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Lab-on-a-Chip Electrochemical Immunosensor Array Integrated with Microfluidics: Development and Characterisation 集成微流体的芯片上电化学免疫传感器阵列:开发和表征
Pub Date : 2022-09-23 DOI: 10.3390/electrochem3040039
Shifa Felemban, P. Vazquez, T. Balbaied, E. Moore
Lab-on-a-chip has recently become an alternative for in situ monitoring for its portability and simple integration with an electrochemical immunoassay. Here, we present an electrochemical cell-on-a-chip configured in a three-electrode system to detect benzo(a)pyrene (BaP) in water. 11-Mercaptoundecanoic acid (MUA), a self-assembled monolayer (SAM), was used to modify a gold chip surface to reduce the randomness of antibody binding. A carboxylic acid group was activated with -ethyl-3-(3-dimethylaminopropyl) (EDC) in combination with N-hyrodsuccinimide (NHS) before antibody immobilisation. The mechanism of the electrochemical reactions on a gold surface and SAM formation were investigated by cyclic voltammetry and contact angle measurements. The data revealed a lower contact angle in the modified chip and a scan rate of 50 mV/s. Through the addition of modification layers and thiol end groups to the SAM, our design allowed the chip surface to became more insulated. All were tested by amperometric detection using the developed Q-sense system. This novel technique detected multiple samples, and completed the analysis reasonably quickly. While the integrated system proved successful in a lab setting, the aim of the research is to use this system for in situ analysis, which can be brought into a water environment to carry out tests with existing processes. In this way, any issues that may arise from an environmental setting can be rectified in an efficient manner.
芯片实验室最近因其便携性和与电化学免疫分析的简单集成而成为原位监测的替代方案。在这里,我们提出了一个电化学电池芯片配置在一个三电极系统,以检测水中苯并(a)芘(BaP)。11-巯基十四酸(MUA)是一种自组装单层(SAM),用于修饰金芯片表面,以降低抗体结合的随机性。在抗体固定前,用-乙基-3-(3-二甲氨基丙基)(EDC)与n -氢琥珀酰亚胺(NHS)联合激活一个羧酸基团。采用循环伏安法和接触角测量法研究了金表面电化学反应和SAM形成的机理。数据表明,改进后的芯片具有较低的接触角和50 mV/s的扫描速率。通过在SAM中添加修饰层和硫醇端基,我们的设计使芯片表面变得更加绝缘。采用开发的q感系统进行安培检测。该新技术检测了多个样品,并相当快地完成了分析。虽然综合系统在实验室环境中证明是成功的,但研究的目的是将该系统用于现场分析,可以将其带入水环境中,以现有工艺进行测试。通过这种方式,可以有效地纠正环境设置可能产生的任何问题。
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引用次数: 1
Effect of Recombinant Antibodies and MIP Nanoparticles on the Electrical Behavior of Impedimetric Biorecognition Surfaces for SARS-CoV-2 Spike Glycoprotein: A Short Report 重组抗体和MIP纳米颗粒对SARS-CoV-2刺突糖蛋白阻抗生物识别表面电行为的影响
Pub Date : 2022-09-02 DOI: 10.3390/electrochem3030037
Douglas Vieira Thomaz, Riccardo Goldoni, G. Tartaglia, C. Malitesta, E. Mazzotta
Electrochemical immunosensors are often described as innovative strategies to tackle urgent epidemiological needs, such as the detection of SARS-CoV-2 main biomarker, the spike glycoprotein. Nevertheless, there is a great variety of receptors, especially recombinant antibodies, that can be used to develop these biosensing platforms, and very few reports compare their suitability in analytical device design and their sensing performances. Therefore, this short report targeted a brief and straightforward investigation of the performance of different impedimetric biorecognition surfaces (BioS) for SARS-CoV-2, which were crafted from three commonly reported recombinant antibodies and molecularly-imprinted polymer (MIP) nanoparticles (nanoMIP). The selected NanoMIP were chosen due to their reported selectivity to the receptor binding domain (RBD) of SARS-CoV-2 spike glycoprotein. Results showed that the surface modification protocol based on MUDA and crosslinking with EDC/NHS was successful for the anchoring of each tested receptor, as the semicircle diameter of the Nyquist plots of EIS increased upon each modification, which suggests the increase of Rct due to the binding of dielectric materials on the conductive surface. Furthermore, the type of monoclonal antibody used to craft the BioS and the artificial receptors led to very distinct responses, being the RBD5305 and the NanoMIP-based BioS the ones that showcased the highest increment of signal in the conditions herein reported, which suggests their adequacy in the development of impedimetric immunosensors for SARS-CoV-2 spike glycoprotein.
电化学免疫传感器通常被描述为解决紧急流行病学需求的创新策略,例如检测SARS-CoV-2的主要生物标志物刺突糖蛋白。然而,有多种受体,尤其是重组抗体,可用于开发这些生物传感平台,很少有报道比较它们在分析设备设计和传感性能方面的适用性。因此,这篇简短的报告针对SARS-CoV-2的不同阻抗生物识别表面(BioS)的性能进行了简短而直接的研究,这些表面由三种常见的重组抗体和分子印迹聚合物(MIP)纳米颗粒(nanoMIP)制成。所选择的NanoMIP是由于它们对SARS-CoV-2刺突糖蛋白受体结合域(RBD)的选择性。结果表明,基于MUDA和EDC/NHS交联的表面修饰方案对每个被测受体的锚定都是成功的,每次修饰后EIS的Nyquist图的半圆直径增加,这表明Rct的增加是由于介电材料在导电表面的结合。此外,用于制作BioS和人工受体的单克隆抗体类型导致了非常不同的反应,其中RBD5305和基于nanomip的BioS在本文报道的条件下显示出最高的信号增量,这表明它们适合用于开发SARS-CoV-2刺突糖蛋白的阻抗性免疫传感器。
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引用次数: 4
Mass Transport Limitations in Electrochemical Conversion of CO2 to Formic Acid at High Pressure 高压下CO2电化学转化为甲酸的传质限制
Pub Date : 2022-09-02 DOI: 10.3390/electrochem3030038
S. Chinnathambi, M. Ramdin, T. Vlugt
Mass transport of different species plays a crucial role in electrochemical conversion of CO2 due to the solubility limit of CO2 in aqueous electrolytes. In this study, we investigate the transport of CO2 and other ionic species through the electrolyte and the membrane, and its impact on the scale-up process of HCOO−/HCOOH formation. The mass transport of ions to the electrode and the membrane is modelled at constant current density. The mass transport limitations of CO2 on the formation of HCOO−/HCOOH is investigated at different pressures ranges from 5–40 bar. The maximum achievable partial current density of formate/formic acid is increased with increasing CO2 pressure. We use an ion exchange membrane model to understand the ion transport behaviour for both the monopolar and bipolar membranes. The cation exchange (CEM) and anion exchange membrane (AEM) model show that ion transport is limited by the electrolyte salt concentrations. For 0.1 M KHCO3, the AEM reaches the limiting current density more quickly than the CEM. For the BPM model, ion transport across the diffusion layer on either side of the BPM is also included to understand the concentration polarization across the BPM. The model revealed that the polarization losses across the bipolar membrane depend on the pH of the electrolyte used for the CO2 reduction reaction (CO2RR). The polarization loss on the anolyte side decreases with an increasing pH, while, on the cathode side, it increases with increasing catholyte pH. With this combined model for the electrode reactions and the membrane transport, we are able to account for the various factors influencing the polarization losses in the CO2 electrolyzer. To complete the analysis, we simulated the full cell polarization curve and fitted with the experimental data.
由于CO2在水溶液中的溶解度限制,不同物质的质量传递在CO2的电化学转化中起着至关重要的作用。在这项研究中,我们研究了二氧化碳和其他离子物种通过电解质和膜的运输,以及它对HCOO−/HCOOH形成的放大过程的影响。离子到电极和膜的质量传输是在恒定电流密度下模拟的。在5 ~ 40 bar的不同压力范围内研究了CO2对HCOO−/HCOOH形成的质量输运限制。甲酸/甲酸的最大可达分电流密度随CO2压力的增加而增加。我们使用离子交换膜模型来理解单极和双极膜的离子传输行为。阳离子交换(CEM)和阴离子交换膜(AEM)模型表明,离子传输受电解质盐浓度的限制。对于0.1 M KHCO3, AEM比CEM更快地达到极限电流密度。对于BPM模型,离子在BPM两侧扩散层上的传输也被考虑在内,以理解BPM上的浓度极化。该模型表明,双极膜上的极化损失取决于用于CO2还原反应(CO2RR)的电解质的pH值。阳极侧的极化损耗随着pH值的增加而降低,而阴极侧的极化损耗随着阴极侧pH值的增加而增加。通过电极反应和膜传输的组合模型,我们能够解释影响CO2电解槽中极化损耗的各种因素。为了完成分析,我们模拟了全电池极化曲线,并与实验数据进行了拟合。
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引用次数: 4
Recent Insight in Transition Metal Anchored on Nitrogen-Doped Carbon Catalysts: Preparation and Catalysis Application 过渡金属锚定氮掺杂碳催化剂的研究进展:制备及催化应用
Pub Date : 2022-09-01 DOI: 10.3390/electrochem3030036
Boyang Li, L. Zhang, Jianrui Zhang, Yaqiong Su
The design and preparation of novel, high-efficiency, and low-cost heterogeneous catalysts are important topics in academic and industry research. In the past, inorganic materials, metal oxide, and carbon materials were used as supports for the development of heterogeneous catalysts due to their excellent properties, such as high specific surface areas and tunable porous structures. However, the properties of traditional pristine carbon materials cannot keep up with the sustained growth and requirements of industry and scientific research, since the introduction of nitrogen atoms into carbon materials may significantly enhance a variety of their physicochemical characteristics, which gradually become appropriate support for synthesizing supported transition metal catalysts. In the past several decades, the transition metal anchored on nitrogen-doped carbon catalysts has attracted a tremendous amount of interest as potentially useful catalysts for diverse chemical reactions. Compared with original carbon support, the doping of nitrogen atoms can significantly regulate the physicochemical properties of carbon materials and allow active metal species uniformly dispersed on the support. The various N species in support also play a critical role in accelerating the catalytic performance in some reactions. Besides, the interaction between support and transition metal active sites can offer an anchor site to stabilize metal species during the preparation process and then improve reaction performance, atomic utilization, and stability. In this review, we highlight the recent advances and the remaining challenges in the preparation and application of transition metal anchored on nitrogen-doped carbon catalysts.
设计和制备新型、高效、低成本的多相催化剂是学术界和工业界研究的重要课题。过去,无机材料、金属氧化物和碳材料由于具有高比表面积和可调多孔结构等优异的性能,被用作多相催化剂的载体。然而,传统的原始碳材料的性能已经跟不上工业和科研的持续增长和要求,因为在碳材料中引入氮原子可以显著增强其多种物理化学特性,逐渐成为合成负载型过渡金属催化剂的合适载体。在过去的几十年里,过渡金属锚定在氮掺杂碳催化剂上,作为多种化学反应的潜在有用催化剂,引起了人们的极大兴趣。与原始碳载体相比,氮原子的掺杂可以显著调节碳材料的物理化学性质,使活性金属物质均匀分散在载体上。在某些反应中,载体中的各种N对加速催化性能也起着关键作用。此外,载体和过渡金属活性位点之间的相互作用可以提供一个锚点,在制备过程中稳定金属物种,从而提高反应性能、原子利用率和稳定性。本文综述了氮掺杂碳系过渡金属催化剂的制备和应用的最新进展和面临的挑战。
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引用次数: 5
Electrochemical Analysis of Heavy Metal Ions Using Conducting Polymer Interfaces 基于导电聚合物界面的重金属离子电化学分析
Pub Date : 2022-08-26 DOI: 10.3390/electrochem3030034
G. Salinas, B. Frontana-Uribe
Conducting polymers (CPs) are highly conjugated organic macromolecules, where the electrical charge is transported in intra- and inter-chain pathways. Polyacetylene, polythiophene and its derivatives, polypyrrole and its derivatives, and polyaniline are among the best-known examples. These compounds have been used as electrode modifiers to gain sensitivity and selectivity in a large variety of analytical applications. This review, after a brief introduction to the electrochemistry of CPs, summarizes the application of CPs’ electrode interfaces towards heavy metals’ detection using potentiometry, pulse anodic stripping voltammetry, and alternative non-classical electrochemical methods.
导电聚合物(CPs)是一种高度共轭的有机大分子,其电荷通过链内和链间途径传输。聚乙炔、聚噻吩及其衍生物、聚吡咯及其衍生物和聚苯胺是最著名的例子。这些化合物已被用作电极修饰剂,以获得灵敏度和选择性在各种分析应用。本文简要介绍了CPs的电化学性质,总结了CPs电极界面在电位法、脉冲阳极溶出伏安法和其他非经典电化学方法等重金属检测中的应用。
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引用次数: 8
Modelling of Irreversible Homogeneous Reaction on Finite Diffusion Layers 有限扩散层上不可逆均相反应的模拟
Pub Date : 2022-08-26 DOI: 10.3390/electrochem3030033
Singaravel Anandhar Salai Sivasundari, R. Senthamarai, M. Devi, Lakshmanan Rajendran, M. Lyons
The mathematical model proposed by Chapman and Antano (Electrochimica Acta, 56 (2010), 128–132) for the catalytic electrochemical–chemical (EC’) processes in an irreversible second-order homogeneous reaction in a microelectrode is discussed. The mass-transfer boundary layer neighbouring an electrode can contribute to the electrode’s measured AC impedance. This model can be used to analyse membrane-transport studies and other instances of ionic transport in semiconductors and other materials. Two efficient and easily accessible analytical techniques, AGM and DTM, were used to solve the steady-state non-linear diffusion equation’s infinite layers. Herein, we present the generalized approximate analytical solution for the solute, product, and reactant concentrations and current for the small experimental values of kinetic and diffusion parameters. Using the Matlab/Scilab program, we also derive the numerical solution to this problem. The comparison of the analytical and numerical/computational results reveals a satisfactory level of agreement.
本文讨论了由Chapman和Antano (Electrochimica Acta, 56(2010), 128-132)提出的用于微电极中不可逆二阶均相反应的催化电化学-化学(EC)过程的数学模型。电极附近的传质边界层会影响电极的交流阻抗。该模型可用于分析薄膜传输研究以及半导体和其他材料中离子传输的其他实例。采用AGM和DTM两种高效、简便的分析技术,求解了稳态非线性扩散方程的无限层。本文给出了溶质、生成物、反应物浓度和电流对于动力学和扩散参数的小实验值的广义近似解析解。利用Matlab/Scilab程序,给出了该问题的数值解。分析结果与数值计算结果的比较显示出令人满意的一致性。
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引用次数: 2
Three-Dimensional Hybrid Nanostructures of Fe3O4 Nanoparticles/Vertically-Aligned Carbon Nanotubes for High-Performance Supercapacitors 用于高性能超级电容器的Fe3O4纳米颗粒/垂直排列碳纳米管三维杂化纳米结构
Pub Date : 2022-08-26 DOI: 10.3390/electrochem3030035
Bin Zhao
A three-dimensional (3D) hybrid nanostructure of Fe3O4 nanoparticles uniformly anchored on vertically-aligned carbon nanotubes (VACNTs) was fabricated by a facile two-step method. Assisted by supercritical carbon dioxide (SCCO2), the Fe precursor was firstly absorbed on CNT surface and then transformed into Fe3O4 nanoparticles by vacuum thermal annealing. Owing to the synergetic effects of well-distributed Fe3O4 nanoparticles (~7 nm) and highly conductive VACNTs, the hybrid electrode exhibits a high specific capacitance of 364.2 F g−1 at 0.5 A g−1 within the potential range from −0.9 to +0.1 V in Na2SO3 electrolyte and an excellent cycling stability of 84.8% capacitance retention after 2000 cycles at a current density of 4 A/g. This 3D hybrid architecture consisting of aligned CNTs and pseudocapacitive metal oxide may be a promising electrode for high-performance supercapacitors.
采用两步法制备了Fe3O4纳米颗粒均匀固定在垂直排列的碳纳米管(VACNTs)上的三维(3D)杂化纳米结构。在超临界二氧化碳(SCCO2)的辅助下,首先将Fe前驱体吸附在碳纳米管表面,然后通过真空热处理将其转化为Fe3O4纳米颗粒。由于分布均匀的Fe3O4纳米颗粒(~7 nm)和高导电性VACNTs的协同作用,在Na2SO3电解质中,在−0.9 ~ +0.1 V电位范围内,混合电极在0.5 a g−1时具有364.2 F g−1的高比电容,在4 a /g电流密度下,循环2000次后具有84.8%的电容保持率。这种由排列的碳纳米管和假电容性金属氧化物组成的三维混合结构可能是一种很有前途的高性能超级电容器电极。
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引用次数: 0
Carbon-α-Fe2O3 Composite Active Material for High-Capacity Electrodes with High Mass Loading and Flat Current Collector for Quasi-Symmetric Supercapacitors 碳-α-Fe2O3复合活性材料用于高容量高质量负载电极和准对称超级电容器扁平集流器
Pub Date : 2022-08-23 DOI: 10.3390/electrochem3030032
Maedeh Najafi, S. Bellani, Valerio Galli, M. Zappia, A. Bagheri, Milad Safarpour, Hossein Beydaghi, Matilde Eredia, Lea Pasquale, R. Carzino, S. Lauciello, J. Panda, R. Brescia, Luca Gabatel, V. Pellegrini, F. Bonaccorso
In this work, we report the synthesis of an active material for supercapacitors (SCs), namely α-Fe2O3/carbon composite (C-Fe2O3) made of elongated nanoparticles linearly connected into a worm-like morphology, by means of electrospinning followed by a calcination/carbonization process. The resulting active material powder can be directly processed in the form of slurry to produce SC electrodes with mass loadings higher than 1 mg cm−2 on practical flat current collectors, avoiding the need for bulky porous substrate, as often reported in the literature. In aqueous electrolyte (6 M KOH), the so-produced C-Fe2O3 electrodes display capacity as high as ~140 mAh g−1 at a scan rate of 2 mV s−1, while showing an optimal rate capability (capacity of 32.4 mAh g−1 at a scan rate of 400 mV s−1). Thanks to their poor catalytic activity towards water splitting reactions, the electrode can operate in a wide potential range (−1.6 V–0.3 V vs. Hg/HgO), enabling the realization of performant quasi-symmetric SCs based on electrodes with the same chemical composition (but different active material mass loadings), achieving energy density approaching 10 Wh kg−1 in aqueous electrolytes.
在这项工作中,我们报告了一种超级电容器(SCs)活性材料的合成,即α-Fe2O3/碳复合材料(C-Fe2O3),由细长的纳米颗粒线性连接成蠕虫状,通过静电纺丝和煅烧/碳化工艺制成。所得到的活性物质粉末可以直接以浆料的形式加工,在实用的扁平集热器上生产质量负载高于1 mg cm - 2的SC电极,避免了像文献中经常报道的那样需要笨重的多孔基板。在6 M KOH水溶液中,C-Fe2O3电极在扫描速率为2 mV s−1时的容量高达~140 mAh g−1,在扫描速率为400 mV s−1时的容量为32.4 mAh g−1。由于其对水分解反应的催化活性较差,电极可以在宽电位范围内工作(- 1.6 V - 0.3 V vs. Hg/HgO),从而实现基于具有相同化学成分(但活性物质质量负载不同)的电极的高性能准对称SCs,在水电解质中实现接近10 Wh kg−1的能量密度。
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引用次数: 2
Electrochemical Profiling of Plants 植物的电化学分析
Pub Date : 2022-08-04 DOI: 10.3390/electrochem3030030
Mansi Gandhi, K. Amreen
The profiling, or fingerprinting, of distinct varieties of the Plantae kingdom is based on the bioactive ingredients, which are systematically segregated to perform their detailed analysis. The secondary products portray a pivotal role in defining the ecophysiology of distinct plant species. There is a crucial role of the profiling domain in understanding the various features, characteristics, and conditions related to plants. Advancements in variable technologies have contributed to the development of highly specific sensors for the non-invasive detection of molecules. Furthermore, many hyphenated techniques have led to the development of highly specific integrated systems that allow multiplexed detection, such as high-performance liquid chromatography, gas chromatography, etc., which are quite cumbersome and un-economical. In contrast, electrochemical sensors are a promising alternative which are capable of performing the precise recognition of compounds due to efficient signal transduction. However, due to a few bottlenecks in understanding the principles and non-redox features of minimal metabolites, the area has not been explored. This review article provides an insight to the electrochemical basis of plants in comparison with other traditional approaches and with necessary positive and negative outlooks. Studies consisting of the idea of merging the fields are limited; hence, relevant non-phytochemical reports are included for a better comparison of reports to broaden the scope of this work.
植物界的不同品种的分析或指纹是基于生物活性成分,这些成分被系统地分离出来进行详细分析。次生产物在确定不同植物物种的生态生理方面起着关键作用。在了解与植物有关的各种特征、特征和条件方面,分析领域起着至关重要的作用。可变技术的进步促进了用于非侵入性分子检测的高度特异性传感器的发展。此外,许多连字技术已经导致了高特异性集成系统的发展,允许多路检测,如高效液相色谱,气相色谱等,这是相当麻烦和不经济的。相比之下,电化学传感器是一种很有前途的替代方案,由于有效的信号转导,它能够对化合物进行精确识别。然而,由于在了解微量代谢物的原理和非氧化还原特性方面存在一些瓶颈,这一领域尚未得到探索。本文综述了植物的电化学基础,并与其他传统方法进行了比较,并对其进行了积极和消极的展望。合并领域的研究是有限的;因此,相关的非植物化学报告被包括在内,以便更好地比较报告,以扩大这项工作的范围。
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引用次数: 3
Comparative Study of Corrosion Inhibition Efficacy of Alkaloid Extract of Artemesia vulgaris and Solanum tuberosum in Mild Steel Samples in 1 M Sulphuric Acid 蒿和龙葵生物碱提取物在1 M硫酸中对低碳钢样品缓蚀效果的比较研究
Pub Date : 2022-07-29 DOI: 10.3390/electrochem3030029
D. Parajuli, S.R.K. Sharma, H. Oli, Dilip Singh Bohara, D. Bhattarai, Arjun Prasad Tiwari, A. Yadav
Two different types of alkaloids are successfully extracted from two plants Artemisia vulgaris (AV) and Solanum tuberosum (ST) in the laboratory and used as corrosion inhibitors for mild steel samples. The corrosion inhibition potential of these alkaloids is determined by weight loss and potentiodynamic polarization measurement methods. Based on the weight loss measurement study of a sample immersed for 6 h in 1000 ppm inhibitor solution of AV and ST alkaloids, the corrosion inhibition efficiency is found to be 92.58% and 90.79%, respectively. The potentiodynamic polarization measurement shows 88.06% and 83.22% corrosion inhibition efficiency for AV and ST alkaloids, respectively, for the sample immersed for 1 h in 1000 ppm inhibitor solution. These promising efficiency and suitable immersion time effect can lead to the development of good green inhibitors.
在实验室中成功地从两种植物Artemisia vulgaris (AV)和Solanum tuberosum (ST)中提取了两种不同类型的生物碱,并将其用作低碳钢样品的缓蚀剂。用失重法和动电位极化法测定了这些生物碱的缓蚀电位。通过对样品在含AV和ST生物碱的1000 ppm缓蚀剂溶液中浸泡6 h的失重测量研究,发现缓蚀剂的缓蚀效率分别为92.58%和90.79%。电位极化测量结果表明,在1000ppm缓蚀剂溶液中浸泡1h, AV和ST生物碱的缓蚀率分别为88.06%和83.22%。这些有前景的效率和合适的浸泡时间效应将导致良好的绿色缓蚀剂的开发。
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引用次数: 10
期刊
Electrochem
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