Tianjin Key Laboratory of Structure and Performance for Functional Molecules, College of Chemistry, Tianjin Normal University, Tianjin 300387, China.
Molecules. 2023 Mar 20;28(6):2781. doi: 10.3390/molecules28062781.
Electrochemical nitrogen reduction reaction (ENRR) offers a sustainable alternative to the environmentally hazardous Haber-Bosch process for producing ammonia. However, it suffers from an unsatisfactory performance due to its limited active sites and competitive hydrogen evolution reaction. Herein, we design a hydrophobic oleylamine-modified zeolitic imidazolate framework-coated nanoporous silver composite structure (NPS@O-ZIF). The composite achieves a high ammonia yield of (41.3 ± 0.9) μg·h·cm and great Faradaic efficiency of (31.7 ± 1.2)%, overcoming the performances of NPS@ZIF and traditional silver nanoparticles@O-ZIF. Our strategy affords more active sites and accessible channels for reactant species due to the porous structure of NPS cores and restrains the evolution of hydrogen by introducing the hydrophobic molecule coated on the ZIF surfaces. Hence, the design of the hydrophobic core-shell composite catalyst provides a valuably practical strategy for ENRR as well as other water-sensitive reactions.
电化学氮还原反应（ENRR）为生产氨提供了一种替代哈伯-博世工艺的可持续方法，该工艺对环境有害。然而，由于其活性位点有限和竞争的析氢反应，其性能仍不尽如人意。在此，我们设计了一种疏水性油胺修饰的沸石咪唑酯骨架涂覆的纳米多孔银复合结构（NPS@O-ZIF）。该复合材料实现了（41.3 ± 0.9）μg·h·cm 的高氨产率和（31.7 ± 1.2）%的优异法拉第效率，超过了 NPS@ZIF 和传统的银纳米颗粒@O-ZIF 的性能。由于 NPS 核的多孔结构，我们的策略为反应物种提供了更多的活性位点和可及的通道，并通过在 ZIF 表面涂覆疏水分子来抑制氢气的演化。因此，疏水核壳复合催化剂的设计为 ENRR 以及其他对水敏感的反应提供了一种非常有价值的实用策略。
