Hydroxyl-mediated interfacial oxophilicity engineering for efficient CO2-to-C2+ oxygenates conversion at industrial current densities
Bibliographic record
Abstract
Electrocatalytic CO 2 reduction (eCO 2 RR) to multi-carbon (C 2+ ) products is a promising pathway for renewable energy storage and carbon neutrality. However, selectively steering the reaction toward high-value C 2+ oxygenates, rather than ethylene, remains a major challenge due to the intertwined reaction pathways following the initial C–C coupling step. Herein, we propose a hydroxyl-mediated interfacial oxophilic engineering strategy to selectively stabilize oxygenated intermediates and promote their directional transformation into C 2+ oxygenates. In situ spectroscopic analyses and DFT calculations reveal that hydroxyl species preferentially anchor at low-coordinated Cu sites at the Cu/Cu 2 O interface, creating a locally oxophilic and chemically asymmetric microenvironment. This interfacial hydroxyl layer not only stabilizes Cu δ+ species under high current densities but also promotes the retention of *OCCHO and *CHO-like intermediates, while disfavoring their deoxygenation to ethylene. As a result, the catalyst achieves a C 2+ oxygenates Faradaic efficiency of 68% at an industrially relevant current density of 200 mA cm -2 in a 5 cm 2 membrane electrode assembly. This work highlights the critical role of interfacial oxophilicity in governing product selectivity and offers a generalizable design principle for constructing high-performance eCO 2 RR catalysts that break the traditional trade-off between C–C coupling efficiency and product selectivity. Hydroxyl-mediated Cu/Cu 2 O interfaces create a locally oxophilic, chemically asymmetric microenvironment, stabilizing Cu δ+ species and selectively retaining oxygenated intermediates (*OCCHO/*CHO), while suppressing ethylene formation. This enables highly selective C 2+ oxygenate production with 68% Faradaic efficiency at 200 mA cm -2 . This strategy highlights a generalizable design principle for engineering high-performance eCO 2 RR catalysts with enhanced C 2+ oxygenate selectivity. • Hydroxyl-mediated interface stabilizes Cu δ+ at high current densities. • Oxophilic, asymmetric microenvironment retains *OCCHO/*CHO intermediates. • Achieving 68% C 2+ oxygenate selectivity at 200 mA cm -2 in a 5cm 2 MEA.
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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 | 0.000 | 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".