Optics Determines the Electrochemiluminescence Signal of Bead-Based Immunoassays

Han, Dongni; Jiang, Dechen; Valenti, Giovanni; Paolucci, Francesco; Kanoufi, Frédéric; Chaumet, Patrick C.; Fang, Danjun; Sojic, Neso

doi:10.1021/acssensors.3c01878

Cited by 8 publications

(2 citation statements)

References 80 publications

(120 reference statements)

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“…ECL peaks near the PFO when ECL intensities at clean/bare electrode regions approach their minimum value. The refractive index of PFO ( n = 1.3) is a close match to that of water, but if the ECL enhancement near the transparent oil were indeed a lens/mirror or light propagation effect, then it would be more pronounced the more light is there to be either focused or reflected. This is not the case.…”

Section: Resultsmentioning

confidence: 99%

Insulator-on-Conductor Fouling Amplifies Aqueous Electrolysis Rates

Rodriguez,

Martyniuk,

Iyer

et al. 2024

J. Am. Chem. Soc.

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The chemical industry is a major consumer of fossil fuels. Several chemical reactions of practical value proceed with the gain or loss of electrons, opening a path to integrate renewable electricity into chemical manufacturing. However, most organic molecules have low aqueous solubility, causing green and cheap electricity-driven reactions to suffer from intrinsically low reaction rates in industry's solvent of choice: water. Here, we show that a strategic, partial electrode fouling with hydrophobic insulators (oils and plastics) offsets kinetic limitations caused by poor reactant solubility, opening a new path for the direct integration of renewable electricity into the production of commodity chemicals. Through electrochemiluminescence microscopy, we reveal for the oxidation of organic reactants up to 6-fold reaction rate increase at the "fouled" oil− electrolyte−electrode interface relative to clean electrolyte−electrode areas. Analogously, electrodes partially masked (fouled) with plastic patterns, deposited either photolithographically (photoresists) or manually (inexpensive household glues and sealants), outperform clean electrodes. The effect is not limited to reactants of limited water solubility, and, for example, net gold electrodeposition rates are up to 22% larger at fouled than clean electrodes. In a system involving a surface-active reactant, rate augmentation is driven by the synergy between insulator-confined reactant enrichment and insulator-induced current crowding, whereas only the latter and possibly localized decrease in iR drop near the insulator are relevant in a system composed of non-surface-active species. Our counterintuitive electrode design enhances electrolysis rates despite the diminished area of intimate electrolyte−electrode contact and introduces a new path for upscaling aqueous electrochemical processes.

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Section: Resultsmentioning

confidence: 99%

Insulator-on-Conductor Fouling Amplifies Aqueous Electrolysis Rates

Rodriguez,

Martyniuk,

Iyer

et al. 2024

J. Am. Chem. Soc.

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“…This reactivity mapping approach provided useful insight into coreactant efficiency, [68] stability of the labels, [69] the dynamics of the ECL emission [70] and optical effects arising from the propagation of light through the bead. [71] Specifically, ECL intensity and its evolution in time are related to the electrode surface properties and the efficiency of the TPrA oxidation step. [69,70] In general, ECL emission occurs in the micrometric region (ca.…”

Section: Original Ecl Imaging Strategies For Enhanced Bioanalysismentioning

confidence: 99%

Electrochemiluminescence Microscopy

Knežević,

Han,

Liu

et al. 2024

Angewandte Chemie

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Electrochemiluminescence (ECL) is rapidly evolving from an analytical method into an optical microscopy. The orthogonality of the electrochemical trigger and the optical readout distinguishes it from classic microscopy and electrochemical techniques, owing to its near‐zero background, remarkable sensitivity, and absence of photobleaching and phototoxicity. In this review, we summarize the recent advances in ECL imaging technology, emphasising original configurations which enable the imaging of biological entities and the improvement of the analytical properties by increasing the complexity and multiplexing of bioassays. Additionally, mapping the (electro)chemical reactivity in space provides valuable information on nanomaterials and facilitates deciphering ECL mechanisms for improving their performances in diagnostics and (electro)catalysis. Finally, we highlight the recent achievements in imaging at the ultimate limits of single molecules, single photons or single chemical reactions, and the current challenges to translate the ECL imaging advances to other fields such as material science, catalysis and biology.

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Nanostructured Bubbles‐Enhanced Fluorescence for Ultrasensitive Portable MicroRNA Detection

Tang,

Xiang,

Yang

et al. 2024

Adv Funct Materials

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The unmet on‐site clinical diagnostics are increasingly demanding portable bioassays, but compromised by sensitivity and throughput. Herein, a nanostructured bubbles‐enhanced fluorescence (nBEF) assay is reported by interfacing with smartphone imaging system to enable portable, ultrasensitive, and specific miRNA detection in parallel. In nBEF, the high‐curvature bubbles allow physically enhancing optical propagation, chemically enhancing fluorescence, assembling more DNA probes, undergoing faster self‐suspension and more efficient self‐aggregation fluorescence enhancement relative to their smooth counterparts. By coupling with bubble‐driven signal amplification by a plug‐and‐play DNA concatemer, and with a smartphone imaging system, this nBEF assay achieves a portable and ultrasensitive fluorescent assay of miRNA at the femtomolar level with one‐base resolution in a single test, and is capable of monitoring drug‐induced miRNA dynamic expression and accurate cancer diagnosis (AUC = 1) through profiling 40 plasma samples after RNA extraction. This assay further integrates an R‐value analysis in RGB module with the smartphone to realize automated, on‐site miRNA readout. Such a high‐performance nBEF assay provides a low‐cost, portable, and highly sensitive tool to enable accurate clinical diagnosis.

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Optics Determines the Electrochemiluminescence Signal of Bead-Based Immunoassays

Cited by 8 publications

References 80 publications

Insulator-on-Conductor Fouling Amplifies Aqueous Electrolysis Rates

Insulator-on-Conductor Fouling Amplifies Aqueous Electrolysis Rates

Electrochemiluminescence Microscopy

Nanostructured Bubbles‐Enhanced Fluorescence for Ultrasensitive Portable MicroRNA Detection

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