Silicon-based materials have demonstrated remarkable potential in high-energy-density batteries owing to their high theoretical capacity.However,the significant volume expansion of silicon seriously hinders its utiliz...Silicon-based materials have demonstrated remarkable potential in high-energy-density batteries owing to their high theoretical capacity.However,the significant volume expansion of silicon seriously hinders its utilization as a lithium-ion anode.Herein,a functionalized high-toughness polyimide(PDMI) is synthesized by copolymerizing the 4,4'-Oxydiphthalic anhydride(ODPA) with 4,4'-oxydianiline(ODA),2,3-diaminobenzoic acid(DABA),and 1,3-bis(3-aminopropyl)-tetramethyl disiloxane(DMS).The combination of rigid benzene rings and flexible oxygen groups(-O-) in the PDMI molecular chain via a rigidness/softness coupling mechanism contributes to high toughness.The plentiful polar carboxyl(-COOH) groups establish robust bonding strength.Rapid ionic transport is achieved by incorporating the flexible siloxane segment(Si-O-Si),which imparts high molecular chain motility and augments free volume holes to facilitate lithium-ion transport(9.8 × 10^(-10) cm^(2) s^(-1) vs.16 × 10^(-10) cm^(2) s~(-1)).As expected,the SiO_x@PDMI-1.5 electrode delivers brilliant long-term cycle performance with a remarkable capacity retention of 85% over 500 cycles at 1.3 A g^(-1).The well-designed functionalized polyimide also significantly enhances the electrochemical properties of Si nanoparticles electrode.Meanwhile,the assembled SiO_x@PDMI-1.5/NCM811 full cell delivers a high retention of 80% after 100 cycles.The perspective of the binder design strategy based on polyimide modification delivers a novel path toward high-capacity electrodes for high-energy-density batteries.展开更多
The inferior conductivity and drastic volume expansion of silicon still remain the bottleneck in achieving high energy density Lithium-ion Batteries(LIBs).The design of the three-dimensional structure of electrodes by...The inferior conductivity and drastic volume expansion of silicon still remain the bottleneck in achieving high energy density Lithium-ion Batteries(LIBs).The design of the three-dimensional structure of electrodes by compositing silicon and carbon materials has been employed to tackle the above challenges,however,the exorbitant costs and the uncertainty of the conductive structure persist,leaving ample room for improvement.Herein,silicon nanoparticles were innovatively composited with eco-friendly biochar sourced from cotton to fabricate a 3D globally consecutive conductive network.The network serves a dual purpose:enhancing overall electrode conductivity and serving as a scaffold to maintain electrode integrity.The conductivity of the network was further augmented by introducing P-doping at the optimum doping temperature of 350℃.Unlike the local conductive sites formed by the mere mixing of silicon and conductive agents,the consecutive network can affirm the improvement of the conductivity at a macro level.Moreover,first-principle calculations further validated that the rapid diffusion of Li^(+)is attributed to the tailored electronic microstructure and charge rearrangement of the fiber.The prepared consecutive conductive Si@P-doped carbonized cotton fiber anode outperforms the inconsecutive Si@Graphite anode in both cycling performance(capacity retention of 1777.15 mAh g^(-1) vs.682.56 mAh g^(-1) after 150 cycles at 0.3 C)and rate performance(1244.24 mAh g^(-1) vs.370.28 mAh g^(-1) at 2.0 C).The findings of this study may open up new avenues for the development of globally interconnected conductive networks in Si-based anodes,thereby enabling the fabrication of high-performance LIBs.展开更多
The solvation structure of Li^(+) in chemical prelithiation reagent plays a key role in improving the low initial Coulombic efficiency(ICE) and poor cycle performance of silicon-based materials. Never theless, the che...The solvation structure of Li^(+) in chemical prelithiation reagent plays a key role in improving the low initial Coulombic efficiency(ICE) and poor cycle performance of silicon-based materials. Never theless, the chemical prelithiation agent is difficult to dope active Li^(+) in silicon-based anodes because of their low working voltage and sluggish Li^(+) diffusion rate. By selecting the lithium–arene complex reagent with 4-methylbiphenyl as an anion ligand and 2-methyltetrahydrofuran as a solvent, the as-prepared micro-sized Si O/C anode can achieve an ICE of nearly 100%. Interestingly, the best prelithium efficiency does not correspond to the lowest redox half-potential(E_(1/2)), and the prelithiation efficiency is determined by the specific influencing factors(E_(1/2), Li^(+) concentration, desolvation energy, and ion diffusion path). In addition, molecular dynamics simulations demonstrate that the ideal prelithiation efficiency can be achieved by choosing appropriate anion ligand and solvent to regulate the solvation structure of Li^(+). Furthermore, the positive effect of prelithiation on cycle performance has been verified by using an in-situ electrochemical dilatometry and solid electrolyte interphase film characterizations.展开更多
Photoelectrochemical(PEC)water splitting holds significant promise for sustainable energy harvesting that enables efficient conversion of solar energy into green hydrogen.Nevertheless,achievement of high performance i...Photoelectrochemical(PEC)water splitting holds significant promise for sustainable energy harvesting that enables efficient conversion of solar energy into green hydrogen.Nevertheless,achievement of high performance is often limited by charge carrier recombination,resulting in unsatisfactory saturation current densities.To address this challenge,we present a novel strategy for achieving ultrahigh current density by incorporating a bridge layer between the Si substrate and the NiOOH cocatalyst in this paper.The optimal photoanode(TCO/n-p-Si/TCO/Ni)shows a remarkably low onset potential of 0.92 V vs.a reversible hydrogen electrode and a high saturation current density of 39.6 mA·cm^(-2),which is about 92.7%of the theoretical maximum(42.7 mA·cm^(-2)).In addition,the photoanode demonstrates stable operation for 60 h.Our systematic characterizations and calculations demonstrate that the bridge layer facilitates charge transfer,enhances catalytic performance,and provides corrosion protection to the underlying substrate.Notably,the integration of this photoanode into a PEC device for overall water splitting leads to a reduction of the onset potential.These findings provide a viable pathway for fabricating highperformance industrial photoelectrodes by integrating a substrate and a cocatalyst via a transparent and conductive bridge layer.展开更多
In this work,the combined addition of strontium/indium(Sr/In)to the magnesium anode for Mg-Air Cells is investigated to improve discharge performance by modifying the anode/electrolyte interface.Indium exists as solid...In this work,the combined addition of strontium/indium(Sr/In)to the magnesium anode for Mg-Air Cells is investigated to improve discharge performance by modifying the anode/electrolyte interface.Indium exists as solid solution atoms in theα-Mg matrix without its second-phase generation,and at the same time facilitates grain refinement,dendritic segregation and Mg17Sr2-phases precipitation.During discharge operation,Sr modifies the film composition via its compounds and promoted the redeposition of In at the substrate/film interface;their co-deposition behavior on the anodic reaction surface enhances anode reaction kinetics,suppresses the negative difference effect(NDE)and mitigates the“chunk effect”(CE),which is contributed to uniform dissolution and low self-corrosion hydrogen evolution rate(HER).Therefore,Mg-Sr-xIn alloy anodes show excellent discharge performance,e.g.,0.5Sr-1.0In shows an average discharge voltage of 1.4234 V and a specific energy density of 1990.71 Wh kg^(-1)at 10 mA cm^(-2).Furthermore,the decisive factor(CE and self-discharge HE)for anodic efficiency are quantitively analyzed,the self-discharge is the main factor of cell efficiency loss.Surprisingly,all Mg-Sr-xIn anodes show anodic efficiency greater than 60%at high current density(≥10 mA cm^(-2)),making them excellent candidate anodes for Mg-Air cells at high-power output.展开更多
Silicon(Si)is a promising anode material for rechargeable batteries due to its high theoretical capacity and abundance,but its practical application is hindered by the continuous growth of porous solid-electrolyte int...Silicon(Si)is a promising anode material for rechargeable batteries due to its high theoretical capacity and abundance,but its practical application is hindered by the continuous growth of porous solid-electrolyte interphase(SEI),leading to capacity fade.Herein,a LiF-Pie structured SEI is proposed,with LiF nanodomains encapsulated in the inner layer of the organic cross-linking silane matrix.A series of advanced techniques such as cryogenic electron microscopy,time-of-flight secondary ion mass spectrometry,and matrix-assisted laser desorption/ionization time-of-flight mass spectrometry have provided detailed insights into the formation mechanism,nanostructure,and chemical composition of the interface.With such SEI,the capacity retention of LiCoO_(2)||Si is significantly improved from 49.6%to 88.9%after 300 cycles at 100 mA g^(-1).These findings provide a desirable interfacial design principle with enhanced(electro)chemical and mechanical stability,which are crucial for sustaining Si anode functionality,thereby significantly advancing the reliability and practical application of Si-based anodes.展开更多
Lithium metal batteries(LMBs)are emerging as a promising energy storage solution owing to their high energy density and specific capacity.However,the non-uniform plating of lithium and the potential rupture of the sol...Lithium metal batteries(LMBs)are emerging as a promising energy storage solution owing to their high energy density and specific capacity.However,the non-uniform plating of lithium and the potential rupture of the solid-electrolyte interphase(SEI)during extended cycling use may result in dendrite growth,which can penetrate the separator and pose significant short-circuit risks.Forming a stable SEI is essential for the long-term operation of the batteries.Fluorine-rich SEI has garnered significant attention for its ability to effectively passivate electrodes,regulate lithium deposition,and inhibit electrolyte corrosion.Understanding the structural components and preparation methods of existing fluorinated SEI is crucial for optimizing lithium metal anode performance.This paper reviews the research on optimizing LiF passivation interfaces to protect lithium metal anodes.It focuses on four types of compositions in fluorinated SEI that work synergistically to enhance SEI performance.For instance,combining compounds with LiF can further enhance the mechanical strength and ionic conductivity of the SEI.Integrating metals with LiF significantly improves electrochemical performance at the SEI/anode interface,with a necessary focus on reducing electron tunneling risks.Additionally,incorporating polymers with LiF offers balanced improvements in interfacial toughness and ionic conductivity,though maintaining structural stability over long cycles remains a critical area for future research.Although alloys combined with LiF increase surface energy and lithium affinity,challenges such as dendrite growth and volume expansion persist.In summary,this paper emphasizes the crucial role of interfacial structures in LMBs and offers comprehensive guidance for future design and development efforts in battery technology.展开更多
Aqueous zinc-ion batteries are regarded as promising electrochemical energy-storage systems for various applications because of their high safety,low costs,and high capacities.However,dendrite formation and side react...Aqueous zinc-ion batteries are regarded as promising electrochemical energy-storage systems for various applications because of their high safety,low costs,and high capacities.However,dendrite formation and side reactions during zinc plating or stripping greatly reduce the capacity and cycle life of a battery and subsequently limit its practical application.To address these issues,we modified the surface of a zinc anode with a functional bilayer composed of zincophilic Cu and flexible polymer layers.The zincophilic Cu interfacial layer was prepared through CuSO_(4)solution pretreatment to serve as a nucleation site to facilitate uniform Zn deposition.Meanwhile,the polymer layer was coated onto the Cu interface layer to serve as a protective layer that would prevent side reactions between zinc and electrolytes.Benefiting from the synergistic effect of the zincophilic Cu and protective polymer layers,the symmetric battery exhibits an impressive cycle life,lasting over 2900 h at a current density of 1 m A·cm^(-2)with a capacity of 1 m A·h·cm^(-2).Moreover,a full battery paired with a vanadium oxide cathode achieves a remarkable capacity retention of 72%even after 500 cycles.展开更多
Carbon materials are widely recognized as highly promising electrode materials for various energy storage system applications.Coal tar residues(CTR),as a type of carbon-rich solid waste with high value-added utilizati...Carbon materials are widely recognized as highly promising electrode materials for various energy storage system applications.Coal tar residues(CTR),as a type of carbon-rich solid waste with high value-added utilization,are crucially important for the development of a more sustainable world.In this study,we employed a straightforward direct carbonization method within the temperature range of 700-1000℃to convert the worthless solid waste CTR into economically valuable carbon materials as anodes for potassium-ion batteries(PIBs).The effect of carbonization temperature on the microstructure and the potassium ions storage properties of CTR-derived carbons(CTRCs)were systematically explored by structural and morphological characterization,alongside electrochemical performances assessment.Based on the co-regulation between the turbine layers,crystal structure,pore structure,functional groups,and electrical conductivity of CTR-derived carbon carbonized at 900℃(CTRC-900H),the electrode material with high reversible capacity of 265.6m Ah·g^(-1)at 50 m A·g^(-1),a desirable cycling stability with 93.8%capacity retention even after 100 cycles,and the remarkable rate performance for PIBs were obtained.Furthermore,cyclic voltammetry(CV)at different scan rates and galvanostatic intermittent titration technique(GITT)have been employed to explore the potassium ions storage mechanism and electrochemical kinetics of CTRCs.Results indicate that the electrode behavior is predominantly governed by surface-induced capacitive processes,particularly under high current densities,with the potassium storage mechanism characterized by an“adsorption-weak intercalation”mechanism.This work highlights the potential of CTR-based carbon as a promising electrode material category suitable for high-performance PIBs electrodes,while also provides valuable insights into the new avenues for the high value-added utilization of CTR.展开更多
As an emerging electrochemical energy storage technology,potassium-ion batteries(PIBs),which are considered a“beyond Li-ion”battery system,have attracted tremendous attention due to their potential for providing a h...As an emerging electrochemical energy storage technology,potassium-ion batteries(PIBs),which are considered a“beyond Li-ion”battery system,have attracted tremendous attention due to their potential for providing a high energy density,and having abundant resource,and a low cost.However,their commercialization is hindered by the lack of practical anode materials.Among various reported anodes,conventional carbon materials,including graphite,soft carbon,and hard carbon,have emerged as promising candidates because of their abundance,low cost,high conductivity,and tunable structures.However,these materials have problems such as a low initial Coulombic efficiency,significant volume expansion,and unsatisfactory cyclability and rate performance.Various strategies to solve these have been explored,including optimizing the interlayer spacing,structural design,surface coating,constructing a multifunctional framework,and forming composites.This review provides a comprehensive overview of the recent progress in conventional carbon anodes,highlighting structural design strategies,mechanisms for improving the electrochemical performance,and underscores the critical role of these materials in promoting the practical application of PIBs.展开更多
Biomass-derived hard carbons,usually prepared by pyrolysis,are widely considered the most promising anode materials for sodium-ion bat-teries(SIBs)due to their high capacity,low poten-tial,sustainability,cost-effectiv...Biomass-derived hard carbons,usually prepared by pyrolysis,are widely considered the most promising anode materials for sodium-ion bat-teries(SIBs)due to their high capacity,low poten-tial,sustainability,cost-effectiveness,and environ-mental friendliness.The pyrolysis method affects the microstructure of the material,and ultimately its so-dium storage performance.Our previous work has shown that pyrolysis in a sealed graphite vessel im-proved the sodium storage performance of the car-bon,however the changes in its microstructure and the way this influences the sodium storage are still unclear.A series of hard carbon materials derived from corncobs(CCG-T,where T is the pyrolysis temperature)were pyrolyzed in a sealed graphite vessel at different temperatures.As the pyrolysis temperature increased from 1000 to 1400℃ small carbon domains gradually transformed into long and curved domains.At the same time,a greater number of large open pores with uniform apertures,as well as more closed pores,were formed.With the further increase of pyrolysis temperature to 1600℃,the long and curved domains became longer and straighter,and some closed pores gradually became open.CCG-1400,with abundant closed pores,had a superior SIB performance,with an initial reversible ca-pacity of 320.73 mAh g^(-1) at a current density of 30 mA g^(-1),an initial Coulomb efficiency(ICE)of 84.34%,and a capacity re-tention of 96.70%after 100 cycles.This study provides a method for the precise regulation of the microcrystalline and pore structures of hard carbon materials.展开更多
Silicon is considered to be one of the most promising anode materials for lithium-ion batteries(LIBs),but its application is limited by the large volume expansion during alloying and dealloying.The constructing of a h...Silicon is considered to be one of the most promising anode materials for lithium-ion batteries(LIBs),but its application is limited by the large volume expansion during alloying and dealloying.The constructing of a high-performance solid electrolyte interface(SEI) film on the surface of the anode material is considered to be one of the effective strategies to mitigate volume expansion of silicon-based anode.In this study,an intermittent discharge strategy which helps to improve the utilization efficiency of electrolyte additive of lithium difluorobisoxalate phosphate(LiDFBOP) is proposed to construct a highly conductive and dense SEI film.The results of electrochemical and physical characterization and theoretical calculations show that the intermittent discharge in the voltage range from open circuit voltage(OCV) to 1.8 V facilitates the diffusion of the soluble products,creates the conditions for the repeated direct contact between Si@C anode and LiDFBOP additive,increases the decomposition of LiDFBOP additive,and thus produces a uniform,dense and inorganics-rich(Li_(2)C_(2)O_(4),LiF and Li_(x)PO_yF_z) SEI film.Subsequently,this SEI film helps to ensure the even intercalation/de-intercalation of Li^(+) in the SEI film and the homogeneous diffusion of Li^(+) inside the Si particles,decreasing the internal stresses and anisotropic phase transitions,maintaining the integrity of Si particles,inhibiting the volume expansion and thu s improving the electrochemical performance of cells.This study not only improves the utilization efficiency of expensive additives through a simply and low-cost method,but also enriches the strategy to improve the electrochemical performance of Si@C anode through interfacial engineering.展开更多
Mg batteries have high energy density,economic safety,and environmental friendliness.They show great potential as an ideal energy storage technology.This review summarizes the limitations of Mg batteries and explores ...Mg batteries have high energy density,economic safety,and environmental friendliness.They show great potential as an ideal energy storage technology.This review summarizes the limitations of Mg batteries and explores the complex reactions at the Mg anode/electrolyte interface.It focuses on critical issues such as the dissolution of Mg anodes,the evolution of hydrogen gas,the formation of a passivation layer that hinders Mg^(2+)migration,and dendrite growth.To address these interface problems,the review discusses strategies to improve interface reactions.These include the structural design of Mg anodes,suitable substitute materials for the anode,and artificial solid electrolyte interphase films.Finally,it outlines the future research directions for the ideal Mg anode interfaces.The goal is to develop more efficient interface design schemes and optimization strategies to advance Mg battery technology further.展开更多
Aqueous zinc(Zn)-ion batteries(ZIBs)have garnered significant attention as promising energy storage devices,primarily due to their low cost,high power density,and excellent safety profile.However,the commercial viabil...Aqueous zinc(Zn)-ion batteries(ZIBs)have garnered significant attention as promising energy storage devices,primarily due to their low cost,high power density,and excellent safety profile.However,the commercial viability of these batteries is hindered by several issues related to the Zn metal anode,including dendritic growth,hydrogen evolution reaction(HER),surface corrosion,and passivation.This review delves into the root causes and key factors influencing these challenges from both electrochemical thermodynamics and kinetics perspectives.Subsequently,viable strategies to mitigate these issues are systematically summarized,including Zn anode reconstruction,artificial solid-electrolyte interphase(SEI)protection,electrolyte formulation optimization,and separator functionalization.Recent research advancements are examined thoroughly,with a focus on the mechanisms behind these approaches and the resulting battery performance.The review also critically assesses the strengths and limitations of these solutions.Finally,we highlight crucial research directions aimed at advancing the practical application of Zn metal anodes in future aqueous ZIBs.展开更多
Rechargeable magnesium batteries are promising alternatives to traditional lithium batteries because of the high abundance of Mg compounds in earth crust,their low toxicity,and possible favorable properties as electro...Rechargeable magnesium batteries are promising alternatives to traditional lithium batteries because of the high abundance of Mg compounds in earth crust,their low toxicity,and possible favorable properties as electrodes'material.However,Mg metal anodes face several challenges,notably the natively existence of an inactive oxide layer on their surfaces,which reduces their effectiveness.Additionally,interactions of Mg electrodes with electrolyte solutions'components can lead to the formation of insulating surface layers,that can fully block them for ions transport.This review addresses these issues by focusing on surface treatments strategies to enhance electrochemical performance of Mg anodes.It highlights chemical and physical modification techniques to prevent oxidation and inactive-layers formation,as well as their practical implications for MIBs.We also examined the impact of Mg anodes'surface engineering on their electrochemical reversibility and cycling efficiency.Finally,future research directions to improve the performance and commercial viability of magnesium anodes and advance development of high-capacity,safe,and cost-effective energy storage systems based on magnesium electrochemistry are discussed.展开更多
Silicon(Si)is considered one of the most promising anode materials for next-generation lithium-ion batteries due to its ultrahigh theoretical capacity.However,its application is significantly limited by severe volume ...Silicon(Si)is considered one of the most promising anode materials for next-generation lithium-ion batteries due to its ultrahigh theoretical capacity.However,its application is significantly limited by severe volume expansion,leading to structural degradation and poor cycling stability.Polymer binders play a critical role in addressing these issues by providing mechanical stabilization.Inspired by the mechanically adaptive architecture of spider webs,where stiff radial threads and extensible spiral threads act in synergy,a dual-thread architecture polymer binder(PALT)with energy dissipation ability enabled by integrating rigid and flexible domains is designed.The rigid poly(acrylic acid lithium)(PAALi)segments offer structural reinforcement,while the soft segments(poly(lipoic acid-tannic acid),LT)introduce dynamic covalent bonds and multiple hydrogen bonds that function as reversible sacrificial bonds,enhancing energy dissipation during cycling.Comprehensive experimental and computational analyses demonstrate effectively reduced stress concentration,improved structural integrity,and stable electrochemical performance over prolonged cycling.The silicon anode incorporating the PALT binder exhibits a satisfying capacity loss per cycle of 0.042% during 350 charge/discharge cycles at 3580 m A g^(-1).This work highlights a bioinspired binder design strategy that combines intrinsic rigidity with dynamic stress adaptability to advance the mechanical and electrochemical stability of silicon anodes.展开更多
This study presents a novel approach to enhance silicon anode performance through barium titanate(BTO)incorporation,with the establishment of a force-electric coupling model.By introducing piezoelectric BTO into silic...This study presents a novel approach to enhance silicon anode performance through barium titanate(BTO)incorporation,with the establishment of a force-electric coupling model.By introducing piezoelectric BTO into silicon matrices,we successfully improved both the mechanical stability and electrochemical kinetics of the anode.The developed force-electric coupling model explains how BTO mitigates stress accumulation during lithiation while optimizing the kinetics of Li^(+)and electron transfer.Experimental verification and multiphysical simulation indicate that Si@BTO effectively eliminates structural degradation during the cycling process and significantly reduces the charge transfer resistance.The force-electric coupling mechanism further facilitates stable solid electrolyte interphase(SEI)formation.When paired with LiFePO_(4)cathodes,Si@BTO maintains 76% capacity retention after 500 cycles at a 10 C rate.This work establishes a basic force-electric coupling model framework and offers insights into the development of advanced silicon anode batteries with exceptional performance.展开更多
Polyacrylic acid(PAA)-based binders have been demonstrated to significantly enhance the cycling stability of pure silicon(Si)anodes compared to other binder types.However,there is a notable lack of systematic and in-d...Polyacrylic acid(PAA)-based binders have been demonstrated to significantly enhance the cycling stability of pure silicon(Si)anodes compared to other binder types.However,there is a notable lack of systematic and in-depth investigation into the relationship between the molecular weight(MW)of PAA and its performance in pure Si anodes,leading to an absence of reliable theoretical guidance for designing and optimizing of PAA-based binders for these anodes.Herein,we select a series of PAA with varying MWs as binders for Si nanoparticle(SiNP)anodes to systematically identify the optimal MW of PAA for enhancing the electrochemical performance of SiNP anodes.The actual MWs of the various PAA were confirmed by gel permeation chromatography to accurately establish the relationship between MW and binder performance.Within an ultrawide weight average molecular weight(M_(w))range of 35.9-4850 kDa,we identify that the PAA binder with a M_(w)of 1250 kDa(PAA125)exhibits the strongest mechanical strength and the highest adhesion strength,attributed to its favorable molecular chain orientation and robust interchain interactions.These characteristics enable the SiNP anodes utilizing PAA125 to maintain the best interfacial chemistry and bulk mechanical structure stability,leading to optimal electrochemical performance.Notably,the enhancement in cycling stability of SiNP anode by PAA125 under practical application conditions is further validated by the 1.1 Ah LLNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)/SiNP@PAA125 pouch cell.展开更多
Microbial fuel cells(MFCs)are promising for realizing wastewater remediation and electricity co-generation,which may significantly promote the formation of an environmentally friendly,clean energy society.Unfortunatel...Microbial fuel cells(MFCs)are promising for realizing wastewater remediation and electricity co-generation,which may significantly promote the formation of an environmentally friendly,clean energy society.Unfortunately,most of the available MFCs show relatively low electricity generation.Anodes,the major component of MFCs,play the most critical role in electron transfer and organic decomposition,which directly determine the performance of MFCs.In the past decades,various carbonaceous materials and carbon-supported conductive composites have been extensively exploited to optimize the electron transfer on the anode due to their versatile properties,such as large surface area and excellent electrical conductivity.The development of anode materials with a particular structure and performance to satisfy field-scale long-term operation of MFCs remains a huge research challenge,which attracts great attention and urgently needs in-depth exploration of the material engineering of anodes for MFCs.In this review,recent advances in the development and optimization of anodes for MFCs are summarized,and applications of MFCs with advanced anodes in the remediation of different types of wastewater are discussed.Advances of anodes for promoting electron transfer,microbial attachment and organic decomposition are the main focuses.The superiorities of MFCs on different aspects of wastewater remediation are elucidated,along with perspectives on future research of MFCs,aiming to provide useful guidance in related fields.展开更多
Dendrite growth represents one of the most significant challenges that impede the development of aqueous zinc-ion batteries.Herein,Gd^(3+)ions are introduced into conventional electrolytes as a microlevelling agent to...Dendrite growth represents one of the most significant challenges that impede the development of aqueous zinc-ion batteries.Herein,Gd^(3+)ions are introduced into conventional electrolytes as a microlevelling agent to achieve dendrite-free zinc electrodeposition.Simulation and experimental results demonstrate that these Gd^(3+)ions are preferentially adsorbed onto the zinc surface,which enables dendritefree zinc anodes by activating the microlevelling effect during electrodeposition.In addition,the Gd^(3+)additives effectively inhibit side reactions and facilitate the desolvation of[Zn(H_(2)O)_(6)]^(2+),leading to highly reversible zinc plating/stripping.Due to these improvements,the zinc anode demonstrates a significantly prolonged cycle life of 2100 h and achieves an exceptional average Coulombic efficiency of 99.72%over 1400 cycles.More importantly,the Zn//NH_(4)V_(4)O_(10)full cell shows a high capacity retention rate of 85.6%after 1000 cycles.This work not only broadens the application of metallic cations in battery electrolytes but also provides fundamental insights into their working mechanisms.展开更多
基金supported by the National Natural Science Foundation of China (51673017)the National Natural Science Foundation of China (21404005)+1 种基金the Fundamental Research Funds for the Central Universities (XK1802-2)the Natural Science Foundation of Jiangsu Province (BK20150273)。
文摘Silicon-based materials have demonstrated remarkable potential in high-energy-density batteries owing to their high theoretical capacity.However,the significant volume expansion of silicon seriously hinders its utilization as a lithium-ion anode.Herein,a functionalized high-toughness polyimide(PDMI) is synthesized by copolymerizing the 4,4'-Oxydiphthalic anhydride(ODPA) with 4,4'-oxydianiline(ODA),2,3-diaminobenzoic acid(DABA),and 1,3-bis(3-aminopropyl)-tetramethyl disiloxane(DMS).The combination of rigid benzene rings and flexible oxygen groups(-O-) in the PDMI molecular chain via a rigidness/softness coupling mechanism contributes to high toughness.The plentiful polar carboxyl(-COOH) groups establish robust bonding strength.Rapid ionic transport is achieved by incorporating the flexible siloxane segment(Si-O-Si),which imparts high molecular chain motility and augments free volume holes to facilitate lithium-ion transport(9.8 × 10^(-10) cm^(2) s^(-1) vs.16 × 10^(-10) cm^(2) s~(-1)).As expected,the SiO_x@PDMI-1.5 electrode delivers brilliant long-term cycle performance with a remarkable capacity retention of 85% over 500 cycles at 1.3 A g^(-1).The well-designed functionalized polyimide also significantly enhances the electrochemical properties of Si nanoparticles electrode.Meanwhile,the assembled SiO_x@PDMI-1.5/NCM811 full cell delivers a high retention of 80% after 100 cycles.The perspective of the binder design strategy based on polyimide modification delivers a novel path toward high-capacity electrodes for high-energy-density batteries.
基金supported by the National Natural Science Foundation of China(No.12205252)the Basic Public Welfare Re-search Special Project of Zhejiang Province(No.LZY22B040001)+4 种基金the Quzhou Science and Technology Plan Project(No.2022K39)Science and Technology Project of Quzhou Research Institute,Zhejiang University(Nos.IZQ2021KJ2032,IZQ2022KJ3014,and IZQ2022KJ3002)Independent scientific Research Project of Quzhou Research Institute,Zhejiang University(No.IZQ2021RCZX007)New“115 talents”Project ofQuzhou,National Nature Science Foundation of China(No.52172244)Fundamental Research Funds for the Central University(No.226202200053).
文摘The inferior conductivity and drastic volume expansion of silicon still remain the bottleneck in achieving high energy density Lithium-ion Batteries(LIBs).The design of the three-dimensional structure of electrodes by compositing silicon and carbon materials has been employed to tackle the above challenges,however,the exorbitant costs and the uncertainty of the conductive structure persist,leaving ample room for improvement.Herein,silicon nanoparticles were innovatively composited with eco-friendly biochar sourced from cotton to fabricate a 3D globally consecutive conductive network.The network serves a dual purpose:enhancing overall electrode conductivity and serving as a scaffold to maintain electrode integrity.The conductivity of the network was further augmented by introducing P-doping at the optimum doping temperature of 350℃.Unlike the local conductive sites formed by the mere mixing of silicon and conductive agents,the consecutive network can affirm the improvement of the conductivity at a macro level.Moreover,first-principle calculations further validated that the rapid diffusion of Li^(+)is attributed to the tailored electronic microstructure and charge rearrangement of the fiber.The prepared consecutive conductive Si@P-doped carbonized cotton fiber anode outperforms the inconsecutive Si@Graphite anode in both cycling performance(capacity retention of 1777.15 mAh g^(-1) vs.682.56 mAh g^(-1) after 150 cycles at 0.3 C)and rate performance(1244.24 mAh g^(-1) vs.370.28 mAh g^(-1) at 2.0 C).The findings of this study may open up new avenues for the development of globally interconnected conductive networks in Si-based anodes,thereby enabling the fabrication of high-performance LIBs.
基金supported by the National Natural Science Foundation of China (21875107, U1802256, and 22209204)Leading Edge Technology of Jiangsu Province (BK20220009), the Natural Science Foundation of Jiangsu Province (BK20221140)+2 种基金the China Postdoctoral Science Foundation (2022M713364)Jiangsu Specially Appointed Professors ProgramPriority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)。
文摘The solvation structure of Li^(+) in chemical prelithiation reagent plays a key role in improving the low initial Coulombic efficiency(ICE) and poor cycle performance of silicon-based materials. Never theless, the chemical prelithiation agent is difficult to dope active Li^(+) in silicon-based anodes because of their low working voltage and sluggish Li^(+) diffusion rate. By selecting the lithium–arene complex reagent with 4-methylbiphenyl as an anion ligand and 2-methyltetrahydrofuran as a solvent, the as-prepared micro-sized Si O/C anode can achieve an ICE of nearly 100%. Interestingly, the best prelithium efficiency does not correspond to the lowest redox half-potential(E_(1/2)), and the prelithiation efficiency is determined by the specific influencing factors(E_(1/2), Li^(+) concentration, desolvation energy, and ion diffusion path). In addition, molecular dynamics simulations demonstrate that the ideal prelithiation efficiency can be achieved by choosing appropriate anion ligand and solvent to regulate the solvation structure of Li^(+). Furthermore, the positive effect of prelithiation on cycle performance has been verified by using an in-situ electrochemical dilatometry and solid electrolyte interphase film characterizations.
基金supported by Multi-Year Research Grants from the University of Macao(MYRG-GRG2023-00010-IAPME,MYRG-GRG2024-00038-IAPME,MYRG2022-00026-IAPME)the Science and Technology Development Fund(FDCT)from Macao SAR(0023/2023/AFJ,0050/2023/RIB2,006/2022/ALC,0087/2024/AFJ,0111/2022/A2).
文摘Photoelectrochemical(PEC)water splitting holds significant promise for sustainable energy harvesting that enables efficient conversion of solar energy into green hydrogen.Nevertheless,achievement of high performance is often limited by charge carrier recombination,resulting in unsatisfactory saturation current densities.To address this challenge,we present a novel strategy for achieving ultrahigh current density by incorporating a bridge layer between the Si substrate and the NiOOH cocatalyst in this paper.The optimal photoanode(TCO/n-p-Si/TCO/Ni)shows a remarkably low onset potential of 0.92 V vs.a reversible hydrogen electrode and a high saturation current density of 39.6 mA·cm^(-2),which is about 92.7%of the theoretical maximum(42.7 mA·cm^(-2)).In addition,the photoanode demonstrates stable operation for 60 h.Our systematic characterizations and calculations demonstrate that the bridge layer facilitates charge transfer,enhances catalytic performance,and provides corrosion protection to the underlying substrate.Notably,the integration of this photoanode into a PEC device for overall water splitting leads to a reduction of the onset potential.These findings provide a viable pathway for fabricating highperformance industrial photoelectrodes by integrating a substrate and a cocatalyst via a transparent and conductive bridge layer.
文摘In this work,the combined addition of strontium/indium(Sr/In)to the magnesium anode for Mg-Air Cells is investigated to improve discharge performance by modifying the anode/electrolyte interface.Indium exists as solid solution atoms in theα-Mg matrix without its second-phase generation,and at the same time facilitates grain refinement,dendritic segregation and Mg17Sr2-phases precipitation.During discharge operation,Sr modifies the film composition via its compounds and promoted the redeposition of In at the substrate/film interface;their co-deposition behavior on the anodic reaction surface enhances anode reaction kinetics,suppresses the negative difference effect(NDE)and mitigates the“chunk effect”(CE),which is contributed to uniform dissolution and low self-corrosion hydrogen evolution rate(HER).Therefore,Mg-Sr-xIn alloy anodes show excellent discharge performance,e.g.,0.5Sr-1.0In shows an average discharge voltage of 1.4234 V and a specific energy density of 1990.71 Wh kg^(-1)at 10 mA cm^(-2).Furthermore,the decisive factor(CE and self-discharge HE)for anodic efficiency are quantitively analyzed,the self-discharge is the main factor of cell efficiency loss.Surprisingly,all Mg-Sr-xIn anodes show anodic efficiency greater than 60%at high current density(≥10 mA cm^(-2)),making them excellent candidate anodes for Mg-Air cells at high-power output.
基金supported by the National Key Research and Development Program of China(Grant No.2022YFB2502200)the National Natural Science Foundation of China(NSFC nos.52172257 and 22409211)+2 种基金the China Postdoctoral Science Foundation(No.2023M743739)the Postdoctoral Fellowship Program of CPSF(No.GZC20232939)CAS Youth Interdisciplinary Team。
文摘Silicon(Si)is a promising anode material for rechargeable batteries due to its high theoretical capacity and abundance,but its practical application is hindered by the continuous growth of porous solid-electrolyte interphase(SEI),leading to capacity fade.Herein,a LiF-Pie structured SEI is proposed,with LiF nanodomains encapsulated in the inner layer of the organic cross-linking silane matrix.A series of advanced techniques such as cryogenic electron microscopy,time-of-flight secondary ion mass spectrometry,and matrix-assisted laser desorption/ionization time-of-flight mass spectrometry have provided detailed insights into the formation mechanism,nanostructure,and chemical composition of the interface.With such SEI,the capacity retention of LiCoO_(2)||Si is significantly improved from 49.6%to 88.9%after 300 cycles at 100 mA g^(-1).These findings provide a desirable interfacial design principle with enhanced(electro)chemical and mechanical stability,which are crucial for sustaining Si anode functionality,thereby significantly advancing the reliability and practical application of Si-based anodes.
基金support from the National Natural Science Foundation of China(No.U2333210)the Sichuan Science and Technology Program,China(No.21SYSX0011)。
文摘Lithium metal batteries(LMBs)are emerging as a promising energy storage solution owing to their high energy density and specific capacity.However,the non-uniform plating of lithium and the potential rupture of the solid-electrolyte interphase(SEI)during extended cycling use may result in dendrite growth,which can penetrate the separator and pose significant short-circuit risks.Forming a stable SEI is essential for the long-term operation of the batteries.Fluorine-rich SEI has garnered significant attention for its ability to effectively passivate electrodes,regulate lithium deposition,and inhibit electrolyte corrosion.Understanding the structural components and preparation methods of existing fluorinated SEI is crucial for optimizing lithium metal anode performance.This paper reviews the research on optimizing LiF passivation interfaces to protect lithium metal anodes.It focuses on four types of compositions in fluorinated SEI that work synergistically to enhance SEI performance.For instance,combining compounds with LiF can further enhance the mechanical strength and ionic conductivity of the SEI.Integrating metals with LiF significantly improves electrochemical performance at the SEI/anode interface,with a necessary focus on reducing electron tunneling risks.Additionally,incorporating polymers with LiF offers balanced improvements in interfacial toughness and ionic conductivity,though maintaining structural stability over long cycles remains a critical area for future research.Although alloys combined with LiF increase surface energy and lithium affinity,challenges such as dendrite growth and volume expansion persist.In summary,this paper emphasizes the crucial role of interfacial structures in LMBs and offers comprehensive guidance for future design and development efforts in battery technology.
基金financially supported by the Science and Technology Development Project of Henan Province,China(No.242102241042)the Joint Fund of Henan Province Science and Technology R&D Program(No.225200810093)+1 种基金the Startup Research of Henan Academy of Sciences(No.231817001)the Key Innovation Projects for Postgraduates of Henan Academy of Sciences(No.24331712)。
文摘Aqueous zinc-ion batteries are regarded as promising electrochemical energy-storage systems for various applications because of their high safety,low costs,and high capacities.However,dendrite formation and side reactions during zinc plating or stripping greatly reduce the capacity and cycle life of a battery and subsequently limit its practical application.To address these issues,we modified the surface of a zinc anode with a functional bilayer composed of zincophilic Cu and flexible polymer layers.The zincophilic Cu interfacial layer was prepared through CuSO_(4)solution pretreatment to serve as a nucleation site to facilitate uniform Zn deposition.Meanwhile,the polymer layer was coated onto the Cu interface layer to serve as a protective layer that would prevent side reactions between zinc and electrolytes.Benefiting from the synergistic effect of the zincophilic Cu and protective polymer layers,the symmetric battery exhibits an impressive cycle life,lasting over 2900 h at a current density of 1 m A·cm^(-2)with a capacity of 1 m A·h·cm^(-2).Moreover,a full battery paired with a vanadium oxide cathode achieves a remarkable capacity retention of 72%even after 500 cycles.
基金financially supported by the Research Project Supported by Shanxi Scholarship Council of China(No.2022-049)the Natural Science Foundation of Shanxi Province,China(No.20210302123167)。
文摘Carbon materials are widely recognized as highly promising electrode materials for various energy storage system applications.Coal tar residues(CTR),as a type of carbon-rich solid waste with high value-added utilization,are crucially important for the development of a more sustainable world.In this study,we employed a straightforward direct carbonization method within the temperature range of 700-1000℃to convert the worthless solid waste CTR into economically valuable carbon materials as anodes for potassium-ion batteries(PIBs).The effect of carbonization temperature on the microstructure and the potassium ions storage properties of CTR-derived carbons(CTRCs)were systematically explored by structural and morphological characterization,alongside electrochemical performances assessment.Based on the co-regulation between the turbine layers,crystal structure,pore structure,functional groups,and electrical conductivity of CTR-derived carbon carbonized at 900℃(CTRC-900H),the electrode material with high reversible capacity of 265.6m Ah·g^(-1)at 50 m A·g^(-1),a desirable cycling stability with 93.8%capacity retention even after 100 cycles,and the remarkable rate performance for PIBs were obtained.Furthermore,cyclic voltammetry(CV)at different scan rates and galvanostatic intermittent titration technique(GITT)have been employed to explore the potassium ions storage mechanism and electrochemical kinetics of CTRCs.Results indicate that the electrode behavior is predominantly governed by surface-induced capacitive processes,particularly under high current densities,with the potassium storage mechanism characterized by an“adsorption-weak intercalation”mechanism.This work highlights the potential of CTR-based carbon as a promising electrode material category suitable for high-performance PIBs electrodes,while also provides valuable insights into the new avenues for the high value-added utilization of CTR.
文摘As an emerging electrochemical energy storage technology,potassium-ion batteries(PIBs),which are considered a“beyond Li-ion”battery system,have attracted tremendous attention due to their potential for providing a high energy density,and having abundant resource,and a low cost.However,their commercialization is hindered by the lack of practical anode materials.Among various reported anodes,conventional carbon materials,including graphite,soft carbon,and hard carbon,have emerged as promising candidates because of their abundance,low cost,high conductivity,and tunable structures.However,these materials have problems such as a low initial Coulombic efficiency,significant volume expansion,and unsatisfactory cyclability and rate performance.Various strategies to solve these have been explored,including optimizing the interlayer spacing,structural design,surface coating,constructing a multifunctional framework,and forming composites.This review provides a comprehensive overview of the recent progress in conventional carbon anodes,highlighting structural design strategies,mechanisms for improving the electrochemical performance,and underscores the critical role of these materials in promoting the practical application of PIBs.
文摘Biomass-derived hard carbons,usually prepared by pyrolysis,are widely considered the most promising anode materials for sodium-ion bat-teries(SIBs)due to their high capacity,low poten-tial,sustainability,cost-effectiveness,and environ-mental friendliness.The pyrolysis method affects the microstructure of the material,and ultimately its so-dium storage performance.Our previous work has shown that pyrolysis in a sealed graphite vessel im-proved the sodium storage performance of the car-bon,however the changes in its microstructure and the way this influences the sodium storage are still unclear.A series of hard carbon materials derived from corncobs(CCG-T,where T is the pyrolysis temperature)were pyrolyzed in a sealed graphite vessel at different temperatures.As the pyrolysis temperature increased from 1000 to 1400℃ small carbon domains gradually transformed into long and curved domains.At the same time,a greater number of large open pores with uniform apertures,as well as more closed pores,were formed.With the further increase of pyrolysis temperature to 1600℃,the long and curved domains became longer and straighter,and some closed pores gradually became open.CCG-1400,with abundant closed pores,had a superior SIB performance,with an initial reversible ca-pacity of 320.73 mAh g^(-1) at a current density of 30 mA g^(-1),an initial Coulomb efficiency(ICE)of 84.34%,and a capacity re-tention of 96.70%after 100 cycles.This study provides a method for the precise regulation of the microcrystalline and pore structures of hard carbon materials.
基金Department of Education of Gansu Province: Industrial Support Plan Project (2022CYZC-23)National Natural Science Foundation of China (22269012)Gansu Key Research and Development Program (23YFGA0053)。
文摘Silicon is considered to be one of the most promising anode materials for lithium-ion batteries(LIBs),but its application is limited by the large volume expansion during alloying and dealloying.The constructing of a high-performance solid electrolyte interface(SEI) film on the surface of the anode material is considered to be one of the effective strategies to mitigate volume expansion of silicon-based anode.In this study,an intermittent discharge strategy which helps to improve the utilization efficiency of electrolyte additive of lithium difluorobisoxalate phosphate(LiDFBOP) is proposed to construct a highly conductive and dense SEI film.The results of electrochemical and physical characterization and theoretical calculations show that the intermittent discharge in the voltage range from open circuit voltage(OCV) to 1.8 V facilitates the diffusion of the soluble products,creates the conditions for the repeated direct contact between Si@C anode and LiDFBOP additive,increases the decomposition of LiDFBOP additive,and thus produces a uniform,dense and inorganics-rich(Li_(2)C_(2)O_(4),LiF and Li_(x)PO_yF_z) SEI film.Subsequently,this SEI film helps to ensure the even intercalation/de-intercalation of Li^(+) in the SEI film and the homogeneous diffusion of Li^(+) inside the Si particles,decreasing the internal stresses and anisotropic phase transitions,maintaining the integrity of Si particles,inhibiting the volume expansion and thu s improving the electrochemical performance of cells.This study not only improves the utilization efficiency of expensive additives through a simply and low-cost method,but also enriches the strategy to improve the electrochemical performance of Si@C anode through interfacial engineering.
基金supported by National Natural Science Foundation of China(52371095)Innovation Research Group of Universities in Chongqing(CXQT21030)+2 种基金Chongqing Overseas Chinese Entrepreneurship and Innovation Support Program(cx2023117)Chongqing Natural Science Foundation(CSTB2022NSCQ-LZX0054,CSTB2024TIADCYKJCXX0001)Chongqing Youth Expert Studio。
文摘Mg batteries have high energy density,economic safety,and environmental friendliness.They show great potential as an ideal energy storage technology.This review summarizes the limitations of Mg batteries and explores the complex reactions at the Mg anode/electrolyte interface.It focuses on critical issues such as the dissolution of Mg anodes,the evolution of hydrogen gas,the formation of a passivation layer that hinders Mg^(2+)migration,and dendrite growth.To address these interface problems,the review discusses strategies to improve interface reactions.These include the structural design of Mg anodes,suitable substitute materials for the anode,and artificial solid electrolyte interphase films.Finally,it outlines the future research directions for the ideal Mg anode interfaces.The goal is to develop more efficient interface design schemes and optimization strategies to advance Mg battery technology further.
基金financial support by the open foundation of State Key Laboratory of Chemical Engineering(SKL-Ch E-24B03)the Natural Science Foundation of Shandong Province,China(ZR2021QE098)financial support from the Start-Up Research Fund from the University of Macao(SRG2024-00034-IAPME).
文摘Aqueous zinc(Zn)-ion batteries(ZIBs)have garnered significant attention as promising energy storage devices,primarily due to their low cost,high power density,and excellent safety profile.However,the commercial viability of these batteries is hindered by several issues related to the Zn metal anode,including dendritic growth,hydrogen evolution reaction(HER),surface corrosion,and passivation.This review delves into the root causes and key factors influencing these challenges from both electrochemical thermodynamics and kinetics perspectives.Subsequently,viable strategies to mitigate these issues are systematically summarized,including Zn anode reconstruction,artificial solid-electrolyte interphase(SEI)protection,electrolyte formulation optimization,and separator functionalization.Recent research advancements are examined thoroughly,with a focus on the mechanisms behind these approaches and the resulting battery performance.The review also critically assesses the strengths and limitations of these solutions.Finally,we highlight crucial research directions aimed at advancing the practical application of Zn metal anodes in future aqueous ZIBs.
基金supported by the Global Joint Research Program funded by the Pukyong National University(202411790001)the Nano&Material Technology Development Program through the National Research Foundation of Korea(NRF)+2 种基金funded by the Ministry of Science and ICT(RS-2024-00446825)the Technology Innovation Program(RS-2024-00418815)funded by the Ministry of Trade,Industry&Energy(MOTIE,Korea)。
文摘Rechargeable magnesium batteries are promising alternatives to traditional lithium batteries because of the high abundance of Mg compounds in earth crust,their low toxicity,and possible favorable properties as electrodes'material.However,Mg metal anodes face several challenges,notably the natively existence of an inactive oxide layer on their surfaces,which reduces their effectiveness.Additionally,interactions of Mg electrodes with electrolyte solutions'components can lead to the formation of insulating surface layers,that can fully block them for ions transport.This review addresses these issues by focusing on surface treatments strategies to enhance electrochemical performance of Mg anodes.It highlights chemical and physical modification techniques to prevent oxidation and inactive-layers formation,as well as their practical implications for MIBs.We also examined the impact of Mg anodes'surface engineering on their electrochemical reversibility and cycling efficiency.Finally,future research directions to improve the performance and commercial viability of magnesium anodes and advance development of high-capacity,safe,and cost-effective energy storage systems based on magnesium electrochemistry are discussed.
基金the National Natural Science Foundation of China(32201497)for the financial support of this research。
文摘Silicon(Si)is considered one of the most promising anode materials for next-generation lithium-ion batteries due to its ultrahigh theoretical capacity.However,its application is significantly limited by severe volume expansion,leading to structural degradation and poor cycling stability.Polymer binders play a critical role in addressing these issues by providing mechanical stabilization.Inspired by the mechanically adaptive architecture of spider webs,where stiff radial threads and extensible spiral threads act in synergy,a dual-thread architecture polymer binder(PALT)with energy dissipation ability enabled by integrating rigid and flexible domains is designed.The rigid poly(acrylic acid lithium)(PAALi)segments offer structural reinforcement,while the soft segments(poly(lipoic acid-tannic acid),LT)introduce dynamic covalent bonds and multiple hydrogen bonds that function as reversible sacrificial bonds,enhancing energy dissipation during cycling.Comprehensive experimental and computational analyses demonstrate effectively reduced stress concentration,improved structural integrity,and stable electrochemical performance over prolonged cycling.The silicon anode incorporating the PALT binder exhibits a satisfying capacity loss per cycle of 0.042% during 350 charge/discharge cycles at 3580 m A g^(-1).This work highlights a bioinspired binder design strategy that combines intrinsic rigidity with dynamic stress adaptability to advance the mechanical and electrochemical stability of silicon anodes.
基金the financial support of the National Natural Science Foundation of China(NSFC,No.12074093)。
文摘This study presents a novel approach to enhance silicon anode performance through barium titanate(BTO)incorporation,with the establishment of a force-electric coupling model.By introducing piezoelectric BTO into silicon matrices,we successfully improved both the mechanical stability and electrochemical kinetics of the anode.The developed force-electric coupling model explains how BTO mitigates stress accumulation during lithiation while optimizing the kinetics of Li^(+)and electron transfer.Experimental verification and multiphysical simulation indicate that Si@BTO effectively eliminates structural degradation during the cycling process and significantly reduces the charge transfer resistance.The force-electric coupling mechanism further facilitates stable solid electrolyte interphase(SEI)formation.When paired with LiFePO_(4)cathodes,Si@BTO maintains 76% capacity retention after 500 cycles at a 10 C rate.This work establishes a basic force-electric coupling model framework and offers insights into the development of advanced silicon anode batteries with exceptional performance.
基金funding supports of the National Natural Science Foundation of China(52402315,52172244,51874104,and 52172190)the"Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang"(2023R01007)the Zhejiang Provincial"Jianbing"and"Lingyan"R&D Programs(Grant No.2024C01262)。
文摘Polyacrylic acid(PAA)-based binders have been demonstrated to significantly enhance the cycling stability of pure silicon(Si)anodes compared to other binder types.However,there is a notable lack of systematic and in-depth investigation into the relationship between the molecular weight(MW)of PAA and its performance in pure Si anodes,leading to an absence of reliable theoretical guidance for designing and optimizing of PAA-based binders for these anodes.Herein,we select a series of PAA with varying MWs as binders for Si nanoparticle(SiNP)anodes to systematically identify the optimal MW of PAA for enhancing the electrochemical performance of SiNP anodes.The actual MWs of the various PAA were confirmed by gel permeation chromatography to accurately establish the relationship between MW and binder performance.Within an ultrawide weight average molecular weight(M_(w))range of 35.9-4850 kDa,we identify that the PAA binder with a M_(w)of 1250 kDa(PAA125)exhibits the strongest mechanical strength and the highest adhesion strength,attributed to its favorable molecular chain orientation and robust interchain interactions.These characteristics enable the SiNP anodes utilizing PAA125 to maintain the best interfacial chemistry and bulk mechanical structure stability,leading to optimal electrochemical performance.Notably,the enhancement in cycling stability of SiNP anode by PAA125 under practical application conditions is further validated by the 1.1 Ah LLNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)/SiNP@PAA125 pouch cell.
文摘Microbial fuel cells(MFCs)are promising for realizing wastewater remediation and electricity co-generation,which may significantly promote the formation of an environmentally friendly,clean energy society.Unfortunately,most of the available MFCs show relatively low electricity generation.Anodes,the major component of MFCs,play the most critical role in electron transfer and organic decomposition,which directly determine the performance of MFCs.In the past decades,various carbonaceous materials and carbon-supported conductive composites have been extensively exploited to optimize the electron transfer on the anode due to their versatile properties,such as large surface area and excellent electrical conductivity.The development of anode materials with a particular structure and performance to satisfy field-scale long-term operation of MFCs remains a huge research challenge,which attracts great attention and urgently needs in-depth exploration of the material engineering of anodes for MFCs.In this review,recent advances in the development and optimization of anodes for MFCs are summarized,and applications of MFCs with advanced anodes in the remediation of different types of wastewater are discussed.Advances of anodes for promoting electron transfer,microbial attachment and organic decomposition are the main focuses.The superiorities of MFCs on different aspects of wastewater remediation are elucidated,along with perspectives on future research of MFCs,aiming to provide useful guidance in related fields.
基金supported by the Scientific Research and Technology Development Project of China National Petroleum Corporation(Grant Nos.2024ZG50,2022DQ03-03)the National Natural Science Foundation of China(Grant Nos.52372252)the Science and Technology Innovation Program of Hunan Province(Grant Nos.2024RC1022).
文摘Dendrite growth represents one of the most significant challenges that impede the development of aqueous zinc-ion batteries.Herein,Gd^(3+)ions are introduced into conventional electrolytes as a microlevelling agent to achieve dendrite-free zinc electrodeposition.Simulation and experimental results demonstrate that these Gd^(3+)ions are preferentially adsorbed onto the zinc surface,which enables dendritefree zinc anodes by activating the microlevelling effect during electrodeposition.In addition,the Gd^(3+)additives effectively inhibit side reactions and facilitate the desolvation of[Zn(H_(2)O)_(6)]^(2+),leading to highly reversible zinc plating/stripping.Due to these improvements,the zinc anode demonstrates a significantly prolonged cycle life of 2100 h and achieves an exceptional average Coulombic efficiency of 99.72%over 1400 cycles.More importantly,the Zn//NH_(4)V_(4)O_(10)full cell shows a high capacity retention rate of 85.6%after 1000 cycles.This work not only broadens the application of metallic cations in battery electrolytes but also provides fundamental insights into their working mechanisms.
