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天然高岭土基氧化铜催化剂的简便合成:一种用于催化还原4-硝基苯酚的高效多相催化剂。

Facile Synthesis of Natural Kaolin-Based CuO Catalyst: An Efficient Heterogeneous Catalyst for the Catalytic Reduction of 4-Nitrophenol.

作者信息

Asmare Zinabu Gashaw, Aragaw Belete Asefa, Atlabachew Minaleshewa

机构信息

Chemistry Department, College of Science, Bahir Dar University, PO Box 79 Bahir Dar, Ethiopia.

Chemistry Department, College of Natural and Computational Sciences, Debre Tabor University, PO Box 272 Debre Tabor, Ethiopia.

出版信息

ACS Omega. 2024 Nov 21;9(49):48014-48031. doi: 10.1021/acsomega.4c04029. eCollection 2024 Dec 10.

Abstract

Water contamination by nitro compounds from various industrial processes has significantly contributed to environmental pollution and severely threatened aquatic ecosystems. Inexpensive, efficient, and environmentally benign catalysts are required for the catalytic reduction of such nitro compounds. This study reports the fabrication of various nanocomposites (NCs) of copper oxide nanoparticles (CuO NPs) supported on a kaolin sheet using straightforward and simple one-pot synthesis procedures that control the metal precursor to kaolin ratios. The selected as-synthesized CuO/kaolin NC was characterized using a range of advanced spectroscopic and microscopic methods, such as X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), ultraviolet-visible (UV-vis) spectroscopy, field emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), energy dispersive X-ray spectroscopy (EDX), high-angle annular dark-field scanning TEM (HAADF-STEM), and N adsorption/desorption analysis. The characterization results confirmed the successful incorporation of CuO NPs into the kaolin sheets, which had an average size of about 18.7 nm. The fabricated CuO/kaolin NC was used as a heterogeneous catalyst for the efficient reduction of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) in the presence of sodium borohydride (NaBH) in an aqueous system at room temperature. The catalyst demonstrated superior catalytic performance with high 4-NP conversion into 4-AP (>99%) in the aqueous phase (50 mL, 20 mg L) within 6 min. In addition, the reaction kinetics of 4-NP reduction was also investigated, and the reaction followed the pseudo-first-order kinetics equation with the apparent rate constant of 1.76 min. Furthermore, the Arrhenius and Eyring parameters for the catalytic hydrogenation reaction of 4-NP were calculated in order to investigate the catalytic reaction process in more detail. Moreover, the catalyst exhibited excellent reusability and stability over seven repeated catalytic test cycles without any noticeable decline in catalytic activity. Therefore, this paper could provide a novel, efficient, and environmentally promising clay-based non-noble metal oxide nanocatalyst to reduce nitro compounds in the aqueous system.

摘要

各种工业过程中产生的硝基化合物对水的污染已严重加剧了环境污染,并对水生生态系统构成了严重威胁。催化还原此类硝基化合物需要廉价、高效且环境友好的催化剂。本研究报告了使用简单直接的一锅合成法制备负载在高岭土片层上的各种氧化铜纳米颗粒(CuO NPs)纳米复合材料(NCs),该方法可控制金属前驱体与高岭土的比例。使用一系列先进的光谱和显微镜方法对合成的CuO/高岭土NC进行了表征,如X射线衍射(XRD)、傅里叶变换红外光谱(FT-IR)、紫外可见(UV-vis)光谱、场发射扫描电子显微镜(FE-SEM)、透射电子显微镜(TEM)、能量色散X射线光谱(EDX)、高角度环形暗场扫描TEM(HAADF-STEM)和N吸附/脱附分析。表征结果证实了CuO NPs成功掺入高岭土片层中,其平均尺寸约为18.7 nm。制备的CuO/高岭土NC在室温下的水体系中,用作非均相催化剂,在硼氢化钠(NaBH)存在下将4-硝基苯酚(4-NP)高效还原为4-氨基苯酚(4-AP)。该催化剂表现出优异的催化性能,在水相(50 mL,20 mg/L)中于6分钟内将4-NP转化为4-AP的转化率高达99%以上。此外,还研究了4-NP还原的反应动力学,该反应遵循准一级动力学方程,表观速率常数为1.76 min⁻¹。此外,计算了4-NP催化加氢反应的阿伦尼乌斯参数和艾林参数,以便更详细地研究催化反应过程。此外,该催化剂在七个重复催化测试循环中表现出优异的可重复使用性和稳定性,催化活性没有明显下降。因此,本文可为在水体系中还原硝基化合物提供一种新型、高效且具有环境前景的粘土基非贵金属氧化物纳米催化剂。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/eb58/11635686/5b91a66f0c96/ao4c04029_0001.jpg

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