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CRISPR/Cas12a-Powered Gold/Nickel Foam Surface-Enhanced Raman Spectroscopy Biosensor for Nucleic Acid specific Detection in foods 用于食品中特定核酸检测的 CRISPR/Cas12a 动力金/镍泡沫表面增强拉曼光谱生物传感器
IF 4.2 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-17 DOI: 10.1039/d4an00778f
Yan Liu, Shi rui Gou, Long Qiu, Zhi wen Xu, Shiping Yang, Haifeng Yang, Yu Zhao
Food is a necessary source of energy, but it also serve as a pathway for transmitting infectious pathogens, making food safety a matter of great concern. Rapid, accurate, and specific detection methods for foodborne viruses are crucial. Surface Enhanced Raman Scattering (SERS), due to its superior sensitivity and characteristic fingerprint spectra, holding enormous potential. However, due to the limitations of SERS, it requires specific conditions to achieve specificity. In order to enhance the specificity and accuracy of nucleic acid detection based on SERS, we have developed a CRISPR-Cas12a mediated SERS technique to identify target DNA harnessing the targeting recognition capability of CRISPR-Cas12a and ultra-sensitive SERS tags. Successfully addressing SERS for its lack of specific detection capability. This system includes a c gold/nickel foam substrate(Au-NFs) and a reporter (ssDNA-ROX). The qualitative and quantitative analysis of target DNA in drinking water was performed by monitoring the intensity change of Rox Raman reporter molecules. The results showed that the sensor detected DNA within 30min and the limit of detection (LOD) was 8.23fM. It is expected to become one of the alternative methods for nucleic acid detection for its rapid detection and high-specificity.
食物是人体必需的能量来源,但同时也是传染病病原体的传播途径,因此食品安全问题备受关注。针对食源性病毒的快速、准确和特异性检测方法至关重要。表面增强拉曼散射(SERS)因其卓越的灵敏度和特征指纹光谱而具有巨大的潜力。然而,由于 SERS 的局限性,它需要特定的条件才能达到特异性。为了提高基于 SERS 的核酸检测的特异性和准确性,我们开发了一种 CRISPR-Cas12a 介导的 SERS 技术,利用 CRISPR-Cas12a 的靶向识别能力和超灵敏 SERS 标签来识别目标 DNA。成功解决了 SERS 缺乏特异性检测能力的问题。该系统包括金/镍泡沫基底(Au-NFs)和报告物(ssDNA-ROX)。通过监测 Rox 拉曼报告分子的强度变化,对饮用水中的目标 DNA 进行了定性和定量分析。结果表明,该传感器能在 30 分钟内检测到 DNA,检测限 (LOD) 为 8.23fM。由于其检测速度快、特异性高,有望成为核酸检测的替代方法之一。
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引用次数: 0
The stray light induced redshift of absorption peaks of inorganic anions in the far ultraviolet region-an "artifact". 杂散光导致无机阴离子在远紫外区的吸收峰发生红移--这是一种 "伪影"。
IF 3.6 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-16 DOI: 10.1039/d4an00400k
Jun Ma, Ning Duan, Fuyuan Xu, Ke Xiao

In the analytical process of spectrophotometry, the prerequisite for accurate qualitative and quantitative analysis is obtaining the intrinsic spectra of the analyte. However, the intrinsic properties of spectra can sometimes be masked by easily overlooked non-intrinsic factors, such as those from measuring instruments, leading to erroneous spectral identification. In this study, we documented an unusual redshift phenomenon in the far ultraviolet spectral region. With a spectrophotometer under the nitrogen atmosphere, we selected 14 representative inorganic anions and investigated their absorption spectral behaviors at different optical pathlengths and concentrations. It was intriguing to observe that the absorption peaks with maximum absorption wavelengths below a watershed wavelength of 200 nm underwent a redshift as pathlength and concentration increased, while those above 200 nm did not exhibit a significant redshift phenomenon. In-depth formula simulations and experimental verifications demonstrated that this peculiar spectral behavior was caused by unavoidable stray light in the spectrophotometer. Some methodological and instrumental recommendations are given in the paper. Our study results may serve as a reminder to carefully identify non-intrinsic phenomena when studying absorption spectra in the far ultraviolet region, and provide guidance on spectral corrections in scientific research and practical applications.

在分光光度法的分析过程中,准确定性和定量分析的前提是获得被分析物的固有光谱。然而,光谱的固有特性有时会被测量仪器等容易被忽视的非固有因素所掩盖,从而导致错误的光谱鉴定。在这项研究中,我们记录了远紫外光谱区的一种不寻常的红移现象。我们利用氮气环境下的分光光度计,选择了 14 种具有代表性的无机阴离子,研究了它们在不同光程和浓度下的吸收光谱行为。有趣的是,随着光程和浓度的增加,最大吸收波长在分水岭波长 200 nm 以下的吸收峰发生了红移,而 200 nm 以上的吸收峰则没有明显的红移现象。深入的公式模拟和实验验证表明,这种特殊的光谱行为是由分光光度计中不可避免的杂散光造成的。文中给出了一些方法和仪器方面的建议。我们的研究结果可以提醒人们在研究远紫外区吸收光谱时仔细识别非本征现象,并为科学研究和实际应用中的光谱校正提供指导。
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引用次数: 0
A Novel NIR Fluorescent Probe for Visualizing Hydrogen Sulfide in Alzheimer's Disease 用于观察阿尔茨海默病中硫化氢的新型近红外荧光探针
IF 4.2 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-16 DOI: 10.1039/d4an00819g
Sai Hong, Yabing Gan, Dian Liu, Ting Yu, Huijun Zhou, Haitao Li, Feng Liu, Peng Yin
Alzheimer's disease (AD) represents a devastating form of neurodegeneration, hallmarked by a relentless erosion of memory and cognitive faculties. One key player in this complex pathology is hydrogen sulfide (H2S), a gaseous neurotransmitter that is highly concentrated in the brain. Its fluctuating levels have been compellingly linked to the onset and progression of AD. Despite the availability of numerous fluorescent probes for detecting H2S, targeted imaging of this neurotransmitter within AD models remains underexplored. To bridge this gap, we have engineered an innovative near-infrared (NIR) "turn-on" fluorescent probe, designated as Probe 1. Crafted around a dicyanoisophorone scaffold, the probe incorporates a strategic methoxy modification to facilitate a bathochromic spectral shift. Impressively, upon binding with H2S, Probe 1 exhibited a robust 46-fold enhancement in fluorescence at a wavelength of 680 nm. We successfully deployed this probe to visualize both exogenous and endogenous H2S in living cells and zebrafish. Further, our pathogenic investigations have corroborated that diminished H2S levels are intricately linked to an escalation in amyloid plaque formation. Most crucially, we employed probe 1 to capture real-time images of H2S concentrations within the hippocampal tissue of AD mouse models. This revealed a significant depletion in H2S levels, thereby underscoring the probe's immense potential as an effective tool for the diagnosis and prevention of Alzheimer's disease.
阿尔茨海默病(AD)是一种破坏性的神经变性,其特征是记忆和认知能力的无情侵蚀。硫化氢(H2S)是这一复杂病理过程中的一个关键因素,它是一种高度集中在大脑中的气态神经递质。硫化氢水平的波动与注意力缺失症的发病和进展有着密切的联系。尽管目前已有许多检测 H2S 的荧光探针,但在 AD 模型中对这种神经递质的靶向成像研究仍然不足。为了弥补这一不足,我们设计了一种创新的近红外(NIR)"开启 "荧光探针,命名为探针 1。该探针以二氰异佛尔酮为支架,并结合了战略性的甲氧基修饰,以促进浴色光谱偏移。令人印象深刻的是,探针 1 与 H2S 结合后,在 680 纳米波长处的荧光增强了 46 倍。我们成功地利用这种探针在活细胞和斑马鱼体内检测外源和内源 H2S。此外,我们的病理研究证实,H2S 水平的降低与淀粉样斑块的形成密切相关。最重要的是,我们利用探针1捕获了AD模型小鼠海马组织内H2S浓度的实时图像。这显示了 H2S 水平的显著下降,从而凸显了探针作为诊断和预防阿尔茨海默病有效工具的巨大潜力。
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引用次数: 0
Ultrasensitive detection of the H5N1 nucleic acid fragment by ICP-MS using DNA dendrimer-carried silver nanoparticle labeling. 利用 DNA 树枝形分子携带的银纳米粒子标记,通过 ICP-MS 超灵敏检测 H5N1 核酸片段。
IF 3.6 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-15 DOI: 10.1039/d4an00746h
Chao Huang, Yanni Jiao, Lijun Shao, Wei Li, Shengyong Ding, Dafeng Jiang, Wei Jiang

The importance of avian influenza virus (AIV) detection in clinical diagnosis and prognosis has been deeply recognized. In this study, the ultrasensitive detection of AIV subtype H5N1 was achieved by ICP-MS combined with DNA dendrimer-carried silver nanoparticle (AgNP) labeling. First, a magnetic control system was constructed by anchoring double-strand DNAs (dsDNAs) which contained a complementary sequence of H5N1 and two locked triggers on the surface of magnetic beads (MBs). When H5N1 was present, the two triggers were released and initiated dendrimer hybridization chain reactions which led to the generation of DNA dendrimer-carried AgNPs on the surface of the MBs. Finally, the AgNPs were collected via magnetic separation, digested by nitric acid, and tested using ICP-MS. The signal intensities of 107Ag were positively correlated with the concentrations of H5N1. Notably, the DNA dendrimer assembly contributed to significant signal amplification and good sensitivity with the limit of detection as low as 2.0 × 10-11 mol L-1. Moreover, the method displayed favorable selectivity against mismatched H5N1 and good recoveries in human serum samples. It is a promising analytical tool for the H5N1 virus and other subtypes of AIV, and has potential value in clinical diagnosis and prognosis of infectious diseases.

禽流感病毒(AIV)检测在临床诊断和预后判断中的重要性已得到广泛认可。本研究采用 ICP-MS 结合 DNA 树枝状分子载体银纳米粒子(AgNP)标记技术,实现了对 H5N1 亚型禽流感病毒的超灵敏检测。首先,通过在磁珠(MBs)表面锚定含有 H5N1 互补序列和两个锁定触发器的双链 DNA(dsDNAs),构建了一个磁性控制系统。当 H5N1 出现时,两个触发器被释放并引发树枝状聚合物杂交链反应,从而在 MB 表面生成 DNA 树枝状聚合物携带的 AgNPs。最后,通过磁性分离收集 AgNPs,用硝酸消化,并使用 ICP-MS 进行检测。107Ag 的信号强度与 H5N1 的浓度呈正相关。值得注意的是,DNA 树枝状聚合物的组装有助于显著的信号放大和良好的灵敏度,检测限低至 2.0 × 10-11 mol L-1。此外,该方法对不匹配的 H5N1 具有良好的选择性,在人血清样本中的回收率也很高。对于 H5N1 病毒和其他亚型的 AIV 病毒,该方法是一种很有前途的分析工具,在传染病的临床诊断和预后方面具有潜在价值。
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引用次数: 0
Estimation of biological variance in coherent Raman microscopy data of two cell lines using chemometrics. 利用化学计量学估算两种细胞系相干拉曼显微镜数据中的生物方差。
IF 3.6 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-15 DOI: 10.1039/d4an00648h
Rajendhar Junjuri, Matteo Calvarese, MohammadSadegh Vafaeinezhad, Federico Vernuccio, Marco Ventura, Tobias Meyer-Zedler, Benedetta Gavazzoni, Dario Polli, Renzo Vanna, Italia Bongarzone, Silvia Ghislanzoni, Matteo Negro, Juergen Popp, Thomas Bocklitz

Broadband Coherent Anti-Stokes Raman Scattering (BCARS) is a valuable spectroscopic imaging tool for visualizing cellular structures and lipid distributions in biomedical applications. However, the inevitable biological changes in the samples (cells/tissues/lipids) introduce spectral variations in BCARS data and make analysis challenging. In this work, we conducted a systematic study to estimate the biological variance in BCARS data of two commonly used cell lines (HEK293 and HepG2) in biomedical research. The BCARS data were acquired from two different experimental setups (Leibniz Institute of Photonics Technology (IPHT) in Jena and Politecnico di Milano (POLIMI) in Milano) to evaluate the reproducibility of results. Also, spontaneous Raman data were independently acquired at POLIMI to validate those results. First, Kramers-Kronig (KK) algorithm was utilized to retrieve Raman-like signals from the BCARS data, and a pre-processing pipeline was subsequently used to standardize the data. Principal component analysis - Linear discriminant analysis (PCA-LDA) was performed using two cross-validation (CV) methods: batch-out CV and 10-fold CV. Additionally, the analysis was repeated, considering different spectral regions of the data as input to the PCA-LDA. Finally, the classification accuracies of the two BCARS datasets were compared with the results of spontaneous Raman data. The results demonstrated that the CH band region (2770-3070 cm-1) and spectral data in the 1500-1800 cm-1 region have significantly contributed to the classification. A maximum of 100% balanced accuracies were obtained for the 10-fold CV for both BCARS setups. However, in the case of batch-out CV, it is 92.4% for the IPHT dataset and 98.8% for the POLIMI dataset. This study offers a comprehensive overview for estimating biological variance in biomedical applications. The insights gained from this analysis hold promise for improving the reliability of BCARS measurements in biomedical applications, paving the way for more accurate and meaningful spectroscopic analyses in the study of biological systems.

宽带相干反斯托克斯拉曼散射(Broadband Coherent Anti-Stokes Raman Scattering,BCARS)是生物医学应用中观察细胞结构和脂质分布的重要光谱成像工具。然而,样品(细胞/组织/脂质)中不可避免的生物变化会在 BCARS 数据中引入光谱变化,从而使分析变得具有挑战性。在这项工作中,我们进行了一项系统研究,以估计生物医学研究中常用的两种细胞系(HEK293 和 HepG2)的 BCARS 数据中的生物变异。BCARS 数据来自两个不同的实验装置(耶拿莱布尼兹光子技术研究所(IPHT)和米兰理工大学(POLIMI)),以评估结果的可重复性。此外,还在 POLIMI 独立获取了自发拉曼数据,以验证这些结果。首先,利用克雷默-克罗尼格(KK)算法从 BCARS 数据中检索拉曼类信号,随后使用预处理管道对数据进行标准化处理。主成分分析-线性判别分析(PCA-LDA)采用两种交叉验证(CV)方法进行:批量交叉验证和 10 倍交叉验证。此外,考虑将数据的不同光谱区域作为 PCA-LDA 的输入,重复进行了分析。最后,将两个 BCARS 数据集的分类准确度与自发拉曼数据的结果进行了比较。结果表明,CH 波段区域(2770-3070 cm-1)和 1500-1800 cm-1 区域的光谱数据对分类有显著贡献。两种 BCARS 设置的 10 倍 CV 均获得了最高 100%的平衡准确度。但是,在批量输出 CV 的情况下,IPHT 数据集的准确率为 92.4%,POLIMI 数据集的准确率为 98.8%。本研究为估算生物医学应用中的生物方差提供了一个全面的概述。从本分析中获得的见解有望提高生物医学应用中 BCARS 测量的可靠性,为在生物系统研究中进行更准确、更有意义的光谱分析铺平道路。
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引用次数: 0
Outstanding Reviewers for Analyst in 2023. 2023 年分析师杰出评审员。
IF 3.6 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-15 DOI: 10.1039/d4an90050b

We would like to take this opportunity to thank all of Analyst reviewers for helping to preserve quality and integrity in the chemical science literature. We would also like to highlight our Outstanding Reviewers for Analyst in 2023.

我们想借此机会感谢《分析家》的所有审稿人,感谢他们帮助维护化学科学文献的质量和完整性。此外,我们还想重点介绍 2023 年《分析》杂志的杰出审稿人。
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引用次数: 0
Corrective protocol to predict interference free sensor response for paper-based solution sampling coupled with heavy metal sensitive ion-selective electrodes. 用于预测纸基溶液采样与重金属敏感离子选择电极耦合的无干扰传感器响应的校正协议。
IF 3.6 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-15 DOI: 10.1039/d4an00841c
Mingpeng Yang, Rochelle Silva, Ke Zhao, Ruiyu Ding, Jit Loong Cyrus Foo, Liya Ge, Grzegorz Lisak

Paper-based microfluidics combined with potentiometric measurement has emerged as an attractive approach for detecting various chemical ionic moieties. Detection of heavy metal ions, using paper substrates as solution sampling and delivery systems remains challenging despite efforts to introduce several physico-chemical paper substrate modifications to stop adsorption of ions onto the paper substrates. This study quantitatively investigates the adsorption of heavy metal ions on the paper substrates during paper-based potentiometric measurements and explains the super-Nernstian response of potentiometric sensors through local depletion of heavy metal ions from the solution. Consequently, based on the investigated ion adsorption, a corrective potential protocol was established for the electrodes coupled with paper-based solution sampling by predicting interference free sensor response from paper-based measurement. Furthermore, the ion adsorption was also recorded for mixed metal ion solutions to understand competitive primary/interfering ions adsorption onto the paper substrates and establish corrective measures to predict interference free sensor response. In this method, no modifications of the paper substrates are necessary before actual potentiometric measurements. The proposed corrective protocol allows prediction of sensor response based on the paper-based solution sampling potentiometric measurement, providing a simple methodological approach based on correction of potential readout of the potentiometric sensor, thus completely resigning from the need of modifying paper substrate for measurements of heavy metal ions.

纸基微流体技术与电位测量相结合,已成为检测各种化学离子分子的一种极具吸引力的方法。使用纸基质作为溶液取样和传输系统检测重金属离子仍然具有挑战性,尽管人们努力对纸基质进行了多种物理化学改性,以阻止离子吸附到纸基质上。本研究定量研究了纸基电位计测量过程中重金属离子在纸基上的吸附情况,并通过溶液中重金属离子的局部耗竭解释了电位计传感器的超纳斯特响应。因此,根据所研究的离子吸附情况,通过预测纸基测量的无干扰传感器响应,为与纸基溶液采样相结合的电极建立了校正电位协议。此外,还记录了混合金属离子溶液的离子吸附情况,以了解纸基底上的竞争性主离子/干扰离子吸附情况,并制定校正措施来预测无干扰传感器响应。在这种方法中,实际电位测量前无需对纸基底进行任何修改。所提出的纠正方案允许根据纸基溶液取样电位测量来预测传感器响应,提供了一种基于电位传感器电位读数纠正的简单方法,从而完全摆脱了在测量重金属离子时修改纸基的需要。
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引用次数: 0
Phenotyping of single plant cells on a microfluidic cytometry platform with fluorescent, mechanical and electrical modules 在带荧光、机械和电子模块的微流体细胞仪平台上对单个植物细胞进行表型分析
IF 4.2 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-15 DOI: 10.1039/d4an00682h
Shuaihua Zhang, Tianjiao Zhang, Shuaiqi Wang, Ziyu Han, Xuexin Duan, Jiehua Wang
Compared to animal cells, phenotypic characterization of single plant cells on microfluidic platforms is still rare. In this work, we performed population statistics on the morphological, biochemical, physical and electrical properties of Arabidopsis protoplasts under different external and internal conditions, using progressively improved microfluidic platforms. First, we analyzed the different effects of three phytohormones (auxin, cytokinin and gibberellin) on the primary cell wall (PCW) regeneration process using a microfluidic flow cytometry platform equipped with a single-channel fluorescence sensor. Second, we correlated the intracellular reactive oxygen species (ROS) level induced by heavy metal stress with the concurrent PCW regeneration process by using a dual-channel fluorescence sensor. Third, by integrating compression channels, we were able to effectively discriminate variations in cell size while monitoring the intensity of intracellular ROS signaling. Fourth, by combining an electrical impedance electrode with the compression channel, we analyzed the differences in electrical and mechanical properties of wild-type and mutant plant cells before and after primary cell wall regeneration. Overall, our work demonstrates the feasibility and sensitivity of microfluidic flow cytometry in high-throughput phenotyping of plant cells and provides a reference for assessing metabolic and physiological indicators of individual plant cells in multiple dimensions.
与动物细胞相比,在微流控平台上对单个植物细胞进行表型鉴定的情况还很少见。在这项工作中,我们利用逐步改进的微流控平台,对拟南芥原生质体在不同内外条件下的形态、生化、物理和电学特性进行了群体统计。首先,我们利用配备单通道荧光传感器的微流体流式细胞仪平台,分析了三种植物激素(辅助素、细胞分裂素和赤霉素)对原生细胞壁(PCW)再生过程的不同影响。其次,我们利用双通道荧光传感器将重金属胁迫诱导的细胞内活性氧(ROS)水平与同时进行的 PCW 再生过程相关联。第三,通过整合压缩通道,我们能够在监测细胞内 ROS 信号强度的同时有效区分细胞大小的变化。第四,通过将电阻抗电极与压缩通道相结合,我们分析了野生型和突变型植物细胞在原生细胞壁再生前后的电学和机械特性差异。总之,我们的工作证明了微流控流式细胞仪在植物细胞高通量表型分析中的可行性和灵敏度,为多维度评估单个植物细胞的代谢和生理指标提供了参考。
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引用次数: 0
Insights into the terahertz response of L-Glutamic acid and its receptor 透视 L-谷氨酸及其受体的太赫兹响应
IF 4.2 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-12 DOI: 10.1039/d4an00697f
Yu Wu, zhongjie zhu, Jinrong Yang, Jie Wang, Te Ji, Huachun Zhu, Weiwei Peng, Min Chen, Hongwei Zhao
L-Glutamic acid (L-Glu) is the basic unit of proteins and also serves as an important neurotransmitter in the central nervous system, its structural properties are critical for the biological function and selective receptor recognition. Although the molecule has been extensively studied, the low frequency vibrational behavior that is closely related to the conformational changes, and the intermolecular interactions between L-Glu and its receptors are still unclear. In this study, we acquired the fingerprint spectrum of L-Glu by using air plasma terahertz (THz) time-domain spectroscopy in the 0.5-18 THz range. The low frequency vibrational characteristics of L-Glu were investigated through density functional theory (DFT) calculations. The THz responses of ligand binding domain of NMDAR-L-Glu complex were studied by ONIOM method, with a focus on discussing the normal modes and interactions of ligand L-Glu and water molecules. The results illustrate that THz spectroscopy exhibits a sensitive response to the influence of L-Glu on the structure of NMDAR. The water molecules in protein have various strong vibration modes in the THz band, showing specificity and diversity and complexity of vibrational behavior. There is a potential for influencing and regulating the structural stability of NMDAR-L-Glu complex through water molecules.
谷氨酸(L-Glu)是蛋白质的基本单位,也是中枢神经系统中一种重要的神经递质,其结构特性对生物功能和选择性受体识别至关重要。尽管对该分子进行了广泛的研究,但与构象变化密切相关的低频振动行为以及 L-Glu 与其受体之间的分子间相互作用仍不清楚。在这项研究中,我们利用空气等离子体太赫兹(THz)时域光谱技术获得了 L-Glu 在 0.5-18 THz 范围内的指纹谱。通过密度泛函理论(DFT)计算研究了 L-Glu 的低频振动特性。利用 ONIOM 方法研究了 NMDAR-L-Glu 复合物配体结合域的太赫兹响应,重点讨论了配体 L-Glu 与水分子的法向模式和相互作用。结果表明,太赫兹光谱对 L-Glu 对 NMDAR 结构的影响具有灵敏的响应。蛋白质中的水分子在太赫兹波段具有各种强振动模式,显示出振动行为的特异性、多样性和复杂性。有可能通过水分子影响和调节 NMDAR-L-Glu 复合物的结构稳定性。
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引用次数: 0
Understanding Electrocatalytic Mechanisms and Ultra-Trace Uranyl Detection with Pd Nanoparticles Electrodeposited in Deep Eutectic Solvents 了解在深共晶溶剂中电解沉积钯纳米粒子的电催化机制和超痕量铀检测技术
IF 4.2 3区 化学 Q2 CHEMISTRY, ANALYTICAL Pub Date : 2024-07-12 DOI: 10.1039/d4an00788c
Arkaprava Layek, Sushil M Patil, Ruma Gupta, Priya Yadav, Kavitha Jayachandran, Dilip Kumar Maity, N CHOUDHURY
This research investigates the electrocatalytic mechanisms and ultra-trace detection abilities of uranyl ions (UO₂²⁺) using palladium nanoparticles (PdNPs) electrodeposited in deep eutectic solvents (DESs). The unique properties of DESs, such as their adjustable viscosity and ionic conductivity, offer an advantageous and environmentally friendly medium for Pd nanoparticle electrodeposition, resulting in highly active and stable electrocatalysts. Various characterization techniques, including scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and X-ray diffraction (XRD), were used to examine the morphology, size distribution, and crystallographic structure of the Pd nanoparticles. Electrochemical tests revealed that the Pd-modified electrodes show exceptional electrocatalytic activity and current sensitivity towards uranyl ions, with detection limits as low as 3.4nM. Density functional theory (DFT) calculations were conducted to elucidate the mechanism of the electrocatalytic reduction of UO₂²⁺ by the PdNPs, providing a plausible explanation for the high sensitivity of PdNPs in detecting uranyl ions based on the calculated structural parameters and reaction energetics. This study underscores the potential of Pd nanoparticles electrodeposited in DESs as a promising method for sensitive uranyl ion detection, contributing to advancements in environmental monitoring and nuclear safety.
本研究利用在深共晶溶剂(DESs)中电沉积的钯纳米粒子(PdNPs)研究铀酰离子(UO₂²⁺)的电催化机制和超痕量检测能力。深共晶溶剂(DESs)的独特性质,如可调节的粘度和离子导电性,为钯纳米粒子的电沉积提供了有利的环境友好型介质,从而产生了高活性、高稳定性的电催化剂。研究人员采用了多种表征技术,包括扫描电子显微镜(SEM)、X 射线光电子能谱(XPS)和 X 射线衍射(XRD),对钯纳米粒子的形态、尺寸分布和晶体结构进行了研究。电化学测试表明,Pd 改性电极对铀酰离子具有优异的电催化活性和电流灵敏度,检测限低至 3.4nM。通过密度泛函理论(DFT)计算,阐明了 PdNPs 电催化还原 UO₂²⁺的机理,并根据计算得出的结构参数和反应能量,为 PdNPs 检测铀酰离子的高灵敏度提供了合理的解释。这项研究强调了电沉积在 DESs 中的钯纳米粒子作为一种灵敏的铀离子检测方法的潜力,有助于推进环境监测和核安全。
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