Green processing of steel slag and lithium-ion battery liquid waste poses a global environmental challenge. This study utilizes waste acid (containing Co2+, H+ and NO3–) and alkali solutions (containing Li+, Na+, OH– and CO32–) from lithium-ion battery manufacturing to recover metal cations from steel slag (containing Ca2+, Mg2+, Al3+, Fe3+, and Mn2+), preparing high-entropy CoCaMgMnAlFe-LDHs catalysts for controllable hydrogen generation via NaBH4 hydrolysis. The ultimate residue, without any residual hazardous metal cations, enabling safe reintroduction into the natural environment. The presence of Co2+ endows the CoCaMgMnAlFe-LDHs catalyst with rapid photo-thermal conversion capability, enabling it to rapidly heat up under infrared radiation and efficiently catalyze the reaction of NaBH4 hydrolysis. The hydrogen generation rate reaches 1.12 mol·h−1·g−1·W−1 driven by 1050 nm infrared radiation. This study provides a novel approach to the environmentally friendly treatment and high-value utilization of steel slag and lithium-ion battery liquid waste.
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