H2O2 treatment boosts activity of NiFe layered double hydroxide for electro-catalytic oxidation of urea

IF 6.9 Q1 Environmental Science Journal of environmental sciences Pub Date : 2023-07-01 DOI:10.1016/j.jes.2022.08.023
Jinshan Wei , Jin Wang , Xiaoming Sun
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Abstract

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 H2O2 treatment strategy for tailoring the surface oxygen ligand of NiFe-layered double hydroxides (NiFe-LDH). The sample after H2O2 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/cm2. 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 CO2 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/cm2 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.

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H2O2处理提高了NiFe层状双氢氧化物电催化氧化尿素的活性
尿素氧化反应(UOR)除了为废水处理提供了一种制氢方法,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H2O2处理策略,用于定制NiFe层状双氢氧化物(NiFe-LDH)的表面氧配体。H2O2处理后的样品(NiFeO-LDH)显示出UOR效率的显著提高,电势为1.37V(RHE)以达到10mA/cm2的电流密度。如XPS和拉曼分析所揭示的,这种增强归因于O配体在NiFeO LDH上的富集吸附。DFT计算表明,形成了两种可能类型的氧配体:吸附在表面的氧和暴露在羟基上的氧,降低了CO2产物的解吸能,从而降低了起始电位。该策略进一步扩展到泡沫镍上的NiFe-LDH纳米片,以在1.8V(RHE)下达到440mA/cm2的UOR的更高电流密度。简单的表面O配体操作也有望为许多其他电催化氧化提供机会。
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来源期刊
Journal of environmental sciences
Journal of environmental sciences Environmental Science (General)
CiteScore
12.80
自引率
0.00%
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0
审稿时长
17 days
期刊介绍: Journal of Environmental Sciences is an international peer-reviewed journal established in 1989. It is sponsored by the Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, and it is jointly published by Elsevier and Science Press. It aims to foster interdisciplinary communication and promote understanding of significant environmental issues. The journal seeks to publish significant and novel research on the fate and behaviour of emerging contaminants, human impact on the environment, human exposure to environmental contaminants and their health effects, and environmental remediation and management. Original research articles, critical reviews, highlights, and perspectives of high quality are published both in print and online.
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