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Progress and pitfalls in measuring the double-layer capacitance of platinum electrodes 铂电极双层电容测量的进展与缺陷
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-07-05 DOI: 10.1016/j.coelec.2025.101727
Nicci L. Fröhlich, Marc T.M. Koper
Despite extensive research, the double-layer structure at Pt/aqueous electrolyte interfaces (quantified by the double-layer capacitance, Cdl) remains incompletely understood as even for the model Pt(111)/HClO4 interface, anomalous Cdl trends have been reported. These trends were previously ascribed to differences in measurement techniques (i.e. dc methods such as cyclic voltammetry versus ac methods such as electrochemical impedance spectroscopy [EIS]). However, by repeating these measurements using EIS, we clarify that these anomalous Cdl trends are not measurement artefacts but instead reflect intrinsic properties of the Pt(111)/HClO4 interface, necessitating continued investigation. We further highlight the complexity introduced by electrosorbed Hads and/or OHads species resulting from catalytic H2O dissociation, which contribute an adsorption (pseudo)capacitance, Cads. This complicates the deconvolution of Cdl from total capacitance, a challenge further exacerbated by structure-dependent adsorption between different Pt facets. Our goal is to clarify how these factors affect capacitance interpretation at Pt/aqueous electrolyte interfaces, particularly highlighting the progress and challenges in accurately extracting Cdl values from prior studies.
尽管进行了广泛的研究,但Pt/水电解质界面的双层结构(由双层电容Cdl量化)仍然不完全清楚,即使对于模型Pt(111)/HClO4界面,也报道了异常的Cdl趋势。这些趋势以前被归因于测量技术的差异(即直流方法,如循环伏安法与交流方法,如电化学阻抗谱[EIS])。然而,通过使用EIS重复这些测量,我们澄清了这些异常的Cdl趋势不是测量的人工产物,而是反映了Pt(111)/HClO4界面的固有性质,需要继续研究。我们进一步强调了由催化H2O解离产生的电吸附Hads和/或OHads物种引入的复杂性,它们有助于吸附(伪)电容,Cads。这使得Cdl从总电容中反褶积变得复杂,不同Pt面之间的结构依赖吸附进一步加剧了这一挑战。我们的目标是澄清这些因素如何影响Pt/水电解质界面的电容解释,特别是强调从先前的研究中准确提取Cdl值的进展和挑战。
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引用次数: 0
Time: The potentially powerful, often-overlooked variable in electrochemical sensing of per- and polyfluoroalkyl substances 时间:全氟烷基和多氟烷基物质电化学传感中潜在的强大的、经常被忽视的变量
IF 6.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-07-02 DOI: 10.1016/j.coelec.2025.101726
Samantha C. Cullom , Jeffrey E. Dick
Modern electrochemistry places a heavy emphasis on the importance of thermodynamic measurements for environmental sensing. While most electrochemical sensors require some type of binding mechanism, analytes do not bind to sensors instantaneously; the binding process takes time, suggesting that we must examine reaction kinetics as well. With emerging environmental pollutants of concern, such as per- and polyfluoroalkyl substances (PFAS), electrochemists must consider the kinetic relationship between the electrochemical sensor and the analyte. Various types of environmental electrochemical sensors, such as enzymes, antibodies, aptamers, and molecularly imprinted polymers (MIPs), exist. Each type of sensor can be used in the environment, but MIPs have recently demonstrated strong potential to qualitatively and quantitatively detect and identify PFAS species at the earliest onset of environmental contamination. Additionally, the mathematical and experimental approaches to MIP binding have room to expand beyond the thermodynamic isotherm models and into a time-dependent kinetic model.
现代电化学非常重视热力学测量对环境传感的重要性。虽然大多数电化学传感器需要某种类型的结合机制,但分析物不会立即与传感器结合;结合过程需要时间,这表明我们也必须研究反应动力学。随着新出现的环境污染物,如全氟烷基和多氟烷基物质(PFAS)的关注,电化学化学家必须考虑电化学传感器和分析物之间的动力学关系。存在各种类型的环境电化学传感器,如酶、抗体、适体和分子印迹聚合物(MIPs)。每种类型的传感器都可以在环境中使用,但MIPs最近显示出在环境污染最早开始时定性和定量检测和识别PFAS物种的强大潜力。此外,MIP结合的数学和实验方法有空间扩展到热力学等温线模型和时间相关的动力学模型。
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引用次数: 0
Portable electrochemical sensors for per- and polyfluoroalkyl substances: Design, challenges, and opportunities for field deployment 用于全氟烷基和多氟烷基物质的便携式电化学传感器:现场部署的设计、挑战和机遇
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-07-01 DOI: 10.1016/j.coelec.2025.101725
Nishi Gondhiya, Abd Ur Rehman, Daniel Andreescu, Silvana Andreescu
The widespread presence of per- and polyfluoroalkyl substances (PFAS) in the environment presents a complex global challenge due to their persistence, resistance to degradation, and harmful effects. Electrochemical sensors offer the sensitivity needed to detect PFAS at regulatory limits and show promise for large-scale environmental monitoring without the need for costly laboratory equipment. This review highlights recent advances in electrochemical sensing technologies and their potential as field-deployable devices for rapid screening and on site PFAS detection. Examples include sensor platforms based on redox-active reporters, molecularly imprinted polymers (MIPs), redox dyes, metal organic frameworks (MOFs), covalent organic frameworks (COFs), nanoparticle impacts, and nanobubble and nanopore technologies, coupled with direct or indirect signal transduction strategies. We discuss promising sensor designs and detection mechanisms and outline the key challenges and future directions needed to advance their practical deployment in environmental monitoring applications.
全氟烷基和多氟烷基物质(PFAS)在环境中的广泛存在,由于其持久性、抗降解性和有害影响,构成了一个复杂的全球性挑战。电化学传感器提供了在法规限制下检测PFAS所需的灵敏度,并且在不需要昂贵的实验室设备的情况下显示出大规模环境监测的前景。本文综述了电化学传感技术的最新进展及其作为快速筛选和现场PFAS检测的现场可部署设备的潜力。例子包括基于氧化还原活性报告的传感器平台、分子印迹聚合物(MIPs)、氧化还原染料、金属有机框架(mfs)、共价有机框架(COFs)、纳米颗粒冲击、纳米泡和纳米孔技术,以及直接或间接的信号转导策略。我们讨论了有前途的传感器设计和检测机制,并概述了推进其在环境监测应用中的实际部署所需的关键挑战和未来方向。
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引用次数: 0
The role of interfacial water in promoting C–C coupling during CO2 electroreduction CO2电还原过程中界面水促进C-C耦合的作用
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-06-19 DOI: 10.1016/j.coelec.2025.101722
Anthony Shoji Hall , David Raciti
The electrochemical reduction of CO2 (CO2RR) into hydrocarbons and oxygenates presents a promising pathway toward a carbon-neutral energy cycle, but achieving selective product formation remains a challenge. While extensive efforts have focused on catalyst design and electrolyte composition, the role of the interfacial water properties, an often-overlooked parameter, has only recently come under investigation. Water serves as the primary proton donor (in aqueous electrolytes) in the absence of hydronium, which can influence the competition between CO2RR and the hydrogen evolution reaction (HER). Despite studies dating back to the 1980s demonstrating that electrolyte composition significantly impacts CO2RR performance, the effects of the electrolyte composition on the interfacial water properties have remained largely unexplored. Recent findings suggest that tuning the interfacial water properties can influence C–C coupling by altering solvation environments and stabilize reaction intermediates. This perspective explores how tuning the interfacial water properties improves C–C coupling, providing a new strategy for improving catalysis.
电化学还原CO2 (CO2RR)为碳氢化合物和含氧化合物提供了一条通往碳中性能量循环的有希望的途径,但实现选择性产物形成仍然是一个挑战。虽然人们在催化剂设计和电解质组成方面投入了大量的精力,但界面水性质(一个经常被忽视的参数)的作用直到最近才得到研究。在不存在水合氢离子的情况下,水作为主要质子供体(在含水电解质中),会影响CO2RR之间的竞争和析氢反应(HER)。尽管早在20世纪80年代就有研究表明,电解质成分会显著影响CO2RR性能,但电解质成分对界面水性质的影响在很大程度上仍未被探索。最近的研究表明,调整界面水性质可以通过改变溶剂化环境和稳定反应中间体来影响C-C耦合。这一观点探讨了调整界面水性质如何改善C-C耦合,为改善催化提供了一种新的策略。
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引用次数: 0
Feasibility of the hydrogen production by assistance of ethanol: A critical perspective 乙醇辅助制氢的可行性:一个批判的观点
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-06-17 DOI: 10.1016/j.coelec.2025.101723
Seiti Inoue Venturini, Manuel J.S. Farias, Germano Tremiliosi-Filho
Traditional electrolytic water splitting is one of the usual ways to produce molecular hydrogen. However, the specific slow kinetics of the complementary anodic molecular oxygen generation harm the efficiency of hydrogen evolution. One of the ways to get around this problem is to replace the slow oxygen reaction by another anodic reaction, with higher faradaic efficiency, such as those involving biomass derivatives, especially the ethanol, setting up the electrochemical ethanol reformer. Thus, in this work is made a critical review of recent researchers regarding the development of catalytic materials for both, hydrogen reaction and ethanol oxidation.
传统的电解水裂解是生产氢分子的常用方法之一。然而,互补阳极分子产氧特有的慢动力学损害了析氢效率。解决这一问题的方法之一是用另一种法拉第效率更高的阳极反应代替缓慢的氧反应,例如涉及生物质衍生物的反应,特别是乙醇,建立电化学乙醇重整器。因此,在这项工作中,对最近研究人员关于氢反应和乙醇氧化催化材料的发展进行了批判性的回顾。
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引用次数: 0
Harnessing instrumentation and artificial intelligence for new insights and applications in single-entity electrochemistry 利用仪器和人工智能在单一实体电化学中的新见解和应用
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-06-16 DOI: 10.1016/j.coelec.2025.101724
Gabriel Gemadzie , Peter McPike , Aliaksei Boika
The field of single-entity electrochemistry (SEE) has rapidly evolved, driven by innovative advancements in instrumentation, sophisticated data analysis powered by artificial intelligence (AI) and machine learning (ML), and an expanding range of applications across multiple disciplines. This review highlights significant recent progress in instrument developments that enhance the spatial and temporal resolution of SEE measurements, as well as data analysis employing AI methodologies to improve the processing, interpretation, and accuracy of complex electrochemical datasets. Additionally, we provide an overview of impactful recent applications of SEE in energy storage, catalysis, environmental monitoring, and biosensing, demonstrating the critical importance and transformative potential of single-entity measurements. By integrating advanced instrumentation with powerful data analytical frameworks, SEE continues to reveal unique insights at the nanoscale, bridging fundamental electrochemical research and practical applications.
由于仪器仪表的创新进步,人工智能(AI)和机器学习(ML)驱动的复杂数据分析以及跨多个学科的应用范围不断扩大,单实体电化学(SEE)领域正在迅速发展。这篇综述强调了仪器开发方面的重大进展,这些进展提高了SEE测量的空间和时间分辨率,以及采用人工智能方法进行数据分析,以改善复杂电化学数据集的处理、解释和准确性。此外,我们还概述了SEE在能源存储、催化、环境监测和生物传感方面的最新应用,展示了单一实体测量的关键重要性和变革潜力。通过将先进的仪器与强大的数据分析框架相结合,SEE继续在纳米尺度上揭示独特的见解,弥合基础电化学研究和实际应用。
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引用次数: 0
Sensors and biosensors: From architecture to analytes 传感器和生物传感器:从建筑到分析物
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-06-09 DOI: 10.1016/j.coelec.2025.101721
Rasa Pauliukaite
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引用次数: 0
Surface electrochemistry of low-dimensional materials 低维材料的表面电化学
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-06-02 DOI: 10.1016/j.coelec.2025.101720
Enrique Herrero, Galina Tsirlina
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引用次数: 0
Plastic waste upcycling through electrocatalysis 通过电催化对塑料垃圾进行升级回收
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-06-02 DOI: 10.1016/j.coelec.2025.101712
Yuan Ji, Chunxiao Liu, Tingting Zheng, Chuan Xia
The widespread use and chemical durability of plastics have contributed to the escalating issue of white pollution. Among various mitigation strategies, recycling waste plastics stands out as one of the most effective and sustainable solutions. Electrochemical methods, featuring mild operating conditions, tunable reaction selectivity, and low carbon emissions, have emerged as promising approaches for plastic recycling. This mini review offers a concise summary of recent advances in the electrocatalytic conversion of plastic waste. We highlight key strategies that involve the selective electrooxidation of monomers derived from plastic hydrolysis, the coupling of anodic and cathodic reactions to increase energy efficiency, and the incorporation of heteroatoms to expand the functionality of target products. We conclude by discussing emerging approaches for non-hydrolyzable plastics and the integration of electrocatalysis with complementary methods for broader applicability and scalable circular recycling.
塑料的广泛使用和化学耐久性导致了白色污染问题的不断升级。在各种缓解战略中,回收废塑料是最有效和可持续的解决方案之一。电化学方法具有操作条件温和、反应选择性可调、低碳排放等特点,是塑料回收的一种很有前途的方法。这篇迷你评论提供了塑料废物电催化转化的最新进展的简要总结。我们强调了关键策略,包括塑料水解衍生的单体的选择性电氧化,阳极和阴极反应的耦合以提高能源效率,以及杂原子的结合以扩大目标产物的功能。最后,我们讨论了非水解塑料的新兴方法,以及电催化与更广泛适用性和可扩展循环回收的互补方法的整合。
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引用次数: 0
Detection and remediation of harmful algal blooms: Opportunities for electrochemists? 有害藻华的检测和修复:电化学的机会?
IF 7.9 2区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-05-27 DOI: 10.1016/j.coelec.2025.101711
William S. Atkinson , Cleya Saju , Jake M. Yang
Larger and more frequent recurrences of harmful algal blooms (HABs) are becoming an urgent challenge globally with potentially deadly and economically devastating consequences. HAB monitoring and remediation is a multidisciplinary field which would benefit from inputs from electrochemists. Phytoplankton cells naturally contain various biomarkers such as species-specific DNAs, toxins, and chlorophyll pigments which can be strategically targeted via electrochemistry, either directly or indirectly, for sensing purposes. In this review, we discuss recent electrochemical advances that enable early HAB warning systems with the inclusion of AI to be developed as well as the separation of algae from water via electrocoagulation methods.
更大规模和更频繁的有害藻华(HABs)的复发正在成为全球面临的紧迫挑战,具有潜在的致命和经济破坏性后果。有害藻华的监测和补救是一个多学科领域,将受益于电化学的投入。浮游植物细胞天然含有各种生物标志物,如物种特异性dna、毒素和叶绿素色素,这些生物标志物可以通过电化学直接或间接地靶向,用于传感目的。在这篇综述中,我们讨论了最近的电化学进展,这些进展使包含AI的早期赤潮预警系统得以开发,以及通过电凝方法从水中分离藻类。
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引用次数: 0
期刊
Current Opinion in Electrochemistry
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