Electrochemical Systems for CO2 Electrolysis and Hydrocarbon Upgrade
Bibliographic record
Abstract
This thesis investigates electrochemical reactions and systems that produce fuels and commodity chemicals, specifically focusing on cathodic CO2 electroreduction in acidic media and the anodic electrooxidation of ethylene and propylene. It combines detailed experimental work and theoretical analysis to advance our understanding of these pivotal reactions.CO2 electroreduction (CO2R) is emerging as a method for transforming carbon emissions into valuable chemicals and fuels. Traditionally, the productive reduction of CO2 to multicarbon products has been limited, with less than 2% efficiency; the majority reacts with hydroxide, forming carbonate in alkaline and neutral reactors. This work demonstrates that, in acidic conditions, a high CO2 utilization rate of 77% can be achieved by suppressing hydrogen evolution through the strategy of applying high concentration of surface alkali cations. In this new system, I recognize a limit in stability due to the high alkali concentration; and a limit in selectivity to multicarbon products due to the local pH. Addressing the stability issues associated with high alkali cation concentrations, I then introduce a fixed cation-modified electrode that enhances stability (operating over 150 hours in an alkali cation-free electrolyte) and performance by optimizing the local reaction environment. On the anodic front, I identified hydrocarbon oxidation as a promising new anodic reaction, offering a high-revenue alternative to the traditional oxygen evolution reaction. This highlights the potential for electrochemical oxidation of ethylene and propylene into ethylene glycol and propylene glycol, respectively, using renewable electricity. Initial studies delve into the reaction mechanisms, energy of surface intermediates, and catalyst phase changes that influence glycol selectivity, investigations in which I employ a combination of experimental and computational techniques. The findings offer guidelines for the design of catalysts and systems that complement CO2 electrolysis in scale and efficiency. Overall, this thesis provides insights and methodologies applicable to renewable energy and the sustainable production of fuels and chemicals.
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How this classification was reachedexpand
Full frame machine prediction
Teacher imitationNot calibrated prevalence, not ground truth. Human validation pending. The Gemma side is a direct model label for every work in the frame, read from the title-only record. The Codex side is a classifier learned from the 10,348 direct Codex labels and calibrated to design-weighted sample rates; fields without enough sample support carry no Codex call. Candidate is the union of the two sides; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels.
Distilled classifier scores by category (both heads)
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.001 | 0.001 |
| Meta-epidemiology (narrow) | 0.001 | 0.000 |
| Meta-epidemiology (broad) | 0.001 | 0.000 |
| Bibliometrics | 0.001 | 0.001 |
| Science and technology studies | 0.001 | 0.001 |
| Scholarly communication | 0.001 | 0.002 |
| Open science | 0.001 | 0.001 |
| Research integrity | 0.001 | 0.002 |
| Insufficient payload (model declined to judge) | 0.006 | 0.004 |
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 source (direct Gemma or distilled Codex), 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".