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    28 December 2018, Volume 24 Issue 6
    Special Issue in Honor of Professor Baolian Yi on His 80th Birthday
    Table of Contents
    2018, 24(6):  0-0. 
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    Special Issue in Honor of Professor Baolian Yi on His 80th Birthday
    Chinese Society of Electrochemistry
    2018, 24(6):  571-571.  doi:10.13208/j.electrochem.180872
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    Research Progress in Hydrogen Evolution Low Noble/Non-Precious Metal Catalysts of Water Electrolysis
    LI Yang, LUO Zhao-yan, GE Jun-jie, LIU Chang-peng, XING Wei
    2018, 24(6):  572-588.  doi:10.13208/j.electrochem.180855
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    Hydrogen energy technology with hydrogen as an energy carrier is gaining more and more attention due to its cleanliness and high energy density. Hydrogen fuel cell vehicles have been listed as one of the ultimate energy technologies in the 21st century. Among them, sustainable hydrogen production technology is a necessary prerequisite for the future development of hydrogen energy economy. Electrolyzed water technology driven by renewable resources represents an important way to support the sustainable development of hydrogen energy economy. The development and utilization of high activity, low cost hydrogen evolution catalysts is a key factor in improving the efficiency and reducing the cost of water electrolysis technology. This paper mainly introduces the recent research progress of hydrogen evolution catalysts including low platinum catalysts and non-platinum transition metal catalysts such as metal sulfides metal phosphides, metal selenides, etc; catalytic properties, synthesis methods, and structure-catalytic properties. Finally, the advantages and challenges of water electrolysis low platinum and non-platinum transition metal catalysts in the future development are prospected.
    Recent Progress in Pt-Based Catalysts for Oxygen Reduction Reaction
    LI Jing, FENG Xin, WEI Zi-dong
    2018, 24(6):  589-601.  doi:10.13208/j.electrochem.180850
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    One major challenge for a large-scale commercialization of the proton-exchange membrane fuel cells (PEMFCs) technologies that enable a shift to ‘zero-emission’ personal transportation, is the expensive and unstable Pt catalysts, which are mainly used to catalyze the sluggish kinetics of the oxygen reduction reaction (ORR) occurred on the air electrode of PEMFCs. Many research works have targets to improve the stability of Pt-based catalysts and to construct Pt/transitional metal alloys with low Pt loading amount. Herein, we provide a minireview for the Pt-based ORR catalysts based on our recent work, which covers a brief background introduction, the stability improvement of pure Pt catalysts, the construction of Pt-alloy type catalysts and a future perspective. It is believed that the alloy catalysts with a sophistical structure design at an atomic level owns a promising future prospect.
    Constructions of Noble Metal Nanocrystals with Specific Crystal Facets and High Surface Area
    CHEN Qiao-li, LI Hui-qi, JIANG Ya-qi, XIE Zhao-xiong
    2018, 24(6):  602-614.  doi:10.13208/j.electrochem.180851
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    Noble metal nanocrystals (NCs) have widespread applications in catalysis. Their catalytic performances are strongly related to the surface structures while the atomic utilization efficiency of noble metal is considerably correlated with the surface area. Thus, advantages of both specific surface structure and large surface area are highly required to show off simultaneously so as to optimize the catalytic performance and decrease the usage of noble metal. However, it seems that the two advantages are incompatible with each other in one NC since it is difficult for small NCs to keep their specific facets, while NCs with specific surface structure usually crystallize into the large size leading to small surface area. The construction of noble metal NCs with specific surface area and large surface area is a great challenge. This review introduces the strategies to prepare noble metal NCs integrated with both specific surface facets and high surface area from the controllable synthesis of morphologies. The current researches in this field are summarized by introducing specific cases. Subsequently, typical applications in catalysis are presented to demonstrate the advantages of noble metal NCs with both specific facets and high surface area. Finally, the perspectives concerning about the development tendency in this field are put forward.
    Fuel Cells Reactor for Chemicals and Electric Energy Cogeneration
    HENG Zhi-lin, YUAN Xiao-zi, YIN Yi-mei,MA Zi-feng
    2018, 24(6):  615-627.  doi:10.13208/j.electrochem.180857
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    As an energy conversion device, fuel cells can efficiently convert chemical energy into electrical energy. With the developing of technology, it is used as a reactor to conduct the synthesis of high value-added chemicals while generating electrical energy. Having benefits such as mild reaction conditions, controllability of the reaction process, high selectivity of the product, as well as high efficiency of energy utilization, it is widely used in many fields such as preparation of high value-added industrial products, gas separation, water treatment, etc. This paper introduces the current trends and statuses of fuel cell reactors in the cogeneration of chemicals and electric energy according to the reduction reaction at the cathode and the oxidation reaction of the anode. The problems related to the fuel cell reactor are described, and possible solutions are discussed in terms of the catalyst research, process research and others. Finally, the research in several new fuel cell reactors is briefly introduced and its development is prospected.
    Progress of Self-Humidifying Membrane Electrode Assembly for Low Temperature Proton Exchange Membrane Fuel Cell
    CHI Bin, YE Yue-kun, JIANG Shi-jie, LIAO Shi-jun
    2018, 24(6):  628-638.  doi:10.13208/j.electrochem.180860
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    The self/non-humidification membrane electrode assembly(SH-MEA)is an important pathway towards the self- humidification fuel cell and plays a crucial role for the large scale commercialization of low temperature proton exchange membrane fuel cell (LT-PEMFC), because it not only can reduce the volume and complexity of fuel cell system, resulting in the decrease of the cost, but also can improve the output power density of the fuel cell system. Currently, the researches on the self-humidifying MEA of LT-PEMFC mainly focus on three aspects: the preparation of self-humidification proton exchange membrane, the construction of self-humidification catalyst layer, and the construction of composite self-humidifying layers. In this paper, the research progress and development trend in self-humidifying MEA for low temperature proton exchange membrane fuel cell in recent years are reviewed.
    A Review of Proton Exchange Membrane Fuel Cell Catalyst Layer by Electrospinning
    LIU Yong, DING Han, SI De-chun, PENG Jie, ZHANG Jian-bo
    2018, 24(6):  639-654.  doi:10.13208/j.electrochem.180849
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    The limitation of catalyst layer for proton exchange membrane fuel cell (PEMFC) in cost, durability and performance constitutes the bottleneck for the commercialization of fuel cell vehicles. Electrospun catalyst layer, with high catalyst utilization, increased triple phase boundary (TPB) and triple phase channel (TPC), has been developed by many researchers. This paper reviews the research progress in the electrospun catalyst layer for PEMFC, combined with the author’s work. Firstly, the development progress of catalyst layer is summarized, and the catalyst layer is classified and analyzed based on its fabrication method and structure character. Next, the fabrication process, physical property characterization, electrochemical performance analysis and durability characterization of the electrospun nanofiber catalyst layer are described. Finally, further develoment tendency in catalyst layer for PEMFC is viewed by comparion of three kinds of catalyst layers from the viewpoints of TPB, TPC and mass production. Future research topics are discussed
    Stabilization Strategies of Pt Catalysts forProton Exchange Membrane Fuel Cells
    HE Da-ping,MU Shi-chun
    2018, 24(6):  655-663.  doi:10.13208/j.electrochem.180859
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    The low service lifetime of proton exchange membrane fuel cells (PEMFCs) is the main bottleneck for their commercial applications. One of the main factors is that the expensive metal Pt catalyst is easy to degradation under the harsh working environment of PEMFC (such as variable voltage, strong acidity, gas-liquid two-phase flow), which leads to the inevitable decay of the catalytic performance, thus, seriously restricting the lifetime of PEMFC. Therefore, the electrochemical stability of Pt-based electrocatalysts has become an important and hot topic to improve the PEMFC lifetime. In this paper, we review the recent development in enhancing the stability of Pt electrocatalysts for PEMFC, mainly focusing on the achievements obtained by our group, especially, the polymer stabilization strategy, carbon encapsulation/confinement stabilization strategy, and support stabilization strategy. In addition, the challenges in these Pt catalyst stabilization strategies are summarized, and the corresponding measures and future research trends in facing these challenges are suggested.
    Fuel cell performance curve after MEA optimization Structural Optimization of Low Pt Membrane Electrode Assembly
    RAO Yan, LI Shang, ZHOU Fen, TIAN Tian, ZHONG Qing, WAN Zhao-hui, TAN Jin-ting, PAN Mu
    2018, 24(6):  677-686.  doi:10.13208/j.electrochem.180843
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    Membrane electrode assemblies (MEAs) are the key component of proton exchange membrane fuel cell. For a long time, much attention has been paid to develop MEA technology. At present, the research, development and industrialization of fuel cell has entered a new era. More strict requirements for MEA, especially for the reduction of Pt loading with a challenging target of 0.125 mg·W-1 have to be met. In this paper, the performance losses under low Pt loading are analyzed in terms of activation polarization, ohm polarization and mass-transfer polarization. It is proposed that research should be focused on the activity of the catalyst under the fuel cell operating voltage (0.6 V ~ 0.8 V),and the reasonability of using charge-transfer resistance as the indicator of catalyst activity is discussed. In terms of optimization potential capacity, mass transfer polarization > activation polarization > ohm polarization. Residual performance loss associated with low cathode Pt loading can be mitigated by optimizing the catalytic layer structure, where oxygen flux through the ionomer film to the Pt surface should be minimized with high proton conduction.
    The Pilot Application of Electrochemical Impedance Spectroscopy on Dynamic Proton Exchange Membrane Fuel Cell
    GUO Jian-wei, WANG Jian-long
    2018, 24(6):  687-696.  doi:10.13208/j.electrochem.180854
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    By analyzing Electrochemical Impedance Spectroscopy (EIS) in applications of dynamic proton exchange membrane fuel cell (PEMFC), bottlenecks which restrict EIS tool development have been pointed out in this paper. Though the high-frequency resistance in EIS is largely accepted as cell inner-resistance, this can only be applied for cell with low current. The low-frequency resistance is difficult to be realized due to its relation with mass transfer. Furthermore, the improved Randles equivalent circuits are built up preliminarily, thus, penetrating into studies for mass transfer reaction, cell operation/degeneration, and high temperature fuel cell. Inspiringly, EIS is becoming an analyzing tool for stack and control core for electric-vehicle. Nevertheless, it is still pioneer challenge to make breakthrough towards transient EIS method based on multi-discipline convergence
    Morphological Control of PtCu2 Octahedron and Oxygen Reduction Electrocatalytic Performance of PtCu for Fuel Cell
    CAO Long-sheng, WAN Lei, SHAO Zhi-gang, YU Hong-mei, HOU Ming, YI Bao-lian
    2018, 24(6):  697-706.  doi:10.13208/j.electrochem.180848
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    Platinum acetylacetonate (Pt(acac)2) and copper acetylacetonate (Cu(acac)2) were co-reduced to prepare PtCu2 octahedron alloy catalyst in N,N-dimethylformamiade by solvothermal method. The PtCu2 showed lattice compression, and high ratio of non-oxidized Pt with high electronic binding energy. All those structural features contributed to weak adsorption strength of oxygen species on Pt and lower d-band centre position. The influence of structure-directing agent on morphology of PtCu alloy was systematically studied. In the half cell test, as a result of the uniform morphology and regular octahedron of PtCu2 formed, the mass activity and area specific activity of PtCu2/C reached 6.2 and 27.2 times, respectively, relative to those of Pt/C at 0.9 V vs. RHE. Furthermore, after the accelarated degradation test, the mass activity of PtCu2/C still reached 4.5 times compared to that of Pt/C.
    Effects of SO2 in Air on Performance of Direct Methanol Fuel Cell
    QIN Bin, JING Fen-ning, SUN Xue-jing, SUN Gong-quan, SUN Hai
    2018, 24(6):  707-714.  doi:10.13208/j.electrochem.180858
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    Direct methanol fuel cells (DMFC) generally use oxygen as an oxidant. Contaminants such as sulfides and nitrides in the air can affect the performance of the DMFC. In this work, the effects of SO2 on the performance of DMFC were investigated and the mechanism of poisoning was analyzed, by means of constant current discharge curve, polarization performance curve, cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). In the CV scan, the permeated methanol was oxidized at a low potential to eliminate its effect on the SO2 poisoning behavior test. The results showed that the SO2 poisoning resulted in a decrease in the electrochemical activity surface area (ECSA) of the catalyst. Meanwhile, the EIS data indicated that the poisoning led to an increase in the charge transfer resistance of the oxygen reduction reaction (ORR). Therefore, the poison accelerated decay of the open circuit voltage and operating voltage of the DMFC, and decreased the peak power density. Further investigations of three recovery strategies, dry air purging and load-shifting I-V operations could only partially restore the performance of DMFC. However, CV scanning could accomplish the recovery more completely.
    Caging Porous Co-N-C Nanocomposites in 3D Graphene as Active and Aggregation-Resistant electrocatalyst for Oxygen Reduction Reaction
    XIU Lu-yang,YU Meng-zhou,YANG Peng-ju,WANG Zhi-yu,QIU Jie-shan
    2018, 24(6):  715-725.  doi:10.13208/j.electrochem.180847
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    Oxygen reduction reaction (ORR) is the cornerstone reaction of many renewable energy technologies such as fuel cells and rechargeable metal-air batteries. The Pt-based electrocatalysts exhibit the highest activity toward ORR, but their large implementation is greatly prohibiting by unaffordable cost and inferior durability. During electrode manufacturing and electrochemical reaction, severe aggregation of catalyst nanoparticles induced by size effect further limits the operational performance of electrocatalysts. We report a new strategy for fabrication of active and aggregation-resistant ORR electrocatalyst by caging metal-organic frameworks derived Co-N-C nanocomposites in permeable and porous 3D graphene cages via sprayed drying the mixed colloids of ZIF-67 nanoparticles and graphene oxide, followed by annealing. The 3D graphene cages around Co-N-C nanocomposites not only provide a continuous conductive network for charge transfer, but also prevent the active phase from aggregation during electrode manufacturing and electrochemical reactions. When evaluated as an ORR electrocatalyst, the material exhibited comparable activity but superior stability to commercial Pt/C catalyst in an alkaline electrolyte.
    Fe-N Doped Hollow Carbon Nanospheres Linked by Carbon Nanotubes for Oxygen Reduction Reaction
    ZHANG Ya-lin, CHEN Chi, ZOU Liang-liang, ZOU Zhi-qing, YANG Hui
    2018, 24(6):  726-732.  doi:10.13208/j.electrochem.180842
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    The development of non-precious metal catalysts for oxygen reduction reaction (ORR) is essential for large-scale application of proton exchange membrane fuel cells. Herein, we present the in situ formed Fe-N doped hollow carbon nanospheres linked by carbon nanotubes composite, synthesized by using ZIF-8 as sacrificed template to form polydopamine (PDA) hollow nanospheres, followed by complexing with FeCl3, high temperature heat-treatment and NH3-etching. ZIF-8 was gradually decomposed simultaneously with PDA coating due to the loss of Zn2+ grabbed by PDA. NH3 etching resulted in the improved surface area, while the reducibility of NH3 resulted in the formation of Fe4N nanoparticles, which benefits the ORR activity of the catalyst. The half-wave potential of the as-prepared of PDA-Fe/N/C-NH3 was 0.79 V, only 60 mV lower than that of commercial Pt/C. The stability and methanol tolerance of PDA-Fe/N/C-NH3 were even superior to that of commercial Pt/C, indicating the good potential of PDA-Fe/N/C-NH3 for the application of fuel cells.
    Facile Synthesis of Pt-Cu Alloy Nanodendrites as High-Performance Electrocatalysts for Oxygen Reduction Reaction
    LUO Liu-xuan, WEI Guang-hua, SHEN Shui-yun, ZHU Feng-juan, KE Chang-chun, YAN Xiao-hui, ZHANG Jun-liang
    2018, 24(6):  733-739.  doi:10.13208/j.electrochem.180856
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    Structures and compositions have significant effects on the catalytic properties of nanomaterials. Herein, a facile etching-based method was employed to synthesize Pt-Cu nanodendrites (NDs) with uniform and homogeneous alloy structures for enhancing oxygen reduction reaction (ORR). The formation of dendritic morphology was ascribed to the etching effect caused by the oxidative etchants of the Br-/O2 pair. The atomic ratio of Pt/Cu in Pt-Cu NDs could be easily tuned by altering the ratio of the Pt/Cu precursors, without deteriorating the dendritic morphology. The most active carbon-supported Pt1Cu1 NDs (Pt1Cu1 NDs/C) exhibited the area-specific activity of 1.17 mA·cm-2@0.9 V (vs. RHE), which is ~5.32 times relative to that of commercial Pt/C. Moreover, Pt1Cu1 NDs/C also possessed a remarkable electrochemical durability, preserving its superior ORR catalytic activity even after 12000 potential cycles during the accelerated degradation test. Such excellent catalytic activity and electrochemical durability of Pt1Cu1 NDs/C toward ORR were resulted from the combined electronic and structural effects, which are imparted by the Pt-Cu alloy structure and the dendritic morphology.
    Palladium Adatoms on Gold Nanoparticles as Electrocatalysts for Ethanol Electro-Oxidation in Alkaline Solutions
    CHEN Hui-mei, ZHU Shang-qian, HUANG Jia-le, SHAO Min-hua
    2018, 24(6):  740-747.  doi:10.13208/j.electrochem.180841
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    Palladium (Pd) is a good catalyst for ethanol electro-oxidation in alkaline solutions. The activity of Pd is further improved in this study by modifying the gold (Au) nanoparticles with Pd adatoms using a simple spontaneous deposition process. The Pd overlayer on the Au core (Au@Pd) is un-uniform with some Au atoms exposed to the electrolyte. The activity of Au@Pd/C toward ethanol oxidation reaction (EOR) is much higher than that of Pd/C in an alkaline solution. The peak current density of Au@Pd/C is 4.6 times higher than that of Pd/C with a 100 mV lower onset potential. The enhanced activity may be due to the electronic effect from the Au core, and the bifunctional reaction mechanism.
    Acid Treated Carbon as Anodic Electrocatalysts toward Direct Ascorbic Acid Alkaline Membrane Fuel Cells
    CHEN He-mu, QIU Chen-xi, CONG Yuan-yuan, LIU Hui-yuan
    2018, 24(6):  748-756.  doi:10.13208/j.electrochem.180844
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    In order to improve the hydrophilicity and electrocatalytic activity, commercial carbon black (BP 2000) was subjected to acid treatment to obtain acid-treated carbon (ATC). The generation of rich oxygen-containing groups on the surface of the ATC was proved by X-ray photoelectron spectra (XPS), Fourier transform-infra red spectra (FTIR), thermogravimetric analysis (TG) and contact angle measurement. UV-vis spectra were firstly recorded to calculate activation energy (Ea) of ascorbic acid (AA) chemical oxidation in alkaline conditions by oxygen in air and the Ea value was determined to be 37.1 kJ·mol-1. Additionally, electrochemical impedance spectra (EIS) were used to evaluate unprecedented Eaelectrochem of ATC as electrocatalysts toward ascorbic acid (AA) oxidation in alkaline media. The Eaelectrochem values of electrochemical oxidation in alkaline membrane electrode assembly (MEA) setup of a single cell without and with ATC as the anodic electrocatalysts were calculated to be 34.5 and 26.5 kJ·mol-1, respectively. The diminished Eaelectrochem suggests that ATC does function as an effective anodic electrocatalyst. Furthermore, the ATC was applied in direct ascorbic acid alkaline membrane fuel cell (DAAFC) for the first time. We optimized a series of parameters for the fabrication of MEAs including catalyst coated membrane (CCM) or catalyst coated gas diffusion layer membrane (CDM), loading of anodic electrocatalyst, and ionomer content in the electrocatalyst slurry. It turned out that the CCM with the ATC loading of 0.5 mg·cm-2 and 25wt% ionomer reached a high power density of 18.5 mW·cm-2, which is higher than that of using PtRu/C as anodic electrocatalyst (less than 5.0 mW·cm-2). In addition, the DAAFC fed with 15 mL·min-1 of the fuel containing 0.5 mol·L-1 AA and 1 mol·L-1 NaOH aq. could stably hold a power density at 4 mW·cm-2 for 25 min.
    Pd/C Catalysts for CO2 Electroreduction to CO:Pd Loading Effect
    GAO Dun-feng, YAN Cheng-cheng, WANG Guo-xiong, BAO Xin-he
    2018, 24(6):  757-765.  doi:10.13208/j.electrochem.180845
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    Nanostructured heterogeneous catalysts have been widely used in the electrochemical carbon dioxide (CO2) reduction reaction (CO2RR), which can simultaneously achieve the electrocatalytic conversion of CO2 to fuels and the storage of renewable energy sources. Carbon supported palladium nanoparticles (Pd/C) catalysts have been previously reported to show excellent CO2RR performance. However, the crucial role of the metal loading in supported electrocatalysts has been rarely reported. In this work, we study the Pd loading effect on the structure of Pd/C catalysts as well as their activity and selectivity of CO2RR to CO. The Pd loadings in Pd/C catalysts were well controlled by an effective liquid synthesis method. The Pd nanoparticles were homogeneously dispersed on the carbon support, and the Pd loading played a minor role in the particle size. The as-prepared Pd/C catalysts were studied in an optimized electrolyte, 0.1 mmol·L-1 KHCO3. It shows a volcano relationship between CO Faradaic efficiency (FE) and the Pd loading, with the highest CO FE of 91.2% over the 20wt% Pd/C catalyst at -0.89 V versus the reversible hydrogen electrode (vs. RHE). The geometric CO partial current density had a positive correlation with the Pd loading, while the highest turnover frequency for CO production was observed over the 2.5wt% Pd/C catalyst (~ 918 h-1 at -0.89 V vs. RHE). The Pd loading effects on the activity and selectivity of CO2RR to CO could be attributed to the number of active sites, reaction kinetics, and the stabilization of key intermediates, as well as the mass transport of reactants, intermediates and products. This work provides new insight into the loading effect, an important reactivity descriptor determining the CO2RR performance.
    Voltage Distribution of Self-Humidifying Air-Cooled PEMFC
    TAN Kai-feng, CHEN Wei-rong, HAN Ming, ZHANG Xue-xia
    2018, 24(6):  766-771.  doi:10.13208/j.electrochem.180852
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    In this work, the self-adaptive characteristics of self-humidifying air-cooled PEMFC stack was investigated. The performance and the unit-cell voltage distribution of the stack were measured and analyzed through the unit-cell I-V curve fitting. The operating conditions for this experimental study were set as follows: hydrogen pressure at the anode was 2 bar, the fan power used for the reactant oxygen feed and stack cooling was at 0.3 W, and the duration and time gap of water purged from hydrogen chamber were 1 s and 10 s, respectively. The experimental results showed that the self-humidifying air-cooled PEMFC stack used for this work could be in stable operation with a certain fan power, e.g., 0.3 W, at self-adaptive mode without the requirement of external control circuit. The unit voltage distribution of the air-cooled PEMFC stack was highly affected by the load current. Under the operation with higher current density, the unit-cell voltage distribution of the stack was less uniform due to the difference in the internal resistance of the unit-cells and the excessive temperature existed in the stack. Based on the data analyses, an approximate exponential relationship was found between the voltage fluctuation rate and the load current density.
    Durability Performance of the High-Power Fuel Cell System
    WANG Ke-yong, SHI Wei-yu, WANG Ren-fang, LIU Jia, HOU Zhong-jun
    2018, 24(6):  772-776.  doi:10.13208/j.electrochem.180846
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    Fuel cell durability is the crucial challenge in fuel cell vehicle, and the lifetime of more than 5000 hours is believed to be necessary for vehicle application. Few works on durability test of the full fuel cell system have been reported. In this work, the long lifetime HySYS-30 fuel cell system was developed in Sunrise Power based on the improved MEA durability and system control strategy. The durability performance of the system was investigated under vehicle duty cycle for more than 6000 hours, and only 8.1% performance loss was observed, implying that the durability of HySYS-30 fuel cell system could be more than 5000 hours.
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