All-solid-state batteries(ASSB) with lithium anode have attracted ever-increasing attention towards developing safer batteries with high energy densities.While great advancement has been achieved in developing solid e...All-solid-state batteries(ASSB) with lithium anode have attracted ever-increasing attention towards developing safer batteries with high energy densities.While great advancement has been achieved in developing solid electrolytes(SE) with superb ionic conductivity rivalling that of the current liquid technology,it has yet been very difficult in their successful application to ASSBs with sustaining rate and cyclic performances.Here in this work,we have realized a stable ASSB using the Li_(6.25)PS_(5.25)Cl_(0.75) fast ionconducting electrolyte together with LiNbO_3 coated LiCoO_2 as cathode and lithium foil as the anode.The effective diffusion coefficient of Li-ions in the battery is higher than 10^(-12) cm~2 s^(-1),and the significantly enhanced electrochemical matching at the cathode-electrolyte interface was essential to enable long-term stability against high oxidation potential,with the LCO@LNO/Li_(6.25)PS_(5.25)Cl_(0.75)/Li battery to retain 74.12% capacity after 430 cycles at 100 μA cm-2 and 59.7% of capacity after 800 cycles at 50 μA cm^(-2),at a high charging cut-off voltage of 4.2 V.This demonstrates that the Li_(6.25)PS_(5.25)Cl_(0.75) can be an excellent electrolyte for the realization of stable ASSBs with high-voltage cathodes and metallic lithium as anode,once the electrochemical compatibility between cathode and electrolyte can be addressed with a suitable buffer coating.展开更多
Heteroatom doped graphene materials are considered as promising anode for high-performance sodium-ion batteries(SIBs).Defective and porous structure especially with large specific surface area is generally considered ...Heteroatom doped graphene materials are considered as promising anode for high-performance sodium-ion batteries(SIBs).Defective and porous structure especially with large specific surface area is generally considered as a feasible strategy to boost reaction kinetics;however,the unwanted side reaction at the anode hinders the practical application of SIBs.In this work,a precisely controlled Al_(2)O_(3)coated nitrogen doped vertical graphene nanosheets(NVG)anode material has been proposed,which exhibits excellent sodium storage capacity and cycling stability.The ultrathin Al_(2)O_(3)coating on the NVG is considered to help construct an advantageous interface between electrode and electrolyte,both alleviating the electrolyte decomposition and enhancing sodium adsorption ability.As a result,the optimal Al_(2)O_(3)coated NVG materials delivers a high reversible capacity(835.0 mAh g^(-1))and superior cycling stability(retention of 92.3%after 5000 cycles).This work demonstrates a new way to design graphene-based anode materials for highperformance sodium-ion batteries.展开更多
Vertical graphene(VG),possessing superior chemical,physical,and structural peculiarities,holds great promise as a building block for constructing a high-energy density lithium-sulfur(Li-S)battery.Therefore,it is desir...Vertical graphene(VG),possessing superior chemical,physical,and structural peculiarities,holds great promise as a building block for constructing a high-energy density lithium-sulfur(Li-S)battery.Therefore,it is desirable to develop a new VG growth technique with a novel structure to enable wide applications.Herein,we devise a novel complex permittivity-dependent plasma confinement-assisted VG growth technique,via asymmetric growing a VG layer on one side of N-doped carbon nanofibers for the first time,using a unique lab-built high flux plasma-enhanced chemical vapor deposition system,as a bifunctional nanofiber membrane to construct Li-S batteries with low neg-ative/positive(N/P)and electrolyte/sulfur(E/S)ratios.The unique nanofiber membrane could simultaneously protect the cathode and anode,enabling an excellent electrochemical performance with low N/P and E/S ratios in Li-S bat-teries.Such a full cell delivers high gravimetric energy density and volumetric energy density of 340 Wh kg^(-1) and 547 Wh L^(-1),respectively,at low N/P(2:1)and E/S(4:1)ratios.Furthermore,a pouch cell achieves a high areal capacity of 7.1 mAh cm^(-2) at a sulfur loading of 6 mg cm^(-2).This work put forward a novel pathway for the design of high-energy density Li-S batteries.展开更多
基金supported in part by the 1000 Talents Program of China, the Zhengzhou Materials Genome Institute (ZMGI)the Natural Science Foundation of China (Nos. 51001091, 91233101)the Fundamental Research Program from the Ministry of Science and Technology of China (no. 2014CB931704)。
文摘All-solid-state batteries(ASSB) with lithium anode have attracted ever-increasing attention towards developing safer batteries with high energy densities.While great advancement has been achieved in developing solid electrolytes(SE) with superb ionic conductivity rivalling that of the current liquid technology,it has yet been very difficult in their successful application to ASSBs with sustaining rate and cyclic performances.Here in this work,we have realized a stable ASSB using the Li_(6.25)PS_(5.25)Cl_(0.75) fast ionconducting electrolyte together with LiNbO_3 coated LiCoO_2 as cathode and lithium foil as the anode.The effective diffusion coefficient of Li-ions in the battery is higher than 10^(-12) cm~2 s^(-1),and the significantly enhanced electrochemical matching at the cathode-electrolyte interface was essential to enable long-term stability against high oxidation potential,with the LCO@LNO/Li_(6.25)PS_(5.25)Cl_(0.75)/Li battery to retain 74.12% capacity after 430 cycles at 100 μA cm-2 and 59.7% of capacity after 800 cycles at 50 μA cm^(-2),at a high charging cut-off voltage of 4.2 V.This demonstrates that the Li_(6.25)PS_(5.25)Cl_(0.75) can be an excellent electrolyte for the realization of stable ASSBs with high-voltage cathodes and metallic lithium as anode,once the electrochemical compatibility between cathode and electrolyte can be addressed with a suitable buffer coating.
基金supported by the National Natural Science Foundation of China(Nos.51602290,91233101,11174256)the Fundamental Research Program from the Ministry of Science and Technology of China(No.2014CB31704)Project funded by China Postdoctoral Science Foundation(No.2016M592310)。
文摘Heteroatom doped graphene materials are considered as promising anode for high-performance sodium-ion batteries(SIBs).Defective and porous structure especially with large specific surface area is generally considered as a feasible strategy to boost reaction kinetics;however,the unwanted side reaction at the anode hinders the practical application of SIBs.In this work,a precisely controlled Al_(2)O_(3)coated nitrogen doped vertical graphene nanosheets(NVG)anode material has been proposed,which exhibits excellent sodium storage capacity and cycling stability.The ultrathin Al_(2)O_(3)coating on the NVG is considered to help construct an advantageous interface between electrode and electrolyte,both alleviating the electrolyte decomposition and enhancing sodium adsorption ability.As a result,the optimal Al_(2)O_(3)coated NVG materials delivers a high reversible capacity(835.0 mAh g^(-1))and superior cycling stability(retention of 92.3%after 5000 cycles).This work demonstrates a new way to design graphene-based anode materials for highperformance sodium-ion batteries.
基金National Natural Science Foundation of China,Grant/Award Numbers:51972287,U2004172,51502269Foundation for University Key Teachers of Henan Province,Grant/Award Number:2020GGJS009Natural Science Foundation of Henan Province,Grant/Award Number:202300410368。
文摘Vertical graphene(VG),possessing superior chemical,physical,and structural peculiarities,holds great promise as a building block for constructing a high-energy density lithium-sulfur(Li-S)battery.Therefore,it is desirable to develop a new VG growth technique with a novel structure to enable wide applications.Herein,we devise a novel complex permittivity-dependent plasma confinement-assisted VG growth technique,via asymmetric growing a VG layer on one side of N-doped carbon nanofibers for the first time,using a unique lab-built high flux plasma-enhanced chemical vapor deposition system,as a bifunctional nanofiber membrane to construct Li-S batteries with low neg-ative/positive(N/P)and electrolyte/sulfur(E/S)ratios.The unique nanofiber membrane could simultaneously protect the cathode and anode,enabling an excellent electrochemical performance with low N/P and E/S ratios in Li-S bat-teries.Such a full cell delivers high gravimetric energy density and volumetric energy density of 340 Wh kg^(-1) and 547 Wh L^(-1),respectively,at low N/P(2:1)and E/S(4:1)ratios.Furthermore,a pouch cell achieves a high areal capacity of 7.1 mAh cm^(-2) at a sulfur loading of 6 mg cm^(-2).This work put forward a novel pathway for the design of high-energy density Li-S batteries.