The point-to-point contact mechanism in all-solid-state Li-S batteries(ASSLSBs)is not as efficient as a liquid electrolyte which has superior mobility in the electrode,resulting in a slower reaction kinetics and inade...The point-to-point contact mechanism in all-solid-state Li-S batteries(ASSLSBs)is not as efficient as a liquid electrolyte which has superior mobility in the electrode,resulting in a slower reaction kinetics and inadequate ionic/electronic conduction network between the S(or Li_(2)S),conductive carbon,and solid-state electrolytes(SSEs)for achieving a swift(dis)charge reaction.Herein,a series of hybrid ionic/electronic conduction triple-phase interfaces with transition metal and nitrogen co-doping were designed.The graphitic ordered mesoporous carbon frameworks(TM-N-OMCs;TM=Fe,Co,Ni,and Cu)serve as hosts for Li_(2)S and Li_(6)PS_(5)Cl(LPSC)and provide abundant reaction sites on the triple interface.Results from both experimental and computational research display that the combination of Cu-N co-dopants can promote the Li-ion diffusion for rapid transformation of Li_(2)S with adequate ionic(6.73×10^(−4)S·cm^(−1))/electronic conductivities(1.77×10^(−2)S·cm^(−1))at 25℃.The as-acquired Li_(2)S/Cu-N-OMC/LPSC electrode exhibits a high reversible capacity(1147.7 mAh·g^(−1))at 0.1 C,excellent capacity retention(99.5%)after 500 cycles at 0.5 C,and high areal capacity(7.08 mAh·cm^(−2)).展开更多
基金supported by the National Natural Science Foundation of China(No.T2241003)the National Key Research and Development Program of China(No.2022YFB4003500)the Key R&D project of Hubei Province,China(No.2021AAA006).
文摘The point-to-point contact mechanism in all-solid-state Li-S batteries(ASSLSBs)is not as efficient as a liquid electrolyte which has superior mobility in the electrode,resulting in a slower reaction kinetics and inadequate ionic/electronic conduction network between the S(or Li_(2)S),conductive carbon,and solid-state electrolytes(SSEs)for achieving a swift(dis)charge reaction.Herein,a series of hybrid ionic/electronic conduction triple-phase interfaces with transition metal and nitrogen co-doping were designed.The graphitic ordered mesoporous carbon frameworks(TM-N-OMCs;TM=Fe,Co,Ni,and Cu)serve as hosts for Li_(2)S and Li_(6)PS_(5)Cl(LPSC)and provide abundant reaction sites on the triple interface.Results from both experimental and computational research display that the combination of Cu-N co-dopants can promote the Li-ion diffusion for rapid transformation of Li_(2)S with adequate ionic(6.73×10^(−4)S·cm^(−1))/electronic conductivities(1.77×10^(−2)S·cm^(−1))at 25℃.The as-acquired Li_(2)S/Cu-N-OMC/LPSC electrode exhibits a high reversible capacity(1147.7 mAh·g^(−1))at 0.1 C,excellent capacity retention(99.5%)after 500 cycles at 0.5 C,and high areal capacity(7.08 mAh·cm^(−2)).
