The practical application of lithium(Li)metal batteries(LMBs)faces challenges due to the irreversible Li deposition/dissolution process,which promotes Li dendrite growth with severe parasitic reactions during cycling....The practical application of lithium(Li)metal batteries(LMBs)faces challenges due to the irreversible Li deposition/dissolution process,which promotes Li dendrite growth with severe parasitic reactions during cycling.To address these issues,achieving uniform Li‐ion flux and improving Li‐ion conductivity of the separator are the top priorities.Herein,a separator(PCELS)with enhanced Li‐ion conductivity,composed of polymer,ceramic,and electrically conductive carbon,is proposed to facilitate fast Li‐ion transport kinetics and increase Li deposition uniformity of the LMBs.The PCELS immobilizes PF6–anions with high adsorption energies,leading to a high Li‐ion transference number.Simultaneously,the PCELS shows excellent electrolyte wettability on both its sides,promoting rapid ion transport.Moreover,the electrically conductive carbon within the PCELS provides additional electron transport channels,enabling efficient charge transfer and uniform Li‐ion flux.With these advantages,the PCELS achieves rapid Li‐ion transport kinetics and uniform Li deposition,demonstrating excellent cycling stability over 100 cycles at a high current density of 12.0 mA cm^(-2).Furthermore,the PCELS shows stable cycling performances in Li–S cell tests and delivers an excellent capacity retention of 95.45%in the Li|LiFePO_(4) full‐cell test with a high areal capacity of over 5.5 mAh cm^(-2).展开更多
Lithium metal batteries(LMBs)offer high energy densities but face challenges including poor reversibility and Li dendrite growth.Herein,we evaluate two flexible composite current collectors composed of reduced graphen...Lithium metal batteries(LMBs)offer high energy densities but face challenges including poor reversibility and Li dendrite growth.Herein,we evaluate two flexible composite current collectors composed of reduced graphene oxide and carbon nanotubes(rGO/CNT)to investigate how Li storage mechanisms influence electrochemical performance.By modulating the number of layers in rGO,the few-layered rGO/CNT collector(FL-CC)stores Li through a pure plating mechanism,whereas the multi-layered rGO/CNT collector(ML-CC)stores lithium via a hybrid intercalation/plating mechanism.The hybrid mechanism in ML-CC promotes reversible Li-ion storage,reduces active Li-ion loss,and suppresses dendrite formation.As a result,ML-CC achieves superior cycling stability compared to FLCC in both LMBs and anode-free LMB tests paired with LiFePO_(4)cathodes at a practical areal capacity of 4.5 mAh cm^(-2).This study highlights the importance of structural design in current collectors and demonstrates that incorporating lithiatable materials can significantly enhance the electrochemical stability of anode-free LMBs.展开更多
基金supported by Ministry of Science and ICT,South Korea(RS‐2024‐00407282)National Research Foundation of Korea(RS‐2024‐00408156).
文摘The practical application of lithium(Li)metal batteries(LMBs)faces challenges due to the irreversible Li deposition/dissolution process,which promotes Li dendrite growth with severe parasitic reactions during cycling.To address these issues,achieving uniform Li‐ion flux and improving Li‐ion conductivity of the separator are the top priorities.Herein,a separator(PCELS)with enhanced Li‐ion conductivity,composed of polymer,ceramic,and electrically conductive carbon,is proposed to facilitate fast Li‐ion transport kinetics and increase Li deposition uniformity of the LMBs.The PCELS immobilizes PF6–anions with high adsorption energies,leading to a high Li‐ion transference number.Simultaneously,the PCELS shows excellent electrolyte wettability on both its sides,promoting rapid ion transport.Moreover,the electrically conductive carbon within the PCELS provides additional electron transport channels,enabling efficient charge transfer and uniform Li‐ion flux.With these advantages,the PCELS achieves rapid Li‐ion transport kinetics and uniform Li deposition,demonstrating excellent cycling stability over 100 cycles at a high current density of 12.0 mA cm^(-2).Furthermore,the PCELS shows stable cycling performances in Li–S cell tests and delivers an excellent capacity retention of 95.45%in the Li|LiFePO_(4) full‐cell test with a high areal capacity of over 5.5 mAh cm^(-2).
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea goverment(MSIT)(RS-2025-02218301)supported by the Nano&Material Technology Development Program through the National Research Foundation of Korea(NRF)funded by Ministry of Science and ICT(No.RS-2024-00412289).
文摘Lithium metal batteries(LMBs)offer high energy densities but face challenges including poor reversibility and Li dendrite growth.Herein,we evaluate two flexible composite current collectors composed of reduced graphene oxide and carbon nanotubes(rGO/CNT)to investigate how Li storage mechanisms influence electrochemical performance.By modulating the number of layers in rGO,the few-layered rGO/CNT collector(FL-CC)stores Li through a pure plating mechanism,whereas the multi-layered rGO/CNT collector(ML-CC)stores lithium via a hybrid intercalation/plating mechanism.The hybrid mechanism in ML-CC promotes reversible Li-ion storage,reduces active Li-ion loss,and suppresses dendrite formation.As a result,ML-CC achieves superior cycling stability compared to FLCC in both LMBs and anode-free LMB tests paired with LiFePO_(4)cathodes at a practical areal capacity of 4.5 mAh cm^(-2).This study highlights the importance of structural design in current collectors and demonstrates that incorporating lithiatable materials can significantly enhance the electrochemical stability of anode-free LMBs.
