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关于增强抗坏血酸比色检测的一项新研究:绿色合成驱动的基于Mo(VI)/FeNPs生物传感器中氧化铁纳米颗粒的结晶度、稳定性和催化性能

A novel study on enhancing ascorbic acid colorimetric detection: Green synthesis-driven crystallinity, stability, and catalytic performance of iron oxide nanoparticles in Mo(VI)/FeNPs-based biosensors.

作者信息

Ahmouda Kaouthar, Oucif Khaled Mohammed Tayeb

机构信息

Department of Process Engineering and Petrochemistry, Faculty of Technology, University of El Oued, El Oued, 39000, Algeria; Renewable Energy Research Unit in Arid Zones, University of El Oued, El Oued, 39000, Algeria.

Department of Process Engineering and Petrochemistry, Faculty of Technology, University of El Oued, El Oued, 39000, Algeria; Renewable Energy Research Unit in Arid Zones, University of El Oued, El Oued, 39000, Algeria.

出版信息

Plant Physiol Biochem. 2025 May;222:109723. doi: 10.1016/j.plaphy.2025.109723. Epub 2025 Mar 1.


DOI:10.1016/j.plaphy.2025.109723
PMID:40056741
Abstract

The goal of this study is to investigate how the green synthesis influences the crystallinity, stability, and catalytic performance of green-synthesized iron oxide nanoparticles (FeNPs) in Mo(VI)/FeNPs-based biosensors for ascorbic acid (AA) colorimetric detection. By examining the correlation between total antioxydant capacity (TAC) and FeNPs' structural properties, phase composition, and defect levels, the study aims to establish how plant-mediated synthesis drives FeNPs' catalytic efficiency, ultimately enhancing biosensor sensitivity and lowering detection limits (LOD and LOQ). Statistical analyses, including ANOVA and Pearson correlation, are applied to validate the relationship between TAC and FeNPs' characteristics, reinforcing the role of green synthesis in enhancing biosensor performance. In this study, FTIR spectroscopy was employed to analyze unoxidized free AA groups, offering detailed insights into oxidation preferences across various Mo(VI)/FeNPs pairs. The results showed that AA was preferentially oxidized at the four biosensors with a consistent oxidation peak at 820 nm across all Mo(VI)/FeNPs pairs, with a linear correlation to AA concentrations from 0.05 to 100 mM. FTIR analysis of unoxidized AA supported these findings, revealing that AA oxidation was most efficient at Mo(VI)/ROS-FeNPs and Mo(VI)/ARM-FeNPs biosensors compared to Mo(VI)/JUN-FeNPs and Mo(VI)/MAT-FeNPs. Likewise, the highest sensitivity, reflected by the lowest LOD (0.01183 ± 0.00116 mM and 0.01521 ± 0.00187) and LOQ (0.0393 ± 0.00386 mM and 0.0506 ± 0.00623), was observed in Mo(VI)/ROS-FeNPs and Mo(VI)/ARM-FeNPs, whereas Mo(VI)/JUN-FeNPs and Mo(VI)/MAT-FeNPs exhibited higher LOD (0.03237 ± 0.00318 mM and 0.03550 ± 0.00348) and LOQ (0.107887 ± 0.01058 mM and 0.11834 ± 0.01159), confirming the impact of FeNPs' catalytic performance on detection sensitivity. One-way ANOVA analysis confirmed that these variations in LOD (F = 42.7, p < 0.0001) and LOQ (F = 58.3, p < 0.0001) were statistically significant (p < 0.05), indicating that intrinsic properties of FeNPs strongly influence the catalytic performance of the biosensors. Post-hoc Tukey's test revealed that FeNPs synthesized with extracts of higher TAC, such as Rosmarinus officinalis and Artemisia herba-alba, achieved significantly lower LOD and LOQ values compared to those prepared with Juniperus phoenicia and Matricaria pubescens extracts, signifying superior catalytic performance. The catalytic performances of FeNPs in AA oxidation are closely linked to their stability and crystallinity. XRD analysis revealed that higher-TAC extracts, like Rosmarinus officinalis and Artemisia herba-alba, yielded FeNPs with minor defects, with a greater percentage of the γ - FeO phase, indicating enhanced stability and crystallinity. In contrast, extracts with lower TAC, such as Juniperus phoenicia and Matricaria pubescens, produced FeNPs with more defects, with a higher percentage of the α - FeO phase. Statistical analysis of ANOVA and Pearson correlation confirmed a significant influence of TAC on FeNPs' phase composition (F = 89.3, p = 0.002), with a strong positive correlation to γ - FeO (r = 0.99, p = 0.004) and a negative correlation to α - FeO (r = -0.99, p = 0.004). These results highlight the role of TAC in promoting γ - FeO formation, enhancing FeNPs' stability and crystallinity. This emphasizes that high TAC contributes to improved stability and crystallinity, and thereby enhances AA oxidation by driving FeNPs' catalytic performance in Mo(VI)/FeNPs biosensors.

摘要

本研究的目的是探究绿色合成如何影响基于钼(VI)/铁纳米颗粒(FeNPs)的生物传感器中绿色合成的氧化铁纳米颗粒(FeNPs)的结晶度、稳定性及催化性能,用于抗坏血酸(AA)的比色检测。通过研究总抗氧化能力(TAC)与FeNPs的结构性质、相组成及缺陷水平之间的相关性,本研究旨在确定植物介导的合成如何驱动FeNPs的催化效率,最终提高生物传感器的灵敏度并降低检测限(LOD和LOQ)。应用包括方差分析(ANOVA)和皮尔逊相关性分析在内的统计分析方法来验证TAC与FeNPs特性之间的关系,强化绿色合成在提高生物传感器性能方面的作用。在本研究中,采用傅里叶变换红外光谱(FTIR)分析未氧化的游离AA基团,深入了解不同钼(VI)/FeNPs对之间的氧化偏好。结果表明,在所有钼(VI)/FeNPs对中,AA在四个生物传感器上优先被氧化,在820 nm处有一致的氧化峰,与0.05至100 mM的AA浓度呈线性相关。对未氧化AA的FTIR分析支持了这些发现,表明与钼(VI)/JUN - FeNPs和钼(VI)/MAT - FeNPs相比,AA在钼(VI)/ROS - FeNPs和钼(VI)/ARM - FeNPs生物传感器上的氧化效率最高。同样,钼(VI)/ROS - FeNPs和钼(VI)/ARM - FeNPs表现出最高的灵敏度,最低检测限(LOD)为(0.01183±0.00116 mM和0.01521±0.00187),定量限(LOQ)为(0.0393±0.00386 mM和0.0506±0.00623),而钼(VI)/JUN - FeNPs和钼(VI)/MAT - FeNPs表现出更高的LOD(0.03地37±0.00318 mM和0.03550±0.00348)和LOQ(0.107887±0.01058 mM和0.11834±0.01159),证实了FeNPs的催化性能对检测灵敏度的影响。单向方差分析证实,这些LOD(F = 42.7,p < 0.0001)和LOQ(F = 58.3,p < 0.0001)的差异具有统计学意义(p < 0.05),表明FeNPs的固有性质强烈影响生物传感器的催化性能。事后Tukey检验表明,用总抗氧化能力较高的提取物(如迷迭香和苦艾)合成的FeNPs与用腓尼基刺柏和毛母菊提取物制备的FeNPs相比,实现了显著更低的LOD和LOQ值,表明具有卓越的催化性能。FeNPs在AA氧化中的催化性能与其稳定性和结晶度密切相关。X射线衍射(XRD)分析表明,总抗氧化能力较高的提取物(如迷迭香和苦艾)产生的FeNPs缺陷较少,γ - FeO相的百分比更高,表明稳定性和结晶度增强。相比之下,总抗氧化能力较低的提取物(如腓尼基刺柏和毛母菊)产生的FeNPs缺陷更多,α - FeO相的百分比更高。方差分析(ANOVA)和皮尔逊相关性的统计分析证实了总抗氧化能力对FeNPs相组成有显著影响(F = 89.3,p = 0.002),与γ - FeO呈强正相关(r = 0.99,p = 0.G04),与α - FeO呈负相关(r = -0.99,p = 0.004)。这些结果突出了总抗氧化能力在促进γ - FeO形成、增强FeNPs稳定性和结晶度方面的作用。这强调高总抗氧化能力有助于提高稳定性和结晶度,从而通过驱动钼(VI)/FeNPs生物传感器中FeNPs的催化性能来增强AA氧化。

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