College of Materials Science and Engineering, Key Laboratory of Optoelectronic Devices and Systems, College of Physics and Optoelectronic Engineering, Shenzhen University, Shenzhen 518060, China.
College of Materials Science and Engineering, Key Laboratory of Optoelectronic Devices and Systems, College of Physics and Optoelectronic Engineering, Shenzhen University, Shenzhen 518060, China.
J Environ Sci (China). 2023 Jul;129:152-160. doi: 10.1016/j.jes.2022.08.023. Epub 2022 Aug 23.
Urea oxidation reaction (UOR) provides a method for hydrogen production besides wastewater treatment, but the current limited catalytic activity has prevented the application. Herein, we develop a novel HO treatment strategy for tailoring the surface oxygen ligand of NiFe-layered double hydroxides (NiFe-LDH). The sample after HO treatment (NiFeO-LDH) shows significant enhancement on UOR efficiency, with the potential of 1.37 V (RHE) to reach a current density of 10 mA/cm. The boost is attributed to the richness adsorption O ligand on NiFeO-LDH as revealed by XPS and Raman analysis. DFT calculation indicates formation of two possible types of oxygen ligands: adsorbed oxygen on the surface and exposed from hydroxyl group, lowered the desorption energy of CO product, which lead to the lowered onset potential. This strategy is further extended to NiFe-LDH nano sheet on Ni foam to reach a higher current density of 440 mA/cm of UOR at 1.8 V (RHE). The facile surface O ligand manipulation is also expected to give chance to many other electro-catalytic oxidations.
尿素氧化反应 (UOR) 除了用于污水处理外，还提供了一种制氢的方法，但目前有限的催化活性阻碍了其应用。在此，我们开发了一种新的 HO 处理策略，用于调整 NiFe 层状双氢氧化物 (NiFe-LDH) 的表面氧配体。经过 HO 处理的样品 (NiFeO-LDH) 对 UOR 效率有显著的提高作用，在 RHE 下达到 1.37 V 的电位时可达到 10 mA/cm 的电流密度。这种提升归因于 XPS 和拉曼分析表明 NiFeO-LDH 上富含吸附 O 配体。DFT 计算表明形成了两种可能的氧配体类型：表面吸附氧和来自羟基的暴露氧，降低了 CO 产物的脱附能，从而降低了起始电位。该策略进一步扩展到 Ni 泡沫上的 NiFe-LDH 纳米片，在 1.8 V (RHE) 时 UOR 的电流密度可达到 440 mA/cm。这种简便的表面 O 配体调控策略也有望为许多其他电催化氧化反应提供机会。
