering the spatial distribution of reagents. Static refers to one stage addition and dynamic refers to staged addition to avoid decomposition of H2O2 to H2O and O2. This approach achieves near-complete metal recovery (>98%) from spent LiNi0.8Co0.1Mn0.1O2 cathode materials while reducing H2O2 consumption by 20.1%. The core of this efficiency leap is unraveled through a multi-scale mechanistic decoding. Conventional one pot addition triggers rapid H2O2 decomposition at the interface, as confirmed by molecular dynamics simulations. In contrast, the dynamic dosing strategy promotes a synergistic surface reaction. Density functional theory calculations reveal a significant increase in adsorption energy to −2.72 eV upon H2SO4/H2O2 co-adsorption, suggesting a targeted proton coupled electron transfer process that may generate hydroperoxyl radicals (·HO2) at the interface, which could serve as the active reducing species for metal reduction, thereby bypassing wasteful bulk decomposition. This molecular level synergy is further evidenced by a substantial reduction in activation energy, particularly for Mn (58.8% lower). This work establishes a new paradigm in reagent management for efficient resource recovery.