High-Throughput Co-Design of Catalysts and Organic Electrolytes for CO2-to-C2H4 Electrosynthesis

HTCo-Des will develop a systematic high-throughput (HT) platform to co-design non-aqueous electrolyte microenvironments and Cu-based high-entropy electrocatalysts (HEEs) for CO2-to-C2H4 conversion in parallel membrane-electrode-assembly (MEA) cells. The integrated HT workflow will accelerate discovery cycles, enforce standardisation and calibration, and minimise human bias through automation, generating reproducible, uncertainty-quantified structure-property maps of solvent/proton-donor-mediated interfacial effects to guide rational Cu-based HEEs design. The project will deliver the first quantitative design rules linking solvent-proton-donor chemistry and alloy composition to *CO coverage, *OCCO stabilisation, hydrogenation kinetics, and suppression of the hydrogen evolution reaction (HER). Factorial experiments will yield kinetic fingerprints (Tafel slopes, apparent activation energies, reaction orders) and degradation maps from accelerated stress tests, enabling predictive control of selectivity and durability. Complementary ex-situ and in-situ studies, together with rigorous electrochemical benchmarking, will establish electronic-structure/structure-property relationships that explain why specific HEEs and microenvironments favour C-C coupling. Under optimised conditions we target ≥85% faradaic efficiency to C2H4 and ≥100 mA cm-2 C2H4 partial current density sustained for ≥150 h, with ≤10% loss in C2H4 FE and ≤100 mV rise in cell voltage. These outcomes will advance CO2 electrolysis performance, bringing the technology closer to practical deployment and supporting decarbonisation of the chemical industry.