Degree
Master of Science (MS)
Department
Chemistry
Document Type
Thesis
Abstract
Electrochemical CO2 reduction (eCO2RR) offers a sustainable route to convert CO2 into value-added fuels and chemicals, particularly multicarbon (C2+) products due to their higher energy density and economic value compared to C1 counterparts. Industrial adoption of eCO2RR technology is hindered by the difficulty in stably reaching superior Faradaic efficiency (FE) for C2+ products at ≥ 200 mA cm-2 at low applied overpotential due to sluggish C–C coupling kinetics, competing reactions, and catalyst instability. Hence, we examine the recent advances in eCO2RR catalyst engineering strategies, such as nanostructural and electronic modifications of Cu-based catalysts (e.g., interfacial, surface, facet, and defect engineering, doping/alloying, and tandem/cascade catalysis) and emerging non-Cu systems (e.g., Ni2P, Ni-Ga and Pd-Au alloys, MOF-derived heterostructures, high-entropy alloys/oxides, and metal-free systems containing B/N co-doped Lewis pair catalysts that break conventional scaling relations) for high-current C2+ production. Mechanistic insights into C–C coupling pathways for the selective formation of C2+ hydrocarbons/oxygenates are summarized alongside system-level optimizations involving cell configurations, paired electrolysis, and electrolyte engineering to overcome mass transport limitations and reduce energy penalties. The study revealed that Cu-based systems, such as pure-water-fed flow-based MEAs, could achieve up to 87% ������2+ at ����2+ > 4.35 A cm-2 for ~1,000 h. However, our techno-economic analysis indicates that only ~3.4% of the 203 examined catalytic systems meet industrial benchmarks of ����2+ ≥200 mA cm-2, stability ≥100 h, and ������2+ ≥80%. Future eCO2RR system designs should be engineered to selectively produce single C2+ products using scalable cell architectures towards industrial deployment for carbon-neutral chemical manufacturing solutions.
Date
2-6-2026
Recommended Citation
Edor, Godwin Uche, "Emerging Catalysts and System Designs for High-Current-Density CO2 Electroreduction to Multicarbon Fuels and Chemicals Toward Industrial-Scale Applications" (2026). Masters Theses. 21.
https://scholarshub.louisiana.edu/masters_theses/21
DOI
https://proquest.com/docview/3347849821
First Committee Chair
Hui Yan
First Committee Member
August Gallo
Second Committee Member
Thomas Junk