Rational Design of Hydroxyl‐Rich Ti3C2Tx MXene Quantum Dots for High‐Performance Electrochemical N2 Reduction

To enable an efficient and cost‐effective electrocatalytic N2 reduction reaction (NRR) the development of an electrocatalyst with a high NH3 yield and good selectivity is required. In this work, Ti3C2Tx MXene‐derived quantum dots (Ti3C2Tx QDs) with abundant active sites enable the development of efficient NRR electrocatalysts. Given surface functional groups play a key role on the electrocatalytic performance, density functional theory calculations are first conducted, clarifying that hydroxyl groups on Ti3C2Tx offer excellent NRR activity. Accordingly, hydroxyl‐rich Ti3C2Tx QDs (Ti3C2OH QDs) are synthesized as NRR catalysts by alkalization and intercalation. This material offers an NH3 yield and Faradaic efficiency of 62.94 µg h−1 mg−1cat. and 13.30% at −0.50 V, respectively, remarkably higher than reported MXene catalysts. This work demonstrates that MXene catalysts can be mediated through the optimization of both QDs sizes and functional groups for efficient ammonia production at room temperature. Hydroxyl‐rich MXene Ti3C2Tx quantum dots (Ti3C2OH QDs) are rationally designed for electrochemical nitrogen fixation. This material possesses increased active sites (Ti‐edge) and optimized surface functional groups (OH) based on the computational effort. The electrocatalyst exhibits high performance and excellent selectivity synchronously with the NH3 yield and Faradaic efficiency of 62.94 µg h−1 mg−1cat. And 13.30% at −0.50 V, respectively.