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Front Cover: Electrocatalytic Performance and Kinetic Behavior of Anion-Intercalated Borate-Based NiFe LDH in Alkaline OER (ChemElectroChem 22/2024) 封面:碱性 OER 中阴离子钙化硼酸盐基镍铁 LDH 的电催化性能和动力学行为(ChemElectroChem 22/2024)
IF 3.5 4区 化学 Q2 ELECTROCHEMISTRY Pub Date : 2024-11-19 DOI: 10.1002/celc.202482201
Maike Berger, Alexandra Markus, Stefan Palkovits, Prof. Regina Palkovits

The front cover shows a karate fighter who is supposed to represent our electrodes system. She kicks into water and splits the water into O2 and H2 bubbles. The feet with which she splits the water are “coated” with our catalyst material NiFe LDH. The same schematic of LDH as in the article was used to illustrate the structure giving reference to our article. Her fists glow with electricity. A wind turbine can be seen in the background to emphasize that green electricity is being used. The woman is standing in a mineral cave and a mineral is shown at the bottom left, which is intended to establish a link to borate/borax minerals. More information can be found in the Research Article by Regina Palkovits and co-workers (DOI: 10.1002/celc.202400457).

封面上的空手道斗士代表了我们的电极系统。她踢入水中,将水分成 O2 和 H2 气泡。她劈水的脚上 "涂有 "我们的催化剂材料 NiFe LDH。我们使用了与文章中相同的 LDH 结构示意图,以参考我们的文章。她的拳头发出电光。背景中可以看到一个风力涡轮机,强调使用的是绿色电力。该女子站在一个矿洞中,左下方显示了一种矿物,意在与硼酸盐/硼砂矿物建立联系。更多信息请参阅 Regina Palkovits 及其合作者的研究文章(DOI: 10.1002/celc.202400457)。
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引用次数: 0
Front Cover: High-performance Porous Electrodes for Flow Batteries: Improvements of Specific Surface Areas and Reaction Kinetics (ChemElectroChem 21/2024) 封面:用于液流电池的高性能多孔电极:比表面积和反应动力学的改进(ChemElectroChem 21/2024)
IF 3.5 4区 化学 Q2 ELECTROCHEMISTRY Pub Date : 2024-11-07 DOI: 10.1002/celc.202482101
Lyuming Pan, Zixiao Guo, Hucheng Li, Yilin Wang, Haoyao Rao, Qinping Jian, Jing Sun, Jiayou Ren, Zhenyu Wang, Bin Liu, Meisheng Han, Yubai Li, Xinzhuang Fan, Wenjia Li, Lei Wei

Redox flow batteries (RFBs) play a crucial role in large-scale energy storage, with electrode design being essential to their performance. Porous electrodes enhance macroscopic/mesoscopic flow, microscopic ion diffusion, and interfacial electrochemical reactions, leading to improved power density and energy efficiency. This review focuses on the design and strategies of RFB optimized electrodes, promoting the achievement of carbon neutrality. More information can be found in the Review Article by Xinzhuang Fan, Wenjia Li, Lei Wei, and co-workers (10.1002/celc.202400460).

氧化还原液流电池(RFB)在大规模储能中发挥着至关重要的作用,而电极设计对其性能至关重要。多孔电极可增强宏观/微观流动、微观离子扩散和界面电化学反应,从而提高功率密度和能源效率。本综述侧重于 RFB 优化电极的设计和策略,以促进实现碳中和。更多信息,请参阅范新庄、李文佳、魏磊及合作者的评论文章(10.1002/celc.202400460)。
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引用次数: 0
Cover Feature: Cost-Effective Solutions for Lithium-Ion Battery Manufacturing: Comparative Analysis of Olefine and Rubber-Based Alternative Binders for High-Energy Ni-Rich NCM Cathodes (ChemElectroChem 21/2024) 封面专题:锂离子电池制造的成本效益解决方案:用于高能量富镍 NCM 阴极的烯烃基和橡胶基替代粘合剂的比较分析(ChemElectroChem 21/2024)
IF 3.5 4区 化学 Q2 ELECTROCHEMISTRY Pub Date : 2024-11-07 DOI: 10.1002/celc.202482102
Susan Montes, Alexander Beutl, Andrea Paolella, Marcus Jahn, Artur Tron

The Cover Feature explores olefin and rubber-based polymers as alternatives to PVDF for binder materials in high-energy Ni-rich NCM LiNixCoyMnzO2 (NCM, x ≥ 0.8) Li-ion cathodes. The evaluation of PIB, SBS, NBR, and HNBR binders includes their physical, chemical, and electrochemical properties and production costs, showing effective competition against PVDF-NMP, by offering stable performance, lower costs and reduced contamination due to their fluorine-free nature. More details are available in the Research Article by Alexander Beutl, Artur Tron, and co-workers (10.1002/celc.202400465).

封面专题探讨了在高能量富镍 NCM LiNixCoyMnzO2(NCM,x ≥ 0.8)锂离子阴极中,烯烃基和橡胶基聚合物作为 PVDF 粘合剂材料的替代品。对 PIB、SBS、NBR 和 HNBR 粘合剂的评估包括它们的物理、化学和电化学性能以及生产成本,结果表明这些粘合剂具有稳定的性能、较低的成本以及因其不含氟而减少的污染,因而能有效地与 PVDF-NMP 竞争。更多详细信息,请参阅 Alexander Beutl、Artur Tron 及其合作者的研究文章(10.1002/celc.202400465)。
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引用次数: 0
PVDF and PEO Catholytes in Solid-State Cathodes Made by Conventional Slurry Casting 传统浆料浇铸法制造的固态阴极中的 PVDF 和 PEO 阴极
IF 3.5 4区 化学 Q2 ELECTROCHEMISTRY Pub Date : 2024-10-30 DOI: 10.1002/celc.202400472
Benjamin R. Howell, Joshua W. Gallaway

All-solid-state Li batteries are desired for better safety and energy density than Li-ion batteries. However, the lack of a penetrating liquid electrolyte requires a much different approach to the design of cathodes. The solid catholyte must enable good Li+ conduction, form good interfaces with active material particles, and have the strength to bind the cathode together during repeated volume changes. Catholyte formulation is often simply adapted from Li-ion design principles, adding a Li salt to the PVDF binder. Here we show that such a PVDF binder at 10 wt % loading is a starved catholyte condition that compromises cell performance. By substituting a 70 : 30 blend of PVDF:PEO, performance is improved while maintaining nearly the same areal loading of LFP active material. Increasing the catholyte fraction to 16 % can also improve performance, but in this case the benefit of including PEO is lessened, with PVDF alone being an adequate catholyte. EIS analysis shows that PEO helps to form charge transfer interfaces at 10 % catholyte, but that its inclusion can degrade interfaces when there is ample catholyte at 16 %. It is also shown that catholyte agglomeration can impede bulk Li conduction, indicating that microstructural factors are of critical importance.

与锂离子电池相比,全固态锂电池具有更好的安全性和能量密度。然而,由于缺乏可渗透的液态电解质,阴极的设计需要采用截然不同的方法。固体阴极溶液必须能够实现良好的锂+传导,与活性材料颗粒形成良好的界面,并在反复的体积变化过程中具有将阴极结合在一起的强度。阴极溶液的配方通常是根据锂离子设计原理进行简单调整,在 PVDF 粘合剂中添加锂盐。在这里,我们展示了这种 PVDF 粘合剂在 10 wt % 负载时的阴极溶质饥饿状态,从而影响了电池的性能。通过用 70 :30 的 PVDF:PEO 混合物,在保持几乎相同的 LFP 活性材料面积负载的同时,性能也得到了改善。将电解质比例提高到 16% 也能提高性能,但在这种情况下,加入 PEO 的好处就会减少,因为 PVDF 本身就是一种足够的电解质。EIS 分析表明,在 10% 的阴极溶解度下,PEO 有助于形成电荷转移界面,但在 16% 的阴极溶解度下,加入 PEO 会降低界面的性能。分析还表明,电解质聚结会阻碍块状锂的传导,这表明微观结构因素至关重要。
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引用次数: 0
Ex Situ Electro-Organic Synthesis – A Method for Unrestricted Reaction Control and New Options for Paired Electrolysis 原位电有机合成--不受限制的反应控制方法和配对电解的新选择
IF 3.5 4区 化学 Q2 ELECTROCHEMISTRY Pub Date : 2024-10-30 DOI: 10.1002/celc.202400489
Helena Pletsch, Yang Lyu, Dominik P. Halter

Classic in situ electro-organic synthesis with substrates in an electrolyzer must compromise process conditions to balance electro- and thermochemical steps at both electrodes. This often restricts efficiency and product selectivity, since requirements may deviate for electrochemical (catalyst activation) and chemical (organic synthesis) steps, as well as for paired anode- and cathode reactions. Breaking this barrier, we report ex situ electro-organic synthesis as a versatile method that enables unique product selectivity and unusual product pairs. We exemplify the concept for pairing H2 evolution (HER) with anodic alcohol oxidation. The two-step method accomplishes this by separating cathode reactions from organic substrate oxidation, and anodic electrocatalyst activation from chemical conversion of organic substrates in time and space. First, the electro-oxidation of Ni(OH)2 anodes to NiOOH is paired with H2 production by alkaline water electrolysis. Then, “charged” NiOOH electrodes are removed from the electrolyzer and used in external vessels to oxidize model substrate benzyl alcohol under regeneration of Ni(OH)2. Free choice of reaction media outside the electrolyzer allows to selectively obtain benzoic acid (in water) or benzaldehyde (in n-hexane), whereas classic in situ electrosynthesis only produces the acid together with H2. Perspectively, the method enables electrosynthesis of previously inaccessible products paired to H2 generation.

利用电解槽中的基质进行传统的原位电有机合成时,必须对工艺条件进行折衷,以平衡两个电极上的电化学和热化学步骤。这通常会限制效率和产品选择性,因为电化学(催化剂活化)和化学(有机合成)步骤以及成对的阳极和阴极反应的要求可能不同。我们的报告打破了这一障碍,将原位电有机合成作为一种多功能方法,实现了独特的产品选择性和不寻常的产品对。我们举例说明了将 H2 演化(HER)与阳极醇氧化配对的概念。这种两步法在时间和空间上将阴极反应从有机底物氧化中分离出来,并将阳极电催化剂活化从有机底物的化学转化中分离出来,从而实现了这一目的。首先,将 Ni(OH)2 阳极电氧化成 NiOOH 与碱性水电解产生 H2 配对。然后,从电解槽中取出 "带电 "的 NiOOH 电极,在外部容器中使用,在 Ni(OH)2 的再生作用下氧化模型底物苯甲醇。通过自由选择电解槽外的反应介质,可以选择性地获得苯甲酸(在水中)或苯甲醛(在正己烷中),而传统的原位电合成只能产生酸和 H2。从长远来看,这种方法可以电合成以前无法获得的与 H2 生成配对的产物。
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引用次数: 0
Annihilation Electrochemiluminescence Triggered by Bipolar Electrochemistry 双极电化学引发的湮灭电化学发光
IF 3.5 4区 化学 Q2 ELECTROCHEMISTRY Pub Date : 2024-10-30 DOI: 10.1002/celc.202400522
Leslie R. Arias-Aranda, Gerardo Salinas, Haidong Li, Conor F. Hogan, Alexander Kuhn, Laurent Bouffier, Neso Sojic

Bipolar electrochemistry (BE) combined with electrochemiluminescence (ECL) has gained considerable attention as a versatile and powerful analytical technique operating in a wireless manner. However, only co-reactant ECL has been reported so far when using a BE setup. In this work, the generation of annihilation ECL at the anodic extremity of a bipolar electrode (BPE) is demonstrated in two different spatial arrangements of the electrodes. The reported approach is based on a synergetic effect between the asymmetric electroactivity induced across the BPE, which produces different redox states of [Ru(bpy)3]2+, and the electro-migration mechanism of the formed ionic species, allowing the localization and concentration of the ECL emission. The presented approach demonstrating annihilation ECL via BE, paves the way for the design of easy and straightforward light-emitting platforms for multiple applications.

双极电化学(BE)与电化学发光(ECL)相结合,作为一种以无线方式运行的多功能、功能强大的分析技术,受到了广泛关注。然而,迄今为止,只有使用 BE 设置时产生共反应 ECL 的报道。在这项工作中,通过两种不同的电极空间布局,展示了在双极电极(BPE)阳极产生湮灭 ECL 的情况。所报告的方法基于双极性电极(BPE)上的不对称电活性(产生不同氧化还原态的[Ru(py)3]2+)与所形成离子物种的电迁移机制之间的协同效应,从而实现了 ECL 发射的定位和集中。所展示的通过 BE 实现湮灭 ECL 的方法为设计多种应用的简便直接的发光平台铺平了道路。
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引用次数: 0
Screening of Cation Exchange Membranes for an Anthraquinone-Ferrocyanide Flow Battery 筛选阳离子交换膜用于蒽醌-亚铁氰化物液流电池
IF 3.5 4区 化学 Q2 ELECTROCHEMISTRY Pub Date : 2024-10-30 DOI: 10.1002/celc.202400516
Lavrans F. Söffker, Thomas Turek, Ulrich Kunz, Luis F. Arenas

The disodium salt of 9,10-anthraquinone-2,7-disulphonic acid (2,7-AQDS) is an interesting platform for developing anthraquinone derivative negolytes for aqueous organic flow batteries. Recently, ammonium sulphate supporting electrolytes have been considered for improved stability and solubility. This work advances the 2,7-AQDS/ferrocyanide flow battery with an ammonium sulphate supporting electrolyte (pH 5) by studying the suitability of six commercially available cation exchange membranes: E-620, NR-212, FS-930, F-1075-PK, F-1850 and N-115. Cell cycling under galvanostatic regime plus potential hold was performed to determine coulombic efficiency, energy efficiency and accessible capacity for each membrane as well as capacity fade rate for three selected membranes under extended operation. Cell cycling under galvanostatic control only was carried out to observe transient membrane behavior alongside accessible capacity and apparent capacity fade rate. It was found that the capacity set by the limiting negolyte is consistent with 1.5 electrons per 2,7-AQDS molecule and that energy efficiency shows a simple direct relationship to membrane thickness, with one exception. Meanwhile, four membranes displayed similar apparent capacity fade rates at this laboratory scale irrespective of their thickness, with capacity loss explained in terms of crossover. The best overall performance was attained by the thinnest membranes, E-620 and NR-212.

9,10-蒽醌-2,7-二磺酸二钠盐(2,7-AQDS)是开发用于水性有机液流电池的蒽醌衍生物负解质的一个有趣平台。最近,硫酸铵支撑电解质被认为可以提高稳定性和溶解性。这项工作通过研究六种市售阳离子交换膜的适用性,推进了使用硫酸铵支撑电解质(pH 值为 5)的 2,7-AQDS/ferrocyanide 液流电池:E-620、NR-212、FS-930、F-1075-PK、F-1850 和 N-115。在电流静态机制和电位保持条件下进行电池循环,以确定每种膜的库仑效率、能量效率和可获取容量,以及三种选定膜在长时间运行条件下的容量衰减率。仅在电流静态控制下进行电池循环,以观察膜的瞬态行为以及可获得容量和表观容量衰减率。研究发现,限制性负溶质所设定的容量与每个 2,7-AQDS 分子 1.5 个电子相一致,能量效率与膜厚度呈简单的直接关系,但有一个例外。同时,在这种实验室规模下,无论膜的厚度如何,四种膜都显示出相似的表观容量衰减率,容量损失可以用交叉来解释。整体性能最好的是最薄的膜 E-620 和 NR-212。
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引用次数: 0
Lithium Doping Enhances the Aqueous Zinc Ion Storage Performance of V3O7 ⋅ H2O Nanorods 掺锂提高了 V3O7 ⋅ H2O 纳米棒的锌离子水溶液储存性能
IF 3.5 4区 化学 Q2 ELECTROCHEMISTRY Pub Date : 2024-10-30 DOI: 10.1002/celc.202400504
Yingfang Hu, Siwen Zhang, Yujin Ren, Rongyuan Ge, Yaowen Shi, Xinyu Feng, Hui Li, Baohua Jia, Bosi Yin, Tianyi Ma

Aqueous zinc-ion batteries (AZIBs) offer significant advantages, including high safety, environmental protection and abundant zinc sources. V-based layer-like oxides are promising candidates as cathode materials for ZIBs; however, they face challenges such as low electrical conductivity, poor cycling stability, and limited Zn2+ storage capacity. In this study, Li-V3O7 ⋅ H2O electrode materials were successfully synthesized using a hydrothermal method. The doping of lithium ions has led to a significant expansion of the interlayer spacing within the electrode structure, which enhances ion mobility and improves ion transport speed as well as charge-discharge rates. Additionally, the increased spacing allows for the accommodation of more zinc ions, resulting in greater specific capacity and energy storage. More importantly, this modification reduces structural strain, minimizes the dissolution of vanadium-based materials, and maintains electrode integrity over multiple cycles, thereby improving cycling stability. Consequently, the properties of V3O7 ⋅ H2O electrodes were substantially enhanced through lithium-ion doping. The Li-V3O7 ⋅ H2O cathode has a specific capacity of 411.8 mAh g−1 at low current and maintains 83 % of its capacity at 4.0 A g−1 for 4800 cycles, indicating a noteworthy improvement over pristine V3O7 ⋅ H2O. Exhibiting outstanding conductivity, discharge capacity, and cycling stability, it holds immense promise for future high-performance energy storage.

水性锌离子电池(AZIBs)具有安全性高、环保和锌资源丰富等显著优势。钒基类层状氧化物是有希望成为锌离子电池阴极材料的候选材料;然而,它们面临着电导率低、循环稳定性差和 Zn2+ 储存能力有限等挑战。本研究采用水热法成功合成了 Li-V3O7 ⋅ H2O 电极材料。锂离子的掺杂使电极结构中的层间间距显著扩大,从而增强了离子迁移率,提高了离子传输速度和充放电速率。此外,间距的增加还能容纳更多的锌离子,从而提高比容量和储能能力。更重要的是,这种改性降低了结构应变,最大限度地减少了钒基材料的溶解,并在多次循环中保持了电极的完整性,从而提高了循环稳定性。因此,通过掺杂锂离子,V3O7 ⋅ H2O 电极的性能得到了大幅提升。锂-V3O7⋅H2O阴极在低电流时的比容量为 411.8 mAh g-1,在 4.0 A g-1 的条件下循环 4800 次仍能保持 83% 的容量,与原始 V3O7 ⋅H2O相比有显著提高。它具有出色的导电性、放电容量和循环稳定性,在未来的高性能储能领域大有可为。
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引用次数: 0
Key Ingredients for the Modeling of Single-Atom Electrocatalysts 单原子电催化剂建模的关键要素
IF 3.5 4区 化学 Q2 ELECTROCHEMISTRY Pub Date : 2024-10-29 DOI: 10.1002/celc.202400476
Giovanni Di Liberto, Gianfranco Pacchioni

Single-atom catalysis is gaining interest also because of its potential applications in a broad spectrum of electrochemical reactions. The reactivity of single-atom catalysts (SACs) is typically modeled with first principles approaches taking insight from heterogenous catalysis. An increasing number of studies show that the chemistry of SACs is more complex than often assumed, and shares many aspects in common with coordination chemistry. This evidence raises challenges for computational electrocatalysis of SACs. In this perspective we highlight a few fundamental ingredients that one need to consider to provide reliable predictions on the reactivity of SACs for electrochemical applications. We discuss the role of the local coordination of the metal active phase, the need to use self-interaction corrected functionals, in particular when systems have magnetic ground states. We highlight the formation of unconventional intermediates with respect to classical metal electrodes, the need to include the stability of SACs in electrochemical conditions and the role of solvation in the analysis of new potential catalytic systems. This brief account can be considered as a tutorial underlining the importance of treating the reactivity of SACs. In fact, neglecting some of these aspects could lead to unreliable predictions failing in the design of new electrocatalysts.

单原子催化因其在广泛的电化学反应中的潜在应用而日益受到关注。单原子催化剂(SAC)的反应性通常采用第一原理方法建模,并从异质催化中汲取灵感。越来越多的研究表明,单原子催化剂的化学性质比通常假设的更为复杂,而且在许多方面与配位化学有共同之处。这些证据对 SAC 的计算电催化提出了挑战。在这一视角中,我们强调了为电化学应用提供可靠的 SAC 反应性预测需要考虑的几个基本要素。我们讨论了金属活性相局部配位的作用、使用自相互作用校正函数的必要性,特别是当系统具有磁性基态时。我们强调了与经典金属电极相比,非常规中间产物的形成、SAC 在电化学条件下稳定性的必要性,以及溶解在分析新的潜在催化系统中的作用。这篇简短的论述可视为一篇教程,强调了处理 SAC 反应性的重要性。事实上,忽视其中某些方面可能会导致不可靠的预测,从而无法设计出新的电催化剂。
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引用次数: 0
Surface-Engineered Pt-Ni(111) Nanocatalysts for Boosting Their ORR Performance via Thermal Treatment 表面工程铂镍(111)纳米催化剂通过热处理提高 ORR 性能
IF 3.5 4区 化学 Q2 ELECTROCHEMISTRY Pub Date : 2024-10-29 DOI: 10.1002/celc.202400491
Can Li, Xiaobo Chen, Jinfong Pan, Guangwen Zhou, Jiye Fang

The electrochemical oxygen reduction reaction (ORR) is critical for fuel cell application, and modifying surface structures of electrocatalysts has proven effective in improving their catalytic performances. In this study, we investigated surface-engineered Pt−Ni nano-octahedra subjected to annealing in various atmospheres. All octahedral nanocrystals retained their Pt−Ni {111} facets at an elevated temperature following the annealing treatments. Air annealing led to the formation of nickel-rich shells on the Pt−Ni surface. In contrast, hydrogen (H₂) as a reducing gas facilitated the reduction of surface Ni species, incorporating them into the Pt−Ni bulk alloy, which resulted in superior mass activity and specific activity for ORR-approximately 2.4 and 2.3 times as high as those from the unmodified counterpart, respectively. After 20,000 potential cycles, the H₂/Ar-annealed Pt−Ni nano-octahedra maintained a mass activity of 3.92 A/, surpassing the initial mass activity of the unannealed counterparts (2.95 A/). These findings demonstrate a viable approach for tailoring catalyst surfaces to enhance performance in various energy storage and conversion applications.

电化学氧还原反应(ORR)对燃料电池的应用至关重要,而改变电催化剂的表面结构已被证明能有效改善其催化性能。在本研究中,我们研究了在不同气氛中退火的表面工程铂镍纳米八面体。经过退火处理后,所有八面体纳米晶体在高温下都保留了铂镍{111}面。空气退火会在铂镍表面形成富含镍的外壳。与此相反,氢气(H₂)作为还原气体促进了表面镍物种的还原,并将其纳入铂镍块状合金中,从而使 ORR 的质量活性和比活度更高,分别是未改性对应物的约 2.4 倍和 2.3 倍。经过 20,000 次电位循环后,H₂/Ar-退火的铂镍纳米八面体的质量活性保持在 3.92 A/,超过了未退火的对应物的初始质量活性(2.95 A/)。这些研究结果表明,定制催化剂表面以提高其在各种能量存储和转换应用中的性能是一种可行的方法。
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引用次数: 0
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