Electrochemical science advances最新文献

{"title":"Role of porosity and diffusion coefficient in porous electrode used in supercapacitors – Correlating theoretical and experimental studies","authors":"Puja De,&nbsp;Joyanti Halder,&nbsp;Chinmayee Chowde Gowda,&nbsp;Sakshi Kansal,&nbsp;Surbhi Priya,&nbsp;Satvik Anshu,&nbsp;Ananya Chowdhury,&nbsp;Debabrata Mandal,&nbsp;Sudipta Biswas,&nbsp;Brajesh Kumar Dubey,&nbsp;Amreesh Chandra","doi":"10.1002/elsa.202100159","DOIUrl":"10.1002/elsa.202100159","url":null,"abstract":"<p>Porous electrodes are fast emerging as essential components for next-generation supercapacitors. Using porous structures of Co₃O₄, Mn₃O₄, α-Fe₂O₃, and carbon, their advantages over the solid counterpart is unequivocally established. The improved performance in porous architecture is linked to the enhanced active specific surface and direct channels leading to improved electrolyte interaction with the redox-active sites. A theoretical model utilizing Fick's law is proposed, that can consistently explain the experimental data. The porous structures exhibit ∼50%–80% increment in specific capacitance, along with high rate capabilities and excellent cycling stability due to the higher diffusion coefficients.</p>","PeriodicalId":93746,"journal":{"name":"Electrochemical science advances","volume":"3 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elsa.202100159","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"43602581","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Electrochemical conversion of CO2 in non-conventional electrolytes: Recent achievements and future challenges","authors":"Elizabeth Sargeant,&nbsp;Paramaconi Rodríguez","doi":"10.1002/elsa.202100178","DOIUrl":"10.1002/elsa.202100178","url":null,"abstract":"<p>Electrochemical reduction of CO₂ in traditional aqueous electrolytes suffers from low faradaic efficiency towards desired products which can be traced back to low CO₂ solubility and strong competition from the hydrogen evolution reaction. The use of non-conventional electrolytes aims to mitigate these issues. This review will give a focused overview summarizing some of the most recent contributions on the electrochemical conversion of CO₂ in organic solvents, ionic liquids, solid electrolytes, and brines. We summarize the findings in terms of activity, selectivity, and durability for each of the systems. In addition, it provides an outlook about the role of water, cations, and anions in the reaction. We also highlight the challenges of the electrochemical reduction of CO₂ in each of the electrolytes. All the studies referred to in this review contribute meaningfully to reaching the technical targets for CO₂ electrolyzers in non-conventional electrolytes.</p>","PeriodicalId":93746,"journal":{"name":"Electrochemical science advances","volume":"3 4","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elsa.202100178","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"44698985","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Evolution of the analytical signal in electrochemistry from electrocapillary curve to a digital electrochemical pattern of a multicomponent sample","authors":"Sergey Volodarovich Sokolkov","doi":"10.1002/elsa.202100212","DOIUrl":"10.1002/elsa.202100212","url":null,"abstract":"<p>The number of publications on the electrochemical analysis of liquids increases year by year. The growth of publication activity is largely due to the development of new biosensors and the introduction of nanomaterials into the practice of electrochemical analysis. It is not the task of the author to review the entire array of publications, since the basic principles of electrochemical analysis in most publications remain practically unchanged. The purpose of this critical review is to find answers to two important questions for the development of electroanalysis. First, are all of the used electrochemical methods providing a measurement in the strict metrological sense of this term? That is, do they provide the necessary accuracy, validity, reliability, and reproducibility of the measurement results? Secondly, is electroanalytics capable of meeting the challenge of the information revolution by significantly increasing the information efficiency of each individual measurement? To answer these questions, we will identify the main sources of sensor signal noise by considering the electrochemical sensor as the primary decoder of “chemical information” into an analytical signal. Then we will evaluate the information efficiency of various measurement methods by using the approach of thermodynamics of information processes and considering a sensor as an open thermodynamic system.</p>","PeriodicalId":93746,"journal":{"name":"Electrochemical science advances","volume":"3 3","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elsa.202100212","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"46738385","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Mesoporosity and nitrogen doping: The leading effect in oxygen reduction reaction activity and selectivity at nitrogen-doped carbons prepared by using polyethylene oxide-block-polystyrene as a sacrificial template","authors":"Marco Mazzucato,&nbsp;Giorgia Daniel,&nbsp;Valentina Perazzolo,&nbsp;Riccardo Brandiele,&nbsp;Gian Andrea Rizzi,&nbsp;Abdirisak Ahmed Isse,&nbsp;Armando Gennaro,&nbsp;Christian Durante","doi":"10.1002/elsa.202100203","DOIUrl":"10.1002/elsa.202100203","url":null,"abstract":"<p>Four mesoporous carbons (MCs) with tunable pore size were synthesized by soft template synthesis, employing a resorcinol-formaldehyde resin as a carbon precursor and a polyethylene oxide-block-polystyrene block copolymer as a sacrificial template in which the length of the polystyrene block (165, 300, 500, and 1150 units) allowed the modulation of the surface area of MCs (567, 582, 718 and 840 m² g⁻¹, respectively). The complete set of MCs was also doped with nitrogen by ball milling in the presence of cyanamide and stabilized in a second thermal treatment at 750°C, leading to nitrogen content of ∼2.65% in all samples. The two sets of MCs were used for evaluating both the effect of textural properties and nitrogen doping in the electrochemical reduction of oxygen in acid electrolytes. Each catalyst was characterized by means of elemental analysis and N₂ physisorption analysis, whereas the selected series of samples were also characterized by transmission electron microscopy, scanning electron microscopy, X-ray photoemission spectroscopy, inductively coupled plasma mass spectroscopy (ICP-MS), and Raman analysis. Voltammetric rotating ring-disk measurements in 0.5 M H₂SO₄ demonstrated that the catalytic activity for the O₂ reduction scales with the surface area in the non-doped series, and also the selectivity for the two-electron process leading to H₂O₂ increases in the samples having wider pores and higher surface area, even if the leading mechanism is the tetraelectronic process leading to H₂O. The doping with nitrogen leads to a general increase of the catalytic activity with a shift of the O₂ peak potential to more positive values of 75–150 mV. In the doped series, nitrogen doping prevails on the textural properties for guiding the selectivity toward the two- or four-electron process, since a similar H₂O₂ yield was observed for all N-MC samples. The possible presence of FeN<i>_x</i> sites derived from the ball milling fixation of nitrogen was evaluated by using the NO-stripping technique.</p>","PeriodicalId":93746,"journal":{"name":"Electrochemical science advances","volume":"3 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elsa.202100203","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"43883432","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Ubiquinone electrochemistry in analysis and sensing","authors":"Peter Ó Conghaile,&nbsp;Damien W. M. Arrigan","doi":"10.1002/elsa.202100214","DOIUrl":"10.1002/elsa.202100214","url":null,"abstract":"<p>Ubiquinone (UQ) is a lipophilic compound present in most living organisms, where UQ's interesting but complex electrochemistry serves an important role in the transfer of electrons and protons within and across the mitochondrial membrane. We briefly review the electrochemical characteristics of UQ and its reduced state, ubiquinol, in solution and immobilized on electrodes, together with its application in electrochemical sensing and detection systems, for example, measuring redox status with reference to reactive oxidative species. The importance of the local environment, solvent, electrolyte, organic membrane, and pH, on the electrochemical behavior of UQ, is also discussed. We discuss techniques used for the direct detection of UQ such as liquid chromatography-electrochemistry. Mediated electrochemistry of UQ allows for quantitative measurements of ions, small molecules, and other analytes such as glucose via chemical sensors and biosensors.</p>","PeriodicalId":93746,"journal":{"name":"Electrochemical science advances","volume":"3 3","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-02-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elsa.202100214","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49510106","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Enzyme based field effect transistor: State-of-the-art and future perspectives","authors":"Lucia Sarcina,&nbsp;Eleonora Macchia,&nbsp;Angelo Tricase,&nbsp;Cecilia Scandurra,&nbsp;Anna Imbriano,&nbsp;Fabrizio Torricelli,&nbsp;Nicola Cioffi,&nbsp;Luisa Torsi,&nbsp;Paolo Bollella","doi":"10.1002/elsa.202100216","DOIUrl":"10.1002/elsa.202100216","url":null,"abstract":"<p>The review discloses the historical and technological evolution of enzyme-based field-effect transistors (EnFETs) underlying the importance of gate electrode modification toward the implementation of novel FETs configurations such as extended-gate FET (EG-FETs) or EG organic FETs (EG-OFETs). The working principle of the EnFETs as postulated by Bergveld in 1970, who defined the EnFET as an ion-selective FET (ISFET) modified with enzyme-membrane, is also discussed considering the analytical equations related to the EnFET output response. For each category, namely EnFETs, EG-FETs, and EG-OFETs, we reviewed the key devices’ configurations that addressed the research in this field in the last 40 years with particular attention to the analytical figures of merit.</p>","PeriodicalId":93746,"journal":{"name":"Electrochemical science advances","volume":"3 3","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elsa.202100216","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41326026","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Recent advances in ion-sensitive field-effect transistors for biosensing applications","authors":"Xiaohao Ma,&nbsp;Ruiheng Peng,&nbsp;Wei Mao,&nbsp;Yuanjing Lin,&nbsp;Hao Yu","doi":"10.1002/elsa.202100163","DOIUrl":"10.1002/elsa.202100163","url":null,"abstract":"<p>Over the past decades, considerable development and improvement can be observed in the area of the ion-sensitive field-effect transistor (ISFET) for biosensing applications. The mature semiconductor industry provides a solid foundation for the commercialization of the ISFET-based sensors and extensive research has been conducted to improve the performance of ISFET, with a special research focus on the materials, device structures, and readout topologies. In this review, the basic theories and mechanisms of ISFET are first introduced. Research on ISFET gate materials is reviewed, followed by a summary of typical gate structures and signal readout methods for the ISFET sensing system. After that, a variety of biosensing applications including ions, deoxyribonucleic acid, proteins, and microbes are presented. Finally, the prospects and challenges of the ISFET-based biosensors are discussed.</p>","PeriodicalId":93746,"journal":{"name":"Electrochemical science advances","volume":"3 3","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elsa.202100163","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"46181281","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Influence of carbon binder domain on the performance of lithium-ion batteries: Impact of size and fractal dimension","authors":"Anshuman Chauhan,&nbsp;Ermek Asylbekov,&nbsp;Susanne Kespe,&nbsp;Hermann Nirschl","doi":"10.1002/elsa.202100151","DOIUrl":"10.1002/elsa.202100151","url":null,"abstract":"<p>A lithium-ion battery (LIB) cathode comprises three major components: active material, electrical conductivity additive, and binder. The combination of binder and electrical conductivity additive leads to the formation of composite clusters known as the carbon binder domain (CBD) clusters. Preparation of a LIB cathode strongly influences the dispersion of the above-mentioned constituents leading to the formation of distinct pore and electrical conduction networks. The resulting structure thus governs the performance of LIBs. The presence of CBD is essential for the structural integrity and sufficient electrical conductivity of the LIB cathode. However, CBD abundance in LIB cathodes leads to unfavorable gravimetrical and volumetrical consequences owing to its electrochemical inertness. Increasing CBD content adds to the weight of the LIBs, thus negatively impacting the energy density. Furthermore, increased electrical conductivity is won at a cost of ionic conductivity as CBD clusters breach the pore networks in the cathode microstructure. The following study establishes a link between the various possibilities of CBD cluster size and fractal dimension that may eventualize during the mixing process of slurry preparation to the resulting microstructural properties and hence to the performance of LIBs by means of idealized cathode geometries. Since the performance determining processes occur at the microstructural scale, which are often very tedious to study via experimental research, the study makes use of spatially resolving microstructural, numerical, simulations. The results demonstrate that the CBD cluster size has a strong influence on the cathode microstructure. The CBD cluster fractal dimension on the other hand displayed a minor influence on the structural properties of the cathode, and the size of the cluster primary particles was shown to be the dominant factor. Finally, performance evaluation simulations confirmed the trends seen in structural properties with changing cluster size and fractal dimension.</p>","PeriodicalId":93746,"journal":{"name":"Electrochemical science advances","volume":"3 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elsa.202100151","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"44356841","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Ionic transport modeling for liquid electrolytes - Experimental evaluation by concentration gradients and limited currents","authors":"Maximilian Schalenbach,&nbsp;Burkhard Hecker,&nbsp;Bernhard Schmid,&nbsp;Yasin Emre Durmus,&nbsp;Hermann Tempel,&nbsp;Hans Kungl,&nbsp;Rüdiger-A. Eichel","doi":"10.1002/elsa.202100189","DOIUrl":"10.1002/elsa.202100189","url":null,"abstract":"<p>A direct current in an electrochemical cell with a diluted liquid electrolyte leads to the displacement of ions within the solvent, while diffusion works against the resulting concentration differences. This study aims to experimentally evaluate a physicochemical ion transport model (source code provided) that describes current-driven concentration gradients in diluted electrolytes. Hereto, an aqueous 0.1 M CuSO₄ electrolyte between metallic copper electrodes serves as an experimental test system. Spatially resolved optical measurements are used to monitor the evolution of the ion concentration gradient in the electrolyte. Moreover, measured limited currents are related to computationally modeled concentration gradients. A constant parameterization of the diffusion coefficient, molar conductivity and ion transport number lead to a slight overestimation of the cathodic ion depletion and cell resistance, whereas a literature data based concentration dependent parameterization matches better to the measured data. The limited current is considered under a computational parameter variation and thereby related to the physicochemical impact of different electrolyte properties on the ion transport. This approach highlights the differences between purely diffusion limited currents and the limited current resulting from the combined electric field and diffusion driven ion motion. A qualitative schematic sketch of the physical mechanisms of the ion movement is presented to illustrate the current driven ion displacement in liquid electrolytes.</p>","PeriodicalId":93746,"journal":{"name":"Electrochemical science advances","volume":"3 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elsa.202100189","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"47574256","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Tuning the moisture stability of multiphase β-Li3PS4 solid electrolyte materials","authors":"Xin Lu,&nbsp;Osmane Camara,&nbsp;Zigeng Liu,&nbsp;Anna Windmüller,&nbsp;Chih-Long Tsai,&nbsp;Hermann Tempel,&nbsp;Shicheng Yu,&nbsp;Hans Kungl,&nbsp;Rüdiger-A. Eichel","doi":"10.1002/elsa.202100208","DOIUrl":"10.1002/elsa.202100208","url":null,"abstract":"<p>Efficiently improving the moisture stability of β-Li₃PS₄ materials could significantly reduce production costs and eventually enable the mass application. Nanoporous multiphase β-Li₃PS₄ materials prepared via solvent-assistant routes usually contain solvent or solvent decomposition segments associated with the amorphous Li₃PS₄ phase in their structures. Herein, the solvent ethyl propionate (EP) remains in the β-Li₃PS₄ even after 220 h of annealing at 220°C. The possibility of tuning the moisture stability of β-Li₃PS₄ by adjusting the content of the solvent is investigated by environmental scanning electron microscopy (ESEM) combined with other structural analysis techniques. The results demonstrated that the hydrogen-containing amorphous Li₃PS₄ not only stabilizes the β-phase at room temperature but also improves the moisture stability of the material. Although the rapid hydrolysis occurs on the surface of solvent-containing β-Li₃PS₄ materials under ambient conditions within 10 s, with 4 wt% EP content, the material can be exposed to 1.6% relative humidity (R.H.) for at least 8 h without any structural or microstructural change. Even with the lower amount of EP (1.2 wt%) in the Li₃PS₄ structure, the material can withstand 1% R.H. for more than 8 h, which allows the material to be manufactured in a dry room. Our observation proposes a simple method to slightly modify the moisture stability of β-Li₃PS₄ to match the different manufacturing conditions.</p>","PeriodicalId":93746,"journal":{"name":"Electrochemical science advances","volume":"3 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/elsa.202100208","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41760833","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}