Electrochemically Triggered Dynamics within a Hybrid Metal–Organic Electrocatalyst
Bibliographic record
Abstract
A wide array of systems, ranging from enzymes to synthetic catalysts, exert adaptive motifs to maximize their functionality. In a related manner, select metal–organic frameworks (MOFs) and similar systems exhibit structural modulations under stimuli such as the infiltration of guest species. Probing their responsive behavior in situ is a challenging but important step toward understanding their function and subsequently building functional systems. In this report, we investigate the dynamic behavior of an electrocatalytic Mn–porphyrin-containing MOF system (Mn-MOF). We discover, using a combination of electrochemistry and in situ probes of UV–vis absorption, resonance Raman, and infrared spectroscopy, a restructuration of this system via a reversible cleavage of the porphyrin carboxylate ligands under an applied voltage. We further show, by combining experimental data and DFT calculations, as a proof of concept, the capacity to utilize the Mn-MOF for electrochemical CO2 fixation and to spectroscopically capture the reaction intermediates in its catalytic cycle. The findings of this work and the methodology developed open opportunities in the application of MOFs as dynamic, enzyme-inspired electrocatalytic systems.
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How this classification was reachedexpand
Full frame distilled prediction
Teacher imitationNot calibrated prevalence, not ground truth. Human validation pending. Learned from the 10,348 direct Codex labels and 10,348 direct Gemma labels. Candidate is the union of thresholded teacher heads; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels or direct frontier model labels.
Codex and Gemma teacher scores by category
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.001 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.001 | 0.001 |
| Bibliometrics | 0.000 | 0.001 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.002 | 0.000 |
| Research integrity | 0.000 | 0.001 |
| Insufficient payload (model declined to judge) | 0.000 | 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 teacher head, 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".