Electrochimica Acta最新文献

{"title":"Sensitivity of lipid bilayer sensing of pore-forming toxins relies on electrical properties of nanoscale-thick submembrane reservoir separating solid support and phospholipid membrane","authors":"Inga Gabriunaite, Tomas Sabirovas, Filipas Ambrulevičius, Linas Labanauskas, Ringailė Lapinskaitė, Arturas Polita, David J. Vanderah, Gintaras Valincius, Aušra Valiūnienė","doi":"10.1016/j.electacta.2025.146189","DOIUrl":"https://doi.org/10.1016/j.electacta.2025.146189","url":null,"abstract":"The comparative study of two types of tethered bilayer membranes (tBLMs), one formed on atomically smooth gold films and the other on fluorine-doped tin oxide (FTO) films on glass is reported. These solid substrates exhibited different surface morphology and roughness. After tailoring with thiol or silane compounds, both formed intact tBLMs as demonstrated by electrochemical impedance spectroscopy (EIS). In contrast to the flat Au surfaces, the FTO substrates showed the presence of local water pockets, which caused a lower electrical resistance of the submembrane space separating the bilayers and the solid substrate.The EIS data analysis showed that the residual lateral defects, with an average radius between 10 and 20 nm, are heterogeneously distributed over the surface of the tBLMs. The concentration of defects on the surface is very low, ranging from 10 to 30 defects per 1000 μm². Both types of tBLMs responded to the pore-forming toxin, the α-hemolysin (αHL) from <em>Staphylococcus aureus</em> in a concentration dependent manner. The EIS response and the sensitivity to the toxin were stronger for tBLMs on FTO than on Au. We show that, independent of the solid substrate, the property that affects the sensitivity of tBLM sensors to membrane-damaging toxins is related to the resistance of the submembrane reservoir. The lower the resistance, the higher the sensitivity. Although we cannot exclude other factors such as membrane composition, buffer salts, and pH, we conclude that, in general, submembrane resistance is the fundamental factor determining the sensitivity of tBLM sensors.","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"133 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766690","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}

{"title":"Achieve an atomic-level understanding of the anion/concentration effect on transport properties for aqueous zinc halide electrolytes","authors":"Bochun Liang, Tairan Wang, Huan Chen, Yaqin Zhang, Xinyao Ma, Jun Fan","doi":"10.1016/j.electacta.2025.146165","DOIUrl":"https://doi.org/10.1016/j.electacta.2025.146165","url":null,"abstract":"Despite the growing research interest in aqueous zinc-ion batteries (AZIBs), the detailed atomic-level understanding of the structure-property relationship in AZIBs electrolytes remains incomplete. In this study, we employ molecular dynamics simulations to study the properties of three zinc halide salt electrolytes (ZnCl₂, ZnBr₂, and ZnI₂) at concentrations ranging from 0.44 m to 4 m. We observed the diffusion coefficients decrease as the concentration increases, and the overall diffusion coefficients follow the sequence of ZnI₂ &gt; ZnBr₂ &gt; ZnCl₂. Further study revealed that this is attributed to the different degrees of ion clustering and the resultant disruption of the water network across different systems. Furthermore, we found that ionic conductivities of all three salts increase first and then decrease beyond an inflection point as the concentration rises, which is closely associated with the proportion of Zn²⁺ in solvent-separated ion pairs. This work aims to deepen the understanding of aqueous zinc salt electrolytes and inform the design of high-performance AZIBs.","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"58 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766688","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}

{"title":"Co-deposition of Co, Ni, and Ru from the choline chloride-ethylene glycol deep eutectic solvent","authors":"Renata Palowska, Marcin Kozieł, Agnieszka Brzózka, Grzegorz D. Sulka","doi":"10.1016/j.electacta.2025.146179","DOIUrl":"https://doi.org/10.1016/j.electacta.2025.146179","url":null,"abstract":"In this research, we explore the co-deposition of Co, Ni, and Ru from ethaline – a mixture of choline chloride and ethylene glycol in a 1:2 molar ratio. Co, Ni, and Ru were co-deposited from ethaline-based solutions containing their respective chloride salts, with LiCl and H₂SO₄ added in some cases. Deposition was carried out at constant potentials ranging from -1.00 V to -1.34 V, at 70°C, for up to 4 h. The morphology of the resulting deposits was examined using scanning electron microscopy, while their composition was analyzed by energy-dispersive X-ray spectroscopy and X-ray diffraction. The obtained Co-Ni deposit morphologies ranged from mostly smooth, dense layers to platelets and dendritic formations, influenced by the presence of H₂SO₄ and LiCl in the solution. In contrast, the addition of Ru resulted in a more porous, netlike deposit. Composition analyses confirmed the presence of all three target elements but showed a significant reduction in Co content in deposits obtained from multi-component baths. Selected Co-Ni-Ru deposits were tested as hydrogen evolution catalysts in 1.0 M KOH and 0.5 M H₂SO₄, where they showed good activity.","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"73 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766689","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}

{"title":"Understanding the effect of particle size and size standard deviation on lithium-ion concentration and discharge behavior of heterogeneous electrode","authors":"Junpei Wang, Shaohai Dong, Yuhang Lyu, Zhan-Sheng Guo","doi":"10.1016/j.electacta.2025.146176","DOIUrl":"https://doi.org/10.1016/j.electacta.2025.146176","url":null,"abstract":"With the growing demand for electric vehicles and renewable energy storage, enhancing battery energy density has become a focal point of current research. Increasing electrode thickness is an effective strategy, but it is accompanied by the complexification of the microstructure, leading to reduced lithium-ion transport efficiency. In particular, the particle size and size standard deviation of active materials significantly influence the electrode microstructure. This study developed a new MATLAB algorithm to construct a heterogeneous particle packing cell model, using particle radius and size standard deviation as key parameters. The effects of particle size and size spatial distribution on battery performance were investigated by analyzing the Li-ion concentration distribution and the depth of discharge. The results showed that the short diffusion paths of small particles facilitated more effective lithiation. Random mixing of large and small particles significantly enhanced lithium-ion transport compared to large particles alone. Furthermore, the standard deviation of particle size had a notable impact on battery performance, and electrodes with different particle radii exhibited different sensitivities to this standard deviation. An optimal particle size standard deviation was identified that could enhance lithium-ion diffusion and improve rate performance. Additionally, the spatial distribution of particle sizes along the electrode thickness also affected lithium-ion transport behavior. The lithium-ion transport results under these different particle distributions provide valuable insights for the design of electrode microstructures, potentially advancing battery technology.","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"21 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758038","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}

{"title":"A square filter-press alkaline water electrolyzer for wide power range operation via flow enhancement and parasitic current suppression","authors":"Si-Tong Liu, Run-Xia He, Zhen-Guo Guo, Bing Li, Fang Li, Jun Ding, Jian-Bo He","doi":"10.1016/j.electacta.2025.146186","DOIUrl":"https://doi.org/10.1016/j.electacta.2025.146186","url":null,"abstract":"Hydrogen production via direct water electrolysis under conditions of large power fluctuations presents a major challenge in renewable energy storage applications. This study introduces a novel square filter-press alkaline water electrolyzer featuring independent gas outlet manifolds, specifically developed to ensure efficient hydrogen production across a wide range of power fluctuation conditions. Compared with conventional circular electrolyzer designs, the modified configuration demonstrated enhanced gas purity and Faradaic efficiency even at low current densities (as low as 10 mA cm^-2). Additionally, the new design achieved reduced electrolysis voltages, especially at higher current densities. These performance improvements are attributed to optimized manifold structures that enable efficient gas evacuation, thereby minimizing inefficiencies caused by gas bubble entrapment. The study also identifies and analyzes two types of parasitic currents, LPPC and SPPC, to better understand and mitigate their impact on both gas purity and electrolysis efficiency. These innovations significantly expand the operational power range of electrolyzer systems, enhancing their compatibility with renewable energy sources' inherent power fluctuations while improving overall efficiency and operational safety.","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"235 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758043","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}

{"title":"Synergetic Electrochemical Degradation of Amoxicillin (AMX) with Sustainable Transition Metal Oxides-Anode and Waste-derived Carbon-Cathode System from a Circular Economy Approach","authors":"Jorge Adrián Castro-Fernández, Álvaro Ramírez, Martín Muñoz-Morales, Erika Bustos, Javier Llanos","doi":"10.1016/j.electacta.2025.146181","DOIUrl":"https://doi.org/10.1016/j.electacta.2025.146181","url":null,"abstract":"This work explores a novel electrochemical approach for the efficient degradation of amoxicillin (AMX), a widely used antibiotic and emerging water pollutant. This is the first time reported a system combines an IrO₂-Ta₂O₅|Ti anode with cathodes modified using activated carbon derived from two types of waste biomass: <em>Phragmites australis</em> (PA) and <em>Spergularia rubra</em> (SR), having in mind the circular economy. This study evaluated the influence of aeration and current density on AMX degradation efficiency. Results showed that the carbon-modified cathodes enhanced the production of hydrogen peroxide (H₂O₂) via the two-electron oxygen reduction reaction, which facilitated the generation of reactive hydroxyl radicals (^•OH), which improve significantly the degradation rate of AMX. Under optimal conditions (aeration and 2.54 mA cm^-2 current density), the system achieved complete AMX degradation within 30 minutes, with substantial reductions in energy consumption (0.1096 and 0.0895 kWh m^-3 order^-1 for PA and SR, respectively, when applying 2.54 mA cm^-2) compared to conventional platinum cathodes (4.9844 kWh m^-3 order^-1 for Pt). Acute toxicity assays conducted with <em>Vibrio fischeri</em> demonstrated a significant reduction in the toxicity (measured as inhibition percentage), with values of 8.49% and 8.79%, respectively (<em>vs</em> 21.88 % of initial sample). These findings highlight the potential of integrating waste-derived carbon materials with transition metal oxide anodes for sustainable water treatment processes, offering a promising alternative to traditional electrochemical systems for the degradation of pharmaceutical contaminants supporting the sustainable development goal number six (SDG 6) focus on clean water and sanitation.","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"38 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758039","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}

{"title":"Assessment of Interface Passivation in AgBiS2 Q-dot Sensitized Solar Cell on the carrier transport and recombination","authors":"Dimuthumal Rajakaruna, Hong-yi Tan, Chang-Feng Yan, Jayasundera Bandara","doi":"10.1016/j.electacta.2025.146173","DOIUrl":"https://doi.org/10.1016/j.electacta.2025.146173","url":null,"abstract":"Silver bismuth sulfide has been discovered to be an appropriate light-harvesting material but the carrier transport restrictions and trap-assisted recombination in Q-dot AgBiS₂ limit the device efficiency. To address inherent charge carrier transport restrictions and trap-assisted recombination in q-dot AgBiS₂, this work studied the effect of interface passivation of AgBiS₂ Q-dot by a thin-nanostructured ZnS layer on carrier transport and recombination.The charge-transfer and carrier recombination processes investigated by open-circuit voltage decay curves and <strong>e</strong>lectrochemical impedance spectroscopy indicate the decrease in inherent trap-assisted Shockley-Read-Hall (SRH) recombination in bare AgBiS₂ due to the passivation of AgBiS₂ by ZnS while an increase in the charge recombination resistance and improvement in carrier lifetime resulting in enhanced solar cell performance. A very thin ZnS passivation layer on AgBiS₂ also boosts the light absorption, resulting in a red shift in the light absorption peak. The formation of AgBiS₂ and ZnS was confirmed by XRD, EDS, and TEM analysis and the explicit role of the ZnS passivation layer on the electron transport layer and the light harvesting AgBiS₂ Q-dots was investigated. Using a polysulfide electrolyte and optimal ZnS layers on TiO₂ and AgBiS₂ nanostructures in the FTO/m-TiO₂/ZnS(1)/AgBiS₂/ZnS(2) electrode design enhanced the efficiency and the passivation can also be implemented for a solid-hole transport material.","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"73 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758044","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}

{"title":"Switching between Boosting and Suppression of Sensitivity and Selectivity of Inkjet-Printed Graphene Electrodes for Biomolecule Detection","authors":"Fabian Weyand, Stefano Gianvittorio, Filippo Longo, Jing Wang, Andreas Lesch","doi":"10.1016/j.electacta.2025.146174","DOIUrl":"https://doi.org/10.1016/j.electacta.2025.146174","url":null,"abstract":"Sensitivity and selectivity are key parameters for electrochemical sensors, typically dictated by the properties of the sensing electrode's surface. Here, we demonstrate for the first time that the enhancement of both parameters for detecting surface-sensitive analytes can be repeatedly switched \"on\" and \"off\" on-demand by applying defined rapid and simple heating protocols to inkjet-printed graphene electrodes. Electroactive benchmark probes, which provide different interaction mechanisms with graphene surfaces are applied to characterize both electrodes. The voltammetric detection of uric acid (UA) with switched-on electrodes culminates in a more than 60-fold lower detection limit (0.39 µM) and 60-fold higher sensitivity (34.4 mA cm^-2 m<span>m</span>^-1) compared to the one switched-off, offering optimal sensing characteristics at low concentrations. Excellent selectivity is demonstrated for multi-component mixtures of UA, ascorbic acid (AA), dopamine (DA) and xanthine (XA). In contrast, switched-off electrodes provide reproducible signals and a wide linear range at high concentrations, complementing the switched-on electrodes for applications where high concentrations are of interest. Spectroscopy and scanning probe microscopy techniques are applied to correlate the reversible surface modifications with the observed differences in the electrochemical performances. Finally, as practical advantage of the enhancement effect, the detection of electrochemically redox markers for viable bacterial cells is presented. The reproducible large-scale production of disposable graphene electrodes, coupled with the ability to modulate quickly and simply the electrochemical performance on request offers great opportunities for a broad range of electrochemical applications.","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"37 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758042","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}

{"title":"Indirect determination of trace concentrations of amoxicillin in environmental samples using a low-cost, disposable additively manufactured sensor","authors":"Anastácio A. Boane, Raquel G. Rocha, Rodrigo A.A. Muñoz, André L. dos Santos, Eduardo M. Richter","doi":"10.1016/j.electacta.2025.146175","DOIUrl":"https://doi.org/10.1016/j.electacta.2025.146175","url":null,"abstract":"Amoxicillin (AMX) is the most consumed antibiotic from the β-lactam group due to its effectiveness against a broad spectrum of bacterial infections. Given the widespread application of AMX, there is a significant risk of environmental damage and global repercussions due to the hazardous nature of effluents generated by the pharmaceutical industry. Herein, we developed a simple, rapid, cost-effective, and sensitive procedure for the indirect electrochemical determination of AMX in water samples. The method utilizes differential pulse voltammetry (DPV) combined with a low-cost disposable working electrode fabricated through additive manufacturing (3D printing). Three sequential steps are proposed to enhance the detectability of AMX using the 3D-printed electrode: (i) chemical and electrochemical activation of the 3D-printed electrode surface in an alkaline medium (0.5 mol L⁻¹ NaOH); (ii) preconcentration of AMX through its adsorption onto the electrode surface; and (iii) oxidation of adsorbed AMX to its quinone-derived form, followed by its sensitive detection via electrochemical reduction and subsequent reoxidation. The mechanism of the electrochemical reactions was investigated and discussed using electrochemical techniques and supported by literature data. Under optimized DPV conditions, the activated 3D-printed electrode demonstrated excellent analytical performance, exhibiting a linear range from 0.1 to 5.0 µmol L⁻¹ and a limit of detection (LOD) of 0.01 µmol L⁻¹ (10 nmol L⁻¹). The possibility of using various detection strategies (AMX direct oxidation, reduction of AMX's oxidation product, and its re-oxidation) enhanced the selectivity of the voltammetric method, with no significant interference from multiple potential interferents (Pb²⁺, phenol, glucose, ascorbic acid, uric acid, ibuprofen, clavulanate, paracetamol, chloramphenicol, sulfanilamide, tetracycline, and ciprofloxacin). Using a simple sample preparation procedure (addition of or dilution in a supporting electrolyte), recovery values ranging from 82 to 106% for AMX in various water samples (river, lake, tap, and drinking water) were achieved.","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"62 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758040","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}

{"title":"Deciphering the role of alloying elements in spontaneous passivation by element-resolved electrochemistry: From pure metals to equiatomic CoCrFeNi","authors":"Chenyang Xie, Junsoo Han, Fan Sun, Kevin Ogle","doi":"10.1016/j.electacta.2025.146177","DOIUrl":"https://doi.org/10.1016/j.electacta.2025.146177","url":null,"abstract":"The influence of alloying elements Co, Fe, Ni on the spontaneous passivation behavior of Cr−containing alloys (Cr = 25 at%) in 0.1 M H₂SO₄ was investigated using element-resolved electrochemistry. A bottom-up strategy was used from pure metals to quaternary alloys. The dissolution - polarization curves of pure metals showed strong correlation with that of alloys containing the corresponding elements. For most alloys, the dissolution curve closely aligns with that of the pure metal with the lowest dissolution rate at a given potential. For CoCrFeNi, Ni limits dissolution in the cathodic domain and the critical dissolution rate is determined by the overlap of Ni and Cr dissolution curves.","PeriodicalId":305,"journal":{"name":"Electrochimica Acta","volume":"58 1","pages":""},"PeriodicalIF":6.6,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758045","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}