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1.
Anal Chem ; 96(1): 394-400, 2024 Jan 09.
Artigo em Inglês | MEDLINE | ID: mdl-38149960

RESUMO

The intercalation capacity of a porous electrode in real batteries is not uniform spatially due to the inevitable structural and compositional inhomogeneity and site-dependent ion and electron transport features. Reliable methods to quantify the capacity distribution are highly desirable but absent so far in battery research. In this paper, a novel optical technique, oblique incident reflection difference (OIRD), was employed to monitor in situ the electrochemical ion (de)intercalation behavior of Prussian blue analogue (PBA) porous films. The OIRD signal responded synchronously to the ion (de)intercalation, and the change in the OIRD signal (ΔI) was positively correlated with the local electrochemical capacity, thereby enabling mapping of the spatially resolved ion storage capacity of the films. Optical analysis further showed that the OIRD response originated from the ion (de)intercalation-induced dielectric constant change of PBA films. This work therefore offers an intriguing in situ and spatially resolved tool for the study of rechargeable batteries.

2.
Anal Chem ; 94(30): 10841-10849, 2022 08 02.
Artigo em Inglês | MEDLINE | ID: mdl-35863931

RESUMO

Extracellular electron transfer (EET) is a critical process involved in microbial fuel cells. Spatially resolved mapping of EET flux is of essential significance due to the inevitable spatial inhomogeneity over the bacteria/electrode interface. In this work, EET flux of a typical bioanode constructed by inhabiting Shewanella putrefaciens CN32 on a porous polyaniline (PANI) film was successfully mapped using a newly established oblique incident reflectivity difference (OIRD) technique. In the open-circuit state, the PANI film was reduced by the electrons released from the bacteria via the EET process, and the resultant redox state change of PANI was sensitively imaged by OIRD in a real-time and noninvasive manner. Due to the strong correlation between the EET flux and OIRD signal, the OIRD differential image represents spatially resolved EET flux, and the in situ OIRD signal reveals the dynamic behavior during the EET process, thus providing important spatiotemporal information complementary to the bulky electrochemical data.


Assuntos
Fontes de Energia Bioelétrica , Shewanella , Eletrodos , Transporte de Elétrons , Elétrons , Oxirredução
3.
Anal Chem ; 93(30): 10697-10703, 2021 08 03.
Artigo em Inglês | MEDLINE | ID: mdl-34282896

RESUMO

Quantitative detection of multiple biological small molecules is critical for health evaluation and disease diagnosis. In this study, a microarray chip featuring a bienzyme-immobilized polyaniline nanowire forest on fluorine-doped tin oxide (bienzyme-PANI/FTO) is developed for this purpose. On such a chip, the target molecules are oxidized under the catalysis of their attached oxidases to produce hydrogen peroxide, which further induces the partial oxidation of local PANI nanowires in the presence of horseradish peroxidase (HRP) enzyme. The redox state change of PANI nanowires is monitored by the oblique incident reflectivity difference (OIRD) technique in a real-time and wireless manner, thus allowing for quantitative analysis of the target molecules. As typical model targets, hydrogen peroxide, glucose, lactic acid, and cholesterol are successfully detected with low detection limits, excellent specificities, and broad detection ranges, all of which fully meet the requirements for clinical analysis of human serum samples. Simultaneous detection of multiple targets on an individual chip is further demonstrated using the OIRD scanning mode. Meanwhile, by simple electrochemical reduction of the PANI nanowires, the chip is reusable for more than eight detection cycles without evident decay in its performance. The detection principle of this chip is also universal to other small molecules, and thus, it shows great promise as a valuable device to analyze biological small molecules.


Assuntos
Técnicas Biossensoriais , Nanofios , Compostos de Anilina , Florestas , Humanos
4.
Lab Chip ; 23(10): 2477-2486, 2023 05 16.
Artigo em Inglês | MEDLINE | ID: mdl-37097479

RESUMO

Oblique-incidence reflectivity difference (OIRD) is a compelling technique for real-time, label-free and non-destructive detection of antibody microarray chips, but its sensitivity needs essential improvement for clinical diagnosis. In this study, we report an innovative high-performance OIRD microarray by using poly[oligo(ethylene glycol) methacrylate-co-glycidyl methacrylate] (POEGMA-co-GMA) brush grafted fluorine-doped tin oxide (FTO) as the chip substrate. The polymer brush enhances the interfacial binding reaction efficiency of targets from the complicated sample matrix due to its high antibody loading and excellent anti-fouling merits; the FTO-polymer brush layered structure, on the other hand, excites the interference enhancement effect of OIRD to achieve enhanced intrinsic optical sensitivity. Synergistically, the sensitivity of this chip is significantly improved compared to rival chips, achieving a limit of detection (LOD) as low as 25 ng mL-1 for the model target C-reactive protein (CRP) in 10% human serum. This work explores the tremendous influence of the chip interfacial structure on the OIRD sensitivity and proposes a rational interfacial engineering strategy to boost the performance of the label-free OIRD based microarray and other bio-devices.


Assuntos
Flúor , Polímeros , Humanos , Polímeros/química , Anticorpos , Análise em Microsséries/métodos
5.
Lab Chip ; 22(20): 3910-3919, 2022 10 11.
Artigo em Inglês | MEDLINE | ID: mdl-36097822

RESUMO

Oblique-incidence reflectivity difference (OIRD) is a novel optical technique for protein microarray detection with the characteristics of being real-time, label-free, high-throughput and compatible with arbitrary chip substrates. It is necessary yet challenging to improve the sensitivity of the OIRD microarray and gain a clear understanding of the enhancement mechanism for practical applications. In this study, we report a microarray chip specifically designed for OIRD to improve its sensitivity by using an electrochemically etched nanostructured fluorine-doped tin oxide (FTO) slide as the substrate. Compared with chips printed on a conventional glass slide and pristine FTO, the OIRD sensitivity and signal-to-noise ratio of this microarray are significantly improved, reaching a limit of detection (LOD) as low as 50 ng mL-1 for the streptavidin target in 10% human serum, which is one order of magnitude lower than that of the glass-based chip. On-chip ELISA and theoretical calculation reveal that the enhanced sensitivity is not only because of its higher capture efficiency towards the target, but also benefits from the optical enhancement enabled by its unique nanostructured sensing interface. This work provides a new universal strategy for designing high performance OIRD-based chips via rational interfacial engineering, thus paving the way to a label-free OIRD immunoassay and real-time analysis of biomolecular interactions.


Assuntos
Flúor , Nanoestruturas , Humanos , Imunoensaio , Incidência , Nanoestruturas/química , Estreptavidina , Compostos de Estanho
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