An integrated photocatalytic redox architecture for simultaneous overall conversion of CO2 and H2O toward CH4 and H2O2
Why this work is in the frame
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Bibliographic record
Abstract
Solar-driven overall conversion of CO 2 and H 2 O into fuels and chemicals shows an ultimate strategy for carbon neutrality yet remains a huge challenge. Herein, an integrated photocatalytic redox architecture of Zn NPs/GaN Nanowires (NWs)/Si is explored for light-driven overall conversion of CO 2 and H 2 O into CH 4 and H 2 O 2 simultaneously without any external sacrificial agents and additives. The as-designed architecture affords a benchmark CH 4 activity of 189 mmol g cat −1 h −1 with a high selectivity of 93.6%, in the synchronized formation of H 2 O 2 at a considerable rate of 25 m g −1 h −1 . Moreover, a considerable turnover number of 27,280 mol CH 4 per mol Zn was achieved over a long-term operation of 80 h. By operando spectroscopic characterizations, isotope experiments, and density functional theory calculations, it is unraveled that Zn sites are synergetic with GaN to drive CO 2 -to-CH 4 conversion with a lowered energy barrier of 0.27 eV while inhibiting hydrogen evolution reaction with a relatively high energy barrier of 0.93 eV. Notably, owing to the unique surface properties of GaN, water is split into *OH and *H, followed by the formation of H 2 O 2 because of the alleviated adsorption strength of *OH by Zn NPs. Together, the hierarchical architecture enables the achievement of high activity and high selectivity of CH 4 from CO 2 reduction in distilled water along with the generation of H 2 O 2 . This work provides an integrated photocatalytic redox architecture for the synchronized production of CH 4 and H 2 O 2 with the only inputs of CO 2 , distilled water, and light.
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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 | 0.001 |
| 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 it