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一种使用浸渍有氢氧化镍纳米颗粒的天然磷酸盐的可持续方法:一种用于酒精氧化的经济高效解决方案。

A sustainable approach using natural phosphates impregnated with nickel hydroxide nanoparticles: a cost-effective solution for alcohol oxidation'.

作者信息

Chemchoub Sanaa, El Attar Anas, Belgada Abdessamad, Younssi Saad Alami, Jama Charafeddine, Bentiss Fouad, El Rhazi Mama

机构信息

University of Hassan II of Casablanca, Faculty of Sciences and Technology, Laboratory of Materials, Membranes and Environment-BP 146 20650 Mohammedia Morocco

Univ. Lille, CNRS, INRAE, Centrale Lille, UMET - Unité Matériaux et Transformations UMR 8207 F-59000 Lille France.

出版信息

Nanoscale Adv. 2024 Dec 6;7(2):583-600. doi: 10.1039/d4na00850b. eCollection 2025 Jan 14.

Abstract

This study introduces a novel and effective approach for the electrocatalytic oxidation of alcohols, showcasing the development of a highly active and cost-effective anode catalyst for methanol and ethanol. A dual-embedded Ni electrode, named (Ni@NATPhos/Ni), is based on a carbon paste electrode modified with natural phosphate impregnated with nickel ions. A layer of nickel nanoparticles was then added electrochemical deposition, using a precise combination of wet impregnation and potentiostatic electrodeposition techniques. Characterization using XRD and TEM revealed the formation of crystalline structures such as nickel pyrophosphate (NiPO) and orthophosphate (Ni(PO)), along with nickel hydroxides (Ni(OH)), resulting in well-distributed homogenous nickel nanosized particles of approximately 30 nm. The electrocatalytic performance of Ni@NATPhos/Ni was assessed and compared with an unmodified carbon paste electrode in alkaline media. With peak current densities of 110 mA cm for methanol and 83 mA cm for ethanol oxidation, the synthesized catalyst demonstrated significantly improved catalytic efficiency. After 500 CV cycles, the dual-embedded electrode Ni@NATPhos/Ni demonstrated excellent stability, retaining 70.33% and 61.58% of its initial current values for ethanol and methanol, respectively, and exhibiting high tolerance to intermediate species poisoning. Electrochemical impedance spectroscopy (EIS) conducted after stability testing revealed an increase in solution resistance, indicative of the complete oxidation of intermediate species in the alkaline solution. The synthesized Ni@NATPhos/Ni electrode emerges as a promising and robust catalyst for alcohol oxidation reactions, offering significant advancements in electrocatalytic efficiency and stability.

摘要

本研究介绍了一种新颖且有效的醇类电催化氧化方法,展示了一种用于甲醇和乙醇的高活性且经济高效的阳极催化剂的开发。一种名为(Ni@NATPhos/Ni)的双嵌入镍电极,基于用浸渍镍离子的天然磷酸盐修饰的碳糊电极。然后通过湿浸渍和恒电位电沉积技术的精确组合,采用电化学沉积法添加了一层镍纳米颗粒。使用XRD和TEM进行的表征揭示了焦磷酸镍(NiPO)和正磷酸盐(Ni(PO))等晶体结构的形成,以及氢氧化镍(Ni(OH)),从而形成了分布均匀的约30 nm的均匀镍纳米颗粒。在碱性介质中评估了Ni@NATPhos/Ni的电催化性能,并与未修饰的碳糊电极进行了比较。对于甲醇氧化,峰值电流密度为110 mA cm,对于乙醇氧化,峰值电流密度为83 mA cm,合成的催化剂表现出显著提高的催化效率。在500次循环伏安循环后,双嵌入电极Ni@NATPhos/Ni表现出优异的稳定性,乙醇和甲醇分别保留其初始电流值的70.33%和61.58%,并且对中间物种中毒表现出高耐受性。稳定性测试后进行的电化学阻抗谱(EIS)显示溶液电阻增加,表明碱性溶液中的中间物种被完全氧化。合成的Ni@NATPhos/Ni电极成为醇类氧化反应中一种有前途且稳健的催化剂,在电催化效率和稳定性方面取得了显著进展。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4465/11730763/8b2d238f6459/d4na00850b-f1.jpg

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