To evaluate the H_(2)O_(2)‐tolerance of non‐Pt oxygen reduction reaction(ORR)catalysts as well as in‐vestigate the H_(2)O_(2)‐induced decay mechanism,the selection of an appropriate H_(2)O_(2) concentration is a p...To evaluate the H_(2)O_(2)‐tolerance of non‐Pt oxygen reduction reaction(ORR)catalysts as well as in‐vestigate the H_(2)O_(2)‐induced decay mechanism,the selection of an appropriate H_(2)O_(2) concentration is a prerequisite.However,the concentration criterion is still unclear because of the lack of in‐operando methods to determine the actual concentration of H_(2)O_(2) in fuel cell catalyst layers.In this work,an electrochemical probe method was successfully established to in‐operando monitor the H_(2)O_(2) in non‐Pt catalyst layers for the first time.The local concentration of H_(2)O_(2) was revealed to reach 17 mmol/L,which is one order of magnitude higher than that under aqueous electrodes test conditions.Powered by the new knowledge,a concentration criterion of at least 17 mmol/L is suggested.This work fills in the large gap between aqueous electrode tests and the real fuel cell working conditions,and highlights the importance of in‐operando monitoring methods.展开更多
Electrochemical CO_(2)reduction(CO_(2)RR)is a promising technology for mitigating global climate change.The catalyst layer(CL),where the reduction reaction occurs,plays a pivotal role in determining mass transport and...Electrochemical CO_(2)reduction(CO_(2)RR)is a promising technology for mitigating global climate change.The catalyst layer(CL),where the reduction reaction occurs,plays a pivotal role in determining mass transport and electrochemical performance.However,accurately characterizing local structures and quantifying mass transport remains a significant challenge.To address these limitations,a systematic characterization framework based on deep learning(DL)is proposed.Five semantic segmentation models,including Segformer and DeepLabV3plus,were compared with conventional image processing techniques,among which DeepLabV3plus achieved the highest segmentation accuracy(>91.29%),significantly outperforming traditional thresholding methods(72.35%–77.42%).Experimental validation via mercury intrusion porosimetry(MIP)confirmed its capability to precisely extract key structural parameters,such as porosity and pore size distribution.Furthermore,a series of ionomer content gradient experiments revealed that a CL with an ionomer/catalyst(I/C)ratio of 0.2 had the optimal pore network structure.Numerical simulations and electrochemical tests demonstrated that this CL enabled a twofold increase in gas diffusion distance,thereby promoting long-range mass transport and significantly enhancing CO production rates.This work establishes a multi-scale analysis framework integrating“structural characterization,mass transport simulation,and performance validation,”offering both theoretical insights and practical guidance for the rational design of CO_(2)RR CLs.展开更多
Improving the performance of proton exchange membrane fuel cells(PEMFCs)requires deep understanding of the reac-tive transport processes inside the catalyst layers(CLs).In this study,a particle-overlapping model is de...Improving the performance of proton exchange membrane fuel cells(PEMFCs)requires deep understanding of the reac-tive transport processes inside the catalyst layers(CLs).In this study,a particle-overlapping model is developed for accu-rately describing the hierarchical structures and oxygen reactive transport processes in CLs.The analytical solutions derived from this model indicate that carbon particle overlap increases ionomer thickness,reduces specific surface areas of ionomer and carbon,and further intensifies the local oxygen transport resistance(R_(other)).The relationship between Rother and roughness factor predicted by the model in the range of 800-1600 sm^(-1) agrees well with the experiments.Then,a multiscale model is developed by coupling the particle-overlapping model with cell-scale models,which is validated by comparing with the polarization curves and local current density distribution obtained in experiments.The relative error of local current density distribution is below 15%in the ohmic polarization region.Finally,the multiscale model is employed to explore effects of CL structural parameters including Pt loading,I/C,ionomer coverage and carbon particle radius on the cell performance as well as the phase-change-induced(PCI)flow and capillary-driven(CD)flow in CL.The result demonstrates that the CL structural parameters have significant effects on the cell performance as well as the PCI and CD flows.Optimizing the CL structure can increase the current density and further enhance the heat-pipe effect within the CL,leading to overall higher PCI and CD rates.The maximum increase of PCI and CD rates can exceed 145%.Besides,the enhanced heat-pipe effect causes the reverse flow regions of PCI and CD near the CL/PEM interface,which can occupy about 30%of the CL.The multiscale model significantly contributes to a deep understanding of reactive trans-port and multiphase heat transfer processes inside PEMFCs.展开更多
The catalyst layer is an essential component of fuel cells,exerting a decisive influence on performance,particularly under degradation processes.Characterization derived from accelerated stress tests(ASTs)provide valu...The catalyst layer is an essential component of fuel cells,exerting a decisive influence on performance,particularly under degradation processes.Characterization derived from accelerated stress tests(ASTs)provide valuable insights into the long-term degradation from the perspective of changes in physical and chemical properties,thereby offering a scientific foundation for evaluating advanced materials and strategies.In this review,multidimensional and multi-characterization application scenarios based on ASTs data are systematically summarized.Firstly,the degradation mechanism of catalyst layer(CL)under AST conditions is discussed,with an emphasis on platinum aging and carbon support corrosion.In addition,electrochemical and microphysical characterization tools applicable to different AST test protocols,such as electrochemical surface area(ECSA),electrochemical impedance spectrum(EIS)mapping combined with distribution of relaxation times(DRT),and microscopic physical evolution and tracking techniques for each internal chemical component,are also presented in detail.Finally,through the existing research progress and hotspots,the application prospect of data fusion is elaborated and the important research direction of material optimization and performance prediction based on AST data is emphasized,aiming to provide insights into the study of catalytic layer degradation in fuel cells and promote the continuous development of the field.展开更多
Catalyst layer(CL)is the core component of proton exchange membrane(PEM)fuel cells,which determines the performance,durability,and cost.However,difficulties remain for a thorough understanding of the CLs’inhomogeneou...Catalyst layer(CL)is the core component of proton exchange membrane(PEM)fuel cells,which determines the performance,durability,and cost.However,difficulties remain for a thorough understanding of the CLs’inhomogeneous structure,and its impact on the physicochemical and electrochemical properties,operating performance,and durability.The inhomogeneous structure of the CLs is formed during the manufacturing process,which is sensitive to the associated materials,composi-tion,fabrication methods,procedures,and conditions.The state-of-the-art visualization and characterization techniques are crucial to examine the CL structure.The structure-dependent physicochemical and electrochemical properties are then thoroughly scrutinized in terms of fundamental concepts,theories,and recent progress in advanced experimental techniques.The relation between the CL structure and the associated effective properties is also examined based on experimental and theoretical findings.Recent studies indicated that the CL inhomogeneous structure also strongly affects the performance and degradation of the whole fuel cell,and thus,the interconnection between the fuel cell performance,failure modes,and CL structure is comprehensively reviewed.An analytical model is established to understand the effect of the CL structure on the effective properties,performance,and durability of the PEM fuel cells.Finally,the challenges and prospects of the CL structure-associated studies are highlighted for the development of high-performing PEM fuel cells.展开更多
Unraveling the essence of electronic structure effected by d-d orbital coupling of transition metal and methanol oxidation reaction(MOR)performance can fundamentally guide high efficient catalyst design.Herein,density...Unraveling the essence of electronic structure effected by d-d orbital coupling of transition metal and methanol oxidation reaction(MOR)performance can fundamentally guide high efficient catalyst design.Herein,density functional theory(DFT)calculations were performed at first to study the d–d orbital interaction of metallic Pt Pd Cu,revealing that the incorporation of Pd and Cu atoms into Pt system can enhance d-d electron interaction via capturing antibonding orbital electrons of Pt to fill the surrounding Pd and Cu atoms.Under the theoretical guidance,Pt Pd Cu medium entropy alloy aerogels(Pt Pd Cu MEAAs)catalysts have been designed and systematically screened for MOR under acid,alkaline and neutral electrolyte.Furthermore,DFT calculation and in-situ fourier transform infrared spectroscopy analysis indicate that Pt Pd Cu MEAAs follow the direct pathway via formate as the reactive intermediate to be directly oxidized to CO_(2).For practical direct methanol fuel cells(DMFCs),the Pt Pd Cu MEAAs-integrated ultra-thin catalyst layer(4–5μm thickness)as anode exhibits higher peak power density of 35 m W/cm^(2) than commercial Pt/C of 20 m W/cm^(2)(~40μm thickness)under the similar noble metal loading and an impressive stability retention at a 50-m A/cm^(2) constant current for 10 h.This work clearly proves that optimizing the intermediate adsorption capacity via d-d orbital coupling is an effective strategy to design highly efficient catalysts for DMFCs.展开更多
Reducing the Ir loading while preserving catalytic performance and mechanical robustness in anodic catalyst layers remains a critical challenge for the large-scale implementation of proton exchange membrane water elec...Reducing the Ir loading while preserving catalytic performance and mechanical robustness in anodic catalyst layers remains a critical challenge for the large-scale implementation of proton exchange membrane water electrolysis(PEMWE).Herein,we present a structural engineering strategy involving neodymium-doped Ir/IrO_(2)(Nd-Ir/IrO_(2))hollow nanospheres with precisely adjustable shell thickness and cavity dimensions.The optimized catalyst demonstrates excellent oxygen evolution reaction(OER)performance in acidic media,achieving a remarkably low overpotential of 259 mV at a benchmark current density of 10 mA cm^(-2) while exhibiting substantially enhanced durability compared to commercial IrO_(2) and Ir/IrO_(2) counterparts.Notably,the Nd-Ir/IrO_(2) catalyst delivers a mass activity of 541.6 A gIr^(-1) at 1.50 V vs RHE,representing a 74.5-fold enhancement over conventional IrO_(2).Through comprehensive electrochemical analysis and advanced characterization techniques reveal that,the hierarchical hollow architecture simultaneously addresses multiple critical requirements:(i)abundant exposed active sites enabled by an enhanced electrochemical surface area,(ii)optimized mass transport pathways through engineered porosity,and(iii)preserved structural integrity via a continuous conductive framework,collectively enabling significant Ir loading reduction without compromising catalytic layer performance.Fundamental mechanistic investigations further disclose that Nd doping induces critical interfacial Nd-O-Ir configurations that stabilize lattice oxygen,together with intensified electron effect among mixed valent Ir that inhibits the overoxidation of Ir active sites during the OER process,synergistically ensuring enhanced catalytic durability.Our work establishes a dual-modulation paradigm integrating nanoscale architectural engineering with atomic-level heteroatom doping,providing a viable pathway toward high-performance PEMWE systems with drastically reduced noble metal requirements.展开更多
Reducing a Pt loading with improved power output and durability is essential to promote the large-scale application of proton exchange membrane fuel cells(PEMFCs).To achieve this goal,constructing optimized structure ...Reducing a Pt loading with improved power output and durability is essential to promote the large-scale application of proton exchange membrane fuel cells(PEMFCs).To achieve this goal,constructing optimized structure of catalyst layers with efficient mass transportation channels plays a vital role.Herein,PEMFCs with order-structured cathodic electrodes were fabricated by depositing Pt nanoparticles by Ebeam onto vertically aligned carbon nanotubes(VACNTs)growth on Al foil via plasma-enhanced chemical vapor deposition.Results demonstrate that the proportion of hydrophilic Pt-deposited region along VACNTs and residual hydrophobic region of VANCTs without Pt strongly influences the cell performance,in particular at high current densities.When Pt nanoparticles deposit on the top depth of around 600 nm on VACNTs with a length of 4.6μm,the cell shows the highest performance,compared with others with various lengths of VACNTs.It delivers a maximum power output of 1.61 W cm^(-2)(H_(2)/O_(2),150 k Pa)and 0.79 W cm^(-2)(H_(2)/Air,150 k Pa)at Pt loading of 50μg cm^(-2),exceeding most of previously reported PEMFCs with Pt loading of<100μg cm^(-2).Even though the Pt loading is down to 30μg cm^(-2)(1.36 W cm^(-2)),the performance is also better than 100μg cm^(-2)(1.24 W cm^(-2))of commercial Pt/C,and presents better stability.This excellent performance is critical attributed to the ordered hydrophobic region providing sufficient mass passages to facilitate the fast water drainage at high current densities.This work gives a new understanding for oxygen reduction reaction occurred in VACNTs-based ordered electrodes,demonstrating the most possibility to achieve a substantial reduction in Pt loading<100μg cm^(-2) without sacrificing in performance.展开更多
Mass transport is crucial to the performance of proton exchange membrane fuel cells,especially at high current densities.Generally,the oxygen and the generated water share same transmission medium but move towards opp...Mass transport is crucial to the performance of proton exchange membrane fuel cells,especially at high current densities.Generally,the oxygen and the generated water share same transmission medium but move towards opposite direction,which leads to serious mass transfer problems.Herein,a series of patterned catalyst layer were prepared with a simple one-step impressing method using nylon sieves as templates.With grooves 100μm in width and 8μm in depth on the surface of cathode catalyst layer,the maximum power density of fuel cell increases by 10%without any additional durability loss while maintaining a similar electrochemical surface area.The concentration contours calculated by finite element analysis reveal that the grooves built on the surface of catalyst layer serve to accumulate the water nearby while oxygen tends to transfer through relatively convex region,which results from capillary pressure difference caused by the pore structure difference between the two regions.The separation of oxidant gas and generated water avoids mass confliction thus boosts mass transport efficiency.展开更多
The catalyst layer(CL)is the core component in determining the electrical-thermal-water performance and cost of proton exchange membrane fuel cell(PEMFC).Systemic analysis and rapid prediction tools are required to im...The catalyst layer(CL)is the core component in determining the electrical-thermal-water performance and cost of proton exchange membrane fuel cell(PEMFC).Systemic analysis and rapid prediction tools are required to improve the design efficiency of CL.In this study,a 3D multi-phase model integrated with the multi-level agglomerate model for CL is developed to describe the heat and mass transfer processes inside PEMFC.Moreover,a research framework combining the response surface method(RSM)and artificial neural network(ANN)model is proposed to conduct a quantitative analysis,and further a rapid and accurate prediction.With the help of this research framework,the effects of CL composition on the electrical-thermal-water performance of PEMFC are investigated.The results show that the mass of platinum,the mass of carbon,and the volume fraction of dry ionomer has a significant impact on the electrical-thermal-water performance.At the selected points,the sensitivity of the decision variables is ranked:volume fraction of dry ionomer>mass of platinum>mass of carbon>agglomerate radius.In particular,the sensitivity of the volume fraction of dry ionomer is over 50%at these points.Besides,the comparison results show that the ANN model could implement a more rapid and accurate prediction than the RSM model based on the same sample set.This in-depth study is beneficial to provide feasible guidance for high-performance CL design.展开更多
An extensive study has been conducted on the proton exchange membrane fuel cells （PEMFCs） with reducing Pt loading. This is commonly achieved by developing methods to increase the utilization of the platinum in the ...An extensive study has been conducted on the proton exchange membrane fuel cells （PEMFCs） with reducing Pt loading. This is commonly achieved by developing methods to increase the utilization of the platinum in the catalyst layer of the electrodes. In this paper, a novel process of the catalyst layers was introduced and investigated. A mixture of carbon powder and Nafion solution was sprayed on the glassy carbon electrode （GCE） to form a thin carbon layer. Then Pt particles were deposited on the surface by reducing hexachloroplatinic （IV） acid hexahydrate with methanoic acid. SEM images showed a continuous Pt gradient profile among the thickness direction of the catalytic layer by the novel method. The Pt nanowires grown are in the size of 3 nm （diameter） x l0 nm （length） by high solution TEM image. The novel catalyst layer was characterized by cyclic voltammetry （CV） and scanning electron microscope （SEM） as compared with commercial Pt/C black and Pt catalyst layer obtained from sputtering. The results showed that the platinum nanoparticles deposited on the carbon powder were highly utilized as they directly faced the gas diffusion layer and offered easy access to reactants （oxygen or hydrogen）.展开更多
The electrode ionomer plays a crucial role in the catalyst layer(CL) of a proton-exchange membrane fuel cell(PEMFC) and is closely associated with the proton conduction and gas transport properties,structural stabilit...The electrode ionomer plays a crucial role in the catalyst layer(CL) of a proton-exchange membrane fuel cell(PEMFC) and is closely associated with the proton conduction and gas transport properties,structural stability,and water management capability.In this review,we discuss the CL structural characteristics and highlight the latest advancements in ionomer material research.Additionally,we comprehensively introduce the design concepts and exceptional performances of porous electrode ionomers,elaborate on their structural properties and functions within the fuel cell CL,and investigate their effect on the CL microstructure and performance.Finally,we present a prospective evaluation of the developments in the electrode ionomer for fabricating CL,offering valuable insights for designing and synthesizing more efficient electrode ionomer materials.By addressing these facets,this review contributes to a comprehensive understanding of the role and potential of electrode ionomers for enhancing PEMFC performance.展开更多
The constant increase in energy demand and related environmental issues have made fuel cells an attractive technology as an alternative to conventional energy technologies.Like any technology,fuel cells face drawbacks...The constant increase in energy demand and related environmental issues have made fuel cells an attractive technology as an alternative to conventional energy technologies.Like any technology,fuel cells face drawbacks that scientific society has been focused on to improve and optimize the overall technology.Thus,the cost is the main inhibitor for this technology due to the significantly high cost of the materials used in catalyst layers.The current discussion mainly focuses on the fundamental electrochemical half-cell reaction of hydrogen oxidation reaction(HOR)and oxygen reduction reaction(ORR)that are taking place in the catalyst layers consisting of Platinum-based and Platinum-non noble metals.For this purpose,studies from the literature are presented and analyzed by highlighting and comparing the variations on the catalytic activity within the experimental catalyst layers and the conventional ones.Furthermore,an economic analysis of the main platinum group metals(PGMs)such as Platinum,Palladium and Ruthenium is introduced by presenting the economic trends for the last decade.展开更多
Proton exchange membrane fuel cell(PEMFC)is a device that converts chemical energy into electrical energy,and the design of catalytic layer of its air electrode should not only contain abundant and easily accessible r...Proton exchange membrane fuel cell(PEMFC)is a device that converts chemical energy into electrical energy,and the design of catalytic layer of its air electrode should not only contain abundant and easily accessible reactive sites,but also have highly connected electrons,protons,and reactants mass transfer channels.Therefore,the electrode must possess a specific three-dimensional(3D)geometric structure and orderly distributed functionalized channels to ensure full utilization of catalytic active sites and enable continuous reaction processes.Herein,we review the recent research progress of porous carbon-based oxygen reduction reaction(ORR)catalysts for cathodic catalytic layer in PEMFC.Firstly,the reaction mechanism of PEMFC as well as the optimization principles were briefly introduced,followed by a detailed discussion on the design and preparation of PEMFC cathode ORR catalysts with hierarchical porous structures from the main methods,such as hard template,soft template,combination of hard and soft templates,self-assembled template,electrostatic spinning,and 3D printing.Additionally,the performance characterization of PEMFC cathode catalysts with porous structure was elaborated from three aspects:electrochemical performance testing,numerical investigations of oxygen transport,and in-situ characterization and operation techniques.Finally,the future challenges and opportunities for the PEMFC cathodic catalytic layer were envisioned.展开更多
Appropriate hydrophobicity and porosity of the proton-exchange membrane fuel cell(PEMFC)cathode catalyst layer(CCL)are essential for efficient charge and mass transport.In this study,the effects of the CCL hydrophobic...Appropriate hydrophobicity and porosity of the proton-exchange membrane fuel cell(PEMFC)cathode catalyst layer(CCL)are essential for efficient charge and mass transport.In this study,the effects of the CCL hydrophobicity and porosity on PEMFC performance were comprehensively investigated.Compared to a normal CCL,a cathode hydrophobic duallayer catalyst structure(with a 2:1 Pt loading ratio between the inner and outer layers and 9.3%polytetrafluoroethylene(PTFE)in the outer layer)exhibited a 29.8%increase in power density.Among the tested pore-forming agents,ammonium bicarbonate(NH_4HCO_(3))was the most suitable because of its low pyrolysis temperature.The maximum power density of the CCL with a porous structure(prepared with a Pt/C:NH_4HCO_(3)mass ratio of 1:3)was 38.3%higher than that of the normal CCL.By simultaneously optimizing the pore structure and hydrophobicity of the CCL,the maximum power density of the cathode hydrophobic dual-layer CCL(DCL)with pores showed a 44.7%increase compared to that of the normal CCL.This study demonstrates for the first time that simultaneously optimizing cathode porosity and hydrophobicity can enhance PEMFC performance.展开更多
The influence of the drop-casted nickel boride catalyst loading on glassy carbon electrodes was investigated in a spectroelectrochemical ATR-FTIR thin-film flow cell applied in alkaline glycerol electrooxidation.The c...The influence of the drop-casted nickel boride catalyst loading on glassy carbon electrodes was investigated in a spectroelectrochemical ATR-FTIR thin-film flow cell applied in alkaline glycerol electrooxidation.The continuously operated radial flow cell consisted of a borehole electrode positioned 50μm above an internal reflection element enabling operando FTIR spectroscopy.It is identified as a suitable tool for facile and reproducible screening of electrocatalysts under well-defined conditions,additionally providing access to the selectivities in complex reaction networks such as glycerol oxidation.The fast product identification by ATR-IR spectroscopy was validated by the more time-consuming quantitative HPLC analysis of the pumped electrolyte.High degrees of glycerol conversion were achieved under the applied laminar flow conditions using 0.1 M glycerol and 1 M KOH in water and a flow rate of 5μL min^(–1).Conversion and selectivity were found to depend on the catalyst loading,which determined the catalyst layer thickness and roughness.The highest loading of 210μg cm^(–2)resulted in 73%conversion and a higher formate selectivity of almost 80%,which is ascribed to longer residence times in rougher films favoring readsorption and C–C bond scission.The lowest loading of 13μg cm^(–2)was sufficient to reach 63%conversion,a lower formate selectivity of 60%,and,correspondingly,higher selectivities of C_(2)species such as glycolate amounting to 8%.Thus,only low catalyst loadings resulting in very thin films in the fewμm thickness range are suitable for reliable catalyst screening.展开更多
The catalyst layer （CL） of proton exchange mem-brane fuel cell （PEMFC） involves various particles and pores in meso-scale, which has an important effect on the mass, charge （proton and electron） and heat transpo...The catalyst layer （CL） of proton exchange mem-brane fuel cell （PEMFC） involves various particles and pores in meso-scale, which has an important effect on the mass, charge （proton and electron） and heat transport coupled with the electrochemical reactions. The coarse-grained molecular dynamics （CG-MD） method is employed as a meso-scale structure reconstruction technique to mimic the self-organization phenomena in the fabrication steps of a CL. The meso-scale structure obtained at the equilibrium state is further analyzed by molecular dynamic （MD） software to provide the necessary microscopic parameters for understanding of multi-scale and-physics processes in CLs. The primary pore size distribution （PSD） and active platinum （Pt） surface areas are also calculated and then compared with the experiments. In addition, we also highlight the implementation method to combine microscopic elementary kinetic reaction schemes with the CG-MD approaches to provide insight into the reactions in CLs. The concepts from CG modeling with particle hydrodynamics （SPH） and the problems on coupling of SPH with finite element modeling （FEM） methods are further outlined and discussed to understand the effects of the meso-scale transport phenomena in fuel cells.展开更多
The performance of an electrocatalyst, which is needed e.g. for key energy conversion reactions such as hydrogen evolution, oxygen reduction or CO2 reduction, is determined not only by the inherent structure of active...The performance of an electrocatalyst, which is needed e.g. for key energy conversion reactions such as hydrogen evolution, oxygen reduction or CO2 reduction, is determined not only by the inherent structure of active sites but also by the properties of the interfacial structures at catalytic surfaces. Ionic liquids（ILs）, as a unique class of metal salts with melting point below 100 ℃, present themselves as ideal modulators for manipulations of the interfacial structures. Due to their excellent properties such as good chemical stability, high ionic conductivity, wide electrochemical windows and tunable solvent properties the performance of electrocatalysts can be substantially improved through ILs. In the current minireview, we highlight the critical role of the IL phase at the microenvironments created by the IL, the liquid electrolyte, catalytic nanoparticles and/or support materials, by detailing the promotional effect of IL in electrocatalysis as reaction media, binders, and surface modifiers. Updated exemplary applications of IL in electrocatalysis are given and moreover, the latest developments of IL modified electrocatalysts following the ＂Solid Catalyst with Ionic Liquid Layer（SCILL）＂ concept are presented.展开更多
Computational models that ensure accurate and fast responses to the variations in operating conditions,such as the cell tem-perature and relative humidity(RH),are essential monitoring tools for the real-time control o...Computational models that ensure accurate and fast responses to the variations in operating conditions,such as the cell tem-perature and relative humidity(RH),are essential monitoring tools for the real-time control of proton exchange membrane(PEM)fuel cells.To this end,fast cell-area-averaged numerical simulations are developed and verifi ed against the present experiments under various RH levels.The present simulations and measurements are found to agree well based on the cell voltage(polarization curve)and power density under variable RH conditions(RH=40%,RH=70%,and RH=100%),which verifi es the model accuracy in predicting PEM fuel cell performance.In addition,computationally feasible reduced-order models are found to deliver a fast output dataset to evaluate the charge/heat/mass transfer phenomena as well as water production and two-phase fl ow transport.Such fast and accurate evaluations of the overall fuel cell operation can be used to inform the real-time control systems that allow for the improved optimization of PEM fuel cell performance.展开更多
To understand the catalytic conversion of lignin into high-value products,lignin depolymerization was performed using a layered polymetallic oxide(CuMgAlO_(x))catalyst.The effects of the conversion temperature,hydroge...To understand the catalytic conversion of lignin into high-value products,lignin depolymerization was performed using a layered polymetallic oxide(CuMgAlO_(x))catalyst.The effects of the conversion temperature,hydrogen pressure,and reaction time were studied,and the ability of CuMgAlO_(x)to break the C–O bond was evaluated.The CuMgAlO_(x)(Mg/Al=3:1)catalyst contained acidic sites and had a relatively homogeneous elemental distribution with a high pore size and specific surface area.Theβ-O-4 was almost completely converted by disassociating the C–O bond,resulting in yields of 14.74%ethylbenzene,47.58%α-methylphenyl ethanol,and 36.43%phenol.The highest yield of lignin-derived monophenols was 85.16%under reaction conditions of 280℃ and 3 Mpa for 4 h.As the reaction progressed,depolymerization and condensation reactions occurred simultaneously.Higher temperatures(>280℃)and pressures(>3 Mpa)tended to produce solid char.This study establishes guidelines for the high-value application of industrial lignin in the catalytic conversion of polymetallic oxides.展开更多
文摘To evaluate the H_(2)O_(2)‐tolerance of non‐Pt oxygen reduction reaction(ORR)catalysts as well as in‐vestigate the H_(2)O_(2)‐induced decay mechanism,the selection of an appropriate H_(2)O_(2) concentration is a prerequisite.However,the concentration criterion is still unclear because of the lack of in‐operando methods to determine the actual concentration of H_(2)O_(2) in fuel cell catalyst layers.In this work,an electrochemical probe method was successfully established to in‐operando monitor the H_(2)O_(2) in non‐Pt catalyst layers for the first time.The local concentration of H_(2)O_(2) was revealed to reach 17 mmol/L,which is one order of magnitude higher than that under aqueous electrodes test conditions.Powered by the new knowledge,a concentration criterion of at least 17 mmol/L is suggested.This work fills in the large gap between aqueous electrode tests and the real fuel cell working conditions,and highlights the importance of in‐operando monitoring methods.
基金supported by the National Natural Science Foundation of China(Grant No.52394204)the Shanghai Municipal Science and Technology Major Project,and Shanghai Jiao Tong University Decision Consulting,China(JCZXSJB2024-12).
文摘Electrochemical CO_(2)reduction(CO_(2)RR)is a promising technology for mitigating global climate change.The catalyst layer(CL),where the reduction reaction occurs,plays a pivotal role in determining mass transport and electrochemical performance.However,accurately characterizing local structures and quantifying mass transport remains a significant challenge.To address these limitations,a systematic characterization framework based on deep learning(DL)is proposed.Five semantic segmentation models,including Segformer and DeepLabV3plus,were compared with conventional image processing techniques,among which DeepLabV3plus achieved the highest segmentation accuracy(>91.29%),significantly outperforming traditional thresholding methods(72.35%–77.42%).Experimental validation via mercury intrusion porosimetry(MIP)confirmed its capability to precisely extract key structural parameters,such as porosity and pore size distribution.Furthermore,a series of ionomer content gradient experiments revealed that a CL with an ionomer/catalyst(I/C)ratio of 0.2 had the optimal pore network structure.Numerical simulations and electrochemical tests demonstrated that this CL enabled a twofold increase in gas diffusion distance,thereby promoting long-range mass transport and significantly enhancing CO production rates.This work establishes a multi-scale analysis framework integrating“structural characterization,mass transport simulation,and performance validation,”offering both theoretical insights and practical guidance for the rational design of CO_(2)RR CLs.
基金supported by the National Key Research and Development Program(2021YFB4001701)National Nature Science Foundation of China(52376074)the Fundamental Research Funds for the Central Universities.
文摘Improving the performance of proton exchange membrane fuel cells(PEMFCs)requires deep understanding of the reac-tive transport processes inside the catalyst layers(CLs).In this study,a particle-overlapping model is developed for accu-rately describing the hierarchical structures and oxygen reactive transport processes in CLs.The analytical solutions derived from this model indicate that carbon particle overlap increases ionomer thickness,reduces specific surface areas of ionomer and carbon,and further intensifies the local oxygen transport resistance(R_(other)).The relationship between Rother and roughness factor predicted by the model in the range of 800-1600 sm^(-1) agrees well with the experiments.Then,a multiscale model is developed by coupling the particle-overlapping model with cell-scale models,which is validated by comparing with the polarization curves and local current density distribution obtained in experiments.The relative error of local current density distribution is below 15%in the ohmic polarization region.Finally,the multiscale model is employed to explore effects of CL structural parameters including Pt loading,I/C,ionomer coverage and carbon particle radius on the cell performance as well as the phase-change-induced(PCI)flow and capillary-driven(CD)flow in CL.The result demonstrates that the CL structural parameters have significant effects on the cell performance as well as the PCI and CD flows.Optimizing the CL structure can increase the current density and further enhance the heat-pipe effect within the CL,leading to overall higher PCI and CD rates.The maximum increase of PCI and CD rates can exceed 145%.Besides,the enhanced heat-pipe effect causes the reverse flow regions of PCI and CD near the CL/PEM interface,which can occupy about 30%of the CL.The multiscale model significantly contributes to a deep understanding of reactive trans-port and multiphase heat transfer processes inside PEMFCs.
基金supported by National Natural Science Foundation of China(22279091)Fundamental Funds for the Central Universities。
文摘The catalyst layer is an essential component of fuel cells,exerting a decisive influence on performance,particularly under degradation processes.Characterization derived from accelerated stress tests(ASTs)provide valuable insights into the long-term degradation from the perspective of changes in physical and chemical properties,thereby offering a scientific foundation for evaluating advanced materials and strategies.In this review,multidimensional and multi-characterization application scenarios based on ASTs data are systematically summarized.Firstly,the degradation mechanism of catalyst layer(CL)under AST conditions is discussed,with an emphasis on platinum aging and carbon support corrosion.In addition,electrochemical and microphysical characterization tools applicable to different AST test protocols,such as electrochemical surface area(ECSA),electrochemical impedance spectrum(EIS)mapping combined with distribution of relaxation times(DRT),and microscopic physical evolution and tracking techniques for each internal chemical component,are also presented in detail.Finally,through the existing research progress and hotspots,the application prospect of data fusion is elaborated and the important research direction of material optimization and performance prediction based on AST data is emphasized,aiming to provide insights into the study of catalytic layer degradation in fuel cells and promote the continuous development of the field.
基金financially supported by the Natural Sciences and Engineering Research Council of Canada(NSERC)via a Discovery Grant,and Canadian Urban Transit Research&Innovation Consortium(CUTRIC)via Project No.160028.
文摘Catalyst layer(CL)is the core component of proton exchange membrane(PEM)fuel cells,which determines the performance,durability,and cost.However,difficulties remain for a thorough understanding of the CLs’inhomogeneous structure,and its impact on the physicochemical and electrochemical properties,operating performance,and durability.The inhomogeneous structure of the CLs is formed during the manufacturing process,which is sensitive to the associated materials,composi-tion,fabrication methods,procedures,and conditions.The state-of-the-art visualization and characterization techniques are crucial to examine the CL structure.The structure-dependent physicochemical and electrochemical properties are then thoroughly scrutinized in terms of fundamental concepts,theories,and recent progress in advanced experimental techniques.The relation between the CL structure and the associated effective properties is also examined based on experimental and theoretical findings.Recent studies indicated that the CL inhomogeneous structure also strongly affects the performance and degradation of the whole fuel cell,and thus,the interconnection between the fuel cell performance,failure modes,and CL structure is comprehensively reviewed.An analytical model is established to understand the effect of the CL structure on the effective properties,performance,and durability of the PEM fuel cells.Finally,the challenges and prospects of the CL structure-associated studies are highlighted for the development of high-performing PEM fuel cells.
基金financially supported by the National Natural Science Foundation of China(Nos.52073214 and 22075211)Guangxi Natural Science Fund for Distinguished Young Scholars(No.2024GXNSFFA010008)+5 种基金Natural Science Foundation of Shandong Province(Nos.ZR2023MB049 and ZR2021QB129)China Postdoctoral Science Foundation(No.2020M670483)Science Foundation of Weifang University(No.2023BS11)supported by the open research fund of the Laboratory of Xinjiang Native Medicinal and Edible Plant Resources Chemistry at Kashi Universitysupported by the Tianhe Qingsuo Open Research Fund of TSYS in 2022 and NSCC-TJNankai University Large-scale Instrument Experimental Technology R&D Project(No.21NKSYJS09)。
文摘Unraveling the essence of electronic structure effected by d-d orbital coupling of transition metal and methanol oxidation reaction(MOR)performance can fundamentally guide high efficient catalyst design.Herein,density functional theory(DFT)calculations were performed at first to study the d–d orbital interaction of metallic Pt Pd Cu,revealing that the incorporation of Pd and Cu atoms into Pt system can enhance d-d electron interaction via capturing antibonding orbital electrons of Pt to fill the surrounding Pd and Cu atoms.Under the theoretical guidance,Pt Pd Cu medium entropy alloy aerogels(Pt Pd Cu MEAAs)catalysts have been designed and systematically screened for MOR under acid,alkaline and neutral electrolyte.Furthermore,DFT calculation and in-situ fourier transform infrared spectroscopy analysis indicate that Pt Pd Cu MEAAs follow the direct pathway via formate as the reactive intermediate to be directly oxidized to CO_(2).For practical direct methanol fuel cells(DMFCs),the Pt Pd Cu MEAAs-integrated ultra-thin catalyst layer(4–5μm thickness)as anode exhibits higher peak power density of 35 m W/cm^(2) than commercial Pt/C of 20 m W/cm^(2)(~40μm thickness)under the similar noble metal loading and an impressive stability retention at a 50-m A/cm^(2) constant current for 10 h.This work clearly proves that optimizing the intermediate adsorption capacity via d-d orbital coupling is an effective strategy to design highly efficient catalysts for DMFCs.
基金supported by the Taishan Scholar Program of Shandong Province,China(tsqn202211162)National Natural Science Foundation of China(22372088 and 22102079)+1 种基金Natural Science Foundation of Shandong Province of China(ZR2021YQ10)the Materials/Parts Technology Development Program(RS-2024-00432627)funded by the Ministry of Trade,Industry and Energy,Korea.
文摘Reducing the Ir loading while preserving catalytic performance and mechanical robustness in anodic catalyst layers remains a critical challenge for the large-scale implementation of proton exchange membrane water electrolysis(PEMWE).Herein,we present a structural engineering strategy involving neodymium-doped Ir/IrO_(2)(Nd-Ir/IrO_(2))hollow nanospheres with precisely adjustable shell thickness and cavity dimensions.The optimized catalyst demonstrates excellent oxygen evolution reaction(OER)performance in acidic media,achieving a remarkably low overpotential of 259 mV at a benchmark current density of 10 mA cm^(-2) while exhibiting substantially enhanced durability compared to commercial IrO_(2) and Ir/IrO_(2) counterparts.Notably,the Nd-Ir/IrO_(2) catalyst delivers a mass activity of 541.6 A gIr^(-1) at 1.50 V vs RHE,representing a 74.5-fold enhancement over conventional IrO_(2).Through comprehensive electrochemical analysis and advanced characterization techniques reveal that,the hierarchical hollow architecture simultaneously addresses multiple critical requirements:(i)abundant exposed active sites enabled by an enhanced electrochemical surface area,(ii)optimized mass transport pathways through engineered porosity,and(iii)preserved structural integrity via a continuous conductive framework,collectively enabling significant Ir loading reduction without compromising catalytic layer performance.Fundamental mechanistic investigations further disclose that Nd doping induces critical interfacial Nd-O-Ir configurations that stabilize lattice oxygen,together with intensified electron effect among mixed valent Ir that inhibits the overoxidation of Ir active sites during the OER process,synergistically ensuring enhanced catalytic durability.Our work establishes a dual-modulation paradigm integrating nanoscale architectural engineering with atomic-level heteroatom doping,providing a viable pathway toward high-performance PEMWE systems with drastically reduced noble metal requirements.
基金finically supported by the National Natural Science Foundation of China(22075055)the Guangxi Science and Technology Project(AB16380030)the Innovation Project of Guangxi Graduate Education(YCSW2020052)。
文摘Reducing a Pt loading with improved power output and durability is essential to promote the large-scale application of proton exchange membrane fuel cells(PEMFCs).To achieve this goal,constructing optimized structure of catalyst layers with efficient mass transportation channels plays a vital role.Herein,PEMFCs with order-structured cathodic electrodes were fabricated by depositing Pt nanoparticles by Ebeam onto vertically aligned carbon nanotubes(VACNTs)growth on Al foil via plasma-enhanced chemical vapor deposition.Results demonstrate that the proportion of hydrophilic Pt-deposited region along VACNTs and residual hydrophobic region of VANCTs without Pt strongly influences the cell performance,in particular at high current densities.When Pt nanoparticles deposit on the top depth of around 600 nm on VACNTs with a length of 4.6μm,the cell shows the highest performance,compared with others with various lengths of VACNTs.It delivers a maximum power output of 1.61 W cm^(-2)(H_(2)/O_(2),150 k Pa)and 0.79 W cm^(-2)(H_(2)/Air,150 k Pa)at Pt loading of 50μg cm^(-2),exceeding most of previously reported PEMFCs with Pt loading of<100μg cm^(-2).Even though the Pt loading is down to 30μg cm^(-2)(1.36 W cm^(-2)),the performance is also better than 100μg cm^(-2)(1.24 W cm^(-2))of commercial Pt/C,and presents better stability.This excellent performance is critical attributed to the ordered hydrophobic region providing sufficient mass passages to facilitate the fast water drainage at high current densities.This work gives a new understanding for oxygen reduction reaction occurred in VACNTs-based ordered electrodes,demonstrating the most possibility to achieve a substantial reduction in Pt loading<100μg cm^(-2) without sacrificing in performance.
基金supported by the National Natural Science Foundation of China(21838003,91834301)the Shanghai Scientific and Technological Innovation Project(18JC1410600,19JC1410400)+2 种基金the Social Development Program of Shanghai(17DZ1200900)the Innovation Program of Shanghai Municipal Education Commissionthe Fundamental Research Funds for the Central Universities(222201718002)。
文摘Mass transport is crucial to the performance of proton exchange membrane fuel cells,especially at high current densities.Generally,the oxygen and the generated water share same transmission medium but move towards opposite direction,which leads to serious mass transfer problems.Herein,a series of patterned catalyst layer were prepared with a simple one-step impressing method using nylon sieves as templates.With grooves 100μm in width and 8μm in depth on the surface of cathode catalyst layer,the maximum power density of fuel cell increases by 10%without any additional durability loss while maintaining a similar electrochemical surface area.The concentration contours calculated by finite element analysis reveal that the grooves built on the surface of catalyst layer serve to accumulate the water nearby while oxygen tends to transfer through relatively convex region,which results from capillary pressure difference caused by the pore structure difference between the two regions.The separation of oxidant gas and generated water avoids mass confliction thus boosts mass transport efficiency.
基金financially supported by the National Key R&D Program of China (2022YFE0101300)the National Natural Science Foundation of China (52176203)。
文摘The catalyst layer(CL)is the core component in determining the electrical-thermal-water performance and cost of proton exchange membrane fuel cell(PEMFC).Systemic analysis and rapid prediction tools are required to improve the design efficiency of CL.In this study,a 3D multi-phase model integrated with the multi-level agglomerate model for CL is developed to describe the heat and mass transfer processes inside PEMFC.Moreover,a research framework combining the response surface method(RSM)and artificial neural network(ANN)model is proposed to conduct a quantitative analysis,and further a rapid and accurate prediction.With the help of this research framework,the effects of CL composition on the electrical-thermal-water performance of PEMFC are investigated.The results show that the mass of platinum,the mass of carbon,and the volume fraction of dry ionomer has a significant impact on the electrical-thermal-water performance.At the selected points,the sensitivity of the decision variables is ranked:volume fraction of dry ionomer>mass of platinum>mass of carbon>agglomerate radius.In particular,the sensitivity of the volume fraction of dry ionomer is over 50%at these points.Besides,the comparison results show that the ANN model could implement a more rapid and accurate prediction than the RSM model based on the same sample set.This in-depth study is beneficial to provide feasible guidance for high-performance CL design.
基金supported by the Royal Academy of Engineering,United Kingdom
文摘An extensive study has been conducted on the proton exchange membrane fuel cells （PEMFCs） with reducing Pt loading. This is commonly achieved by developing methods to increase the utilization of the platinum in the catalyst layer of the electrodes. In this paper, a novel process of the catalyst layers was introduced and investigated. A mixture of carbon powder and Nafion solution was sprayed on the glassy carbon electrode （GCE） to form a thin carbon layer. Then Pt particles were deposited on the surface by reducing hexachloroplatinic （IV） acid hexahydrate with methanoic acid. SEM images showed a continuous Pt gradient profile among the thickness direction of the catalytic layer by the novel method. The Pt nanowires grown are in the size of 3 nm （diameter） x l0 nm （length） by high solution TEM image. The novel catalyst layer was characterized by cyclic voltammetry （CV） and scanning electron microscope （SEM） as compared with commercial Pt/C black and Pt catalyst layer obtained from sputtering. The results showed that the platinum nanoparticles deposited on the carbon powder were highly utilized as they directly faced the gas diffusion layer and offered easy access to reactants （oxygen or hydrogen）.
基金supported by the National Natu-ral Science Foundation of China(Nos.21625102,21971017,and 22102008)National Key Research and Development Program of China(No.2020YFB1506300)Postdoctoral Fund of China(Nos.2020T130055 and 2020M670143).
文摘The electrode ionomer plays a crucial role in the catalyst layer(CL) of a proton-exchange membrane fuel cell(PEMFC) and is closely associated with the proton conduction and gas transport properties,structural stability,and water management capability.In this review,we discuss the CL structural characteristics and highlight the latest advancements in ionomer material research.Additionally,we comprehensively introduce the design concepts and exceptional performances of porous electrode ionomers,elaborate on their structural properties and functions within the fuel cell CL,and investigate their effect on the CL microstructure and performance.Finally,we present a prospective evaluation of the developments in the electrode ionomer for fabricating CL,offering valuable insights for designing and synthesizing more efficient electrode ionomer materials.By addressing these facets,this review contributes to a comprehensive understanding of the role and potential of electrode ionomers for enhancing PEMFC performance.
文摘The constant increase in energy demand and related environmental issues have made fuel cells an attractive technology as an alternative to conventional energy technologies.Like any technology,fuel cells face drawbacks that scientific society has been focused on to improve and optimize the overall technology.Thus,the cost is the main inhibitor for this technology due to the significantly high cost of the materials used in catalyst layers.The current discussion mainly focuses on the fundamental electrochemical half-cell reaction of hydrogen oxidation reaction(HOR)and oxygen reduction reaction(ORR)that are taking place in the catalyst layers consisting of Platinum-based and Platinum-non noble metals.For this purpose,studies from the literature are presented and analyzed by highlighting and comparing the variations on the catalytic activity within the experimental catalyst layers and the conventional ones.Furthermore,an economic analysis of the main platinum group metals(PGMs)such as Platinum,Palladium and Ruthenium is introduced by presenting the economic trends for the last decade.
基金supported by the Natural Science Special Project of Scientific Research Program of Shaanxi Provincial Department of Education(No.24JK0468)the Youth Innovation Team of Shaanxi Universities(No.2022TD071)Xi’an Key Laboratory of Textile and Chemical Additives Performance Assessment Reward and Subsidy Project(No.2021JH-201-0004).
文摘Proton exchange membrane fuel cell(PEMFC)is a device that converts chemical energy into electrical energy,and the design of catalytic layer of its air electrode should not only contain abundant and easily accessible reactive sites,but also have highly connected electrons,protons,and reactants mass transfer channels.Therefore,the electrode must possess a specific three-dimensional(3D)geometric structure and orderly distributed functionalized channels to ensure full utilization of catalytic active sites and enable continuous reaction processes.Herein,we review the recent research progress of porous carbon-based oxygen reduction reaction(ORR)catalysts for cathodic catalytic layer in PEMFC.Firstly,the reaction mechanism of PEMFC as well as the optimization principles were briefly introduced,followed by a detailed discussion on the design and preparation of PEMFC cathode ORR catalysts with hierarchical porous structures from the main methods,such as hard template,soft template,combination of hard and soft templates,self-assembled template,electrostatic spinning,and 3D printing.Additionally,the performance characterization of PEMFC cathode catalysts with porous structure was elaborated from three aspects:electrochemical performance testing,numerical investigations of oxygen transport,and in-situ characterization and operation techniques.Finally,the future challenges and opportunities for the PEMFC cathodic catalytic layer were envisioned.
基金supported by the Basic Science Center Program for Ordered Energy Conversion of the National Natural Science Foundation of China(Grant No.52488201)the National Key R&D Program of China(Grant No.2021YFF0500504)the Fundamental Research Funds for the Central Universities。
文摘Appropriate hydrophobicity and porosity of the proton-exchange membrane fuel cell(PEMFC)cathode catalyst layer(CCL)are essential for efficient charge and mass transport.In this study,the effects of the CCL hydrophobicity and porosity on PEMFC performance were comprehensively investigated.Compared to a normal CCL,a cathode hydrophobic duallayer catalyst structure(with a 2:1 Pt loading ratio between the inner and outer layers and 9.3%polytetrafluoroethylene(PTFE)in the outer layer)exhibited a 29.8%increase in power density.Among the tested pore-forming agents,ammonium bicarbonate(NH_4HCO_(3))was the most suitable because of its low pyrolysis temperature.The maximum power density of the CCL with a porous structure(prepared with a Pt/C:NH_4HCO_(3)mass ratio of 1:3)was 38.3%higher than that of the normal CCL.By simultaneously optimizing the pore structure and hydrophobicity of the CCL,the maximum power density of the cathode hydrophobic dual-layer CCL(DCL)with pores showed a 44.7%increase compared to that of the normal CCL.This study demonstrates for the first time that simultaneously optimizing cathode porosity and hydrophobicity can enhance PEMFC performance.
文摘The influence of the drop-casted nickel boride catalyst loading on glassy carbon electrodes was investigated in a spectroelectrochemical ATR-FTIR thin-film flow cell applied in alkaline glycerol electrooxidation.The continuously operated radial flow cell consisted of a borehole electrode positioned 50μm above an internal reflection element enabling operando FTIR spectroscopy.It is identified as a suitable tool for facile and reproducible screening of electrocatalysts under well-defined conditions,additionally providing access to the selectivities in complex reaction networks such as glycerol oxidation.The fast product identification by ATR-IR spectroscopy was validated by the more time-consuming quantitative HPLC analysis of the pumped electrolyte.High degrees of glycerol conversion were achieved under the applied laminar flow conditions using 0.1 M glycerol and 1 M KOH in water and a flow rate of 5μL min^(–1).Conversion and selectivity were found to depend on the catalyst loading,which determined the catalyst layer thickness and roughness.The highest loading of 210μg cm^(–2)resulted in 73%conversion and a higher formate selectivity of almost 80%,which is ascribed to longer residence times in rougher films favoring readsorption and C–C bond scission.The lowest loading of 13μg cm^(–2)was sufficient to reach 63%conversion,a lower formate selectivity of 60%,and,correspondingly,higher selectivities of C_(2)species such as glycolate amounting to 8%.Thus,only low catalyst loadings resulting in very thin films in the fewμm thickness range are suitable for reliable catalyst screening.
文摘The catalyst layer （CL） of proton exchange mem-brane fuel cell （PEMFC） involves various particles and pores in meso-scale, which has an important effect on the mass, charge （proton and electron） and heat transport coupled with the electrochemical reactions. The coarse-grained molecular dynamics （CG-MD） method is employed as a meso-scale structure reconstruction technique to mimic the self-organization phenomena in the fabrication steps of a CL. The meso-scale structure obtained at the equilibrium state is further analyzed by molecular dynamic （MD） software to provide the necessary microscopic parameters for understanding of multi-scale and-physics processes in CLs. The primary pore size distribution （PSD） and active platinum （Pt） surface areas are also calculated and then compared with the experiments. In addition, we also highlight the implementation method to combine microscopic elementary kinetic reaction schemes with the CG-MD approaches to provide insight into the reactions in CLs. The concepts from CG modeling with particle hydrodynamics （SPH） and the problems on coupling of SPH with finite element modeling （FEM） methods are further outlined and discussed to understand the effects of the meso-scale transport phenomena in fuel cells.
基金supported by the funding of the German Research Council (DFG), which, within the framework of its Excellence Initiative, supports the Cluster of Excellence “Engineering of Advanced Materials” (www.eam.uni-erlangen.de) at the University of Erlangen-Nürnberg
文摘The performance of an electrocatalyst, which is needed e.g. for key energy conversion reactions such as hydrogen evolution, oxygen reduction or CO2 reduction, is determined not only by the inherent structure of active sites but also by the properties of the interfacial structures at catalytic surfaces. Ionic liquids（ILs）, as a unique class of metal salts with melting point below 100 ℃, present themselves as ideal modulators for manipulations of the interfacial structures. Due to their excellent properties such as good chemical stability, high ionic conductivity, wide electrochemical windows and tunable solvent properties the performance of electrocatalysts can be substantially improved through ILs. In the current minireview, we highlight the critical role of the IL phase at the microenvironments created by the IL, the liquid electrolyte, catalytic nanoparticles and/or support materials, by detailing the promotional effect of IL in electrocatalysis as reaction media, binders, and surface modifiers. Updated exemplary applications of IL in electrocatalysis are given and moreover, the latest developments of IL modified electrocatalysts following the ＂Solid Catalyst with Ionic Liquid Layer（SCILL）＂ concept are presented.
基金by the Natural Sciences and Engineering Research Council of Canada(NSERC)via a Discovery Grant,Canadian Urban Transit Research and Innovation Consortium(CUTRIC)(No.160028).
文摘Computational models that ensure accurate and fast responses to the variations in operating conditions,such as the cell tem-perature and relative humidity(RH),are essential monitoring tools for the real-time control of proton exchange membrane(PEM)fuel cells.To this end,fast cell-area-averaged numerical simulations are developed and verifi ed against the present experiments under various RH levels.The present simulations and measurements are found to agree well based on the cell voltage(polarization curve)and power density under variable RH conditions(RH=40%,RH=70%,and RH=100%),which verifi es the model accuracy in predicting PEM fuel cell performance.In addition,computationally feasible reduced-order models are found to deliver a fast output dataset to evaluate the charge/heat/mass transfer phenomena as well as water production and two-phase fl ow transport.Such fast and accurate evaluations of the overall fuel cell operation can be used to inform the real-time control systems that allow for the improved optimization of PEM fuel cell performance.
基金supported by the National Natural Science Fund for Distinguished Young Scholars(52125601).
文摘To understand the catalytic conversion of lignin into high-value products,lignin depolymerization was performed using a layered polymetallic oxide(CuMgAlO_(x))catalyst.The effects of the conversion temperature,hydrogen pressure,and reaction time were studied,and the ability of CuMgAlO_(x)to break the C–O bond was evaluated.The CuMgAlO_(x)(Mg/Al=3:1)catalyst contained acidic sites and had a relatively homogeneous elemental distribution with a high pore size and specific surface area.Theβ-O-4 was almost completely converted by disassociating the C–O bond,resulting in yields of 14.74%ethylbenzene,47.58%α-methylphenyl ethanol,and 36.43%phenol.The highest yield of lignin-derived monophenols was 85.16%under reaction conditions of 280℃ and 3 Mpa for 4 h.As the reaction progressed,depolymerization and condensation reactions occurred simultaneously.Higher temperatures(>280℃)and pressures(>3 Mpa)tended to produce solid char.This study establishes guidelines for the high-value application of industrial lignin in the catalytic conversion of polymetallic oxides.
