Lithium(Li)deposition and nucleation at solid electrolyte interphase(SEI)is the main origin for the capacity decay in Li metal batteries(LMBs).SEI conversion with enhanced electrochemical and mechanical properties is ...Lithium(Li)deposition and nucleation at solid electrolyte interphase(SEI)is the main origin for the capacity decay in Li metal batteries(LMBs).SEI conversion with enhanced electrochemical and mechanical properties is an effective approach to achieve uniform nucleation of Li^(+)and stabilize the lithium metal anode.However,complex interfacial reaction mechanisms and interface compatibility issues hinder the development of SEI conversion strategies for stabilizing lithium metal anodes.Herein,we presented the release of I_(3)^(-)in–NH_(2)-modified metal–organic frameworks for a Li metal surface SEI phase conversion strategy.The–NH_(2)group in MOF pores induced the formation of I_(3)^(-)from I_(2),which was further spontaneously reacted with inactive Li_(2)O transforming into high-performance LiI and LiIO_(3)interphase.Furthermore,theoretical calculation provided deeply insight into the unique reconstructed interfacial formation and electrochemical mechanism of rich LiI and LiIO_(3)SEI.As a result,the Li^(+)deposition and nucleation were improved,facilitating the transport kinetics of Li^(+)and inhibiting the growth of lithium dendrites.The assembled solid-state Li||LiFePO_(4)full cells exhibited superior long-term stability of 800 cycles and high Coulombic efficiency(>99%),Li||LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)pouch cell also displayed superior practical performance over 200 cycles at 2 C,high loading of 5 mg cm^(-2)and safety performance.This innovative SEI design strategy promotes the development of high-performance solid-state Li metal batteries.展开更多
Solid electrolyte interphase(SEI)plays a critical role in stabilizing zinc batteries,yet insufficient attention has been given to its in-situ growth kinetics and the post-stripping morphology of zinc anodes,both affec...Solid electrolyte interphase(SEI)plays a critical role in stabilizing zinc batteries,yet insufficient attention has been given to its in-situ growth kinetics and the post-stripping morphology of zinc anodes,both affecting the SEI-forming quality.Herein,we showcase a synergistic effect between uniform Zn stripping and rapid SEI formation through introducing tetramethylurea(TMU)into Zn(BF_(4))_(2)-based electrolytes.TMU participates in the Zn^(2+)solvation structure and reshapes the electrolyte hydrogen-bond network,enabling a water-poor electric double layer that mitigates the corrosion-induced stripping inhomogeneity.Subsequently,a multi-component and inorganic-rich SEI with high uniformity is rapidly deposited during the plating process.This SEI with abundant zincophilic sites activates instantaneous nucleation and hence guides dense and uniform Zn deposition.With enhanced Zn stripping/plating symmetry,the long-term effectiveness of SEI is guaranteed,contributing to the high reversibility over 3200 h at 1 mA cm^(-2)/2 mAh cm^(-2).Impressively,the Zn//NaV_(3)O_(8)full cell(4.43 mAh cm^(-2))can be steadily cycled at 0.1 A g^(-1)under an intermittent-rest protocol.The stable operation of an Ah-level pouch cell over 100 cycles further demonstrates the scalability of this strategy and highlights the significance of achieving high stripping/plating symmetry and a long-term effective SEI toward practical zinc batteries.展开更多
基金financial support from National Natural Science Foundation of China(22271178,U2032131,21972103)International Cooperation Key Project of Science and Technology Department of Shaanxi,China(2022KWZ-06)+3 种基金the Youth Talent Promotion Project of Science and Technology Association of Universities of Shaanxi Province(20210602)Research Project of Xi’an Science and Technology Bureau(2022GXFW0011)Science and Technology New Star in Shaanxi Province(2023KJXX-045)Shaanxi Provincial Department of Education Service Local Special Project,Industrialization Cultivation Project(23JC007)。
文摘Lithium(Li)deposition and nucleation at solid electrolyte interphase(SEI)is the main origin for the capacity decay in Li metal batteries(LMBs).SEI conversion with enhanced electrochemical and mechanical properties is an effective approach to achieve uniform nucleation of Li^(+)and stabilize the lithium metal anode.However,complex interfacial reaction mechanisms and interface compatibility issues hinder the development of SEI conversion strategies for stabilizing lithium metal anodes.Herein,we presented the release of I_(3)^(-)in–NH_(2)-modified metal–organic frameworks for a Li metal surface SEI phase conversion strategy.The–NH_(2)group in MOF pores induced the formation of I_(3)^(-)from I_(2),which was further spontaneously reacted with inactive Li_(2)O transforming into high-performance LiI and LiIO_(3)interphase.Furthermore,theoretical calculation provided deeply insight into the unique reconstructed interfacial formation and electrochemical mechanism of rich LiI and LiIO_(3)SEI.As a result,the Li^(+)deposition and nucleation were improved,facilitating the transport kinetics of Li^(+)and inhibiting the growth of lithium dendrites.The assembled solid-state Li||LiFePO_(4)full cells exhibited superior long-term stability of 800 cycles and high Coulombic efficiency(>99%),Li||LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)pouch cell also displayed superior practical performance over 200 cycles at 2 C,high loading of 5 mg cm^(-2)and safety performance.This innovative SEI design strategy promotes the development of high-performance solid-state Li metal batteries.
基金supported by the National Natural Science Foundation of China(52372252)the Science and Technology Innovation Program of Hunan Province(2024RC1022)+1 种基金the Hunan Provincial Natural Science Foundation of China(2025JJ60356)the Changsha Municipal Natural Science Foundation(kq2502024).
文摘Solid electrolyte interphase(SEI)plays a critical role in stabilizing zinc batteries,yet insufficient attention has been given to its in-situ growth kinetics and the post-stripping morphology of zinc anodes,both affecting the SEI-forming quality.Herein,we showcase a synergistic effect between uniform Zn stripping and rapid SEI formation through introducing tetramethylurea(TMU)into Zn(BF_(4))_(2)-based electrolytes.TMU participates in the Zn^(2+)solvation structure and reshapes the electrolyte hydrogen-bond network,enabling a water-poor electric double layer that mitigates the corrosion-induced stripping inhomogeneity.Subsequently,a multi-component and inorganic-rich SEI with high uniformity is rapidly deposited during the plating process.This SEI with abundant zincophilic sites activates instantaneous nucleation and hence guides dense and uniform Zn deposition.With enhanced Zn stripping/plating symmetry,the long-term effectiveness of SEI is guaranteed,contributing to the high reversibility over 3200 h at 1 mA cm^(-2)/2 mAh cm^(-2).Impressively,the Zn//NaV_(3)O_(8)full cell(4.43 mAh cm^(-2))can be steadily cycled at 0.1 A g^(-1)under an intermittent-rest protocol.The stable operation of an Ah-level pouch cell over 100 cycles further demonstrates the scalability of this strategy and highlights the significance of achieving high stripping/plating symmetry and a long-term effective SEI toward practical zinc batteries.
