Key Words:TOTAL-ENERGY CALCULATIONS; WAVE
Abstract:The production of three separated, high-value chemicals (H2O2, urea and H-2) from CO2, N-2, and H2O represents a significant challenge. It is a prospective and innovative way to simultaneously produce these chemicals in an anion exchange membrane (AEM) electrolyzer, which couples anodic 2e- water oxidation (2e-WOR) and cathodic CO2, N-2 and water reduction reaction (CNWRR), but has not yet been realized. Here, we found that bifunctional CuxTi(1-x)O(2-y) catalysts can be employed in the electrochemical production of H2O2, urea and H-2 from CO2, N-2 and water, and the optimized Cu0.12Ti0.88O2-y catalyst exhibits an excellent productivity of 11.8 mu mol cm(- 2) min(- 1), 0.3 mg cm(-2)h(- 1) and 0.82 mmol cm(-2)h(- 1) for H2O2, urea and H-2 at 4.0 V (50 mA cm(- 2)) in AEM electrolyzer, respectively. Theoretical calculations reveal that the superior performance of the 2e-WOR and CNWRR is attributed to the Cu doping effect, which not only promotes the coupling of *OH but also optimizes the adsorption energy barriers of COOH* and NNH*. It is worth noting that the AEM electrolyzer assembled by bifunctional Cu0.12Ti0.88O2-y reaches a current density of 50 mA cm(-2) with a cell voltage of 4.0 V and exhibits excellent stability of 50-hour continuous operation.
Volume:499
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Translation or Not:no