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Current status of ferro-/ferricyanide for redox flow batteries 用于氧化还原液流电池的铁/铁氰化物的现状
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-28 DOI: 10.1016/j.coelec.2024.101581
Maryam Mouselly , Hussain Alawadhi , Sirugaloor Thangavel Senthilkumar

The ferro-/ferricyanide couple has been extensively investigated as a redox species in various redox flow batteries (RFBs) due to its advantageous electrochemical properties, user-friendliness, and affordable cost. However, the high concentration and stability of ferro-/ferricyanide are important for developing high-energy density and long-cycle life RFBs. Different methods have been explored to increase its concentration through diverse ion effects and cation modification while also exploring the effects of pH, light, and air sensitivity on its stability. This review will provide an overview of recent research on the concentration enhancement of ferro-/ferricyanide and its stability for RFBs.

铁/铁氰化物偶联物因其有利的电化学特性、用户友好性和经济实惠的成本,已被广泛研究用作各种氧化还原液流电池(RFB)中的氧化还原物种。然而,高浓度和稳定的铁氰化物对开发高能量密度和长循环寿命的 RFB 十分重要。人们探索了不同的方法,通过不同的离子效应和阳离子修饰来提高其浓度,同时还探索了 pH 值、光和空气敏感性对其稳定性的影响。本综述将概述有关提高铁/铁氰化物浓度及其在射频电池中稳定性的最新研究。
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引用次数: 0
Machine learning-guided design, synthesis, and characterization of atomically dispersed electrocatalysts 机器学习指导下的原子分散电催化剂设计、合成和表征
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-21 DOI: 10.1016/j.coelec.2024.101578
Sirui Li , Hanguang Zhang , Edward F. Holby , Piotr Zelenay , Wilton J.M. Kort-Kamp

The recent integration of machine learning into materials design has revolutionized the understanding of structure–property relationships and optimization of material properties beyond the trial-and-error paradigm. On one hand, machine learning has significantly accelerated the development of atomically dispersed metal-nitrogen-carbon (M-N-C) electrocatalysts, which traditionally heavily relied on heuristic approaches. On the other hand, the primary challenge of leveraging machine learning to expedite M-N-C materials discovery lies in the cost associated with data collection. We review recent machine learning integration strategies for M-N-C catalyst development, including discussions on the typical algorithms such as symbolic regression and convolutional neural networks employed for the theoretical design, synthesis optimization via active learning, and advanced microscopy characterization. Subsequently, we provide our perspective on potential near-future directions for furthering machine learning-assisted development of new M-N-C catalysts and elucidating the complex physicochemical mechanisms governing the selectivity, activity, and durability in this class of materials.

最近,机器学习与材料设计的结合彻底改变了人们对结构-性能关系的理解,并使材料性能的优化超越了试错模式。一方面,机器学习大大加快了原子分散金属-氮-碳(M-N-C)电催化剂的开发速度,而传统的电催化剂主要依赖启发式方法。另一方面,利用机器学习加速 M-N-C 材料发现的主要挑战在于与数据收集相关的成本。我们回顾了最近用于 M-N-C 催化剂开发的机器学习集成策略,包括讨论理论设计、通过主动学习优化合成以及高级显微表征所采用的符号回归和卷积神经网络等典型算法。随后,我们就机器学习辅助开发新型 M-N-C 催化剂的近期潜在方向提出了自己的观点,并阐明了这一类材料的选择性、活性和耐久性的复杂物理化学机制。
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引用次数: 0
Modeling oxygen reduction activity loss mechanisms in atomically dispersed Fe–N–C electrocatalysts 原子分散的 Fe-N-C 电催化剂中氧还原活性损失机制建模
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-21 DOI: 10.1016/j.coelec.2024.101579
Sirui Li , Wilton J.M. Kort-Kamp , Piotr Zelenay , Edward F. Holby

Materials degradation is a major factor that limits the wider adoption of renewable and clean energy technologies. This is particularly true for the Pt group metal-free (PGM-free) atomically dispersed metal-nitrogen-carbon (M-N-C) catalysts. While many experimental studies have investigated and reported the phenomenological aspects of M-N-C degradation, only a few modeling studies have considered degradation mechanisms at the atomic level. Understanding the mechanisms responsible for activity loss occurring in atomically dispersed M-N-C’s is crucial towards rationally designing active, durable, and less expensive Earth-abundant catalysts. Towards this end, we have surveyed recent literature concerning the modeling of corrosion mechanisms that impact M-N-C catalysts (Fe–N–C, in particular) and offer our own perspectives on the future direction of this field.

材料降解是限制可再生能源和清洁能源技术广泛应用的一个主要因素。对于铂族无金属(PGM-free)原子分散金属-氮-碳(M-N-C)催化剂来说尤其如此。虽然许多实验研究已经调查并报告了 M-N-C 降解的现象,但只有少数建模研究考虑了原子层面的降解机制。了解原子分散的 M-N-C 中发生活性损失的机理,对于合理设计活性、耐久性和低成本的地球富集催化剂至关重要。为此,我们对近期有关影响 M-N-C 催化剂(尤其是 Fe-N-C)腐蚀机制建模的文献进行了调查,并对该领域的未来发展方向提出了自己的看法。
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引用次数: 0
Current-mediated suppression of hydrogen evolution reaction in determination of Zn-metal Coulombic efficiency 在测定锌-金属库仑效率时以电流为媒介抑制氢进化反应
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-08 DOI: 10.1016/j.coelec.2024.101571
Mingyu Lee , Hyuntae Lee , Jaewoong Han , Chanyeon Kim , Hongkyung Lee

Coulombic efficiency (CE) is a crucial metric in battery research, particularly for aqueous Zinc (Zn)-metal batteries. Nonetheless, the accurate determination of Zn CE is complicated due to a lack of awareness about charge loss triggered by the hydrogen evolution reaction (HER) and non-standardized testing conditions. This study reveals the governing factors affecting the Zn CE measurement under different testing conditions, such as applied current density, Zn-plating capacity, and half-cell platforms. Through literature and experimental studies, it is evident that the Zn CE inherently increases with higher current densities and capacities. When decoupling the actual potentials of HER and Zn deposition, HER-triggered parasitic reactions can be self-suppressed owing to greater overpotential for HER than for Zn-plating at higher current densities. A consistent trend was observed when using different Zn salts and current collectors. This awareness can help standardize CE measuring protocols for validating novel concepts and materials.

库仑效率(CE)是电池研究中的一个重要指标,尤其是对于锌(Zn)金属水电池而言。然而,由于缺乏对氢进化反应(HER)引发的电荷损失的认识以及测试条件不规范,准确测定锌CE非常复杂。本研究揭示了不同测试条件下影响 Zn CE 测量的主要因素,如应用电流密度、镀锌容量和半电池平台。通过文献和实验研究发现,锌 CE 会随着电流密度和容量的增加而增加。如果将 HER 和 Zn 沉积的实际电位脱钩,由于在较高电流密度下 HER 的过电位大于 Zn 镀层的过电位,HER 触发的寄生反应可以自我抑制。在使用不同的锌盐和电流收集器时,观察到了一致的趋势。这种认识有助于标准化 CE 测量协议,以验证新概念和新材料。
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引用次数: 0
Electroanalysis as a method for monitoring photocatalytic processes: A perspective beyond remediation 电分析作为一种监测光催化过程的方法:超越补救的视角
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-30 DOI: 10.1016/j.coelec.2024.101570
Pádraig McDonagh , Nathan Skillen , Peter K.J. Robertson , Denis McCrudden

The advancement of photocatalytic technologies requires complete system efficiency, and to this end, electrochemical sensors have the potential to complement and enhance the development of semiconductor catalyst and reactor design. A particular advantage of electroanalysis is that the sensors may be incorporated directly into photocatalytic reactors to allow real-time in situ analysis. This can then facilitate more accurate process control in the photocatalytic reactor. This report highlights the use of electroanalysis to monitor photocatalytic processes, considering applications where it has been used to date. Relevant properties of the sensors, with particular interest on sensitivity and response times are detailed alongside comparison to the more commonly used analytical techniques. It also explores the most recent progressions beyond monitoring photocatalytic remediation processes including photocatalytic valorization and reactive oxygen species monitoring.

光催化技术的发展需要全面的系统效率,为此,电化学传感器有可能补充和加强半导体催化剂和反应器设计的发展。电分析法的一个特别优势是可以将传感器直接集成到光催化反应器中,进行实时分析。这将有助于对光催化反应器进行更精确的过程控制。本报告重点介绍了使用电分析法监测光催化过程的情况,并考虑了迄今为止使用电分析法的应用领域。报告详细介绍了传感器的相关特性,尤其是灵敏度和响应时间,并与更常用的分析技术进行了比较。报告还探讨了光催化修复过程监测以外的最新进展,包括光催化估值和活性氧监测。
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引用次数: 0
Interfacial science for electrosynthesis 电合成界面科学
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-11 DOI: 10.1016/j.coelec.2024.101569
Taemin Kim , Ye Ji Kim , Anna Wuttig

Interfacial science and electroorganic syntheses are inextricably linked because all electrochemical reactions occur at the interface between the electrode and the solution. Thus, the surface chemistry of the electrode material impacts the organic reaction selectivity. In this short review, we highlight emergent examples of electrode surface chemistries that enable selective electroorganic synthesis in three reaction classes: (1) hydrogenation, (2) oxidation, and (3) reductive C–C bond formation between two electrophiles. We showcase the breadth of techniques, including materials and in-situ characterization, requisite to establish mechanistic schemes consistent with the observed reactivity patterns. Leveraging an electrode's unique surface chemistry will provide complementary approaches to tune the selectivity of electroorganic syntheses and unlock an electrode's catalytic properties.

界面科学与电有机合成密不可分,因为所有电化学反应都发生在电极与溶液的界面上。因此,电极材料的表面化学会影响有机反应的选择性。在这篇简短的综述中,我们将重点介绍在以下三类反应中实现选择性电有机合成的电极表面化学新实例:(1) 加氢反应;(2) 氧化反应;(3) 两个亲电体之间还原性 C-C 键的形成。我们展示了包括材料和原位表征在内的各种技术,这些技术是建立与观察到的反应模式相一致的机理方案所必需的。利用电极独特的表面化学性质将为调整电有机合成的选择性和释放电极的催化特性提供补充方法。
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引用次数: 0
Organic fuels oxidation: A common misunderstanding related to non-noble fuel cell catalysts 有机燃料氧化:与非贵族燃料电池催化剂有关的常见误解
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-07-02 DOI: 10.1016/j.coelec.2024.101567
Galina A. Tsirlina

This opinion addresses a basic impossibility to use Ni-containing and similar mediator electrocatalysts for fuel cell anodes if the fuel is organic, and air (or oxygen) is the oxidant. The reason is that oxidation onset potential is always higher than O2/H2O equilibrium potential. These anodes can operate in fuel cells with peroxide, but the voltages reported for direct urea peroxide fuel cells demonstrate contradiction with urea oxidation onset potentials. Ni-containing anodes for “boosting” in water electrolysis and in electrochemical reforming present more heathy research branch.

如果燃料是有机物,而空气(或氧气)是氧化剂,则不可能将含镍和类似介质电催化剂用于燃料电池阳极。原因是氧化起始电位总是高于 O2/H2O 平衡电位。这些阳极可以在含有过氧化物的燃料电池中工作,但报告的直接过氧化尿素燃料电池的电压与尿素氧化起始电位存在矛盾。在水电解和电化学重整中用于 "增压 "的含镍阳极是更热门的研究领域。
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引用次数: 0
Hydrogels-empowered all-in-one supercapacitors: Current insights and prospects 水凝胶供电的一体化超级电容器:现状与前景
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-29 DOI: 10.1016/j.coelec.2024.101564
Arjun Kumar Bojarajan, Sambasivam Sangaraju

Flexible and wearable electronics are poised to revolutionize various domains, but the practical implementation of these devices is hindered by the significant difficulty of energy storage devices. An effective solution can be found in the advancement of high-performance supercapacitors by developing with the qualities of being integrated, elastic, and self-healable, without requiring additional film layers. Hydrogels greatly contributed to achieving this owing to their interesting properties, conductivity, and flexibility. This short review explores the recent progressions in all-in-one supercapacitors powered by hydrogels, highlighting their functional mechanisms of self-healing, ion transmission, and synchronous deformation. We discussed the potential applications in wearable electronics, medical devices, and flexible energy storage systems, focusing on design optimization and new functionalities. Furthermore, we provide insights into future research directions, guiding the exploration of novel additives and achieving high and stable performance.

柔性和可穿戴电子设备将给各个领域带来革命性的变化,但这些设备的实际应用却因能量存储设备的巨大困难而受到阻碍。通过开发具有集成性、弹性和自愈性的高性能超级电容器,而无需额外的薄膜层,可以找到有效的解决方案。水凝胶因其有趣的特性、导电性和柔韧性,为实现这一目标做出了巨大贡献。这篇简短的综述探讨了由水凝胶驱动的一体化超级电容器的最新进展,强调了其自修复、离子传输和同步变形的功能机制。我们讨论了在可穿戴电子设备、医疗设备和柔性储能系统中的潜在应用,重点关注设计优化和新功能。此外,我们还深入探讨了未来的研究方向,为探索新型添加剂和实现高稳定性能提供了指导。
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引用次数: 0
Dissolved iron in alkaline media: Techniques and insights for understanding its effects on water-splitting reactions 碱性介质中的溶解铁:了解其对分水反应影响的技术和见解
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-29 DOI: 10.1016/j.coelec.2024.101568
Arthur Bukowski , Pierre-Yves Olu , Armand Gering , Marian Chatenet , Antoine Bonnefont

Dissolved iron in alkaline media is an important topic influencing a wide array of electrochemical reactions and most notably those occurring in alkaline water electrolysers. This work compiles the study techniques and strategies that have been used in the past few years to help tackle this challenging issue. Focus is made on iron solubility in the studied medias, the importance of using a quality reference electrolyte, where and how to measure iron content in the system, and also on what is agreed and what is debated concerning the influence of dissolved iron on the hydrogen evolution reaction and oxygen evolution reaction, notably in the way these electrolyte impurities do enhance or alter the reactions kinetics.

碱性介质中的溶解铁是影响一系列电化学反应的重要课题,尤其是发生在碱性水电解槽中的反应。本研究汇编了过去几年中用于帮助解决这一挑战性问题的研究技术和策略。重点讨论了铁在所研究介质中的溶解度、使用优质参比电解质的重要性、在何处以及如何测量系统中的铁含量,还讨论了关于溶解铁对氢进化反应和氧进化反应的影响的共识和争论,特别是这些电解质杂质增强或改变反应动力学的方式。
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引用次数: 0
Advancements in the in-situ growth of catalysts for water electrolysis: Substrate considerations, performance evaluations, and future perspectives 水电解催化剂原位生长的进展:基质考虑、性能评估和未来展望
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-29 DOI: 10.1016/j.coelec.2024.101566
Ning Yang , Haonan Li , Jingyang Hao , Xiao Lin , Simon Kondrat , Christopher Hardacre , Wen-Feng Lin

In-situ growth of catalysts for water electrolysis has gained significant advancements recently, it involves cultivating active electrocatalysts on conductive substrates such as metal foams and carbon-based materials, the latter play a pivotal role in influencing the morphology and architecture of catalysts and offer enhanced conductivity, abundant active sites, and improved mass transport. Numerous studies have predominantly focused on evaluating specific catalyst materials within various classifications and their preparation methods, but without addressing roles of supports. This review focuses on substrate considerations, performance evaluations, and prospectives. It provides a deeper understanding of the various strategies employed for in-situ growth of electrocatalysts and emphasizes the importance of different conductive substrates with case studies on the factors that affect catalytic activity. Furthermore, the prospects and challenges towards practical applications under some challenging conditions are highlighted. This review provides valuable strategies for the further development of rational design of catalyst–substrate as an enabling electrode.

水电解催化剂的原位生长最近取得了重大进展,它涉及在金属泡沫和碳基材料等导电基底上培养活性电催化剂,后者在影响催化剂的形态和结构方面起着关键作用,并具有更强的导电性、丰富的活性位点和更好的质量传输。大量研究主要集中于评估各种分类中的特定催化剂材料及其制备方法,但没有涉及支撑物的作用。本综述侧重于基质考虑、性能评估和前景展望。通过对影响催化活性的因素进行案例研究,本综述加深了对电催化剂原位生长所采用的各种策略的理解,并强调了不同导电基底的重要性。此外,还强调了在一些具有挑战性的条件下实际应用的前景和挑战。这篇综述为进一步合理设计催化剂基底作为使能电极提供了宝贵的策略。
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引用次数: 0
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Current Opinion in Electrochemistry
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