Current Opinion in Electrochemistry最新文献

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Measuring the flatband potential in 2D semiconductors: Pitfalls and a possible SECCM solution 测量二维半导体中的平带电位：陷阱和可能的SECCM解决方案

IF 7.9 2区化学 Q1 CHEMISTRY, PHYSICAL

Current Opinion in Electrochemistry

Pub Date : 2025-04-28 DOI: 10.1016/j.coelec.2025.101703

Ava R. Chard, Justin B. Sambur

The flatband potential (V_fb) is a critical parameter in semiconductor electrochemistry, defining the potential at which no excess charge exists at the semiconductor/electrolyte interface. It serves as a key reference for interpreting charge transfer kinetics and current–voltage behavior. However, conventional methods like Mott–Schottky analysis fail for atomically thin 2D materials due to the breakdown of the depletion approximation. This perspective examines the limitations of traditional V_fb measurements for 2D semiconductors and the experimental challenges that arise. To address these issues, we propose using scanning electrochemical cell microscopy (SECCM) to spatially resolve the potential of zero charge (V_pzc), equivalent to V_fb. This approach mitigates sample heterogeneity issues, such as pinholes or multilayer defects, and offers a pathway to more accurate electrochemical characterization. Ultimately, this method will enhance understanding of current–potential behavior in 2D materials, supporting the design of advanced systems for photoelectrocatalysis, energy conversion, and sensing.

平坦带电位（Vfb）是半导体电化学中的一个关键参数，它定义了半导体/电解质界面上不存在多余电荷的电位。它是解释电荷转移动力学和电流-电压行为的关键参考。然而，传统的方法，如莫特-肖特基分析失败的原子薄的二维材料，由于损耗近似的破坏。这一视角考察了传统的二维半导体Vfb测量的局限性以及由此产生的实验挑战。为了解决这些问题，我们提出使用扫描电化学电池显微镜（SECCM）来空间解析零电荷电位（Vpzc），相当于Vfb。这种方法减轻了样品的非均质性问题，如针孔或多层缺陷，并为更准确的电化学表征提供了途径。最终，该方法将增强对二维材料中电流-电位行为的理解，支持设计用于光电催化、能量转换和传感的先进系统。

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引用次数: 0

Operando methods for the elucidation of electrolyte effects in electrocatalysis 阐明电催化中电解质效应的操作方法

IF 7.9 2区化学 Q1 CHEMISTRY, PHYSICAL

Current Opinion in Electrochemistry

Pub Date : 2025-04-17 DOI: 10.1016/j.coelec.2025.101700

Kees E. Kolmeijer, Rik V. Mom

The electrolyte pH, ion composition, and solvent are important design parameters in electrocatalytic systems, which directly impact the system’s catalytic activity, selectivity and stability. However, the relationship between the electrolyte composition and electrocatalytic performance is complex, and at present difficult to predict. To elucidate the underlying principles that govern electrolyte effects in electrocatalysis, operando techniques capable of resolving the active site structures at the electrode–electrolyte interface play a crucial role. Here, we review the current capabilities of these operando techniques and analyze how they can be used to find the rules of the game for electrolyte engineering.

电解液pH、离子组成和溶剂是电催化系统重要的设计参数，直接影响系统的催化活性、选择性和稳定性。然而，电解质组成与电催化性能之间的关系是复杂的，目前很难预测。为了阐明电催化中控制电解质效应的基本原理，能够解析电极-电解质界面活性位点结构的operando技术起着至关重要的作用。在这里，我们回顾了这些operando技术的当前能力，并分析了如何使用它们来找到电解质工程的游戏规则。

引用次数: 0

Effects of electrolyte cations on the oxygen evolution reaction 电解质阳离子对析氧反应的影响

IF 7.9 2区化学 Q1 CHEMISTRY, PHYSICAL

Current Opinion in Electrochemistry

Pub Date : 2025-04-16 DOI: 10.1016/j.coelec.2025.101697

Boqiang Chen, Dunwei Wang, Matthias M. Waegele

The oxidation of water to molecular oxygen, referred to as the oxygen evolution reaction (OER), is often the kinetic bottleneck in the formation of renewable fuels. The rate of the OER is strongly dependent on electrolyte properties, such as pH, ionic strength, and the identities of anions and cations. To advance OER catalysis, it is essential to understand the mechanisms by which the electrolyte influences the rate of the OER. In this article, we discuss recent work concerned with the effects of electrolyte cations on the OER. We examine how cations modulate apparent Arrhenius parameters, their effects on the interfacial water structure, their direct interactions with intermediates, and how they alter the rate through non-kinetic effects. The survey reveals that cations can influence the OER through a diversity of mechanisms and that their effects strongly depend on catalyst composition and reaction conditions.

水氧化为分子氧，称为析氧反应（OER），通常是形成可再生燃料的动力学瓶颈。OER的速率很大程度上取决于电解质的性质，如pH值、离子强度以及阴离子和阳离子的特性。为了推进OER催化，必须了解电解质影响OER速率的机制。在本文中，我们讨论了最近有关电解质阳离子对OER的影响的工作。我们研究了阳离子如何调节表观阿伦尼乌斯参数，它们对界面水结构的影响，它们与中间体的直接相互作用，以及它们如何通过非动力学效应改变速率。调查表明，阳离子可以通过多种机制影响OER，其影响在很大程度上取决于催化剂的组成和反应条件。

引用次数: 0

3D-printed thermoplastic sensors for electrochemical biosensing 用于电化学生物传感的3d打印热塑性传感器

IF 7.9 2区化学 Q1 CHEMISTRY, PHYSICAL

Current Opinion in Electrochemistry

Pub Date : 2025-04-15 DOI: 10.1016/j.coelec.2025.101699

Christos Kokkinos

While the importance of electrochemical sensors in diagnostics is well established—offering rapid and selective biomarker determinations in complex matrices—there is a continuous request for simpler, more cost-effective and sustainable sensor fabrication procedures. 3D-printing technologies, particularly fused deposition modeling (FDM), allow for the digital, rapid, and labor-free fabrication of disposable (bio)sensors, while also enabling the printing of fully integrated, miniaturized plastic devices within points-of-need settings. This review highlights recent trends in the development of 3D-printed thermoplastic (bio)sensors and mini devices that utilize bioelements and artificial biomimetic materials for biomolecules monitoring. Additionally, it provides an overview of the synthesis of tailor-made 3D printable conductive filaments incorporating biofunctional materials, from which ready-to-use sensors are fabricated for direct biosensing.

虽然电化学传感器在诊断中的重要性已经确立，可以在复杂的基质中提供快速和选择性的生物标志物测定，但人们一直要求更简单，更具成本效益和可持续的传感器制造工艺。3d打印技术，特别是熔融沉积建模（FDM），可以实现一次性（生物）传感器的数字化、快速和免人工制造，同时还可以在需要的地方打印完全集成的小型化塑料设备。本文综述了利用生物元素和人工仿生材料进行生物分子监测的3d打印热塑性（生物）传感器和微型设备的最新发展趋势。此外，它还概述了结合生物功能材料的定制3D可打印导电细丝的合成，从中制备了用于直接生物传感的即用型传感器。

引用次数: 0

Cation effects in electrochemical CO2 reduction 电化学CO2还原中的阳离子效应

IF 7.9 2区化学 Q1 CHEMISTRY, PHYSICAL

Current Opinion in Electrochemistry

Pub Date : 2025-04-14 DOI: 10.1016/j.coelec.2025.101698

Adnan Ozden , Yanwei Lum

Electrochemical CO₂ reduction (CO₂R) provides a pathway toward the sustainable production of chemicals. Recent catalyst- and system-level innovations have enabled electrosynthesis of multi-carbon products at practical productivities (>200 mA cm⁻²) and single-pass CO₂ conversion efficiencies (>80 %). However, practical CO₂R requires high single product selectivity (>85 %) without compromising readily-achieved metrics. Coupling these metrics in a single system warrants clear understanding of the electrical double layer at the catalyst–electrolyte interface. Combining selective catalysts with cation effects can effectively tune CO₂R kinetics at the catalyst–electrolyte interface. Here we overview recent progress and current understanding on the sophisticated nature of the cation effects and underscore critical parameters that influence cation distributions in the electrical double layer. We highlight the emerging characterization and computational approaches to elucidate cation effects on CO₂R. Finally, we emphasize research directions through which cation effects could be coupled with other micro-reaction environment tuning strategies for further selectivity and efficiency improvements.

电化学CO2还原（CO2R）为化学品的可持续生产提供了一条途径。最近的催化剂和系统级创新使多碳产品的电合成具有实际生产力（200毫安厘米−2）和单道二氧化碳转化效率（80%）。然而，实际的CO2R需要高的单一产品选择性（> 85%），而不影响容易实现的指标。将这些指标耦合到一个系统中，可以清楚地了解催化剂-电解质界面上的双电层。选择性催化剂与阳离子效应的结合可以有效地调节催化剂-电解质界面上的CO2R动力学。在这里，我们概述了最近的进展和目前对阳离子效应复杂性质的理解，并强调了影响双电层中阳离子分布的关键参数。我们强调了新兴的表征和计算方法来阐明对CO2R的影响。最后，我们强调了阳离子效应可以与其他微反应环境调节策略耦合以进一步提高选择性和效率的研究方向。

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引用次数: 0

Nanoconfined constructs for electrochemical aptamer-based in vivo biosensing 基于电化学适体体的体内生物传感纳米结构

IF 7.9 2区化学 Q1 CHEMISTRY, PHYSICAL

Current Opinion in Electrochemistry

Pub Date : 2025-04-11 DOI: 10.1016/j.coelec.2025.101695

Grayson F. Huldin , Junming Huang , Kaiyu X. Fu

In the last two decades, electrochemical aptamer-based (EAB) sensors have grown rapidly due to their high sensitivity, good selectivity, excellent biocompatibility, and flexible architectures among the wide range of biosensing platforms. Yet, achieving continuous, long-term, and in vivo monitoring remains challenging due to obstacles like device miniaturization, signal amplification, and sensor stability. To tackle these hurdles, researchers are leveraging nanostructured electrodes, leading to new EAB designs with improved in vivo biosensing performance. This opinion provides a brief overview of the development and latest progress in nanoconfined constructs for EAB in vivo biosensing. We illustrate fundamental sensing principles, the various nanostructures being explored, and their respective advantages. These nanostructured EABs hold promise for applications spanning disease diagnostics, environmental surveillance, and food safety management. Finally, we address the persistent challenges EABs face and discuss potential future directions, offering insights into how these sensors can continue to evolve and foster more effective healthcare technologies.

近二十年来，基于电化学适体（EAB）的传感器以其高灵敏度、良好的选择性、良好的生物相容性和灵活的结构在各种生物传感平台中得到了迅速发展。然而，由于设备小型化、信号放大和传感器稳定性等障碍，实现连续、长期和体内监测仍然具有挑战性。为了克服这些障碍，研究人员正在利用纳米结构电极，从而设计出具有更好的体内生物传感性能的新型EAB。本文简要介绍了用于EAB体内生物传感的纳米结构的发展和最新进展。我们阐述了基本的传感原理，各种正在探索的纳米结构，以及它们各自的优势。这些纳米结构的EABs有望应用于疾病诊断、环境监测和食品安全管理。最后，我们讨论了eab面临的持续挑战，并讨论了潜在的未来方向，提供了这些传感器如何继续发展和促进更有效的医疗保健技术的见解。

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引用次数: 0

Expanding our view on active sites in electrocatalysis 拓展了我们对电催化活性位点的认识

IF 7.9 2区化学 Q1 CHEMISTRY, PHYSICAL

Current Opinion in Electrochemistry

Pub Date : 2025-04-11 DOI: 10.1016/j.coelec.2025.101692

Ana M. Gómez–Marín , Katrin F. Domke

At the heart of electrocatalyst design and development lies the concept of active sites that are usually identified as those sites for adsorption where the conversion of interest occurs. However, electrochemical interfaces are complex systems where the exact structure and dynamics of interfacial species during a reaction greatly depend on the local reactive microenvironment, including co-adsorbates and solvent molecules, that may include structural transformations upon adsorption, the charge-transfer dynamics, and/or the x,y charge-induced electric field distribution. We review the concept of active sites in electrocatalysis within these lines in light of recent studies that point out the necessity to expand the still widely spread idea of quasi-static atomic-scale sites toward the picture of a dynamically reactive microenvironment: the active site can extend over several tens on nanometers due to surface structural transformations during the reaction, includes interdependent components such as electrode and electrolyte as well as target reactant geometric and electronic structures, and often spontaneously rearranges during the electrocatalytic reaction. Thus, to define optimal reactions conditions, the reactive microenvironment as a whole needs to be considered.

电催化剂设计和开发的核心是活性位点的概念，活性位点通常被确定为发生感兴趣转化的吸附位点。然而，电化学界面是复杂的系统，在反应过程中，界面物质的确切结构和动力学很大程度上取决于局部的反应微环境，包括共吸附物和溶剂分子，这可能包括吸附时的结构转变、电荷转移动力学和/或x、y电荷诱导的电场分布。根据最近的研究，我们回顾了电催化中活性位点的概念，这些研究指出有必要将仍然广泛传播的准静态原子尺度位点的概念扩展到动态反应微环境的图景中。由于反应过程中的表面结构变化，活性位点可以延伸几十纳米，包括相互依赖的成分，如电极和电解质以及目标反应物的几何和电子结构，并且在电催化反应过程中经常自发地重新排列。因此，为了确定最佳的反应条件，需要从整体上考虑反应微环境。

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引用次数: 0

Recent advancements related to silver-based electrocatalysts for carbon dioxide reduction reaction to carbon monoxide 银基电催化剂在二氧化碳还原成一氧化碳反应中的最新进展

IF 7.9 2区化学 Q1 CHEMISTRY, PHYSICAL

Current Opinion in Electrochemistry

Pub Date : 2025-04-11 DOI: 10.1016/j.coelec.2025.101696

Cristina Tricella, Mohsin Muhyuddin, Roberto Nisticò, Sergio Tosoni, Carlo Santoro

Electrochemical CO₂ reduction reaction (CO₂RR) is a progressive step toward the reduction of planetary carbon footprint. In this way, CO₂ can be valorized into valuable products, and particularly, CO₂ can be reduced to gaseous products (e.g. CO or methane) or into liquid products (i.e. C₁, C₂, C₃, etc.). Interestingly, CO₂RR and hydrogen reduction reaction (HER) are competitive reactions; therefore, syngas (CO + H₂) can also be produced at different H₂:CO ratios. Depending on the transition metal used as an electrocatalyst for the CO₂RR, the selectivity toward a specific product can be properly tuned. In this opinion, the attention is focused on the reduction of CO₂ to CO using Ag-based electrocatalysts. Reaction mechanisms to produce H₂, CO, and formate are described and highlighted. The effect of the morphology is described, and the performance of Ag-based electrocatalysts toward CO₂-to-CO and syngas production is presented, focusing on the recent available literature.

电化学CO2还原反应（CO2RR）是减少地球碳足迹的一个渐进步骤。这样，CO2就可以被活化成有价值的产物，特别是CO2可以被还原成气态产物（如CO或甲烷）或液态产物（如C1、C2、C3等）。有趣的是，CO2RR和氢还原反应（HER）是竞争性反应；因此，合成气（CO + H2）也可以在不同的H2:CO比下生产。根据用作CO2RR电催化剂的过渡金属，可以适当地调整对特定产物的选择性。在这种观点下，人们的注意力集中在使用银基电催化剂将CO2还原为CO上。反应机理产生H2， CO和甲酸的描述和强调。描述了形貌的影响，并介绍了银基电催化剂在co -to- co和合成气生产中的性能，重点介绍了最近的文献。

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引用次数: 0

Unlocking emerging catalytic applications of single-entity collision electrochemistry 解锁单一实体碰撞电化学的新兴催化应用

IF 7.9 2区化学 Q1 CHEMISTRY, PHYSICAL

Current Opinion in Electrochemistry

Pub Date : 2025-04-08 DOI: 10.1016/j.coelec.2025.101694

Yixiao Wang, Wei Ma

Establishing the link between catalytic activity and the structure of individual entities in an ensemble system can be challenging, as the presented data are often averaged in bulk system. Single-entity collision electrochemistry (SECE) stands out as a powerful tool for investigating the intrinsic catalytic activities of single entities with high sensitivity, high throughput, and fast response. Recent advancements in SECE technology have demonstrated significant potential in various emerging applications, particularly in the rapid screening of catalysts and supports, in situ identification of catalytic activity and assembly structure, and real-time monitoring of dynamic catalytic behaviors. This review summarizes the recent research results, pioneering studies, and future trends in this field. It also discusses the challenges faced by SECE in exploring new application scenarios.

建立催化活性与整体系统中单个实体结构之间的联系可能具有挑战性，因为所提供的数据通常是在整体系统中平均的。单实体碰撞电化学（SECE）具有高灵敏度、高通量和快速响应能力，是研究单实体内在催化活性的有力工具。近年来，see技术的进步在各种新兴应用中显示出巨大的潜力，特别是在催化剂和载体的快速筛选、催化活性和组装结构的原位鉴定以及动态催化行为的实时监测方面。本文综述了该领域的最新研究成果、前沿研究以及未来发展趋势。本文还讨论了sce在探索新的应用场景时所面临的挑战。

引用次数: 0

Overcoming dichotomy between surface and bulk of electrode: Conducting polymers 克服电极表面和体积之间的二分法：导电聚合物

IF 7.9 2区化学 Q1 CHEMISTRY, PHYSICAL

Current Opinion in Electrochemistry

Pub Date : 2025-04-04 DOI: 10.1016/j.coelec.2025.101691

Viktor Gueskine , Penghui Ding , Reverant Crispin , Mikhail Vagin

The surface of the solid-state electrodes constructed from atomic crystals is inherently uncertain due to its chemical unsaturation as its atoms lack the surrounding by the atoms of the same type as in the bulk and its exposure to a different phase. This complicates the evaluation of properties for the high surface area electrodes achieved by porosity. Conducting polymers (CP) are intrinsically conductive molecular solids built from polymeric conjugated molecules without covalent bounds between them. The molecular character of CP implies the translation of identical state from the bulk to the surface of the film without additional surface-induced defects. The absence of covalent bonds between backbones enables the access of external electrolyte to individual chain of CP forming the electrical double layer at the molecular scale. Here we discuss the combination of molecular porosity of CP with its inherent selectivity of ion transport as a special case of porous electrode. We also discuss how the Gibbs phase rule can help in understanding CP electrochemistry.

由原子晶体构成的固态电极的表面由于其化学不饱和而具有固有的不确定性，因为它的原子缺乏与体中相同类型的原子的包围，并且暴露于不同的相。这使得通过孔隙率获得的高表面积电极的性能评估变得复杂。导电聚合物（CP）是由聚合物共轭分子组成的具有内在导电性的分子固体，它们之间没有共价键。CP的分子特性意味着相同的状态从体到膜表面的转换，而没有额外的表面缺陷。骨干间共价键的缺失使得外部电解质能够接触到CP的单个链，从而在分子尺度上形成双电层。作为多孔电极的一种特殊情况，我们讨论了CP的分子孔隙度及其固有的离子传输选择性。我们还讨论了吉布斯相律如何帮助理解CP电化学。

引用次数: 0

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