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Operando X-ray radiography of liquid water distribution in 100 mm polymer electrolyte fuel cell channels 对 100 毫米聚合物电解质燃料电池通道中的液态水分布进行 X 射线操作成像
IF 4.7 3区 工程技术 Q1 Chemistry Pub Date : 2024-06-18 DOI: 10.1016/j.elecom.2024.107772
Akihiko Kato , Satoshi Yamaguchi , Wataru Yoshimune , Kazuhisa Isegawa , Masashi Maeda , Daisuke Hayashi , Takahisa Suzuki , Satoru Kato

Preventing the accumulation of water in the gas diffusion layer (GDL) proves effective in enhancing the performance of polymer electrolyte fuel cells (PEFCs). To understand the water transport phenomena in GDLs and channels of PEFCs, cell hardware for operando synchrotron X-ray radiography was developed with a 100 mm channel length, facilitating the separate quantification of liquid water in the cathode and anode GDLs. The presence of liquid water in the cathode and anode GDLs was confirmed during operation with a supply of dry gas in a counter-flow configuration. Furthermore, the amount of liquid water in the cathode and anode GDLs increased toward the cathode inlet, while the amount of water in the cathode and anode channel regions increased toward each outlet. The liquid water distribution in the GDLs along the channel direction can be attributed to water transport from cathode to anode (back-diffusion), decreasing toward the anode outlet. Therefore, conducting radiography experiments aligned parallel to the GDLs and perpendicular to the channel could provide valuable insights for a more comprehensive understanding of water transport in cells.

事实证明,防止水在气体扩散层(GDL)中积聚可有效提高聚合物电解质燃料电池(PEFC)的性能。为了了解 PEFC 的气体扩散层和通道中的水传输现象,我们开发了通道长度为 100 毫米的用于操作同步辐射 X 射线成像的电池硬件,便于对阴极和阳极气体扩散层中的液态水进行单独量化。阴极和阳极 GDL 中液态水的存在已在以逆流配置供应干燥气体的运行过程中得到证实。此外,阴极和阳极 GDL 中的液态水量向阴极入口方向增加,而阴极和阳极通道区域中的水量则向每个出口方向增加。GDL 中的液态水沿通道方向的分布可归因于水从阴极向阳极的传输(反向扩散),而向阳极出口方向的分布则有所减少。因此,进行平行于 GDLs 并垂直于通道的射线照相实验可为更全面地了解细胞中的水传输提供有价值的见解。
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引用次数: 0
Real-time and operando observation of intermediates on TiO2 photoelectrocatalysis by soft X-ray absorption spectroscopy 利用软 X 射线吸收光谱对 TiO2 光电催化中间产物进行实时和操作观察
IF 5.4 3区 工程技术 Q1 Chemistry Pub Date : 2024-06-08 DOI: 10.1016/j.elecom.2024.107771
Kaoruho Sakata , Kenta Amemiya

The oxygen evolution reaction (OER) on the TiO2 surface at the solid–liquid interface was observed in real-time and operando using fluorescence-yield X-ray absorption spectroscopy (XAS) in the soft X-ray region. The OER was observed during a potential sweep with UV light on or off, focusing on the oxygen K-edge XAS. Although conventional XAS measurements require long measurement times, the spectra during the reaction were obtained every 3 s in the present experiment via wavelength-dispersive XAS technique. An increase in the X-ray absorption intensity at approximately 533.8 eV was observed during the potential sweep only with UV light on. The observed spectral change is discussed in relation to the reaction mechanism of the OER. The present technique can be applied to a wide range of analyses of (photo-) electrocatalysis and electrochemical reactions at solid–liquid interfaces to observe their products and intermediates during the reaction.

利用软 X 射线区域的荧光-产率 X 射线吸收光谱(XAS)实时观察了固液界面 TiO2 表面的氧进化反应(OER)。在紫外光开启或关闭的电位扫描过程中观察了 OER,重点是氧 K 边 XAS。虽然传统的 XAS 测量需要较长的测量时间,但在本实验中,通过波长色散 XAS 技术,每隔 3 秒就能获得反应过程中的光谱。在电位扫描过程中,只有在紫外光下才能观察到约 533.8 eV 处的 X 射线吸收强度增加。观察到的光谱变化与 OER 的反应机制有关。本技术可广泛应用于固液界面(光)电催化和电化学反应的分析,以观察反应过程中的产物和中间产物。
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引用次数: 0
Enhanced electrochemical performance of molten salt synthesized V2CTx MXene@VOx composite in Zn ion aqueous electrolytes 增强熔盐合成的 V2CTx MXene@VOx 复合材料在锌离子水溶液电解质中的电化学性能
IF 5.4 3区 工程技术 Q1 Chemistry Pub Date : 2024-06-06 DOI: 10.1016/j.elecom.2024.107770
Jinru Wen , Hongyan Dan , Chunyang Li , Chunlong Dai , Zifeng Lin

The development of MXenes using Lewis acidic salts for etching (MS-MXenes) in molten salts presents a novel, fluorine-free method attracting considerable interest. However, the behavior of various MS-MXenes and their derivatives in aqueous environments remains largely unexplored. Particularly, vanadium-based MXenes demonstrate intriguing properties in Zn ion aqueous electrolytes. Herein, a fluorine-free V2CTx MXene@VOx is synthesized by molten salt etching under an argon atmosphere. The electrochemical properties of V2CTx@VOx are tested in various aqueous electrolytes, including Zn(TFSI)2, ZnSO4, ZnBr2, ZnAc2, and ZnCl2 solutions. The V2CTx@VOx shows high redox capacities in all these Zn ion electrolytes, with the peak performance observed in 1 M ZnBr2, achieving a maximum capacity of 172 mAh g−1 at 1 mV s−1. This performance rivals that of V2CTx MXene prepared through wet-chemical methods. These results underscore the potential of MS-MXenes materials in aqueous energy storage applications.

在熔盐中使用路易斯酸盐进行蚀刻(MS-MXenes)的 MXenes 的开发是一种新颖的无氟方法,引起了人们的极大兴趣。然而,各种 MS-MXenes 及其衍生物在水环境中的行为在很大程度上仍未得到探索。特别是,钒基 MXenes 在锌离子水性电解质中表现出了耐人寻味的特性。本文在氩气环境下通过熔盐蚀刻合成了无氟 V2CTx MXene@VOx。测试了 V2CTx@VOx 在各种水电解质(包括 Zn(TFSI)2、ZnSO4、ZnBr2、ZnAc2 和 ZnCl2 溶液)中的电化学特性。V2CTx@VOx 在所有这些锌离子电解质中都显示出很高的氧化还原容量,在 1 M ZnBr2 中达到峰值,在 1 mV s-1 时的最大容量为 172 mAh g-1。这一性能可与通过湿化学方法制备的 V2CTx MXene 相媲美。这些结果凸显了 MS-MXenes 材料在水性储能应用中的潜力。
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引用次数: 0
Synergistic effects of co-doping WO3 with Al and Pt on photoelectrochromic performance WO3 与 Al 和 Pt 的共掺杂对光电变色性能的协同效应
IF 5.4 3区 工程技术 Q1 Chemistry Pub Date : 2024-05-28 DOI: 10.1016/j.elecom.2024.107762
Jacinta Akoth Okwako , Seung Han Song , Sunghyoek Park , Hung Van Tran , Bernard O. Aduda , Sebastian Waita , Young-Sik Hong , Sungjun Hong , Chi-Hwan Han

In this work, we conduct a detailed study to understand the photoelectrochromic properties of Al-Pt co-doped tungsten oxide (WO3). Similarly, we support the photoelectrochromic findings with material characterization, providing additional understanding of the photoelectrochromic performance exhibited by the prepared samples. Additionally, we discuss the effects of Al and Pt doping on photoelectrochromic performance in detail, with a focus on X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) combined with EDS, X-ray photoelectron spectroscopy (XPS), and optical transmittance. XRD peaks confirm the presence of hexagonally-structured WO3 in the prepared samples with a polycrystalline nature, and a similar observation is confirmed via TEM analysis. Surface characterizations conducted through SEM and EDS analyses unveil the morphologies and particle sizes. Optical studies show a bandgap of 1.88 eV and 1.95 eV for Al doped and Al-Pt co-doped WO3, indicating bandgap shrinkage in comparison to the optical bandgap of WO3 of 2.36 eV. The Al-Pt co-doping results in a significant enhancement in photoelectrochromic performance, attaining an optical modulation of 43.61 % at 550 nm and consequently 85 % of the initial transmittance recovered after 2 h of bleaching in the dark. This is an improvement in comparison to the Al doped sample which attains a coloration depth of 43.15 % at 550 nm with only 75 % of the original transmittance being recovered after 2 h under dark conditions.

在这项工作中,我们进行了详细研究,以了解 Al-Pt 共掺氧化钨 (WO3) 的光致变色特性。同样,我们通过材料表征来支持光致变色研究结果,从而进一步了解所制备样品的光致变色性能。此外,我们还详细讨论了铝和铂掺杂对光致变色性能的影响,重点是 X 射线衍射 (XRD)、扫描电子显微镜 (SEM)、结合 EDS 的透射电子显微镜 (TEM)、X 射线光电子能谱 (XPS) 和光学透射率。X 射线衍射峰证实制备的样品中存在多晶性质的六方结构 WO3,TEM 分析也证实了类似的观察结果。通过 SEM 和 EDS 分析进行的表面表征揭示了其形态和颗粒大小。光学研究显示,铝掺杂和铝铂共掺杂的 WO3 的带隙分别为 1.88 eV 和 1.95 eV,这表明与 WO3 2.36 eV 的光学带隙相比,带隙有所缩小。Al-Pt 共掺杂显著提高了光致变色性能,在 550 纳米波长处达到 43.61% 的光学调制,因此在黑暗中漂白 2 小时后,恢复了 85% 的初始透射率。与掺杂铝的样品相比,这种样品在 550 纳米波长处的着色深度为 43.15%,在黑暗条件下漂白 2 小时后仅能恢复 75% 的原始透光率。
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引用次数: 0
Highlighting the operating regimes of microchannel electrodes under laminar flow: Mapping of photoluminescence and electrochemiluminescence through semi-transparent electrodes 突显层流条件下微通道电极的工作状态:通过半透明电极绘制光致发光和电致化学发光图
IF 5.4 3区 工程技术 Q1 Chemistry Pub Date : 2024-05-24 DOI: 10.1016/j.elecom.2024.107759
Yumeng Ma, Catherine Sella, Thomas Delahaye, Laurent Thouin

Semi-transparent platinum electrodes were designed and optimized to implement photoluminescence (PL) and electrochemiluminescence (ECL) in microchannels under flow conditions. The luminescence properties of tris(2,2′-bipyridyl)ruthenium(II) (Ru(bpy)32+) were used to map steady-state emitted light through semi-transparent microchannel electrodes. Several diffusive-convective regimes were thus imposed in order to experimentally highlight the operating conditions of the electrodes, in particular the active zones at their upstream edges contributing to the Faradaic current. PL and ECL profiles were established on the electrode surfaces as a function of flow rate. The PL profiles confirmed the control of the process by mass transport. The data were validated by numerical simulations within the limits of experimental accuracy. ECL emission in presence of the co-reactant tri-n-propylamine (TPA) was also limited by mass transport. However, in comparison the characteristics of the ECL profiles demonstrated the complexity of the underlying mechanism involving Ru(bpy)32+ regeneration and TPA consumption.

对半透明铂电极进行了设计和优化,以便在流动条件下的微通道中实现光致发光(PL)和电化学发光(ECL)。利用三(2,2′-联吡啶基)钌(II) (Ru(bpy)32+) 的发光特性,绘制了通过半透明微通道电极的稳态发光图。因此,为了在实验中突出电极的工作条件,特别是电极上游边缘对法拉第电流起作用的活性区,我们施加了几种扩散-对流制度。在电极表面建立了随流速变化的 PL 和 ECL 曲线。PL 曲线证实了质量传输对过程的控制。在实验精度范围内进行的数值模拟验证了这些数据。共反应物三正丙胺(TPA)存在时的 ECL 发射也受到质量迁移的限制。不过,相比之下,ECL 曲线的特征表明了涉及 Ru(bpy)32+ 再生和 TPA 消耗的基本机制的复杂性。
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引用次数: 0
Ion-selective paper-based chromogenic strip and electrochemical sensor for the detection of ammonium ions 用于检测铵离子的离子选择性纸基显色带和电化学传感器
IF 5.4 3区 工程技术 Q1 Chemistry Pub Date : 2024-05-23 DOI: 10.1016/j.elecom.2024.107757
Pawankumar Rai , Ashish K. Singh , Srishti Mehrotra , Sandeep K. Sharma

The fraudulent practice of adding ammonium salts to milk in order to enhance the nitrogen content has serious health implications including renal failure. Ammonium ion detection has been targeted through the conventional analytical methods however, lack of portability and complex operation limits their use for field applications. In this scenario, paper-based test strips and electrochemical sensors can provide strategies for point-of-test applications. Here, an ion-selective paper-based chromogenic strip and an electrochemical sensor has been developed for detection and quantification of ammonium ions. The developed paper-based chromogenic strip showed detection limit of 0.008 % (w/v) for ammonium ions, whereas, electrochemical sensor showed an LOD of 0.0062 ± 0.0023 % (w/v) with a sensitivity of 1.6 × 10−5 A.% −1.mm−2. The developed paper-based chromogenic strip and electrochemical sensor can be employed by regulatory bodies and dairy industries to ensure the safety and quality of milk.

在牛奶中添加铵盐以提高氮含量的欺诈性做法会对健康造成严重影响,包括肾功能衰竭。铵离子检测一直是传统分析方法的目标,但由于缺乏便携性和复杂的操作,限制了它们在现场应用中的使用。在这种情况下,纸质试纸和电化学传感器可为检测点应用提供策略。在此,我们开发了一种离子选择性纸质显色条和电化学传感器,用于铵离子的检测和定量。所开发的纸质显色条对铵离子的检测限为 0.008 %(w/v),而电化学传感器的检测限为 0.0062 ± 0.0023 %(w/v),灵敏度为 1.6 × 10-5 A.% -1.mm-2 。监管机构和乳品行业可采用所开发的纸质显色条和电化学传感器来确保牛奶的安全和质量。
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引用次数: 0
Relationship between particle shape and fast-charging capability of a dry-processed graphite electrode in lithium-ion batteries 锂离子电池中干法加工石墨电极的颗粒形状与快速充电能力之间的关系
IF 5.4 3区 工程技术 Q1 Chemistry Pub Date : 2024-05-21 DOI: 10.1016/j.elecom.2024.107761
Jun Ho Hwang , Hyundong Yoo , Seungeun Oh , Hansu Kim

Improving lithium-ion transport in electrodes by controlling electrode microstructure is a promising option for enhancing the fast-charging capability of graphite anodes in lithium-ion batteries. Dry processing of electrodes based on a polytetrafluoroethylene binder has attracted considerable attention as an alternative to solvent-based wet processing. The morphology of graphite particles has a significant impact on electrode microstructure, but few reports have been published on dry-processed graphite anodes. In this work, we found that the morphology of graphite particles is a key factor to determine the fast-charging capability of the dry-processed graphite electrode as well as the microstructure of the dry-processed graphite electrode. X-ray microscopy combined with mercury porosimetry and symmetrical cell electrochemical impedance spectroscopy reveal that the difference in porosity between the top and bottom layers of a dry electrode with spherical graphite particles is greater than that of flake-shaped graphite particles, resulting in enhanced lithium-ion transport in the electrode and improved fast-charging capability at a high charging rate of 5C (17.5 mA cm−2). These findings supply insights into the effective design of dry-processed graphite anodes with an emphasis on fast-charging capability as well as the development of graphite anode materials for dry-processing based lithium-ion batteries.

通过控制电极的微观结构来改善电极中的锂离子传输,是提高锂离子电池中石墨负极快速充电能力的一个可行方案。基于聚四氟乙烯粘合剂的电极干法加工作为溶剂型湿法加工的一种替代方法,已经引起了广泛关注。石墨颗粒的形态对电极的微观结构有重大影响,但有关干法加工石墨负极的报道却寥寥无几。在这项工作中,我们发现石墨颗粒的形态是决定干法石墨电极快速充电能力以及干法石墨电极微观结构的关键因素。X 射线显微镜结合汞孔测定法和对称电池电化学阻抗谱发现,球形石墨颗粒干法电极上下两层的孔隙率差异大于片形石墨颗粒,从而增强了电极中的锂离子传输,提高了在 5C 高充电速率(17.5 mA cm-2)下的快速充电能力。这些发现为有效设计以快速充电能力为重点的干法加工石墨负极以及开发用于干法加工锂离子电池的石墨负极材料提供了启示。
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引用次数: 0
Rechargeable zinc-air battery with bifunctional electrocatalyst of copper oxide and graphene nanoplatelets 使用氧化铜和石墨烯纳米片双功能电催化剂的可充电锌-空气电池
IF 5.4 3区 工程技术 Q1 Chemistry Pub Date : 2024-05-20 DOI: 10.1016/j.elecom.2024.107760
Barbara A.C. Sá , Tatiana S. Andrade , Rafael R. de Souza , Antero R. Santos Neto , Mariandry Rodriguez , Francisco G.E. Nogueira , Márcio C. Pereira

Rechargeable zinc-air batteries have been identified as promising technologies for energy storage. However, developing cost-effective electrocatalysts that can efficiently facilitate the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) is crucial for their advancement. This work investigates synthesized electrocatalysts composed of graphene-Cu2O deposited on carbon cloth by doctor blading casting method as bifunctional electrodes in a rechargeable Zn-air battery. The battery integrated with graphene-Cu2O as the air-cathode electrocatalyst showed superior performance in terms of cycling stability compared to that without Cu2O. This enhanced performance is attributed to the reversibility of Cu+/Cu2+ species during the redox reactions facilitated by the high electrical conductivity of graphene. Therefore, the results suggest the potential of the synthesized electrodes for advancing the development of rechargeable Zn-air batteries.

可充电锌-空气电池已被确定为前景广阔的储能技术。然而,开发能有效促进氧进化反应(OER)和氧还原反应(ORR)的高性价比电催化剂对其发展至关重要。本研究采用刮削铸造法合成了沉积在碳布上的石墨烯-Cu2O 电催化剂,并将其作为可充电锌-空气电池的双功能电极。与不含 Cu2O 的电池相比,集成了石墨烯-Cu2O 作为空气阴极电催化剂的电池在循环稳定性方面表现出更优越的性能。这种性能的提高归因于石墨烯的高导电性促进了氧化还原反应过程中 Cu+/Cu2+ 物种的可逆性。因此,这些结果表明合成的电极具有推动可充电锌-空气电池发展的潜力。
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引用次数: 0
Development of an efficient electrochemical sensor based on CuAl-LDH using an electrostatic repulsion approach for the selective determination of dopamine in the presence of uric acid and ascorbic acid species 利用静电排斥方法开发基于 CuAl-LDH 的高效电化学传感器,用于在尿酸和抗坏血酸存在时选择性测定多巴胺
IF 5.4 3区 工程技术 Q1 Chemistry Pub Date : 2024-05-19 DOI: 10.1016/j.elecom.2024.107756
Saeedeh Shahparast , Karim Asadpour-Zeynali

This study provides a unique electrochemical sensor that exhibits both excellent sensitivity and selectivity, while also being environmentally friendly. The CuAl-LDH/GCE sensor, proposed as the recommended sensor, was synthesized using a straightforward one-step co-precipitation procedure. It was first used to measure dopamine levels using differential pulse voltammetry. At the ideal pH level of 8, dopamine has a positive charge, but ascorbic acid and uric acid have a negative charge. LDH, on the other hand, carries a negative charge and exhibits high electrostatic attraction towards dopamine, but is electrostatically repelled by negatively charged ascorbic acid and uric acid. Hence, CuAl-LDH/GCE has the potential to specifically ascertain the existence of dopamine in the presence of these particular species. The examination of the composition and morphology of CuAl-LDH was conducted using various analytical techniques, including scanner electron microscopy (FESEM), transmission electron microscope (TEM), element mapping (MAP), Fourier transform infrared (FTIR), energy-dispersive X-ray spectroscopy (EDX), Brunauer Emmett Teller (BET), X-ray photoelectron diffraction (XRD), and Raman techniques. Under ideal circumstances, the calibration graph of dopamine was generated using differential pulse voltammetry. A linear range of 4.194–1151.54 μM was achieved for dopamine, with a limit of detection of 0.33 μM. The findings of the study indicate that the sensor created for dopamine determination has exceptional stability, repeatability, and reproducibility. The sensor that was presented was effectively used for the measurement of dopamine in both pharmaceutical ampoules and human plasma samples.

本研究提供了一种独特的电化学传感器,既具有出色的灵敏度和选择性,又对环境友好。作为推荐传感器的 CuAl-LDH/GCE 传感器是通过简单的一步共沉淀程序合成的。首先利用差分脉冲伏安法测量多巴胺的含量。在理想的 pH 值为 8 时,多巴胺带正电荷,而抗坏血酸和尿酸带负电荷。而 LDH 带有负电荷,对多巴胺有很强的静电吸引力,但对带负电荷的抗坏血酸和尿酸有静电排斥。因此,CuAl-LDH/GCE 有可能在这些特殊物种存在的情况下特异性地确定多巴胺的存在。对 CuAl-LDH 的成分和形态的研究采用了多种分析技术,包括扫描电子显微镜 (FESEM)、透射电子显微镜 (TEM)、元素图谱 (MAP)、傅立叶变换红外光谱 (FTIR)、能量色散 X 射线光谱 (EDX)、布鲁瑙尔-埃米特-泰勒 (BET)、X 射线光电子衍射 (XRD) 和拉曼技术。在理想情况下,使用差分脉冲伏安法生成多巴胺的校准图。多巴胺的线性范围为 4.194-1151.54 μM,检测限为 0.33 μM。研究结果表明,为测定多巴胺而设计的传感器具有出色的稳定性、可重复性和再现性。所展示的传感器可有效用于测量药物安瓿和人体血浆样品中的多巴胺。
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引用次数: 0
Age- and sex-dependent electrochemistry of Ginkgo biloba leaves 银杏叶电化学的年龄和性别依赖性
IF 5.4 3区 工程技术 Q1 Chemistry Pub Date : 2024-05-17 DOI: 10.1016/j.elecom.2024.107758
Antonio Doménech-Carbó , Josefa Prieto-Mossi , Noemí Montoya

The voltammetric response of microparticulate deposits resulting from the evaporation of ethanolic extracts of leaves of Ginkgo biloba L. trees in contact with aqueous acetate buffer has been studied. Voltammetric data associated with the oxidation of polyphenolic secondary metabolites permits the discrimination of individuals by sex and age. Evaluation of age variation of reactivity with reactive oxygen species (ROS) was also described.

研究了银杏叶乙醇提取物与醋酸水缓冲液接触蒸发后产生的微颗粒沉积物的伏安反应。与多酚次生代谢物氧化相关的伏安法数据允许按性别和年龄区分个体。此外,还对活性氧(ROS)反应性的年龄变化进行了评估。
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引用次数: 0
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Electrochemistry Communications
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