Inverse ZnO/AuCu Electrocatalyst Enabling Tunable CO-Rich Syngas for Electrified Carbon Cycling in Steelmaking

Electrochemical CO2 reduction (CO2RR) presents a scalable route to decarbonize steelmaking by producing CO-rich syngas from captured CO2 and renewable electricity. Here, we report an inverse ZnO/AuCu electrocatalyst with a tunable oxide-metal interface. The catalyst achieves a CO Faradaic efficiency of 85.6% and a current density of −158.2 mA cm–2 at −1.0 V vs. RHE, demonstrating industrial-level performance. The engineered interface enables precise control over the CO/H2 ratio in the produced syngas, spanning from 0.3 to 10.3. This flexibility allows for tailoring the syngas to align with the thermochemical requirements of iron ore reduction. density functional theory (DFT) calculations reveal that the ZnO/AuCu interface synergistically promotes CO2 activation by lowering the energy barrier for the rate-determining *COOH formation, resulting from an elevated d-band center, and a reduced work function. Life cycle assessment (LCA) demonstrates that integrating ZnO/AuCu catalyst into blast furnace workflows could reduce CO2 emissions by ∼80% and improve electricity utilization by an order of magnitude relative to fossil-based pathways. This work establishes a materials-driven strategy that bridges catalyst design and industrial carbon recycling, paving the way for sustainable steel manufacturing.