Fluorescent pH-Nanosensors for the in-Operando Visualization of Fast Dynamics, Interfacial pH in Electrochemical Reactions
Bibliographic record
Abstract
The in-operando visualization of interfacial pH distribution, at electrode-electrolyte interface, provides crucial insights into the mechanism and performance of many electrochemical processes. However, due to the fast dynamics and wide pH range, the spatiotemporal visualization of such interfacial pH changes requires the development of appropriate probes capable of capturing evolution of pH changes in the harsh chemical environments that normally occur in electrochemical processes. In this study, ratiometric, fluorescent, pH-sensitive nanosensors were fabricated with a wide pH measurement range (pH 3.5 to 11), for the in-operando visualisation of fast-dynamic, interfacial pH changes during an electrocoagulation process. The developed nanosensors were synthesised from the crosslinked polyacrylamide matrix, covalently linked to three pH-sensitive dyes and a reference fluorophore, to provide ratiometric nanosensors with protective but proton permeable matrix and comparable sensitivity and responsiveness to the free dyes. Using the developed nanosensors and an electrochemically coupled laser confocal fluorescence microscope, the in-operando visualization of the dynamic interfacial pH distribution during electrocoagulation of synthetic and real oil-sands produced water was achieved for the first time. The results (Figure 1) revealed the differences between the real and synthetic produced water and reflected the crucial roles of factors such as the rate of water electrolysis and chemical composition of the system on the evolution of the pH boundary layer and the interfacial pH. Overall, this study provides powerful probes (nanosensors) that can be utilized to study interfacial pH changes in a wide range of electrochemical reactions such as batteries and electrolyzers. Figure 1: Selected time series, processed images shows the differences in the interfacial pH boundary layers evolved during the electrocoagulation treatment of synthetic and real produced water. In-operando imaging was conducted using the developed nanosensors and an electrochemically coupled laser scanning confocal microscopy. Figure 1
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How this classification was reachedexpand
Full frame machine prediction
Teacher imitationNot calibrated prevalence, not ground truth. Human validation pending. The Gemma side is a direct model label for every work in the frame, read from the title-only record. The Codex side is a classifier learned from the 10,348 direct Codex labels and calibrated to design-weighted sample rates; fields without enough sample support carry no Codex call. Candidate is the union of the two sides; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels.
Distilled classifier scores by category (both heads)
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.001 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.000 | 0.001 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.001 | 0.001 |
| Insufficient payload (model declined to judge) | 0.001 | 0.000 |
Machine scores (provisional)
The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.
Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from itClassification
machine, unvalidatedMachine predicted; a candidate call from one source (direct Gemma or distilled Codex), not a consensus.
How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".