Control design is important for proton exchange membrane fuel cell (PEMFC) generator. This work researched the anode system of a 60-kW PEMFC generator. Both anode pressure and humidity must be maintained at ideal leve...Control design is important for proton exchange membrane fuel cell (PEMFC) generator. This work researched the anode system of a 60-kW PEMFC generator. Both anode pressure and humidity must be maintained at ideal levels during steady operation. In view of characteristics and requirements of the system, a hybrid intelligent PID controller is designed specifically based on dynamic simulation. A single neuron PI controller is used for anode humidity by adjusting the water injection to the hydrogen cell. Another incremental PID controller, based on the diagonal recurrent neural network (DRNN) dynamic identification, is used to control anode pressure to be more stable and exact by adjusting the hydrogen flow rate. This control strategy can avoid the coupling problem of the PEMFC and achieve a more adaptive ability. Simulation results showed that the control strategy can maintain both anode humidity and pressure at ideal levels regardless of variable load, nonlinear dynamic and coupling characteristics of the system. This work will give some guides for further control design and applications of the total PEMFC generator.展开更多
Atmospheric pressure plasma-liquid interactions exist in a variety of applications,including wastewater treatment,wound sterilization,and disinfection.In practice,the phenomenon of liquid surface depression will inevi...Atmospheric pressure plasma-liquid interactions exist in a variety of applications,including wastewater treatment,wound sterilization,and disinfection.In practice,the phenomenon of liquid surface depression will inevitably appear.The applied gas will cause a depression on the liquid surface,which will undoubtedly affect the plasma generation and further affect the application performance.However,the effect of liquid surface deformation on the plasma is still unclear.In this work,numerical models are developed to reveal the mechanism of liquid surface depressions affecting plasma discharge characteristics and the consequential distribution of plasma species,and further study the influence of liquid surface depressions of different sizes generated by different helium flow rates on the plasma.Results show that the liquid surface deformation changes the initial spatial electric field,resulting in the rearrangement of electrons on the liquid surface.The charges deposited on the liquid surface further increase the degree of distortion of the electric field.Moreover,the electric field and electron distribution affected by the liquid surface depression significantly influence the generation and distribution of active species,which determines the practical effectiveness of the relevant applications.This work explores the phenomenon of liquid surface depression,which has been neglected in previous related work,and contributes to further understanding of plasma-liquid interactions,providing better theoretical guidance for related applications and technologies.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
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 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
Renewable energy is critical to building a sustainable society,but its true potential can only be unlocked by developing efficient,environmentally friendly energy storage systems.Advances in storage technologies,inclu...Renewable energy is critical to building a sustainable society,but its true potential can only be unlocked by developing efficient,environmentally friendly energy storage systems.Advances in storage technologies,including cost-effective and green materials,are quickly becoming the cornerstone of sustainable energy solutions.The most effective battery technology available now is lithium-ion batteries(LIBs).However,the sustainability of battery material production and the degradation of LIB functionality at subzero temperatures pose significant challenges,highlighting the urgent need for alternative and sustainable low-temperature(LT)electrode materials.To overcome these issues,a green synthesis approach is proposed to fabricate SnO_(2) nanoparticles using an aqueous extract of banana peel,while the leftover peel serves as a carbon precursor to produce a SnO_(2)/hard carbon composite.The optimized SnO_(2)/hard carbon(7:3)composite was used as the anode and showcased a remarkable reversible capacity of 1110 mAh g^(-1) at room temperature and retained about 660 mAh g^(-1) at-20℃ and 100 mA g^(-1) after 100 cycles,with a capacity of 383 mAh g^(-1) even at-30℃.Stable cycling performance was achieved by the synergistic interaction of SnO_(2) and hard carbon,which improved lithium-ion diffusion and mitigated volume expansion.This eco-friendly and scalable approach shows great promise for developing high-performance anodes for the next generation of LT LIBs.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
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
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
Water-cooled system have significantly enhanced the power generation efficiency of offshore wind turbines.However,these innovative systems are susceptible to substantial biological fouling,maintenance challenges,and h...Water-cooled system have significantly enhanced the power generation efficiency of offshore wind turbines.However,these innovative systems are susceptible to substantial biological fouling,maintenance challenges,and high upkeep costs.Therefore,the development of a specialized front-end filter tailored for direct current water-cooled system is importance.This involves the integration of dimensionally stable anode(DSA)and nickel alloy cathode,valued for their corrosion resistance in seawater,into a novel front-end filter system for Water-cooled applications.This system has the dual capability of generating hydrogen and chlorine for self-cleaning purposes.Implementing a flushing pulse electrolysis mode,it effectively mitigates electrode failure induced by cathodic calcium and magnesium deposition,thereby significantly prolonging electrode lifespan.Laboratory tests comprising system assembly and performance evaluations were conducted,with the system programmed to operate for 5 minutes every 24 hours under continuous flushing by natural seawater to simulate real-world conditions.After more than 11 months of continuous flushing,observations reveal that the DSA mesh and nickel alloy mesh maintain intact structural integrity and normal functioning.Subsequent 1꞉1 physical prototype Sea trial further validated the soundness of the system design and electrolytic control parameters.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
Aqueous zinc battery promotes great interest due to its high safety and significant energy density.However,the Zn anode shows severity of dendrite growth and hydrogen evolution reaction(HER).Addressing these challenge...Aqueous zinc battery promotes great interest due to its high safety and significant energy density.However,the Zn anode shows severity of dendrite growth and hydrogen evolution reaction(HER).Addressing these challenges requires effective manipulation of the inner Helmholtz plane(IHP).Thereby,we secure a novel strategy for generating water-locking IHP through the in-situ growth of a hygroscopic Zn-ethanolamine(Zn-EA)protective layer on the Zn surface.This layer forms via coordination between ZnCl_(2) salt and ethanolamine,effectively reducing the intermediate/free water.Moreover,ethanolamine contains zincophilic sites(C–O and–NH_(2))further promote the uniform Zn deposition.The in-situ Raman confirms the ability of the hygroscopic layer to lock the active water away from the Zn surface.Therefore,Zn-EA@Zn anode exhibits an impressive life stability of 288 h at 20 mA cm^(-2) and 20 mAh cm^(-2) with an extended lifespan of 2100 h at 1 mA cm^(-2) and 1 mAh cm^(-2).Furthermore,the Zn-EA@Zn||Cu demonstrates 100%Coulombic efficiency over 4275 cycles,while Zn-EA@Zn||V2O_(3)/NC full cell retains a specific capacity of 170 mAh g^(-1) at 5 A g^(-1) after 1000 cycles,and the pouch cell maintains 0.5 mAh cm^(-2) after 460 cycles at 2 mA cm^(-2).Therefore,this approach is paving the way for the development of advanced zinc metal batteries.展开更多
Li metal anodes,with high theoretical capacity(3860 mAh g^(-1))and low redox potential,are promising for high-capacity rechargeable batteries.Especially,ultra-thin Li metal anodes can improve energy density and minimi...Li metal anodes,with high theoretical capacity(3860 mAh g^(-1))and low redox potential,are promising for high-capacity rechargeable batteries.Especially,ultra-thin Li metal anodes can improve energy density and minimize lithium excess.However,their poor processability leads to non-uniform Li layers and unstable plating/stripping behavior.In this study,we present a current collector interphase(CCI)-based strategy using a Cu foil coated with a lithiophilic Si3N4 layer,followed by molten Li dip-coating to form around 20 lm Li layer.Furthermore,the scalable dip-coating method,compatibility with large-area current collectors(up to 100 cm^(2)),and stable cycling in pouch cells demonstrate the practical viability of the proposed SNLMA design for commercial lithium metal batteries.During the process,an in-situ Li–Si–N alloy gradient interphase forms at the interface,enhancing wettability and mechanical integrity.This unique gradient CCI provides synergistic lithiophilicity and structural stability,enabling high-performance Li metal batteries.The resulting LixSiy and LixNy phases reduce nucleation barriers and enable uniform Li deposition.As a result,the Si3N4–Li anode paired with a high-loading LCO cathode(22 mg cm^(-2))achieved 83%capacity retention after 100 cycles.This work offers a scalable and practical CCI design for next-generation Li metal batteries.展开更多
Sodium-based dual-ion batteries(SDIBs)have been attracting increasing attention in recent years owing to their low cost,environmental benignancy,and high operating voltage.However,the sluggish ion kinetics of conventi...Sodium-based dual-ion batteries(SDIBs)have been attracting increasing attention in recent years owing to their low cost,environmental benignancy,and high operating voltage.However,the sluggish ion kinetics of conventional carbon anodes that cannot match the fast capacitive anion intercalation behavior of graphite cathodes constraints on improving power density of SDIBs.Herein,we present an ingenious carbon microdomain engineering strategy to fabricate high-performance carbon anode with ion-mediated high-activity nitrogen species and molecular-scale closed-pore architectures.Experimental characterizations and theoretical investigations demonstrate that Zn^(2+)-mediated structural engineering tailors oxidized nitrogen species,which proficiently accelerate the sodium-ion desolvation kinetics;meanwhile the acetate-mediated pore-forming process modulates closed pores,which synergistically afford abundant sodium storage sites for high plateau-region capacity.As a result,the optimized microdomain engineered carbon material(MEC_(3))tailored with the optimal amount of zinc acetate demonstrates an outstanding plateau-region capacity of 253 mAh g^(-1)even at 1 C,among the highest reported values.Consequently,the MEC_(3)||expanded graphite dual-ion battery exhibits an unprecedented cycling stability at high current rate,maintaining 80.6%capacity retention after 10,000 cycles at 10 C,among the best reports.This microdomain engineering strategy provides a new design principle for overcoming kinetic limitations of carbonaceous materials in plateau-dominated sodium storage systems.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
Aqueous zinc(Zn)-ion batteries hold great promise as renewable energy storage system for carbon-neutral energy transition.However,Zn anodes suffer from poor Zn plating/stripping reversibility due to Zn dendrite growth...Aqueous zinc(Zn)-ion batteries hold great promise as renewable energy storage system for carbon-neutral energy transition.However,Zn anodes suffer from poor Zn plating/stripping reversibility due to Zn dendrite growth and side reactions.Existing Zn interfacial modification strategies based on single-component or homogeneous structure are insufficient to address these issues comprehensively.Herein,we rationally designed an organic-inorganic hybrid interfacial layer with rigid-to-soft graded structure for dendrite-free and stable Zn anodes.A liquid plasma-assisted oxidation technology is developed to rapidly construct a porous ZnO inner framework in situ.This ZnO layer offers high interfacial energy,mechanical robustness,and an open structure that facilitates ion transport while firmly anchoring a subsequently coated soft polymer layer.The resulting architecture presents a structurally graded and functionally complementary interface,enabling effective dendrite suppression,continuous Zn ion transport,and enhanced corrosion resistance.As a result,a long cycling stability of more than 6000 h can be achieved at 1 mA cm^(-2)for 1 mAh cm^(-2)in symmetric cells.When used as anodes for zinc-iodine full battery,the hybrid interlayer can effectively prevent the Zn anodes from the corrosion by polyiodine,enabling stable cycling and negligible capacity decay(~0.02‰per cycle)for over 10,000 cycles at 2.0 A g^(-1).This work demonstrates a promising interfacial design strategy and introduces a novel liquid plasma-assisted oxidation route for fabricating high-performance Zn anodes towards next-generation aqueous batteries.展开更多
As an earth-abundant and natural biopolymer,cellulose has received significant attention in aqueous zinc-ion batteries(AZIBs)due to its inherent sustainability and non-toxicity,aligning perfectly with the core advanta...As an earth-abundant and natural biopolymer,cellulose has received significant attention in aqueous zinc-ion batteries(AZIBs)due to its inherent sustainability and non-toxicity,aligning perfectly with the core advantages of AZIBs.Nevertheless,the practical implementation of cellulose-based materials is limited by their intrinsically low ionic conductivity.Herein,we introduce a novel zincophilic artificial protective layer by strategically hybridizing hydroxypropyl cellulose(HPC)with zinc trifluoromethanesulfonate on a zinc metal anode(HZ@Zn).Characterization and calculations demonstrate that the multihydroxyl architecture of HPC constructs hydrogen bond networks,whereas the Zn^(2+)-coordinated HPC domains function as preferential nucleation sites for zinc deposition.These interactions collectively enhance ion transport and accelerate desolvation kinetics.Additionally,the hybrid layer's mechanical flexibility and interfacial adhesion ensure the integrity of the artificial protective layer during long cycling.Thanks to this synergistic effect,HZ@Zn shows exceptional electrochemical performance,including a low desolvation activation energy of 14.38 kJ mol^(-1)and ultra-long cycling stability.Symmetric cells demonstrate exceptional longevity,exceeding 9,500 h at 0.5 mA cm^(-2)/0.25 mAh cm^(-2),whereas HZ@Zn‖PANI full cells maintain 89.8%capacity retention after 4000 cycles at 5 A g^(-1).This study establishes biopolymers as versatile platforms for effectively stabilizing the zinc metal anode.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
基金Project (No. 2002AA517020) supported by the Hi-Tech Research and Development Program (863) of China
文摘Control design is important for proton exchange membrane fuel cell (PEMFC) generator. This work researched the anode system of a 60-kW PEMFC generator. Both anode pressure and humidity must be maintained at ideal levels during steady operation. In view of characteristics and requirements of the system, a hybrid intelligent PID controller is designed specifically based on dynamic simulation. A single neuron PI controller is used for anode humidity by adjusting the water injection to the hydrogen cell. Another incremental PID controller, based on the diagonal recurrent neural network (DRNN) dynamic identification, is used to control anode pressure to be more stable and exact by adjusting the hydrogen flow rate. This control strategy can avoid the coupling problem of the PEMFC and achieve a more adaptive ability. Simulation results showed that the control strategy can maintain both anode humidity and pressure at ideal levels regardless of variable load, nonlinear dynamic and coupling characteristics of the system. This work will give some guides for further control design and applications of the total PEMFC generator.
基金supported by National Natural Science Foundation of China(No.52377145).
文摘Atmospheric pressure plasma-liquid interactions exist in a variety of applications,including wastewater treatment,wound sterilization,and disinfection.In practice,the phenomenon of liquid surface depression will inevitably appear.The applied gas will cause a depression on the liquid surface,which will undoubtedly affect the plasma generation and further affect the application performance.However,the effect of liquid surface deformation on the plasma is still unclear.In this work,numerical models are developed to reveal the mechanism of liquid surface depressions affecting plasma discharge characteristics and the consequential distribution of plasma species,and further study the influence of liquid surface depressions of different sizes generated by different helium flow rates on the plasma.Results show that the liquid surface deformation changes the initial spatial electric field,resulting in the rearrangement of electrons on the liquid surface.The charges deposited on the liquid surface further increase the degree of distortion of the electric field.Moreover,the electric field and electron distribution affected by the liquid surface depression significantly influence the generation and distribution of active species,which determines the practical effectiveness of the relevant applications.This work explores the phenomenon of liquid surface depression,which has been neglected in previous related work,and contributes to further understanding of plasma-liquid interactions,providing better theoretical guidance for related applications and technologies.
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 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funded by the projects AP19578472“Electrophoretic deposition of composite multilayer gel-polymer electrolyte for 3D lithium-ion batteries”the Research Targeted Programs BR24992766“Development of methods and technologies for environmentally friendly“green”processing of polymer waste for energy storage”from the Ministry of ScienceHigher Education of the Republic of Kazakhstan and 111024CRP2010 and 20122022FD4135 from Nazarbayev University。
文摘Renewable energy is critical to building a sustainable society,but its true potential can only be unlocked by developing efficient,environmentally friendly energy storage systems.Advances in storage technologies,including cost-effective and green materials,are quickly becoming the cornerstone of sustainable energy solutions.The most effective battery technology available now is lithium-ion batteries(LIBs).However,the sustainability of battery material production and the degradation of LIB functionality at subzero temperatures pose significant challenges,highlighting the urgent need for alternative and sustainable low-temperature(LT)electrode materials.To overcome these issues,a green synthesis approach is proposed to fabricate SnO_(2) nanoparticles using an aqueous extract of banana peel,while the leftover peel serves as a carbon precursor to produce a SnO_(2)/hard carbon composite.The optimized SnO_(2)/hard carbon(7:3)composite was used as the anode and showcased a remarkable reversible capacity of 1110 mAh g^(-1) at room temperature and retained about 660 mAh g^(-1) at-20℃ and 100 mA g^(-1) after 100 cycles,with a capacity of 383 mAh g^(-1) even at-30℃.Stable cycling performance was achieved by the synergistic interaction of SnO_(2) and hard carbon,which improved lithium-ion diffusion and mitigated volume expansion.This eco-friendly and scalable approach shows great promise for developing high-performance anodes for the next generation of LT LIBs.
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Supported by the Project of Design of Anti-corrosion and Anti-fouling Solutions for Offshore Wind Power Water-Cooled Systems(No.E428161)the National Natural Science Foundation of China(No.42176047)。
文摘Water-cooled system have significantly enhanced the power generation efficiency of offshore wind turbines.However,these innovative systems are susceptible to substantial biological fouling,maintenance challenges,and high upkeep costs.Therefore,the development of a specialized front-end filter tailored for direct current water-cooled system is importance.This involves the integration of dimensionally stable anode(DSA)and nickel alloy cathode,valued for their corrosion resistance in seawater,into a novel front-end filter system for Water-cooled applications.This system has the dual capability of generating hydrogen and chlorine for self-cleaning purposes.Implementing a flushing pulse electrolysis mode,it effectively mitigates electrode failure induced by cathodic calcium and magnesium deposition,thereby significantly prolonging electrode lifespan.Laboratory tests comprising system assembly and performance evaluations were conducted,with the system programmed to operate for 5 minutes every 24 hours under continuous flushing by natural seawater to simulate real-world conditions.After more than 11 months of continuous flushing,observations reveal that the DSA mesh and nickel alloy mesh maintain intact structural integrity and normal functioning.Subsequent 1꞉1 physical prototype Sea trial further validated the soundness of the system design and electrolytic control parameters.
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the financial support from the Natural Science Foundation of Shaanxi(2025RS-CXTD-003)National Natural Science Foundation of China(U24A20299)+2 种基金Natural Science Foundation of Ningbo(2024J011)National Natural Science Foundation of China(Grant No.22279103)Fundamental Research Funds for the Central Universities.
文摘Aqueous zinc battery promotes great interest due to its high safety and significant energy density.However,the Zn anode shows severity of dendrite growth and hydrogen evolution reaction(HER).Addressing these challenges requires effective manipulation of the inner Helmholtz plane(IHP).Thereby,we secure a novel strategy for generating water-locking IHP through the in-situ growth of a hygroscopic Zn-ethanolamine(Zn-EA)protective layer on the Zn surface.This layer forms via coordination between ZnCl_(2) salt and ethanolamine,effectively reducing the intermediate/free water.Moreover,ethanolamine contains zincophilic sites(C–O and–NH_(2))further promote the uniform Zn deposition.The in-situ Raman confirms the ability of the hygroscopic layer to lock the active water away from the Zn surface.Therefore,Zn-EA@Zn anode exhibits an impressive life stability of 288 h at 20 mA cm^(-2) and 20 mAh cm^(-2) with an extended lifespan of 2100 h at 1 mA cm^(-2) and 1 mAh cm^(-2).Furthermore,the Zn-EA@Zn||Cu demonstrates 100%Coulombic efficiency over 4275 cycles,while Zn-EA@Zn||V2O_(3)/NC full cell retains a specific capacity of 170 mAh g^(-1) at 5 A g^(-1) after 1000 cycles,and the pouch cell maintains 0.5 mAh cm^(-2) after 460 cycles at 2 mA cm^(-2).Therefore,this approach is paving the way for the development of advanced zinc metal batteries.
基金supported by the Nano&Material Technology Development Program through the National Research Foundation of Korea(NRF)funded by Ministry of Science and ICT(RS-2024-00405905)This research was supported by BrainLink program funded by the Ministry of Science and ICT through the National Research Foundation of Korea(RS-2023-00236798)Following are results of a study on the“Busan Regional Innovation System&Education(RISE)”Project,supported by the Ministry of Education and Busan Metropolitan City。
文摘Li metal anodes,with high theoretical capacity(3860 mAh g^(-1))and low redox potential,are promising for high-capacity rechargeable batteries.Especially,ultra-thin Li metal anodes can improve energy density and minimize lithium excess.However,their poor processability leads to non-uniform Li layers and unstable plating/stripping behavior.In this study,we present a current collector interphase(CCI)-based strategy using a Cu foil coated with a lithiophilic Si3N4 layer,followed by molten Li dip-coating to form around 20 lm Li layer.Furthermore,the scalable dip-coating method,compatibility with large-area current collectors(up to 100 cm^(2)),and stable cycling in pouch cells demonstrate the practical viability of the proposed SNLMA design for commercial lithium metal batteries.During the process,an in-situ Li–Si–N alloy gradient interphase forms at the interface,enhancing wettability and mechanical integrity.This unique gradient CCI provides synergistic lithiophilicity and structural stability,enabling high-performance Li metal batteries.The resulting LixSiy and LixNy phases reduce nucleation barriers and enable uniform Li deposition.As a result,the Si3N4–Li anode paired with a high-loading LCO cathode(22 mg cm^(-2))achieved 83%capacity retention after 100 cycles.This work offers a scalable and practical CCI design for next-generation Li metal batteries.
基金support from the National Key R&D Program of China(2022YFB2402600)the National Natural Science Foundation of China(52125105,52572282,52472269,52273312,22309200)+3 种基金Guangdong Basic and Applied Basic Research Foundation(2024A1515010201,2024A1515012379,2024A1515011670,2023A1515011519)Guangdong Special Support Program Outstanding Young Talents in Science and Technology Innovation(2021TQ05L894)Shenzhen Science and Technology Planning Project(JSGG20220831104004008,SGDX20230116092055008,KCXST20221021111606016)the NSRF via the Program Management Unit for Human Resources&Institutional Development,Research and Innovation(B49G680115).
文摘Sodium-based dual-ion batteries(SDIBs)have been attracting increasing attention in recent years owing to their low cost,environmental benignancy,and high operating voltage.However,the sluggish ion kinetics of conventional carbon anodes that cannot match the fast capacitive anion intercalation behavior of graphite cathodes constraints on improving power density of SDIBs.Herein,we present an ingenious carbon microdomain engineering strategy to fabricate high-performance carbon anode with ion-mediated high-activity nitrogen species and molecular-scale closed-pore architectures.Experimental characterizations and theoretical investigations demonstrate that Zn^(2+)-mediated structural engineering tailors oxidized nitrogen species,which proficiently accelerate the sodium-ion desolvation kinetics;meanwhile the acetate-mediated pore-forming process modulates closed pores,which synergistically afford abundant sodium storage sites for high plateau-region capacity.As a result,the optimized microdomain engineered carbon material(MEC_(3))tailored with the optimal amount of zinc acetate demonstrates an outstanding plateau-region capacity of 253 mAh g^(-1)even at 1 C,among the highest reported values.Consequently,the MEC_(3)||expanded graphite dual-ion battery exhibits an unprecedented cycling stability at high current rate,maintaining 80.6%capacity retention after 10,000 cycles at 10 C,among the best reports.This microdomain engineering strategy provides a new design principle for overcoming kinetic limitations of carbonaceous materials in plateau-dominated sodium storage systems.
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support from the Australian Research Council Discovery Program(DP220103416,DP240102177)Australian Research Council Future Fellowships(FT200100730,FT210100804).
文摘Aqueous zinc(Zn)-ion batteries hold great promise as renewable energy storage system for carbon-neutral energy transition.However,Zn anodes suffer from poor Zn plating/stripping reversibility due to Zn dendrite growth and side reactions.Existing Zn interfacial modification strategies based on single-component or homogeneous structure are insufficient to address these issues comprehensively.Herein,we rationally designed an organic-inorganic hybrid interfacial layer with rigid-to-soft graded structure for dendrite-free and stable Zn anodes.A liquid plasma-assisted oxidation technology is developed to rapidly construct a porous ZnO inner framework in situ.This ZnO layer offers high interfacial energy,mechanical robustness,and an open structure that facilitates ion transport while firmly anchoring a subsequently coated soft polymer layer.The resulting architecture presents a structurally graded and functionally complementary interface,enabling effective dendrite suppression,continuous Zn ion transport,and enhanced corrosion resistance.As a result,a long cycling stability of more than 6000 h can be achieved at 1 mA cm^(-2)for 1 mAh cm^(-2)in symmetric cells.When used as anodes for zinc-iodine full battery,the hybrid interlayer can effectively prevent the Zn anodes from the corrosion by polyiodine,enabling stable cycling and negligible capacity decay(~0.02‰per cycle)for over 10,000 cycles at 2.0 A g^(-1).This work demonstrates a promising interfacial design strategy and introduces a novel liquid plasma-assisted oxidation route for fabricating high-performance Zn anodes towards next-generation aqueous batteries.
基金supported by the National Natural Science Foundation of China(32071715)the National Science Foundation of Tianjin City(22JCZDJC00560)。
文摘As an earth-abundant and natural biopolymer,cellulose has received significant attention in aqueous zinc-ion batteries(AZIBs)due to its inherent sustainability and non-toxicity,aligning perfectly with the core advantages of AZIBs.Nevertheless,the practical implementation of cellulose-based materials is limited by their intrinsically low ionic conductivity.Herein,we introduce a novel zincophilic artificial protective layer by strategically hybridizing hydroxypropyl cellulose(HPC)with zinc trifluoromethanesulfonate on a zinc metal anode(HZ@Zn).Characterization and calculations demonstrate that the multihydroxyl architecture of HPC constructs hydrogen bond networks,whereas the Zn^(2+)-coordinated HPC domains function as preferential nucleation sites for zinc deposition.These interactions collectively enhance ion transport and accelerate desolvation kinetics.Additionally,the hybrid layer's mechanical flexibility and interfacial adhesion ensure the integrity of the artificial protective layer during long cycling.Thanks to this synergistic effect,HZ@Zn shows exceptional electrochemical performance,including a low desolvation activation energy of 14.38 kJ mol^(-1)and ultra-long cycling stability.Symmetric cells demonstrate exceptional longevity,exceeding 9,500 h at 0.5 mA cm^(-2)/0.25 mAh cm^(-2),whereas HZ@Zn‖PANI full cells maintain 89.8%capacity retention after 4000 cycles at 5 A g^(-1).This study establishes biopolymers as versatile platforms for effectively stabilizing the zinc metal anode.
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.
