Pub Date : 2024-07-02DOI: 10.1149/1945-7111/ad5d9c
M. Vesali-Naseh, Zahra Rastian, Hossein Moshakker
In this systematic review, all electrochemical glucose biosensors based on carbon nanotube (CNT) composites from 2001 to 2021 (n=6807) have been reviewed. After excluding duplicates, irrelevant, and unqualified papers, 184 articles were selected for data extraction. The operating data include working electrode, test solution, detection potential, sensitivity, detection limit, linear range, response time, selectivity, enzyme coverage, Michaelis–Menten constants, and ambient condition (i.e. pH, temperature and humidity). In addition, the in vivo and in vitro media (including invasive and non-invasive detection) and the most repeated interferences have been specified. All of the CNTs-based hybrids for modifying working electrodes have been classified regarding the various components such as metallic species (elemental, oxide, alloy and complex), polymers and different electroactive species. The enzymeless and enzymatic biosensors as well as dual-enzyme electrodes using GOx, GDH, and HRP have also been categorized. Moreover, the different natural and artificial mediators and fixing agents, were determined.
{"title":"Review—Carbon Nanotube-Based Electrochemical Glucose Biosensors","authors":"M. Vesali-Naseh, Zahra Rastian, Hossein Moshakker","doi":"10.1149/1945-7111/ad5d9c","DOIUrl":"https://doi.org/10.1149/1945-7111/ad5d9c","url":null,"abstract":"\u0000 In this systematic review, all electrochemical glucose biosensors based on carbon nanotube (CNT) composites from 2001 to 2021 (n=6807) have been reviewed. After excluding duplicates, irrelevant, and unqualified papers, 184 articles were selected for data extraction. The operating data include working electrode, test solution, detection potential, sensitivity, detection limit, linear range, response time, selectivity, enzyme coverage, Michaelis–Menten constants, and ambient condition (i.e. pH, temperature and humidity). In addition, the in vivo and in vitro media (including invasive and non-invasive detection) and the most repeated interferences have been specified. All of the CNTs-based hybrids for modifying working electrodes have been classified regarding the various components such as metallic species (elemental, oxide, alloy and complex), polymers and different electroactive species. The enzymeless and enzymatic biosensors as well as dual-enzyme electrodes using GOx, GDH, and HRP have also been categorized. Moreover, the different natural and artificial mediators and fixing agents, were determined.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141685018","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-02DOI: 10.1149/1945-7111/ad5e01
F. Sedeqi, S. Santhanam, Matthias Riegraf, Marc Riedel, M. Heddrich, S. Ansar
The ability of high-temperature solid oxide cell (SOC) electrochemical reactors to efficiently convert atmospheric carbon to high value chemicals for industrial and energy storage applications via CO2 and co-electrolysis makes them a key technology for active carbon utilisation. However, due to additional operational risks from thermochemical reactions on thermal management, limited experimental capacity, and relative novelty, CO2 and co-electrolysis lag behind steam electrolysis in large-scale adoption. Here, a 1D+1D SOC model based on fundamental first principles considering three-dimensional heat transfer was improved via a unique method for representing co-electrolysis electrochemistry, solving with low computational effort. Validation against experimental data for two compositions and pressures, showed high levels of accuracy with respect to characteristic cell voltages, temperatures, and outlet compositions. The model also showed CO2 reduction during co-electrolysis mainly occurred via reverse water gas shift, while CO2 electrolysis still accounted for up to 35% of the total share. Pressurised co-electrolysis operation promotes exothermic methanation, causing pronounced heating of the reactor, consequently reducing the isothermal current density. Therefore, low to moderate pressurisation is likely most suited for coupling with downstream synthesis processes to avoid the installation of unnecessarily large systems and associated high costs.
{"title":"Solid Oxide Cell Reactor Model for Transient and Stationary Electrochemical H2O and CO2 Conversion Process Studies","authors":"F. Sedeqi, S. Santhanam, Matthias Riegraf, Marc Riedel, M. Heddrich, S. Ansar","doi":"10.1149/1945-7111/ad5e01","DOIUrl":"https://doi.org/10.1149/1945-7111/ad5e01","url":null,"abstract":"\u0000 The ability of high-temperature solid oxide cell (SOC) electrochemical reactors to efficiently convert atmospheric carbon to high value chemicals for industrial and energy storage applications via CO2 and co-electrolysis makes them a key technology for active carbon utilisation. However, due to additional operational risks from thermochemical reactions on thermal management, limited experimental capacity, and relative novelty, CO2 and co-electrolysis lag behind steam electrolysis in large-scale adoption. Here, a 1D+1D SOC model based on fundamental first principles considering three-dimensional heat transfer was improved via a unique method for representing co-electrolysis electrochemistry, solving with low computational effort. Validation against experimental data for two compositions and pressures, showed high levels of accuracy with respect to characteristic cell voltages, temperatures, and outlet compositions. The model also showed CO2 reduction during co-electrolysis mainly occurred via reverse water gas shift, while CO2 electrolysis still accounted for up to 35% of the total share. Pressurised co-electrolysis operation promotes exothermic methanation, causing pronounced heating of the reactor, consequently reducing the isothermal current density. Therefore, low to moderate pressurisation is likely most suited for coupling with downstream synthesis processes to avoid the installation of unnecessarily large systems and associated high costs.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141685140","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-01DOI: 10.1149/1945-7111/ad5ef8
T. Waldmann, C. Hogrefe, Marius Flügel, Ivana Pivarníková, C. Weisenberger, Estefane Delz, Marius Bolsinger, Lioba Boveleth, Neelima Paul, M. Kasper, Max Feinauer, Robin Schäfer, Katharina Bischof, Timo Danner, Volker Knoblauch, Peter Müller‐Buschbaum, R. Gilles, A. Latz, M. Hölzle, M. Wohlfahrt‐Mehrens
Lithium deposition on anode surfaces can lead to fast capacity degradation and decreased safety properties of Li-ion cells. To avoid the critical aging mechanism of lithium deposition, its detection is essential. We present workflows for the efficient detection of Li deposition on electrode and cell level. The workflows are based on a variety of complementary advanced physico-chemical methods which were validated against each other for both graphite and graphite/Si electrodes: Electrochemical analysis, scanning electron microscopy, glow discharge-optical emission spectroscopy and neutron depth profiling, ex situ optical microscopy, in situ optical microscopy of cross-sectioned full cells, measurements in 3-electrode full cells, as well as 3D microstructurally resolved simulations. General considerations for workflows for analysis of battery cells and materials are discussed. The efficiency can be increased by parallel or serial execution of methods, stop criteria, and design of experiments planning. An important point in case of investigation of Li depositions are rest times during which Li can re-intercalate into the anode or react with electrolyte. Three workflows are presented to solve the questions on the occurrence of lithium deposition in an aged cell, the positions of lithium deposition in a cell, and operating conditions which avoid lithium depositions in a cell.
{"title":"Efficient Workflows for Detecting Li Depositions in Lithium-Ion Batteries","authors":"T. Waldmann, C. Hogrefe, Marius Flügel, Ivana Pivarníková, C. Weisenberger, Estefane Delz, Marius Bolsinger, Lioba Boveleth, Neelima Paul, M. Kasper, Max Feinauer, Robin Schäfer, Katharina Bischof, Timo Danner, Volker Knoblauch, Peter Müller‐Buschbaum, R. Gilles, A. Latz, M. Hölzle, M. Wohlfahrt‐Mehrens","doi":"10.1149/1945-7111/ad5ef8","DOIUrl":"https://doi.org/10.1149/1945-7111/ad5ef8","url":null,"abstract":"Lithium deposition on anode surfaces can lead to fast capacity degradation and decreased safety properties of Li-ion cells. To avoid the critical aging mechanism of lithium deposition, its detection is essential. We present workflows for the efficient detection of Li deposition on electrode and cell level. The workflows are based on a variety of complementary advanced physico-chemical methods which were validated against each other for both graphite and graphite/Si electrodes: Electrochemical analysis, scanning electron microscopy, glow discharge-optical emission spectroscopy and neutron depth profiling, ex situ optical microscopy, in situ optical microscopy of cross-sectioned full cells, measurements in 3-electrode full cells, as well as 3D microstructurally resolved simulations. General considerations for workflows for analysis of battery cells and materials are discussed. The efficiency can be increased by parallel or serial execution of methods, stop criteria, and design of experiments planning. An important point in case of investigation of Li depositions are rest times during which Li can re-intercalate into the anode or react with electrolyte. Three workflows are presented to solve the questions on the occurrence of lithium deposition in an aged cell, the positions of lithium deposition in a cell, and operating conditions which avoid lithium depositions in a cell.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141705199","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-07-01DOI: 10.1149/1945-7111/ad5d68
Bertrand J. Neyhouse, F. Brushett
The complex interplay between numerous parasitic processes—voltage losses, crossover, decay—challenges interpretation of cycling characteristics in redox flow batteries (RFBs). Mathematical models offer a means to predict cell performance prior to testing and to interpret experimentally measured cycling data, however most implementations require extensive domain expertise, programming knowledge, and/or computational resources. Here, we expand on our previously developed zero-dimensional modeling framework by deriving closed-form expressions for key performance metrics. The resulting closed-form model streamlines the computational structure and allows for spreadsheet modeling of cell cycling behavior, which we highlight by developing a simulation package in Microsoft® Excel®. We then apply this model to analyze previously published experimental data from our group and others, highlighting its utility in numerous diagnostic configurations—bulk electrolysis, compositionally unbalanced symmetric cell cycling, and full cell cycling. Given the accessibility of this modeling toolkit, it has potential to be a widely deployable tool for RFB research and education, aiding in data interpretation and performance prediction.
{"title":"A Spreadsheet-Based Redox Flow Battery Cell Cycling Model Enabled by Closed-Form Approximations","authors":"Bertrand J. Neyhouse, F. Brushett","doi":"10.1149/1945-7111/ad5d68","DOIUrl":"https://doi.org/10.1149/1945-7111/ad5d68","url":null,"abstract":"\u0000 The complex interplay between numerous parasitic processes—voltage losses, crossover, decay—challenges interpretation of cycling characteristics in redox flow batteries (RFBs). Mathematical models offer a means to predict cell performance prior to testing and to interpret experimentally measured cycling data, however most implementations require extensive domain expertise, programming knowledge, and/or computational resources. Here, we expand on our previously developed zero-dimensional modeling framework by deriving closed-form expressions for key performance metrics. The resulting closed-form model streamlines the computational structure and allows for spreadsheet modeling of cell cycling behavior, which we highlight by developing a simulation package in Microsoft® Excel®. We then apply this model to analyze previously published experimental data from our group and others, highlighting its utility in numerous diagnostic configurations—bulk electrolysis, compositionally unbalanced symmetric cell cycling, and full cell cycling. Given the accessibility of this modeling toolkit, it has potential to be a widely deployable tool for RFB research and education, aiding in data interpretation and performance prediction.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141692204","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
This work describes the elaboration and the electroanalytical tests of a new electrode based on a mixture of graphite and biopolymer-modified montmorillonite nanocomposite. Initially, the nanocomposite was synthesized using sodic montmorillonite (NaMT) and sodium alginate (Naalg) extracted from Tunisian algae. The resulting nanocomposite was characterized by X-ray diffraction (XRD), infrared spectroscopy (UATR), and differential scanning calorimetry (DSC). XRD analysis revealed an increase in the basal spacing d001 and the appearance of reflections (020) and (220) of guluronan groups. Infrared spectra showed characteristic polymer bands such as symmetric and antisymmetric stretching vibrations of the carboxylic group in the nanocomposite spectra indicating the modification. Thermal analysis displayed a shift in the temperature of Naalg decomposition to a higher temperature in the nanocomposite thermogram. The obtained nanocomposite was then used in the development of an electrode. The resulting hybrid electrode was tested for metronidazole (MTZ) analysis using cyclic voltammetry (CV) and square wave voltammetry (SWV). Various parameters including pH, scan rate, MTZ concentration, frequency, etc., were investigated. The results revealed the irreversibility of the studied molecule and indicated that the reduction mechanism involves both diffusion and adsorption behaviors. SWV showed a better sensitivity to detect MTZ than the CV technique. Promising results were obtained, suggesting prospects for this new hybrid electrode.
{"title":"Cyclic and Square Wave Voltammetry Analysis of MTZ Using Reactive Electrode Based on Montmorillonite and Na-Alginate","authors":"MounaTouati Hadjyoussef, Abir Dakhli, Memia Benna Zayani","doi":"10.1149/1945-7111/ad603a","DOIUrl":"https://doi.org/10.1149/1945-7111/ad603a","url":null,"abstract":"This work describes the elaboration and the electroanalytical tests of a new electrode based on a mixture of graphite and biopolymer-modified montmorillonite nanocomposite. Initially, the nanocomposite was synthesized using sodic montmorillonite (NaMT) and sodium alginate (Naalg) extracted from Tunisian algae. The resulting nanocomposite was characterized by X-ray diffraction (XRD), infrared spectroscopy (UATR), and differential scanning calorimetry (DSC). XRD analysis revealed an increase in the basal spacing d001 and the appearance of reflections (020) and (220) of guluronan groups. Infrared spectra showed characteristic polymer bands such as symmetric and antisymmetric stretching vibrations of the carboxylic group in the nanocomposite spectra indicating the modification. Thermal analysis displayed a shift in the temperature of Naalg decomposition to a higher temperature in the nanocomposite thermogram.\u0000 The obtained nanocomposite was then used in the development of an electrode. The resulting hybrid electrode was tested for metronidazole (MTZ) analysis using cyclic voltammetry (CV) and square wave voltammetry (SWV). Various parameters including pH, scan rate, MTZ concentration, frequency, etc., were investigated. The results revealed the irreversibility of the studied molecule and indicated that the reduction mechanism involves both diffusion and adsorption behaviors. SWV showed a better sensitivity to detect MTZ than the CV technique. Promising results were obtained, suggesting prospects for this new hybrid electrode.\u0000 \u0000 \u0000 \u0000","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141716207","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
A stable and highly visible-light responsive semiconductor material of AgCuO/Cu2O was prepared to develop a colorimetric and photoelectrochemical (PEC) dual-sensing mode for broad-range Hg2+ detection. The AgCuO/Cu2O was evidenced with Hg2+-enhanced peroxidase activity. In the solution, the appearance of Hg2+ promotes AgCuO/Cu2O to catalyze more 3, 3′, 5, 5′-tetramethylbenzidine (TMB) oxidization, deepening the color of the TMB solution and increasing the light absorption, thus realizing the colorimetric detection of Hg2+. The linear response range is 1 nmol·L-1 to 10 μmol·L-1, and the detection limit is 3.5 nmol·L-1. On the electrode surface, the emergence of Hg2+ facilitates AgCuO/Cu2O to convert more 4-chloro-1-naphthol (4-CN) into insoluble precipitates benzo-4-chlorohexadienone (4-CD), depressing the PEC signal and realizing the PEC detection of Hg2+ with a linear response range of 10 pmol·L-1 to 10 μmol·L-1 and a detection limit of 8.7 pmol·L-1. The enhancement of the enzyme-mimicking activity of AgCuO/Cu2O by Hg2+ is closely related to the in-situ formation of the Ag-Hg amalgam. The colorimetric and the PEC sensing modal complement each other, significantly broadening the detection range of Hg2+ and ensuring the reliability and accuracy of the results. The work paves the way for sensitive, selective, and accurate determination of Hg2+ in serum samples.
{"title":"AgCuO/Cu2O Nanozyme-Based Colorimetric and Photoelectrochemical Dual-Models Strategy for Sensing Hg2+ in Serum","authors":"Xinxin Gu, Tao Cheng, Tairu Yin, Xiaoyu Guo, Xinling Liu, Ying Wen, Haifeng Yang, Yiping Wu","doi":"10.1149/1945-7111/ad586d","DOIUrl":"https://doi.org/10.1149/1945-7111/ad586d","url":null,"abstract":"\u0000 A stable and highly visible-light responsive semiconductor material of AgCuO/Cu2O was prepared to develop a colorimetric and photoelectrochemical (PEC) dual-sensing mode for broad-range Hg2+ detection. The AgCuO/Cu2O was evidenced with Hg2+-enhanced peroxidase activity. In the solution, the appearance of Hg2+ promotes AgCuO/Cu2O to catalyze more 3, 3′, 5, 5′-tetramethylbenzidine (TMB) oxidization, deepening the color of the TMB solution and increasing the light absorption, thus realizing the colorimetric detection of Hg2+. The linear response range is 1 nmol·L-1 to 10 μmol·L-1, and the detection limit is 3.5 nmol·L-1. On the electrode surface, the emergence of Hg2+ facilitates AgCuO/Cu2O to convert more 4-chloro-1-naphthol (4-CN) into insoluble precipitates benzo-4-chlorohexadienone (4-CD), depressing the PEC signal and realizing the PEC detection of Hg2+ with a linear response range of 10 pmol·L-1 to 10 μmol·L-1 and a detection limit of 8.7 pmol·L-1. The enhancement of the enzyme-mimicking activity of AgCuO/Cu2O by Hg2+ is closely related to the in-situ formation of the Ag-Hg amalgam. The colorimetric and the PEC sensing modal complement each other, significantly broadening the detection range of Hg2+ and ensuring the reliability and accuracy of the results. The work paves the way for sensitive, selective, and accurate determination of Hg2+ in serum samples.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141344711","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-14DOI: 10.1149/1945-7111/ad586f
M.S. Raziyan, A. Palevičius, G. Janusas
Given the multitude of global health concerns, it is crucial to promptly and precisely identify biomarkers like alpha-fetoprotein (AFP) in order to facilitate the early identification and treatment of diverse illnesses, with a special emphasis on cancer. Conventional detection techniques often exhibit limitations in terms of intricacy, temporal requirements, and ease of use, underscoring the pressing want for inventive resolutions. The use of electrochemical biosensors has shown great potential in the field of AFP detection, because they provide efficient, highly responsive, and economically viable detection capabilities. This study examines current advancements in electrochemical biosensors specifically designed for the detection of alpha-fetoprotein (AFP), with a focus on the incorporation of state-of-the-art materials, sophisticated manufacturing methods, and novel biorecognition approaches. This study seeks to meet the urgent need for dependable and easily available diagnostic tools in the worldwide battle against cancer and other illnesses by offering a thorough examination of the current advancements in electrochemical biosensors. By making progress in AFP detection technologies, our goal is to have a positive impact on healthcare outcomes, improve illness management, and eventually reduce the global burden of disease.
{"title":"Review—Electrochemical Biosensors for Alpha-Fetoprotein Detection: Recent Advances and Future Perspectives","authors":"M.S. Raziyan, A. Palevičius, G. Janusas","doi":"10.1149/1945-7111/ad586f","DOIUrl":"https://doi.org/10.1149/1945-7111/ad586f","url":null,"abstract":"\u0000 Given the multitude of global health concerns, it is crucial to promptly and precisely identify biomarkers like alpha-fetoprotein (AFP) in order to facilitate the early identification and treatment of diverse illnesses, with a special emphasis on cancer. Conventional detection techniques often exhibit limitations in terms of intricacy, temporal requirements, and ease of use, underscoring the pressing want for inventive resolutions. The use of electrochemical biosensors has shown great potential in the field of AFP detection, because they provide efficient, highly responsive, and economically viable detection capabilities. This study examines current advancements in electrochemical biosensors specifically designed for the detection of alpha-fetoprotein (AFP), with a focus on the incorporation of state-of-the-art materials, sophisticated manufacturing methods, and novel biorecognition approaches. This study seeks to meet the urgent need for dependable and easily available diagnostic tools in the worldwide battle against cancer and other illnesses by offering a thorough examination of the current advancements in electrochemical biosensors. By making progress in AFP detection technologies, our goal is to have a positive impact on healthcare outcomes, improve illness management, and eventually reduce the global burden of disease.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141338536","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-14DOI: 10.1149/1945-7111/ad586c
Meenesh R. Singh, Priyanka G Singh, V. V. Gande, Rohit Chauhan, Nitin Minocha
Nernst-Einstein equation can provide a reasonable estimate of the ionic conductivity of dilute solutions. For concentrated solutions, alternate methods such as Green-Kubo relations and Einstein relations are more suitable to account for ion-ion interactions. Such computations can be expensive for multicomponent systems. Simplified mathematical expressions like the Nernst-Einstein equation do not exist for concentrated multicomponent mixtures. Newman's treatment of multicomponent concentrated solutions yields a conductivity relation in terms of species concentration and Onsager phenomenological coefficients. However, the estimation of these phenomenological coefficients is not straightforward. Here, mathematical formulations that relate the phenomenological coefficients with the friction coefficients are developed, leading to simplified, ready-to-use expressions of conductivity and transference numbers that can be used for a wide range of ionic mixtures. This approach involves spectral decomposition of the matrix of Onsager phenomenological coefficients. The general analytical expressions for conductivity and transference number are simplified for binary electrolytes, and numerical solutions are provided for ternary and quaternary mixtures with ion dissociation.
{"title":"Simplified Universal Equations for Ionic Conductivity and Transference Number","authors":"Meenesh R. Singh, Priyanka G Singh, V. V. Gande, Rohit Chauhan, Nitin Minocha","doi":"10.1149/1945-7111/ad586c","DOIUrl":"https://doi.org/10.1149/1945-7111/ad586c","url":null,"abstract":"\u0000 Nernst-Einstein equation can provide a reasonable estimate of the ionic conductivity of dilute solutions. For concentrated solutions, alternate methods such as Green-Kubo relations and Einstein relations are more suitable to account for ion-ion interactions. Such computations can be expensive for multicomponent systems. Simplified mathematical expressions like the Nernst-Einstein equation do not exist for concentrated multicomponent mixtures. Newman's treatment of multicomponent concentrated solutions yields a conductivity relation in terms of species concentration and Onsager phenomenological coefficients. However, the estimation of these phenomenological coefficients is not straightforward. Here, mathematical formulations that relate the phenomenological coefficients with the friction coefficients are developed, leading to simplified, ready-to-use expressions of conductivity and transference numbers that can be used for a wide range of ionic mixtures. This approach involves spectral decomposition of the matrix of Onsager phenomenological coefficients. The general analytical expressions for conductivity and transference number are simplified for binary electrolytes, and numerical solutions are provided for ternary and quaternary mixtures with ion dissociation.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141338316","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-14DOI: 10.1149/1945-7111/ad5872
Suanto Syahputra, E. Sgreccia, A. Nallayagari, F. Vacandio, Saulius Kaciulis, M. Di Vona, Philippe Knauth
Nanocomposites containing B,N-codoped carbon quantum dots (CQDs) and an anion exchange ionomer based on poly(2,6-dimethylpolyphenyleneoxide) with trimethylammonium groups on long side chains (PPO-LC) were studied as catalytic electrodes for the oxygen reduction reaction (ORR). The objective was to reveal the impact of graphitic vs pyridinic/pyrrolic nitrogen on the ORR electrocatalysis. The CQDs were prepared by hydrothermal synthesis and analyzed by X-ray photoelectron spectroscpy to ascertain the B and N content and their position. The electrodes were prepared by drop-casting an ink of CQDs and PPO-LC on acid-treated carbon paper support. Characterizations of the electrodes included water contact angle, capacitance measurements, Fourier transform infrared spectra as well as scanning electron microscopy and optical microscopy. The onset and half-wave potentials, limiting current densities, Koutecky-Levich and Tafel plots revealed that the sample with only pyridinic/pyrrolic nitrogen showed the lowest electrocatalytic performance, underlining the importance of graphitic nitrogen for good ORR activity. Four-electron reduction was observed for the samples containing graphitic nitrogen. The onset potential (0.92 V/RHE) was among the best in the literature for carbonaceous materials. Finally, durability tests were performed indicating a good long-time stability of the electrodes; the electrode degradation was analyzed by impedance spectroscopy.
研究人员将含有掺杂 B、N 的碳量子点（CQDs）和基于长侧链上带有三甲基铵基团的聚（2,6-二甲基聚苯氧化物）阴离子交换离子体（PPO-LC）的纳米复合材料作为氧还原反应（ORR）的催化电极。目的是揭示石墨氮与吡啶/吡咯氮对 ORR 电催化的影响。CQDs 采用水热合成法制备，并通过 X 射线光电子能谱分析确定了 B 和 N 的含量及其位置。电极是通过在酸处理过的碳纸支架上滴铸 CQDs 和 PPO-LC 墨水制备的。电极的表征包括水接触角、电容测量、傅立叶变换红外光谱以及扫描电子显微镜和光学显微镜。起始电位和半波电位、极限电流密度、Koutecky-Levich 图和 Tafel 图显示，仅含有吡啶/吡咯烷氮的样品电催化性能最低，这凸显了石墨氮对良好 ORR 活性的重要性。含有石墨氮的样品出现了四电子还原。起始电位（0.92 V/RHE）是碳质材料文献中最好的。最后，耐久性测试表明电极具有良好的长期稳定性；电极降解情况通过阻抗光谱进行了分析。
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Pub Date : 2024-06-14DOI: 10.1149/1945-7111/ad5870
I. Comnea‐Stancu, Raluca‐Ioana Stefan‐van Staden, J. V. van Staden
Metabolomics has become a key factor for identifying new biomarkers able to be used for early diagnosis of cancer. A zinc oxide-α-cyclodextrin nanocarbon nanocomposite 3D stochastic microsensor (α-CD/ZnO/nanoC) was designed and integrated into an intelligent 3D stochastic enantioselective platform for the enantioanalysis of arginine and leucine in whole blood samples. The α-CD/ZnO/nanoC pastes were morphologicaly characterized by scanning electron microscopy, and electrochemically characterized by cyclic voltammetry and electrochemical impedance spectroscopy. L-Leucine was determined on a working concentration range between 110-11-110-8mol L-1 with a limit of detection of 310-12mol L-1; D-leucine was determined on a working concentration range between 110-16-110-11mol L-1 with a limit of detection of 310-17mol L-1; L-arginine was determined on a working concentration range between 110-12-110-9mol L-1 with a limit of detection of 310-13mol L-1; D-arginine was determined on a working concentration range between 110-14-110-11mol L-1 with a limit of detection of 310-15mol L-1. High sensitivities, selectivities, and enantioselectivities were recorded when the platform was used for the enantioanalysis of arginine and leucine. High recoveries were recorded at the enantioanalysis of arginine/leucine, with low relative standard deviations.
{"title":"Enantioanalysis of Leucine and Arginine: A Key Factor in Lung Cancer Metabolomics","authors":"I. Comnea‐Stancu, Raluca‐Ioana Stefan‐van Staden, J. V. van Staden","doi":"10.1149/1945-7111/ad5870","DOIUrl":"https://doi.org/10.1149/1945-7111/ad5870","url":null,"abstract":"\u0000 Metabolomics has become a key factor for identifying new biomarkers able to be used for early diagnosis of cancer. A zinc oxide-α-cyclodextrin nanocarbon nanocomposite 3D stochastic microsensor (α-CD/ZnO/nanoC) was designed and integrated into an intelligent 3D stochastic enantioselective platform for the enantioanalysis of arginine and leucine in whole blood samples. The α-CD/ZnO/nanoC pastes were morphologicaly characterized by scanning electron microscopy, and electrochemically characterized by cyclic voltammetry and electrochemical impedance spectroscopy. L-Leucine was determined on a working concentration range between 110-11-110-8mol L-1 with a limit of detection of 310-12mol L-1; D-leucine was determined on a working concentration range between 110-16-110-11mol L-1 with a limit of detection of 310-17mol L-1; L-arginine was determined on a working concentration range between 110-12-110-9mol L-1 with a limit of detection of 310-13mol L-1; D-arginine was determined on a working concentration range between 110-14-110-11mol L-1 with a limit of detection of 310-15mol L-1. High sensitivities, selectivities, and enantioselectivities were recorded when the platform was used for the enantioanalysis of arginine and leucine. High recoveries were recorded at the enantioanalysis of arginine/leucine, with low relative standard deviations.","PeriodicalId":509718,"journal":{"name":"Journal of The Electrochemical Society","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141341311","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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