Efficient hydrogen evolution from sodium borohydride catalysed by amine-decorated cross-linked polymer immobilised ionic liquid stabilised palladium nanoparticles
Bibliographic record
Abstract
Palladium nanoparticles (PdNP) stabilised by confinement in crosslinked amine-decorated, polymer-immobilised ionic liquids (PIILs) catalyse the hydrolytic evolution of hydrogen from NaBH 4 under mild conditions. A series of three PIIL supports NH 2 -Im x PIIL ( x = 1, (2a); x = 2, (2b); x = 3, (2c), where x corresponds to the number of imidazolium cations in the repeat unit) were prepared with an increasing number of imidazolium cations such that bis(styryl)-based crosslinkers 1a and 1b contain one and two imidazolium cations, respectively, while 1c is a more extensive tris(styryl)-based crosslinker with three imidazolium cations. The composition of the support influences the performance of the corresponding polymer immobilised ionic liquid stabilised (PIILS) palladium nanoparticles, PdNP@NH 2 -Im x PIILS ( x = 1, (4a); x = 2, (4b); x = 3, (4c)) as catalysts for the hydrolysis of NaBH 4 and a comparison of the most efficient system against its unmodified counterpart (i.e., PdNP@H-Im 2 PIILS) confirmed that incorporation of the surface coordinated amine improved catalyst performance. Palladium nanoparticles stabilised by NH 2 -Im 2 PIIL was the most efficient catalyst and the maximum initial turnover frequency of 81 mol H2 molPd −1 min −1 is higher than the 59 and 32 mol H2 molPd −1 min −1 obtained with PdNPs supported by NH 2 -Im 1 PIIL and NH 2 -Im 3 PIIL, respectively, as well as the 19 mol H2 molPd −1 min −1 obtained with commercial 10 wt.% Pd/C. The results of kinetic studies, apparent activation energies, and deuterium isotope effects have been compared with those in the literature and support a mechanism involving rate-limiting activation of an O–H bond in water. Catalyst reuse studies showed that PdNP@NH 2 -Im 2 PIILS recycled with remarkable efficiency as high conversions were maintained across five runs with the catalyst retaining over 92% of its initial activity, an improvement on the 70% retention of activity with palladium nanoparticles supported by linear amine-modified imidazolium-based polymer, which demonstrates the beneficial effect of introducing crosslinking.
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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 | 0.000 |
| 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 | 0.000 |
| Open science | 0.001 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.002 | 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".