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Investigation of the modification of gold electrodes by electrochemical molecularly imprinted polymers as a selective layer for the trace level electroanalysis of PAH 将电化学分子印迹聚合物修饰金电极作为多环芳烃痕量电分析选择层的研究
IF 4.7 3区 工程技术 Q2 ELECTROCHEMISTRY Pub Date : 2024-11-12 DOI: 10.1016/j.elecom.2024.107837
Farah Ibrahim , Alexandre Sala , Armand Fahs , Aoife Morrin , Clément Nanteuil , Guillaume Laffite , Ian A. Nicholls , Fiona Regan , Hugues Brisset , Catherine Branger
Electrochemical molecularly imprinted polymers (e-MIPs) were grafted for the first time as a thin layer to the surface of a gold electrode to perform trace level electroanalysis of benzo(a)pyrene (BaP). This was achieved by controlled/living radical photopolymerization of a redox tracer monomer (ferrocenylmethyl methacrylate, FcMMA) with ethylene glycol dimethacrylate in the presence of benzo(a)pyrene as the template molecule. For that purpose, a novel photoiniferter-derived SAM was first deposited on the gold surface. The SAM formation was monitored by cyclic voltammetry and electrochemical impedance spectroscopy. Then, the “grafting from” of the e-MIP was achieved upon photoirradiation during a controlled time. Differential pulse voltammetry was used to quantify BaP in aqueous solution by following the modification of the signal of FcMMA. A limit of detection of 0.19 nM in water and a linear range of 0.66 nM to 4.30 nM, were determined, thus validating the enhancement of sensitivity induced by the close contact between the e-MIP and the electrode, and the improved transfer electron.
电化学分子印迹聚合物(e-MIPs)首次以薄层形式接枝到金电极表面,用于苯并(a)芘(BaP)的痕量电分析。这是通过氧化还原示踪单体(甲基丙烯酸二茂铁甲基酯,FcMMA)与乙二醇二甲基丙烯酸酯在苯并芘作为模板分子存在的情况下进行受控/活自由基光聚合实现的。为此,首先在金表面沉积了一种新型光增感剂衍生的 SAM。通过循环伏安法和电化学阻抗谱监测了 SAM 的形成。然后,在可控时间内进行光照射,实现 e-MIP 的 "接枝"。通过跟踪 FcMMA 信号的变化,使用差分脉冲伏安法对水溶液中的 BaP 进行定量。结果表明,在水中的检测限为 0.19 nM,线性范围为 0.66 nM 至 4.30 nM,从而验证了 e-MIP 与电极之间的紧密接触和电子转移的改进提高了灵敏度。
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引用次数: 0
In-situ solvothermal synthesis of free-binder NiCo2S4/nickel foam electrode for supercapacitor application: Effects of CTAB surfactant 用于超级电容器的自由粘合剂 NiCo2S4/ 镍泡沫电极的原位溶热合成:CTAB 表面活性剂的影响
IF 4.7 3区 工程技术 Q2 ELECTROCHEMISTRY Pub Date : 2024-11-12 DOI: 10.1016/j.elecom.2024.107838
A.R. Sarbishei, S.M. Masoudpanah, M. Hasheminiasari, S.A. Sanei
The free-binder NiCo2S4/nickel foam electrode was prepared using a two-step solvothermal method: double-layered hydroxide formation and sulfurization. The effects of cetyltrimethylammonium bromide (CTAB) on the structural, microstructural, and electrochemical properties throughout the sulfurization process were investigated using various characterization techniques. By adding the CTAB surfactant, the sheetlike morphology of NiCo2S4 material was transformed to a fine particular morphology. Using one mmol CTAB surfactant, the specific capacitance of NiCo2S4/nickel foam increased from 578 to 835 C g−1 due to the downsizing of particles, inducing the higher electroactive sites for redox reactions. An asymmetric capacitor of NiCo2S4 as positive and CuCo2S4 as negative electrodes demonstrated an energy density of 23.2 Wh kg−1 at a power density of 5040 W kg−1.
采用两步溶热法制备了自由粘合剂 NiCo2S4/泡沫镍电极:双层氢氧化物形成和硫化。在整个硫化过程中,采用各种表征技术研究了十六烷基三甲基溴化铵(CTAB)对结构、微观结构和电化学性能的影响。加入 CTAB 表面活性剂后,NiCo2S4 材料的片状形态转变为精细的特殊形态。在使用 1 mmol CTAB 表面活性剂的情况下,由于颗粒变小,NiCo2S4/镍泡沫的比电容从 578 C g-1 增加到 835 C g-1,从而产生了更高的氧化还原反应电活性位点。以 NiCo2S4 为正极、CuCo2S4 为负极的不对称电容器在功率密度为 5040 W kg-1 时的能量密度为 23.2 Wh kg-1。
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引用次数: 0
Corrosion of nickel foam electrodes during hydrothermal reactions: The influence of a simple protective carbon black coating 水热反应过程中泡沫镍电极的腐蚀:简单碳黑保护层的影响
IF 4.7 3区 工程技术 Q2 ELECTROCHEMISTRY Pub Date : 2024-11-10 DOI: 10.1016/j.elecom.2024.107835
Gillian Collins , Tara N. Barwa , Luke Glennon , P. Rupa Kasturi , Carmel B. Breslin
Nickel foam (NF) substrates are widely used to support electrocatalysts, and this is frequently achieved using hydrothermal reactions, where the NF is immersed in the hydrothermal reactor together with the electrocatalyst precursors. However, other reactions including the corrosion of the NF and changes to the pH occur simultaneously, and these can affect the quality of the final electrocatalyst. Herein, a simple approach is devised to minimise these unwanted reactions. Carbon black (CB) was non-covalently functionalised at room temperature using tannic acid to give very stable and good dispersions of fCB in deionised water. Using a simple sonication step, the NF was coated with a uniform layer of the dispersed fCB. This layer served to minimise the corrosion of the underlying NF during the hydrothermal reactions with very good protection observed up to a temperature of 160 °C in deionised water at a pH of 2.0. The corrosion currents of the NF and fCB@NF were estimated at 8.7 µA and 3.9 µA, respectively, at room temperature in this acidic solution. Using a model reaction, the successful nucleation and growth of MnCo2O4 cubes was observed at fCB@NF, but not at the corroding NF.
泡沫镍(NF)基材被广泛用于支持电催化剂,这通常是通过水热反应来实现的,即把 NF 与电催化剂前体一起浸入水热反应器中。然而,同时还会发生其他反应,包括 NF 的腐蚀和 pH 值的变化,这些都会影响最终电催化剂的质量。在此,我们设计了一种简单的方法来尽量减少这些不必要的反应。使用单宁酸在室温下对炭黑(CB)进行非共价官能化,从而在去离子水中得到非常稳定和良好的 fCB 分散体。通过一个简单的超声步骤,就能在 NF 上涂上一层均匀分散的 fCB。在 pH 值为 2.0、温度高达 160 °C 的去离子水中,这层涂层可以最大程度地减少水热反应过程中对下层 NF 的腐蚀,起到很好的保护作用。在室温下的酸性溶液中,NF 和 fCB@NF 的腐蚀电流估计分别为 8.7 µA 和 3.9 µA。利用模型反应,在 fCB@NF 上观察到了 MnCo2O4 立方体的成功成核和生长,但在腐蚀 NF 上却没有观察到。
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引用次数: 0
Low-power and cost-effective readout circuit design for compact semiconductor gas sensor systems 用于紧凑型半导体气体传感器系统的低功耗、高性价比读出电路设计
IF 4.7 3区 工程技术 Q2 ELECTROCHEMISTRY Pub Date : 2024-11-07 DOI: 10.1016/j.elecom.2024.107834
Soon-Kyu Kwon , Jun-Nyeong Kim , Hyung-Gi Byun , Hyeon-June Kim
This study introduces a novel readout circuit architecture that enhances semiconductor gas sensor systems by reducing power consumption, enabling miniaturization, and improving economic viability. Validated at the PCB level, the design shows strong commercial potential by addressing power efficiency and signal accuracy challenges. The technology is adaptable for applications in environmental monitoring, industrial safety, and medical diagnostics, where efficient and reliable gas sensing is essential.
本研究介绍了一种新型读出电路结构,通过降低功耗、实现微型化和提高经济可行性来增强半导体气体传感器系统。经过 PCB 层面的验证,该设计通过解决能效和信号精度方面的难题,显示出强大的商业潜力。该技术可应用于环境监测、工业安全和医疗诊断等对高效可靠的气体传感至关重要的领域。
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引用次数: 0
Fabrication of patterned TiO2 nanotube layers utilizing a 3D printer platform and their electrochromic properties 利用 3D 打印机平台制造图案化 TiO2 纳米管层及其电致变色特性
IF 4.7 3区 工程技术 Q2 ELECTROCHEMISTRY Pub Date : 2024-11-02 DOI: 10.1016/j.elecom.2024.107833
Kwang-Mo Kang , Seok-Han Lee , Sang-Youn Kim , Yoon-Chae Nah
Anodization enables nano-structure fabrication through electrochemical parameter control. While various approaches exist for creating localized or patterned oxide layers, many are complex and time-consuming. This study adopted a commercial 3D printer for high-speed (1 mm/s) anodization, forming TiO2 nanotube layers on Ti substrates in G-code-designed patterns. Comprehensive characterization using XRD, SEM, XPS, and simulated electric field distribution analysis revealed well-defined nanostructures and provided insights into the formation mechanism. Furthermore, viologen-anchored TiO2 showed significantly improved electrochromic performance compared to pristine TiO2, with a higher reflectance difference (46.2% vs. 6.85%). This 3D printing-anodization hybrid method offers a rapid approach to fabricating patterned TiO2 nanostructures, showing promise for electrochromic devices with enhanced optical modulation capabilities.
阳极氧化可通过电化学参数控制制造纳米结构。虽然有多种方法可以制造局部或图案化的氧化层,但许多方法都很复杂且耗时。本研究采用商用 3D 打印机进行高速(1 毫米/秒)阳极氧化,在钛基底上以 G 代码设计的图案形成 TiO2 纳米管层。利用 XRD、SEM、XPS 和模拟电场分布分析进行的综合表征揭示了定义明确的纳米结构,并提供了对形成机制的见解。此外,与原始二氧化钛相比,紫胶锚定二氧化钛的电致变色性能有了显著提高,反射率差异更大(46.2% 对 6.85%)。这种三维打印-阳极氧化混合方法提供了一种快速制造图案化二氧化钛纳米结构的方法,为具有更强光学调制能力的电致变色设备带来了希望。
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引用次数: 0
Wirefree Electrochemistry for Enhanced Detection and Treatment of Disease 用于增强疾病检测和治疗的免接线电化学技术
IF 4.7 3区 工程技术 Q2 ELECTROCHEMISTRY Pub Date : 2024-11-02 DOI: 10.1016/j.elecom.2024.107832
Oisín Foley Doyle , Robert J. Forster
Wirefree, or bipolar electrochemistry, BPE, has the potential to transform patient outcomes through early diagnosis using ultrasensitive sensors for multiple biomarkers and personalised treatments such as enhanced cell growth, differentiation and destruction as well as local delivery of therapeutics. We highlight the emerging field of wirefree electroceuticals and show how BPE could enable precise modulation of neural circuits, non-pharmaceutical therapies for conditions like Parkinson’s disease and chronic pain management, as well as on-demand drug delivery with high spatial and temporal precision. Moreover, it explores the integration of advanced nanomaterials illustrating their pivotal role in enhancing electrode performance and biocompatibility, thereby maximising their potential diagnostic and therapeutic efficacy especially in vivo.
无导线电化学或双极电化学(BPE)有可能通过使用超灵敏传感器对多种生物标志物进行早期诊断,并提供个性化治疗,如增强细胞生长、分化和破坏以及局部给药,从而改变患者的治疗效果。我们重点介绍了新兴的无导线电疗领域,并展示了 BPE 如何实现对神经回路的精确调节、对帕金森病和慢性疼痛治疗等疾病的非药物疗法,以及高空间和时间精度的按需给药。此外,报告还探讨了先进纳米材料的集成,说明了它们在提高电极性能和生物相容性方面的关键作用,从而最大限度地发挥其潜在的诊断和治疗功效,尤其是在体内。
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引用次数: 0
The influence of acetone and isopropanol crossover on the direct isopropanol fuel cell 丙酮和异丙醇交叉对直接异丙醇燃料电池的影响
IF 4.7 3区 工程技术 Q2 ELECTROCHEMISTRY Pub Date : 2024-10-21 DOI: 10.1016/j.elecom.2024.107823
Dominik Venus , Moritz Valeske , Matthew Brodt , Peter Wasserscheid , Simon Thiele
Liquid organic hydrogen carriers (LOHC) offer a promising option to store and release hydrogen on demand within existing infrastructure. The direct isopropanol fuel cell (DIFC) uses the electrochemical acetone/isopropanol LOHC couple and combines the advantages of high fuel energy density at ambient conditions with CO2-free direct electricity production. Like other alcohol fuel cells, the DIFC combines two kinetically slow reactions, the isopropanol oxidation reaction (IOR) and the oxygen reduction reaction (ORR), requiring considerable overpotentials to drive the reactions. Accordingly, deconvoluting kinetic characteristics in the full cell is difficult. Therefore, this work uses the electrolytic electrochemical dehydrogenation unit (EDU), consisting of the IOR and the kinetically fast hydrogen evolution reaction in acidic media. This EDU then serves as an IOR full-cell model to get insights on the DIFC. Correspondingly, the demonstrated work is a comparison study investigating in-house fabricated catalyst-coated membrane electrode assemblies as hydrogen fuel cells, DIFC, and EDU. It investigates characteristic features of the DIFC and demonstrates how the acetone and isopropanol crossover affect the cathode of the DIFC.
液态有机氢载体(LOHC)为在现有基础设施内按需储存和释放氢气提供了一种前景广阔的选择。直接异丙醇燃料电池(DIFC)使用电化学丙酮/异丙醇液态有机氢载体偶联物,将环境条件下的高燃料能量密度与无二氧化碳直接发电的优势结合在一起。与其他酒精燃料电池一样,DIFC 结合了两个动力学速度较慢的反应,即异丙醇氧化反应(IOR)和氧还原反应(ORR),需要相当大的过电位来驱动反应。因此,很难对整个电池的动力学特性进行分解。因此,这项研究采用了电解电化学脱氢单元(EDU),由酸性介质中的 IOR 和动力学快速氢进化反应组成。然后,该 EDU 可作为 IOR 全电池模型来深入了解 DIFC。相应地,展示的工作是对内部制造的催化剂涂层膜电极组件作为氢燃料电池、DIFC 和 EDU 进行比较研究。它研究了 DIFC 的特征,并展示了丙酮和异丙醇交叉如何影响 DIFC 的阴极。
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引用次数: 0
Highly enhanced electrocatalytic OER with facile electrodeposition of MIL–53(Fe)/NiAl–LDH/NF and NiAl–LDH/MIL–53(Fe)/NF 利用 MIL-53(Fe)/NiAl-LDH/NF 和 NiAl-LDH/MIL-53(Fe)/NF 的简易电沉积高度增强电催化 OER
IF 4.7 3区 工程技术 Q2 ELECTROCHEMISTRY Pub Date : 2024-10-15 DOI: 10.1016/j.elecom.2024.107825
Afsaneh Ahmadi , Mohammad Chahkandi , Mahboobeh Zargazi , Jin Suk Chung
This research investigates a new approach to improve the electrocatalytic rate of the Oxygen Evolution Reaction (OER), a key step in water electrolysis. The study focuses on two promising materials: MIL–53(Fe) and NiAl–LDH. MIL–53(Fe) offers several advantages: high catalytic activity, large surface area, and good chemical stability. NiAl–LDH is attractive due to its layered structure, tolerance to a wide range of pH levels, scalability, and cost-effectiveness. However, their limitations like low conductivity and restricted accessibility of active sites hinder their performance in water splitting applications. To address these limitations, novel composite thin films were created using a technique called layer–by–layer (LBL) electrophoretic deposition. These films, built on nickel foam (NF) substrates, included two configurations: MIL–53(Fe)/NiAl–LDH/NF and NiAl–LDH/MIL–53(Fe)/NF. The MIL-53(Fe)/NiAl-LDH/NF composite exhibited remarkable OER activity in alkaline electrolytes, requiring overpotentials of only 200, 270, and 370 mV to reach current densities of 20, 50, and 100 mA cm−2, respectively. The Tafel slope of 54.86 mVdec−1 suggests rapid reaction kinetics. Additionally, it demonstrated excellent long-term stability, lasting for at least 20 h. The success of the MIL–53(Fe)/NiAl–LDH/NF composite can be attributed to the LBL technique. This method creates a composite with a larger surface area, significantly improving OER efficiency. In contrast, the MIL–53(Fe)/NiAl–LDH/NF configuration had the opposite effect. The NF pores became blocked by the MIL–53(Fe) layer, reducing the overall surface area, hindering electron transfer, and thereby limiting oxygen production. The LBL deposition method used in this study proves its effectiveness in designing efficient electrocatalysts. This opens up possibilities for creating other multicomponent materials for energy applications. The findings provide valuable insights for future research on these promising composite materials, potentially leading to the development of cost-effective and high-performance catalysts for various electrochemical applications.
这项研究探讨了一种提高氧进化反应(OER)电催化率的新方法,氧进化反应是水电解过程中的一个关键步骤。研究重点是两种有前途的材料:MIL-53(Fe) 和 NiAl-LDH。MIL-53(Fe) 具有几个优点:催化活性高、表面积大、化学稳定性好。NiAl-LDH 因其层状结构、对多种 pH 值的耐受性、可扩展性和成本效益而具有吸引力。然而,它们的局限性,如低电导率和活性位点访问受限,阻碍了它们在水分离应用中的性能。为了解决这些局限性,我们采用一种称为逐层(LBL)电泳沉积的技术制作了新型复合薄膜。这些薄膜建立在泡沫镍(NF)基底上,包括两种结构:MIL-53(Fe)/NiAl-LDH/NF和NiAl-LDH/MIL-53(Fe)/NF。在碱性电解质中,MIL-53(Fe)/NiAl-LDH/NF 复合材料表现出显著的 OER 活性,只需要 200、270 和 370 mV 的过电位就能分别达到 20、50 和 100 mA cm-2 的电流密度。54.86 mVdec-1 的塔菲尔斜率表明反应动力学速度很快。MIL-53(Fe)/NiAl-LDH/NF 复合材料的成功归功于 LBL 技术。这种方法能使复合材料具有更大的表面积,从而显著提高 OER 效率。相比之下,MIL-53(Fe)/NiAl-LDH/NF 配置则产生了相反的效果。NF 孔隙被 MIL-53(Fe)层阻塞,减少了整体表面积,阻碍了电子传递,从而限制了氧气的产生。本研究中使用的 LBL 沉积方法证明了其在设计高效电催化剂方面的有效性。这为创造其他多组分能源应用材料提供了可能性。这些发现为今后研究这些前景广阔的复合材料提供了宝贵的启示,有可能为各种电化学应用开发出具有成本效益的高性能催化剂。
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引用次数: 0
Novel and simple electrochemical sensing platform based on polypyrrole nanotubes/ZIF-67 nanocomposite/screen printed graphite electrode for sensitive determination of metronidazole 基于聚吡咯纳米管/ZIF-67 纳米复合材料/丝网印刷石墨电极的新型简便电化学传感平台,用于灵敏测定甲硝唑
IF 4.7 3区 工程技术 Q2 ELECTROCHEMISTRY Pub Date : 2024-10-12 DOI: 10.1016/j.elecom.2024.107824
Somayeh Tajik , Hadi Beitollahi , Fariba Garkani Nejad
Here, a simple, fast, and sensitive voltammetric sensor based on screen printed graphite electrode (SPGE) modified with polypyrrole nanotubes/zeolitic imidazolate framework-67 (PPy NTs/ZIF-67) nanocomposite is introduced for the metronidazole (MNZ) determination. The PPy NTs/ZIF-67 nanocomposite was synthesized and characterized by using X-ray diffraction (XRD) spectroscopy, field emission scanning electron microscopy (FE-SEM), and energy-dispersive X-ray spectroscopy (EDS) techniques. The developed sensor based on PPy NTs-ZIF-67 nanocomposite modified SPGE shows an obvious reduction peak at −650 mV for MNZ, mainly due to the synergistic effects of the ZIF-67 and PPy NTs. Differential pulse voltammetry (DPV) was found to be the most suitable method for MNZ detection, showing a linear dynamic range of 0.01–500.0 µM and a low limit of detection (LOD) of 0.004 µM. In investigating the practicability, the PPy NTs/ZIF-67/SPGE sensor demonstrated efficient practicability with satisfactory recoveries (97.1 % to 103.5 %) and low relative standard deviation (RSD) values of 1.8–3.6 % for MNZ determination in MNZ tablets and urine samples.
本文介绍了一种基于丝网印刷石墨电极(SPGE)和聚吡咯纳米管/唑基咪唑啉框架-67(PPy NTs/ZIF-67)纳米复合材料修饰的简单、快速、灵敏的伏安传感器,用于甲硝唑(MNZ)的测定。利用 X 射线衍射(XRD)光谱、场发射扫描电子显微镜(FE-SEM)和能量色散 X 射线光谱(EDS)技术合成了 PPy NTs/ZIF-67 纳米复合材料,并对其进行了表征。所开发的基于 PPy NTs-ZIF-67 纳米复合材料修饰的 SPGE 传感器在 -650 mV 处对 MNZ 有明显的还原峰,这主要是由于 ZIF-67 和 PPy NTs 的协同作用。研究发现,差分脉冲伏安法(DPV)是最适合检测 MNZ 的方法,其线性动态范围为 0.01-500.0 µM,检出限(LOD)低至 0.004 µM。在实用性研究中,PPy NTs/ZIF-67/SPGE 传感器在 MNZ 药片和尿样中的 MNZ 检测中表现出高效的实用性,回收率令人满意(97.1 % 至 103.5 %),相对标准偏差 (RSD) 值低至 1.8 % 至 3.6 %。
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引用次数: 0
Monitoring spirooxazine–merocyanine photoisomerization with ion-current rectifying quartz nanopipettes 用离子电流整流石英纳米吸头监测螺嗪-猩红嗪光异构化过程
IF 4.7 3区 工程技术 Q2 ELECTROCHEMISTRY Pub Date : 2024-10-05 DOI: 10.1016/j.elecom.2024.107820
Emer B. Farrell, Gareth Redmond, Robert P. Johnson
The characterization and discrimination of chemical compounds is imperative in both academia and industry, but currently relies on expensive and/or bulky instrumentation. Herein, we demonstrate that the ion transport properties of bare quartz nanopipettes containing aprotic acetonitrile electrolyte can be used discriminate isomers based on polarization and solvation, through changes to interfacial solvent ordering at the nanopore wall. This is demonstrated by monitoring the photoinduced isomerization of spirooxazine to merocyanine using the ion-current rectification of a quartz-nanopipette containing acetonitrile electrolyte, which results in an increase in rectification ratio (RR) from 3.6 ± 0.3 to 5.1 ± 0.2. This change is comparable to traditional UV–Vis absorbance and fluorescence measurements of the same process, with the appearance of a small shoulder-like absorbance peak from 400 to 500 nm, and a strong fluorescence signal at 430 nm.
对化合物进行表征和鉴别是学术界和工业界的当务之急,但目前依赖于昂贵和/或笨重的仪器。在本文中,我们证明了含有沸腾乙腈电解液的裸石英纳米吸头的离子传输特性,可以通过改变纳米孔壁的界面溶剂有序性,根据极化和溶解来分辨异构体。通过使用含有乙腈电解液的石英纳米吸头的离子电流整流来监测光诱导螺嗪向美罗菁华的异构化,结果显示整流比(RR)从 3.6 ± 0.3 增加到 5.1 ± 0.2。这一变化可与传统的紫外可见吸光度和荧光测量相媲美,在同一过程中,400 至 500 纳米波长处会出现一个小的肩状吸光度峰,430 纳米波长处会出现一个强烈的荧光信号。
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引用次数: 0
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Electrochemistry Communications
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