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pH monitoring in high ionic concentration environments: performance study of graphene-based sensors 高离子浓度环境中的 pH 值监测:石墨烯基传感器的性能研究。
IF 1.8 4区 化学 Q3 CHEMISTRY, ANALYTICAL Pub Date : 2024-11-02 DOI: 10.1007/s44211-024-00682-9
Xin Qi, Wei Jin, Cao Tang, Xue Xiao, Rui Li, Yanqing Ma, Lei Ma

Graphene-based pH sensors, acclaimed for their exceptional sensitivity to environmental variations, have garnered significant interest in scientific research. However, the sensor performance in high ionic concentration environments is limited, due to the Debye length ion screening effect. In this study, an innovative graphene channel pH sensing device was developed and modified by cross-linked poly(methyl methacrylate) (PMMA). Furthermore, even in high ionic concentrations, the pH value can be precisely measured by this sensor. The sensor has remarkable sensitivity, and high response rate of − 70.49 mV/pH within the pH range from 7 to 10. Notably, the sensors retain uniform response direction and sensitivity under different ionic concentrations environmental and maintain consistent reversibility and stability. This advancement in sensor technology paves the way for broader applications in complex ionic environments.

Graphical abstract

Left : A graphene-based pH sensor modified with a cross-linked PMMA film; Right : Sensitivity comparison of graphene-based sensors to pH under different electrolyte concentrations. This work presents a cross-linked PMMA film-modified graphene-based pH sensor that maintains high sensitivity even in high ionic strength environments.

基于石墨烯的 pH 传感器因其对环境变化的超高灵敏度而备受赞誉,在科学研究中引起了极大的兴趣。然而,由于德拜长度离子筛选效应,传感器在高离子浓度环境中的性能受到限制。本研究开发了一种创新的石墨烯通道 pH 传感装置,并通过交联聚甲基丙烯酸甲酯(PMMA)对其进行了修饰。此外,即使在高离子浓度下,该传感器也能精确测量 pH 值。该传感器灵敏度极高,在 pH 值为 7 至 10 的范围内,响应速度高达 - 70.49 mV/pH。值得注意的是,该传感器在不同离子浓度环境下都能保持一致的响应方向和灵敏度,并能保持稳定的可逆性和稳定性。传感器技术的这一进步为在复杂离子环境中的更广泛应用铺平了道路。
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引用次数: 0
Ionic liquid applications in analytical chemistry 离子液体在分析化学中的应用。
IF 1.8 4区 化学 Q3 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-28 DOI: 10.1007/s44211-024-00668-7
Kenta Fujii
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引用次数: 0
Correction: Effect of the alkyl chain length of α,ω‑dichloroalkane on the Gibbs energy of transfer for functional groups 更正:α,ω-二氯乙烷烷基链长度对官能团转移吉布斯能的影响。
IF 1.8 4区 化学 Q3 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-22 DOI: 10.1007/s44211-024-00669-6
Kohei Uematsu, Erina Tanaka, Takanari Tanaka, Hajime Katano
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引用次数: 0
Construction of all-solid-state ion-selective sensors using electrolyte-containing polymers 利用含电解质聚合物构建全固态离子选择性传感器。
IF 1.8 4区 化学 Q3 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-17 DOI: 10.1007/s44211-024-00678-5
Hiroki Ohashi, Keisei Sowa, Yuki Kitazumi, Osamu Shirai

All-solid-state NO3, K+, NH4+, Na+, and Ca2+ ion-selective sensors (ISEs) were prepared using polyvinyl butyral (S-LEC®K KX-5). In the present case, polyvinyl butyral was used as a porous material to keep the internal solution of the respective ISE. All sensors exhibited near-Nernst responses in the concentration region between approximately 10–5 and 0.1 mol dm–3. To avoid the influence of KCl as interfering ions, MgSO4 was used as an electrolyte within the salt bridge. Although the liquid junction potential was generated, the potential difference was stabilized within about few minutes. The NO3-ISE showed high stability with no potential drift during 12 h of continuous measurements and maintained high sensitivity even after 3 weeks of storage in ultrapure water. Solidification of the internal solution is expected to make the sensor smaller and increase its mechanical strength. As an actual measurement, the sodium concentration in plasma samples using the Na+-ISE was measured to confirm agreement with literature values.

Graphical abstract

使用聚乙烯醇缩丁醛(S-LEC®K KX-5)制备了全固态 NO3-、K+、NH4+、Na+ 和 Ca2+ 离子选择性传感器(ISE)。在这种情况下,聚乙烯醇缩丁醛被用作多孔材料,以保持相应 ISE 的内部溶液。在约 10-5 至 0.1 mol dm-3 的浓度范围内,所有传感器都表现出接近于 Nernst 的响应。为了避免 KCl 作为干扰离子的影响,盐桥内使用了 MgSO4 作为电解质。虽然产生了液结电位,但电位差在几分钟内就趋于稳定。NO3--ISE 显示出很高的稳定性,在 12 小时的连续测量中没有电位漂移,即使在超纯水中存放 3 周后仍能保持很高的灵敏度。内部溶液的凝固预计会使传感器变小并增加其机械强度。在实际测量中,使用 Na+-ISE 测量了血浆样本中的钠浓度,证实与文献值一致。
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引用次数: 0
Kinetic study on bimolecular photochemical quenching of tris(2,2′-bipyridyl)ruthenium(II) complex in water–ethylene glycol binary media 水-乙二醇二元介质中三(2,2'-联吡啶)钌(II)复合物双分子光化学淬灭的动力学研究。
IF 1.8 4区 化学 Q3 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-17 DOI: 10.1007/s44211-024-00680-x
Yuki Hamano, Takuhiro Otsuka, Takeshi Higashiguchi, Nobuo Uehara, Arinori Inagawa

The bimolecular photochemical quenching of the tris(2,2′-bipyridyl)ruthenium (II) complex by ferricyanide ions in water–ethylene glycol binary media was investigated using a spectrophotometric approach, as previously reported by our research group. Time-resolved spectroscopy revealed that dynamic photochemical quenching occurred via a diffusion-dominated pathway. The static quenching process was found to occur significantly when the concentration of ethylene glycol was greater than 40 wt%. The analysis of the Stern–Volmer plots revealed that the emitters and quenchers tended to show ionic associations in water–ethylene glycol compared to our previous results with a water–glycerol binary solvent system. This is attributed to hydrophobicity, which is consistent with pioneering works that report that the addition of ethylene glycol to pure water forms hydrophobic regions, leading to dehydration of the complex ions.

Graphical abstract

根据我们研究小组之前的报告,我们采用分光光度法研究了三(2,2'-联吡啶基)钌(II)配合物在水-乙二醇二元介质中被铁氰化钾离子双分子光化学淬灭的过程。时间分辨光谱法显示,动态光化学淬灭是通过以扩散为主的途径进行的。当乙二醇的浓度大于 40 wt% 时,静态淬火过程会显著发生。对斯特恩-伏尔默图的分析表明,与我们之前在水-甘油二元溶剂系统中的结果相比,在水-乙二醇中发射体和淬灭体有呈现离子关联的趋势。这归因于疏水性,这与前人的研究结果一致,即在纯水中加入乙二醇会形成疏水区域,导致络合离子脱水。
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引用次数: 0
Aptasensor based on cascaded fluorescent sensor assisted by exonuclease III for ultra-sensitive detection of Hg2+ 基于外切酶 III 辅助级联荧光传感器的光传感器,用于超灵敏检测 Hg2。
IF 1.8 4区 化学 Q3 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-11 DOI: 10.1007/s44211-024-00677-6
Xing Liu, Zhen Liu, Yiliang Pan, Xilin Xiao

Construct a sensitive and rapid detection fluorescence biosensor with the assistance of exonuclease III to achieve efficient detection of Hg2+. Nucleic acid aptamer H0 specifically recognizes Hg2+, and under the action of exonuclease III, H0 bound to Hg2+ is hydrolyzed, which in turn fails to trigger the catalytic hairpin self-assembly amplification reaction, resulting in a decrease in the number of double-stranded DNA bound to the fluorescent dye SYBR Green I in the solution, and a decrease in the fluorescence intensity. The results showed that the concentration of Hg2+ showed a good linear relationship with the fluorescence intensity of the sensing system within the range of 3.8–10 pmol/L, and the detection limit was 0.53 pmol/L. The recoveries of Xiangjiang River water used for the analysis of the actual samples were in the range of 99.57–103.58%, and the relative standard deviations of the determined values were 2.4–3.7%. The method is simple, sensitive, specific, cost-effective and can be applied to water samples.

Graphical abstract

借助外切酶 III 构建灵敏快速的检测荧光生物传感器,实现对 Hg2+ 的高效检测。核酸适配体 H0 能特异性识别 Hg2+,在外切酶 III 的作用下,与 Hg2+ 结合的 H0 被水解,进而无法触发催化发夹自组装扩增反应,导致溶液中与荧光染料 SYBR Green I 结合的双链 DNA 数量减少,荧光强度下降。结果表明,在3.8-10 pmol/L范围内,Hg2+浓度与传感系统的荧光强度呈良好的线性关系,检测限为0.53 pmol/L。湘江水样的实际分析回收率为99.57%~103.58%,测定值的相对标准偏差为2.4%~3.7%。该方法操作简单、灵敏度高、特异性强、成本低,可用于水样分析。
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引用次数: 0
Characteristic volatile product analysis of moldy cigar wrapper and filler using gas chromatography–ion mobility spectrometry 利用气相色谱-离子迁移谱法对发霉的雪茄茄衣和茄心进行特征性挥发物分析。
IF 1.8 4区 化学 Q3 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-07 DOI: 10.1007/s44211-024-00676-7
Min Wei, Yongli Wang, Yujing Shan, Lin Rong, Ling Zhu, Min Guo, Yong Pan, Yinyu Xiang

Monitoring the changes of food products with easily applicable technique is important for the quality control of the products. Cigar wrapper and filler easily get moldy due to the existence of the native bacterial in the material and the moisture storage/production condition. Herein, we investigate the volatile compounds produced during the culture of tobacco using chromatography–ion mobility spectrometry (GC–IMS). 114 and 112 volatile compounds are determined with GC–IMS for the cultured cigar wrapper and cigar filler, respectively. Detailed fingerprint analysis and principal component analysis identify a series of compounds that can be used for the evaluation of the degree of mold development on cigar wrapper/filler. The results reported in this work may provide useful information for the quality evaluation of food products.

Graphical abstract

使用简单适用的技术监测食品的变化对于产品质量控制非常重要。由于材料中存在原生细菌以及潮湿的储存/生产条件,雪茄包装纸和填充物很容易发霉。在此,我们使用色谱-离子迁移谱法(GC-IMS)研究了烟草培养过程中产生的挥发性化合物。用 GC-IMS 测定出培养的雪茄包装纸和雪茄填充物分别含有 114 和 112 种挥发性化合物。通过详细的指纹分析和主成分分析,确定了一系列可用于评估雪茄茄衣/填充物霉菌发展程度的化合物。这项工作所报告的结果可为食品质量评估提供有用的信息。
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引用次数: 0
Fabrication of natural enzyme-covered / amino-modified Pd-Pt bimetallic-doped zeolitic imidazolate framework for ultrasensitive detection of metabolites 用于代谢物超灵敏检测的天然酶覆盖/氨基修饰钯铂双金属掺杂唑咪唑框架的制备。
IF 1.8 4区 化学 Q3 CHEMISTRY, ANALYTICAL Pub Date : 2024-10-03 DOI: 10.1007/s44211-024-00670-z
Chen-Chen Bai, Jin-ye Lang, Xin-yu Wang, Jia-meng Zhao, Lin-Yi Dong, Jun-Jie Liu, Xian-Hua Wang

The present article introduced an natural enzyme-covered/amino-modified Pd–Pt bimetallic-doped zeolitic imidazolate framework (NAPPZ) for ultrasensitive and specific detection of glucose. The dodecahedral nanomaterial zeolitic imidazolate framework (ZIF-8)-loaded Pd–Pt bimetallic nanoparticles endowed the composite with peroxidase-like activity. The modification with glucose oxidase (GOx) facilitated the rapid access of H2O2 produced through glucose oxidation to the Pd–Pt nanoparticles vicinity reducing diffusion. GOx specifically catalyzes the transformation of glucose into H2O2, which then H2O2 rapidly migrates to the Pd–Pt nanoparticles, catalyzing the oxidation of colorless o-phenylenediamine into the orange–yellow product 2,3-diaminophenazine. Based on the aforementioned cascade reaction, the NAPPZ and NAPPZ based on ChOx were utilized for detecting glucose in human urine samples and cholesterol in milk, respectively. The NAPPZ strategy presented a broad detection range (20–1100 μmol L−1) and a low detection limit (15.9 μmol L−1) for glucose, and the NAPPZ based on ChOx strategy approach offered a broad detection range (10–500 μmol L−1) and low detection limit (6.4 μmol L−1) for cholesterol. Therefore, this novel method holds significant potential in the areas of clinical diagnostics and food safety.

本文介绍了一种天然酶包被/氨基修饰的钯铂双金属掺杂唑基咪唑酸盐框架(NAPPZ),用于超灵敏特异性检测葡萄糖。十二面体纳米材料沸石咪唑酸盐框架(ZIF-8)负载的钯铂双金属纳米粒子赋予了该复合材料过氧化物酶样活性。用葡萄糖氧化酶(GOx)修饰后,通过葡萄糖氧化产生的 H2O2 可快速进入钯-铂纳米粒子,并通过还原扩散。GOx 能特异性地催化葡萄糖转化为 H2O2,然后 H2O2 快速迁移到 Pd-Pt 纳米粒子,催化无色的邻苯二胺氧化成橙黄色的产物 2,3-二氨基吩嗪。基于上述级联反应,NAPPZ 和基于 ChOx 的 NAPPZ 分别用于检测人体尿液样本中的葡萄糖和牛奶中的胆固醇。NAPPZ 方法对葡萄糖的检测范围广(20-1100 μmol L-1),检测限低(15.9 μmol L-1);基于 ChOx 的 NAPPZ 方法对胆固醇的检测范围广(10-500 μmol L-1),检测限低(6.4 μmol L-1)。因此,这种新型方法在临床诊断和食品安全领域具有巨大潜力。
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引用次数: 0
Dynamic extraction of residual solvents from pharmaceutical formulations using a needle-type extraction device 使用针式萃取装置动态萃取药物制剂中的残留溶剂。
IF 1.8 4区 化学 Q3 CHEMISTRY, ANALYTICAL Pub Date : 2024-09-28 DOI: 10.1007/s44211-024-00674-9
Ikuo Ueta, Daisuke Kondo, Suguru Masuda, Yuki Ariizumi, Ryosuke Kikuchi, Koki Nakagami, Yoshihiro Saito

This study developed a rapid screening method to determine residual solvents contained in a tablet formulation using a needle-type extraction device. For this, the tablet formulation was pulverized and the powdered sample was rapidly inserted into a pipette tip. After fixing the sample with quartz wool, the pipette tip was capped with a silicon septum. A needle-type extraction device packed with Carbopack X and a carbon molecular sieve was inserted into the pipette tip through the septum, and the gas sample was collected. During this gas sampling, pure N2 gas was introduced into the pipette tip. The extraction time for collecting 100 mL of the sample was approximately 10 min. After gas sampling, the extraction needle was connected to a gas-tight syringe and 0.5 mL of pure N2 gas (desorption gas) was collected. The extraction needle was then inserted into a heated gas chromatographic injection port. The extracted residual solvents were then thermally desorbed and determined using a gas chromatograph-flame ionization detector. The detector response is very low for carbon tetrachloride, although the proposed method showed sufficient sensitivity for five Class 1 compounds. Additionally, this study clearly indicated that the purge efficiency of residual solves with dynamic extraction is different between powdered pharmaceutical formulations.

Graphical abstract

本研究开发了一种快速筛选方法,利用针式萃取装置测定片剂配方中含有的残留溶剂。为此,先将片剂制剂粉碎,然后将粉末状样品快速插入移液器吸头。用石英棉固定样品后,用硅胶隔膜盖住移液器吸头。将装有 Carbopack X 和碳分子筛的针式萃取装置通过隔膜插入移液管吸头,收集气体样品。在气体采样过程中,将纯净的 N2 气体引入移液器顶端。收集 100 毫升样品的萃取时间约为 10 分钟。气体取样后,将萃取针连接到气密注射器上,收集 0.5 毫升纯净的 N2 气体(解吸气体)。然后将萃取针插入加热的气相色谱进样口。然后对萃取出的残留溶剂进行热解吸,并使用气相色谱仪-火焰离子化检测器进行测定。虽然拟议方法对五种 1 类化合物显示出足够的灵敏度,但四氯化碳的检测器响应非常低。此外,这项研究还清楚地表明,不同粉末状药物制剂的动态萃取对残留溶剂的净化效率是不同的。
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引用次数: 0
Analysis of methamphetamine in urine by GC/MS coupled with solid-phase dispersive extraction and solid-phase derivatization 利用气相色谱/质谱结合固相分散萃取和固相衍生化技术分析尿液中的甲基苯丙胺。
IF 1.8 4区 化学 Q3 CHEMISTRY, ANALYTICAL Pub Date : 2024-09-27 DOI: 10.1007/s44211-024-00675-8
Koichi Saito, Noriko Segawa, Rie Ito

In this study, we investigated a solid-phase dispersive extraction (SPDE) method and solid-phase derivatization method using the same solid-phase gel to extract methamphetamine (MA) from urine samples more efficiently and perform trifluoroacetic acid (TFA) derivatization for MA analysis by gas chromatography/mass spectrometry (GC/MS). N-Methylbenzylamine (NMe-BA) was added to the urine sample as a surrogate, and MA was extracted by SPDE using Oasis® HLB gel as a solid-phase agent. After drying the solid-phase gel of the SPDE, anhydrous TFA was added to the MA-absorbed HLB gel in order to derivatize MA with TFA on the solid-phase, followed by elution of the TFA derivative from this gel using ethyl acetate. As a validation of the analytical method, the limit of detection (S/N = 3) and the limit of quantification (S/N > 10) of MA were 0.002 µg/mL and 0.01 µg/mL, respectively. And the average recovery rate was 97.6–100.1%, repeatability was 5.6–10.7%, and intermediate precision was 10.1–11.4% for low (0.02 µg/mL), intermediate (0.1 µg/mL), and high (1 µg/mL) concentrations of MA added in urine. The developed pretreatment method enabled continuous extraction, cleanup, and TFA derivatization of urinary MA on the same solid-phase. Thus, urinary MA can be analyzed easily, rapidly, and with high sensitivity and accuracy.

Graphical abstract

本研究探讨了一种固相分散萃取(SPDE)方法和固相衍生化方法,使用同一种固相凝胶更有效地萃取尿样中的甲基苯丙胺(MA),并进行三氟乙酸(TFA)衍生化,用于气相色谱/质谱(GC/MS)分析甲基苯丙胺。在尿样中加入 N-甲基苄胺(NMe-BA)作为替代物,然后使用 Oasis® HLB 凝胶作为固相剂,通过 SPDE 法提取 MA。将 SPDE 的固相凝胶干燥后,向吸收了 MA 的 HLB 凝胶中加入无水 TFA,以便用 TFA 在固相上衍生 MA,然后用乙酸乙酯洗脱凝胶中的 TFA 衍生物。该分析方法的检出限(信噪比为 3)和定量限(信噪比大于 10)分别为 0.002 µg/mL 和 0.01 µg/mL。对于尿液中添加的低浓度(0.02 µg/mL)、中浓度(0.1 µg/mL)和高浓度(1 µg/mL)MA,平均回收率为97.6%-100.1%,重复性为5.6%-10.7%,中间精密度为10.1%-11.4%。所开发的预处理方法可在同一固相上对尿液中的 MA 进行连续提取、净化和 TFA 衍生。因此,尿液 MA 分析简便、快速、灵敏度高且准确。
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引用次数: 0
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Analytical Sciences
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