Single-Phase Spinel NiCo<sub>2</sub>O<sub>4</sub> as Highly Active and Stable Electrocatalysts for Urea Oxidation Reaction in Urea Electrolysis

W4413980353 · 수집 2026-10-04 18:16:39

T10030 Electrocatalysts for Energy Conversion

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Exploring and designing a stable and active catalyst for the urea electro-oxidation reaction (UOR, CO-(NH2)2 + 6OH- → CO2 + N2 + 5H2O + 6e-) is crucial for the long-term sustainability of ecological systems and clean energy production. We found that spinel NiCo2O4 is a stable and active electrocatalyst for UOR at a relatively low anodic potential without triggering the competing oxygen evolution reaction (OER). A urea electrolysis cell (CO-(NH2)2 + H2O → CO2 + N2 + 2H2) utilizing a spinel NiCo2O4 anode and a commercial Pt cathode was further characterized through galvanostatic polarization tests, demonstrating excellent structural stability at various current densities. Post-mortem analysis of long-term urea electrolysis measurements suggested that NiCo2O4 electrocatalysts maintained a stable spinel structure. However, redistribution of Ni3+ to Ni2+ valence on the catalyst surface was observed, in contrast to the intact Co valence, indicating that (i) Ni sites are active toward urea adsorption and sequential electro-oxidation; (ii) while urea oxidation proceeds primarily through the direct electro-oxidation mechanism, chemical reactions between the Ni3+ site and urea occur during long-term electrochemical UOR operation. Density functional theory (DFT) simulations were used to calculate the adsorption energies of urea molecules on NiO, Co3O4, and NiCo2O4, revealing the importance of regulating the configuration of adsorbed urea molecules on the NiCo2O4 surface.

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