Recycling spent lithium-ion(Li+)batteries is critical for achieving environmental conservation and the strategic recovery of essential resources.Compared with conventional methods for recovering cathode materials,whic...Recycling spent lithium-ion(Li+)batteries is critical for achieving environmental conservation and the strategic recovery of essential resources.Compared with conventional methods for recovering cathode materials,which are energy-intensive and prone to secondary pollution,the direct regeneration approach has emerged as a rapid and highly efficient method,gaining widespread attention in recent years.However,this approach faces major challenges,including degraded electrochemical performances and limited economic value.This study,therefore,proposes a high-value direct regeneration strategy to convert degraded spent LiFePO_(4)(S-LFP)into a gradient manganese(Mn)-doped regenerated LiFe_(0.7)Mn_(0.3)PO_(4)/C(R-LFMP)composite.This method leverages the inherent microcracks and Li vacancies present in S-LFP,likely acting as diffusion channels for the Mn^(2+)/Li^(+)ions.Through a two-step mechanochemical ball-milling and carbothermal reduction process,this approach achieves simultaneous Li replenishment and surface-localised Mn gradient doping with enhanced structural control.Notably,the R-LFMP exhibits an exceptional electrochemical performance.At 0.1 C,it delivers a discharge capacity of 161.4 mA h g^(−1)and an energy density of 563.5 Wh kg^(−1)(representing a 60.5%improvement over S-LFP).Additionally,it maintains 83%capacity retention after 900 cycles at 0.5C,a considerable enhancement compared to commercial LFMP(62%).Furthermore,the regenerated cathode material generates a net profit of$7.102 kg^(−1),surpassing the profitability of conventional recycling methods by 90%.Overall,this study introduces a transformative and sustainable LFP regeneration technology,achieving breakthroughs in electrochemical restoration and high-value recycling,while paving the way for the closed-loop utilisation of LFP-based energy storage systems.展开更多
Steering the directional carrier migration across the interface is a central mission for efficient photocatalytic reactions.In this work,an atomic-shared heterointerface is constructed between the defect-rich ZnIn_(2)...Steering the directional carrier migration across the interface is a central mission for efficient photocatalytic reactions.In this work,an atomic-shared heterointerface is constructed between the defect-rich ZnIn_(2)S_(4)(HVs-ZIS)and CoIn_(2)S_(4)(CIS)via a defect-guided heteroepitaxial growth strategy.The strong interface coupling induces adequate carriers exchanging passageway between HVs-ZIS and CIS,enhancing the internal electric field(IEF)in the ZnIn_(2)S_(4)/CoIn_(2)S_(4)(HVs-ZIS/CIS)heterostructure.The defect structure in HVs-ZIS induces an additional defect level,improving the separation efficiency of photocarriers.Moreover,promoted by the IEF and intimate heterointerface,photogenerated electrons trapped by the defect level can migrate to the valence band of CIS,contributing to massive photogenerated electrons with intense reducibility in HVs-ZIS/CIS.Consequently,the HVs-ZIS/CIS heterostructure performs a boosted H_(2)evolution activity of 33.65 mmol g^(-1)h^(-1).This work highlights the synergistic effects of defect and strong interface coupling in regulating carrier transfer and paves a brave avenue for constructing efficient heterostructure photocatalysts.展开更多
基金supported by the National Key Research and Development Program of China(2023YFB3809300).
文摘Recycling spent lithium-ion(Li+)batteries is critical for achieving environmental conservation and the strategic recovery of essential resources.Compared with conventional methods for recovering cathode materials,which are energy-intensive and prone to secondary pollution,the direct regeneration approach has emerged as a rapid and highly efficient method,gaining widespread attention in recent years.However,this approach faces major challenges,including degraded electrochemical performances and limited economic value.This study,therefore,proposes a high-value direct regeneration strategy to convert degraded spent LiFePO_(4)(S-LFP)into a gradient manganese(Mn)-doped regenerated LiFe_(0.7)Mn_(0.3)PO_(4)/C(R-LFMP)composite.This method leverages the inherent microcracks and Li vacancies present in S-LFP,likely acting as diffusion channels for the Mn^(2+)/Li^(+)ions.Through a two-step mechanochemical ball-milling and carbothermal reduction process,this approach achieves simultaneous Li replenishment and surface-localised Mn gradient doping with enhanced structural control.Notably,the R-LFMP exhibits an exceptional electrochemical performance.At 0.1 C,it delivers a discharge capacity of 161.4 mA h g^(−1)and an energy density of 563.5 Wh kg^(−1)(representing a 60.5%improvement over S-LFP).Additionally,it maintains 83%capacity retention after 900 cycles at 0.5C,a considerable enhancement compared to commercial LFMP(62%).Furthermore,the regenerated cathode material generates a net profit of$7.102 kg^(−1),surpassing the profitability of conventional recycling methods by 90%.Overall,this study introduces a transformative and sustainable LFP regeneration technology,achieving breakthroughs in electrochemical restoration and high-value recycling,while paving the way for the closed-loop utilisation of LFP-based energy storage systems.
基金supported by the National Natural Science Foundation of China(52072196,52002200,52102106,52202262,22379081,22379080)the Major Basic Research Program of Natural Science Foundation of Shandong Province(ZR2020ZD09)+1 种基金the Natural Science Foundation of Shandong Province(ZR2020QE063,ZR202108180009,ZR2023QE059)the Project funded by China Postdoctoral Science Foundation(2023M741871)。
文摘Steering the directional carrier migration across the interface is a central mission for efficient photocatalytic reactions.In this work,an atomic-shared heterointerface is constructed between the defect-rich ZnIn_(2)S_(4)(HVs-ZIS)and CoIn_(2)S_(4)(CIS)via a defect-guided heteroepitaxial growth strategy.The strong interface coupling induces adequate carriers exchanging passageway between HVs-ZIS and CIS,enhancing the internal electric field(IEF)in the ZnIn_(2)S_(4)/CoIn_(2)S_(4)(HVs-ZIS/CIS)heterostructure.The defect structure in HVs-ZIS induces an additional defect level,improving the separation efficiency of photocarriers.Moreover,promoted by the IEF and intimate heterointerface,photogenerated electrons trapped by the defect level can migrate to the valence band of CIS,contributing to massive photogenerated electrons with intense reducibility in HVs-ZIS/CIS.Consequently,the HVs-ZIS/CIS heterostructure performs a boosted H_(2)evolution activity of 33.65 mmol g^(-1)h^(-1).This work highlights the synergistic effects of defect and strong interface coupling in regulating carrier transfer and paves a brave avenue for constructing efficient heterostructure photocatalysts.
