Alumina nanostructures were obtained by two-step anodization process.The porous anodic aluminum oxide(AAO)membranes were anodized in oxalic acid,which was subsequently treated with chemical etching process with 1.0 mo...Alumina nanostructures were obtained by two-step anodization process.The porous anodic aluminum oxide(AAO)membranes were anodized in oxalic acid,which was subsequently treated with chemical etching process with 1.0 mol/L sodiumhydroxide solution,or mixed solution of phosphoric acid(6.0%)and chromic acid(1.8%),respectively.Field emission scanningelectron microscopy(FE-SEM)and transmission electron microscopy(TEM)were employed to character the morphology andstructure of the obtained alumina nanostructure.It is found that alumina nanowires are generated in the acidic chemical etchingsolution,while nanotube structures are formed in the alkaline solution.The influence of acid and alkaline solution on aluminamorphologies in the chemical etching process was discussed.展开更多
A double-layer TiO2 nanotube arrays were formed by two-step anodization of Ti foils in different electrolytes. First, Ti in 0.5 wt% HF was anodized to form thin nanotube layer. Afterwards a second anodization was cond...A double-layer TiO2 nanotube arrays were formed by two-step anodization of Ti foils in different electrolytes. First, Ti in 0.5 wt% HF was anodized to form thin nanotube layer. Afterwards a second anodization was conducted in a formamide based electrolyte, which allowed the second layer of nanotube growing directly underneath the first one. From FESEM investigation we found that the thickness of second layer corresponded to the anodization time, the increasing of which would lead to the excessive etching on the first layer. The first layer protected the lower one from fluoride corrosion during anodization process. The double layer TiO2 nanotube arrays showed no benefit to photodegradation effect in methyl orange degradation experiments.展开更多
SiC/Al-based composite foams were prepared by a two-step foaming method.The influence of the SiC content and its distribution uniformity on the foaming stability,cell structure,and mechanical properties of the aluminu...SiC/Al-based composite foams were prepared by a two-step foaming method.The influence of the SiC content and its distribution uniformity on the foaming stability,cell structure,and mechanical properties of the aluminum foams was investigated.The macro/micro-features of the aluminum foams were characterized and analyzed.Results demonstrate that an appropriate increase in SiC content and the uniform distribution of SiC can improve the foaming stability,optimize the cell diameter and cell wall thickness,ameliorate the cell distribution,and enhance the hardness and compressive strength of the aluminum foams.However,either insufficient or excessive SiC leads to uneven distribution of SiC particles,which is unfavorable to foaming stability and good cell structure formation.With 6wt%SiC,both the foaming stability and cell structure of the aluminum foam reach the optimal state,resulting in the highest compressive strength and optimal energy absorption capacity.展开更多
Aqueous zinc-ion batteries(AZIBs)have garnered considerable attention as promising post-lithium energy storage technologies owing to their intrinsic safety,cost-effectiveness,and competitive gravimetric energy density...Aqueous zinc-ion batteries(AZIBs)have garnered considerable attention as promising post-lithium energy storage technologies owing to their intrinsic safety,cost-effectiveness,and competitive gravimetric energy density.However,their practical commercialization is hindered by critical challenges on the anode side,including dendrite growth and parasitic reactions at the anode/electrolyte interface.Recent studies highlight that rational electrolyte structure engineering offers an effective route to mitigate these issues and strengthen the electrochemical performance of the zinc metal anode.In this review,we systematically summarize state-of-the-art strategies for electrolyte optimization,with a particular focus on the zinc salts regulation,electrolyte additives,and the construction of novel electrolytes,while elucidating the underlying design principles.We further discuss the key structure–property relationships governing electrolyte behavior to provide guidance for the development of next-generation electrolytes.Finally,future perspectives on advanced electrolyte design are proposed.This review aims to serve as a comprehensive reference for researchers exploring high-performance electrolyte engineering in AZIBs.展开更多
Two-step-processed(TSP)inverted p-i-n perovskite solar cells(PSCs)have demonstrated significant promise in tandem applications.However,the power conversion efficiency(PCE)of TSP p-i-n PSCs rarely exceeds 24%.Here,we d...Two-step-processed(TSP)inverted p-i-n perovskite solar cells(PSCs)have demonstrated significant promise in tandem applications.However,the power conversion efficiency(PCE)of TSP p-i-n PSCs rarely exceeds 24%.Here,we demonstrate that TSP perovskite films exhibit a vertically gradient distribution of residual PbI_(2)clusters,which form Schottky heterojunctions with the perovskite,leading to substantial interfacial energy-level mismatches within NiO_(x)-based TSP p-i-n PSCs.These limitations were effectively addressed via a vertical interfacial engineering enabled by dual-interface modification incorporating tin trifluoromethanesulfonate(Sn(OTF)_(2))and 4-Fluorophenylethylamine chloride(F-PEA)at the NiO_(x)/perovskite and perovskite/C60 interfaces,respectively.The functional Sn(OTF)_(2)not only enhances the conductivity of NiO_(x)films but also suppresses ion migration,while inducing the formation of a Pb-Sn mixed perovskite interlayer that precisely regulates the energy level at the NiO_(x)/perovskite interface.Complementally,F-PEA post-treatment effectively converts surface residual PbI_(2)clusters into a 2D perovskite capping layer,which simultaneously passivates surface defects and enhances energy-level alignment at the perovskite/C60 interface.Consequently,the optimized NiO_(x)-based TSP p-i-n PSCs achieve a notable PCE of 25.6%with superior operational stability.This study elucidates the underlying mechanisms limiting the efficiency of TSP p-i-n PSCs,while establishing design principles for these devices targeting 26%efficiency.展开更多
Niobium-based oxides show great potential in anode materials for fast-charging lithium-ion batteries,but their practical application remains hindered by intrinsically low conductivity.In this study,we successfully syn...Niobium-based oxides show great potential in anode materials for fast-charging lithium-ion batteries,but their practical application remains hindered by intrinsically low conductivity.In this study,we successfully synthesize nano-sized Wadsley-Roth FeNb_(11)O_(29)through Fe-driven phase transformation of Nb_(2)O_(5),which delivers a high specific capacity(280.5 mA h g^(−1)at 0.25 C)along with abundant redox-active sites.Moreover,the Wadsley-Roth shear structure of FeNb_(11)O_(29)facilitates rapid Li^(+)diffusion and guarantees exceptional structural stability.Theoretical calculations further confirm that FeNb_(11)O_(29)has a narrow band gap,which significantly enhances the conductivity.Owing to these merits,FeNb_(11)O_(29)achieves a full charge/discharge cycle within merely 25 s at 75 C rate and retains remarkable cycling stability over 2500 cycles.As a consequence,our assembled FeNb_(11)O_(29)||LiFePO_(4)full cell demonstrates ultra-long cyclability(>10000 cycles)and outstanding fast-charging capability(complete cycling within 2 min at 30 C).These findings highlight nano-sized FeNb_(11)O_(29)as a highly promising anode candidate for next-generation fast-charging LIBs.展开更多
Aqueous sodium-ion batteries(ASIBs)have attracted great attention in aqueous batteries due to their merit of high safety.However,the constrained work potential and insufficient chemical stability of anode materials in...Aqueous sodium-ion batteries(ASIBs)have attracted great attention in aqueous batteries due to their merit of high safety.However,the constrained work potential and insufficient chemical stability of anode materials in aqueous electro-lytes hinder the large-scale application of ASIBs.Sodium titanium phosphate,NaTi_(2)(PO_(4))_(3)(NTP),is considered one of the most promising anode materials for ASIBs due to its excellent electrochemical performance and tunable structure.Recently,great achievements have been made in the development of NTP,however,a comprehensive review of existing studies is still lacking.This article firstly introduces the basic properties of NTP and analyzes the existing challenges.Subsequently,it will provide a comprehensive overview of the key strategies related to the design and modification of NTP materials with optimized electrochemical performance.Finally,based on the current research status and practical needs,suggestions,and future perspectives for advancing NTP in practical applications of ASIBs are presented.This review aims to guide the future research trajectory from basic material innovation to industrial applications,thus promoting the large-scale commercializa-tion of ASIBs.展开更多
Lithium(Li)dendrites,resulting from poor ion desolvation and transport behavior at the anode/electrolyte interface during electrodeposition,severely impede the practicality of Li metal anodes.Inspired by the transmemb...Lithium(Li)dendrites,resulting from poor ion desolvation and transport behavior at the anode/electrolyte interface during electrodeposition,severely impede the practicality of Li metal anodes.Inspired by the transmembrane cascade transport mechanism of biological ion pumps,we design a biomimetic dual-cascade separator(BDS)based on gradient pore core–shell Gd_(2)O_(3)@ZIF-7 nanoparticles to stabilize Li metal anodes.The mesoporous Gd_(2)O_(3)core,via Lewis acidic surface,weakens Li^(+) -solvent interactions,thereby reconstructing the solvation structure and achieving pre-desolvation.The microporous ZIF-7 shell then promotes final desolvation through strong confinement effect and N-rich site coordination,while its nanochannels homogenize Li^(+) transport.This synergistic meso/microporous gradient creates a unique dual-cascade effect for ion desolvation and transport.Consequently,BDS achieves a low desolvation energy barrier,a high Li^(+) transference number(0.71),and dendrite-free Li deposition.The average Coulombic efficiency rises from 72.7%to 98.4%,the cycling performance of the Li||Li symmetrical cell improves by 3.2 times,and the capacity retention of LiFePO_4(LFP)||Li full cell increases from 38.3%to73.4%after 500 cycles.This work offers a novel separator design concept,deepens Li deposition understanding,and guides separators from passive protection to active regulation.展开更多
Parasitic interface side reactions and uncontrollable Zn deposition seriously erode the cycling performance of aqueous zinc ion batteries,thus impeding the large-scale application.Herein,an organic acid molecule with ...Parasitic interface side reactions and uncontrollable Zn deposition seriously erode the cycling performance of aqueous zinc ion batteries,thus impeding the large-scale application.Herein,an organic acid molecule with a unique molecular structure,camphorsulfonic acid(CSA),is first proposed to remodel the interface microenvironment as an electrolyte additive.The proton provided by CSA can neutralize the hydroxide ions generated by side reactions and inhibit the accumulation of alkaline by-products.The sulfonic acid groups are firmly adsorbed on the Zn anode surface,thereby enabling the regulation of interfacial species.Specifically,oxygen-containing functional groups combined with hydrophobic rigid carbon rings achieve a water-poor interface environment and promote the transfer of Zn^(2+),providing a suitable environment for Zn deposition.As a result,Zn//Zn symmetrical battery can run for over 2800 h(2 mA cm^(-2)-2 mAh cm^(-2)),demonstrating 28-times lifespan compared to the battery without CSA.Furthermore,Zn//KVO full cell presents excellent performance of 800 cycles at 3 A g^(-1).Besides,the pouch cell with CSA can also operate a capacity of 153.8 mAh after 60 cycles at 0.5 A g^(-1) with96.5%capacity retention rate.This work provides an organism-inspired additive selection for stabilizing the interface chemistry of the Zn anode.展开更多
Seawater electrolysis has been explored as a viable and sustainable method for green hydrogen production in regions characterized by freshwater scarcity but abundant renewable energy resources.However,the high concent...Seawater electrolysis has been explored as a viable and sustainable method for green hydrogen production in regions characterized by freshwater scarcity but abundant renewable energy resources.However,the high concentration of chlorine ions(Cl^(-))in seawater leads to severe corrosion of metallic electrodes,which significantly challenges the stability of electrode catalysts in seawater electrolysis.Owing to the Cl^(-)corrosion and the competitive oxygen/chlorine evolution reactions,the design of durable and active anode catalysts is key to achieving practical seawater electrolysis.To address this challenge,this review systematically analyzes the chlorine-induced corrosion mechanisms of anode catalysts,evaluates various anticorrosion strategies,and explores future prospects for enhancing anode durability.Three mainstream anticorrosion strategies are summarized and assessed for their effectiveness in mitigating the chlorineinduced damage to anode catalysts:the physical surface coatings,electrostatic repulsion,and Cl^(-)adsorption regulation.In addition,some emerging strategies are further introduced to highlight the future trends of state-of-the-art techniques for seawater electrolysis.This review aims to provide novel insights and practical guidance for developing more stable and efficient anode catalysts for hydrogen production via seawater electrolvsis.展开更多
Carbon coatings for silicon(Si)-based anode materials are essential for designing high-performance Li-ion batteries(LIBs).The coatings prevent direct contact with the electrolyte and enhance anode performance.However,...Carbon coatings for silicon(Si)-based anode materials are essential for designing high-performance Li-ion batteries(LIBs).The coatings prevent direct contact with the electrolyte and enhance anode performance.However,conventional carbon coatings are limited by their volume expansion and structural degradation,which lead to capacity fading and reduced durability.This study introduces a scalable and practical one-step carbon-coating strategy for directly coating silicon suboxide(SiO_(x))-based materials using aqueous quasi-defect-free reduced graphene oxide(QrGO)without post-treatment,unlike conventional graphene oxide(GO)-based coating methods.This simple process enables uniform encapsulation with QrGO for a highly adhesive and conductive coating.The QrGO-based composite anode material has several advantages,including reduced cracking due to volume expansion and enhanced charge carrier transport,as well as an increased Si content of 20 wt.%compared to the 5 wt.%in typical commercial Si-based active materials.In particular,the capacity retention of the QrGO-coated Si electrodes dramatically increases at high C-rate.The full cell exhibited long-term stability and capacity that were twice that of commercial SiO_(x)-based cells.Therefore,the QrGO-based one-step coating process represents a scalable,transformative,and commercially viable strategy for developing high-performance LIBs.展开更多
Aqueous zinc metal batteries(AZMBs)are promising candidates for next-generation energy storage,but their commercialization is hindered by zinc anode challenges,notably parasitic reactions and dendrite growth.Herein,we...Aqueous zinc metal batteries(AZMBs)are promising candidates for next-generation energy storage,but their commercialization is hindered by zinc anode challenges,notably parasitic reactions and dendrite growth.Herein,we present a biodegradable biomass-derived protective layer,primarily composed of curcumin,as a zincophilic interface for AZMBs.The curcumin-based layer,fabricated via a homogeneous solution process,exhibits strong adhesion,uniform coverage,and robust mechanical integrity.Rich polar functional groups in curcumin facilitate homogeneous Zn~(2+)flux and suppress side reactions.The curcumin-based layer shows a favorable affinity for zinc trifluoromethanesulfonate(Zn(OTf)_(2))electrolyte,which is the representative of organic zinc salts,enabling optimal thickness for both protection and ion transport.The protected Zn anodes demonstrate an extended lifespan of 2500 h in symmetrical cells and a high Coulombic efficiency of 99.15%.Furthermore,Zn(OTf)_(2)-based system typically exhibits poor stability at high current densities.Fortunately,the lifespan of symmetrical cells was extended by 40-fold at the high current density.When paired with an Na V_(3)O_(8)·1.5H_(2)O(NVO)cathode,the system achieves 86.5%capacity retention after 3000 cycles at a large specific current density of 10 A g^(-1).These results underscore the efficacy of the curcumin-based protective layer in enhancing the reversibility and stability of metal electrodes,specifically relieving the instability of Zn(OTf)_(2)-based systems at high current densities,advancing its commercial viability.展开更多
Sulfide solid electrolytes are considered promising candidates for all-solid-state lithium batteries(ASSLBs)because of their high ionic conductivity and favorable mechanical properties.However,the uncontrolled growth ...Sulfide solid electrolytes are considered promising candidates for all-solid-state lithium batteries(ASSLBs)because of their high ionic conductivity and favorable mechanical properties.However,the uncontrolled growth of lithium dendrites at the lithium metal-electrolytes interface remains a major obstacle to their practical application.In this work,we introduced a scalable three-dimensional(3D)Li-B skeleton structure designed to suppress dendrite formation.The alloy anode demonstrates a lower Young's modulus,which helps alleviate the accumulation of localized stresses at the interface.Additionally,the 3D alloy anode provided a uniform potential distribution,which promoted homogeneous lithium deposition.Benefiting from these structural advantages,symmetric cells with the Li-B alloy achieved a high critical current density of 2.8 mA cm^(-2).Notably,Li-B‖LPSCI‖LVO-NCM ASSLBs exhibited long-term cycling stability,retaining 97.8%of their capacity after 1500 cycles at 2 C.Furthermore,ASSLBs incorporating the Li-B alloy showed cycling stability comparable with Li-In-based cells,while delivering a higher energy density.Overall,this work presents a practical strategy that may accelerate the commercialization of sulfide-based ASSLBs.展开更多
Unlike conventional electrochromic devices,Zinc anode-based electrochromic devices(ZECDs)ensure excellent charge balance between the electrochromic layer and Zn anode during the coloring/bleaching by reversible metal ...Unlike conventional electrochromic devices,Zinc anode-based electrochromic devices(ZECDs)ensure excellent charge balance between the electrochromic layer and Zn anode during the coloring/bleaching by reversible metal deposition/stripping on the Zn anode.Meanwhile,the inherent potential difference between the metal anode and the electrochromic layer can drive the spontaneous coloration/bleaching of ZECDs,featuring energy retrieval functionality.This review discusses the working mechanisms,performance indexes of ZECDs,and the impact of material selection on ZECD performance.Furthermore,we comprehensively summarize the latest research progress of ZECDs in energy storage,smart windows,and multicolor displays.We argue that using high-transparency zinc mesh,additive manufacturing processes,and self-healing electrochromic materials can significantly advance the commercialization of large-area ZECDs.Finally,“electrode-free”device structures,renewable or replaceable electrolytes,and strategies to suppress zinc dendrites are prospected to overcome cost-effectiveness and lifespan issues of ZECDs.This review aims at enabling more efficient and advanced ZECDs for multifunctional applications.展开更多
Aqueous zinc(Zn)metal batteries are restricted due to Zn anodes facing notorious Zn dendrites and water-induced side reactions,which impede cycle performance.Herein,a zincophilic-hydrophobic interface layer is fabrica...Aqueous zinc(Zn)metal batteries are restricted due to Zn anodes facing notorious Zn dendrites and water-induced side reactions,which impede cycle performance.Herein,a zincophilic-hydrophobic interface layer is fabricated via an electrospinning method,where zincophilic silver(Ag)nanoparticles are evenly anchored in the hydrophobic polyvinylidene fluoride fiber matrix(Ag@PVDF),aiming to stabilize the Zn anode.The zincophilic nanoparticles can act as Zn nucleation sites and balance the interfacial electric field,ensuring a homogenous Zn deposition.Meanwhile,the hydrophobic fiber framework can prevent water-induced side reactions and modulate the Zn ion flux distribution.Consequently,the Ag@PVDF-Zn//Ag@PVDF-Zn symmetric cell delivers a superior lifespan over 2600 h(1.0 mA cm^(-2),1.0 mAh cm^(-2)).In addition,based on the stable Ag@PVDF-Zn anode,the Ag@PVDF-Zn//I_(2) full cell delivers84.3%capacity retention after 800 cycles at 2.0 C,and the aqueous Zn ion hybrid supercapacitor maintains a stable cycling performance over 15,000 cycles.This work highlights zincophilic-hydrophobic interface engineering to enable robust Zn anodes.展开更多
The development of electrochemical energy storage systems capable of operating under low-temperature conditions is crucial for enabling renewable energy applications in extreme environments.Although lithium-ion batter...The development of electrochemical energy storage systems capable of operating under low-temperature conditions is crucial for enabling renewable energy applications in extreme environments.Although lithium-ion batteries(LIBs)occupied the market of rechargeable batteries,their limited lithium salt and awful low-temperature performance severely hamper their widely application.In contrast,sodium-ion batteries(SIBs)have attracted extensive attention as a promising alternative,owing to the naturally abundant sodium salt and its favorable physicochemical properties(smaller Stokes radius and lower desolvation energy),which enable better ionic conductivity and rate capability at low temperatures.However,the practical deployment of SIBs in cold environments remains hindered by sluggish electrochemical kinetics,unstable electrode-electrolyte interfaces,and structural degradation,particularly at the anode.To address these problems,considerable efforts have been made to explore anode materials for low-temperature SIBs(LT-SIBs).This paper reviews recent advances in the design and synthesis of advanced anode materials for LT-SIBs.It discusses the influence mechanism of temperature on the performance of the anode and summarizes the latest modification strategies to improve the low-temperature electrochemical performance of intercalation-/conversion-/alloying-type and Na anodes.Finally,the review outlines the prospects and directions for future research on low-temperature anodes.It is hoped that this review will offer meaningful guidance for the development of anode materials for SIBs operation in all climates.展开更多
The development of aqueous zinc batteries(AZBs)is severely constrained by uncontrolled dendrite growth and parasitic interfacial reactions.Conventional solvation-dominated additives can mitigate these issues by alteri...The development of aqueous zinc batteries(AZBs)is severely constrained by uncontrolled dendrite growth and parasitic interfacial reactions.Conventional solvation-dominated additives can mitigate these issues by altering the Zn^(2+)solvation structure,but they often compromise ion transport.Here,we introduce a molecular design principle for a non-solvating additive(NSA)based on inductive effects.Ethyl trifluoroacetate(ETFA),obtained by introducing an electron-withdrawing–CF_(3) group adjacent to the–C=O moiety of ethyl acetate(EA),participates minimally in the solvation structure but preferentially undergoes Gibbs adsorption at the Zn-electrolyte interface.This process reduces interfacial tension,reconstructs the electrical double layer,and orients ETFA molecules such that the hydrophilic–C=O groups face the electrolyte,modulating hydrogen-bonding networks,while the hydrophobic–CF_(3) groups anchor onto Zn to regulate deposition.As a result,dendrite formation and side reactions are simultaneously suppressed.With only 1 vol%ETFA,Zn-Cu cells achieve over 4000 stable cycles with 99.89%Coulombic efficiency.Zn-I_(2) full cells employing the modified electrolyte maintain stable operation for more than 500 cycles(6.8 mg cm^(-2),10μm Zn,N/P=2.86),and 0.3 Ah Zn-I_(2) pouch cells(30 mg cm^(-2),100μm Zn)can cycle stably for over 200 cycles.These findings highlight the critical role of Gibbs adsorption in interfacial regulation and provide insights for the molecular design of high-performance additives for stable Zn anodes.展开更多
The deployment of flexible zinc-ion batteries is impeded by dendrite growth from random anode defects.Conventional defect-elimination strategies often compromise flexibility and fail to achieve uniform interfaces.We p...The deployment of flexible zinc-ion batteries is impeded by dendrite growth from random anode defects.Conventional defect-elimination strategies often compromise flexibility and fail to achieve uniform interfaces.We propose a paradigm shift:reconfiguring random defects into engineered,monodisperse artificial micro-curves to homogenize electric fields and guide aligned zinc(Zn)deposition.Using moisture-assisted flash heating,we transform zincophilic silver(Ag)coatings on carbon fibers into uniformly dispersed micro-curved particles(Ag Particles@CC),creating identical nucleation sites with optimal zinc ion(Zn^(2+))adsorption energetics.Theoretical simulations confirm these structures eliminate localized field concentrations,enabling homogeneous plating/stripping.This design demonstrates remarkable performance,with ultrastable 1500 cycles at 10 mA cm^(-2)(98.6%avg.Coulombic efficiency)and symmetric cell operation>650 h(57.7 mV hysteresis).Crucially,interparticle discontinuities preserve intrinsic flexibility,enabling flexible pouch cells(Ag Particles@CC-Zn//NaV_(3)O_(8)·1,5H_(2)O)to successfully power wearable devices such as smartwatches and smartphones.This work establishes defect reconfiguration via artificial micro-curvature engineering as a universal strategy toward dendritesuppressed,flexible energy storage.展开更多
The practical use of lithium metal anodes(LMAs)is impeded by uncontrolled dendrite growth,primarily caused by uneven Li-ion flux and significant volume changes during cycling.To overcome these challenges,we present bi...The practical use of lithium metal anodes(LMAs)is impeded by uncontrolled dendrite growth,primarily caused by uneven Li-ion flux and significant volume changes during cycling.To overcome these challenges,we present binder-free holey wrinkled-multilayered graphene(HWMG)scaffolds for highperformance LMAs with long cycle life.Holey graphene oxide(HGO)sheets were restacked into particle-like holey wrinkled-multilayered graphene oxide(HWMGO)in a high-concentration GO suspension,in which few-layer HGOs were quickly stabilized and wrinkled during the drying process,and upon reduction,they transformed into HWMG.HWMG exhibited excellent adhesion due to chemical interactions via edge-located functional groups.Its particle-like morphology,with numerous nanopores and high porosity,conferred outstanding mechanical flexibility and low tortuosity,enabling uniform Li-ion flux,buffering volume expansion,and suppressing dendrite growth.As a result,excellent long-term stability over 800 cycles and a voltage hysteresis of ca.7 mV over 6000 h were realized for the HWMG scaffolds,and a high areal capacity of 3.34 mAh cm^(-2) at 0.3 C after 350 cycles was demonstrated in a full-cell configuration.This work promotes the practical application of LMAs by offering a scalable scaffold design that suppresses dendrites and enhances cycle life.展开更多
The electric double layer(EDL)at the electrochemical interface is crucial for ion transport,charge transfer,and surface reactions in aqueous rechargeable zinc batteries(ARZBs).However,Zn anodes routinely encounter per...The electric double layer(EDL)at the electrochemical interface is crucial for ion transport,charge transfer,and surface reactions in aqueous rechargeable zinc batteries(ARZBs).However,Zn anodes routinely encounter persistent dendrite growth and parasitic reactions,driven by the inhomogeneous charge distribution and water-dominated environment within the EDL.Compounding this,classical EDL theory,rooted in meanfield approximations,further fails to resolve molecular-scale interfacial dynamics under battery-operating conditions,limiting mechanistic insights.Herein,we established a multiscale theoretical calculation framework from single molecular characteristics to interfacial ion distribution,revealing the EDL’s structure and interactions between different ions and molecules,which helps us understand the parasitic processes in depth.Simulations demonstrate that water dipole and sulfate ion adsorption at the inner Helmholtz plane drives severe hydrogen evolution and by-product formation.Guided by these insights,we engineered a“water-poor and anion-expelled”EDL using 4,1’,6’-trichlorogalactosucrose(TGS)as an electrolyte additive.As a result,Zn||Zn symmetric cells with TGS exhibited stable cycling for over 4700 h under a current density of 1 mA cm^(−2),while NaV_(3)O_(8)·1.5H_(2)O-based full cells kept 90.4%of the initial specific capacity after 800 cycles at 5 A g^(−1).This work highlights the power of multiscale theoretical frameworks to unravel EDL complexities and guide high-performance ARZB design through integrated theory-experiment approaches.展开更多
基金Project(BG2005009)supported by Jiangsu Provincial Hi-Tech Research Program
文摘Alumina nanostructures were obtained by two-step anodization process.The porous anodic aluminum oxide(AAO)membranes were anodized in oxalic acid,which was subsequently treated with chemical etching process with 1.0 mol/L sodiumhydroxide solution,or mixed solution of phosphoric acid(6.0%)and chromic acid(1.8%),respectively.Field emission scanningelectron microscopy(FE-SEM)and transmission electron microscopy(TEM)were employed to character the morphology andstructure of the obtained alumina nanostructure.It is found that alumina nanowires are generated in the acidic chemical etchingsolution,while nanotube structures are formed in the alkaline solution.The influence of acid and alkaline solution on aluminamorphologies in the chemical etching process was discussed.
基金Funded by National Basic Research Program of China(No.2009CB939704)
文摘A double-layer TiO2 nanotube arrays were formed by two-step anodization of Ti foils in different electrolytes. First, Ti in 0.5 wt% HF was anodized to form thin nanotube layer. Afterwards a second anodization was conducted in a formamide based electrolyte, which allowed the second layer of nanotube growing directly underneath the first one. From FESEM investigation we found that the thickness of second layer corresponded to the anodization time, the increasing of which would lead to the excessive etching on the first layer. The first layer protected the lower one from fluoride corrosion during anodization process. The double layer TiO2 nanotube arrays showed no benefit to photodegradation effect in methyl orange degradation experiments.
基金Doctoral Startup Fund(20192066,20212028)Laijin Excellent Doctoral Fund(20202021)+1 种基金Scientific and Technological Innovation of Colleges and Universities in Shanxi Province(2020L0342)Fundamental Research Program of Shanxi Province(202303021222178)。
文摘SiC/Al-based composite foams were prepared by a two-step foaming method.The influence of the SiC content and its distribution uniformity on the foaming stability,cell structure,and mechanical properties of the aluminum foams was investigated.The macro/micro-features of the aluminum foams were characterized and analyzed.Results demonstrate that an appropriate increase in SiC content and the uniform distribution of SiC can improve the foaming stability,optimize the cell diameter and cell wall thickness,ameliorate the cell distribution,and enhance the hardness and compressive strength of the aluminum foams.However,either insufficient or excessive SiC leads to uneven distribution of SiC particles,which is unfavorable to foaming stability and good cell structure formation.With 6wt%SiC,both the foaming stability and cell structure of the aluminum foam reach the optimal state,resulting in the highest compressive strength and optimal energy absorption capacity.
基金supported by the Natural Science Foundation of China(Nos.52125202,52202100,and U24A2065)the Natural Science Foundation of Jiangsu Province(BK20243016)Fundamental Research Funds for the Central Universities,China Postdoctoral Science Foundation(No.2024T171166).
文摘Aqueous zinc-ion batteries(AZIBs)have garnered considerable attention as promising post-lithium energy storage technologies owing to their intrinsic safety,cost-effectiveness,and competitive gravimetric energy density.However,their practical commercialization is hindered by critical challenges on the anode side,including dendrite growth and parasitic reactions at the anode/electrolyte interface.Recent studies highlight that rational electrolyte structure engineering offers an effective route to mitigate these issues and strengthen the electrochemical performance of the zinc metal anode.In this review,we systematically summarize state-of-the-art strategies for electrolyte optimization,with a particular focus on the zinc salts regulation,electrolyte additives,and the construction of novel electrolytes,while elucidating the underlying design principles.We further discuss the key structure–property relationships governing electrolyte behavior to provide guidance for the development of next-generation electrolytes.Finally,future perspectives on advanced electrolyte design are proposed.This review aims to serve as a comprehensive reference for researchers exploring high-performance electrolyte engineering in AZIBs.
基金financially supported by the National Nature Science Foundation of China (62504130)National Key Research and Development Program of China (2018YFB0704100)+3 种基金the Key university laboratory of highly efficient utilization of solar energy and sustainable development of Guangdong (Y01256331)the Technology Development Project of Henan Province (252102240047)the Pico Center at SUSTech CRF which receives support from the Presidential FundDevelopment and Reform Commission of Shenzhen Municipality
文摘Two-step-processed(TSP)inverted p-i-n perovskite solar cells(PSCs)have demonstrated significant promise in tandem applications.However,the power conversion efficiency(PCE)of TSP p-i-n PSCs rarely exceeds 24%.Here,we demonstrate that TSP perovskite films exhibit a vertically gradient distribution of residual PbI_(2)clusters,which form Schottky heterojunctions with the perovskite,leading to substantial interfacial energy-level mismatches within NiO_(x)-based TSP p-i-n PSCs.These limitations were effectively addressed via a vertical interfacial engineering enabled by dual-interface modification incorporating tin trifluoromethanesulfonate(Sn(OTF)_(2))and 4-Fluorophenylethylamine chloride(F-PEA)at the NiO_(x)/perovskite and perovskite/C60 interfaces,respectively.The functional Sn(OTF)_(2)not only enhances the conductivity of NiO_(x)films but also suppresses ion migration,while inducing the formation of a Pb-Sn mixed perovskite interlayer that precisely regulates the energy level at the NiO_(x)/perovskite interface.Complementally,F-PEA post-treatment effectively converts surface residual PbI_(2)clusters into a 2D perovskite capping layer,which simultaneously passivates surface defects and enhances energy-level alignment at the perovskite/C60 interface.Consequently,the optimized NiO_(x)-based TSP p-i-n PSCs achieve a notable PCE of 25.6%with superior operational stability.This study elucidates the underlying mechanisms limiting the efficiency of TSP p-i-n PSCs,while establishing design principles for these devices targeting 26%efficiency.
基金financially supported by the National Natural Science Foundation of China (52272209)
文摘Niobium-based oxides show great potential in anode materials for fast-charging lithium-ion batteries,but their practical application remains hindered by intrinsically low conductivity.In this study,we successfully synthesize nano-sized Wadsley-Roth FeNb_(11)O_(29)through Fe-driven phase transformation of Nb_(2)O_(5),which delivers a high specific capacity(280.5 mA h g^(−1)at 0.25 C)along with abundant redox-active sites.Moreover,the Wadsley-Roth shear structure of FeNb_(11)O_(29)facilitates rapid Li^(+)diffusion and guarantees exceptional structural stability.Theoretical calculations further confirm that FeNb_(11)O_(29)has a narrow band gap,which significantly enhances the conductivity.Owing to these merits,FeNb_(11)O_(29)achieves a full charge/discharge cycle within merely 25 s at 75 C rate and retains remarkable cycling stability over 2500 cycles.As a consequence,our assembled FeNb_(11)O_(29)||LiFePO_(4)full cell demonstrates ultra-long cyclability(>10000 cycles)and outstanding fast-charging capability(complete cycling within 2 min at 30 C).These findings highlight nano-sized FeNb_(11)O_(29)as a highly promising anode candidate for next-generation fast-charging LIBs.
基金supported by the Natural Sci-ence Foundation of Fujian Province (No.2024J011210)the High-Level Talent Start-Up Foundation of Xiamen Institute of Technology (No.YKJ23017R)。
文摘Aqueous sodium-ion batteries(ASIBs)have attracted great attention in aqueous batteries due to their merit of high safety.However,the constrained work potential and insufficient chemical stability of anode materials in aqueous electro-lytes hinder the large-scale application of ASIBs.Sodium titanium phosphate,NaTi_(2)(PO_(4))_(3)(NTP),is considered one of the most promising anode materials for ASIBs due to its excellent electrochemical performance and tunable structure.Recently,great achievements have been made in the development of NTP,however,a comprehensive review of existing studies is still lacking.This article firstly introduces the basic properties of NTP and analyzes the existing challenges.Subsequently,it will provide a comprehensive overview of the key strategies related to the design and modification of NTP materials with optimized electrochemical performance.Finally,based on the current research status and practical needs,suggestions,and future perspectives for advancing NTP in practical applications of ASIBs are presented.This review aims to guide the future research trajectory from basic material innovation to industrial applications,thus promoting the large-scale commercializa-tion of ASIBs.
基金the financial support from the National Natural Science Foundation of China(22408182)the Young Talents of Science and Technology in Universities of Inner Mongolia Autonomous Region(NJYT24024)the Natural Science Foundation of Inner Mongolia Autonomous Region(2023QN02007 and 2025QN02009)。
文摘Lithium(Li)dendrites,resulting from poor ion desolvation and transport behavior at the anode/electrolyte interface during electrodeposition,severely impede the practicality of Li metal anodes.Inspired by the transmembrane cascade transport mechanism of biological ion pumps,we design a biomimetic dual-cascade separator(BDS)based on gradient pore core–shell Gd_(2)O_(3)@ZIF-7 nanoparticles to stabilize Li metal anodes.The mesoporous Gd_(2)O_(3)core,via Lewis acidic surface,weakens Li^(+) -solvent interactions,thereby reconstructing the solvation structure and achieving pre-desolvation.The microporous ZIF-7 shell then promotes final desolvation through strong confinement effect and N-rich site coordination,while its nanochannels homogenize Li^(+) transport.This synergistic meso/microporous gradient creates a unique dual-cascade effect for ion desolvation and transport.Consequently,BDS achieves a low desolvation energy barrier,a high Li^(+) transference number(0.71),and dendrite-free Li deposition.The average Coulombic efficiency rises from 72.7%to 98.4%,the cycling performance of the Li||Li symmetrical cell improves by 3.2 times,and the capacity retention of LiFePO_4(LFP)||Li full cell increases from 38.3%to73.4%after 500 cycles.This work offers a novel separator design concept,deepens Li deposition understanding,and guides separators from passive protection to active regulation.
基金financially supported by The Excellent Youth Project of the Education Department of Hunan Province(No.24B0008)the National Natural Science Foundation of China(No.52377222)。
文摘Parasitic interface side reactions and uncontrollable Zn deposition seriously erode the cycling performance of aqueous zinc ion batteries,thus impeding the large-scale application.Herein,an organic acid molecule with a unique molecular structure,camphorsulfonic acid(CSA),is first proposed to remodel the interface microenvironment as an electrolyte additive.The proton provided by CSA can neutralize the hydroxide ions generated by side reactions and inhibit the accumulation of alkaline by-products.The sulfonic acid groups are firmly adsorbed on the Zn anode surface,thereby enabling the regulation of interfacial species.Specifically,oxygen-containing functional groups combined with hydrophobic rigid carbon rings achieve a water-poor interface environment and promote the transfer of Zn^(2+),providing a suitable environment for Zn deposition.As a result,Zn//Zn symmetrical battery can run for over 2800 h(2 mA cm^(-2)-2 mAh cm^(-2)),demonstrating 28-times lifespan compared to the battery without CSA.Furthermore,Zn//KVO full cell presents excellent performance of 800 cycles at 3 A g^(-1).Besides,the pouch cell with CSA can also operate a capacity of 153.8 mAh after 60 cycles at 0.5 A g^(-1) with96.5%capacity retention rate.This work provides an organism-inspired additive selection for stabilizing the interface chemistry of the Zn anode.
基金sponsored by the National Natural Science Foundation of China(52302039,52301043)the Guangdong Basic and Applied Basic Research Foundation(2024A1515240056)+3 种基金the Shenzhen Science and Technology Program(GXWD20231129113217001)the Shenzhen Key Laboratory of New Materials Technology(SYSPG20241211173609003)the Postdoctoral Research Startup Expenses of Shenzhen(NA25501001)Shenzhen Introduce High-level Talents and Scientific Research Start-up Funds(NA11409005)。
文摘Seawater electrolysis has been explored as a viable and sustainable method for green hydrogen production in regions characterized by freshwater scarcity but abundant renewable energy resources.However,the high concentration of chlorine ions(Cl^(-))in seawater leads to severe corrosion of metallic electrodes,which significantly challenges the stability of electrode catalysts in seawater electrolysis.Owing to the Cl^(-)corrosion and the competitive oxygen/chlorine evolution reactions,the design of durable and active anode catalysts is key to achieving practical seawater electrolysis.To address this challenge,this review systematically analyzes the chlorine-induced corrosion mechanisms of anode catalysts,evaluates various anticorrosion strategies,and explores future prospects for enhancing anode durability.Three mainstream anticorrosion strategies are summarized and assessed for their effectiveness in mitigating the chlorineinduced damage to anode catalysts:the physical surface coatings,electrostatic repulsion,and Cl^(-)adsorption regulation.In addition,some emerging strategies are further introduced to highlight the future trends of state-of-the-art techniques for seawater electrolysis.This review aims to provide novel insights and practical guidance for developing more stable and efficient anode catalysts for hydrogen production via seawater electrolvsis.
基金supported by Korea Electrotechnology Research Institute(KERI)Primary research program through the National Research Council of Science&Technology(NST)funded by the Ministry of Science and ICT(MSIT)(No.25A01015)by the Technology Innovation Program(20019091)funded by the Ministry of Trade,Industry&Energy(MOTIE,Korea)by the National Research Council of Science&Technology(NST)grant from the Korea government(MSIT)(No.GTL24012-000).
文摘Carbon coatings for silicon(Si)-based anode materials are essential for designing high-performance Li-ion batteries(LIBs).The coatings prevent direct contact with the electrolyte and enhance anode performance.However,conventional carbon coatings are limited by their volume expansion and structural degradation,which lead to capacity fading and reduced durability.This study introduces a scalable and practical one-step carbon-coating strategy for directly coating silicon suboxide(SiO_(x))-based materials using aqueous quasi-defect-free reduced graphene oxide(QrGO)without post-treatment,unlike conventional graphene oxide(GO)-based coating methods.This simple process enables uniform encapsulation with QrGO for a highly adhesive and conductive coating.The QrGO-based composite anode material has several advantages,including reduced cracking due to volume expansion and enhanced charge carrier transport,as well as an increased Si content of 20 wt.%compared to the 5 wt.%in typical commercial Si-based active materials.In particular,the capacity retention of the QrGO-coated Si electrodes dramatically increases at high C-rate.The full cell exhibited long-term stability and capacity that were twice that of commercial SiO_(x)-based cells.Therefore,the QrGO-based one-step coating process represents a scalable,transformative,and commercially viable strategy for developing high-performance LIBs.
基金the financial support from Research Institute for Smart Energy at the Hong Kong Polytechnic University(Grant No.CDB2)the support of the Hong Kong PhD Fellowship Scheme(Grant No.PF21-65328)。
文摘Aqueous zinc metal batteries(AZMBs)are promising candidates for next-generation energy storage,but their commercialization is hindered by zinc anode challenges,notably parasitic reactions and dendrite growth.Herein,we present a biodegradable biomass-derived protective layer,primarily composed of curcumin,as a zincophilic interface for AZMBs.The curcumin-based layer,fabricated via a homogeneous solution process,exhibits strong adhesion,uniform coverage,and robust mechanical integrity.Rich polar functional groups in curcumin facilitate homogeneous Zn~(2+)flux and suppress side reactions.The curcumin-based layer shows a favorable affinity for zinc trifluoromethanesulfonate(Zn(OTf)_(2))electrolyte,which is the representative of organic zinc salts,enabling optimal thickness for both protection and ion transport.The protected Zn anodes demonstrate an extended lifespan of 2500 h in symmetrical cells and a high Coulombic efficiency of 99.15%.Furthermore,Zn(OTf)_(2)-based system typically exhibits poor stability at high current densities.Fortunately,the lifespan of symmetrical cells was extended by 40-fold at the high current density.When paired with an Na V_(3)O_(8)·1.5H_(2)O(NVO)cathode,the system achieves 86.5%capacity retention after 3000 cycles at a large specific current density of 10 A g^(-1).These results underscore the efficacy of the curcumin-based protective layer in enhancing the reversibility and stability of metal electrodes,specifically relieving the instability of Zn(OTf)_(2)-based systems at high current densities,advancing its commercial viability.
基金supported by the National Natural Science Foundation of China(Grant Nos.52002094)the Guangdong Basic and Applied Basic Research Foundation(Grant Nos.2025A1515011995)+3 种基金the Shenzhen Science and Technology Innovation Program(GXWD20221030205923001)the Shandong Provincial Natural Science Foundation of China(Grant Nos.ZR2024QE525)the Shenzhen Key Laboratory of New Materials Technology(Grant Nos.SYSPG20241211173609003)the State Key Laboratory of Precision Welding&Joining of Materials and Structures(Grant Nos.2024-Z-17,2024-T-08)。
文摘Sulfide solid electrolytes are considered promising candidates for all-solid-state lithium batteries(ASSLBs)because of their high ionic conductivity and favorable mechanical properties.However,the uncontrolled growth of lithium dendrites at the lithium metal-electrolytes interface remains a major obstacle to their practical application.In this work,we introduced a scalable three-dimensional(3D)Li-B skeleton structure designed to suppress dendrite formation.The alloy anode demonstrates a lower Young's modulus,which helps alleviate the accumulation of localized stresses at the interface.Additionally,the 3D alloy anode provided a uniform potential distribution,which promoted homogeneous lithium deposition.Benefiting from these structural advantages,symmetric cells with the Li-B alloy achieved a high critical current density of 2.8 mA cm^(-2).Notably,Li-B‖LPSCI‖LVO-NCM ASSLBs exhibited long-term cycling stability,retaining 97.8%of their capacity after 1500 cycles at 2 C.Furthermore,ASSLBs incorporating the Li-B alloy showed cycling stability comparable with Li-In-based cells,while delivering a higher energy density.Overall,this work presents a practical strategy that may accelerate the commercialization of sulfide-based ASSLBs.
基金supports from the National Natural Science Foundation of China(62105185,52202320)the“Qilu Young Scholar”program(62460082163097)of Shandong University,open foundation of the State Key Laboratory of Vanadium and Titanium Resources Comprehensive Utilization(2023P4FZG08A)+1 种基金Fundamental Research Funds for the Central Universities(No.862201013153)Shandong Excellent Young Scientists Fund Program(Overseas)(2023HWYQ-060).
文摘Unlike conventional electrochromic devices,Zinc anode-based electrochromic devices(ZECDs)ensure excellent charge balance between the electrochromic layer and Zn anode during the coloring/bleaching by reversible metal deposition/stripping on the Zn anode.Meanwhile,the inherent potential difference between the metal anode and the electrochromic layer can drive the spontaneous coloration/bleaching of ZECDs,featuring energy retrieval functionality.This review discusses the working mechanisms,performance indexes of ZECDs,and the impact of material selection on ZECD performance.Furthermore,we comprehensively summarize the latest research progress of ZECDs in energy storage,smart windows,and multicolor displays.We argue that using high-transparency zinc mesh,additive manufacturing processes,and self-healing electrochromic materials can significantly advance the commercialization of large-area ZECDs.Finally,“electrode-free”device structures,renewable or replaceable electrolytes,and strategies to suppress zinc dendrites are prospected to overcome cost-effectiveness and lifespan issues of ZECDs.This review aims at enabling more efficient and advanced ZECDs for multifunctional applications.
基金(partially)funded by the BK21 FOUR Program of Graduate School,Kyung Hee University(GS-1-JO-ON-info2120241890)。
文摘Aqueous zinc(Zn)metal batteries are restricted due to Zn anodes facing notorious Zn dendrites and water-induced side reactions,which impede cycle performance.Herein,a zincophilic-hydrophobic interface layer is fabricated via an electrospinning method,where zincophilic silver(Ag)nanoparticles are evenly anchored in the hydrophobic polyvinylidene fluoride fiber matrix(Ag@PVDF),aiming to stabilize the Zn anode.The zincophilic nanoparticles can act as Zn nucleation sites and balance the interfacial electric field,ensuring a homogenous Zn deposition.Meanwhile,the hydrophobic fiber framework can prevent water-induced side reactions and modulate the Zn ion flux distribution.Consequently,the Ag@PVDF-Zn//Ag@PVDF-Zn symmetric cell delivers a superior lifespan over 2600 h(1.0 mA cm^(-2),1.0 mAh cm^(-2)).In addition,based on the stable Ag@PVDF-Zn anode,the Ag@PVDF-Zn//I_(2) full cell delivers84.3%capacity retention after 800 cycles at 2.0 C,and the aqueous Zn ion hybrid supercapacitor maintains a stable cycling performance over 15,000 cycles.This work highlights zincophilic-hydrophobic interface engineering to enable robust Zn anodes.
基金supported by the National Natural Science Foundation of China(No.52301266)the Guangdong Basic and Applied Basic Research Foundation(No.2025A1515012152)+1 种基金the Science and Technology Planning Project of Guangzhou(No.2024A04J3332)the Chenzhou National Sustainable Development Agenda Innovation Demonstration Zone Provincial Special Project(No.2023sfq11)。
文摘The development of electrochemical energy storage systems capable of operating under low-temperature conditions is crucial for enabling renewable energy applications in extreme environments.Although lithium-ion batteries(LIBs)occupied the market of rechargeable batteries,their limited lithium salt and awful low-temperature performance severely hamper their widely application.In contrast,sodium-ion batteries(SIBs)have attracted extensive attention as a promising alternative,owing to the naturally abundant sodium salt and its favorable physicochemical properties(smaller Stokes radius and lower desolvation energy),which enable better ionic conductivity and rate capability at low temperatures.However,the practical deployment of SIBs in cold environments remains hindered by sluggish electrochemical kinetics,unstable electrode-electrolyte interfaces,and structural degradation,particularly at the anode.To address these problems,considerable efforts have been made to explore anode materials for low-temperature SIBs(LT-SIBs).This paper reviews recent advances in the design and synthesis of advanced anode materials for LT-SIBs.It discusses the influence mechanism of temperature on the performance of the anode and summarizes the latest modification strategies to improve the low-temperature electrochemical performance of intercalation-/conversion-/alloying-type and Na anodes.Finally,the review outlines the prospects and directions for future research on low-temperature anodes.It is hoped that this review will offer meaningful guidance for the development of anode materials for SIBs operation in all climates.
基金financially supported by the Science and Technology Foundation of Henan Province(252102230017)the Doctoral Foundation of Henan University of Technology(2019BS005)+2 种基金the Talent Research Start-up Fund Project of Tongling University(2021tlxyrc23)the Natural Science Research Project of the Anhui Educational Committee(2023AH040234)the Scientific Research Projects of Tongling University(2022tlxyszZD04)。
文摘The development of aqueous zinc batteries(AZBs)is severely constrained by uncontrolled dendrite growth and parasitic interfacial reactions.Conventional solvation-dominated additives can mitigate these issues by altering the Zn^(2+)solvation structure,but they often compromise ion transport.Here,we introduce a molecular design principle for a non-solvating additive(NSA)based on inductive effects.Ethyl trifluoroacetate(ETFA),obtained by introducing an electron-withdrawing–CF_(3) group adjacent to the–C=O moiety of ethyl acetate(EA),participates minimally in the solvation structure but preferentially undergoes Gibbs adsorption at the Zn-electrolyte interface.This process reduces interfacial tension,reconstructs the electrical double layer,and orients ETFA molecules such that the hydrophilic–C=O groups face the electrolyte,modulating hydrogen-bonding networks,while the hydrophobic–CF_(3) groups anchor onto Zn to regulate deposition.As a result,dendrite formation and side reactions are simultaneously suppressed.With only 1 vol%ETFA,Zn-Cu cells achieve over 4000 stable cycles with 99.89%Coulombic efficiency.Zn-I_(2) full cells employing the modified electrolyte maintain stable operation for more than 500 cycles(6.8 mg cm^(-2),10μm Zn,N/P=2.86),and 0.3 Ah Zn-I_(2) pouch cells(30 mg cm^(-2),100μm Zn)can cycle stably for over 200 cycles.These findings highlight the critical role of Gibbs adsorption in interfacial regulation and provide insights for the molecular design of high-performance additives for stable Zn anodes.
基金supported by the National Natural Science Foundation of China(52202218)the Fundamental Research Funds for the Central Universities(CUSF-DH-T-2023044)。
文摘The deployment of flexible zinc-ion batteries is impeded by dendrite growth from random anode defects.Conventional defect-elimination strategies often compromise flexibility and fail to achieve uniform interfaces.We propose a paradigm shift:reconfiguring random defects into engineered,monodisperse artificial micro-curves to homogenize electric fields and guide aligned zinc(Zn)deposition.Using moisture-assisted flash heating,we transform zincophilic silver(Ag)coatings on carbon fibers into uniformly dispersed micro-curved particles(Ag Particles@CC),creating identical nucleation sites with optimal zinc ion(Zn^(2+))adsorption energetics.Theoretical simulations confirm these structures eliminate localized field concentrations,enabling homogeneous plating/stripping.This design demonstrates remarkable performance,with ultrastable 1500 cycles at 10 mA cm^(-2)(98.6%avg.Coulombic efficiency)and symmetric cell operation>650 h(57.7 mV hysteresis).Crucially,interparticle discontinuities preserve intrinsic flexibility,enabling flexible pouch cells(Ag Particles@CC-Zn//NaV_(3)O_(8)·1,5H_(2)O)to successfully power wearable devices such as smartwatches and smartphones.This work establishes defect reconfiguration via artificial micro-curvature engineering as a universal strategy toward dendritesuppressed,flexible energy storage.
基金supported by the National Research Foundation of Korea(NRF)grants funded by the Korean government(MSIT)(RS-2024-00409952,RS-2024-00347936,and RS-202400407282)supported by the GRRC Program of Gyeonggi Province(GRRCHanyang2020-B01)supported by the Commercialization Promotion Agency for R&D Outcomes(COMPA)grant funded by the Korean Government(MSIT)(RS-2023-00304763)。
文摘The practical use of lithium metal anodes(LMAs)is impeded by uncontrolled dendrite growth,primarily caused by uneven Li-ion flux and significant volume changes during cycling.To overcome these challenges,we present binder-free holey wrinkled-multilayered graphene(HWMG)scaffolds for highperformance LMAs with long cycle life.Holey graphene oxide(HGO)sheets were restacked into particle-like holey wrinkled-multilayered graphene oxide(HWMGO)in a high-concentration GO suspension,in which few-layer HGOs were quickly stabilized and wrinkled during the drying process,and upon reduction,they transformed into HWMG.HWMG exhibited excellent adhesion due to chemical interactions via edge-located functional groups.Its particle-like morphology,with numerous nanopores and high porosity,conferred outstanding mechanical flexibility and low tortuosity,enabling uniform Li-ion flux,buffering volume expansion,and suppressing dendrite growth.As a result,excellent long-term stability over 800 cycles and a voltage hysteresis of ca.7 mV over 6000 h were realized for the HWMG scaffolds,and a high areal capacity of 3.34 mAh cm^(-2) at 0.3 C after 350 cycles was demonstrated in a full-cell configuration.This work promotes the practical application of LMAs by offering a scalable scaffold design that suppresses dendrites and enhances cycle life.
基金supported by the National Natural Science Foundation of China(52471240)the Natural Science Foundation of Zhejiang Province(LZ23B030003)+2 种基金the Fundamental Research Funds for the Central Universities(226-2024-00075)support from the Engineering and Physical Sciences Research Council(EPSRC,UK)RiR grant-RIR18221018-1EU COST CA23155。
文摘The electric double layer(EDL)at the electrochemical interface is crucial for ion transport,charge transfer,and surface reactions in aqueous rechargeable zinc batteries(ARZBs).However,Zn anodes routinely encounter persistent dendrite growth and parasitic reactions,driven by the inhomogeneous charge distribution and water-dominated environment within the EDL.Compounding this,classical EDL theory,rooted in meanfield approximations,further fails to resolve molecular-scale interfacial dynamics under battery-operating conditions,limiting mechanistic insights.Herein,we established a multiscale theoretical calculation framework from single molecular characteristics to interfacial ion distribution,revealing the EDL’s structure and interactions between different ions and molecules,which helps us understand the parasitic processes in depth.Simulations demonstrate that water dipole and sulfate ion adsorption at the inner Helmholtz plane drives severe hydrogen evolution and by-product formation.Guided by these insights,we engineered a“water-poor and anion-expelled”EDL using 4,1’,6’-trichlorogalactosucrose(TGS)as an electrolyte additive.As a result,Zn||Zn symmetric cells with TGS exhibited stable cycling for over 4700 h under a current density of 1 mA cm^(−2),while NaV_(3)O_(8)·1.5H_(2)O-based full cells kept 90.4%of the initial specific capacity after 800 cycles at 5 A g^(−1).This work highlights the power of multiscale theoretical frameworks to unravel EDL complexities and guide high-performance ARZB design through integrated theory-experiment approaches.
