Crystalline catalyst-mediated microenvironment engineering boosting CO2 electroreduction to dimethyl carbonate
Bibliographic record
Abstract
Electrochemically converting CO 2 and CH 3 OH into dimethyl carbonate (DMC) is highly desirable but challenging, as it necessitates the catalysts’ simultaneous adsorption and activation of CO 2 and CH 3 OH. Besides, a moderately dense distribution of CO 2 catalytic active site is conductive to facilitating the C–O coupling. To solve these challenges, a nano-sized polyoxometalate (POM), [{Cu 6 (μ 3 -OH) 3 (en) 3 (H 2 O) 3 }(B-α-PW 9 O 34 )]·7 H 2 O ({Cu 6 PW 9 }, en = ethylenediamine), featuring ordered {Cu 6 } cluster and {PW 9 } intervals, is synthesized for electro-production of DMC. Benefiting from the unique architecture, the pre-prepared {Cu 6 PW 9 }/Cu FA catalyst exhibits a favorable DMC yield of 2.4 mol L –1 h –1 and 83.0 % Faradaic efficiency (FE) at room temperature (–1.6 V vs. Ag/AgCl). It is also capable of exerting the catalytic activity at –15 °C. Experimental investigations illustrate that the entire {Cu 6 PW 9 } provides a negatively charged environment to adsorb alkali metal cations (AM) as a cocatalyst to assist both the adsorption and activation of the CO 2 and CH 3 OH reactants. The ordered and discrete active sites coupling with the fixed metal–metal (M–M) distance of the skeleton effectively facilitate the coupling of *CO and *OCH 3 to DMC. This study presents a crystallography-dependent catalyst design strategy for efficient synthesis of DMC under ambient and low-temperature conditions. A nano-sized polyoxometalate featuring ordered {Cu 6 } cluster and {PW 9 } intervals is synthesized for the electro-production of DMC. The discrete and fixed Cu active sites, coupling with the anionic surface of polyoxometalate effectively facilitate the coupling of *CO and *OCH 3 to DMC. This study offers a crystallography-dependent catalyst design strategy for efficient synthesis of DMC. • A crystalline-mediated microenvironment engineering strategy to drive CO 2 into dimethyl carbonate (DMC). • The {Cu 6 PW 9 }/Cu FA could simultaneously adsorb and activate CO 2 and CH 3 OH. • The uniform and discrete Cu cluster promotes C–O coupling between *CO and *OCH 3 .
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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) | 0.001 | 0.001 |
| Meta-epidemiology (broad) | 0.001 | 0.000 |
| Bibliometrics | 0.001 | 0.001 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| 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".