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The distribution and diffusion coefficient of water inside a Nafion® membrane in a running fuel cell under transient conditions analyzed by operando time-resolved CARS spectroscopy 用时间分辨CARS光谱法分析了燃料电池运行过程中水在Nafion®膜内的分布和扩散系数
IF 4.5 Q2 CHEMISTRY, PHYSICAL Pub Date : 2022-01-01 DOI: 10.1016/j.powera.2021.100080
Hiromichi Nishiyama Dr. Ph.D. , Akihiro Iiyama Prof. Ph.D. , Junji Inukai Prof. Ph.D.

The performance and stability of polymer electrolyte membrane fuel cells (PEMFCs) are directly affected by the distribution of water molecules inside the membrane. In this study, coherent anti-Stokes Raman scattering (CARS) spectroscopy was used to measure the distribution of water in a Nafion® membrane under transient conditions after increasing the current density. At the cathodic surface of the membrane, an overshoot in amount of water was observed as a result of the increase in the rate of water production and electro-osmosis, while at the other locations in the membrane was observed a gradual increase of water as a result of water transport. The calculation of the water diffusion coefficient during power generation was subsequently carried out, which was consistent with the results of the previous values obtained statically.

聚合物电解质膜燃料电池(pemfc)的性能和稳定性直接受到膜内水分子分布的影响。在本研究中,相干反斯托克斯拉曼散射(CARS)光谱测量了在瞬态条件下增加电流密度后,水在Nafion®膜中的分布。在膜的阴极表面,由于产水和电渗透速率的增加,观察到水量的过量,而在膜的其他位置,由于水的运输,观察到水的逐渐增加。随后进行了发电过程中水扩散系数的计算,结果与之前的静力计算结果一致。
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引用次数: 3
19F MAS NMR study on anion intercalation into graphite positive electrodes from binary-mixed highly concentrated electrolytes 高浓度二元混合电解质负离子嵌入石墨正极的19fmas NMR研究
IF 4.5 Q2 CHEMISTRY, PHYSICAL Pub Date : 2021-12-01 DOI: 10.1016/j.powera.2021.100075
Joop Enno Frerichs , Lukas Haneke , Martin Winter , Michael Ryan Hansen , Tobias Placke

Dual-graphite batteries (DGBs), which are based on anion intercalation into graphite positive electrodes, exhibit great potential for stationary energy storage due to use of more sustainable and low-cost electrode materials and processing routes. Binary-mixed highly concentrated electrolytes (HCEs) appeal highly suitable for the high operating voltages of DGBs, although the lack of sufficient insights into the formation of graphite intercalation compounds (GICs) limits the cell performance in terms of specific capacity and lifetime so far. Herein, anion intercalation from single-salt HCEs (LiPF6 and LiBF4) and an equimolar binary mixture of LiPF6/LiBF4 are studied in graphite || Li metal cells, revealing an improved performance in terms of specific capacity and Coulombic efficiency in the order LiPF6 > LiPF6/LiBF4 > LiBF4. LiBF4-based cells exhibit an increased onset potential for anion intercalation and higher area specific impedance, suggesting an ineffective interphase formation at graphite. X-ray diffraction reveals GIC formation, while a lower stage number is achieved for the LiBF4-based HCE. 19F MAS NMR spectroscopy analysis at various states-of-charge confirms no significant charge transfer between the intercalated anions and the graphite host and suggest preferred intercalation of PF6- compared to BF4- as well as a high translational and/or rotational mobility of the intercalated anions.

双石墨电池(DGBs)是一种基于负离子插入石墨正极的电池,由于使用了更可持续和低成本的电极材料和加工路线,在固定储能方面表现出巨大的潜力。二元混合的高浓度电解质(HCEs)非常适合dgb的高工作电压,尽管迄今为止缺乏对石墨插层化合物(gic)形成的充分了解限制了电池在比容量和寿命方面的性能。本文研究了单盐HCEs (LiPF6和LiBF4)和LiPF6/LiBF4等摩尔二元混合物在石墨锂金属电池中的阴离子插入,揭示了LiPF6和LiBF4顺序在比容量和库仑效率方面的性能提高;LiPF6 / LiBF4比;LiBF4。基于libf4的细胞表现出更高的阴离子插入电位和更高的面积比阻抗,表明石墨层间相形成无效。x射线衍射显示GIC形成,而基于libf4的HCE达到了较低的级数。在各种电荷状态下的19F MAS NMR分析证实了插入阴离子和石墨宿主之间没有明显的电荷转移,并且表明与BF4相比,PF6更倾向于插入,并且插入阴离子具有较高的平移和/或旋转迁移率。
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引用次数: 1
An all-extruded tubular vanadium redox flow cell - Characterization and model-based evaluation 全挤压管式钒氧化还原流动电池-表征和基于模型的评价
IF 4.5 Q2 CHEMISTRY, PHYSICAL Pub Date : 2021-12-01 DOI: 10.1016/j.powera.2021.100077
Simon Ressel , Peter Kuhn , Simon Fischer , Michael Jeske , Thorsten Struckmann

The vanadium redox flow battery (VRFB) as one of the most promising electrochemical storage systems for stationary applications still needs further cost reductions. Tubular cell designs might reduce production costs by extrusion production of cell components and small sealing lengths. Based on a first study of the authors [1], this work demonstrates the feasibility of extruded tubular VRFB cells with high power density in the flow-by electrode configuration. Extruded cell components are the perfluorosulfonic acid cation exchange membrane with a diameter of 5.0 mm and carbon composite current collectors. The cell performance is experimentally characterized by polarization curve, ohmic resistance and galvanostatic cycling measurements. A maximum volumetric power density of 407 kW/m3 and a maximum current density of 500 mA/cm2 can be achieved. A non linear Ecell/i-model is used to evaluate exchange and limiting current densities while in-situ half cell SoC monitoring is applied to evaluate the extruded membrane.

钒氧化还原液流电池(VRFB)作为固定化应用中最有前途的电化学存储系统之一,仍需进一步降低成本。管状电池设计可以通过挤压生产电池组件和较小的密封长度来降低生产成本。基于作者的第一项研究[1],这项工作证明了在流动电极配置下具有高功率密度的挤压管状VRFB电池的可行性。挤压电池组件为直径为5.0 mm的全氟磺酸阳离子交换膜和碳复合集流器。通过极化曲线、欧姆电阻和恒流循环测量对电池性能进行了实验表征。最大体积功率密度为407 kW/m3,最大电流密度为500 mA/cm2。非线性Ecell/i模型用于评估交换和极限电流密度,而原位半电池SoC监测用于评估挤压膜。
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引用次数: 3
Nanoscale pore measurements in an all-solid-state lithium-ion battery with ultra-small-angle X-ray scattering (USAXS) 全固态锂离子电池纳米孔径的超小角x射线散射(USAXS)测量
IF 4.5 Q2 CHEMISTRY, PHYSICAL Pub Date : 2021-12-01 DOI: 10.1016/j.powera.2021.100076
M. Kodama , A. Takeuchi , M. Uesugi , T. Miyuki , H. Yasuda , S. Hirai

In a high performance all-solid-state lithium-ion battery (ASSLiB), lithium-ion should be smoothly transported to minimize overpotential. Nanoscale pores in the ASSLiB can inhibit ionic transportation; therefore, the pore structure should be measured and nanoscale pores should be prevented for high performance batteries. In this study, laboratory-scale ultra-small-angle X-ray scattering (USAXS) measurements are proposed to evaluate the nanoscale pores in ASSLiBs. The results measured with the USAXS are validated by comparing them with synchrotron radiation (SR) X-ray nanotomography data. The pore volumetric density distributions from the USAXS measurements are very close to those from SR X-ray nanotomography; this demonstrates that the nanoscale pores in ASSLiBs can be measured by USAXS. USAXS measurements of pore structures of solid electrolytes prepared from micron-scale and submicron-scale particles solid electrolyte (SE) reveal that the pore structure is not simply dependent on the SE particle size.

在高性能全固态锂离子电池(ASSLiB)中,锂离子应该平稳输送,以最小化过电位。ASSLiB中纳米级孔隙可以抑制离子的迁移;因此,为了高性能电池,必须测量孔隙结构,防止纳米级孔隙的产生。在这项研究中,提出了实验室尺度的超小角x射线散射(USAXS)测量来评估asslib中的纳米级孔隙。通过与同步辐射(SR) x射线纳米层析成像数据的比较,验证了USAXS测量结果的有效性。USAXS测量的孔隙体积密度分布与SR x射线纳米层析成像非常接近;这表明用USAXS可以测量asslib的纳米级孔隙。用USAXS对微米级和亚微米级固体电解质(SE)颗粒制备的固体电解质的孔隙结构进行了测量,结果表明,固体电解质的孔隙结构并不仅仅取决于SE颗粒的大小。
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引用次数: 2
Effect of roll press on consolidation and electric/ionic-path formation of electrodes for all-solid-state battery 辊压对全固态电池电极固结和电/离子路径形成的影响
IF 4.5 Q2 CHEMISTRY, PHYSICAL Pub Date : 2021-12-01 DOI: 10.1016/j.powera.2021.100078
Maria Yokota, Takuro Matsunaga

This study investigated unpressed and pressed electrodes with the synchrotron radiation X-ray computed laminography (CL) technique to clarify the relationship between the packing structure formation of an electrode processed with a roll press and the performance of all-solid-state batteries. Additionally, we evaluated the length and thickness of percolation paths constructed by the electrode particles using the 3-dimensional structure obtained by the X-ray CL measurement. The smallest packing fraction was in the cathode layers in both the pressed and unpressed electrodes. The cathode packing fraction had a non-uniform distribution shape as a function of the layer thickness. A similar distribution shape was maintained after pressing, except near the surface in contact with the pressing roller. Pressing caused the packing fraction of the cathode layer to become much larger than the unpressed one, especially near the surface where it significantly increased. The thickness of the percolation paths in the cathode layer also increased after pressing. Furthermore, we discovered that the cathode local path thickness, measured by using regions segmented by packing fraction values, had a linear relationship with the packing fraction. Consequently, the performance bottle neck is caused by the local layer that has the smallest packing fraction.

本研究利用同步辐射x射线计算机层析(CL)技术对未压电极和压电极进行了研究,以阐明辊压处理电极的填料结构形成与全固态电池性能之间的关系。此外,我们利用x射线CL测量获得的三维结构评估了电极颗粒构建的渗透路径的长度和厚度。在受压电极和未受压电极的阴极层中,填充率最小。阴极填料分数随层厚呈非均匀分布。除与压辊接触的表面附近外,压后均保持相似的分布形状。压紧导致阴极层的填充物比例比未压紧的填充物比例大得多,特别是在表面附近填充物比例显著增加。压实后阴极层中渗透路径的厚度也有所增加。此外,我们发现阴极局部路径厚度(用填充分数值分割的区域测量)与填充分数呈线性关系。因此,性能瓶颈是由具有最小填充分数的局部层引起的。
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引用次数: 2
Thermal risk evaluation of concentrated electrolytes for Li-ion batteries 锂离子电池用浓电解质热风险评价
IF 4.5 Q2 CHEMISTRY, PHYSICAL Pub Date : 2021-12-01 DOI: 10.1016/j.powera.2021.100079
Liwei Zhao, Atsushi Inoishi, Shigeto Okada

Concentrated electrolytes have been attracting increasing attention due to their unique properties. However, despite the concern about their thermal stability, few research has been done on their exothermic behaviors, especially with the coexistence of electrodes. Herein, we report the results of detailed investigation into the thermal properties of LiBF4, LiPF6, LiTFSI, and LiFSI/carbonate concentrated solutions and their thermal behaviors with the coexistence of fully lithiated graphite. Concentrated LiBF4 solutions showed no practical application possibilities because they were unstable on C6Li. Increasing the salt concentration decreased the thermal stability of LiPF6/PC solutions with the coexistence of C6Li. The organic salt dominated the thermal behavior of the solution when mixed with C6Li. A drastic exothermic reaction happened at 210–220 °C when C6Li was mixed with LiFSI solutions, indicating a very high thermal risk of LiFSI carbonate solutions as LIB electrolytes. In contrast, LiTFSI solutions showed much milder reactions with C6Li. On the other hand, because of the different LiF content in SEI, the exothermic onset temperature of the C6Li mixture with the concentrated solution increased in the order of LiFSI > LiTFSI > LiPF6. Comprehensively, concentrated LiTFSI electrolytes should be a good choice for LIB from the standpoint of battery safety.

浓缩电解质因其独特的性质而受到越来越多的关注。然而,尽管人们关注其热稳定性,但对其放热行为的研究很少,特别是在电极共存的情况下。本文详细研究了LiBF4、LiPF6、LiTFSI和LiFSI/碳酸盐浓溶液的热性能,以及它们在完全锂化石墨共存时的热行为。浓缩的LiBF4溶液由于在C6Li上不稳定,没有实际应用的可能性。随着盐浓度的增加,与C6Li共存的LiPF6/PC溶液的热稳定性降低。当与C6Li混合时,有机盐主导了溶液的热行为。当C6Li与LiFSI溶液混合时,在210-220°C发生了剧烈的放热反应,表明LiFSI碳酸溶液作为LIB电解质具有很高的热风险。相比之下,LiTFSI溶液与C6Li的反应温和得多。另一方面,由于SEI中LiF含量的不同,C6Li混合物与浓溶液的放热起始温度依次为LiFSI >LiTFSI祝辞LiPF6。综上所述,从电池安全的角度来看,浓缩的LiTFSI电解质应该是LIB的一个不错的选择。
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引用次数: 0
Conductive porous carbon (CPC) as an alternative to reticulated vitreous carbon (RVC) in lead acid battery current collectors 导电多孔碳(CPC)替代网状玻璃碳(RVC)用于铅酸电池集流
IF 4.5 Q2 CHEMISTRY, PHYSICAL Pub Date : 2021-12-01 DOI: 10.1016/j.powera.2021.100074
Kamil Wróbel , Jakub Lach , Justyna Wróbel , Piotr Podsadni , Andrzej Czerwiński

Thea article presents the latest research on reticulated carbon collectors in lead-acid batteries. A comparison of the performance characteristics of lead-acid cells and batteries based on two porous conductive carbon materials is presented: commercially available reticulated vitreous carbon (RVC), used in earlier studies, and porous conductive carbon (CPC) developed at the Faculty of Chemistry, University of Warsaw. Lead layers electrodeposited on CPC had better properties and more uniform thickness. Carbon-based negative and positive plates were tested regarding their capacity using different current rates and cycle life. Experiments on complete 2 and 12 V batteries are presented as well. CPC is proven to be as good material as RVC for use as current collectors in lead-acid cells. Obtained results show that there are reticulated carbon materials different from RVC with properties that allow them to be successfully employed in construction of both negative and positive plates in lead-acid batteries.

本文介绍了铅酸电池网状集碳器的最新研究进展。介绍了基于两种多孔导电碳材料的铅酸电池和电池的性能特征的比较:在早期研究中使用的市售网状玻璃碳(RVC)和华沙大学化学系开发的多孔导电碳(CPC)。在CPC上电沉积的铅层性能更好,厚度更均匀。用不同的电流速率和循环寿命测试了碳基负极和正极板的容量。并对完整的2 V和12 V电池进行了实验。在铅酸电池中,CPC被证明是与RVC一样好的集流材料。结果表明,不同于RVC的网状碳材料具有不同的性能,可以成功地应用于铅酸电池的正负极板结构。
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引用次数: 4
Investigating oxidative stability of lithium-ion battery electrolytes using synthetic charge-discharge profile voltammetry 利用合成充放电曲线伏安法研究锂离子电池电解质的氧化稳定性
IF 4.5 Q2 CHEMISTRY, PHYSICAL Pub Date : 2021-10-01 DOI: 10.1016/j.powera.2021.100071
Alma Mathew , Matthew J. Lacey , Daniel Brandell

Electrolytes are an integral part of any electrochemical energy storage systems, including batteries. Among the many properties which determine the applicability of a Li-ion battery electrolyte, electrochemical stability – and for high voltage electrodes, in particular anodic stability – is a key parameter to consider. Despite being simple and straightforward to employ, the conventional linear sweep voltammetry (LSV) technique often leads to an over-estimation of the oxidative stability. In this study, an alternative approach termed Synthetic Charge-discharge Profile Voltammetry (SCPV) is explored to investigate the oxidative electrolyte stability. We have found this to be a convenient method of quantifying the anodic stability of the electrolyte in a more practically representative manner, in which passivation kinetics and electrode potential changes at the electrode-electrolyte interface are more appropriately reproduced. The viability of this technique is explored with liquid electrolytes based on ether, carbonate, sulfone and carbonate-sulfone mixtures, all with lithium hexafluorophosphate (LiPF6) salt, tested for a potential profile equivalent to LiNi0.5Mn1.5O4 electrodes. The credibility of this technique is validated by correlations to the coulombic efficiencies of corresponding half-cells.

电解质是包括电池在内的任何电化学储能系统的组成部分。在决定锂离子电池电解液适用性的众多特性中,电化学稳定性——以及高压电极,特别是阳极稳定性——是需要考虑的一个关键参数。传统的线性扫描伏安法(LSV)虽然简单易用,但往往会导致对氧化稳定性的过高估计。在这项研究中,一种替代方法被称为合成充放电曲线伏安法(SCPV)被探索来研究氧化电解质的稳定性。我们发现这是一种方便的方法,以一种更实际的代表性的方式量化电解质的阳极稳定性,其中钝化动力学和电极电位在电极-电解质界面的变化更适当地再现。该技术的可行性与基于乙醚、碳酸盐、砜和碳酸盐岩-砜混合物的液体电解质进行了探讨,所有液体电解质都含有六氟磷酸锂(LiPF6)盐,测试了相当于LiNi0.5Mn1.5O4电极的电位分布。通过与相应半电池的库仑效率的相关性验证了该技术的可靠性。
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引用次数: 0
Exploring the structural uniformity and integrity of protonic ceramic thin film electrolyte using wet powder spraying 湿粉末喷涂法研究质子陶瓷薄膜电解质的结构均匀性和完整性
IF 4.5 Q2 CHEMISTRY, PHYSICAL Pub Date : 2021-10-01 DOI: 10.1016/j.powera.2021.100067
Wuxiang Feng , Wei Wu , Congrui Jin , Meng Zhou , Wenjuan Bian , Wei Tang , Joshua Y. Gomez , Richard Boardman , Dong Ding

Thin protonic ceramic electrolyte contributes to lower ohmic resistance and enhances electrochemical performance of protonic ceramic electrochemical cells. However, manufacturing of large-scale thin electrolyte remains a challenge. Wet powder spraying is an attractive technique to deposit <10 μm thin electrolyte when advanced atomizing techniques and optimized spraying process are integrated. Here ultrasonic atomization is integrated in the wet powder spray technique to reduce the thickness of electrolyte. Moreover, a parametric study is conducted to optimize the wet powder spray process to deposit uniform and crack-free electrolyte film. It is illustrated that tuning of solid loading rates and spray passes can affect the morphology of the as-sprayed electrolyte film, enabling the structural compactness of the sintered electrolyte layer. To maintain chemical stability of the electrolyte layer during sintering, effect of sintering temperature is further investigated to produce a physically thin, structurally dense, and chemically homogeneous electrolyte layer. The protonic ceramic electrochemical cells fabricated with optimized spraying and sintering parameters demonstrate excellent performance under both fuel cell and electrolysis modes. In addition, the cells exhibit remarkable structural integrity during redox and long-term stability tests.

薄的质子陶瓷电解质有助于降低质子陶瓷电化学电池的欧姆电阻,提高其电化学性能。然而,大规模薄电解质的制造仍然是一个挑战。当先进的雾化技术和优化的喷涂工艺相结合时,湿式粉末喷涂是一种极具吸引力的沉积10 μm薄电解质的技术。在这里,超声波雾化与湿粉喷涂技术相结合,以减少电解质的厚度。此外,还对湿式粉末喷涂工艺进行了参数化研究,以获得均匀无裂纹的电解质膜。结果表明,调整固体加载率和喷涂道数可以影响喷涂电解质膜的形貌,使烧结电解质层结构致密。为了在烧结过程中保持电解质层的化学稳定性,进一步研究了烧结温度的影响,以制备物理薄、结构致密、化学均匀的电解质层。采用优化的喷涂和烧结工艺制备的质子陶瓷电化学电池在燃料电池和电解模式下均表现出优异的性能。此外,在氧化还原和长期稳定性测试中,细胞表现出显著的结构完整性。
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引用次数: 8
A surprising relation between operating temperature and stability of anion exchange membrane fuel cells 阴离子交换膜燃料电池工作温度与稳定性的惊人关系
IF 4.5 Q2 CHEMISTRY, PHYSICAL Pub Date : 2021-10-01 DOI: 10.1016/j.powera.2021.100066
Karam Yassin , Igal G. Rasin , Sapir Willdorf-Cohen , Charles E. Diesendruck , Simon Brandon , Dario R. Dekel

Anion-exchange membrane fuel cells (AEMFCs) show substantially enhanced (initial) performance and efficiency with the increase of operational temperature (where typical values are below 80 °C). This is directly due to the increase in reaction and mass transfer rates with temperature. Common sense suggests however that the increase of ionomeric material chemical degradation kinetics with temperature is likely to offset the above mentioned gain in performance and efficiency. In this computational study we investigate the combined effect of a high operating temperature, up to 120 °C, on the performance and stability of AEMFCs. Our modeling results demonstrate the expected positive impact of operating temperature on AEMFC performance. More interestingly, under certain conditions, AEMFC performance stability is surprisingly enhanced as temperature increases. While increasing cell temperature enhances degradation kinetics, it simultaneously improves water diffusivity through the membrane, resulting in higher hydration levels at the cathode. This, in turn, encourages a decrease in ionomer chemical degradation which depends on the hydration as well as on temperature, leading to a significant increase in AEMFC performance stability and, therefore, in its lifetime. These findings predict the possible advantage (and importance), in terms of performance and durability, of developing high-temperature AEMFCs for automotive and other applications.

阴离子交换膜燃料电池(aemfc)的性能和效率随着工作温度(典型值低于80°C)的增加而显著增强。这是由于反应速率和传质速率随温度的增加而直接引起的。然而,常识表明,离子材料化学降解动力学随温度的增加可能抵消上述性能和效率的增益。在本计算研究中,我们研究了高达120°C的高工作温度对aemfc性能和稳定性的综合影响。我们的建模结果显示了预期的工作温度对AEMFC性能的积极影响。更有趣的是,在一定条件下,AEMFC的性能稳定性随着温度的升高而惊人地增强。在提高电池温度增强降解动力学的同时,它同时提高了水通过膜的扩散率,从而提高了阴极的水化水平。这反过来又促进了离子单体化学降解的减少,这取决于水合作用和温度,从而显著提高了AEMFC的性能稳定性,从而延长了其使用寿命。这些发现预测了开发用于汽车和其他应用的高温aemfc在性能和耐用性方面可能具有的优势(和重要性)。
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引用次数: 13
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