Key Laboratory of Automobile Materials, Ministry of Education, and School of Materials Science and Engineering, Jilin University, Changchun, 130022, China.
Small. 2023 Apr;19(17):e2207661. doi: 10.1002/smll.202207661. Epub 2023 Jan 31.
Electrochemical reduction of nitrate to ammonia (NH ) not only offers a promising strategy for green NH synthesis, but also addresses the environmental issues and balances the perturbed nitrogen cycle. However, current electrocatalytic nitrate reduction processes are still inefficient due to the lack of effective electrocatalysts. Here 3D nanoporous Cu/MnO hybrids are reported as efficient and durable electrocatalysts for nitrate reduction reaction, achieving the NH yield rates of 5.53 and 29.3 mg h mg with 98.2% and 86.2% Faradic efficiency in 0.1 m Na SO solution with 10 and 100 mm KNO , respectively, which are higher than those obtained for most of the reported catalysts under similar conditions. Both the experimental results and density functional theory calculations reveal that the interface effect between Cu/MnO interface could reduce the free energy of rate determining step and suppress the hydrogen evolution reaction, leading to the enhanced catalytic activity and selectivity. This work provides an approach to design advanced materials for NH production via electrochemical nitrate reduction.
电化学还原硝酸盐为氨（NH ）不仅为绿色 NH 合成提供了有前景的策略，而且还解决了环境问题并平衡了受干扰的氮循环。然而，由于缺乏有效的电催化剂，当前的电催化硝酸盐还原过程仍然效率低下。在此，报道了 3D 纳米多孔 Cu/MnO 杂化物作为硝酸盐还原反应的高效且耐用的电催化剂，在 0.1 m Na 2 SO 4 溶液中分别在 10 和 100 mm KNO 3 下，NH 3 产率速率达到 5.53 和 29.3 mg h·mg -1 ，并且具有 98.2%和 86.2%的法拉第效率，这高于在类似条件下大多数报道的催化剂所获得的产率。实验结果和密度泛函理论计算都表明，Cu/MnO 界面之间的界面效应可以降低速率决定步骤的自由能并抑制析氢反应，从而提高催化活性和选择性。这项工作为通过电化学硝酸盐还原生产 NH 3 提供了一种设计先进材料的方法。
