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基于Ce-UiO-66金属有机骨架的NiSe/CeO催化剂及其对甲醇、尿素和甘油的电催化氧化

NiSe/CeO catalysts from Ce-UiO-66 metal-organic skeletons and their electrocatalytic oxidation of methanol, urea and glycerol.

作者信息

Huo Jiaqi, Chang Ying, Xu Aiju, Jia Meilin, Jia Jingchun

机构信息

College of Chemistry and Environmental Science, Inner Mongolia Key Laboratory of Green Catalysis and Inner Mongolia Collaborative Innovation Center for Water Environment Safety, Inner Mongolia Normal University, Hohhot, 010022, China.

出版信息

Phys Chem Chem Phys. 2024 Mar 20;26(12):9413-9423. doi: 10.1039/d3cp06273b.

Abstract

Hydrogen is a viable alternative energy source to fossil fuels. In order to manufacture enough hydrogen to meet the needs of social growth, finding an alternate energy source that is more effective is essential. Electrochemical water cracking is a more appropriate method for producing hydrogen. The methanol oxidation reaction (MOR), urea oxidation reaction (UOR) and glycerol oxidation reaction (GOR) can be used to replace the anodic oxygen evolution reaction (OER) and indirectly accelerate the hydrogen evolution reaction (HER), which has the advantages of saving energy and reducing environmental pollution. In this study, Ni/CeO catalysts were prepared by thermal annealing of MOFs (Ce-UiO-66) containing nickel species and NiSe/CeO nanocrystalline catalysts were obtained through the selenation reaction at different temperatures. The NiSe/CeO-450 °C catalysts exhibited superior catalytic performance for the MOR, UOR, and GOR. The MOR showed a peak current density of roughly 186.68 mA cm and a low oxidation potential of around 1.34 V. Similarly, the UOR demonstrated a peak current density of approximately 142.28 mA cm and a low oxidation potential of around 1.32 V. Furthermore, the GOR exhibited a peak current density of approximately 82.56 mA cm and a low oxidation potential of around 1.37 V. NiSe/CeO-450 °C could improve electrocatalytic performance for the MOR, UOR, and GOR, which is attributed to the more active sites that were exposed as a result of utilizing MOFs (Ce-UiO-66) as a precursor. Additionally, selenation increased the ability to transfer electrons. This research is crucial for the production of inexpensive, easily accessible transition metals in place of expensive noble metals, for the reduction of wastewater pollution from methanol and urea, and for the creation of effective anodic oxidation electrocatalysts.

摘要

氢是化石燃料的一种可行替代能源。为了制造足够的氢以满足社会发展的需求,找到一种更高效的替代能源至关重要。电化学水裂解是一种更合适的制氢方法。甲醇氧化反应(MOR)、尿素氧化反应(UOR)和甘油氧化反应(GOR)可用于替代阳极析氧反应(OER)并间接加速析氢反应(HER),具有节能和减少环境污染的优点。在本研究中,通过对含镍物种的金属有机框架材料(Ce-UiO-66)进行热退火制备了Ni/CeO催化剂,并通过在不同温度下的硒化反应获得了NiSe/CeO纳米晶催化剂。NiSe/CeO-450°C催化剂对MOR、UOR和GOR表现出优异的催化性能。MOR的峰值电流密度约为186.68 mA cm,氧化电位约为1.34 V。同样,UOR的峰值电流密度约为142.28 mA cm,氧化电位约为1.32 V。此外,GOR的峰值电流密度约为82.56 mA cm,氧化电位约为1.37 V。NiSe/CeO-450°C可以提高对MOR、UOR和GOR的电催化性能,这归因于以金属有机框架材料(Ce-UiO-66)为前驱体而暴露出更多的活性位点。此外,硒化提高了电子转移能力。这项研究对于生产廉价、易于获得的过渡金属以替代昂贵的贵金属、减少甲醇和尿素产生的废水污染以及制备有效的阳极氧化电催化剂至关重要。

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