Recycling spent lithium-ion batteries(SLIBs)has become essential to preserve the environment and reclaim vital resources for sustainable development.The typical SLIBs recycling concentrated on separating valuable comp...Recycling spent lithium-ion batteries(SLIBs)has become essential to preserve the environment and reclaim vital resources for sustainable development.The typical SLIBs recycling concentrated on separating valuable components had limitations,including high energy consumption and complicated separation processes.This work suggests a safe hydrometallurgical process to recover usable metallic cobalt from depleted LiCoO_(2)batteries by utilizing citric acid as leachant and hydrogen peroxide as an oxidizing agent,with ethanol as a selective precipitating agent.The anode graphite was also recovered and converted to graphene oxide(GO).The above components were directly resynthesized to cobaltintegrated nitrogen-doped graphene(Co@NG).The Co@NG showed a decent activity towards oxygen reduction reaction(ORR)with a half-wave potential of 0.880 V vs.RHE,almost similar to Pt/C(0.888 V vs.RHE)and with an onset potential of 0.92 V vs.RHE.The metal-nitrogen-carbon(Co-N-C)having the highest nitrogen content has decreased the barrier for ORR since the reaction was enhanced for Co@NG-800,as confirmed by density functional theory(DFT)simulations.The Co@NG cathode catalyst coupled with commercial Pt-Ru/C as anode catalyst exhibits excellent performance for direct methanol fuel cell(DMFC)with a peak power density of 34.7 mW cm^(-2)at a discharge current density of120 m A cm^(-2)and decent stability,indicating the promising utilization of spent battery materials in DMFC applications.Besides,lithium was recovered from supernatant as lithium carbonate by coprecipitation process.This work avoids sophisticated elemental separation by utilizing SLIBs for other renewable energy applications,lowering the environmental concerns associated with recycling.展开更多
基金supported by the Basic Science Research Program through the National Research Foundation of Korea(NRF)the South Korea grant funded by the Korean government(MSIT)(2021R1A4A2000934,2023R1A2C3004336)+1 种基金The computational part of the work was supported by Department of Chemical and Biomolecular Engineering,Institute of Emergent Materials,Sogang University,via NRF Korea grant 2015M3D3A1A01064929a generous supercomputing time from KISTI。
文摘Recycling spent lithium-ion batteries(SLIBs)has become essential to preserve the environment and reclaim vital resources for sustainable development.The typical SLIBs recycling concentrated on separating valuable components had limitations,including high energy consumption and complicated separation processes.This work suggests a safe hydrometallurgical process to recover usable metallic cobalt from depleted LiCoO_(2)batteries by utilizing citric acid as leachant and hydrogen peroxide as an oxidizing agent,with ethanol as a selective precipitating agent.The anode graphite was also recovered and converted to graphene oxide(GO).The above components were directly resynthesized to cobaltintegrated nitrogen-doped graphene(Co@NG).The Co@NG showed a decent activity towards oxygen reduction reaction(ORR)with a half-wave potential of 0.880 V vs.RHE,almost similar to Pt/C(0.888 V vs.RHE)and with an onset potential of 0.92 V vs.RHE.The metal-nitrogen-carbon(Co-N-C)having the highest nitrogen content has decreased the barrier for ORR since the reaction was enhanced for Co@NG-800,as confirmed by density functional theory(DFT)simulations.The Co@NG cathode catalyst coupled with commercial Pt-Ru/C as anode catalyst exhibits excellent performance for direct methanol fuel cell(DMFC)with a peak power density of 34.7 mW cm^(-2)at a discharge current density of120 m A cm^(-2)and decent stability,indicating the promising utilization of spent battery materials in DMFC applications.Besides,lithium was recovered from supernatant as lithium carbonate by coprecipitation process.This work avoids sophisticated elemental separation by utilizing SLIBs for other renewable energy applications,lowering the environmental concerns associated with recycling.