The poor reversibility of Zn anodes induced by dendrite growth,surface passivation,and corrosion,severely hinders the practical applicability of Zn metal batteries.To address these issues,a plasmaassisted aerogel(PAG)...The poor reversibility of Zn anodes induced by dendrite growth,surface passivation,and corrosion,severely hinders the practical applicability of Zn metal batteries.To address these issues,a plasmaassisted aerogel(PAG)interface engineering was proposed as efficient ion transport modulator that can simultaneously regulate uniform Zn^(2+)flux and desolvation behavior during battery operation.The PAG with ordered mesopores acted as an ion sieve to homogenize Zn deposition and accelerate Zn^(2+)flux,which is favorable for corrosion resistance and dendrite suppression.Importantly,the plasma-assisted aerogel with abundant hydrophilic groups can facilitate the desolvation kinetics of Zn^(2+)due to the multiple hydrogen-bonding interaction with the activated water molecules,thus accelerating the Zn^(2+)migration kinetics.Consequently,the Zn/Zn cell assembled with PAG-modified separator demonstrates stable plating and stripping behavior(over 1400 h at 1 mA cm^(-2))and high Coulombic efficiency(99.8%at1 mA cm^(-2)after 1100 cycles),and the Zn‖MnO_(2)full cell shows excellent long-term cycling stability and maintains a high capacity of 154.9 mA h g^(-1)after 1000 cycles at 1 A g^(-1).This study provides a feasible approach for the large-scale fabrication of aerogel functionalized separators to realize ultra-stable Zn metal batteries.展开更多
Designing a step-scheme(S-scheme)heterojunction photocatalyst with vacancy engineering is a reliable approach to achieve highly efficient photocatalytic H_(2)production activity.Herein,a hollow ZnO/ZnS S-scheme hetero...Designing a step-scheme(S-scheme)heterojunction photocatalyst with vacancy engineering is a reliable approach to achieve highly efficient photocatalytic H_(2)production activity.Herein,a hollow ZnO/ZnS S-scheme heterojunction with O and Zn vacancies(VO,Zn-ZnO/ZnS)is rationally constructed via ion-exchange and calcination treatments.In such a photocatalytic system,the hollow structure combined with the introduction of dual vacancies endows the adequate light absorption.Moreover,the O and Zn vacancies serve as the trapping sites for photo-induced electrons and holes,respectively,which are beneficial for promoting the photo-induced carrier separation.Meanwhile,the S-scheme charge transfer mechanism can not only improve the separation and transfer efficiencies of photo-induced carrier but also retain the strong redox capacity.As expected,the optimized VO,Zn-ZnO/ZnS heterojunction exhibits a superior photocatalytic H_(2) production rate of 160.91 mmol g^(-1)h^(-1),approximately 643.6 times and 214.5 times with respect to that obtained on pure ZnO and ZnS,respectively.Simultaneously,the experimental results and density functional theory calculations disclose that the photo-induced carrier transfer pathway follows the S-scheme heterojunction mechanism and the introduction of O and Zn vacancies reduces the surface reaction barrier.This work provides an innovative strategy of vacancy engineering in S-scheme heterojunction for solar-to-fuel energy conversion.展开更多
锂硫电池由于其高能量密度、低成本效益被认为是最有前途的下一代电池体系之一.然而多硫化物的穿梭效应大幅降低了锂硫电池的循环稳定性和寿命,严重阻碍其实际应用.无机金属化合物材料改性的隔膜不仅能抑制多硫化锂(LiPS)的穿梭效应,其...锂硫电池由于其高能量密度、低成本效益被认为是最有前途的下一代电池体系之一.然而多硫化物的穿梭效应大幅降低了锂硫电池的循环稳定性和寿命,严重阻碍其实际应用.无机金属化合物材料改性的隔膜不仅能抑制多硫化锂(LiPS)的穿梭效应,其部分特殊的晶面还能加速多硫化物的氧化还原反应动力学.本文在罗盘状ZnS表面原位生长球状的MoO_(2),制备MoO_(2)/ZnS复合材料.MoO_(2)对多硫化物有着较强的吸附作用,ZnS有着良好的电导率,两者的复合可加速电子传导效率和氧化还原速率.以所制备的MoO_(2)/ZnS作为隔膜改性材料,锂硫电池在5 C的大电流密度下,经过1000次循环后仍可以保持690 mAh g^(-1)的放电比容量,平均每圈的容量衰减率仅为0.014%,表现出优异的循环性能和倍率性能.展开更多
The effects of zirconium addition on the microstructure and mechanical properties of Mg97Y2Zn1 alloy were investigated.The microstructure of as-cast Mg97Y2Zn1 alloy is refined by the addition of zirconium.During the e...The effects of zirconium addition on the microstructure and mechanical properties of Mg97Y2Zn1 alloy were investigated.The microstructure of as-cast Mg97Y2Zn1 alloy is refined by the addition of zirconium.During the extrusion,the initial nucleation sites of the alloy are mainly original grain boundaries and secondary phase.The addition of zirconium could stimulate the DRX process because more grain boundaries are formed,which increases the dynamic recrystallization rate.Both the strength and elongation of the alloy are increased by the addition of zirconium.展开更多
Achieving a highly robust zinc(Zn)metal anode is extremely important for improving the performance of aqueous Zn-ion batteries(AZIBs)for advancing“carbon neutrality”society,which is hampered by the uncontrollable gr...Achieving a highly robust zinc(Zn)metal anode is extremely important for improving the performance of aqueous Zn-ion batteries(AZIBs)for advancing“carbon neutrality”society,which is hampered by the uncontrollable growth of Zn dendrite and severe side reactions including hydrogen evolution reaction,corrosion,and passivation,etc.Herein,an interlayer containing fluorinated zincophilic covalent organic framework with sulfonic acid groups(COF-S-F)is developed on Zn metal(Zn@COF-S-F)as the artificial solid electrolyte interface(SEI).Sulfonic acid group(-SO_(3)H)in COF-S-F can effectively ameliorate the desolvation process of hydrated Zn ions,and the three-dimensional channel with fluoride group(-F)can provide interconnected channels for the favorable transport of Zn ions with ion-confinement effects,endowing Zn@COF-S-F with dendrite-free morphology and suppressed side reactions.Consequently,Zn@COF-S-F symmetric cell can stably cycle for 1,000 h with low average hysteresis voltage(50.5 m V)at the current density of 1.5 m A cm^(-2).Zn@COF-S-F|Mn O_(2)cell delivers the discharge specific capacity of 206.8 m Ah g^(-1)at the current density of 1.2 A g^(-1)after 800 cycles with high-capacity retention(87.9%).Enlightening,building artificial SEI on metallic Zn surface with targeted design has been proved as the effective strategy to foster the practical application of high-performance AZIBs.展开更多
Recently,rechargeable aqueous zinc-based batteries using manganese oxide as the cathode(e.g.,MnO_(2))have gained attention due to their inherent safety,environmental friendliness,and low cost.Despite their potential,a...Recently,rechargeable aqueous zinc-based batteries using manganese oxide as the cathode(e.g.,MnO_(2))have gained attention due to their inherent safety,environmental friendliness,and low cost.Despite their potential,achieving high energy density in Zn||MnO_(2)batteries remains challenging,highlighting the need to understand the electrochemical reaction mechanisms underlying these batteries more deeply and optimize battery components,including electrodes and electrolytes.This review comprehensively summarizes the latest advancements for understanding the electrochemistry reaction mechanisms and designing electrodes and electrolytes for Zn||MnO_(2)batteries in mildly and strongly acidic environments.Furthermore,we highlight the key challenges hindering the extensive application of Zn||MnO_(2)batteries,including high-voltage requirements and areal capacity,and propose innovative solutions to overcome these challenges.We suggest that MnO_(2)/Mn^(2+)conversion in neutral electrolytes is a crucial aspect that needs to be addressed to achieve high-performance Zn||MnO_(2)batteries.These approaches could lead to breakthroughs in the future development of Zn||MnO_(2)batteries,off ering a more sustainable,costeff ective,and high-performance alternative to traditional batteries.展开更多
Zn powder anodes have attracted much attention in aqueous Zn ion battery applications due to advantages such as low cost and processability.However,the high-activity Zn powder anode faces problems such as side reactio...Zn powder anodes have attracted much attention in aqueous Zn ion battery applications due to advantages such as low cost and processability.However,the high-activity Zn powder anode faces problems such as side reactions,hydrogen evolution,and dendrites,which limit the cycling stability of the cell.In this work,the high activity of Zn powder is weakened by introducing low-cost erythritol as a functional additive in the ZnSO_(4) electrolyte to improve the cycle life of the cell.Both theoretical calculations and empirical evidence demonstrate that the incorporation of erythritol alters the coordination sphere of Zn^(2+)and modifies the local molecular architecture of the electrolyte.This modification serves to diminish the reactivity of water molecules,thereby efficaciously suppressing dendrite formation and deleterious ancillary reactions on the zinc powder anode surfaces.Concurrently,erythritol functions as an interfacial cationic captor,enhancing reaction dynamics and facilitating the development of a favorable protective layer throughout the zinc plating/stripping process.Consequently,the symmetric cell paired with an erythritol-containing electrolyte manifests stable cycling performance for an extended duration of 850 h at a current density of 0.288 mA cm^(-2)and areal capacity of 0.144 mAh cm^(-2).Notably,it maintains a cycling life of 400 h even under intensified conditions (2.88 mA cm^(-2)/1.44 mA h cm^(-2)).Furthermore,the constructed Na_(2)V_(6)O_(16)·3H_(2)O full cell illustrated remarkable capacity retention of 155.8 mA h g^(-1)following 800 cycles at a high rate of 5 A g^(-1).展开更多
基金financially supported by the National Natural Science Foundation of China(NSFC)(52203261)Natural Science Foundation of Jiangsu Province(BK20210474)the project of research on the industrial application of"controllable synthesis of nanocarbon-based polymer composites and their application in new energy”(N0.CJGJZD20210408092400002).
文摘The poor reversibility of Zn anodes induced by dendrite growth,surface passivation,and corrosion,severely hinders the practical applicability of Zn metal batteries.To address these issues,a plasmaassisted aerogel(PAG)interface engineering was proposed as efficient ion transport modulator that can simultaneously regulate uniform Zn^(2+)flux and desolvation behavior during battery operation.The PAG with ordered mesopores acted as an ion sieve to homogenize Zn deposition and accelerate Zn^(2+)flux,which is favorable for corrosion resistance and dendrite suppression.Importantly,the plasma-assisted aerogel with abundant hydrophilic groups can facilitate the desolvation kinetics of Zn^(2+)due to the multiple hydrogen-bonding interaction with the activated water molecules,thus accelerating the Zn^(2+)migration kinetics.Consequently,the Zn/Zn cell assembled with PAG-modified separator demonstrates stable plating and stripping behavior(over 1400 h at 1 mA cm^(-2))and high Coulombic efficiency(99.8%at1 mA cm^(-2)after 1100 cycles),and the Zn‖MnO_(2)full cell shows excellent long-term cycling stability and maintains a high capacity of 154.9 mA h g^(-1)after 1000 cycles at 1 A g^(-1).This study provides a feasible approach for the large-scale fabrication of aerogel functionalized separators to realize ultra-stable Zn metal batteries.
文摘Designing a step-scheme(S-scheme)heterojunction photocatalyst with vacancy engineering is a reliable approach to achieve highly efficient photocatalytic H_(2)production activity.Herein,a hollow ZnO/ZnS S-scheme heterojunction with O and Zn vacancies(VO,Zn-ZnO/ZnS)is rationally constructed via ion-exchange and calcination treatments.In such a photocatalytic system,the hollow structure combined with the introduction of dual vacancies endows the adequate light absorption.Moreover,the O and Zn vacancies serve as the trapping sites for photo-induced electrons and holes,respectively,which are beneficial for promoting the photo-induced carrier separation.Meanwhile,the S-scheme charge transfer mechanism can not only improve the separation and transfer efficiencies of photo-induced carrier but also retain the strong redox capacity.As expected,the optimized VO,Zn-ZnO/ZnS heterojunction exhibits a superior photocatalytic H_(2) production rate of 160.91 mmol g^(-1)h^(-1),approximately 643.6 times and 214.5 times with respect to that obtained on pure ZnO and ZnS,respectively.Simultaneously,the experimental results and density functional theory calculations disclose that the photo-induced carrier transfer pathway follows the S-scheme heterojunction mechanism and the introduction of O and Zn vacancies reduces the surface reaction barrier.This work provides an innovative strategy of vacancy engineering in S-scheme heterojunction for solar-to-fuel energy conversion.
文摘锂硫电池由于其高能量密度、低成本效益被认为是最有前途的下一代电池体系之一.然而多硫化物的穿梭效应大幅降低了锂硫电池的循环稳定性和寿命,严重阻碍其实际应用.无机金属化合物材料改性的隔膜不仅能抑制多硫化锂(LiPS)的穿梭效应,其部分特殊的晶面还能加速多硫化物的氧化还原反应动力学.本文在罗盘状ZnS表面原位生长球状的MoO_(2),制备MoO_(2)/ZnS复合材料.MoO_(2)对多硫化物有着较强的吸附作用,ZnS有着良好的电导率,两者的复合可加速电子传导效率和氧化还原速率.以所制备的MoO_(2)/ZnS作为隔膜改性材料,锂硫电池在5 C的大电流密度下,经过1000次循环后仍可以保持690 mAh g^(-1)的放电比容量,平均每圈的容量衰减率仅为0.014%,表现出优异的循环性能和倍率性能.
基金Project (51001072) supported by the National Natural Science Foundation of China
文摘The effects of zirconium addition on the microstructure and mechanical properties of Mg97Y2Zn1 alloy were investigated.The microstructure of as-cast Mg97Y2Zn1 alloy is refined by the addition of zirconium.During the extrusion,the initial nucleation sites of the alloy are mainly original grain boundaries and secondary phase.The addition of zirconium could stimulate the DRX process because more grain boundaries are formed,which increases the dynamic recrystallization rate.Both the strength and elongation of the alloy are increased by the addition of zirconium.
基金financially supported by National Natural Science Foundation of China(Nos.51872090,51772097,52372252)Hebei Natural Science Fund for Distinguished Young Scholar(No.E2019209433)+1 种基金Youth Talent Program of Hebei Provincial Education Department(No.BJ2018020)Natural Science Foundation of Hebei Province(No.E2020209151)。
文摘Achieving a highly robust zinc(Zn)metal anode is extremely important for improving the performance of aqueous Zn-ion batteries(AZIBs)for advancing“carbon neutrality”society,which is hampered by the uncontrollable growth of Zn dendrite and severe side reactions including hydrogen evolution reaction,corrosion,and passivation,etc.Herein,an interlayer containing fluorinated zincophilic covalent organic framework with sulfonic acid groups(COF-S-F)is developed on Zn metal(Zn@COF-S-F)as the artificial solid electrolyte interface(SEI).Sulfonic acid group(-SO_(3)H)in COF-S-F can effectively ameliorate the desolvation process of hydrated Zn ions,and the three-dimensional channel with fluoride group(-F)can provide interconnected channels for the favorable transport of Zn ions with ion-confinement effects,endowing Zn@COF-S-F with dendrite-free morphology and suppressed side reactions.Consequently,Zn@COF-S-F symmetric cell can stably cycle for 1,000 h with low average hysteresis voltage(50.5 m V)at the current density of 1.5 m A cm^(-2).Zn@COF-S-F|Mn O_(2)cell delivers the discharge specific capacity of 206.8 m Ah g^(-1)at the current density of 1.2 A g^(-1)after 800 cycles with high-capacity retention(87.9%).Enlightening,building artificial SEI on metallic Zn surface with targeted design has been proved as the effective strategy to foster the practical application of high-performance AZIBs.
文摘Recently,rechargeable aqueous zinc-based batteries using manganese oxide as the cathode(e.g.,MnO_(2))have gained attention due to their inherent safety,environmental friendliness,and low cost.Despite their potential,achieving high energy density in Zn||MnO_(2)batteries remains challenging,highlighting the need to understand the electrochemical reaction mechanisms underlying these batteries more deeply and optimize battery components,including electrodes and electrolytes.This review comprehensively summarizes the latest advancements for understanding the electrochemistry reaction mechanisms and designing electrodes and electrolytes for Zn||MnO_(2)batteries in mildly and strongly acidic environments.Furthermore,we highlight the key challenges hindering the extensive application of Zn||MnO_(2)batteries,including high-voltage requirements and areal capacity,and propose innovative solutions to overcome these challenges.We suggest that MnO_(2)/Mn^(2+)conversion in neutral electrolytes is a crucial aspect that needs to be addressed to achieve high-performance Zn||MnO_(2)batteries.These approaches could lead to breakthroughs in the future development of Zn||MnO_(2)batteries,off ering a more sustainable,costeff ective,and high-performance alternative to traditional batteries.
基金supported by the Hunan Chenyu Fuji New Energy Technology Co. Ltd (2022zkhx501)the Hunan Province University Teaching Reform and Research Project (HNJG-20230364)the Ministry of Education’s Industry-University Cooperation and Collaborative Talent Development Program(231106707093309)。
文摘Zn powder anodes have attracted much attention in aqueous Zn ion battery applications due to advantages such as low cost and processability.However,the high-activity Zn powder anode faces problems such as side reactions,hydrogen evolution,and dendrites,which limit the cycling stability of the cell.In this work,the high activity of Zn powder is weakened by introducing low-cost erythritol as a functional additive in the ZnSO_(4) electrolyte to improve the cycle life of the cell.Both theoretical calculations and empirical evidence demonstrate that the incorporation of erythritol alters the coordination sphere of Zn^(2+)and modifies the local molecular architecture of the electrolyte.This modification serves to diminish the reactivity of water molecules,thereby efficaciously suppressing dendrite formation and deleterious ancillary reactions on the zinc powder anode surfaces.Concurrently,erythritol functions as an interfacial cationic captor,enhancing reaction dynamics and facilitating the development of a favorable protective layer throughout the zinc plating/stripping process.Consequently,the symmetric cell paired with an erythritol-containing electrolyte manifests stable cycling performance for an extended duration of 850 h at a current density of 0.288 mA cm^(-2)and areal capacity of 0.144 mAh cm^(-2).Notably,it maintains a cycling life of 400 h even under intensified conditions (2.88 mA cm^(-2)/1.44 mA h cm^(-2)).Furthermore,the constructed Na_(2)V_(6)O_(16)·3H_(2)O full cell illustrated remarkable capacity retention of 155.8 mA h g^(-1)following 800 cycles at a high rate of 5 A g^(-1).
