Ultrasensitive chemiluminescence detection based on titanium-doped spinel-structured nanoparticles with abundant oxygen vacancies

IF 4.3 2区化学 Q1 SPECTROSCOPY

Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy Pub Date : 2025-04-14 DOI:10.1016/j.saa.2025.126240

Yutong Liu , Hongzhan Liu , Jiyang Liu , Wenyue Gao , Wei Zhang , Guobao Xu

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引用次数: 0

Abstract

We successfully synthesized spinel-structured ternary nanocatalyst Ti-Co₃O₄/Fe₃O₄ nanoparticles (NPs) for the first time. Ti-Co₃O₄/Fe₃O₄ NPs exhibited superior catalytic performance compared to the synthesized binary catalysts Co₃O₄/Fe₃O₄. Moreover, Ti-Co₃O₄/Fe₃O₄ NPs can enhance the chemiluminescence (CL) intensity of the luminol/H₂O₂ system by over 3800-fold, attributed to the high density of oxygen vacancies (OVs) within the structure. OVs contribute to electron delocalization, improve conductivity, and are recognized as crucial active sites in the catalytic decomposition of H₂O₂. Based on the inhibitory effect of L-ascorbic acid (AA) on the luminol/H₂O₂ CL system, we developed a sensitive, rapid, effective, and highly selective AA CL assay with a linear range of 0.1 μmol/L to 100 μmol/L and a limit of detection (LOD, S/N = 3) of 0.044 μmol/L. The method was successfully applied to quantify AA in vitamin C tablets with recoveries ranging from 99.7 % to 106.3 %. This research provides a promising prospect for the application of spinel-structured nanoparticles in CL detection platforms and offers valuable insights into nanoparticle size modulation and OV engineering for catalytic optimization.

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基于富氧空位掺钛尖晶石结构纳米颗粒的超灵敏化学发光检测

首次成功合成了尖晶石结构的Ti-Co3O4/Fe3O4纳米颗粒三元纳米催化剂。与合成的Co3O4/Fe3O4二元催化剂相比，Ti-Co3O4/Fe3O4 NPs具有更好的催化性能。此外，Ti-Co3O4/Fe3O4 NPs由于结构内高密度的氧空位（OVs），可以使luminol/H2O2体系的化学发光强度提高3800倍以上。OVs有助于电子离域，提高电导率，并且被认为是催化分解H2O2的关键活性位点。基于L-抗坏血酸（AA）对鲁米诺/H2O2 CL体系的抑制作用，建立了一种灵敏、快速、有效、高选择性的AA CL测定方法，检测限（LOD, S/N = 3）为0.044 μmol/L，线性范围为0.1 μmol/L ~ 100 μmol/L。该方法可用于维生素C片中AA的定量分析，回收率为99.7% ~ 106.3%。该研究为尖晶石结构纳米颗粒在CL检测平台中的应用提供了广阔的前景，并为纳米颗粒尺寸调节和催化优化的OV工程提供了有价值的见解。

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来源期刊

Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy 物理-光谱学

CiteScore

8.40

自引率

11.40%

发文量

1364

审稿时长

40 days

期刊介绍： Spectrochimica Acta, Part A: Molecular and Biomolecular Spectroscopy (SAA) is an interdisciplinary journal which spans from basic to applied aspects of optical spectroscopy in chemistry, medicine, biology, and materials science. The journal publishes original scientific papers that feature high-quality spectroscopic data and analysis. From the broad range of optical spectroscopies, the emphasis is on electronic, vibrational or rotational spectra of molecules, rather than on spectroscopy based on magnetic moments. Criteria for publication in SAA are novelty, uniqueness, and outstanding quality. Routine applications of spectroscopic techniques and computational methods are not appropriate. Topics of particular interest of Spectrochimica Acta Part A include, but are not limited to: Spectroscopy and dynamics of bioanalytical, biomedical, environmental, and atmospheric sciences, Novel experimental techniques or instrumentation for molecular spectroscopy, Novel theoretical and computational methods, Novel applications in photochemistry and photobiology, Novel interpretational approaches as well as advances in data analysis based on electronic or vibrational spectroscopy.