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3D-printed electrochemical cell for both detection and degradation of venlafaxine and desvenlafaxine with boron-doped diamond electrode 3d打印掺杂硼金刚石电极的文拉法辛和地文拉法辛检测和降解电化学电池
IF 6.6 3区 材料科学 Q1 ELECTROCHEMISTRY Pub Date : 2026-02-01 DOI: 10.1016/j.electacta.2026.148353
Martin Šefčík, Ghazaleh Kholafazadehastamal, Thomas Peeters, Jan Fischer, Anna Kubíčková, Clive E. Hall, Josephus G. Buijnsters, Simona Baluchová
Venlafaxine (VF) and its active metabolite desvenlafaxine (DVF) are widely prescribed antidepressants that are only partially metabolized and excreted in significant amounts, making them clinically important analytes and environmentally relevant contaminants. In this study, a free-standing boron-doped diamond (BDD) electrode is exploited in a dual role for the electrochemical detection and degradation of VF and DVF, integrated into a custom 3D-printed dual-function electrochemical cell. The nucleation (BDDNS) and growth (BDDGS) sides of the BDD plate were systematically compared under different surface terminations. Oxidized BDDNS (O-BDDNS) provided three well-resolved oxidation peaks for VF, whereas hydrogen-terminated BDDNS (H-BDDNS) yielded a single distinct peak for DVF in 0.1 M H2SO4. Differential pulse voltammetric (DPV) methods were developed with limits of detection of 0.35 µM for VF (peak 1) and 0.34 µM for DVF and wide linear ranges in the low-to-high micromolar region. By exploiting the different surface-termination preferences and multi-peak behaviour of VF, simultaneous determination of VF and DVF was achieved. The methods showed good selectivity toward common interferents and were successfully applied to spiked river water and pharmaceutical capsules using the standard addition approach, giving recoveries close to 100%. In the 3D-printed cell, BDDGS was used for electrochemical advanced oxidation, achieving ∼97% degradation of 1 mM VF and DVF in 0.1 M H2SO4 within 20 min under galvanostatic conditions, following pseudo-first-order kinetics. In situ DPV on BDDNS enabled real-time monitoring of VF decay, demonstrating an integrated detect-and-degrade platform based on BDD and additive manufacturing.
文拉法辛(VF)及其活性代谢物去文拉法辛(DVF)是广泛使用的抗抑郁药,仅部分代谢并大量排出,使其成为临床重要分析物和环境相关污染物。在这项研究中,一个独立的掺硼金刚石(BDD)电极被用于VF和DVF的电化学检测和降解的双重作用,集成到一个定制的3d打印双功能电化学电池中。系统比较了不同表面末端条件下BDD板的成核(BDDNS)面和生长(BDDGS)面。氧化BDDNS (O-BDDNS)在0.1 M H2SO4中产生了三个清晰的VF氧化峰,而端氢BDDNS (H-BDDNS)在0.1 M H2SO4中产生了一个清晰的DVF氧化峰。差分脉冲伏安法(DPV)的检测限分别为VF(峰1)0.35µM和DVF(峰1)0.34µM,在低至高微摩尔区域线性范围宽。利用VF的不同表面终止偏好和多峰行为,实现了VF和DVF的同时测定。该方法对常见干扰物具有良好的选择性,并成功地应用于加样河水和药物胶囊中,加样回收率接近100%。在3d打印电池中,BDDGS被用于电化学高级氧化,在0.1 M H2SO4中,在恒流条件下,按照准一级动力学,在20分钟内实现了1 mM VF和DVF的~ 97%降解。BDDNS上的原位DPV能够实时监测VF衰减,展示了基于BDD和增材制造的集成检测和降解平台。
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引用次数: 0
Tuning electrochemical properties of 3D-printed PLA/carbon black electrodes via diamondized nanocarbon functionalization 通过金刚石纳米碳功能化调整3d打印PLA/炭黑电极的电化学性能
IF 6.6 3区 材料科学 Q1 ELECTROCHEMISTRY Pub Date : 2026-02-01 DOI: 10.1016/j.electacta.2026.148351
Ana C.M. Oliveira, Raquel G. Rocha, Mariana C. Marra, Agata Rodak, Mateusz Cieślik, Robert D. Crapnell, Craig E. Banks, Jacek Ryl, Rodrigo A.A. Muñoz
This work investigates the influence of diamondized nanocarbon (DNC) surface charge on the performance of 3D-printed CB/PLA electrodes for paracetamol detection. Three filaments were prepared by the thermal method, incorporating DNCs with different zeta potentials, one positive (+20 mV) and two negative (-30 mV and -45 mV). Surface characterization by XPS and Raman spectroscopy revealed that DNC charge affects dispersion, polymer coverage, and the exposure of carbon black domains, whereas SEM images showed that positively charged DNCs tend to aggregate, whereas negatively charged DNCs remain well-dispersed. Contact angle measurements indicated increased hydrophilicity for electrodes containing negatively charged DNCs. Electrochemical analysis demonstrated lower charge-transfer resistance and superior current response for these electrodes, with an extended linear range and improved detection limits for paracetamol (∼1.5 times higher than positively charged DNCs). Overall, the results highlight that the DNC zeta potential is a key parameter for optimizing 3D-printed electrodes, providing a simple, low-cost strategy for the fabrication of portable and high-performance electrochemical sensors. Importantly, this is the first report demonstrating that DNC zeta potential significantly influences filament synthesis for electrochemical applications, opening new opportunities for the incorporation of various nanoparticles into filament composite.
本文研究了金刚石纳米碳(DNC)表面电荷对3d打印CB/PLA电极检测扑热息痛性能的影响。采用热法制备了三种不同zeta电位的dnc,一种为正电位(+20 mV),两种为负电位(-30 mV和-45 mV)。XPS和拉曼光谱的表面表征表明,DNC电荷影响分散性、聚合物覆盖率和炭黑域的暴露,而SEM图像显示,带正电荷的DNC倾向于聚集,而带负电荷的DNC则保持良好的分散。接触角测量表明,含有负电荷dnc的电极亲水性增加。电化学分析表明,这些电极具有较低的电荷转移电阻和优异的电流响应,具有扩展的线性范围和提高的对乙酰氨基酚的检出限(比带正电荷的dnc高1.5倍)。总体而言,研究结果强调DNC zeta电位是优化3d打印电极的关键参数,为制造便携式高性能电化学传感器提供了一种简单、低成本的策略。重要的是,这是第一份证明DNC zeta电位显著影响电化学应用的长丝合成的报告,为将各种纳米颗粒纳入长丝复合材料开辟了新的机会。
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引用次数: 0
Investigation of the Electrochemical Chlorodifluoromethylation Reactions of 2H-Indazoles and Quinoxalinones with ClCF2SO2Na 2h -茚唑和喹诺啉酮与ClCF2SO2Na电化学氯二氟甲基化反应的研究
IF 6.6 3区 材料科学 Q1 ELECTROCHEMISTRY Pub Date : 2026-02-01 DOI: 10.1016/j.electacta.2026.148356
Xin Liu, Yuhang Ding, Meichao Li, Zhenlu Shen
The synthetic routes for constructing CF2Cl-containing compounds is being developed due to their increasingly utility in drug modification and organic synthesis. Herein, we report a convenient electrochemical protocol for chlorodifluoromethylation reactions of 2H-indazoles and quinoxalinones using ClCF2SO2Na as the efficient chlorodifluoromethylating reagent via C(sp2)−H functionalization without any transition-metal catalysts and stoichiometric oxidants. Cyclic voltammetry and control experiments indicate that a radical pathway is involved during the reaction. Under this mild and operationally simple process, a variety of desired CF2Cl-substituted products were synthesized in an undivided cell, achieving isolated yields of up to 88%. Other sodium sulfinates functionalized with fluorinated groups, such as −CF2CH3, −CF2Et, −CF2Pr, −CF2COOEt and −CFH2, also emerge as suitable substrates for the developed method, highlighting its broad potential applicability. In addition, the value of the developed method is further demonstrated by gram-scale experiments and downstream transformation reactions.
由于含cf2cl化合物在药物修饰和有机合成中的应用日益广泛,其合成路线正在不断发展。在此,我们报告了一种方便的电化学方案,使用ClCF2SO2Na作为高效的氯二氟甲基化试剂,通过C(sp2)−H官能化反应进行2h -吲哚和喹诺啉酮的氯二氟甲基化反应,无需任何过渡金属催化剂和化学计量氧化剂。循环伏安法和对照实验表明,自由基途径参与了反应过程。在这种温和且操作简单的工艺下,在未分裂的细胞中合成了多种所需的cf2cl取代产物,分离收率高达88%。其他具有氟化基团功能化的亚硫酸钠,如−CF2CH3、−CF2Et、−CF2Pr、−CF2COOEt和−CFH2,也成为该方法的合适底物,突出了其广泛的潜在适用性。此外,通过克尺度实验和下游转化反应进一步证明了该方法的价值。
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引用次数: 0
How much platinum is enough? Stability of Pt-coated titanium films for porous transport layers (PTLs) in acidic and fluoride-containing electrolyte 多少铂金才够?在酸性和含氟电解质中用于多孔传输层(ptl)的pt包覆钛膜的稳定性
IF 6.6 3区 材料科学 Q1 ELECTROCHEMISTRY Pub Date : 2026-02-01 DOI: 10.1016/j.electacta.2026.148352
Gabriel C. da Silva, Xianxian Xie, Michael Vorochta, Ivan Khalakhan, Serhiy Cherevko
Platinum-coated titanium porous transport layers (PTLs) are commonly used in proton exchange membrane water electrolyzers (PEMWE) to ensure electrical contact and corrosion resistance on the anode side. While the impact of platinum on interfacial performance has been extensively studied, the effect of Pt coating thickness on dissolution stability is still not well understood. In this study, model Pt/Ti thin films with tuned Pt thicknesses ranging from 1 to 100 nm are fabricated using magnetron sputtering. The films are examined using operando scanning flow cell inductively coupled plasma mass spectrometry (SFC-ICP-MS). Our findings reveal that thin Pt coatings do not block Ti dissolution under the tested conditions, while coatings of 20 nm or thicker substantially suppress Ti dissolution under specific dynamic operating protocols. In fluoride-containing electrolytes, the most robust and consistent suppression of Ti dissolution across all investigated conditions is achieved with 100 nm Pt coating. These results highlight critical Pt thickness thresholds necessary to suppress Ti corrosion under the operating conditions investigated here and provide a mechanistic foundation for the rational design of PTL coatings prior to validation at the device level.
铂包覆钛多孔传输层(PTLs)通常用于质子交换膜水电解槽(PEMWE),以保证阳极侧的电接触和耐腐蚀性。虽然铂对界面性能的影响已被广泛研究,但铂涂层厚度对溶解稳定性的影响仍不清楚。在本研究中,采用磁控溅射技术制备了Pt/Ti模型薄膜,其厚度范围为1 ~ 100nm。薄膜使用operando扫描流式电池电感耦合等离子体质谱(SFC-ICP-MS)进行检测。我们的研究结果表明,在测试条件下,薄Pt涂层不会阻止Ti的溶解,而在特定的动态操作方案下,20nm或更厚的涂层基本上抑制了Ti的溶解。在含氟电解质中,在所有研究条件下,采用100 nm Pt涂层实现了对Ti溶解的最稳健和一致的抑制。这些结果突出了在本文研究的操作条件下抑制Ti腐蚀所需的关键Pt厚度阈值,并为在设备级验证之前合理设计PTL涂层提供了机制基础。
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引用次数: 0
Pressure and Electrolyte-Modulated Ionic Conductivity of Bubble–Electrode Junctions 气泡电极结的压力和电解质调制离子电导率
IF 6.6 3区 材料科学 Q1 ELECTROCHEMISTRY Pub Date : 2026-02-01 DOI: 10.1016/j.electacta.2026.148354
Chiara Iannace, Simone Ciampi
Electrochemical processes at gas–liquid interfaces remain largely unexplored, despite the ubiquity and functional importance of bubbles in both natural systems as well as in analytical, separation, and purification technologies. Impedance measurements of electrode–bubble junctions demonstrate that a stable nanoscale liquid film persists between a nitrogen bubble and a platinum ultramicroelectrode. This aqueous disjoining film has an unexpectedly high ionic conductivity, which further increases with increasing bubble deformation. The efficiency of ionic transport within this confined liquid pocket is ion-specific and linked to the ability of electrolyte ions, principally anions, to accumulate at the air–water interface. The presence of surface ions and mechanical stiffening of the bubble, as it deforms under the pressure of the electrode, modulate the junction’s resistance, while its capacitance is influenced by the electrostatics of overlapping anionic clouds on the bubble with the positive charge of the electrode. Electrochemiluminescence imaging data confirm sustained charge transfer across the junction, which indicate effective solution bulk-to-confined film mass transport. Our findings establish gas bubble–metal junctions as a new electrochemical platform, and help advance the understanding of bubbles as chemically active entities rather than passive insulating voids.
尽管气泡在自然系统以及分析、分离和净化技术中无处不在,而且具有重要的功能,但气液界面的电化学过程在很大程度上仍未被探索。电极-气泡结的阻抗测量表明,在氮泡和铂超微电极之间存在稳定的纳米级液膜。这种水分离膜具有出乎意料的高离子电导率,随着气泡变形的增加,离子电导率进一步增加。在这个受限的液体口袋中,离子传输的效率是离子特异性的,并且与电解质离子(主要是阴离子)在空气-水界面积聚的能力有关。当气泡在电极压力下变形时,表面离子的存在和气泡的机械硬化会调节结的电阻,而其电容则受到气泡上带有电极正电荷的阴离子云重叠的静电的影响。电化学发光成像数据证实了持续的电荷通过结转移,这表明有效的溶液体到受限膜的质量传输。我们的发现建立了气泡-金属结作为一个新的电化学平台,并有助于推进对气泡作为化学活性实体而不是被动绝缘空洞的理解。
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引用次数: 0
Polyvinyl alcohol-assisted interfacial engineering of vanadium pentoxide cathodes for high performance aqueous zinc-ion batteries 聚乙烯醇辅助高性能锌离子电池五氧化二钒阴极的界面工程
IF 6.6 3区 材料科学 Q1 ELECTROCHEMISTRY Pub Date : 2026-02-01 DOI: 10.1016/j.electacta.2026.148357
Haize Yin, Yu Gao, Sheng Lu, Miao Xu, Yongmin Wu, Dongqing Wu, Yuezeng Su, Wei An, Han Wang
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引用次数: 0
A Conductive Metal-Organic Framework-Modified Electrode for Sensitive Electrochemiluminescent Detection of Cardiac Troponin I 导电金属-有机框架修饰电极电化学发光检测心肌肌钙蛋白I
IF 6.6 3区 材料科学 Q1 ELECTROCHEMISTRY Pub Date : 2026-02-01 DOI: 10.1016/j.electacta.2026.148350
Alenzo Murray, Giovanni Valenti, Priscilla Baker
The design of a sensitive and accurate electrochemiluminescence (ECL) immunosensor for the early detection of cardiac biomarkers at low concentrations is essential to improve patient outcomes. In this study, a conductive metal-organic framework (c-MOF), Cu3(HHTP)2, was drop-coated onto a screen-printed carbon electrode (SPCE) to produce an ultra-efficient electrochemical sensing platform which was subsequently functionalized with cTnI antibodies (Ab) and bovine serum albumin (BSA) for selective detection of the cardiac Troponin I. Cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) confirmed the successful stepwise fabrication of the immunosensor. We investigated the ECL behaviour of the Cu3(HHTP)2-modified SPCE using [Ru(bpy)3]2+ as the luminophore and found that a significant increase in ECL intensity was achieved compared to that of the unmodified SPCE. This enhancement was attributed to the high conductivity, porous structure, the increased surface area of the c-MOF and crucially the HHTP ligand plays a critical role in enabling ECL generation in this system. The analytical performance of the immunosensor was evaluated by monitoring the ECL responses at varying cTnI concentrations. The immunosensor achieved a detection limit of 10.23 ± 1.06 pg/mL in vitro, well below the clinically relevant cTnI thresholds, highlighting its potential for rapid and early-stage cardiac biomarker detection. These findings suggest the Cu3(HHTP)2-based ECL immunosensor represents a viable sensing platform that significantly increases conductivity and ECL efficiency without the need of additional co-reactant species.
设计一种灵敏、准确的电化学发光(ECL)免疫传感器,用于早期检测低浓度的心脏生物标志物,对于改善患者预后至关重要。在这项研究中,将导电金属-有机框架(c-MOF) Cu3(HHTP)2滴涂在丝网印刷碳电极(SPCE)上,产生了一个超高效的电化学传感平台,随后用cTnI抗体(Ab)和牛血清白蛋白(BSA)进行功能化,用于选择性检测心脏肌钙蛋白i。循环伏安(CV)和电化学阻抗谱(EIS)证实了免疫传感器的成功制造。我们使用[Ru(bpy)3]2+作为发光团研究了Cu3(HHTP)2修饰的SPCE的ECL行为,发现与未修饰的SPCE相比,ECL强度显着增加。这种增强归因于高导电性,多孔结构,c-MOF的表面积增加,关键是HHTP配体在该体系中产生ECL方面起着关键作用。通过监测不同cTnI浓度下的ECL反应来评估免疫传感器的分析性能。该免疫传感器在体外的检测限为10.23±1.06 pg/mL,远低于临床相关的cTnI阈值,突出了其快速和早期心脏生物标志物检测的潜力。这些发现表明,基于Cu3(HHTP)2的ECL免疫传感器是一种可行的传感平台,可以显著提高电导率和ECL效率,而无需额外的共反应物。
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引用次数: 0
Towards robust comparison of distributions of relaxation times 对松弛时间分布的鲁棒性比较
IF 6.6 3区 材料科学 Q1 ELECTROCHEMISTRY Pub Date : 2026-01-31 DOI: 10.1016/j.electacta.2026.148339
Žiga Gradišar, Žan Gorenc, Vanja Subotić, Pavle Boškoski
{"title":"Towards robust comparison of distributions of relaxation times","authors":"Žiga Gradišar, Žan Gorenc, Vanja Subotić, Pavle Boškoski","doi":"10.1016/j.electacta.2026.148339","DOIUrl":"https://doi.org/10.1016/j.electacta.2026.148339","url":null,"abstract":"","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"50 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2026-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146089369","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Fully Coupled Multi-Physics Modeling and Synergistic Structural Optimization for High Uniformity 8-inch Wafer Electroplating 高均匀性8英寸硅片电镀的全耦合多物理场建模与协同结构优化
IF 6.6 3区 材料科学 Q1 ELECTROCHEMISTRY Pub Date : 2026-01-31 DOI: 10.1016/j.electacta.2026.148345
Hao Luo, Hu He
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引用次数: 0
Preparation of a Uranium Monocarbide Anode and Electrochemical Characterization in Molten LiCl-KCl-UCl3 单碳化铀阳极的制备及熔融LiCl-KCl-UCl3的电化学表征
IF 6.6 3区 材料科学 Q1 ELECTROCHEMISTRY Pub Date : 2026-01-31 DOI: 10.1016/j.electacta.2026.148346
Justin M. Holland, Darren M. Driscoll, Ethan C. Thomas, Richard L. Fitzhugh
{"title":"Preparation of a Uranium Monocarbide Anode and Electrochemical Characterization in Molten LiCl-KCl-UCl3","authors":"Justin M. Holland, Darren M. Driscoll, Ethan C. Thomas, Richard L. Fitzhugh","doi":"10.1016/j.electacta.2026.148346","DOIUrl":"https://doi.org/10.1016/j.electacta.2026.148346","url":null,"abstract":"","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"52 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2026-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146095531","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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Electrochimica Acta
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