In this paper a pH microprobe technique was developed to measure in-situ the pH value at the electrode/solution interface. Iridium oxide was used as a pH sensitive material with good response behavior in the measured ...In this paper a pH microprobe technique was developed to measure in-situ the pH value at the electrode/solution interface. Iridium oxide was used as a pH sensitive material with good response behavior in the measured solutions. The experimental results indicated that the interfacial pH increased with the applied potential, first jumped to a maximum, then slowly decreased at the controlled potential during the electrodeposition process of functional ceramics.展开更多
Fully implanted brain-computer interfaces(BCIs)are preferred as they eliminate signal degradation caused by interference and absorption in external tissues,a common issue in non-fully implanted systems.To optimize the...Fully implanted brain-computer interfaces(BCIs)are preferred as they eliminate signal degradation caused by interference and absorption in external tissues,a common issue in non-fully implanted systems.To optimize the design of electroencephalography electrodes in fully implanted BCI systems,this study investigates the penetration and absorption characteristics of microwave signals in human brain tissue at different frequencies.Electromagnetic simulations are used to analyze the power density distribution and specific absorption rate(SAR)of signals at various frequen-cies.The results indicate that lower-frequency signals offer advantages in terms of power density and attenuation coeffi-cients.However,SAR-normalized analysis,which considers both power density and electromagnetic radiation hazards,shows that higher-frequency signals perform better at superficial to intermediate depths.Specifically,at a depth of 2 mm beneath the cortex,the power density of a 6.5 GHz signal is 247.83%higher than that of a 0.4 GHz signal.At a depth of 5 mm,the power density of a 3.5 GHz signal exceeds that of a 0.4 GHz signal by 224.16%.The findings suggest that 6.5 GHz is optimal for electrodes at a depth of 2 mm,3.5 GHz for 5 mm,2.45 GHz for depths of 15-20 mm,and 1.8 GHz for 25 mm.展开更多
Electron transfer processes at polymer electrolyte/electrode interfaces play a central role in modern electrochemical devices of energy conversion,however,current understanding of electron transfers through electroche...Electron transfer processes at polymer electrolyte/electrode interfaces play a central role in modern electrochemical devices of energy conversion,however,current understanding of electron transfers through electrochemical interfaces was established exclusively based on the studies of liquid/solid electrochemical interfaces.Thus,similarities and differences of liquid and polymer electrolyte/electrode interfaces need to be mapped out to guide the design of device level electrochemical interfaces.In this work,we employ the sulfonate adsorption/desorption as a probe reaction to understand the electron-transfer steps in polymer and liquid electrolytes.Through cyclic voltametric investigations on the well-define single-crystal Pd_(ML)Pt(111)electrode,we demonstrate that the oxidative adsorption and reductive desorption of sulfonates at the polymer electrolyte/electrode interface are chemically distinct from those in liquid electrolytes,with the former occurring mostly via the proton-coupled pathway while the latter proceeding mainly through the solvation-mediated pathway.Importantly,the sulfonate adsorption/desorption behaviors of alkylsulfonates become increasingly similar to those in Nafion with longer alkyl chains,suggesting that the interfacial hydrophobicity and solvation environment conferred by the perfluorinated polymer play a decisive role in the electron-transfer mechanism.Results reported in this study highlight the mechanistic distinctions between electron-transfer processes at electrochemical interfaces involving polymer and liquid electrolytes,and provide a framework for understanding electron-transfer processes at polymer electrolyte/electrode interfaces.展开更多
Theoretical simulations on complex electrochemical processes have been developed on the basis of the understanding in electrochemistry,which has benefited from quantum mechanics calculations.This article reviews the r...Theoretical simulations on complex electrochemical processes have been developed on the basis of the understanding in electrochemistry,which has benefited from quantum mechanics calculations.This article reviews the recent progress on the theory and applications in electrocatalysis.Two representative reactions,namely water electrolysis and oxygen reduction,are selected to illustrate how the theoretical methods are applied to electrocatalytic reactions.The microscopic nature of these electrochemical reactions under the applied potentials is described and the understanding of the reactions is summarized.The thermodynamics and kinetics of the electrochemical reactions affected by the interplay of the electrochemical potential,the bonding strength and the local surface structure are addressed at the atomic level.展开更多
A suitable interface between the electrode and electrolyte is crucial in achieving highly stable electrochemical performance for Li-ion batteries,as facile ionic transport is required.Intriguing research and developme...A suitable interface between the electrode and electrolyte is crucial in achieving highly stable electrochemical performance for Li-ion batteries,as facile ionic transport is required.Intriguing research and development have recently been conducted to form a stable interface between the electrode and electrolyte.Therefore,it is essential to investigate emerging knowledge and contextualize it.The nanoengineering of the electrode-electrolyte interface has been actively researched at the electrode/electrolyte and interphase levels.This review presents and summarizes some recent advances aimed at nanoengineering approaches to build a more stable electrode-electrolyte interface and assess the impact of each approach adopted.Furthermore,future perspectives on the feasibility and practicality of each approach will also be reviewed in detail.Finally,this review aids in projecting a more sustainable research pathway for a nanoengineered interphase design between electrode and electrolyte,which is pivotal for high-performance,thermally stable Li-ion batteries.展开更多
Rechargeable magnesium-ion(Mg-ion)batteries have attracted wide attention for energy storage.However,magnesium anode is still limited by the irreversible Mg plating/stripping procedure.Herein,a well-designed binary Bi...Rechargeable magnesium-ion(Mg-ion)batteries have attracted wide attention for energy storage.However,magnesium anode is still limited by the irreversible Mg plating/stripping procedure.Herein,a well-designed binary Bi_(2)O_(3)-Bi_(2)S_(3)(BO-BS)heterostructure is fulfilled by virtue of the cooperative interface and energy band engineering targeted fast Mg-ion storage.The built-in electronic field resulting from the asymmetrical electron distribution at the interface of electron-rich S center at Bi_(2)S_(3) side and electron-poor O center at Bi_(2)O_(3) side effectively accelerates the electrochemical reaction kinetics in the Mg-ion battery system.Moreover,the as-designed heterogenous interface also benefits to maintaining the electrode integrity.With these advantages,the BO-BS electrode displays a remarkable capacity of 150.36 mAh g^(−1) at 0.67 A g^(-1) and a superior cycling stability.This investigation would offer novel insights into the rational design of functional heterogenous electrode materials targeted the fast reaction kinetics for energy storage systems.展开更多
The adsorption isotherm of sodium polyacrylate on dicalcium silicate（2CaO-SiO2） in sodium aluminate solution at 80 ℃ was studied.The type of surface adsorption of sodium polyacrylate is saturated adsorption,and the...The adsorption isotherm of sodium polyacrylate on dicalcium silicate（2CaO-SiO2） in sodium aluminate solution at 80 ℃ was studied.The type of surface adsorption of sodium polyacrylate is saturated adsorption,and the adsorption behavior belongs to L-type,according with the monolayer adsorption model of Langmuir equation.The surface coverage of sodium polyacrylate is 1.06 mol/μm2.The relation curve between the surface pressure and the molecular area of adsorption film was obtained by Gibbs formula.The variation of interfacial energy caused by adsorption as well as the relationship between the relation curve and the type of adsorption was discussed.展开更多
Lithium-sulfur(Li-S)battery is recognized for the high theoretical energy density and cost-effective raw materials.However,the instability of Li metal anodes limits the cycle life of Li-S batteries under practical con...Lithium-sulfur(Li-S)battery is recognized for the high theoretical energy density and cost-effective raw materials.However,the instability of Li metal anodes limits the cycle life of Li-S batteries under practical conditions.In this study,we propose a dual interface-passivating regulation strategy using nitrocellulose(NC),a macromolecular nitrate,to stabilize the interface/interphase between the electrolyte and Li metal anode.Specifically,the macromolecular crowding effect and the reduction in lithium polysulfides(LiPSs)activity through nitrate coordination endow NC desirable bifunctionality to simultaneously suppress the depletion of Li salts and LiPSs corrosion,leading to better interface passivation than mono-functional additives such as LiNO_(3)and carboxymethyl cellulose.Consequently,the cycle life of Li-S batteries under practically demanding conditions(50μm Li anodes;4.0 mg cm^(-2)S athodes)is extended to 180 cycles,outperforming those of additive-free or LiNO_(3)-containing commercial electrolytes.This study highlights the potential of bifunctional macromolecular additive design for effectively dual-passivating the anode/electrolyte interface towards highly stable practical Li-S batteries.展开更多
In this paper,we consider the plasma-vacuum interface problem in a cylindrical tube region impressed by a special background magnetic field.The interior region is occupied with plasma,which is governed by the incompre...In this paper,we consider the plasma-vacuum interface problem in a cylindrical tube region impressed by a special background magnetic field.The interior region is occupied with plasma,which is governed by the incompressible inviscid and resistive MHD system without damping term.The exterior vacuum region is governed by the so-called the“pre-Maxwell equations”.And on the free interface,additionally,the effect of surface tension is taken into account.The original region can be transformed into a horizontally periodic slab through the cylindrical coordinate transformation,which will be impressed by a uniform nonhorizontal magnetic field.Appending with the appropriate physical boundary conditions,the global well-posedness of the problem is established by the energy method.展开更多
The growth of dendrites and the side reactions occurring at the Zn anode pose significant challenges to the commercialization of aqueous Zn-ion batteries(AZIBs). These challenges arise from the inherent conflict betwe...The growth of dendrites and the side reactions occurring at the Zn anode pose significant challenges to the commercialization of aqueous Zn-ion batteries(AZIBs). These challenges arise from the inherent conflict between mass transfer and electrochemical kinetics. In this study, we propose the use of a multifunctional electrolyte additive based on the xylose(Xylo) molecule to address these issues by modulating the solvation structure and electrode/electrolyte interface, thereby stabilizing the Zn anode. The introduction of the additive alters the solvation structure, creating steric hindrance that impedes charge transfer and then reduces electrochemical kinetics. Furthermore, in-situ analyses demonstrate that the reconstructed electrode/electrolyte interface facilitates stable and rapid Zn^(2+)ion migration and suppresses corrosion and hydrogen evolution reactions. As a result, symmetric cells incorporating the Xylo additive exhibit significantly enhanced reversibility during the Zn plating/stripping process, with an impressively long lifespan of up to 1986 h, compared to cells using pure ZnSO4electrolyte. When combined with a polyaniline cathode, the full cells demonstrate improved capacity and long-term cyclic stability. This work offers an effective direction for improving the stability of Zn anode via electrolyte design, as well as highperformance AZIBs.展开更多
Production of green hydrogen through water electrolysis powered by renewable energy sources has garnered increasing attention as an attractive strategy for the storage of clean and sustainable energy.Among various ele...Production of green hydrogen through water electrolysis powered by renewable energy sources has garnered increasing attention as an attractive strategy for the storage of clean and sustainable energy.Among various electrolysis technologies,the emerging anion exchange membrane water electrolyser(AEMWE)exhibits the most potential for green hydrogen production,offering a potentially costeffective and sustainable approach that combines the advantages of high current density and fast start from proton exchange membrane water electrolyser(PEMWE)and low-cost catalyst from traditional alkaline water electrolyser(AWE)systems.Due to its relatively recent emergence over the past decade,a series of efforts are dedicated to improving the electrochemical reaction performance to accelerate the development and commercialization of AEMWE technology.A catalytic electrode comprising a gas diffusion layer(GDL)and a catalyst layer(CL)is usually called a gas diffusion electrode(GDE)that serves as a fundamental component within AEMWE,and also plays a core role in enhancing mass transfer during the electrolysis process.Inside the GDEs,bubbles nucleate and grow within the CL and then are transported through the GDL before eventually detaching to enter the electrolyte in the flow field.The transfer processes of water,gas bubbles,charges,and ions are intricately influenced by bubbles.This phenomenon is referred to as bubble-associated mass transfer.Like water management in fuel cells,effective bubble management is crucial in electrolysers,as its failure can result in various overpotential losses,such as activation losses,ohmic losses,and mass transfer losses,ultimately degrading the AEMWE performance.Despite significant advancements in the development of new materials and techniques in AEMWE,there is an urgent need for a comprehensive discussion focused on GDEs,with a particular emphasis on bubbleassociated mass transfer phenomena.This review aims to highlight recent findings regarding mass transfer in GDEs,particularly the impacts of bubble accumulation;and presents the latest advancements in designing CLs and GDLs to mitigate bubble-related issues.It is worth noting that a series of innovative bubble-free-GDE designs for water electrolysis are also emphasized in this review.This review is expected to be a valuable reference for gaining a deeper understanding of bubble-related mass transfer,especially the complex bubble behavior associated with GDEs,and for developing innovative practical strategies to advance AEMWE for green hydrogen production.展开更多
Liquid phosphoric acid(PA),as the proton carrier for high temperature polymer electrolyte membrane fuel cells(HT-PEMFCs),presents challenges such as catalyst poisoning,high gas transport resistance and electrolyte los...Liquid phosphoric acid(PA),as the proton carrier for high temperature polymer electrolyte membrane fuel cells(HT-PEMFCs),presents challenges such as catalyst poisoning,high gas transport resistance and electrolyte loss.These issues significantly impede the performance and durability of HT-PEMFCs,thereby limiting their potential for further application.In this study,poly(2,3,5,6-tetrafluorostylene-4-phosphonic acid)(PWN)with intrinsic proton conduction ability was employed as catalyst layer binder to reveal the impacts of the ionomer's molecular structure on mass transport within the catalyst layer.Our findings demonstrated that increasing the phosphorylation degree of PWN could enhance both pore formation at the catalyst layer and electrode acidophilic capability while improving proton conduction ability and reducing cells'internal resistance.However,adverse effects included increased local oxygen transport resistance and decreased catalyst utilization resulting from electrode acidophilic capability.This research offers valuable insights for the relationships between micro-scale molecule structure,mesoscale electrode architecture,and membrane electrode assembly design in HT-PEMFCs.展开更多
This paper presents an exact solution for the transverse interface crack in the plane strain case. The crack is perpendicular to the interface and in one material. The exact complex stress functions are first obtained...This paper presents an exact solution for the transverse interface crack in the plane strain case. The crack is perpendicular to the interface and in one material. The exact complex stress functions are first obtained with some unknown constants. The satisfactions of all boundary conditions are then checked, the condition at infinity is considered and the unknown constants are determined. Further study may focus on the case with different shear moduli and the influence of the large deformation.展开更多
Lithium metal has been considered to be the most promising anode material for the new generation of energy-storage system.However,challenges still stand in protecting lithium metal from spontaneous reactions with elec...Lithium metal has been considered to be the most promising anode material for the new generation of energy-storage system.However,challenges still stand in protecting lithium metal from spontaneous reactions with electrolytes and preventing the dendritic propagation,both of which would lead to undesirable decrease in Coulombic efficiency.Polysulfone(PSf)membrane with high rigidity and free-volume cavities of approximately 0.3 nm was employed to provide a stable interface on the surface of anodic electrode.The isotropic channels were constructed by the interconnected and uniformly distributed free volumes in the polymer matrix,and were expected to be swelled by solvent molecules and anions of lithium salt and to allow Li+ions to pass through onto the electrode surface.As a result,dendrite-free morphology of deposited lithium was observed.The stabilized interface arose from the PSf film was verified by the promoted performances of Cu|Li cells and steady voltage polarization of Li|Li cells.The full cell with PSf coated anode exhibited excellent cyclability(85%capacity retention rate over 400 cycles at 1C)and an outstanding rate capability(117 m Ah g-1 at 5C).The beneficial performances were further verified by the EIS results.This work provides a new strategic idea to settle the dendritic problems of Li metal anodes.展开更多
Perovskite solar cells(PSCs) have revolutionized photovoltaic research. As a result, a certified power conversion efficiency(PCE) of 25.5% was recorded in late 2020. Although this efficiency is comparable with silicon...Perovskite solar cells(PSCs) have revolutionized photovoltaic research. As a result, a certified power conversion efficiency(PCE) of 25.5% was recorded in late 2020. Although this efficiency is comparable with silicon solar cells;some issues remain partially unsolved, such as lead toxicity, instability of perovskite materials under continuous illumination, moisture and oxygen, and degradation of the metallic counter electrodes. As an alternative to tackle this last concern, carbon materials have been recently used, due to their good electrical and thermal conductivity, and chemical stability, which makes them one of the most promising materials to replace metallic counter electrodes in the fabrication of PSCs. This review highlights the recent advances of carbon-based PSCs, where the carbon electrode(CE) is the main actor.CEs have become very promising candidates for PSCs;they are mainly fabricated using a simple combination of graphite and carbon black powders embedded in a binder matrix, giving a paste that is then solution-processable, resulting in devices with improved quality stability, when compared to metallic electrodes. In this review, CE’s composition is emphasized, since it can give both, high and lowtemperature processed electrodes, compatible with different device configurations. Finally, the tendencies and opportunities to use CE in PSCs devices are presented.展开更多
Nonfullerene organic solar cells(OSCs)have achieved breakthrough with pushing the efficiency exceeding 17%.While this shed light on OSC commercialization,high-performance flexible OSCs should be pursued through soluti...Nonfullerene organic solar cells(OSCs)have achieved breakthrough with pushing the efficiency exceeding 17%.While this shed light on OSC commercialization,high-performance flexible OSCs should be pursued through solution manufacturing.Herein,we report a solution-processed flexible OSC based on a transparent conducting PEDOT:PSS anode doped with trifluoromethanesulfonic acid(CF3SO3H).Through a low-concentration and low-temperature CF3SO3H doping,the conducting polymer anodes exhibited a main sheet resistance of 35Ωsq−1(minimum value:32Ωsq−1),a raised work function(≈5.0 eV),a superior wettability,and a high electrical stability.The high work function minimized the energy level mismatch among the anodes,hole-transporting layers and electron-donors of the active layers,thereby leading to an enhanced carrier extraction.The solution-processed flexible OSCs yielded a record-high efficiency of 16.41%(maximum value:16.61%).Besides,the flexible OSCs afforded the 1000 cyclic bending tests at the radius of 1.5 mm and the long-time thermal treatments at 85°C,demonstrating a high flexibility and a good thermal stability.展开更多
For the diffusion-controlled adsorption, the expression of dynamic surface adsorption P（t） was ob- tained by solving the diffusion equation. Two cases, i.e. the short and long time limits, were mainly discussed in t...For the diffusion-controlled adsorption, the expression of dynamic surface adsorption P（t） was ob- tained by solving the diffusion equation. Two cases, i.e. the short and long time limits, were mainly discussed in this paper. From the measured dynamic surface tension of aqueous surfactant sodium dodecyl sulfate （SDS） solutions at 25 ℃, the adsorption kinetics of SDS at air/solution interface was studied. It was proved that for both of the short and long time limits, the adsorption process of SDS was controlled by diffusion.展开更多
Membrane/solution interface consists of a neutral concentration polai layer(CPL) and a charge layer(CL) under external electrical field, and the neutral CPL can be neglected under high frequency AC electrical field. T...Membrane/solution interface consists of a neutral concentration polai layer(CPL) and a charge layer(CL) under external electrical field, and the neutral CPL can be neglected under high frequency AC electrical field. The relationship of CL thickness e with electrolyte concentration C and fixed ion exchange sites density σ in membrane surface layer can be expressed as e展开更多
Since the electrode/electrolyte interface(EEI)is the main redox center of electrochemical processes,proper manipulation of the EEI microenvironment is crucial to stabilize interfacial behaviors.Here,a finger-paint met...Since the electrode/electrolyte interface(EEI)is the main redox center of electrochemical processes,proper manipulation of the EEI microenvironment is crucial to stabilize interfacial behaviors.Here,a finger-paint method is proposed to enable quick physical modification of glass-fiber separator without complicated chemical technology to modulate EEI of bilateral electrodes for aqueous zinc-ion batteries(ZIBs).An elaborate biochar derived from Aspergillus Niger is exploited as the modification agent of EEI,in which the multi-functional groups assist to accelerate Zn^(2+)desolvation and create a hydrophobic environment to homogenize the deposition behavior of Zn anode.Importantly,the finger-paint interface on separator can effectively protect cathodes from abnormal capacity fluctuation and/or rapid attenuation induced by H_(2)O molecular on the interface,which is demonstrated in modified MnO_(2),V_(2)O_(5),and KMn HCF-based cells.The as-proposed finger-paint method opens a new idea of bilateral interface engineering to facilitate the access to the practical application of the stable zinc electrochemistry.展开更多
Hydrogen evolution reaction(HER)catalytic electrodes under actual working conditions show interesting mass transfer behaviors at solid(electrode)/liquid(electrolyte)/gas(hydrogen)three-phase interfaces.These behaviors...Hydrogen evolution reaction(HER)catalytic electrodes under actual working conditions show interesting mass transfer behaviors at solid(electrode)/liquid(electrolyte)/gas(hydrogen)three-phase interfaces.These behaviors are essential for forming a continuous and effective physical contact region between the electrolyte and the electrode and require further detailed understanding.Here,a case study on 1 T-2 H phase molybdenum disulfide(Mo S_(2))/carbon fiber paper(CFP)catalytic electrodes is performed.Rapid gas-liquid mass transfer at the interface for enhancing the working area stability and capillarity for increasing the electrode working area is found.The real scenario,wherein the energy utilization efficiency of the as-prepared non-noble metal catalytic electrode exceeds that of the noble metal catalytic electrode,is disclosed.Specifically,a fluid dynamics model is developed to investigate the behavior mechanism of hydrogen bubbles from generation to desorption on the catalytic electrode surface with different hydrophilic and hydrophobic properties.These new insights and theoretical evidence on the non-negligible three-phase interface behaviors will identify opportunities and motivate future research in high-efficiency,stability,and low-cost HER catalytic electrode development.展开更多
文摘In this paper a pH microprobe technique was developed to measure in-situ the pH value at the electrode/solution interface. Iridium oxide was used as a pH sensitive material with good response behavior in the measured solutions. The experimental results indicated that the interfacial pH increased with the applied potential, first jumped to a maximum, then slowly decreased at the controlled potential during the electrodeposition process of functional ceramics.
基金The Open Project of State Key Laboratory of Smart Grid Protection and Operation Control in 2022(No.SGNR0000KJJS2302150).
文摘Fully implanted brain-computer interfaces(BCIs)are preferred as they eliminate signal degradation caused by interference and absorption in external tissues,a common issue in non-fully implanted systems.To optimize the design of electroencephalography electrodes in fully implanted BCI systems,this study investigates the penetration and absorption characteristics of microwave signals in human brain tissue at different frequencies.Electromagnetic simulations are used to analyze the power density distribution and specific absorption rate(SAR)of signals at various frequen-cies.The results indicate that lower-frequency signals offer advantages in terms of power density and attenuation coeffi-cients.However,SAR-normalized analysis,which considers both power density and electromagnetic radiation hazards,shows that higher-frequency signals perform better at superficial to intermediate depths.Specifically,at a depth of 2 mm beneath the cortex,the power density of a 6.5 GHz signal is 247.83%higher than that of a 0.4 GHz signal.At a depth of 5 mm,the power density of a 3.5 GHz signal exceeds that of a 0.4 GHz signal by 224.16%.The findings suggest that 6.5 GHz is optimal for electrodes at a depth of 2 mm,3.5 GHz for 5 mm,2.45 GHz for depths of 15-20 mm,and 1.8 GHz for 25 mm.
基金supported by the National Key R&D Program of China(No.2021YFA1501003)。
文摘Electron transfer processes at polymer electrolyte/electrode interfaces play a central role in modern electrochemical devices of energy conversion,however,current understanding of electron transfers through electrochemical interfaces was established exclusively based on the studies of liquid/solid electrochemical interfaces.Thus,similarities and differences of liquid and polymer electrolyte/electrode interfaces need to be mapped out to guide the design of device level electrochemical interfaces.In this work,we employ the sulfonate adsorption/desorption as a probe reaction to understand the electron-transfer steps in polymer and liquid electrolytes.Through cyclic voltametric investigations on the well-define single-crystal Pd_(ML)Pt(111)electrode,we demonstrate that the oxidative adsorption and reductive desorption of sulfonates at the polymer electrolyte/electrode interface are chemically distinct from those in liquid electrolytes,with the former occurring mostly via the proton-coupled pathway while the latter proceeding mainly through the solvation-mediated pathway.Importantly,the sulfonate adsorption/desorption behaviors of alkylsulfonates become increasingly similar to those in Nafion with longer alkyl chains,suggesting that the interfacial hydrophobicity and solvation environment conferred by the perfluorinated polymer play a decisive role in the electron-transfer mechanism.Results reported in this study highlight the mechanistic distinctions between electron-transfer processes at electrochemical interfaces involving polymer and liquid electrolytes,and provide a framework for understanding electron-transfer processes at polymer electrolyte/electrode interfaces.
基金supported by the National Natural Science Foundation of China (Grant Nos 20825311, 20773026, and 20721063)Sci & Tech Comm of Shanghai Municipality (08DZ2270500)Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institute of Higher Learning
文摘Theoretical simulations on complex electrochemical processes have been developed on the basis of the understanding in electrochemistry,which has benefited from quantum mechanics calculations.This article reviews the recent progress on the theory and applications in electrocatalysis.Two representative reactions,namely water electrolysis and oxygen reduction,are selected to illustrate how the theoretical methods are applied to electrocatalytic reactions.The microscopic nature of these electrochemical reactions under the applied potentials is described and the understanding of the reactions is summarized.The thermodynamics and kinetics of the electrochemical reactions affected by the interplay of the electrochemical potential,the bonding strength and the local surface structure are addressed at the atomic level.
基金supported by funding from Bavarian Center for Battery Technology(Baybatt,Hightech Agenda Bayern)and Bayerisch-Tschechische Hochschulagentur(BTHA)(BTHA-AP-202245,BTHA-AP-2023-5,and BTHA-AP-2023-12)supported by the University of Bayreuth-Deakin University Joint Ph.D.Program+1 种基金supported by the Regional Innovation Strategy(RIS)through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(MOE)(2021RIS-003)supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.RS2023-00213749)
文摘A suitable interface between the electrode and electrolyte is crucial in achieving highly stable electrochemical performance for Li-ion batteries,as facile ionic transport is required.Intriguing research and development have recently been conducted to form a stable interface between the electrode and electrolyte.Therefore,it is essential to investigate emerging knowledge and contextualize it.The nanoengineering of the electrode-electrolyte interface has been actively researched at the electrode/electrolyte and interphase levels.This review presents and summarizes some recent advances aimed at nanoengineering approaches to build a more stable electrode-electrolyte interface and assess the impact of each approach adopted.Furthermore,future perspectives on the feasibility and practicality of each approach will also be reviewed in detail.Finally,this review aids in projecting a more sustainable research pathway for a nanoengineered interphase design between electrode and electrolyte,which is pivotal for high-performance,thermally stable Li-ion batteries.
基金supported by the National Natural Science Foundation of China(52172239)Project of State Key Laboratory of Environment-Friendly Energy Materials(SWUST,Grant Nos.22fksy23 and 18ZD320304)+3 种基金the Frontier Project of Chengdu Tianfu New Area Institute(SWUST,Grand No.2022ZY017)Chongqing Talents:Exceptional Young Talents Project(Grant No.CQYC201905041)Natural Science Foundation of Chongqing China(Grant No.cstc2021jcyj-jqX0031)Interdiscipline Team Project under auspices of“Light of West”Program in Chinese Academy of Sciences(Grant No.xbzg-zdsys-202106).
文摘Rechargeable magnesium-ion(Mg-ion)batteries have attracted wide attention for energy storage.However,magnesium anode is still limited by the irreversible Mg plating/stripping procedure.Herein,a well-designed binary Bi_(2)O_(3)-Bi_(2)S_(3)(BO-BS)heterostructure is fulfilled by virtue of the cooperative interface and energy band engineering targeted fast Mg-ion storage.The built-in electronic field resulting from the asymmetrical electron distribution at the interface of electron-rich S center at Bi_(2)S_(3) side and electron-poor O center at Bi_(2)O_(3) side effectively accelerates the electrochemical reaction kinetics in the Mg-ion battery system.Moreover,the as-designed heterogenous interface also benefits to maintaining the electrode integrity.With these advantages,the BO-BS electrode displays a remarkable capacity of 150.36 mAh g^(−1) at 0.67 A g^(-1) and a superior cycling stability.This investigation would offer novel insights into the rational design of functional heterogenous electrode materials targeted the fast reaction kinetics for energy storage systems.
基金Project(50974036)supported by the National Natural Science Foundation of China
文摘The adsorption isotherm of sodium polyacrylate on dicalcium silicate（2CaO-SiO2） in sodium aluminate solution at 80 ℃ was studied.The type of surface adsorption of sodium polyacrylate is saturated adsorption,and the adsorption behavior belongs to L-type,according with the monolayer adsorption model of Langmuir equation.The surface coverage of sodium polyacrylate is 1.06 mol/μm2.The relation curve between the surface pressure and the molecular area of adsorption film was obtained by Gibbs formula.The variation of interfacial energy caused by adsorption as well as the relationship between the relation curve and the type of adsorption was discussed.
基金supported by the National Natural Science Foundation of China(22379021 and 22479021)。
文摘Lithium-sulfur(Li-S)battery is recognized for the high theoretical energy density and cost-effective raw materials.However,the instability of Li metal anodes limits the cycle life of Li-S batteries under practical conditions.In this study,we propose a dual interface-passivating regulation strategy using nitrocellulose(NC),a macromolecular nitrate,to stabilize the interface/interphase between the electrolyte and Li metal anode.Specifically,the macromolecular crowding effect and the reduction in lithium polysulfides(LiPSs)activity through nitrate coordination endow NC desirable bifunctionality to simultaneously suppress the depletion of Li salts and LiPSs corrosion,leading to better interface passivation than mono-functional additives such as LiNO_(3)and carboxymethyl cellulose.Consequently,the cycle life of Li-S batteries under practically demanding conditions(50μm Li anodes;4.0 mg cm^(-2)S athodes)is extended to 180 cycles,outperforming those of additive-free or LiNO_(3)-containing commercial electrolytes.This study highlights the potential of bifunctional macromolecular additive design for effectively dual-passivating the anode/electrolyte interface towards highly stable practical Li-S batteries.
基金supported by the NSFC(11571177)the National Key Research and Development Program of China(2020YFA0713803).
文摘In this paper,we consider the plasma-vacuum interface problem in a cylindrical tube region impressed by a special background magnetic field.The interior region is occupied with plasma,which is governed by the incompressible inviscid and resistive MHD system without damping term.The exterior vacuum region is governed by the so-called the“pre-Maxwell equations”.And on the free interface,additionally,the effect of surface tension is taken into account.The original region can be transformed into a horizontally periodic slab through the cylindrical coordinate transformation,which will be impressed by a uniform nonhorizontal magnetic field.Appending with the appropriate physical boundary conditions,the global well-posedness of the problem is established by the energy method.
文摘The growth of dendrites and the side reactions occurring at the Zn anode pose significant challenges to the commercialization of aqueous Zn-ion batteries(AZIBs). These challenges arise from the inherent conflict between mass transfer and electrochemical kinetics. In this study, we propose the use of a multifunctional electrolyte additive based on the xylose(Xylo) molecule to address these issues by modulating the solvation structure and electrode/electrolyte interface, thereby stabilizing the Zn anode. The introduction of the additive alters the solvation structure, creating steric hindrance that impedes charge transfer and then reduces electrochemical kinetics. Furthermore, in-situ analyses demonstrate that the reconstructed electrode/electrolyte interface facilitates stable and rapid Zn^(2+)ion migration and suppresses corrosion and hydrogen evolution reactions. As a result, symmetric cells incorporating the Xylo additive exhibit significantly enhanced reversibility during the Zn plating/stripping process, with an impressively long lifespan of up to 1986 h, compared to cells using pure ZnSO4electrolyte. When combined with a polyaniline cathode, the full cells demonstrate improved capacity and long-term cyclic stability. This work offers an effective direction for improving the stability of Zn anode via electrolyte design, as well as highperformance AZIBs.
基金support from the National Natural Science Foundation of China(Grant No.52006029)the Promotion Foundation for Young Science and Technology Talents in Jilin Province(Grant No.QT202113)+2 种基金the Special Foundation of Industrial Innovation in Jilin Province(Grant No.2019C056-2)the Special Foundation for Outstanding Young Talents Training in Jilin(Grant No.20200104107)the UK EPSRC(EP/W03784X/1)。
文摘Production of green hydrogen through water electrolysis powered by renewable energy sources has garnered increasing attention as an attractive strategy for the storage of clean and sustainable energy.Among various electrolysis technologies,the emerging anion exchange membrane water electrolyser(AEMWE)exhibits the most potential for green hydrogen production,offering a potentially costeffective and sustainable approach that combines the advantages of high current density and fast start from proton exchange membrane water electrolyser(PEMWE)and low-cost catalyst from traditional alkaline water electrolyser(AWE)systems.Due to its relatively recent emergence over the past decade,a series of efforts are dedicated to improving the electrochemical reaction performance to accelerate the development and commercialization of AEMWE technology.A catalytic electrode comprising a gas diffusion layer(GDL)and a catalyst layer(CL)is usually called a gas diffusion electrode(GDE)that serves as a fundamental component within AEMWE,and also plays a core role in enhancing mass transfer during the electrolysis process.Inside the GDEs,bubbles nucleate and grow within the CL and then are transported through the GDL before eventually detaching to enter the electrolyte in the flow field.The transfer processes of water,gas bubbles,charges,and ions are intricately influenced by bubbles.This phenomenon is referred to as bubble-associated mass transfer.Like water management in fuel cells,effective bubble management is crucial in electrolysers,as its failure can result in various overpotential losses,such as activation losses,ohmic losses,and mass transfer losses,ultimately degrading the AEMWE performance.Despite significant advancements in the development of new materials and techniques in AEMWE,there is an urgent need for a comprehensive discussion focused on GDEs,with a particular emphasis on bubbleassociated mass transfer phenomena.This review aims to highlight recent findings regarding mass transfer in GDEs,particularly the impacts of bubble accumulation;and presents the latest advancements in designing CLs and GDLs to mitigate bubble-related issues.It is worth noting that a series of innovative bubble-free-GDE designs for water electrolysis are also emphasized in this review.This review is expected to be a valuable reference for gaining a deeper understanding of bubble-related mass transfer,especially the complex bubble behavior associated with GDEs,and for developing innovative practical strategies to advance AEMWE for green hydrogen production.
基金supported by The National Key Research and Development Program of China(2021YFB4001204)National Natural Science Foundation of China(22179130,22379143,22479145)。
文摘Liquid phosphoric acid(PA),as the proton carrier for high temperature polymer electrolyte membrane fuel cells(HT-PEMFCs),presents challenges such as catalyst poisoning,high gas transport resistance and electrolyte loss.These issues significantly impede the performance and durability of HT-PEMFCs,thereby limiting their potential for further application.In this study,poly(2,3,5,6-tetrafluorostylene-4-phosphonic acid)(PWN)with intrinsic proton conduction ability was employed as catalyst layer binder to reveal the impacts of the ionomer's molecular structure on mass transport within the catalyst layer.Our findings demonstrated that increasing the phosphorylation degree of PWN could enhance both pore formation at the catalyst layer and electrode acidophilic capability while improving proton conduction ability and reducing cells'internal resistance.However,adverse effects included increased local oxygen transport resistance and decreased catalyst utilization resulting from electrode acidophilic capability.This research offers valuable insights for the relationships between micro-scale molecule structure,mesoscale electrode architecture,and membrane electrode assembly design in HT-PEMFCs.
文摘This paper presents an exact solution for the transverse interface crack in the plane strain case. The crack is perpendicular to the interface and in one material. The exact complex stress functions are first obtained with some unknown constants. The satisfactions of all boundary conditions are then checked, the condition at infinity is considered and the unknown constants are determined. Further study may focus on the case with different shear moduli and the influence of the large deformation.
基金supported by the Opening Project(SKLACPS-C-21)of the State Key Laboratory of Advanced Chemical Power Source,Guizhou Meiling Power Sources Co.Ltd.the Program for Innovative and Entrepreneurial team in Zhuhai(ZH01110405160007PWC)Key Laboratory of Advanced Chemical Power Sources,Guizhou Meiling Power Sources Co.Ltd.,Zunyi 563003,Guizhou,China,for funding the experiments.
文摘Lithium metal has been considered to be the most promising anode material for the new generation of energy-storage system.However,challenges still stand in protecting lithium metal from spontaneous reactions with electrolytes and preventing the dendritic propagation,both of which would lead to undesirable decrease in Coulombic efficiency.Polysulfone(PSf)membrane with high rigidity and free-volume cavities of approximately 0.3 nm was employed to provide a stable interface on the surface of anodic electrode.The isotropic channels were constructed by the interconnected and uniformly distributed free volumes in the polymer matrix,and were expected to be swelled by solvent molecules and anions of lithium salt and to allow Li+ions to pass through onto the electrode surface.As a result,dendrite-free morphology of deposited lithium was observed.The stabilized interface arose from the PSf film was verified by the promoted performances of Cu|Li cells and steady voltage polarization of Li|Li cells.The full cell with PSf coated anode exhibited excellent cyclability(85%capacity retention rate over 400 cycles at 1C)and an outstanding rate capability(117 m Ah g-1 at 5C).The beneficial performances were further verified by the EIS results.This work provides a new strategic idea to settle the dendritic problems of Li metal anodes.
基金financial support of the Colombia Scientific Program within the framework of the call Ecosistema Cientifíco (Contract FP44842-218-2018)。
文摘Perovskite solar cells(PSCs) have revolutionized photovoltaic research. As a result, a certified power conversion efficiency(PCE) of 25.5% was recorded in late 2020. Although this efficiency is comparable with silicon solar cells;some issues remain partially unsolved, such as lead toxicity, instability of perovskite materials under continuous illumination, moisture and oxygen, and degradation of the metallic counter electrodes. As an alternative to tackle this last concern, carbon materials have been recently used, due to their good electrical and thermal conductivity, and chemical stability, which makes them one of the most promising materials to replace metallic counter electrodes in the fabrication of PSCs. This review highlights the recent advances of carbon-based PSCs, where the carbon electrode(CE) is the main actor.CEs have become very promising candidates for PSCs;they are mainly fabricated using a simple combination of graphite and carbon black powders embedded in a binder matrix, giving a paste that is then solution-processable, resulting in devices with improved quality stability, when compared to metallic electrodes. In this review, CE’s composition is emphasized, since it can give both, high and lowtemperature processed electrodes, compatible with different device configurations. Finally, the tendencies and opportunities to use CE in PSCs devices are presented.
基金The authors acknowledge funding from the National Natural Science Foundation of China(61974150 and 51773213)Key Research Program of Frontier Sciences,CAS(QYZDB-SSW-JSC047)+1 种基金the Fundamental Research Funds for the Central Universities,the CAS-EU S&T cooperation partner program(174433KYSB20150013)the Natural Science Foundation of Ningbo(2018A610135).
文摘Nonfullerene organic solar cells(OSCs)have achieved breakthrough with pushing the efficiency exceeding 17%.While this shed light on OSC commercialization,high-performance flexible OSCs should be pursued through solution manufacturing.Herein,we report a solution-processed flexible OSC based on a transparent conducting PEDOT:PSS anode doped with trifluoromethanesulfonic acid(CF3SO3H).Through a low-concentration and low-temperature CF3SO3H doping,the conducting polymer anodes exhibited a main sheet resistance of 35Ωsq−1(minimum value:32Ωsq−1),a raised work function(≈5.0 eV),a superior wettability,and a high electrical stability.The high work function minimized the energy level mismatch among the anodes,hole-transporting layers and electron-donors of the active layers,thereby leading to an enhanced carrier extraction.The solution-processed flexible OSCs yielded a record-high efficiency of 16.41%(maximum value:16.61%).Besides,the flexible OSCs afforded the 1000 cyclic bending tests at the radius of 1.5 mm and the long-time thermal treatments at 85°C,demonstrating a high flexibility and a good thermal stability.
文摘For the diffusion-controlled adsorption, the expression of dynamic surface adsorption P（t） was ob- tained by solving the diffusion equation. Two cases, i.e. the short and long time limits, were mainly discussed in this paper. From the measured dynamic surface tension of aqueous surfactant sodium dodecyl sulfate （SDS） solutions at 25 ℃, the adsorption kinetics of SDS at air/solution interface was studied. It was proved that for both of the short and long time limits, the adsorption process of SDS was controlled by diffusion.
基金Project(02-09-01) supported by Panzhihua Iron and Steel Corporation,China
文摘Membrane/solution interface consists of a neutral concentration polai layer(CPL) and a charge layer(CL) under external electrical field, and the neutral CPL can be neglected under high frequency AC electrical field. The relationship of CL thickness e with electrolyte concentration C and fixed ion exchange sites density σ in membrane surface layer can be expressed as e
基金financial support from the National Natural Science Foundation of China (21571080 and 52202253)the Natural Science Foundation of Jiangsu Province (BK20220914)+2 种基金Project funded by China Postdoctoral Science Foundation (2022M721593)the Jiangsu Funding Program for Excellent Postdoctoral Talent (2022ZB193)the financial support from International Center of Future Science,Jilin University,Changchun,P.R.China (ICFS Seed Funding for Young Researchers)。
文摘Since the electrode/electrolyte interface(EEI)is the main redox center of electrochemical processes,proper manipulation of the EEI microenvironment is crucial to stabilize interfacial behaviors.Here,a finger-paint method is proposed to enable quick physical modification of glass-fiber separator without complicated chemical technology to modulate EEI of bilateral electrodes for aqueous zinc-ion batteries(ZIBs).An elaborate biochar derived from Aspergillus Niger is exploited as the modification agent of EEI,in which the multi-functional groups assist to accelerate Zn^(2+)desolvation and create a hydrophobic environment to homogenize the deposition behavior of Zn anode.Importantly,the finger-paint interface on separator can effectively protect cathodes from abnormal capacity fluctuation and/or rapid attenuation induced by H_(2)O molecular on the interface,which is demonstrated in modified MnO_(2),V_(2)O_(5),and KMn HCF-based cells.The as-proposed finger-paint method opens a new idea of bilateral interface engineering to facilitate the access to the practical application of the stable zinc electrochemistry.
基金supported by the National Natural Science Foundation of China(No.62004051)the Natural Science Foundation of Heilongjiang province(No.LH2020F013)+1 种基金the China Postdoctoral Science Fund(No.2020M670909)the Heilongjiang Postdoctoral Science Fund(No.LBH-Z19017)。
文摘Hydrogen evolution reaction(HER)catalytic electrodes under actual working conditions show interesting mass transfer behaviors at solid(electrode)/liquid(electrolyte)/gas(hydrogen)three-phase interfaces.These behaviors are essential for forming a continuous and effective physical contact region between the electrolyte and the electrode and require further detailed understanding.Here,a case study on 1 T-2 H phase molybdenum disulfide(Mo S_(2))/carbon fiber paper(CFP)catalytic electrodes is performed.Rapid gas-liquid mass transfer at the interface for enhancing the working area stability and capillarity for increasing the electrode working area is found.The real scenario,wherein the energy utilization efficiency of the as-prepared non-noble metal catalytic electrode exceeds that of the noble metal catalytic electrode,is disclosed.Specifically,a fluid dynamics model is developed to investigate the behavior mechanism of hydrogen bubbles from generation to desorption on the catalytic electrode surface with different hydrophilic and hydrophobic properties.These new insights and theoretical evidence on the non-negligible three-phase interface behaviors will identify opportunities and motivate future research in high-efficiency,stability,and low-cost HER catalytic electrode development.
