A flexible air electrode with excellent activity and stability is essential for flexible zinc-air batteries.In this study,we report the rational design of nitrogen-doped carbon nanotube-encapsulated Co9S8 nanopar-ticl...A flexible air electrode with excellent activity and stability is essential for flexible zinc-air batteries.In this study,we report the rational design of nitrogen-doped carbon nanotube-encapsulated Co9S8 nanopar-ticles on carbon cloth(Co9S8/NCNTs/CC),serving as self-supporting air electrodes for both liquid-state and flexible zinc-air batteries.The Co9S8/NCNTs/CC-1 exhibited a half-wave potential of 0.86 V for oxygen re-duction reaction(ORR)and achieved a current density of 10 mA cm-2 for oxygen evolution reaction(OER)at a voltage of only 1.52 V.The well-constructed nanotube on carbon cloth facilitates mass diffu-sion and electron transfer,while enhancing the mechanical flexibility of the material.Density functional theory(DFT)calculations suggested that the synergistic interaction between Co9S8 and NCNTs effectively enhanced the bifunctional electrocatalytic performance of the material.Liquid-state and flexible zinc-air batteries assembled with Co9S8/NCNTs/CC-1 demonstrated outstanding charge-discharge capabilities and long-term stability.展开更多
Developing efficient and stable electrocatalysts has always been the focus of electrochemical research.Here,sea urchin-like nickel-molybdenum bimetallic phosphide nickel-molybdenum alloy(Ni_(4)Mo)and(Ni-Mo-P)were succ...Developing efficient and stable electrocatalysts has always been the focus of electrochemical research.Here,sea urchin-like nickel-molybdenum bimetallic phosphide nickel-molybdenum alloy(Ni_(4)Mo)and(Ni-Mo-P)were successfully synthesized by hydrothermal,annealing and phosphating methods on nickel foam(NF).The unusual shape of the sea urchin facilitates gas release and mass transfer and increases the interaction between catalysts and electrolytes.The Ni_(4)Mo/NF and Ni-Mo-P/NF electrodes only need overpotentials of 72 and 197 mV to reach 50 mA·cm^(−2) under alkaline conditions for hydrogen evolution reaction and oxygen evolution reaction,respectively.The Ni_(4)Mo/NF and Ni-Mo-P/NF asymmetric electrodes were used as anode and cathode for the overall water splitting,respectively.In 1.0 M KOH,at a voltage of 1.485 V,the electrolytic device generated 50 mA·cm^(−2) current density,maintaining for 24 h without reduction.The labor presents a simple method to synthesize a highly active,low-cost,and strongly durable self-supporting electrode for over-water splitting.展开更多
Transition metal-based electrocatalysts are a promising alternative to noble metal catalysts for electrochemical upgrading of biomass-derived 5-hydroxymethylfurfural(HMF)into high-value 2,5-furandicarboxylic acid(FDCA...Transition metal-based electrocatalysts are a promising alternative to noble metal catalysts for electrochemical upgrading of biomass-derived 5-hydroxymethylfurfural(HMF)into high-value 2,5-furandicarboxylic acid(FDCA).However,the rational design of efficient electrocatalysts with precisely tailored structure-activity correlations remains a critical challenge.Herein,we report a hierarchically structured self-supporting electrode(Vo-NiCo(OH)_(2)-NF)synthesized through in situ electrochemical reconstruction of NiCo-Prussian blue analogue(NiCo-PBA)precursor,in which oxygen vacancy(Vo)-rich Co-doped Ni(OH)_(2)nanosheet arrays are vertically aligned on nickel foam(NF),creating an interconnected conductive network.When evaluated for the HMF oxidation reaction(HMFOR),Vo-NiCo(OH)_(2)-NF exhibits exceptional electrochemical performance,achieving near-complete HMF conversion(99%),ultrahigh FDCA Faradaic efficiency(97.5%),and remarkable product yield(96.2%)at 1.45 V,outperforming conventional Co-doped Ni(OH)_(2)(NiCo(OH)_(2)-NF)and pristine Ni(OH)_(2)(Ni(OH)_(2)-NF)electrodes.By combining in situ spectroscopic characterization and theoretical calculations,we elucidate that the synergistic effects of Co-doping and oxygen vacancy engineering effectively modulate the electronic structure of Ni active centers,favor the formation of high-valent Ni^(3+)species,and optimize HMF adsorption,thereby improving the HMFOR performance.This work provides valuable mechanistic insights for catalyst design and may inspire the development of advanced transition metal-based electrodes for efficient biomass conversion systems.展开更多
Vanadium redox flow batteries(VRFBs)are a means of large-scale energy storage due to their excellent scalability,safety,long cycling life,and decoupled power and energy capacities.However,the slow redox kinetics of va...Vanadium redox flow batteries(VRFBs)are a means of large-scale energy storage due to their excellent scalability,safety,long cycling life,and decoupled power and energy capacities.However,the slow redox kinetics of vanadium species on conventional carbon electrodes remains a major limitation to their performance.We investigated the deposition of carbon black,carbon nanotubes,and electrochemically exfoliated graphene(Exf-Gr)onto thermally-activated carbon paper(ACP)by spray coating to increase the electrode electrocatalytic activity.The modified electrodes were characterized using scanning electron microscopy,X-ray diffraction,Raman spectroscopy,X-ray photoelectron microscopy,and surface area analysis,while their electrochemical properties were evaluated by cyclic voltammetry,electrochemical impedance spectroscopy,and singlecell VRFB testing.Among the modified electrodes,Exf-Gr/ACP had the best performance,achieving a 2.9-fold reduction in charge transfer resistance compared to pristine ACP and delivering 2.5 times the discharge capacity in single-cell tests.This improvement is attributed to Exf-Gr’s high surface area,favorable catalytic activity,and excellent dispersion on the ACP substrate.Surface modification with electrochemically exfoliated graphene is a highly effective strategy for improving the electrode performance in VRFB systems,with significant implications for large-scale energy storage.展开更多
The development of shape-customizable and bulk flexible electrochemical devices through processing technologies as versatile as those used for plastics promises to revolutionize the future of battery technology.Howeve...The development of shape-customizable and bulk flexible electrochemical devices through processing technologies as versatile as those used for plastics promises to revolutionize the future of battery technology.However,this pursuit has been fundamentally hindered by the absence of transformative battery materials capable of delivering the necessary electrochemical functions,robust interface adhesion,and,crucially,the suitable rheological properties required for on-demand shaping.In this work,we introduce a concept of a multifunctional plasticine electrode matrix(PEM)featuring nano-interpenetrating networks(nano-IPN)to address this challenge.Utilizing the nonflammable liquid-electrolyte hydration combined with conductive nanomaterials,we have realized a PEM in the form of a multifunctional nanocomposite that integrates ion and electron conduction,component binding,non-flammability,and plasticine-like moldability.With this PEM,we have successfully fabricated a variety of bulk-flexible electrodes with high mass loading of active material(AM)(>70 wt%)using industry-friendly extrusion and compression molding techniques.Moreover,these high AM-loading composite electrodes achieve an unparalleled bulk conformability and flexibility,remaining structurally intact even under severe mechanical stress.Ultimately,we have successfully produced shape-patternable and flexible batteries via extrusion molding.This study underscores the potential of the PEM to revolutionize battery microstructures,interfaces,manufacturing processes,and performance characteristics.展开更多
Taking the underground shale of the Silurian Longmaxi Formation in southern Sichuan Basin as the research object,stress-sensitive experiments on self-supporting fractures and micro-visualization experiments on gas-wat...Taking the underground shale of the Silurian Longmaxi Formation in southern Sichuan Basin as the research object,stress-sensitive experiments on self-supporting fractures and micro-visualization experiments on gas-water flow were conducted under simulated reservoir conditions to study the mechanism of microscopic gas-water flow during the fracture closure process and discuss its engineering applications.The results show that as the effective stress gradually increased from 5 MPa to 60 MPa with an increment of 5 MPa per step,the self-supporting fracture closure exhibited a two-stage characteristic of being fast in the early stage and slow in the later stage,with the inflection point stress ranging from 32 MPa to 35 MPa,and the closure degree of 47%-76%.The effective stress increase gradually rose from 5 MPa per step to 20 MPa per step,and the early fracture closure accelerated,with the maximum closure degree increasing by 8.6%.As the fracture width decreased from 500μm to 50μm,the gas-phase shifted from continuous to discontinuous flow,and the proportion of the critical gas-phase flow to maintain the continuous gas-phase flow increased.In the early stage of fracture closure(fracture width greater than 300μm),the continuous gas-phase flow is controlled by the fracture width-the larger the fracture width,the smaller the proportion of the critical gas-phase flow to maintain the continuous gas-phase flow.In the late stage of fracture closure(fracture width less than 300μm),as the fractures continue to close,the dominant role of the surface roughness of the fractures becomes stronger,and the proportion of the critical gas-phase flow to maintain the continuous gas-phase flow exceeds 70%.A reasonable pressure control during stable production and pressure reduction in the early stage(the peak pressure drop at the wellhead is less than 32 MPa)to delay the self-supporting fracture closure is conducive to the stable and increased production of gas wells.展开更多
Metals,indispensable since the Bronze Age,remain pivotal in modern technologies due to their exceptional properties and versatility.Beyond traditional machining,advanced nano/micro-machining techniques enable the fabr...Metals,indispensable since the Bronze Age,remain pivotal in modern technologies due to their exceptional properties and versatility.Beyond traditional machining,advanced nano/micro-machining techniques enable the fabrication of metallic nano/micro structures with high precision in shape,size,and pattern.These structures endow flexible electrodes with outstanding electrical,mechanical,optical,and electrochemical performance,enabling growing applications in flexible optoelectronics,epidermal electronics,energy harvesting,and biochemical sensing.This review provides a comprehensive overview of the fabrication strategies for flexible electrodes made from metal meshes,metal nanowires,and liquid metals.The current advancements,existing challenges,and emerging technologies are systematically discussed.Furthermore,the progression toward ultra-thin,soft epidermal electrodes is explored,with an emphasis on novel in situ and transfer fabrication methods.We examine the underlying mechanisms,performance indicators,and their integration for on-skin applications,including bioelectric sensing,electrical stimulation,and energy harvesting.Finally,we highlight the remaining challenges in performance improvement and industrialization of flexible and epidermal electrodes,along with future opportunities for integrating multimodal systems and leveraging artificial intelligence to enhance their functionalities.展开更多
Hydrothermal carbonization(HTC)is a promising techno-economic method for biomass waste valorization owing to its advantages over other thermochemical processes.This study focused on carbon sequestration from sugarcane...Hydrothermal carbonization(HTC)is a promising techno-economic method for biomass waste valorization owing to its advantages over other thermochemical processes.This study focused on carbon sequestration from sugarcane bioethanol distillery wastewater via HTC and chemical activation to produce activated carbon(AC).The resulting AC was then applied as an active material for supercapacitor electrodes.The introduction of redox molecules,such as 1,4-anthraquinone(AQ)and 9,10-phenanthrenequinone(PQ),on AC increased charge storage capability via redox transformation and enhanced the electrochemical performance of the supercapacitor elec-trode.Electrochemical testing showed that AC loaded with 16 wt%PQ achieved the highest specific capacitance of 488.21 F g^(-1) with remarkable capacitance retention of 95.3% after 1000 charge-discharge cycles.N-doped AC obtained from the HTC of wastewater and melamine presented a slightly enhanced specific capacitance.Various commercial LEDs with a voltage range of 1.8-3.0 V were illuminated simultaneously by connecting them to two series of symmetric supercapacitors,demonstrating the potential application of our proposed strategy in energy storage systems.This study proposes a simple and efficient strategy to utilize wastewater and achieve net-zero emission goals in a Bio-Circular-Green Economy model.展开更多
Objective:To investigate the spatial gradient of intraoperative impedance across the cochlear electrode array in pediatric cochlear implant recipients and assess its potential as a physiological indicator for the elec...Objective:To investigate the spatial gradient of intraoperative impedance across the cochlear electrode array in pediatric cochlear implant recipients and assess its potential as a physiological indicator for the electrode-neural interface.Methods:A prospective observational study involving 56 pediatric patients underwent cochlear implantation with Cochlear Nucleus devices.Intraoperative polarized impedance and electrically evoked compound action potential(ECAP)threshold were recorded across all 1232 electrodes using AutoNRT software.Eight electrodes with open-or short-circuit were excluded,leaving 1,224 for analysis.Impedance values were categorized by cochlear region(basal,middle,apical),and electrodes with elevated impedance(10-20 kΩ)were analyzed for regional distribution and clinical relevance.Data were analyzed for spatial patterns and correlation with the ECAP threshold profiles.Results:A consistent basal-to-apical increase in impedance was observed(7.7±1.9,9.2±1.4,10.8±1.5 kΩ;p<0.001).Impedance and ECAP threshold were weakly correlated(ρ=-0.20,p<0.001;β=-1.26,p<0.001),with a positive association in the apical region(ρ=0.12,p=0.048).Electrodes with higher impedance(1020 kΩ)were less likely to show elevated or absent TNRT(OR=0.175,p=0.02).The impedance gradient persisted across age groups and was significantly correlated with ECAP threshold patterns.Conclusion:Intraoperative impedance monitoring reveals a strong and physiologically consistent gradient,with higher values in apical electrodes.This gradient reflects anatomical and tissue interface variations,which may offer a valuable physiological indicator for intraoperative electrode positioning and neural interface integrity.展开更多
Thermocells are garnering increasing attention as a promising thermoelectric technology for harvesting low-grade heat.However,their performance is often limited by the scarcity of high-performance redox couples that p...Thermocells are garnering increasing attention as a promising thermoelectric technology for harvesting low-grade heat.However,their performance is often limited by the scarcity of high-performance redox couples that possess both high thermopower and rapid redox kinetics.This work addresses this challenge by leveraging our recently developed copper(Ⅰ/Ⅱ)(Cu^(+)/Cu^(2+))redox couple.We significantly enhance the performance of Cu-based liquid thermocells by integrating a thermosensitive crystallization process with etched carbon cloth electrodes,achieving synergistic improvements in thermodynamic and kinetic performance.The thermosensitive crystallization process establishes a persistent Cu^(2+)concentration gradient,boosting the thermopower from 1.47 to 2.93 mV K^(-1).Moreover,the etched carbon cloth electrodes provide a larger electroactive surface area and demonstrate a higher current density.Consequently,the optimized Cu^(+)/Cu^(2+)system achieved an exceptional normalized power density P_(max)(ΔT)^(-2)of 3.97 mW m^(-2)K^(-2).A thermocell module comprised of 20 cells directly power various electronic devices at a temperature difference of 40 K.This work successfully exhibits potential of Cu^(+)/Cu^(2+)redox couple in thermoelectric conversion and introduces a valuable redox couple for highperformance thermocells.展开更多
Aqueous hydrogen(H_(2))gas batteries with unmatched lifespan are ideal for grid-scale energy storage,yet their deployment remains limited by the lack of low-cost,efficient,and durable hydrogen electrodes.Here,we repor...Aqueous hydrogen(H_(2))gas batteries with unmatched lifespan are ideal for grid-scale energy storage,yet their deployment remains limited by the lack of low-cost,efficient,and durable hydrogen electrodes.Here,we report a high-throughput and durable gas diffusion electrode(GDE)based on a simply preparable carbon-coated nickel(Ni@C)catalyst and the design of H_(2) diffusion channels.By optimizing the carbon layer structure,a balance between the intrinsic activity and stability of the catalyst can be achieved.This Ni@C catalyst exhibits a hydrogen oxidation reaction(HOR)activity of 44 A g^(-1) as well as remarkable hydrogen evolution reaction(HER)performance.Experimental results and theoretical calculations confirm the electronic interaction between the carbon shell and Ni.In combination with a hydrophobic design,a robust and durable Ni@C-GDE has been fabricated.This electrode achieves a low HOR polarization of only 91 mV at 30 mA cm^(-2),outperforming Pt/C-GDE(154 mV),and operates stably over 4500cycles(3200 h)for HOR/HER reversing.Enabled by this electrode,a 10 Ah Ni-H_(2) battery with an energy density of 156.3 Wh kg^(-1) and cost of 62.2$kWh^(-1) is demonstrated.This work offers a viable strategy for practical and scalable hydrogen gas batteries.展开更多
Driven by the trend of device miniaturization and high-density integration,the interaction between adjacent electrodes has become a critical factor affecting the interfacial reliability of thermoelectric(TE)structures...Driven by the trend of device miniaturization and high-density integration,the interaction between adjacent electrodes has become a critical factor affecting the interfacial reliability of thermoelectric(TE)structures.This study investigates the influence of adjoining electrode interactions on the interfacial response of a multi-electrode/TE substrate structure,including interfacial stresses and stress intensity factors at the electrode ends.To solve the corresponding boundary-value problem,the Fourier transforms are adopted to derive a governing integro-differential equation for the interfacial shear stress in multi-electrode systems,incorporating the TE effects as generalized forces on the right-hand side.The results show that both the interfacial tension and transverse stress in the electrodes are significantly affected by the presence of adjacent electrodes.The interaction between neighboring electrodes diminishes as their spacing increases or when an adhesive interlayer is introduced.Furthermore,the softer and thinner electrodes,the softer and thicker adhesive interlayer,and the smaller TE loads are found to be beneficial for improving the interfacial performance.These findings may contribute to the accurate measurement in surface sensors and layout design of multi-point health monitoring systems for TE structures.展开更多
As the core determinant of lithium-ion battery performance,electrode materials play a crucial role in defining the battery's capacity,cycling stability,and durability.During charging and discharging,electrode mate...As the core determinant of lithium-ion battery performance,electrode materials play a crucial role in defining the battery's capacity,cycling stability,and durability.During charging and discharging,electrode materials undergo complex ion intercalation and deintercalation processes,accompanied by defect formation and structural evolution.However,the microscopic mechanisms underlying processes such as cation disordering,lattice oxygen loss,and stage structure formation are still not fully understood.To address these challenges,we have developed the Electrode Dynamic Ion Intercalation/Deintercalation Simulator(EDIS),a software platform designed to simulate the dynamic processes of ion intercalation and deintercalation in electrode materials.Leveraging high-precision machine learning potentials,EDIS can efficiently model structural evolution and lithium-ion diffusion behavior under various states of charge and discharge,achieving accuracy approaching that of quantum mechanical methods in relevant chemical spaces.The software supports quantitative analysis of how variations in lithium-ion concentration and distribution affect lithium-ion transport properties,enables evaluation of the impact of structural defects,and allows for tracking of both structural evolution and transport characteristics during continuous cycling.EDIS is versatile and can be extended to sodium-ion batteries and related systems.By enabling in-depth analysis of these microscopic processes,EDIS provides a robust theoretical tool for mechanistic studies and the rational design of high-performance electrode materials for next-generation lithium-ion batteries.展开更多
To enhance the electrochemical performance of lithium-ion battery anodes with higher silicon content,it is essential to engineer their microstructure for better lithium-ion transport and mitigated volume change as wel...To enhance the electrochemical performance of lithium-ion battery anodes with higher silicon content,it is essential to engineer their microstructure for better lithium-ion transport and mitigated volume change as well.Herein,we suggest an effective approach to control the micropore structure of silicon oxide(SiO_(x))/artificial graphite(AG)composite electrodes using a perforated current collector.The electrode features a unique pore structure,where alternating high-porosity domains and low-porosity domains markedly reduce overall electrode resistance,leading to a 20%improvement in rate capability at a 5C-rate discharge condition.Using microstructure-resolved modeling and simulations,we demonstrate that the patterned micropore structure enhances lithium-ion transport,mitigating the electrolyte concentration gradient of lithium-ion.Additionally,perforating current collector with a chemical etching process increases the number of hydrogen bonding sites and enlarges the interface with the SiO_(x)/AG composite electrode,significantly improving adhesion strength.This,in turn,suppresses mechanical degradation and leads to a 50%higher capacity retention.Thus,regularly arranged micropore structure enabled by the perforated current collector successfully improves both rate capability and cycle life in SiO_(x)/AG composite electrodes,providing valuable insights into electrode engineering.展开更多
Ceramic cells promise ideal energy conversion and storage devices,making the development of efficient and robust air electrodes crucial for their application.In this study,a Ba_(0.4)Sr_(0.5)Cs_(0.1)Co_(0.7)Fe_(0.2)Nb_...Ceramic cells promise ideal energy conversion and storage devices,making the development of efficient and robust air electrodes crucial for their application.In this study,a Ba_(0.4)Sr_(0.5)Cs_(0.1)Co_(0.7)Fe_(0.2)Nb_(0.1)O_(3−δ)(BSCCFN)air electrode,based on Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3−δ)(BSCF),is designed using a perovskite A-B-site ionic Lewis acid strength(ISA)polarization distribution strategy and is successfully applied in both oxygen-ion conducting solid oxide fuel cells(O-SOFCs)and proton-conducting reversible protonic ceramic cells(R-PCCs).When BSCCFN is used as the air electrode in O-SOFCs,a peak power density(PPD)of 1.45 W cm^(−2)is achieved at 650°C,whereas in R-PCCs,a PPD of 1.13 W cm^(−2)and a current density of−1.8 A cm^(−2)at 1.3 V are achieved at the same temperature and show stable reversibility over 100 h.Experimental measurements and theoretical calculations demonstrate that low-ISA Cs+doping accelerates the reaction kinetics of both oxygen ions and protons,while high-ISA Nb^(5+)doping enhances electrode stability.The synergistic effect of Cs^(+)and Nb^(5+)co-doping in the BSCCFN electrode lies in the ISA polarization distribution,which weakens the Co/Fe–O bond covalency,thereby promoting oxygen vacancy formation and facilitating the conduction of oxygen ions and protons.展开更多
Developing effective and practical electrocatalyst under industrial electrolysis conditions is critical for renewable hydrogen production.Herein,we report the self-supporting NiFe LDH-MoS_(x)integrated electrode for w...Developing effective and practical electrocatalyst under industrial electrolysis conditions is critical for renewable hydrogen production.Herein,we report the self-supporting NiFe LDH-MoS_(x)integrated electrode for water oxidation under normal alkaline test condition(1 M KOH at 25℃)and simulated industrial electrolysis conditions(5 M KOH at 65℃).Such optimized electrode exhibits excellent oxygen evolution reaction(OER)performance with overpotential of 195 and 290 mV at current density of 100 and 400 mA·cm^(-2)under normal alkaline test condition.Notably,only over-potential of 156 and 201 mV were required to achieve the current density of 100 and 400mA·cm^(-2)under simulated industrial electrolysis conditions.No significant degradations were observed after long-term durability tests for both conditions.When using in two-electrode system,the operational voltages of 1.44 and 1.72 V were required to achieve a current density of 10 and 100 mA·cm^(-2)for the overall water splitting test(NiFe LDH-MoS_(x)/INF||20%Pt/C).Additionally,the operational voltage of employing NiFe LDH-MoS_(x)/INF as both cathode and anode merely require 1.52 V at 50mA·cm^(-2)at simulated industrial electrolysis conditions.Notably,a membrane electrode assembly(MEA)for anion exchange membrane water electrolysis(AEMWEs)using NiFe LDH-MoS_(x)/INF as an anode catalyst exhibited an energy conversion efficiency of 71.8%at current density of 400 mA·cm^(-2)in 1 M KOH at 60℃.Further experimental results reveal that sulfurized substrate not only improved the conductivity of NiFe LDH,but also regulated its electronic configurations and atomic composition,leading to the excellent activity.The easy-obtained and cost-effective integrated electrodes are expected to meet the large-scale application of industrial water electrolysis.展开更多
Economical,stable,and corrosion-resistant catalytic electrodes are still urgently needed for the oxygen evolution reaction(OER)in water and seawater.Herein,a mild electroless plating strategy is used to achieve large-...Economical,stable,and corrosion-resistant catalytic electrodes are still urgently needed for the oxygen evolution reaction(OER)in water and seawater.Herein,a mild electroless plating strategy is used to achieve large-scale preparation of the“integrated”phosphorus-based precatalyst(FeP-NiP)on nickel foam(NF),which is in situ reconstructed into a highly active and corrosion-resistant(Fe)NiOOH phase for OER.The interaction between phosphate anions(PO_(x)^(y-))and iron ions(Fe^(3+))tunes the electronic structure of the catalytic phase to further enhance OER kinetics.The integrated FeP-NiP@NF electrode exhibits low overpotentials for OER in alkaline water/seawater,requiring only 275/289,320/336,and 349/358 mV to reach 0.1,0.5,and 1.0 A cm^(−2),respectively.The in situ reconstructed PO_(x)^(y-)anion electrostatically repels Cl−in seawater electrolytes,allowing stable operation for over 7 days at 1.0 A cm^(−2) in extreme electrolytes(1.0 M KOH+seawater and 6.0 M KOH+seawater),demonstrating industrial-level stability.This study overcomes the complex synthesis limitations of P-based materials through innovative material design,opening new avenues for electrochemical energy conversion.展开更多
α-MnO_(2) is a promising,inexpensive,and readily producible catalyst for the oxygen reduction reaction(ORR)in alkaline media,but its application is limited by low electronic conductivity.In this study,we enhance the ...α-MnO_(2) is a promising,inexpensive,and readily producible catalyst for the oxygen reduction reaction(ORR)in alkaline media,but its application is limited by low electronic conductivity.In this study,we enhance the performance ofα-MnO_(2) electrodes by systematically varying theα-MnO_(2)-to-Vulcan ratio within the catalyst layer.Electrodes are evaluated in a gas diffusion electrode(GDE)half-cell,where an optimized catalyst layer composition leads to significantly improved ORR performance.By finetuning both theα-MnO_(2)-to-Vulcan ratio and theα-MnO_(2) loading,the electrode outperforms a commercial MnO_(2)-based electrode and approaches the performance of the Pt/C benchmark.The improvement is attributed to the presence of a three-dimensional(3D)Vulcan network electronically connecting catalytically activeα-MnO_(2) sites with the substrate.Additionally,the optimized electrodes are employed in a prototype Al-O_(2) flow cell.Under constant oxygen flow,power densities exceed 250 mW cm^(-2),which is significantly higher than that of conventional Al-air batteries.Electrochemical impedance spectroscopy combined with distribution of relaxation times(DRT)analysis enables the separation of anode and cathode charge transfer impedances without the need for an additional reference electrode.The analysis reveals that the anode contributes more than twice as much impedance as the cathode,highlighting the need for further anode optimization.This work demonstrates a transferable approach for catalyst layer screening under technically relevant conditions in the GDE half-cell.Subsequent measurements in an Al-O_(2) flow cell validate the approach.The methodology is widely applicable to the development of advanced electrodes for a variety of metal-air battery technologies.展开更多
Flexible carbon fiber cloth(CFC)is an important scaffold and/or current collector for active materials in the development of flexible self-supportive electrode materials(SSEMs),especially in lithium-ion batteries.Howe...Flexible carbon fiber cloth(CFC)is an important scaffold and/or current collector for active materials in the development of flexible self-supportive electrode materials(SSEMs),especially in lithium-ion batteries.However,during the intercalation of Li ions into the matrix of CFC(below 0.5 V vs.Li/Li+),the incompatibility in the capacity of the CFC,when used directly as an anode material or as a current collector for active materials,leads to difficulty in the estimation of its actual contribution.To address this issue,we prepared Ni_(5)P_(4)nanosheets on CFC(denoted CFC@Ni_(5)P_(4))and investigated the contribution of CFC in the CFC@Ni_(5)P_(4)by comparing to the powder Ni_(5)P_(4)nanosheets traditionally coated on a copper foil(CuF)(denoted P-Ni_(5)P_(4)).At a current density of 0.4 mA cm^(−2),the as-prepared CFC@Ni_(5)P_(4)showed an areal capacity of 7.38 mAh cm^(−2),which is significantly higher than that of the PNi_(5)P_(4)electrode.More importantly,theoretical studies revealed that the CFC has a high Li adsorption energy that contributes to the low Li-ion diffusion energy barrier of the Ni_(5)P_(4)due to the strong interaction between the CFC and Ni_(5)P_(4),leading to the superior Li-ion storage performance of the CFC@Ni_(5)P_(4)over the pristine Ni_(5)P_(4)sample.This present work unveils the underlying mechanism leading to the achievement of high performance in SSEMs.展开更多
High-entropy materials represent a new category of high-performance materials,first proposed in 2004 and extensively investigated by researchers over the past two decades.The definition of high-entropy materials has c...High-entropy materials represent a new category of high-performance materials,first proposed in 2004 and extensively investigated by researchers over the past two decades.The definition of high-entropy materials has continuously evolved.In the last ten years,the discovery of an increasing number of high-entropy materials has led to significant advancements in their utilization in energy storage,electrocatalysis,and related domains,accompanied by a rise in techniques for fabricating high-entropy electrode materials.Recently,the research emphasis has shifted from solely improving the performance of high-entropy materials toward exploring their reaction mechanisms and adopting cleaner preparation approaches.However,the current definition of high-entropy materials remains relatively vague,and the preparation method of high-entropy materials is based on the preparation method of single metal/low-or medium-entropy materials.It should be noted that not all methods applicable to single metal/low-or medium-entropy materials can be directly applied to high-entropy materials.In this review,the definition and development of high-entropy materials are briefly reviewed.Subsequently,the classification of high-entropy electrode materials is presented,followed by a discussion of their applications in energy storage and catalysis from the perspective of synthesis methods.Finally,an evaluation of the advantages and disadvantages of various synthesis methods in the production process of different high-entropy materials is provided,along with a proposal for potential future development directions for high-entropy materials.展开更多
基金supported by the Natural Sci-ence Foundation of Xinjiang Uygur Autonomous Region(Nos.2022D01E36 and 2022D01E38)the National Natural Science Foun-dation of China(Nos.22369016 and 22065034)the Outstand-ing Doctoral Student Innovation Project of Xinjiang University(No.XJU2024BS055).
文摘A flexible air electrode with excellent activity and stability is essential for flexible zinc-air batteries.In this study,we report the rational design of nitrogen-doped carbon nanotube-encapsulated Co9S8 nanopar-ticles on carbon cloth(Co9S8/NCNTs/CC),serving as self-supporting air electrodes for both liquid-state and flexible zinc-air batteries.The Co9S8/NCNTs/CC-1 exhibited a half-wave potential of 0.86 V for oxygen re-duction reaction(ORR)and achieved a current density of 10 mA cm-2 for oxygen evolution reaction(OER)at a voltage of only 1.52 V.The well-constructed nanotube on carbon cloth facilitates mass diffu-sion and electron transfer,while enhancing the mechanical flexibility of the material.Density functional theory(DFT)calculations suggested that the synergistic interaction between Co9S8 and NCNTs effectively enhanced the bifunctional electrocatalytic performance of the material.Liquid-state and flexible zinc-air batteries assembled with Co9S8/NCNTs/CC-1 demonstrated outstanding charge-discharge capabilities and long-term stability.
基金supported by the Natural Science Research Project of Jiangsu Higher Education Institutions(No.23KJD150005)the Scientific Research Project of Nanjing Xiaozhuang University(No.2022NXY29).
文摘Developing efficient and stable electrocatalysts has always been the focus of electrochemical research.Here,sea urchin-like nickel-molybdenum bimetallic phosphide nickel-molybdenum alloy(Ni_(4)Mo)and(Ni-Mo-P)were successfully synthesized by hydrothermal,annealing and phosphating methods on nickel foam(NF).The unusual shape of the sea urchin facilitates gas release and mass transfer and increases the interaction between catalysts and electrolytes.The Ni_(4)Mo/NF and Ni-Mo-P/NF electrodes only need overpotentials of 72 and 197 mV to reach 50 mA·cm^(−2) under alkaline conditions for hydrogen evolution reaction and oxygen evolution reaction,respectively.The Ni_(4)Mo/NF and Ni-Mo-P/NF asymmetric electrodes were used as anode and cathode for the overall water splitting,respectively.In 1.0 M KOH,at a voltage of 1.485 V,the electrolytic device generated 50 mA·cm^(−2) current density,maintaining for 24 h without reduction.The labor presents a simple method to synthesize a highly active,low-cost,and strongly durable self-supporting electrode for over-water splitting.
基金financial support of the National Natural Science Foundation of China(NSFC)(22372039 and 22305247)the Natural Science Foundation of Fujian Province of China(2021J06010)the Fuzhou University Testing Fund of Precious Apparatus(2025T022)。
文摘Transition metal-based electrocatalysts are a promising alternative to noble metal catalysts for electrochemical upgrading of biomass-derived 5-hydroxymethylfurfural(HMF)into high-value 2,5-furandicarboxylic acid(FDCA).However,the rational design of efficient electrocatalysts with precisely tailored structure-activity correlations remains a critical challenge.Herein,we report a hierarchically structured self-supporting electrode(Vo-NiCo(OH)_(2)-NF)synthesized through in situ electrochemical reconstruction of NiCo-Prussian blue analogue(NiCo-PBA)precursor,in which oxygen vacancy(Vo)-rich Co-doped Ni(OH)_(2)nanosheet arrays are vertically aligned on nickel foam(NF),creating an interconnected conductive network.When evaluated for the HMF oxidation reaction(HMFOR),Vo-NiCo(OH)_(2)-NF exhibits exceptional electrochemical performance,achieving near-complete HMF conversion(99%),ultrahigh FDCA Faradaic efficiency(97.5%),and remarkable product yield(96.2%)at 1.45 V,outperforming conventional Co-doped Ni(OH)_(2)(NiCo(OH)_(2)-NF)and pristine Ni(OH)_(2)(Ni(OH)_(2)-NF)electrodes.By combining in situ spectroscopic characterization and theoretical calculations,we elucidate that the synergistic effects of Co-doping and oxygen vacancy engineering effectively modulate the electronic structure of Ni active centers,favor the formation of high-valent Ni^(3+)species,and optimize HMF adsorption,thereby improving the HMFOR performance.This work provides valuable mechanistic insights for catalyst design and may inspire the development of advanced transition metal-based electrodes for efficient biomass conversion systems.
基金supported by the University of Seoul’s 2025 Research Fund.
文摘Vanadium redox flow batteries(VRFBs)are a means of large-scale energy storage due to their excellent scalability,safety,long cycling life,and decoupled power and energy capacities.However,the slow redox kinetics of vanadium species on conventional carbon electrodes remains a major limitation to their performance.We investigated the deposition of carbon black,carbon nanotubes,and electrochemically exfoliated graphene(Exf-Gr)onto thermally-activated carbon paper(ACP)by spray coating to increase the electrode electrocatalytic activity.The modified electrodes were characterized using scanning electron microscopy,X-ray diffraction,Raman spectroscopy,X-ray photoelectron microscopy,and surface area analysis,while their electrochemical properties were evaluated by cyclic voltammetry,electrochemical impedance spectroscopy,and singlecell VRFB testing.Among the modified electrodes,Exf-Gr/ACP had the best performance,achieving a 2.9-fold reduction in charge transfer resistance compared to pristine ACP and delivering 2.5 times the discharge capacity in single-cell tests.This improvement is attributed to Exf-Gr’s high surface area,favorable catalytic activity,and excellent dispersion on the ACP substrate.Surface modification with electrochemically exfoliated graphene is a highly effective strategy for improving the electrode performance in VRFB systems,with significant implications for large-scale energy storage.
基金financial support from the National Natural Science Foundation of China(52473248,52203123,52125301,22279070 and U21A20170)the State Key Laboratory of Polymer Materials Engineering(Grant No:sklpme 2023-1-05 and sklpme 2024-2-04)+3 种基金the Ministry of Science and Technology of China(No.2019YFA0705703)the Sichuan Science and Technology Program(2023NSFSC0991 and 2025ZNSFSC1411)the Fundamental Research Funds for the Central Universitiespartially sponsored by the Double First-Class Construction Funds of Sichuan University.
文摘The development of shape-customizable and bulk flexible electrochemical devices through processing technologies as versatile as those used for plastics promises to revolutionize the future of battery technology.However,this pursuit has been fundamentally hindered by the absence of transformative battery materials capable of delivering the necessary electrochemical functions,robust interface adhesion,and,crucially,the suitable rheological properties required for on-demand shaping.In this work,we introduce a concept of a multifunctional plasticine electrode matrix(PEM)featuring nano-interpenetrating networks(nano-IPN)to address this challenge.Utilizing the nonflammable liquid-electrolyte hydration combined with conductive nanomaterials,we have realized a PEM in the form of a multifunctional nanocomposite that integrates ion and electron conduction,component binding,non-flammability,and plasticine-like moldability.With this PEM,we have successfully fabricated a variety of bulk-flexible electrodes with high mass loading of active material(AM)(>70 wt%)using industry-friendly extrusion and compression molding techniques.Moreover,these high AM-loading composite electrodes achieve an unparalleled bulk conformability and flexibility,remaining structurally intact even under severe mechanical stress.Ultimately,we have successfully produced shape-patternable and flexible batteries via extrusion molding.This study underscores the potential of the PEM to revolutionize battery microstructures,interfaces,manufacturing processes,and performance characteristics.
基金Supported by the National Science and Technology Major Project of New-Type Oil and Gas Exploration and Development(2025ZD14041)National Science and Technology Major Project of China(2025ZD14053)+2 种基金Science and Technology Project of CNPC(2023ZZ21)Youth Science and Technology Project of CNPC(2024DQ03241)Postdoctoral Research Project of PetroChina Southwest Oil and Gas Field Company(20230304-13)。
文摘Taking the underground shale of the Silurian Longmaxi Formation in southern Sichuan Basin as the research object,stress-sensitive experiments on self-supporting fractures and micro-visualization experiments on gas-water flow were conducted under simulated reservoir conditions to study the mechanism of microscopic gas-water flow during the fracture closure process and discuss its engineering applications.The results show that as the effective stress gradually increased from 5 MPa to 60 MPa with an increment of 5 MPa per step,the self-supporting fracture closure exhibited a two-stage characteristic of being fast in the early stage and slow in the later stage,with the inflection point stress ranging from 32 MPa to 35 MPa,and the closure degree of 47%-76%.The effective stress increase gradually rose from 5 MPa per step to 20 MPa per step,and the early fracture closure accelerated,with the maximum closure degree increasing by 8.6%.As the fracture width decreased from 500μm to 50μm,the gas-phase shifted from continuous to discontinuous flow,and the proportion of the critical gas-phase flow to maintain the continuous gas-phase flow increased.In the early stage of fracture closure(fracture width greater than 300μm),the continuous gas-phase flow is controlled by the fracture width-the larger the fracture width,the smaller the proportion of the critical gas-phase flow to maintain the continuous gas-phase flow.In the late stage of fracture closure(fracture width less than 300μm),as the fractures continue to close,the dominant role of the surface roughness of the fractures becomes stronger,and the proportion of the critical gas-phase flow to maintain the continuous gas-phase flow exceeds 70%.A reasonable pressure control during stable production and pressure reduction in the early stage(the peak pressure drop at the wellhead is less than 32 MPa)to delay the self-supporting fracture closure is conducive to the stable and increased production of gas wells.
基金supported by the Basic and Applied Basic Research Foundation of Guangdong province(2024A1515030155 and 2022A1515010272)Natural Science Foundation of China(61904067)+2 种基金Basic and Applied Basic Research Foundation of Guangzhou city(202102020758)Open funding from State Key Laboratory of Optoelectronic Materials and Technologies(Sun Yat-Sen University,OEMT2022-KF-08)Fundamental Research Funds for the Central Universities(11625109,11621405)。
文摘Metals,indispensable since the Bronze Age,remain pivotal in modern technologies due to their exceptional properties and versatility.Beyond traditional machining,advanced nano/micro-machining techniques enable the fabrication of metallic nano/micro structures with high precision in shape,size,and pattern.These structures endow flexible electrodes with outstanding electrical,mechanical,optical,and electrochemical performance,enabling growing applications in flexible optoelectronics,epidermal electronics,energy harvesting,and biochemical sensing.This review provides a comprehensive overview of the fabrication strategies for flexible electrodes made from metal meshes,metal nanowires,and liquid metals.The current advancements,existing challenges,and emerging technologies are systematically discussed.Furthermore,the progression toward ultra-thin,soft epidermal electrodes is explored,with an emphasis on novel in situ and transfer fabrication methods.We examine the underlying mechanisms,performance indicators,and their integration for on-skin applications,including bioelectric sensing,electrical stimulation,and energy harvesting.Finally,we highlight the remaining challenges in performance improvement and industrialization of flexible and epidermal electrodes,along with future opportunities for integrating multimodal systems and leveraging artificial intelligence to enhance their functionalities.
基金supported by Thailand Science Research and Inno-vation(TSRI)Fundamental Fund,fiscal year 2024(TUFF14/2567)by the Research Unit in Bioenergy and Catalysis(Thammasat University)+2 种基金partially supported by Thailand Science Research and Innovation(TSRI)under Project No.180677funded by Hub Talent:Sustainable Materials for Circular Economy,National Research Council of Thailand(NRCT)supported by Synchrotron Light Research Institute(SLRI:Beamline 3.2b).
文摘Hydrothermal carbonization(HTC)is a promising techno-economic method for biomass waste valorization owing to its advantages over other thermochemical processes.This study focused on carbon sequestration from sugarcane bioethanol distillery wastewater via HTC and chemical activation to produce activated carbon(AC).The resulting AC was then applied as an active material for supercapacitor electrodes.The introduction of redox molecules,such as 1,4-anthraquinone(AQ)and 9,10-phenanthrenequinone(PQ),on AC increased charge storage capability via redox transformation and enhanced the electrochemical performance of the supercapacitor elec-trode.Electrochemical testing showed that AC loaded with 16 wt%PQ achieved the highest specific capacitance of 488.21 F g^(-1) with remarkable capacitance retention of 95.3% after 1000 charge-discharge cycles.N-doped AC obtained from the HTC of wastewater and melamine presented a slightly enhanced specific capacitance.Various commercial LEDs with a voltage range of 1.8-3.0 V were illuminated simultaneously by connecting them to two series of symmetric supercapacitors,demonstrating the potential application of our proposed strategy in energy storage systems.This study proposes a simple and efficient strategy to utilize wastewater and achieve net-zero emission goals in a Bio-Circular-Green Economy model.
文摘Objective:To investigate the spatial gradient of intraoperative impedance across the cochlear electrode array in pediatric cochlear implant recipients and assess its potential as a physiological indicator for the electrode-neural interface.Methods:A prospective observational study involving 56 pediatric patients underwent cochlear implantation with Cochlear Nucleus devices.Intraoperative polarized impedance and electrically evoked compound action potential(ECAP)threshold were recorded across all 1232 electrodes using AutoNRT software.Eight electrodes with open-or short-circuit were excluded,leaving 1,224 for analysis.Impedance values were categorized by cochlear region(basal,middle,apical),and electrodes with elevated impedance(10-20 kΩ)were analyzed for regional distribution and clinical relevance.Data were analyzed for spatial patterns and correlation with the ECAP threshold profiles.Results:A consistent basal-to-apical increase in impedance was observed(7.7±1.9,9.2±1.4,10.8±1.5 kΩ;p<0.001).Impedance and ECAP threshold were weakly correlated(ρ=-0.20,p<0.001;β=-1.26,p<0.001),with a positive association in the apical region(ρ=0.12,p=0.048).Electrodes with higher impedance(1020 kΩ)were less likely to show elevated or absent TNRT(OR=0.175,p=0.02).The impedance gradient persisted across age groups and was significantly correlated with ECAP threshold patterns.Conclusion:Intraoperative impedance monitoring reveals a strong and physiologically consistent gradient,with higher values in apical electrodes.This gradient reflects anatomical and tissue interface variations,which may offer a valuable physiological indicator for intraoperative electrode positioning and neural interface integrity.
基金financially supported by research grants from Innovative Research Group Project of National Natural Science Foundation of China(52021004)the National Key Research and Development Program of China(2022YFB3803300)+1 种基金the National Natural Science Foundation of China(62474026,62205140,12204071)the China Postdoctoral Science Foundation(2022M710532)。
文摘Thermocells are garnering increasing attention as a promising thermoelectric technology for harvesting low-grade heat.However,their performance is often limited by the scarcity of high-performance redox couples that possess both high thermopower and rapid redox kinetics.This work addresses this challenge by leveraging our recently developed copper(Ⅰ/Ⅱ)(Cu^(+)/Cu^(2+))redox couple.We significantly enhance the performance of Cu-based liquid thermocells by integrating a thermosensitive crystallization process with etched carbon cloth electrodes,achieving synergistic improvements in thermodynamic and kinetic performance.The thermosensitive crystallization process establishes a persistent Cu^(2+)concentration gradient,boosting the thermopower from 1.47 to 2.93 mV K^(-1).Moreover,the etched carbon cloth electrodes provide a larger electroactive surface area and demonstrate a higher current density.Consequently,the optimized Cu^(+)/Cu^(2+)system achieved an exceptional normalized power density P_(max)(ΔT)^(-2)of 3.97 mW m^(-2)K^(-2).A thermocell module comprised of 20 cells directly power various electronic devices at a temperature difference of 40 K.This work successfully exhibits potential of Cu^(+)/Cu^(2+)redox couple in thermoelectric conversion and introduces a valuable redox couple for highperformance thermocells.
基金financially supported by the“National Natural Science Foundation of China”(No.22279082)the“Natural Science Foundation of Sichuan”(2025YFHZ0056)。
文摘Aqueous hydrogen(H_(2))gas batteries with unmatched lifespan are ideal for grid-scale energy storage,yet their deployment remains limited by the lack of low-cost,efficient,and durable hydrogen electrodes.Here,we report a high-throughput and durable gas diffusion electrode(GDE)based on a simply preparable carbon-coated nickel(Ni@C)catalyst and the design of H_(2) diffusion channels.By optimizing the carbon layer structure,a balance between the intrinsic activity and stability of the catalyst can be achieved.This Ni@C catalyst exhibits a hydrogen oxidation reaction(HOR)activity of 44 A g^(-1) as well as remarkable hydrogen evolution reaction(HER)performance.Experimental results and theoretical calculations confirm the electronic interaction between the carbon shell and Ni.In combination with a hydrophobic design,a robust and durable Ni@C-GDE has been fabricated.This electrode achieves a low HOR polarization of only 91 mV at 30 mA cm^(-2),outperforming Pt/C-GDE(154 mV),and operates stably over 4500cycles(3200 h)for HOR/HER reversing.Enabled by this electrode,a 10 Ah Ni-H_(2) battery with an energy density of 156.3 Wh kg^(-1) and cost of 62.2$kWh^(-1) is demonstrated.This work offers a viable strategy for practical and scalable hydrogen gas batteries.
基金Project supported by the National Natural Science Foundation of China(Nos.12502117,12272269,11972257)the Natural Science Foundation of Ningxia of China(No.2024AAC03018)+1 种基金the Fundamental Research Funds for the Central Universitiesthe Shanghai Gaofeng Project for University Academic Program Development。
文摘Driven by the trend of device miniaturization and high-density integration,the interaction between adjacent electrodes has become a critical factor affecting the interfacial reliability of thermoelectric(TE)structures.This study investigates the influence of adjoining electrode interactions on the interfacial response of a multi-electrode/TE substrate structure,including interfacial stresses and stress intensity factors at the electrode ends.To solve the corresponding boundary-value problem,the Fourier transforms are adopted to derive a governing integro-differential equation for the interfacial shear stress in multi-electrode systems,incorporating the TE effects as generalized forces on the right-hand side.The results show that both the interfacial tension and transverse stress in the electrodes are significantly affected by the presence of adjacent electrodes.The interaction between neighboring electrodes diminishes as their spacing increases or when an adhesive interlayer is introduced.Furthermore,the softer and thinner electrodes,the softer and thicker adhesive interlayer,and the smaller TE loads are found to be beneficial for improving the interfacial performance.These findings may contribute to the accurate measurement in surface sensors and layout design of multi-point health monitoring systems for TE structures.
基金supported by the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB1040300)the National Natural Science Foundation of China(Grant No.52172258)。
文摘As the core determinant of lithium-ion battery performance,electrode materials play a crucial role in defining the battery's capacity,cycling stability,and durability.During charging and discharging,electrode materials undergo complex ion intercalation and deintercalation processes,accompanied by defect formation and structural evolution.However,the microscopic mechanisms underlying processes such as cation disordering,lattice oxygen loss,and stage structure formation are still not fully understood.To address these challenges,we have developed the Electrode Dynamic Ion Intercalation/Deintercalation Simulator(EDIS),a software platform designed to simulate the dynamic processes of ion intercalation and deintercalation in electrode materials.Leveraging high-precision machine learning potentials,EDIS can efficiently model structural evolution and lithium-ion diffusion behavior under various states of charge and discharge,achieving accuracy approaching that of quantum mechanical methods in relevant chemical spaces.The software supports quantitative analysis of how variations in lithium-ion concentration and distribution affect lithium-ion transport properties,enables evaluation of the impact of structural defects,and allows for tracking of both structural evolution and transport characteristics during continuous cycling.EDIS is versatile and can be extended to sodium-ion batteries and related systems.By enabling in-depth analysis of these microscopic processes,EDIS provides a robust theoretical tool for mechanistic studies and the rational design of high-performance electrode materials for next-generation lithium-ion batteries.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(No.NRF-2021M3H4A1A02048529)the Ministry of Trade,Industry and Energy(MOTIE)of the Korean government under grant No.RS-2022-00155854support from the DGIST Supercomputing and Big Data Center.
文摘To enhance the electrochemical performance of lithium-ion battery anodes with higher silicon content,it is essential to engineer their microstructure for better lithium-ion transport and mitigated volume change as well.Herein,we suggest an effective approach to control the micropore structure of silicon oxide(SiO_(x))/artificial graphite(AG)composite electrodes using a perforated current collector.The electrode features a unique pore structure,where alternating high-porosity domains and low-porosity domains markedly reduce overall electrode resistance,leading to a 20%improvement in rate capability at a 5C-rate discharge condition.Using microstructure-resolved modeling and simulations,we demonstrate that the patterned micropore structure enhances lithium-ion transport,mitigating the electrolyte concentration gradient of lithium-ion.Additionally,perforating current collector with a chemical etching process increases the number of hydrogen bonding sites and enlarges the interface with the SiO_(x)/AG composite electrode,significantly improving adhesion strength.This,in turn,suppresses mechanical degradation and leads to a 50%higher capacity retention.Thus,regularly arranged micropore structure enabled by the perforated current collector successfully improves both rate capability and cycle life in SiO_(x)/AG composite electrodes,providing valuable insights into electrode engineering.
基金funding from the National Natural Science Foundation of China (Award 91745203) supplemented by Central Universities’ Basic Research Funds.
文摘Ceramic cells promise ideal energy conversion and storage devices,making the development of efficient and robust air electrodes crucial for their application.In this study,a Ba_(0.4)Sr_(0.5)Cs_(0.1)Co_(0.7)Fe_(0.2)Nb_(0.1)O_(3−δ)(BSCCFN)air electrode,based on Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3−δ)(BSCF),is designed using a perovskite A-B-site ionic Lewis acid strength(ISA)polarization distribution strategy and is successfully applied in both oxygen-ion conducting solid oxide fuel cells(O-SOFCs)and proton-conducting reversible protonic ceramic cells(R-PCCs).When BSCCFN is used as the air electrode in O-SOFCs,a peak power density(PPD)of 1.45 W cm^(−2)is achieved at 650°C,whereas in R-PCCs,a PPD of 1.13 W cm^(−2)and a current density of−1.8 A cm^(−2)at 1.3 V are achieved at the same temperature and show stable reversibility over 100 h.Experimental measurements and theoretical calculations demonstrate that low-ISA Cs+doping accelerates the reaction kinetics of both oxygen ions and protons,while high-ISA Nb^(5+)doping enhances electrode stability.The synergistic effect of Cs^(+)and Nb^(5+)co-doping in the BSCCFN electrode lies in the ISA polarization distribution,which weakens the Co/Fe–O bond covalency,thereby promoting oxygen vacancy formation and facilitating the conduction of oxygen ions and protons.
文摘Developing effective and practical electrocatalyst under industrial electrolysis conditions is critical for renewable hydrogen production.Herein,we report the self-supporting NiFe LDH-MoS_(x)integrated electrode for water oxidation under normal alkaline test condition(1 M KOH at 25℃)and simulated industrial electrolysis conditions(5 M KOH at 65℃).Such optimized electrode exhibits excellent oxygen evolution reaction(OER)performance with overpotential of 195 and 290 mV at current density of 100 and 400 mA·cm^(-2)under normal alkaline test condition.Notably,only over-potential of 156 and 201 mV were required to achieve the current density of 100 and 400mA·cm^(-2)under simulated industrial electrolysis conditions.No significant degradations were observed after long-term durability tests for both conditions.When using in two-electrode system,the operational voltages of 1.44 and 1.72 V were required to achieve a current density of 10 and 100 mA·cm^(-2)for the overall water splitting test(NiFe LDH-MoS_(x)/INF||20%Pt/C).Additionally,the operational voltage of employing NiFe LDH-MoS_(x)/INF as both cathode and anode merely require 1.52 V at 50mA·cm^(-2)at simulated industrial electrolysis conditions.Notably,a membrane electrode assembly(MEA)for anion exchange membrane water electrolysis(AEMWEs)using NiFe LDH-MoS_(x)/INF as an anode catalyst exhibited an energy conversion efficiency of 71.8%at current density of 400 mA·cm^(-2)in 1 M KOH at 60℃.Further experimental results reveal that sulfurized substrate not only improved the conductivity of NiFe LDH,but also regulated its electronic configurations and atomic composition,leading to the excellent activity.The easy-obtained and cost-effective integrated electrodes are expected to meet the large-scale application of industrial water electrolysis.
基金funding support from Natural Science Foundation of Shanghai(Grant No.23ZR1443900)the National Natural Science Foundation of China(Grant Nos.22178309,22476131 and 22176127)。
文摘Economical,stable,and corrosion-resistant catalytic electrodes are still urgently needed for the oxygen evolution reaction(OER)in water and seawater.Herein,a mild electroless plating strategy is used to achieve large-scale preparation of the“integrated”phosphorus-based precatalyst(FeP-NiP)on nickel foam(NF),which is in situ reconstructed into a highly active and corrosion-resistant(Fe)NiOOH phase for OER.The interaction between phosphate anions(PO_(x)^(y-))and iron ions(Fe^(3+))tunes the electronic structure of the catalytic phase to further enhance OER kinetics.The integrated FeP-NiP@NF electrode exhibits low overpotentials for OER in alkaline water/seawater,requiring only 275/289,320/336,and 349/358 mV to reach 0.1,0.5,and 1.0 A cm^(−2),respectively.The in situ reconstructed PO_(x)^(y-)anion electrostatically repels Cl−in seawater electrolytes,allowing stable operation for over 7 days at 1.0 A cm^(−2) in extreme electrolytes(1.0 M KOH+seawater and 6.0 M KOH+seawater),demonstrating industrial-level stability.This study overcomes the complex synthesis limitations of P-based materials through innovative material design,opening new avenues for electrochemical energy conversion.
基金part of the ALU-STORE project(Aluminum Metal as Energy Carrier for Seasonal Energy Storage)funded by the KIT Future Fieldsthe research performed at CELEST(Center for Electrochemical Energy Storage Ulm-Karlsruhe)+1 种基金funding from the German Federal Ministry of Research,Technology and Space(BMFTR)in the Nano Mat Futur program(03XP0423)basic funding from the Helmholtz Association。
文摘α-MnO_(2) is a promising,inexpensive,and readily producible catalyst for the oxygen reduction reaction(ORR)in alkaline media,but its application is limited by low electronic conductivity.In this study,we enhance the performance ofα-MnO_(2) electrodes by systematically varying theα-MnO_(2)-to-Vulcan ratio within the catalyst layer.Electrodes are evaluated in a gas diffusion electrode(GDE)half-cell,where an optimized catalyst layer composition leads to significantly improved ORR performance.By finetuning both theα-MnO_(2)-to-Vulcan ratio and theα-MnO_(2) loading,the electrode outperforms a commercial MnO_(2)-based electrode and approaches the performance of the Pt/C benchmark.The improvement is attributed to the presence of a three-dimensional(3D)Vulcan network electronically connecting catalytically activeα-MnO_(2) sites with the substrate.Additionally,the optimized electrodes are employed in a prototype Al-O_(2) flow cell.Under constant oxygen flow,power densities exceed 250 mW cm^(-2),which is significantly higher than that of conventional Al-air batteries.Electrochemical impedance spectroscopy combined with distribution of relaxation times(DRT)analysis enables the separation of anode and cathode charge transfer impedances without the need for an additional reference electrode.The analysis reveals that the anode contributes more than twice as much impedance as the cathode,highlighting the need for further anode optimization.This work demonstrates a transferable approach for catalyst layer screening under technically relevant conditions in the GDE half-cell.Subsequent measurements in an Al-O_(2) flow cell validate the approach.The methodology is widely applicable to the development of advanced electrodes for a variety of metal-air battery technologies.
基金National Natural Science Foundation of China,Grant/Award Numbers:21875292,21902188National Key Research and Development Program of China,Grant/Award Number:2019YFA0705702+2 种基金Hunan Provincial Natural Science Foundation,Grant/Award Number:2021JJ30087Natural Science Foundation of Guangdong Province,Grant/Award Number:2020A1515010798Hunan Joint International Laboratory of Advanced Materials and Technology for Clean Energy,Grant/Award Number:2020CB1007。
文摘Flexible carbon fiber cloth(CFC)is an important scaffold and/or current collector for active materials in the development of flexible self-supportive electrode materials(SSEMs),especially in lithium-ion batteries.However,during the intercalation of Li ions into the matrix of CFC(below 0.5 V vs.Li/Li+),the incompatibility in the capacity of the CFC,when used directly as an anode material or as a current collector for active materials,leads to difficulty in the estimation of its actual contribution.To address this issue,we prepared Ni_(5)P_(4)nanosheets on CFC(denoted CFC@Ni_(5)P_(4))and investigated the contribution of CFC in the CFC@Ni_(5)P_(4)by comparing to the powder Ni_(5)P_(4)nanosheets traditionally coated on a copper foil(CuF)(denoted P-Ni_(5)P_(4)).At a current density of 0.4 mA cm^(−2),the as-prepared CFC@Ni_(5)P_(4)showed an areal capacity of 7.38 mAh cm^(−2),which is significantly higher than that of the PNi_(5)P_(4)electrode.More importantly,theoretical studies revealed that the CFC has a high Li adsorption energy that contributes to the low Li-ion diffusion energy barrier of the Ni_(5)P_(4)due to the strong interaction between the CFC and Ni_(5)P_(4),leading to the superior Li-ion storage performance of the CFC@Ni_(5)P_(4)over the pristine Ni_(5)P_(4)sample.This present work unveils the underlying mechanism leading to the achievement of high performance in SSEMs.
基金supported by the National Natural Science Foundation of China(22378431,52004338,51622406,21673298)Hunan Provincial Natural Science Foundation(2023JJ40210,2022JJ20075)+3 种基金the Science and Technology Innovation Program of Hunan Province(2023RC3259)the Key R&D plan of Hunan Province(2024JK2096)Scientifc Research Fund of Hunan Provincial Education Department(23B0699)Central South University Innovation-Driven Research Programme(2023CXQD008).
文摘High-entropy materials represent a new category of high-performance materials,first proposed in 2004 and extensively investigated by researchers over the past two decades.The definition of high-entropy materials has continuously evolved.In the last ten years,the discovery of an increasing number of high-entropy materials has led to significant advancements in their utilization in energy storage,electrocatalysis,and related domains,accompanied by a rise in techniques for fabricating high-entropy electrode materials.Recently,the research emphasis has shifted from solely improving the performance of high-entropy materials toward exploring their reaction mechanisms and adopting cleaner preparation approaches.However,the current definition of high-entropy materials remains relatively vague,and the preparation method of high-entropy materials is based on the preparation method of single metal/low-or medium-entropy materials.It should be noted that not all methods applicable to single metal/low-or medium-entropy materials can be directly applied to high-entropy materials.In this review,the definition and development of high-entropy materials are briefly reviewed.Subsequently,the classification of high-entropy electrode materials is presented,followed by a discussion of their applications in energy storage and catalysis from the perspective of synthesis methods.Finally,an evaluation of the advantages and disadvantages of various synthesis methods in the production process of different high-entropy materials is provided,along with a proposal for potential future development directions for high-entropy materials.
