Recycling of valuable metals from spent ternary Li-ion batteries for the multi-active site electrocatalysts with high-entropy coordination

Recycling and utilization of valuable metals from spent ternary lithium-ion batteries possess significant economic and environmental benefits. Recycling of valuable metals effectively compensates for the high costs, poor selectivity, and low utilization rates of active sites present in single Pt-catalyzed hydrogen evolution reaction (HER). Hence, developing high-efficiency catalysts with multi-metal active centers to synergistically promote H 2 O dissociation and H 2 evolution is critical for accelerating alkaline HER. In response, we first report an ultra-small high-entropy alloys (HEAs) nanoparticle catalyst by mixing valuable metals (Ni, Co, Mn) recycled from spent ternary Li-ion batteries with Pt driven by non-equilibrium high-temperature-shockwave. As expected, due to high-entropy coordination environment, well-designed NiCoMnPt HEAs catalyst possesses multiple activated metal centers, thus achieving much-improved HER performance (ultra-low overpotential of 16.6 mV@10 mA cm −2 ). Experimental and theoretical studies indicate the mutual substitutions among NiCoMnPt atoms cause lattice distortion and induce electronic coupling effect, which optimizes the electronic structure of Pt and makes the deeply activated Pt as fundamental active center for H 2 O dissociation. Accompanied by electrons redistribution, NiCoMn as electron-rich centers further contribute to reducing the H 2 desorption energy barrier and greatly accelerating the hydrogen evolution efficiency. Impressively, this work provides fresh ideas for constructing high-efficiency electrocatalysts beyond HER.