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Determination of the reaction orders for electrode reactions 确定电极反应的反应顺序
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-09 DOI: 10.1016/j.coelec.2024.101597
Er-Fei Zhen, Bing-Yu Liu, Dong-Chen Zhao, Jing-Zhe Zhu, Yan-Xia Chen
Information of reaction orders is prerequisite in unveiling the mechanism(s) of complex electrocatalytic reactions, which is of great help in benchmarking the intrinsic electrocatalytic performance and in establishing the structure–activity relationship. However, electrochemical reaction orders for only few electrocatalytic reactions have hitherto been unambiguously quantified, due to the complexities of the reaction themselves and the complexities of interfacial environments. The apparent reaction orders may depend on the coverage of the adsorbed reactant, reactive intermediates at the electrode interface, their adsorption behavior, the occurrence of parallel pathways as well as existence pre or postchemical reactions. In this short review, theories and methods used for determination of the reaction orders for electrode reactions are summarized and exemplified by taking hydrogen evolution/oxidation reaction (HER/HOR) and oxygen reduction reaction (ORR) under rotating disk electrode configuration as model reactions. Frequently encountered challenges in accurate determination the reaction orders for complex electrocatalytic reactions are discussed.
反应阶次信息是揭示复杂电催化反应机理的先决条件,对确定内在电催化性能基准和建立结构-活性关系大有帮助。然而,由于反应本身的复杂性和界面环境的复杂性,迄今为止只有少数电催化反应的电化学反应阶次被明确量化。表观反应阶次可能取决于吸附反应物的覆盖范围、电极界面上的反应中间体、它们的吸附行为、平行途径的发生以及前化学反应或后化学反应的存在。在这篇简短的综述中,以旋转盘电极构型下的氢进化/氧化反应(HER/HOR)和氧还原反应(ORR)为模型反应,总结并举例说明了用于确定电极反应阶次的理论和方法。讨论了在准确确定复杂电催化反应的反应阶次时经常遇到的挑战。
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引用次数: 0
Electrochemical systems for renewable energy conversion and storage: Focus on flow batteries and regenerative fuel cells 用于可再生能源转换和储存的电化学系统:重点关注液流电池和再生燃料电池
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-03 DOI: 10.1016/j.coelec.2024.101596
Fengjia Xie , Xuming Zhang , Zhefei Pan
As the global shift towards renewable energy accelerates, energy storage solutions capable of providing long-duration, large-scale storage will be critical. Flow batteries and regenerative fuel cells have the potential to play a pivotal role in this transformation by enabling greater integration of variable renewable generation and providing resilient, grid-scale energy storage. This review provides an overview of the working principles of flow batteries and regenerative fuel cells mediated by ammonia, including the hardware, electrochemical reactions, and general performance. The recent advances in flow batteries are highlighted, covering the electrode design and modifications as well as electrolyte design and innovations. The recent advances in regenerative fuel cells are also discussed, focusing on membrane electrode assembly construction and system optimization.
随着全球加速向可再生能源转变,能够提供长时间、大规模储能的储能解决方案将变得至关重要。液流电池和蓄热式燃料电池可在这一转变中发挥关键作用,实现可变可再生能源发电的更大整合,并提供具有弹性的电网级储能。本综述概述了以氨为媒介的液流电池和再生燃料电池的工作原理,包括硬件、电化学反应和一般性能。重点介绍了液流电池的最新进展,包括电极设计和修改以及电解质设计和创新。还讨论了再生燃料电池的最新进展,重点是膜电极组件的构造和系统优化。
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引用次数: 0
Advancements in ordered membrane electrode assembly (MEA) for water electrolysis 用于电解水的有序膜电极组件 (MEA) 取得进展
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-10-02 DOI: 10.1016/j.coelec.2024.101595
Li Yu , Bin Tian , Wentao Huang , Xiaochun Zhou , Weihong Li
Proton exchange membrane (PEM) and anion exchange membrane (AEM) water electrolyzers exhibit superior efficiency and produce higher purity hydrogen compared to traditional alkaline water electrolyzers due to their membrane electrode assembly (MEA) design. However, random structures presented in current MEA designs introduce significant transport resistance for electrons and mass (ion, gas and liquid), consequently degrading the overall performance of electrolyzes. In contrast, ordered MEA structures are characterized by well-defined arrangements of pores, channels or pathways within catalyst layers (CLs), porous transport layers (PTLs), and ion exchange membranes (IEMs). These ordered configurations facilitate efficient highways for the transfer of electrons and mass. Recent diverse ordered MEA designs have demonstrated significant improvements in overall electrochemical efficiency in both PEM and AEM water electrolyzers. In this review, we will examine recent advancements in ordered MEA designs for water electrolyzers focusing on innovations in fabrication methods and interface morphologies, as well as their electrolysis performance. This review may provide comprehensive guidelines for designing ordered MEAs for both PEM and AEM electrolyzers.
与传统的碱性水电解槽相比,质子交换膜(PEM)和阴离子交换膜(AEM)水电解槽因其膜电极组件(MEA)设计而表现出更高的效率,并能产生纯度更高的氢气。然而,目前 MEA 设计中的随机结构为电子和质量(离子、气体和液体)带来了巨大的传输阻力,从而降低了电解槽的整体性能。与此相反,有序 MEA 结构的特点是催化剂层 (CL)、多孔传输层 (PTL) 和离子交换膜 (IEM) 中的孔隙、通道或通路排列整齐。这些有序配置为电子和质量的高效传输提供了便利。最近的各种有序 MEA 设计表明,PEM 和 AEM 水电解槽的整体电化学效率有了显著提高。在本综述中,我们将探讨水电解槽有序 MEA 设计的最新进展,重点关注制造方法和界面形态的创新及其电解性能。本综述可为 PEM 和 AEM 电解槽有序 MEA 的设计提供全面指导。
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引用次数: 0
Artificial protective layers of zinc metal anodes for reversible aqueous zinc ion batteries 用于可逆锌离子水电池的锌金属阳极人工保护层
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-26 DOI: 10.1016/j.coelec.2024.101594
Minghong Duan, Zhihao Yang, Qianqian Hou, Tieqi Huang, Hongtao Liu
Aqueous zinc ion batteries (AZIBs) are ideal candidates for next-generation energy storage technologies because they possess satisfactory safety, environmental friendliness, natural abundance, high theoretical specific capacity, and suitable redox potential. However, AZIBs are suffering serious anode issues, which limit their practical applications. To overcome these problems, architecting artificial protective layer (APL) on zinc metal is one of common modification strategies, which can effectively surpass the side reactions and dendrite generation by the designed functional coverings. In this review, we discuss the different materials applied in the APL and the corresponding specific working mechanism for anode optimization, as well as the challenges and perspectives of the strategies for APLs. The review aims at providing general principles and suggestions on the development of advanced anodes for AZIBs.
锌离子水电池(AZIBs)具有令人满意的安全性、环境友好性、天然丰富性、高理论比容量和合适的氧化还原电势,因此是下一代储能技术的理想候选材料。然而,AZIB 存在严重的阳极问题,限制了其实际应用。为了克服这些问题,在锌金属上构建人工保护层(APL)是常用的改性策略之一,通过设计功能性覆盖层可以有效地克服副反应和枝晶的产生。在这篇综述中,我们讨论了应用于 APL 的不同材料和相应的阳极优化具体工作机制,以及 APL 策略所面临的挑战和前景。本综述旨在为 AZIB 先进阳极的开发提供一般原则和建议。
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引用次数: 0
The chemical effect of a selenium atom on the catalytic site of precious metals 硒原子对贵金属催化位点的化学效应
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-25 DOI: 10.1016/j.coelec.2024.101593
Luis Alberto Estudillo-Wong , Nicolas Alonso-Vante
Transition metal selenides constitute a family of materials used for multi-electron charge transfer reactions (e.g. hydrogen evolution reaction, oxygen reduction reaction) in which activity, selectivity, and tolerance are required. Here we review the engineering of such structures focused on the selenization process of nanoparticulate precious metals supported or not on carbon. The chemical/electrochemical process of selenization proceeding through a so-called soft chemistry route, in which each species (cationic, anionic) interacts under conditions dictated by the solvent medium, is briefly described. The electronic effect of the synthesized materials subjected to the modification effects leading to undefined and/or defined phases (via chemical coordination) of the surface of the metallic atoms is reviewed.
过渡金属硒化物是一系列用于多电子电荷转移反应(如氢进化反应、氧还原反应)的材料,这些反应对材料的活性、选择性和耐受性都有很高的要求。在此,我们将对此类结构的工程学进行回顾,重点关注碳上支持或不支持的纳米贵金属的硒化过程。硒化的化学/电化学过程通过所谓的软化学途径进行,其中每个物种(阳离子、阴离子)在溶剂介质决定的条件下相互作用。综述了合成材料的电子效应,这些电子效应受到改性效应的影响,导致金属原子表面出现未定义和/或确定的相位(通过化学配位)。
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引用次数: 0
Green hydrogen from seawater electrolysis: Recent developments and future perspectives 海水电解产生的绿色氢气:最新进展和未来展望
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-20 DOI: 10.1016/j.coelec.2024.101592
Jaira Neibel Bamba , Alicia Theresse Dumlao , Rosela Mae Lazaro , DJ Donn Matienzo , Joey Ocon
Electrochemical splitting of seawater, especially when powered by renewable energy, presents a promising avenue for generating clean hydrogen without relying on highly pre-processed water from freshwater sources. In this mini-review, we present the fundamental principles of seawater electrolysis, including reaction mechanisms and various electrolyzer configurations, while addressing challenges. The most recent advancements in the field are highlighted, focusing on design strategies for electrocatalysts with high oxygen and hydrogen evolution reaction selectivity, electrolyte optimization, and membrane technologies. Additionally, the economic viability and scalability of seawater electrolysis are discussed, evaluating its feasibility for large-scale implementation. Collectively, this review offers insights into future developments and guides future research in the field, particularly in the rational design of corrosion-resistant seawater splitting technologies.
海水电化学裂解,尤其是以可再生能源为动力的海水电化学裂解,为无需依赖高度预处理的淡水水源而产生清洁氢气提供了一条前景广阔的途径。在这篇小型综述中,我们将介绍海水电解的基本原理,包括反应机制和各种电解槽配置,同时探讨面临的挑战。重点介绍了该领域的最新进展,包括具有高氧气和氢气进化反应选择性的电催化剂设计策略、电解质优化和膜技术。此外,还讨论了海水电解的经济可行性和可扩展性,评估了其大规模实施的可行性。总之,这篇综述为未来的发展提供了见解,并为该领域未来的研究提供了指导,特别是在合理设计耐腐蚀的海水分离技术方面。
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引用次数: 0
Insights into electrode–electrolyte interfaces by in situ scanning tunnelling microscopy 通过原位扫描隧道显微镜深入了解电极-电解质界面
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-12 DOI: 10.1016/j.coelec.2024.101580
Maren-Kathrin Heubach , Yannick Mattausch , Timo Jacob

Fundamental insights into electrode–electrolyte interfaces are crucial for our understanding of electrochemical processes. Standard electrochemical methods, such as cyclic voltammetry, can reveal important information about the systems of interest. Nevertheless, information about structure and morphology of the electrode–electrolyte interface is not that easily accessible. In situ scanning tunnelling microscopy can resolve the electrode as well as the direct interface to the electrolyte in real time during electrochemical measurements. This includes changes of the electrode in the nanometre to micrometre range, for example, during metal deposition or corrosion, as well as the observation of ordered molecular adlayers on the electrode. In this work, we want to highlight the capabilities of such studies to better understand the fundamental processes of electrocatalysis and metal deposition and dissolution, which are essential to electrochemical energy storage systems.

从根本上了解电极-电解质界面对我们理解电化学过程至关重要。循环伏安法等标准电化学方法可以揭示有关系统的重要信息。然而,有关电极-电解质界面结构和形态的信息却不那么容易获得。原位扫描隧道显微镜可以在电化学测量过程中实时解析电极以及与电解质的直接界面。这包括电极在纳米到微米范围内的变化,例如在金属沉积或腐蚀过程中的变化,以及对电极上有序分子吸附层的观察。在这项工作中,我们希望强调此类研究的能力,以便更好地理解电催化和金属沉积与溶解的基本过程,这对电化学储能系统至关重要。
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引用次数: 0
On-board hydrogen production from urea via electrolysis to promote low-temperature catalytic reduction of NOx emissions 通过电解利用尿素生产车载氢气,促进氮氧化物排放的低温催化还原
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-12 DOI: 10.1016/j.coelec.2024.101591
Jagoda J. Manss-Chmielarz , Tobias Morawietz , Aldo S. Gago , K. Andreas Friedrich
Nitrogen oxides emissions pose a significant environmental challenge, particularly in heavily industrialized, high-traffic regions. Global NOx levels continue to rise, despite various aftertreatment techniques being deployed to mitigate emission levels of combustion engine vehicles. Novel approaches to enhance NOx conversion efficiency at low exhaust temperatures (< 200 C) include integrating hydrogen and ammonia injection before selective catalytic reduction modules. Urea electrolysis presents a promising avenue for simultaneous hydrogen and ammonia production. An anion exchange membrane electrolyser emerges as a viable and low-cost solution for on-board hydrogen production, offering compact size and compatibility with existing vehicle systems. Overcoming challenges such as catalyst and component selection, electrolyte viability, and system integration remains critical for realising the full potential of electrolysis-based NOx mitigation strategies in passenger vehicles.
氮氧化物排放给环境带来了巨大挑战,尤其是在重工业化、交通繁忙的地区。尽管采用了各种后处理技术来降低内燃机汽车的排放水平,但全球氮氧化物水平仍在持续上升。在低排气温度(< 200 C)下提高氮氧化物转化效率的新方法包括在选择性催化还原模块之前集成氢气和氨气喷射。尿素电解为同时制氢和制氨提供了一条很有前景的途径。阴离子交换膜电解槽是一种可行的车载制氢低成本解决方案,具有体积小、与现有车辆系统兼容等优点。克服催化剂和组件选择、电解质可行性和系统集成等挑战,对于充分发挥基于电解的乘用车氮氧化物减排战略的潜力仍然至关重要。
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引用次数: 0
High entropy intermetallic compounds: A discovery platform for structure–property correlations and materials design principles in electrocatalysis 高熵金属间化合物:电催化结构-性能相关性和材料设计原理的发现平台
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-06 DOI: 10.1016/j.coelec.2024.101590
Ridha Zerdoumi , Alfred Ludwig , Wolfgang Schuhmann
The electrocatalytic properties of multi-metal materials are predominantly influenced by electronic and geometric effects related to surface and sub-surface atoms. A comprehensive understanding of these effects and their complex interplay is paramount for the efficient development of high-performance catalysts. Along with compositionally complex solid solutions (CCSS), often called high-entropy alloys (HEAs), high-entropy intermetallic compounds (HEIMCs) are an emerging class of materials with distinctive properties originating from both high-entropy alloys and intermetallic compounds. The ordered intermetallic structure is beneficial for identifying structure–property correlations of catalytic surfaces. This minireview provides a summary of the current knowledge of high entropy intermetallic compounds and their role in catalysis, with a particular focus on the key tunable parameters essential for achieving high-performance materials.
多金属材料的电催化特性主要受到与表面和次表面原子有关的电子和几何效应的影响。全面了解这些效应及其复杂的相互作用对于高效开发高性能催化剂至关重要。高熵金属间化合物(HEIMC)与成分复杂固溶体(CCSS)(通常称为高熵合金(HEA))一样,是一类新兴的材料,具有源于高熵合金和金属间化合物的独特性能。有序的金属间结构有利于确定催化表面的结构-性能相关性。这篇微型综述概述了高熵金属间化合物的现有知识及其在催化中的作用,尤其侧重于实现高性能材料所必需的关键可调参数。
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引用次数: 0
Current perspectives on rational design of anode electrocatalysts exhibiting CO-tolerance for fuel cells 合理设计燃料电池耐一氧化碳阳极电催化剂的当前视角
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-08-31 DOI: 10.1016/j.coelec.2024.101582
Daeil Choi , Subin Park , Yun Sik Kang , Sung Jong Yoo

Anode catalysis reduces the cost and remarkably improves the fuel cell performance; however, it is often neglected owing to its fast kinetics. Currently, the majority of hydrogen is obtained by reforming and purifying the hydrocarbons containing impurities such as CO, CO2, and H2S. CO adsorbs more strongly than hydrogen onto the anode catalysts, inhibiting hydrogen oxidation and resulting in performance degradation. Although activity enhancement is essential, impurity tolerance should be preferred over activity for fuel-cell anode catalysts. Various studies have reported improved CO tolerance via lowering the intrinsic CO adsorption energy of the catalyst by tuning the electronic structure or modulating the OH adsorption energy by placing oxophilic materials near the catalysts. Herein, we categorize recent noteworthy studies according to their strategies and present innovative design principles for CO-resistant anode catalysts.

阳极催化可降低成本并显著提高燃料电池的性能;然而,由于其快速的动力学特性,阳极催化常常被忽视。目前,大部分氢气是通过重整和提纯含有 CO、CO 和 HS 等杂质的碳氢化合物获得的。CO 在阳极催化剂上的吸附力比氢更强,会抑制氢氧化,导致性能下降。虽然提高活性至关重要,但对于燃料电池阳极催化剂来说,杂质耐受性应优先于活性。各种研究报告称,通过调整催化剂的电子结构降低催化剂对 CO 的固有吸附能,或通过在催化剂附近放置亲氧材料调节 OH 吸附能,可提高对 CO 的耐受性。在此,我们将近期值得关注的研究按照其策略进行分类,并介绍抗 CO 阳极催化剂的创新设计原则。
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引用次数: 0
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Current Opinion in Electrochemistry
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