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Multivariate optimization and application verification of electrochemical oxidation process for reactive dye wastewater generated by washing 电化学氧化工艺处理活性染料洗涤废水的多元优化及应用验证
IF 5.4 3区 工程技术 Q1 Chemistry Pub Date : 2023-12-01 DOI: 10.1016/j.elecom.2023.107628
Xu Zhao , Zehua Ren , Haodong Bi , Qingbo Yang , Lihui An , Bo Zhu , Hongbo Wang , Jianli Liu

At present, organic wastewater containing dyes has become one of the main threats to the environment, and wastewater pollution caused by dyes released from fabrics during home washing also accounts for a large proportion. In this study, Ti/IrO2 electrodes for dye waste degradation were designed and prepared with Reactive Yellow 210 (RY 210), Reactive Blue 19 (RB 19) and Reactive Blue 21 (RB 21) solutions, and a laboratory electrochemical reactor was constructed. Secondly, in the reactor, the effects of current density (20–60 mA cm−2), electrolyte concentration (NaCl, 0.01–0.03 M L−1), and initial dye concentration (30–70 mg L−1) on the COD degradation rate and energy consumption of the dye solution were explored, and the parameters were optimized by the Box-Behnken design, and the equipment was realized in the washing machine. The results showed that the effect of degradation parameters on the degradation of the three groups of dyes was: current density > initial dye concentration > electrolyte concentration. Through parameter optimization, the average COD degradation rates of the three groups of dyes, Reactive Yellow 210 (RY 210), Reactive Blue 19 (RB 19) and Reactive Blue 21 (RB 21), reached 50.71%, 41.65%, and 33.12%, respectively, and the degradation energy consumption decreased by the same trend as 29.91%, 26.49%, and 65.91%, respectively.

目前,含染料的有机废水已成为对环境的主要威胁之一,而家庭洗涤过程中织物释放的染料所造成的废水污染也占很大比例。本研究设计并制备了活性黄210 (RY 210)、活性蓝19 (RB 19)和活性蓝21 (RB 21)溶液降解染料废水的Ti/IrO2电极,并搭建了实验室电化学反应器。其次,在反应器中探讨了电流密度(20 ~ 60 mA cm−2)、电解液浓度(NaCl, 0.01 ~ 0.03 M L−1)和初始染料浓度(30 ~ 70 mg L−1)对染料溶液COD降解率和能耗的影响,并采用Box-Behnken设计对参数进行了优化,并在洗衣机上实现了该设备。结果表明,降解参数对三组染料降解的影响分别为:电流密度>染料初始浓度>电解液浓度。通过参数优化,活性黄210 (RY 210)、活性蓝19 (RB 19)和活性蓝21 (RB 21)三组染料的COD平均降解率分别达到50.71%、41.65%和33.12%,降解能耗下降趋势相同,分别为29.91%、26.49%和65.91%。
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引用次数: 0
Highly sensitive electrochemical assay based on strand displacement polymerization-assisted CRISPR/Cas12a collateral cleavage 基于链置换聚合辅助CRISPR/Cas12a侧链切割的高灵敏度电化学分析
IF 5.4 3区 工程技术 Q1 Chemistry Pub Date : 2023-12-01 DOI: 10.1016/j.elecom.2023.107629
Yulin Zhu , Xifeng Chen , Jiayue Shi , Haixuan Sun , Hua Chai , Peng Miao

In this work, a novel strand displacement polymerization strategy is designed with a single hairpin-structured DNA probe acting as both of primer and template. After target miRNA-induced structural transitions, extension and displacement reactions occur at the dimer with recycled target miRNA. The generated double-stranded products further activate CRISPR/Cas12a collateral cleavage of substrate DNA at the electrode surface, which can be reflected by the silver stripping peak variations. By analyzing the reduced peak intensity, the concentration of miRNA can be determined. This method combines the strand displacement amplification and CRISPR/Cas12a’s shearing capability. Thus a highly sensitive electrochemical biosensor is established with the limit of detection as low as 31 aM. It may also inspire new ideas of electrochemical platforms integrating CRISPR/Cas system for biological studies and clinical applications.

在这项工作中,设计了一种新的链位移聚合策略,该策略使用单个发夹结构的DNA探针作为引物和模板。靶miRNA诱导的结构转变后,再生靶miRNA二聚体发生延伸和位移反应。生成的双链产物进一步激活了电极表面底物DNA的CRISPR/Cas12a侧切,这可以通过银剥离峰的变化来反映。通过分析减弱的峰强度,可以确定miRNA的浓度。该方法结合了链位移扩增和CRISPR/Cas12a的剪切能力。因此,建立了一种高灵敏度的电化学生物传感器,检测限低至31 aM。这也可能激发整合CRISPR/Cas系统的电化学平台用于生物学研究和临床应用的新思路。
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引用次数: 0
An alkaline ferrocyanide non-enzymatic electrochemical sensor for creatinine detection 用于检测肌酐的碱性亚铁氰化物非酶电化学传感器
IF 5.4 3区 工程技术 Q1 Chemistry Pub Date : 2023-11-24 DOI: 10.1016/j.elecom.2023.107624
Sonal Bajpai, Geoffrey R. Akien, Kathryn E. Toghill

Creatinine is a useful metabolite for the evaluation of Chronic Kidney Disease (CKD). Creatinine concentrations in urine outside of the healthy range of 4 to 15 mM may indicate CKD and other kidney conditions. Early detection and monitoring can provide lifesaving intervention, and as such there is a need to develop rapid, cheap and selective electrochemical creatinine sensors. A simple non-enzymatic creatinine sensing platform enabled by the electrocatalytic response of the metabolite to ferricyanide in alkaline conditions is presented. Studies were made on unmodified glassy carbon (GCE) and screen printed carbon electrodes (SPCE), both giving sensitivity of 21 ± 5 µA mM−1 cm−2 and limit of detection of ca. 60 µM.

肌酐是评估慢性肾脏病(CKD)的有效代谢物。尿液中的肌酐浓度超出 4 至 15 毫摩尔的健康范围,可能预示着慢性肾脏病和其他肾脏疾病。早期检测和监测可提供挽救生命的干预措施,因此有必要开发快速、廉价和选择性的电化学肌酐传感器。本文介绍了一种简单的非酶肌酐传感平台,该平台利用代谢物在碱性条件下对铁氰化物的电催化反应来实现。对未改性玻璃碳 (GCE) 和丝网印刷碳电极 (SPCE) 进行了研究,两者的灵敏度均为 21 ± 5 µA mM-1 cm-2,检测限约为 60 µM。
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引用次数: 0
On demand, wireless electrochemical release of brain derived neurotrophic factor 按需无线电化学释放脑源性神经营养因子
IF 5.4 3区 工程技术 Q1 Chemistry Pub Date : 2023-11-24 DOI: 10.1016/j.elecom.2023.107626
Chunyan Qin , Zhilian Yue , Robert J. Forster , Jun Chen , Gordon G. Wallace

Organic conductive polymers are prime candidates for the on demand or controlled release of neurotrophic proteins which can enhance the electrode-neural interface. In this study, bipolar electrochemistry (BPE) is employed to provide a wireless electrical stimulation that avoids the need for the direct physical connection necessary for conventional approaches. Brain-derived neurotrophic factor (BDNF) was incorporated into polypyrrole (PPy) with poly (2-methoxy-5 aniline sulfonic acid) (PMAS) as a dopant during the course of electrochemical synthesis. The synthetic PPy-PMAS-BDNF material acts as the bipolar electrode and is placed within an electric field generated by two driving electrodes. Controlled release of BDNF is demonstrated, which is wireless powered by BPE. This is likely due to the wirelessly activated redox reactions which induce gaps/channels within the structure. Quantification of the BDNF reveals significant differences in the controlled-release properties of the films driven by BPE compared to conventional wired electrochemistry. Human neuroblastoma cells (SH-SY5Y) cultured on the PPy-PMAS-BDNF electrode were subjected to one-week of wireless electrostimulation. Neurite outgrowth was significantly improved when the polymer containing BDNF and the film BPE stimulation. The data suggest that when the BPE is applied, the cells simultaneously respond to the wirelessly released BDNF and the wireless electrical stimulation through the bipolar electroactive polymer electrode. This synergistic effect promotes enhanced neurite outgrowth across the electrodes.

有机导电聚合物是按需或控制释放神经营养蛋白的主要候选者,可以增强电极-神经界面。在这项研究中,双极电化学(BPE)被用于提供无线电刺激,避免了传统方法所必需的直接物理连接。在电化学合成过程中,脑源性神经营养因子(BDNF)与聚(2-甲氧基-5苯胺磺酸)(PMAS)作为掺杂剂掺入聚吡咯(PPy)中。合成的PPy-PMAS-BDNF材料作为双极电极,并放置在由两个驱动电极产生的电场中。演示了BDNF的控制释放,它由BPE无线供电。这可能是由于无线激活的氧化还原反应在结构内诱导了间隙/通道。BDNF的定量分析表明,与传统的有线电化学相比,BPE驱动的薄膜在控释性能上存在显著差异。在py - pmas - bdnf电极上培养的人神经母细胞瘤细胞(SH-SY5Y)进行为期一周的无线电刺激。当含有BDNF的聚合物和BPE膜刺激时,神经突生长明显改善。数据表明,当施加BPE时,细胞同时对无线释放的BDNF和通过双极电活性聚合物电极的无线电刺激做出反应。这种协同效应促进了神经突在电极上的生长。
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引用次数: 0
Fast on-site simultaneous electroanalysis of fusidic acid and betamethasone in pharmaceuticals and water samples using novel stochastic platform 基于新型随机平台的药物和水样中氟西地酸和倍他米松的快速现场同步电分析
IF 5.4 3区 工程技术 Q1 Chemistry Pub Date : 2023-11-24 DOI: 10.1016/j.elecom.2023.107625
Bianca-Maria Tuchiu , Raluca-Ioana Stefan-van Staden , Jacobus (Koos) Frederick van Staden

Fusidic acid and betamethasone are two pharmaceutically active compounds found in topical dosage forms. Sometimes, they can unintentionally wind up in surface water via skin washing. Therefore, a stochastic platform based on a type of calix[4]arene and polyaniline modified screen-printed electrode was developed for their on-site analysis. For both analytes, remarkably wide dynamic ranges (1.0 × 10−17–1.0 × 10−4 for fusidic acid, and 1.0 × 10−18–1.0 × 10−3 for betamethasone) and considerably low limits of quantitation (1.0 × 10−17 for fusidic acid, and 1.0 × 10−18 for betamethasone) were attained. Moreover, the proposed platform was successfully applied to real samples such as topical dosage form and surface water, obtaining recovery values higher than 90.0 % with relative standard deviation values below 0.1 %.

氟西地酸和倍他米松是在外用剂型中发现的两种药物活性化合物。有时,它们会通过皮肤清洗无意中进入地表水。因此,我们开发了一种基于杯[4]芳烃和聚苯胺修饰的丝网印刷电极的随机平台,用于现场分析。对分析物,非常宽动态范围(1.0 × 10−17 - 1.0 × 10−4梭链孢酸,和1.0 × 10−18 - 1.0 × 10−3倍他米松)和相当低的极限定量(1.0 ×10−17 梭链孢酸,和1.0 × 10−18倍他米松)获得。此外,该平台成功应用于外用剂型和地表水等实际样品,回收率高于90.0 %,相对标准偏差小于0.1 %。
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引用次数: 0
Real-time observation of intermediate species in electrochemical oxygen evolution reactions on CoOx through soft X-ray absorption spectroscopy 软x射线吸收光谱法实时观察CoOx上电化学析氧反应中的中间物质
IF 5.4 3区 工程技术 Q1 Chemistry Pub Date : 2023-11-23 DOI: 10.1016/j.elecom.2023.107627
Kaoruho Sakata , Kenta Amemiya

Real-time monitoring of oxygen species during the oxygen evolution reaction (OER) on cobalt oxide, one of the major OER electrocatalysts, was achieved through operando observation using wavelength-dispersive X-ray absorption spectroscopy (XAS) at the oxygen K-edge. The XAS spectra were collected every 3 s during electrode potential sweeping for the OER, and oxygen intermediate species related to the rate-determining step of the OER were detected just below the onset potential. Moreover, the cobalt L-edge XAS results demonstrate that the Co3O4 species dominates the surface of the electrode at a relatively high potential region, where the OER occurs. The present technique has significant potential for application in the analysis of solid–liquid interfaces, whose fundamental understanding is useful for further improvement of electrocatalysis.

利用波长色散x射线吸收光谱(XAS)在氧k边的operando观测,实现了氧化钴(OER的主要电催化剂之一)析氧反应(OER)过程中氧的实时监测。在OER的电极电位扫描过程中,每隔3s采集一次XAS光谱,在起始电位下方检测到与OER速率决定步骤相关的氧中间体。此外,钴的l边XAS结果表明,Co3O4物质在电极表面的相对高电位区域占主导地位,这是OER发生的地方。本方法在固液界面分析中具有重要的应用潜力,对其基本认识有助于电催化的进一步改进。
{"title":"Real-time observation of intermediate species in electrochemical oxygen evolution reactions on CoOx through soft X-ray absorption spectroscopy","authors":"Kaoruho Sakata ,&nbsp;Kenta Amemiya","doi":"10.1016/j.elecom.2023.107627","DOIUrl":"https://doi.org/10.1016/j.elecom.2023.107627","url":null,"abstract":"<div><p>Real-time monitoring of oxygen species during the oxygen evolution reaction (OER) on cobalt oxide, one of the major OER electrocatalysts, was achieved through operando observation using wavelength-dispersive X-ray absorption spectroscopy (XAS) at the oxygen K-edge. The XAS spectra were collected every 3 s during electrode potential sweeping for the OER, and oxygen intermediate species related to the rate-determining step of the OER were detected just below the onset potential. Moreover, the cobalt L-edge XAS results demonstrate that the Co<sub>3</sub>O<sub>4</sub> species dominates the surface of the electrode at a relatively high potential region, where the OER occurs. The present technique has significant potential for application in the analysis of solid–liquid interfaces, whose fundamental understanding is useful for further improvement of electrocatalysis.</p></div>","PeriodicalId":304,"journal":{"name":"Electrochemistry Communications","volume":null,"pages":null},"PeriodicalIF":5.4,"publicationDate":"2023-11-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S1388248123002023/pdfft?md5=3e57a60b30dd012c6d6a83b3e59f1d7a&pid=1-s2.0-S1388248123002023-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138453825","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
The effect of additional nitrogen source on iron phthalocyanine-based nanocarbon catalysts for oxygen reduction reaction in acidic media 附加氮源对酸性介质中氧还原反应中酞菁铁基纳米碳催化剂的影响
IF 5.4 3区 工程技术 Q1 Chemistry Pub Date : 2023-11-20 DOI: 10.1016/j.elecom.2023.107623
Yogesh Kumar , Elo Kibena-Põldsepp , Srinu Akula , Jekaterina Kozlova , Arvo Kikas , Jaan Aruväli , Vambola Kisand , Kaupo Kukli , Kaido Tammeveski

The focus in the development of catalysts doped with transition metals aims to replace platinum group metal catalysts in fuel cells. However, these non-precious metal catalysts exhibit limited performance in acidic environment for the oxygen reduction reaction (ORR) due to issues such as metal agglomeration and the subsequent loss of active sites. Herein, we synthesised catalysts doped with iron and nitrogen on a composite material consisting of carbide-derived carbon (CDC) and graphene (G), employing an additional nitrogen source dicyandiamide (DCDA), denoted as FeN-CDC/G/DCDA. Our physico-chemical analysis unveiled that the inclusion of DCDA was effective in mitigating metal agglomeration during the synthesis process and increasing the presence of Fe-Nx sites in the catalysts. Notably, the FeN-CDC/G/DCDA catalyst exhibited enhanced ORR activity in acid media with half-wave potential (E1/2) of 0.76 V, surpassing the performance of the FeN-CDC/G catalyst, which had an E1/2 value of 0.70 V. Furthermore, the rotating ring-disk electrode results indicated a reduced formation of hydrogen peroxide when employing the FeN-CDC/G/DCDA catalyst. The findings from this study represent a significant step towards the development of efficient catalysts for fuel cells, underscoring the pivotal role of additional nitrogen doping and its positive impact on the ORR performance.

过渡金属掺杂催化剂的发展重点在于取代燃料电池中的铂族金属催化剂。然而,这些非贵金属催化剂在酸性环境下的氧还原反应(ORR)中由于金属团聚和随后的活性位点损失等问题表现出有限的性能。本文中,我们在由碳化物衍生碳(CDC)和石墨烯(G)组成的复合材料上合成了掺杂铁和氮的催化剂,使用额外的氮源双氰胺(DCDA),标记为FeN-CDC/G/DCDA。我们的理化分析表明,DCDA的加入有效地减轻了合成过程中的金属团聚,并增加了催化剂中Fe-Nx位点的存在。值得注意的是,当半波电位(E1/2)为0.76 V时,FeN-CDC/G/DCDA催化剂在酸性介质中的ORR活性增强,超过了E1/2为0.70 V的FeN-CDC/G催化剂。此外,旋转环盘电极结果表明,当使用FeN-CDC/G/DCDA催化剂时,过氧化氢的形成减少。这项研究的发现代表了燃料电池高效催化剂发展的重要一步,强调了额外氮掺杂的关键作用及其对ORR性能的积极影响。
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引用次数: 0
Using molten-salts as a thermal processing medium for cobalt-free lithium-rich cathode material 用熔盐作为无钴富锂正极材料的热加工介质
IF 5.4 3区 工程技术 Q1 Chemistry Pub Date : 2023-11-18 DOI: 10.1016/j.elecom.2023.107617
Sven Burke , Jay Whitacre

Lithium-rich nickel manganese oxide cathode materials are well known to have limited rate capabilities. In this investigation we demonstrate that modifying a common sol-gel synthetic route by adding simple salts to the precursors during firing can create a molten-salt environment for the synthesis of the material that may results in improved materials and performance attributes. After screening multiple salt species, our findings indicate that the use of NaCl can provide a cost-effective and facile method for increasing the rate capability of these materials.

众所周知,富锂镍锰氧化物正极材料具有有限的速率能力。在这项研究中,我们证明了通过在烧制过程中向前驱体添加简单的盐来修改常见的溶胶-凝胶合成路线,可以为材料的合成创造一个熔融盐环境,从而可以改善材料和性能属性。通过对多种盐的筛选,我们的研究结果表明,使用NaCl可以为提高这些材料的速率能力提供一种经济、简便的方法。
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引用次数: 0
Reduced graphene oxide coated with amorphous lead as positive additive for enhanced performance of lead–carbon batteries 还原氧化石墨烯包覆无定形铅作为正添加剂用于提高铅碳电池的性能
IF 5.4 3区 工程技术 Q1 Chemistry Pub Date : 2023-11-14 DOI: 10.1016/j.elecom.2023.107622
Zeming Li , Simiao Huang , Daiwen Tao , Hui Yang , Jinyu Wang , Qilong Zhang

Composites of reduced graphene oxide coated with amorphous lead (Pb/rGO) were prepared by electrostatic adsorption and hydrothermal methods, and used as positive additives for lead–carbon batteries to enhance discharge specific capacity and cycle life under high-rate partial-state-of-charge (HRPSoC) of batteries. Amorphous Pb inhibits the oxygen evolution reaction (OER) that occurs on the surface of reduced graphene oxide (rGO) and increases the specific capacitance of the positive active material (PAM). In addition, the presence of amorphous Pb enhances the affinity of rGO to PAM, which avoids the separation of additive and PAM during the cycling process. Pb/rGO additives can act as pore forming agents and significantly increase the specific surface area of PAM, which enables the electrolyte to fully react with PAM to inhibit the overgrowth of PbSO4 crystals. Thus, Pb/rGO additives help to improve the electrochemical performance of batteries. To be specific, when the Pb/rGO additive content is 0.7 wt%, battery showed the best discharge specific capacity (102 mAh/g) and cycle life (18,104 cycles), which is 117% and 104% higher than that of blank battery, respectively. And the rate capability is also improved compared to its counterpart. In short, the Pb/rGO composite material has potential application value in lead–carbon batteries.

采用静电吸附和水热法制备了还原氧化石墨烯包覆无定形铅的复合材料(Pb/rGO),并将其作为铅碳电池的正极添加剂,以提高电池在高倍率部分充电状态下的放电比容量和循环寿命。无定形Pb抑制了还原氧化石墨烯(rGO)表面发生的析氧反应(OER),增加了正极活性材料(PAM)的比电容。此外,无定形Pb的存在增强了还原氧化石墨烯对PAM的亲和力,避免了循环过程中添加剂与PAM的分离。Pb/rGO添加剂可以作为成孔剂,显著增加PAM的比表面积,使电解质与PAM充分反应,抑制PbSO4晶体的过度生长。因此,铅/氧化石墨烯添加剂有助于提高电池的电化学性能。其中,当Pb/rGO添加剂含量为0.7 wt%时,电池的放电比容量为102 mAh/g,循环寿命为18104次,分别比空白电池提高117%和104%。与同类产品相比,其速率能力也有所提高。总之,Pb/rGO复合材料在铅碳电池中具有潜在的应用价值。
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引用次数: 0
Current collector-free printed three-dimensional MXene-based anodes for lithium-ion batteries 用于锂离子电池的无集电极印刷三维mxene基阳极
IF 5.4 3区 工程技术 Q1 Chemistry Pub Date : 2023-11-11 DOI: 10.1016/j.elecom.2023.107621
Alisher Kumarov , Emmanuel Chisom Nwaogu , Alnur Zhumadil , Zhumabay Bakenov , Arailym Nurpeissova

This work presents a novel approach for fabricating current collector-free three-dimensional (3D) anodes for Lithium-ion batteries (LIBs) based on MXene, a 2D material with excellent conductivity and lithium-ion intercalation properties. The 3D MXene-based anodes were fabricated through a simple and scalable printing process, eliminating the need for traditional current collectors such as copper foil. The performance of the 3D anodes was characterized in terms of electrochemical properties, including capacity assessment, cycling stability, and rate capability. The results showed that the printed anodes exhibited superior performance, highlighting the potential of this approach for the development of high-performance LIBs. The findings presented in this work have significant implications for the design and manufacturing of next-generation energy storage devices.

这项工作提出了一种基于MXene(一种具有优异导电性和锂离子嵌入性能的2D材料)制造锂离子电池(lib)无电流集电极三维(3D)阳极的新方法。3D基于mxene的阳极通过简单且可扩展的打印工艺制造,消除了对铜箔等传统集流器的需求。三维阳极的电化学性能包括容量评估、循环稳定性和速率能力。结果表明,印刷阳极表现出优异的性能,突出了该方法在高性能锂离子电池开发中的潜力。这项工作的发现对下一代储能装置的设计和制造具有重要意义。
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引用次数: 0
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Electrochemistry Communications
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