electrochemical sensor

电化学传感器
  • 文章类型: Journal Article
    首次探索了钾单原子(KSA)作为增强过氧化氢(H2O2)电化学传感的传感材料。以NaCl为模板制备了具有三维多孔结构(3DNG)的N掺杂碳材料,和KSA通过高温热解固定在3DNG的表面。用TEM表征了NGKSA/3D的结构,HAADF-STEM,XPS,和XRD。电化学研究结果表明,KSA在促进H2O2电催化还原中起着至关重要的作用,不仅优化了H2O2的吸附强度,而且提高了电子转移速率。因此提高了检测H2O2的灵敏度。这项研究证明了KSA具有优异的电催化活性,为H2O2的检测提供了一种有前途的传感材料,为碱金属单原子在电化学传感领域的应用奠定了基础。
    For the first time potassium single-atoms (K SA) are explored as the sensing material to boost electrochemical sensing of hydrogen peroxide (H2O2). The N-doped carbon material with a three-dimensional porous structure (3D NG) was prepared using NaCl as the template, and K SA were anchored to the surface of 3D NG through high-temperature pyrolysis. The structure of K SA/3D NG was characterized by TEM, HAADF-STEM, XPS, and XRD. The results of electrochemical studies indicate that K SA play a crucial role in promoting the electrocatalytic reduction of H2O2, which not only optimized the adsorption strength for H2O2 but also improved the electron transfer rate, therefore improving the sensitivity for detecting H2O2. This study demonstrates the excellent electrocatalytic activity of K SA, which provides a promising sensing material for the detection of H2O2 and lays the foundation for the application of alkali metal single-atoms in the field of electrochemical sensing.
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  • 文章类型: Journal Article
    背景:独特的尺寸,物理和化学性质,纳米酶的超高稳定性在传感领域引起了广泛的关注,但是提高纳米酶的催化活性仍然是一个紧迫的问题。鉴于金属纳米粒子具有超高的模拟酶活性和多酶催化的优势,开发了整合双过氧化物酶样(POD)活性的Au修饰的MoS2纳米片(MoS2/AuNS)。
    结果:通过优化和调整AuNP的密度,以及它的形态和其他参数,获得了MoS2纳米片上AuNPs的单分散和高密度分布,可以大大提高MoS2/AuNS的POD样活性。应用Nafion溶液辅助MoS2/AuNS在电极表面改性,以提高其稳定性。利用导电Nafion溶液在SPCE上修饰MoS2/AuNS纳米酶,构建了电化学H2O2检测平台。并且带负电荷的磺酸基团可以消除带负电荷的电活性物质以提高特异性。然后用抗坏血酸刺激肿瘤细胞产生H2O2作为治疗模型,建立了细胞裂解物中H2O2的超灵敏计时容量法检测方法。ΔQ的对数和H2O2浓度的对数在1μM和500mM之间显示出良好的线性关系,LOD值为0.3μM。
    结论:开发的H2O2传感器具有出色的稳定性,重现性(RSD=2.3%,n=6)和选择性,实现了细胞裂解物中H2O2的定量检测。与用于细胞裂解物中H2O2的商业荧光检测试剂盒相比,值得一提的是,本研究开发的电化学H2O2传感器更简单、更快速,具有更高的灵敏度和更低的成本。这为基于H2O2的准确检测的疾病诊断和治疗评价提供了潜在的替代。
    BACKGROUND: The unique size, physical and chemical properties, and ultra-high stability of nanozymes have attracted extensive attentions in sensing, but improvement of catalytic activity of the nanozymes is still an urgent issue. Given the ultra-high simulated enzyme activity of metal nanoparticles and the advantage of multi-enzyme catalysis, an Au-decorated MoS2 nanosheets (MoS2/Au NS) integrating the double peroxidase-like (POD) activity is developed.
    RESULTS: By optimizing and adjusting the density of AuNPs, as well as its morphology and other parameters, a monodisperse and high-density distribution of AuNPs on MoS2 nanosheets was obtained, which can greatly improve the POD-like activity of MoS2/Au NS. Nafion solution was applied to assist the modification of MoS2/Au NS on the electrode surface so as to improved its stability. An electrochemical H2O2 detection platform was constructed by modifying MoS2/Au NS nanozyme on the SPCE using the conductive Nafion solution. And the negatively charged sulfonic acid group can eliminate negatively charged electroactive substances to improve the specificity. Then ascorbic acid was used to stimulate tumor cells to produce H2O2 as therapeutic model, an ultrasensitive chronocoulometry detection for H2O2 in cell lysate was established. The logarithmically of ΔQ and the logarithmically of H2O2 concentration showed a good linear relationship between 1 μM and 500 mM, with a LOD value of 0.3 μM.
    CONCLUSIONS: The developed H2O2 sensor has excellent stability, reproducibility (RSD = 2.3 %, n = 6) and selectivity, realized the quantitative detection of H2O2 in cell lysate. Compared with commercial fluorescence detection kits for H2O2 in cell lysate, it is worth mentioning that the electrochemical H2O2 sensor developed in this study is simpler and faster, with higher sensitivity and lower cost. This provides a potential substitute for disease diagnosis and treatment evaluation based on accurate detection of H2O2.
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  • 文章类型: Journal Article
    报道了通过质子化的精氨酸功能化的石墨烯量子点诱导的Ti3C2TX纳米片的自组装以及随后的钴(III)还原,合成了钴纳米晶体-石墨烯量子点-Ti3C2TX单片膜电极(Co-GQD-Ti3C2TX)。所得的Co-GQD-Ti3C2TX显示出良好的单片结构,机械性能,分散性和导电性。该结构实现了优异的超级电容器和感测行为。通过在柔性太阳能电池表面的背面印刷粘性Co-GQD-Ti3C2TX水凝胶而产生的自充电超级电容器提供了高比电容(在1Ag-1时为296Fg-1),高速率容量(153Fg-1,20Ag-1),容量保持率(在10,000次循环中为98.1%)和能量密度(299.9Wkg-1时为29.6Whkg-1)。通过在纸上印刷Co-GQD-Ti3C2TX水凝胶生产的电化学芯片对尿酸表现出灵敏的电化学响应。尿酸在0.01至800μM之间的增加导致差分脉冲伏安信号的线性增加,检测限为0.0032μM。集成自充电超级电容器的自供电传感平台,电化学芯片和微型电化学工作站满足于汗液中尿酸的监测,在可穿戴式电子健康监测设备中显示出广阔的应用前景。
    The synthesis of cobalt nanocrystal-graphene quantum dot-Ti3C2TX monolithic film electrode (Co-GQD-Ti3C2TX) is reported via self-assembly of Ti3C2TX nanosheets induced by protonated arginine-functionalized graphene quantum dot and subsequent reduction of cobalt (III). The resulting Co-GQD-Ti3C2TX shows good monolithic architecture, mechanical property, dispersibility and conductivity. The structure achieves excellent supercapacitor and sensing behavior. The self-charging supercapacitor produced by printing viscous Co-GQD-Ti3C2TX hydrogel on the back of flexible solar cell surface provides high specific capacitance (296 F g-1 at 1 A g-1), high-rate capacity (153 F g-1 at 20 A g-1), capacity retention (98.1% over 10,000-cycle) and energy density (29.6 W h kg-1 at 299.9 W kg-1). The electrochemical chip produced by printing Co-GQD-Ti3C2TX hydrogel on paper exhibits sensitive electrochemical response towards uric acid. The increase of uric acid between 0.01 and 800 μM causes a linear increase in differential pulse voltammetry signal with a detection limit of 0.0032 μM. The self-powered sensing platform integrating self-charging supercapacitor, electrochemical chip and micro electrochemical workstation was contentedly applied to monitoring uric acid in sweats and shows one broad application prospect in wearable electronic health monitoring device.
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  • 文章类型: Journal Article
    电化学检测有利于重金属镉的快速、灵敏测定。然而,检测灵敏度有待进一步提高,和一个便携式的,现场检测需要低成本设备。在这里,开发了一种原位铋修饰的预阳极氧化丝网印刷碳电极(SPCE),用于方波阳极溶出伏安法(SWASV)测定Cd2。原位铋修饰增强了Cd2+的富集,并与预阳极氧化一起提高了电极的电子转移速率,从而提高检测灵敏度。电极改性方法结合了预阳极氧化和原位铋沉积,这是非常容易和有效的。此外,自制的PSoCStat恒电位仪与搅拌装置相结合,用于便携式和低成本的电化学检测。经过全面优化,所开发的方法可以达到3分钟的测试时间,检测限为3.55μg/L,线性范围为5-100μg/L,水和大米样品中Cd2的回收率为91.7-107.1%。因此,我们的方法对快速,敏感和现场测定食品样品中的Cd2。
    Electrochemical detection is favorable for the rapid and sensitive determination of heavy metal cadmium. However, the detection sensitivity needs to be further improved, and a portable, low-cost device is needed for on-site detection. Herein, an in-situ bismuth modified pre-anodized screen-printed carbon electrode (SPCE) was developed for Cd2+ determination by square wave anodic stripping voltammetry (SWASV). The in-situ bismuth modification enhances the enrichment of Cd2+, and together with pre-anodization improve the electron transfer rate of electrode, thus enhancing the detection sensitivity. The electrode modification method combines pre-anodization and in-situ bismuth deposition, which is very easy and effective. Furthermore, a self-made PSoC Stat potentiostat coupled with a stirring device was fabricated for portable and low-cost electrochemical detection. After comprehensive optimization, the developed method can reach a testing time of 3 min, a detection limit of 3.55 μg/L, a linear range of 5-100 μg/L, and a recovery rate of 91.7-107.1% in water and rice samples for Cd2+ determination. Therefore, our method holds great promise for the rapid, sensitive and on-site determination of Cd2+ in food samples.
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  • 文章类型: Journal Article
    亚硝酸盐是一种常见的含氮化合物,具有很高的生物毒性,从而对水生生物构成严重威胁。因此,开发一种快速定量测定亚硝酸盐的方法势在必行。在这项研究中,目的是制备一种新型的电化学传感器来测定亚硝酸盐。这是通过在经过逐步电沉积和原位腐蚀的等离子体处理后,在碳布自支撑电极上合成Au/Zn树枝状络合物来实现的。根据最佳实验条件,电极对亚硝酸根离子(pH=8.0)的电氧化表现出显著的催化活性,与未修饰的电极相比,峰值阳极电流显着提高。该传感器具有很宽的线性范围(1-833μM,833-8330μM),高灵敏度(3506μAmM-1cm-2,538μAmM-1cm-2),低检测限(0.43μM),和优异的选择性,再现性,和稳定的亚硝酸盐的测定。此外,该传感器成功应用于自来水中亚硝酸盐的检测,鱼持有池塘水和鸭池塘水,显示良好的回收率,与分光光度结果没有显着差异。结果表明,本研究中开发的电化学传感器代表了开发用于水产养殖应用的先进便携式传感器的简单而有效的方法。
    Nitrite is a common nitrogen-containing compound that possesses high biological toxicity, thereby posing a serious threat to aquatic organisms. Therefore, it is imperative to develop a rapid and quantitative determination approach for nitrite. In this study, the aim was to prepare a novel electrochemical sensor to determine nitrite. This was achieved by synthesizing Au/Zn dendritic complexes on a carbon cloth self-supported electrode after plasma treated by a stepwise strategy of electrodeposition and in-situ corrosion. In accordance with the optimal experimental conditions, the electrode exhibited remarkable catalytic activity for the electrooxidation of nitrite ions (pH = 8.0), accompanied by a considerable enhancement in peak anodic current in comparison to the unmodified electrode. The sensor exhibited a wide linear range (1-833 μM, 833-8330 μM), high sensitivity (3506 μA mM-1 cm-2, 538 μA mM-1 cm-2), a low detection limit (0.43 μM), and excellent selectivity, reproducibility, and stability for the determination of nitrite. Furthermore, the prepared sensor was successfully applied to the detection of nitrite in tap water, fish holding pond water and duck pond water, demonstrating good recovery and no significant difference from the spectrophotometric results. The results suggest that the electrochemical sensor developed in this study represents a straightforward yet efficacious approach to the development of advanced portable sensors for aquaculture applications.
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  • 文章类型: Journal Article
    我们精心构建了一个新的氯霉素(CAP)电化学传感器,以钨酸锌@钴磁性纳米多孔碳@分子印迹聚合物(ZnWO4@Co-MNPC@MIP)为核心。首先,我们使用高效的一步水热法和直接碳化法成功制备了Co-MNPC纳米材料。接下来,我们将ZnWO4与Co-MNPC重组,并通过水热法合成了全新的ZnWO4@Co-MNPC配合物。为了进一步提高其性能,我们将ZnWO4@Co-MNPC与分子印迹聚合物结合,并通过沉淀聚合在ZnWO4@Co-MNPC的表面上涂覆了分子印迹(MIP)壳。这种外壳不仅使传感器具有新的性能,而且使其具有更强的峰值电流,从而更准确地检测CAP。在最优条件下,ZnWO4@Co-MNPC@MIP(MMIP)电极比单组分电极具有更强的CAP检测峰电流,具有相当宽的线性范围:0.007-200μM和200-1400μM。更令人惊讶的是,检测限低至0.0027μM,这使得传感器在面对各种干扰时保持优异的选择性和稳定性,使其成为优异的电化学修饰电极。与磁性非分子印迹传感器(MNIP)相比,MMIP传感器具有较高的检测效率。经过实际应用,我们发现ZnWO4@Co-MNPC@MIP修饰电极在牛奶样品中令人满意。
    We have carefully built a new chloramphenicol (CAP) electrochemical sensor, which takes the zinc tungstate @ cobalt magnetic nanoporous carbon @ molecularly imprinted polymer (ZnWO4@Co-MNPC@MIP) as the core. First, we successfully prepared Co-MNPC nanomaterials using an efficient one-step hydrothermal method and a direct carbonization method. Next, we recombined ZnWO4 with Co-MNPC and synthesized the completely new ZnWO4@Co-MNPC complex by using the hydrothermal method. To further improve its performance, we combined ZnWO4@Co-MNPC with a molecular imprinted polymer and coated a molecular imprinted (MIP) shell on the surface of ZnWO4@Co-MNPC by precipitation polymerization. This shell not only gives the sensor a new performance but also gives it a stronger peak current, resulting in a more accurate detection of CAP. Under optimal conditions, the ZnWO4@Co-MNPC@MIP (MMIP) electrode has a stronger CAP detection peak current than the one-component electrode, with a fairly wide linear range: 0.007-200 μM and 200-1400 μM. Even more surprisingly, the detection limit is as low as 0.0027 μM, which allows the sensor to maintain excellent selectivity and stability in the face of various interferences, making it an excellent electrochemically modified electrode. Compared to magnetic non-molecular imprint sensors (MNIPs), MMIP sensors have higher detection efficiency. After practical application, we found that the ZnWO4@Co-MNPC@MIP modified electrode was satisfactory in milk samples.
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  • 文章类型: Journal Article
    制备了钴纳米粒子(CoNP)官能化碳纳米管(Co@CNT)的纳米复合材料,并将其用于修饰玻碳电极(Co@CNT/GCE)。表征表明Co@CNT的形态是粘附在CNT上的CoNP。有了纳米界面,Co@CNT提供大的表面积,高催化活性,和有效的电子转移,这使得Co@CNT/GCE对槲皮素(QC)和叶酸(FA)表现出令人满意的电化学响应。检测FA和QC的最佳pH值分别为7.0和3.0。Co@CNT/GCE对QC和FA的饱和吸收能力(Γ*)和催化速率常数(kcat)计算为1.76×10-9、3.94×10-10mol•cm-2和3.04×102、0.569×102M-1•s-1。FA和QC的线性范围估计为5.0nM-10μM,LOD(3σ/s)为2.30nM和2.50nM,分别。通过Co@CNT/GCE测定的实际样品中FA和QC的含量与通过HPLC测定的结果相当。加标回收率为90.5~114%,总RSD小于8.67%,这进一步证实了所提出的电极用于实际使用的可靠性。
    A nanocomposite of cobalt nanoparticle (CoNP) functionalized carbon nanotube (Co@CNT) was prepared and used to modify a glassy carbon electrode (Co@CNT/GCE). Characterization indicates the morphology of Co@CNT is CoNPs adhering on CNTs. With the nano-interface, Co@CNT provides large surface area, high catalytic activity, and efficient electron transfer, which makes Co@CNT/GCE exhibiting satisfactory electrochemical response toward quercetin (QC) and folic acid (FA). The optimum pH values for the detection of FA and QC are 7.0 and 3.0, respectively. The saturated absorption capacity (Γ*) and catalytic rate constant (kcat) of Co@CNT/GCE for QC and FA are calculated as 1.76 × 10-9, 3.94 × 10-10 mol∙cm-2 and 3.04 × 102, 0.569 × 102 M-1∙s-1. The linear range for both FA and QC is estimated to be 5.0 nM-10 μM, and the LODs (3σ/s) were 2.30 nM and 2.50 nM, respectively. The contents of FA and QC in real samples determined by Co@CNT/GCE are comparable with the results determined by HPLC. The recoveries were in the range 90.5 ~ 114% and the total RSD was lower than 8.67%, which further confirms the reliability of the proposed electrode for practical use.
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  • 文章类型: Journal Article
    当前用于食品安全检查的分析方法需要在成本效率方面进行改进,检测速度,和易用性。传感器阵列技术已经成为一种食品安全评估方法,该方法应用多个交叉反应传感器通过模式识别来识别特定目标。当传感器阵列用纳米材料制造时,分析物与传感器的结合亲和力和传感器阵列的响应可以显着增强,从而使检测过程更加快速,敏感,而且准确。数据分析对于将来自传感器阵列的信号转换成关于分析物的有意义的信息至关重要。由于传感器阵列可以产生复杂的,响应分析物的高维数据,它们需要使用机器学习算法来降低数据的维数,以获得更可靠的结果。此外,手持智能设备的进步使得读取和分析传感器阵列信号变得更加容易,具有便利性的优点,便携性,和效率。虽然面临一些挑战,人工智能与纳米传感器阵列的集成有望增强食品安全监控。
    Current analytical methods utilized for food safety inspection requires improvement in terms of their cost-efficiency, speed of detection, and ease of use. Sensor array technology has emerged as a food safety assessment method that applies multiple cross-reactive sensors to identify specific targets via pattern recognition. When the sensor arrays are fabricated with nanomaterials, the binding affinity of analytes to the sensors and the response of sensor arrays can be remarkably enhanced, thereby making the detection process more rapid, sensitive, and accurate. Data analysis is vital in converting the signals from sensor arrays into meaningful information regarding the analytes. As the sensor arrays can generate complex, high-dimensional data in response to analytes, they require the use of machine learning algorithms to reduce the dimensionality of the data to gain more reliable outcomes. Moreover, the advances in handheld smart devices have made it easier to read and analyze the sensor array signals, with the advantages of convenience, portability, and efficiency. While facing some challenges, the integration of artificial intelligence with nanosensor arrays holds promise for enhancing food safety monitoring.
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  • 文章类型: Journal Article
    由于多年来排放有毒污染物的通量不断增加,因此设计在去污和污染物检测中具有双重适用性的材料仍然是一个艰巨的挑战。在这里,通过两步水热方法制备了负载在立方体状SrTiO3(NiFe2O4/SrTiO3)复合材料上的NiFe2O4纳米粒子,该方法提供了出色的光催化处理和废水中有毒污染物的电化学传感。通过各种表征方法对制造的复合材料的材料特性进行了详细的研究。NiFe2O4/SrTiO3杂化材料表现出19.81m2/g的高表面积,2.75eV的足够带隙能量,和突出的光致发光特性。在可见光的存在下,NiFe2O4/SrTiO3表现出深刻的光催化能力,可以在120分钟内消除含盐酸金霉素(CTCH)的污水,COD去除率为88.6%,表现优于其他纯材料。同时,废水的毒性检查,还揭示了CTCH可能的降解途径和提出的光催化机理。更重要的是,采用协同NiFe2O4/SrTiO3(NiFe2O4/SrTiO3-GCE)修饰玻碳电极,以精确定量肼(Hz)。NiFe2O4/SrTiO3-GCE在1-10mM范围内对Hz检测服从一阶响应:循环伏安:检测限(LOD)为0.119μM,灵敏度为18.9μAμM-1cm-2,线性扫描伏安:LOD为0.222μM,灵敏度为12.05μAμM-1cm-2。并对修饰电极的稳定性和干扰进行了考察。这项工作提供了宝贵的见解,以产生具有突出的S方案异质结系统的复合材料,用于猝灭电荷载流子复合,从而有助于将来实现环境净化和有毒化学检测领域。
    Devising of materials that afforded dual applicability in decontamination and pollutant detection were still a towering challenge owing to the increasing flux of discharge toxic contaminants over the years. Herein, the NiFe2O4 nanoparticles-loaded on cube-like SrTiO3 (NiFe2O4/SrTiO3) composite was fabricated by a two-step hydrothermal approach providing remarkable photocatalytic treatment and electrochemical sensing of noxious pollutants in wastewater. The material traits of the fabricated composite were scrutinized by myriad characterization approaches. The NiFe2O4/SrTiO3 hybrid material demonstrated high surface area of 19.81 m2/g, adequate band gap energy of 2.75 eV, and prominent photoluminescence characteristics. In the presence of visible light, the NiFe2O4/SrTiO3 exhibited profound photocatalysis capability to eliminate sewage effluent-bearing chlortetracycline hydrochloride (CTCH) with 88.6% COD removal in 120 min, outperforming other pure materials. Meanwhile, the toxicity examination of effluent, the possible degradation pathway of CTCH and the proposed photocatalysis mechanism were also divulged. More importantly, the glassy carbon electrode was modified with synergized NiFe2O4/SrTiO3 (NiFe2O4/SrTiO3-GCE) was adopted for the precise quantification of Hydrazine (Hz). The NiFe2O4/SrTiO3-GCE obeyed first-order response for the Hz detection within the range of 1-10 mM: cyclic voltametric: limit of detection (LOD) of 0.119 μM with sensitivity of 18.9 μA μM-1 cm-2, and linear sweep voltametric: LOD of 0.222 μM with a sensitivity of 12.05 μA μM-1 cm-2. The stability and interference of modified electrode were also inspected. This work furnished valuable insights to yield a composite with the prominent S-scheme heterojunction system for quenching of charge carrier recombination and consequently contributing to the future realization into the domains of environmental clean-up and toxic chemical detection.
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  • 文章类型: Journal Article
    脱氧雪腐镰刀菌烯醇-3-葡萄糖苷(D3G),重要的霉菌毒素脱氧雪腐镰刀菌烯醇(DON)的掩蔽形式,显示潜在的毒性,但由于缺乏快速检测方法而难以控制。在这里,开发了一种创新的基于分子印迹聚合物(MIP)的电化学传感器,用于快速检测D3G。MIP,D3G的有效识别元素,首次使用基于表面功能单体导向策略的邻苯二胺进行电聚合。同时含有Ce3+和Ce4+氧化态的CeO2,作为纳米酶被引入以催化H2O2还原,Mn掺杂产生更多的氧空位,大大提高了催化活性。Mn-CeO2由于其大的表面积和优异的导电性,也是一种有前途的衬底材料。在最优条件下,在0.01-50ng/mL的浓度范围内,D3G检测呈良好的线性关系。所提出的传感器可以检测D3G低至0.003ng/mL,具有优异的选择性,甚至在复杂样品中区分其前体DON。该传感器具有可接受的稳定性和高重现性和准确性,并能成功测定谷物样品中的D3G。据我们所知,这是第一个用于快速D3G检测的电化学传感平台,可以轻松扩展到其他被掩盖的真菌毒素。
    Deoxynivalenol-3-glucoside (D3G), the masked form of the important mycotoxin deoxynivalenol (DON), displays potential toxicity but is difficult to control owing to the lack of rapid detection methods. Herein, an innovative molecularly imprinted polymer (MIP)-based electrochemical sensor was developed for the rapid detection of D3G. MIP, an efficient recognition element for D3G, was electropolymerized using o-phenylenediamine based on a surface functional monomer-directing strategy for the first time. CeO2, which contains both Ce3+ and Ce4+ oxidation states, was introduced as a nanozyme to catalyze H2O2 reduction, while Mn doping generated more oxygen vacancies and considerably improved the catalytic activity. Mn-CeO2 also served as a promising substrate material because of its large surface area and excellent conductivity. Under optimal conditions, a good linear relationship was observed for D3G detection over the concentration range of 0.01-50 ng/mL. The proposed sensor could detect D3G down to 0.003 ng/mL with excellent selectivity, even distinguishing its precursor DON in complex samples. The sensor exhibited acceptable stability with high reproducibility and accuracy, and could successfully determine D3G in grain samples. To the best of our knowledge, this is the first electrochemical sensing platform for rapid D3G detection that can easily be expanded to other masked mycotoxins.
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